Дисертації: "HYBRID ELECTROCHEMICAL"

1

Agrawal, Richa. "Hybrid Electrochemical Capacitors: Materials, Optimization, and Miniaturization." FIU Digital Commons, 2018. https://digitalcommons.fiu.edu/etd/3680.

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With the ever-advancing technology, there is an incessant need for reliable electrochemical energy storage (EES) components that can provide desired energy and power. At the forefront of EES systems are electrochemical capacitors (ECs), also known as supercapacitors that typically have higher power and superior cycle longevity but lower energy densities than their battery counterparts. One of the routes to achieve higher energy density for ECs is using the hybrid EC configuration, which typically utilizes a redox electrode coupled with a counter double-layer type electrode. In this dissertation, both scale-up (coin-cell type) as well as scale-down (on-chip miniaturized) hybrid ECs were designed, constructed and evaluated. The first part of the dissertation comprised material identification, syntheses, and electrochemical analyses. Lithium titanate-anatase titanium oxide (Li4Ti5O12-TiO2) composites were synthesized via electrostatic spray deposition (ESD) and characterized in both half-cell and full-cell assembly against lithium and nanostructured carbon based counter electrodes, respectively. The second redox type material studied for hybrid electrochemical capacitors was ESD derived manganese oxide (MnOx). The MnOx electrodes exhibited a high gravimetric capacitance of 225F g-1 in aqueous media. Further improvement in the rate handling of the MnOx electrodes was achieved by using CNT additives. The MnOx-CNT composites were tested in full-cell assembly against activated carbon counter electrodes and tested for different anode and cathode mass ratios in order to achieve the best energy-power tradeoff, which was the second major goal of the dissertation. The optimized hybrid capacitor was able to deliver a high specific energy density of 30.3 Wh kg-1 and a maximal power density of 4kW kg-1. The last part of the dissertation focused on a scale-down miniaturized hybrid microsupercapacitor; an interdigitated electrode design was adopted in order to shorten the ion-transport pathway, and MnOx and reduced graphene oxide (rGO) were chosen as the redox and double layer components, respectively. The hybrid microsupercapacitor was able to deliver a high stack energy density of 1.02 mWh cm-3 and a maximal stack power density of 3.44 W cm-3, both of which are comparable with thin-film batteries and commercial supercapacitor in terms of volumetric energy and power densities.

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2

Fu, Xuewei. "Graphene-V2O5 Hybrid Aerogels As Electrode Materials For Electrochemical Capacitors." University of Akron / OhioLINK, 2015. http://rave.ohiolink.edu/etdc/view?acc_num=akron1430499247.

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3

Syed, Khurram Raza. "Electrochemical generation of hydrogen." Thesis, Brunel University, 2017. http://bura.brunel.ac.uk/handle/2438/13813.

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Global warming and the energy crisis are two of the greatest challenges on which mankind is currently focused. This has forced governments and other organisations to think how to protect the environment and how to reduce fuel costs. A variety of new and exciting technologies are being investigated to address the energy problem. Alternative energy sources such as solar power, fuel cells, wind power and tidal waves are active areas of commercial and scientific pursuit. A major area of current research is moving towards the hydrogen economy and hydrogen based energy systems. Hydrogen can be produced in many ways, most commonly by steam reforming of hydrocarbon (70% to 85% thermal efficiency) but the downside is that it releases carbon mono oxide (CO)), compared with commercial PEM electrolysers where performance has been reported to be 56 -73% at normal temperature pressure(NTP) with zero carbon emission. Electrochemical production of hydrogen has several advantages: (i) It gives pure hydrogen. (ii) It allows portability (e.g. Solar energy could be used to power the electrochemical cell). (iii) It can be produced on demand. The generation of Hydrogen via electrolysis has been the subject of many studies over the last two hundred years. However, there is still room for further work to improve both the efficiency of the process and methods of storage of the gas. The cleanest method at present is to produce hydrogen by electrolysis, and the main focus of this research is to design and develop such a green energy fuel cell for on-demand application. The aim of the work presented in this thesis was to further investigate the electrolysis method for hydrogen production. An Electrochemical fuel cell contains a minimum of two electrodes: the positively charged electrode called the anode where oxygen bubble will form, and the second negatively charged electrode called the cathode, where hydrogen bubbles will form during a chemical reaction caused by applying electrical current between these electrode. The project was initiated with the objective of finding a low cost solution for on-demand hydrogen generation. To establish a starting point, the first cell (cell-1) design was based on the work of Stephen Barrie Chambers (see chapter 3) to check the performance levels. The fabrication of the cell-1 design resulted in a mixture of hydrogen and oxygen in the same chamber, which means the cell-1 design, has a possible fire and explosion hazard. The device also has the drawback of lower performance of hydrogen production; columbic efficiency is between 40% to 46% at 1 amp to 3 amp current in 30% KOH alkaline solution. However, the advantage of reproducing Stephen’s innovation is that it allowed a quick and deep understanding of hydrogen generation. This thesis presents recent work on the fabrication of low cost electrolysis cells containing continuous flow alkaline (KOH, up to 30%) electrolyte using low cost electrodes (stainless steel 316) and membranes based on ultrahigh molecular weight polyethylene (UHMW PE) to produce hydrogen without the hazard of fire and explosion. In this research an On-Demand Hydrogen Generation cell-3 achieved a 95% hydrogen generation coulombic efficiency, which is about 49% efficiency improvement as compared to the stainless steel electrode, and was 22% better than the nano structured electrode. The typical cell voltage is 2.5 V at current flow ranging from 30 to 120 mA cm-2 in 30% KOH electrolyte. The achievement here of such high efficiencies paves the way for more research in the areas of space management, electrode surface structure and flow control (based on the application requirement). This invention can be used for aeronautic, marine and automotive application as well as in many other areas.

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4

Meera, P. "Nafion based hybrid polymer electrolytes and nanocomposites: design and electrochemical investigations." Thesis(Ph.D.), CSIR-National Chemical Laboratory, Pune, 2009. http://dspace.ncl.res.in:8080/xmlui/handle/20.500.12252/2726.

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5

Djelad, Halima. "Syntesis of hybrid silica-organic materials for the development of electrochemical biosensing applications." Doctoral thesis, Universidad de Alicante, 2019. http://hdl.handle.net/10045/101152.

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6

Kanakaraj, Sathya Narayan. "Processing Carbon Nanotube Fibers for Wearable Electrochemical Devices." University of Cincinnati / OhioLINK, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224577754985.

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7

Klett, Matilda. "Electrochemical Studies of Aging in Lithium-Ion Batteries." Doctoral thesis, KTH, Tillämpad elektrokemi, 2014. http://urn.kb.se/resolve?urn=urn:nbn:se:kth:diva-145057.

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Lithium-ion batteries are today finding use in automobiles aiming at reducing fuel consumption and emissions within transportation. The requirements on batteries used in vehicles are high regarding performance and lifetime, and a better understanding of the interior processes that dictate energy and power capabilities is a key to strategic development. This thesis concerns aging in lithium-ion cells using electrochemical tools to characterize electrode and electrolyte properties that affect performance and performance loss in the cells. A central difficulty regarding battery aging is to manage the coupled effects of temperature and cycling conditions on the various degradation processes that determine the lifetime of a cell. In this thesis, post-mortem analyses on harvested electrode samples from small pouch cells and larger cylindrical cells aged under different conditions form the basis of aging evaluation. The characterization is focused on electrochemical impedance spectroscopy (EIS) measurements and physics-based EIS modeling supported by several material characterization techniques to investigate degradation in terms of properties that directly affect performance. The results suggest that increased temperature alter electrode degradation and limitations relate in several cases to electrolyte transport. Variations in electrode properties sampled from different locations in the cylindrical cells show that temperature and current distributions from cycling cause uneven material utilization and aging, in several dimensions. The correlation between cell performance and localized utilization/degradation is an important aspect in meeting the challenges of battery aging in vehicle applications. The use of in-situ nuclear magnetic resonance (NMR) imaging to directly capture the development of concentration gradients in a battery electrolyte during operation is successfully demonstrated. The salt diffusion coefficient and transport number for a sample electrolyte are obtained from Li+ concentration profiles using a physics-based mass-transport model. The method allows visualization of performance limitations and can be a useful tool in the study of electrochemical systems.

QC 20140512

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8

Carretero, González Nina Magali. "Iridium oxide-carbon hybrid materials as electrodes for neural systems. Electrochemical synthesis and characterization." Doctoral thesis, Universitat Autònoma de Barcelona, 2014. http://hdl.handle.net/10803/283440.

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El desarrollo de interfaces neuronales requiere el uso de nuevos materiales electroactivos y biocompatibles, que al aplicar campos eléctricos no causen efectos secundarios que pueden dañar los tejidos o degradar la funcionalidad del electrodo. A día de hoy, existen diferentes materiales electroactivos que se usan como electrodos en el sistema nervioso: oro, platino, carbón, Pt-Ir o IrOx entre otros, siendo este último el que ha mostrado superiores resultados. Una alta eficiencia electroquímica, estabilidad en condiciones biológicas y biocompatibilidad, han hecho del IrOx el material más prometedor como electrodo para estimulación y registro de señales neuronales. Sin embargo, los avances tecnológicos han generado una demanda de nuevos materiales con propiedades mejoradas y con menos inconvenientes que los actuales (bajos valores de capacidad de carga o la rigidez inherente de este tipo de óxidos, ya que presentan poca compatibilidad con los tejidos blandos). Estas mejoras se pueden conseguir con el uso de materiales híbridos, que unan las diferentes propiedades de los componentes. En este sentido, se han preparado electroquímicamente híbridos IrOx-CNTs, con propiedades mejoradas tras la adicción de nanotubos de carbono. La composición química de estos híbridos es muy parecida a la obtenida para IrOx, aunque la incorporación de nanotubos de carbono hace la superficie más rugosa, aumentando de esta manera el área superficial del material. Estas propiedades, junto con el aumento de la conductividad proporcionada por los nanotubos de carbono, tienen como consecuencia elevados valores de capacidad de carga electroquímica. También, la estabilidad de las capas resultantes mejora en comparación con las muestras de IrOx. Las pruebas de biocompatibilidad realizadas a las muestras IrOx-CNTs han mostrado una alta supervivencia y funcionalidad neural, parecida a la obtenida con IrOx o borosilicato (usado como referencia). Estos datos, validan este tipo de nuevos materiales como prometedores electrodos neurales. También se han preparado híbridos de IrOx con grafito y grafeno. En ambas capas, se ha observado la presencia de partículas de carbón, aunque la presencia de grafeno de única lámina no ha podido ser confirmada, y serán necesarios más experimentos. Las propiedades electroquímicas de estos híbridos, IrOx-grafito e IrOx-grafeno, son similares a las obtenidas para IrOx-CNTs, pero con mayores valores de capacidad de carga. Sin embargo, la estabilidad electroquímica es pobre para el híbrido de grafito, y finalmente la capa se despega, debido presuntamente, a la estructura heterogénea de los híbridos de grafito, en la cual, grandes partículas de carbón no están completamente introducidas en la matriz del IrOx. Híbridos de IrOx con grafeno dopado con nitrógeno se han preparado también, mostrando buenas propiedades y altos valores de capacidad de carga y estabilidad, incluso comparados con los resultados obtenidos para los híbridos con grafeno no dopado. El aumento de la conductividad en estos materiales se puede deber a la presencia de nitrógeno, que induce el aumento de defectos en las láminas de grafeno. La biocompatibilidad de estos materiales híbridos grafíticos está siendo estudiada. Tri-híbridos poliméricos también han sido sintetizados electroquímicamente, IrOx-PEDOT-CNTs. El uso de una matríz polimérica, ofrece más flexibilidad al futuro electrodo, lo que es deseable para aplicaciones en tejidos blandos. Sin embargo, los primeros resultados obtenidos muestran que el polímero encapsula los nanotubos de carbono y el IrOx, minimizando sus propiedades electroquímicas. Como consecuencia, la conducta electroquímica del material híbrido es muy similar a la obtenida en otros polímeros, como PEDOT-PSS. Las pruebas de biocompatibilidad para estos híbridos poliméricos muestran baja viabilidad neuronal, aunque un nuevo modelo de co-cultivos (astrocitos-neuronas) se ha propuesto para mejorar la biocompatibilidad en este tipo de materiales. Los materiales obtenidos en todos los casos, son capas bien adheridas, lo que permite su futuro uso como electrodos o substratos de crecimiento neuronal.
The development of neural interfaces requires new electroactive and biocompatible materials, capable to apply electric fields without secondary effects, as large impedances at the interface or radical formation, which can cause damage in the tissues and the degradation of the electrode functionality. Currently, different types of electroactive materials are available for application as electrodes in the neural system: gold, platinum, glassy carbon, Pt-Ir, TiN or IrOx, among others, being the last, the one with superior performance. Properties such as high electrochemical efficiencies, good bio-stability and significant biocompatibility, have turned out IrOx into one of the most promising material for neural recording and stimulation electrodes. However, new technological breakthroughs have generated a demand of novel materials, with enhanced properties and which also minimize the drawbacks found in the actual ones, as low stability under electrochemical conditions, small values for charge capacity or the inherent rigidity of these oxides, which involves low compatibility with soft tissues. These improvements required may be achieved by hybrid materials, which join different properties from both counterparts. In this sense, IrOx-CNTs have been electrochemically prepared with enhanced properties. The chemical composition at the surface is very similar to that for IrOx, but the incorporation of carbon nanotubes makes the surface rougher, increasing the available interface area of the material. These properties, joined with the conductivity provided by the CNTs, yield very high values for charge storage capacity in electrochemical measurements. Also, the stability of the resulting coatings is improved in comparison with bare IrOx. The biocompatibility tests have shown high cellular survival and neuron functionality, similar to those values obtained for bare IrOx or borosilicate (used for reference), which validates these new materials as promising neural electrodes. IrOx hybrids with graphite and graphene also have been prepared. In both coatings, the presence of carbon particles has been demonstrated, although the confirmation of graphene sheets instead of few-layered graphene needs more experimental studies. The electrochemical properties of these IrOx-graphene and IrOx-graphite hybrids are similar than those obtained for IrOx-CNTs electrodes, with high values of charge storage capacity. However, the stability during consecutive cycling for the graphite-hybrid is poor and the coating is finally delaminated. These results are presumably due to heterogeneous structure in graphite-hybrids, in which the big carbon particles are not completely embedded in the IrOx matrix. Also, IrOx hybrids with N-doped graphene have been prepared, showing promising properties and very high values for charge storage capacity and stability, even when compared with non-doped IrOx-graphene coatings. The enhanced conductivity of these materials can be related with the presence of nitrogen, which induces the increase of the defects in the graphene sheets. The biocompatibility of these graphitic materials is under study. Polymeric tri-hibrids, IrOx-PEDOT-CNTs, have been also electrochemically synthesized. The use of a polymeric matrix is an effort to confer more flexibility to the electrode, which is desirable for soft tissue applications. However, the first results show that the polymer may encapsulate the CNTs and the IrOx particles, minimizing the electrochemical properties of these species. As a consequence, the electrochemical performance of the hybrid material is similar to those obtained for other polymers, as PEDOT-PSS. The biocompatibility tests have shown low neuronal viability in these substrates; however, co-cultures have been proposed as a novel method to improve biocompatibility in these types of materials. The materials obtained in all cases, are well adehered coatings, which leads to an easy future perpespective for their use as electrodes or cells substrates.

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9

SECHI, ELISA. "Development and characterization of nanoporous and hybrid materials through electrochemical techniques for energetic applications." Doctoral thesis, Università degli Studi di Cagliari, 2017. http://hdl.handle.net/11584/249611.

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This PhD project, focused on the achievement of nanoporous and hybrid materials, is divided in two main topics: the first one is the synthesis of nanoporous nickel electrodes through electrochemical dealloying; the second one is the preparation of polyaniline/porous silicon hybrid materials by aniline electropolymerization on n-type porous silicon surface. Both materials have been synthetized and characterized by electrochemical methods in order to study the effect of the parameters of preparation on their properties. A particular attention was pointed out on the photoactivity and catalytic behavior. The main results show that porous nickel can be obtained by selective etching of copper from Ni-Cu deposits, under pulsed voltage conditions. The highest values of surfaces have been obtained adopting a low ratio between the corrosion and relaxation time. These surfaces result fully exploitable for the hydrogen and oxygen evolution reactions, as well as for photoelectrochemical applications. Concerning the porous silicon, the results show that an improved photoactivity can be achieved by electropolymerization of polyaniline, using the electroreduction of diazonium salt as underlayer. The hybrid samples present a higher photocurrent with respect to unmodified porous silicon, from the visible to the near-infrared region. Depending on the electrochemical conditions adopted for the synthesis, an increase in photocurrent more than one order of magnitude has been founded.
This PhD project, focused on the achievement of nanoporous and hybrid materials, is divided in two main topics: the first one is the synthesis of nanoporous nickel electrodes through electrochemical dealloying; the second one is the preparation of polyaniline/porous silicon hybrid materials by aniline electropolymerization on n-type porous silicon surface. Both materials have been synthetized and characterized by electrochemical methods in order to study the effect of the parameters of preparation on their properties. A particular attention was pointed out on the photoactivity and catalytic behavior. The main results show that porous nickel can be obtained by selective etching of copper from Ni-Cu deposits, under pulsed voltage conditions. The highest values of surfaces have been obtained adopting a low ratio between the corrosion and relaxation time. These surfaces result fully exploitable for the hydrogen and oxygen evolution reactions, as well as for photoelectrochemical applications. Concerning the porous silicon, the results show that an improved photoactivity can be achieved by electropolymerization of polyaniline, using the electroreduction of diazonium salt as underlayer. The hybrid samples present a higher photocurrent with respect to unmodified porous silicon, from the visible to the near-infrared region. Depending on the electrochemical conditions adopted for the synthesis, an increase in photocurrent more than one order of magnitude has been founded.

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10

Chandrasekaran, Rajeswari. "Modeling of electrochemical energy storage and energy conversion devices." Diss., Georgia Institute of Technology, 2010. http://hdl.handle.net/1853/37292.

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With increasing interest in energy storage and conversion devices for automobile applications, the necessity to understand and predict life behavior of rechargeable batteries, PEM fuel cells and super capacitors is paramount. These electrochemical devices are most beneficial when used in hybrid configurations rather than as individual components because no single device can meet both range and power requirements to effectively replace internal combustion engines for automobile applications. A system model helps us to understand the interactions between components and enables us to determine the response of the system as a whole. However, system models that are available predict just the performance and neglect degradation. In the first part of the thesis, a framework is provided to account for the durability phenomena that are prevalent in fuel cells and batteries in a hybrid system. Toward this end, the methodology for development of surrogate models is provided, and Pt catalyst dissolution in PEMFCs is used as an example to demonstrate the approach. Surrogate models are more easily integrated into higher level system models than the detailed physics-based models. As an illustration, the effects of changes in control strategies and power management approaches in mitigating platinum instability in fuel cells are reported. A system model that includes a fuel cell stack, a storage battery, power-sharing algorithm, and dc/dc converter has been developed; and preliminary results have been presented. These results show that platinum stability can be improved with only a small impact on system efficiency. Thus, this research will elucidate the importance of degradation issues in system design and optimization as opposed to just initial performance metrics. In the second part of the thesis, modeling of silicon negative electrodes for lithium ion batteries is done at both particle level and cell level. The dependence of the open-circuit potential curve on the state of charge in lithium insertion electrodes is usually measured at equilibrium conditions. Firstly, for modeling of lithium-silicon electrodes at room temperature, the use of a pseudo-thermodynamic potential vs. composition curve based on metastable amorphous phase transitions with path dependence is proposed. Volume changes during lithium insertion/de-insertion in single silicon electrode particle under potentiodynamic control are modeled and compared with experimental data to provide justification for the same. This work stresses the need for experiments for accurate determination of transfer coefficients and the exchange current density before reasoning kinetic hysteresis for the potential gap in Li-Si system. The silicon electrode particle model enables one to analyze the influence of diffusion in the solid phase, particle size, and kinetic parameters without interference from other components in a practical porous electrode. Concentration profiles within the silicon electrode particle under galvanostatic control are investigated. Sluggish kinetics is established from cyclic voltammograms at different scan rates. Need for accurate determination of exchange current density for lithium insertion in silicon nanoparticles is discussed. This model and knowledge thereof can be used in cell-sandwich model for the design of practical lithium ion cells with composite silicon negative electrodes. Secondly, galvanostatic charge and discharge of a silicon composite electrode/separator/ lithium foil is modeled using porous electrode theory and concentrated solution theory. Porosity changes arising due to large volume changes in the silicon electrode with lithium insertion and de-insertion are included and analyzed. The concept of reservoir is introduced for lithium ion cells to accommodate the displaced electrolyte. Influence of initial porosity and thickness of the electrode on utilization at different rates is quantitatively discussed. Knowledge from these studies will guide design of better silicon negative electrodes to be used in dual lithium insertion cells for practical applications.

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11

Cai, Muzhi. "Hybrid materials based on inorganic glasses doped with organophosphorus molecules for light emitting electrochemical cell applications." Thesis, Rennes, INSA, 2019. http://partages.insa-rennes.fr/share/page/document-details?nodeRef=workspace://SpacesStore/cc6fb318-d6f8-4126-8db4-a2a825a605a7.

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La cellule électrochimique électroluminescente (LEC) est un dispositif à couches minces, composé d’un semi-conducteur organique électroluminescent (OSC) et d’ions mobiles en tant que matériau actif intercalé entre une anode et une cathode. Dans le premier chapitre, le contexte et le mécanisme de la LEC ont été introduits. Dans le deuxième chapitre, nous avons dopé la molécule organophosphorée dans un verre de silicate contenant une teneur élevée en lithium par la méthode sol-gel. Dans le troisième chapitre, nous avons travaillé à l’obtention d’un verre de phosphate dopé à une molécule organophosphorée avec une conductivité ionique élevée par frittage Spark Plasma Sintering (SPS). Un verre de phosphate hybride ayant une conductivité ionique d'environ 10 -7 S / cm a été obtenu et une forte photoluminescence a été observée. En outre, les propriétés électrochimiques ont également été étudiées. De plus, lors du processus de préparation de la LEC par SPS, un phénomène intéressant a été découvert. Une émission bleue à large bande a été observée dans le verre d’oxynitrure de phosphate de zinc exempt de terres rares. Le quatrième chapitre est consacré à ce phénomène
The light-emitting electrochemical cell (LEC) is a planar layered device, which is comprised of an electroluminescent organic semiconductor (OSC) and mobile ions as the active material sandwiched between an anode and a cathode. Electrolyte is one of the “short slab” of LEC technology. The main objective of this work is developing a new LEC device based on organophosphorus molecule doped organic-inorganic hybrid glass electrolyte. This hybrid glass cannot be synthesized by using classic melt-quenching technique because the melting temperature of glass is always much higher than the degradation temperature of organic molecule. Thus, in this work, we devote to that how to dope the organophosphorus molecule into the glass with high ionic conductivity. In first chapter, the background and mechanism of LEC were introduced. In the second chapter, we attempted to dope the organophosphorus molecule into silicate glass containing high lithium content by sol-gel method. In third chapter, we are working to obtain organophosphorus molecule doped phosphate glass with high ionic conductivity through spark plasm sintering (SPS). A hybrid phosphate glass with ionic conductivity of around 10 -7 S/cm was obtained, and strong photoluminescence was observed. Besides, the electrochemical properties were investigated as well. Moreover, during the process of preparing the LEC by SPS, an interesting phenomenon was found. A broadband blue emission was observed in rare-earth free zinc phosphate oxynitride glass. The fourth chapter is focus on this interesting phenomenon

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Tolosa, Aura [Verfasser], and Volker [Akademischer Betreuer] Presser. "Electrospun carbon hybrid fibers as binder-free electrodes for electrochemical energy storage / Aura Tolosa ; Betreuer: Volker Presser." Saarbrücken : Saarländische Universitäts- und Landesbibliothek, 2018. http://d-nb.info/1174876948/34.

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13

Tolosa, Rodriguez Aura Monserrat [Verfasser], and Volker [Akademischer Betreuer] Presser. "Electrospun carbon hybrid fibers as binder-free electrodes for electrochemical energy storage / Aura Tolosa ; Betreuer: Volker Presser." Saarbrücken : Saarländische Universitäts- und Landesbibliothek, 2018. http://d-nb.info/1174876948/34.

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14

Salinas-Torres, David. "Tailoring of carbon materials for their use as electrodes in electrochemical capacitors." Doctoral thesis, Universidad de Alicante, 2014. http://hdl.handle.net/10045/45286.

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15

SUN, C. "Electrical energy storage by electrochemical vanadium redox flow battery methods." Doctoral thesis, Università degli studi di Padova, 2018. http://hdl.handle.net/11577/3424975.

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Redox flow batteries (RFBs) are electrochemical cells that are able to reversibly convert the chemical energy stored into the redox couples into electrical power. Vanadium redox flow batteries (VRFBs) exploit redox couples both based on vanadium species. To make VRFB technology commercially viable, technical and economic barriers including high capital cost and rapid capacity decay need to be addressed. The primary objective of this thesis is to achieve high performance VRFB with long durability, mainly by reducing the vanadium permeability through the membrane. Nowadays perfluorosulfonic acid membranes are widely used in VRFB, such as Nafion. Nafion has high chemical and mechanical stability, and it exhibits good proton conductivity. Nevertheless, the VRFB cell with Nafion membrane has fast capacity decay due to the high vanadium crossover. In an effort to overcome the limitations of Nafion, this thesis reports the synthesis and characterization of hybrid inorganic-organic proton-conducting membrane alternatives to classic perfluorinated ionomers. Two families of hybrid membranes were synthesized: 1) Nafion membrane doped with WO3 nanofiller, in order to reduce its vanadium crossover while maintaining the high proton conductivity; 2) synthesis of sulfonated poly (ether ether ketone) (SPEEK) membrane with optimized degree of sulfonation as an alternative low-cost membrane. Then further dope the SPEEK membrane with WO3 to reduce vanadium crossover. For all the hybrid membranes prepared by a solvent-casting procedure, the introduction of WO3 nanoparticles does not alter significantly the thermal degradation events of the polymer host and the hybrid membranes maintain the good thermal stability. MDSC reveals that in hybrid membranes the endothermic events are slightly shifted attributed to the formation of “dynamic crosslinks” between the WO3 nanoparticles and the polymer host, that stabilize the hybrid membrane. The hydrophilic domains of the polymer host are reduced in size as the content of WO3 is raised. The water uptake of hybrid membranes decreases with the increasing loading of WO3 nanofillers; as a consequence, the pathways of charge migration become more tortuous. While the higher charge migration tortuosity would correspond to a dramatically lower permeability to vanadium species. The tortuosity for protons is likely much less than that for vanadium, as the vanadium ions are only passing through the bulk water, while the protons are also delocalized at the polymer-nanofiller interfaces in the presence of interface water. The vanadium permeability of hybrid membranes decreases significantly and the ion selectivity is much improved in comparison with Nafion. The hybrid membranes with highest ion selectivity are chosen for VRFB single cell test. They exhibits a higher coulombic efficiency in comparison with the Nafion 212 reference. The reduced permeation of vanadium species is also revealed by the lower discharge capacity decay and longer self-discharge times for the hybrid membranes. Therefore, the new family of hybrid membranes may be promising candidates for application in VRFBs. The final chapter describes the study by Raman spectroscopy of the species present in the positive feed of a VRFB as a function of the state of charge (SOC). Changes in complexation due to presence of stable oxygenated coordination complexes of vanadium, also interacting strongly with HSO4- and SO42- ligands, are put in evidence. In particular, it is demonstrated that the positive feed includes additional species beyond VO2+ and VO2+, with a particular reference to dimers such as HV2O5- and H3V2O7-. Such species may be accounted to understand in detail the charge-discharge processes taking place at the electrodes of a VRFB. Indeed, on these bases, the processes are expected to involve a broad distribution of V(IV) and V(V) species, that may end up affecting significantly crucial macroscopic features of the overall VRFB.
Le batterie Redox a Flusso (RFB) sono celle elettrochimiche capaci di convertire reversibilmente l'energia chimica immagazzinata in coppie redox in energia elettrica. Le batterie a flusso al vanadio (VRFB) sfruttano coppie redox entrambe basate su specie di vanadio. Per far sì che la tecnologia VRFB sia commercialmente valida, occorre superare barriere tecniche ed economiche che includono elevati costi di capitale ed un rapido decadimento della capacità. L'obiettivo principale di questa tesi è di ottenere VRFB ad alte prestazioni e di lunga durata, principalmente riducendo la permeabilità del vanadio attraverso la membrana. Al giorno d'oggi nelle VRFB vengono utilizzate membrane a base di acido perfluorosolfonico, come il Nafion. Il Nafion ha un'elevata stabilità chimica e meccanica, e presenta una buona conducibilità protonica. La VRFB con membrana al Nafion hanno un rapido decadimento della capacità a causa dell'alto crossover del vanadio. Per superare i limiti del Nafion, questa tesi riporta la sintesi e la caratterizzazione di membrane ibride inorganico-organiche conduttrici di protoni alternative agli ionomeri perfluorurati. Due famiglie di membrane ibride sono state ottenute: 1) membrana di Nafion drogata con nanofiller WO3, per ridurre il crossover del vanadio mantenendo un’elevata conducibilità protonica; 2) sintesi di una membrana a base di poli(etere-etere-chetone) solfonato (SPEEK), con grado di solfonazione ottimizzato. Anche la membrana a base di SPEEK viene poi drogata con WO3 per ridurre il crossover del vanadio. Nelle membrane ibride preparate mediante una procedura di solvent-casting, l'introduzione di nanoparticelle di WO3 non altera in modo significativo gli eventi di degradazione termica della matrice polimerica, mantenendo così una buona stabilità termica. Misure MDSC rivelano che nelle membrane ibride gli eventi termici sono leggermente spostati a causa della formazione di "crosslink dinamici" tra le nanoparticelle di WO3 e la matrice polimerica, che stabilizzano la membrana. La dimensione dei domini idrofili e l’assorbimento d’acqua della mambrana si riducono all’aumentare del contenuto di WO3. Di conseguenza, i percorsi di migrazione di carica diventano più tortuosi. Questa maggiore tortuosità alla migrazione di carica corrisponde ad una permeabilità inferiore delle specie vanadio. Al contrario del vanadio, la tortuosità ha probabilmente un effetto inferiore per i protoni, poiché gli ioni di vanadio attraversano solo i domini massivi di acqua, mentre i protoni vengono scambiati anche alle interfacce polimero-nanofiller. Così, la permeabilità al vanadio delle membrane ibride diminuisce significativamente e la selettività degli ioni è molto migliorata rispetto al Nafion. Le migliori membrane ibride sono scelte per il test in cella VRFB. Esse esibiscono una maggiore efficienza coulombica rispetto al riferimento Nafion 212. La ridotta permeazione delle specie di vanadio è rivelata anche dal minore decadimento della capacità di scarica e dai tempi di autoscarica più lunghi per le membrane ibride. Pertanto, la nuova famiglia di membrane ibride è un promettente candidato per l'applicazione in VRFB. Il capitolo finale descrive lo studio, attraverso la spettroscopia Raman, delle specie presenti nella soluzione positiva (catolita) di una VRFB in funzione dello stato di carica (SOC). Gli equilibri dovuti alla presenza di complessi di coordinazione del vanadio, che interagiscono fortemente con i leganti HSO4- e SO42-, vengono evidenziati. In particolare, viene dimostrato come il catolita includa specie addizionali oltre a VO2+ e VO2+, quali HV2O5- e H3V2O7-. La presenza di tali specie deve essere considerata per comprendere in dettaglio i processi di scarica e carica che avvengono agli elettrodi di una VRFB. Infatti, su queste basi, ci si aspetta il coinvolgimento di un'ampia distribuzione di specie V(IV) e V(V), che potrebbero influenzare le caratteristiche macroscopiche significativamente cruciali di una VRFB.

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16

Dabonot, Aurore. "Nouveaux matériaux pour les supercondensateurs : développement et caractérisation." Thesis, Grenoble, 2014. http://www.theses.fr/2014GRENI092/document.

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Ces travaux de thèse portent sur l'étude de matériaux d'électrodes de supercondensateurs. Ce sont des dispositifs de stockage qui possèdent une densité de puissance importante de l'ordre de plusieurs kW/kg. Des systèmes asymétriques ont été développés dans le but d'augmenter la densité d'énergie de ces dispositifs, tout en essayant de maintenir une densité de puissance élevée. Ils font intervenir une électrode capacitive classique de carbone activé et une électrode faradique. Concernant cette électrode non-bloquante, deux orientations ont été abordées : • Principalement, l'utilisation de titanate de lithium Li4Ti5O12 qui est un matériau d'insertion du lithium habituellement utilisé dans les électrodes de batteries Li-ion. Il est apparu que pour les systèmes hybrides comportant une électrode négative composée uniquement de Li4Ti5O12, la densité d'énergie chute fortement au-delà de 1 kW/kg. L'utilisation d'électrodes négatives composites carbone activé + Li4Ti5O12 est donc préconisée pour maintenir de bonnes performances à la fois en énergie et en puissance. Ainsi, pour une densité de puissance de 2 kW/kg, la densité d'énergie du système hybride développé est encore 1,5 fois supérieure à celle d'un système symétrique carbone activé / carbone activé testé dans les mêmes conditions. • En second plan, l'utilisation du dioxyde de manganèse MnO2, matériau pseudo-capacitif qui fait intervenir des réactions redox. L'étude a porté sur la synthèse de l'oxyde métallique puis sur celle d'un matériau composite réalisé par auto-assemblage. Le but est d'agréger de fines particules de dioxyde de manganèse autour d'un squelette carboné. Une telle microstructure présente l'avantage d'offrir une grande surface spécifique de matière active directement en contact avec un réseau possédant une bonne conductivité électronique. Le matériau composite MnO2 + VGCF obtenu a été testé en électrode positive dans un système asymétrique face à une électrode négative de carbone activé. Cela a permis de multiplier par 1,5 l'étendue de la fenêtre de stabilité de l'électrolyte aqueux par rapport à un système carbone activé / carbone activé. Enfin, dans une optique exploratoire, l'utilisation du diamant en tant que matériau d'électrode de supercondensateur a été étudiée puisqu'il présente dans l'eau une fenêtre de stabilité électrochimique importante d'environ 3 V. L'intérêt de synthétiser des structures tridimensionnelles a été mis en évidence, en particulier une architecture de diamant « en aiguilles » permet de multiplier par 10 la capacité surfacique par rapport à une architecture plane
This work deals with the study of electrode materials for supercapacitors. These storage devices have a significant power density of several kW/kg. Asymmetric systems have been developed in order to increase the energy density of these components while trying to maintain a high power density. They consist of a classic capacitive electrode made of activated carbon and a faradaic electrode. Two approaches have been broached regarding that non-blocking electrode: • Mainly, the use of lithium titanate Li4Ti5O12 which is a lithium insertion material usually used in Li-ion battery electrodes. It appeared that for hybrid systems including a negative electrode only made of Li4Ti5O12, the energy density is greatly reduced beyond 1 kW/kg. The use of composite negative electrodes made of activated carbon and Li4Ti5O12 is recommended so as to maintain good performances both in energy and power. Thus, for a power density of 2 kW/kg, the energy density of the developed hybrid system remains 1.5 superior to the one of an activated carbon / activated carbon symmetric system tested in the same conditions. • Secondly, the use of manganese dioxide MnO2, a pseudo-capacitive material involving redox reactions. The study has been focused on the synthesis of the metal oxide and then on the synthesis of a composite material by self-assembly. The aim is to aggregate small manganese dioxide particles around a carbon backbone. Such a microstructure offers a high specific surface area of active material directly in contact with a network having a good electronic conductivity. The obtained MnO2 + VGCF composite material has been tested as positive electrode in an asymmetric system, facing an activated carbon electrode. Thus, the stability window of the aqueous electrolyte has been multiplied by 1.5 compared to an activated carbon / activated carbon system. Finally, diamond has been considered as a supercapacitor electrode material in an explorative view since it offers a wide electrochemical stability window in water (around 3 V). The interest for tridimensional structures has been evidenced, e.g. a “needles” architecture allows to obtain a surfacic capacity ten times higher than the one obtained with a flat architecture

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17

Bandhauer, Todd Matthew. "Electrochemical-thermal modeling and microscale phase change for passive internal thermal management of lithium ion batteries." Diss., Georgia Institute of Technology, 2011. http://hdl.handle.net/1853/42900.

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Energy-storing electrochemical batteries are the most critical components of high energy density storage systems for stationary and mobile applications. Lithium-ion batteries have received considerable interest for hybrid electric vehicles (HEV) because of their high specific energy, but face inherent thermal management challenges that have not been adequately addressed. In the present investigation, a fully coupled electrochemical and thermal model for lithium-ion batteries is developed to investigate the impact of different thermal management strategies on battery performance. This work represents the first ever study of these coupled electrochemical-thermal phenomena in batteries from the electrochemical heat generation all the way to the dynamic heat removal in actual HEV drive cycles. In contrast to previous modeling efforts focused either exclusively on particle electrochemistry on the one hand or overall vehicle simulations on the other, the present work predicts local electrochemical reaction rates using temperature-dependent data on commercially available batteries designed for high rates (C/LiFePO4) in a computationally efficient manner. Simulation results show that conventional external cooling systems for these batteries, which have a low composite thermal conductivity (~1 W/m-K), cause either large temperature rises or internal temperature gradients. Thus, a novel, passive internal cooling system that uses heat removal through liquid-vapor phase change is developed. Although there have been prior investigations of phase change at the microscales, fluid flow at the conditions expected here is not well understood. A first-principles based cooling system performance model is developed and validated experimentally, and is integrated into the coupled electrochemical-thermal model for assessment of performance improvement relative to conventional thermal management strategies. The proposed cooling system passively removes heat almost isothermally with negligible thermal resistances between the heat source and cooling fluid. Thus, the minimization of peak temperatures and gradients within batteries allow increased power and energy densities unencumbered by thermal limitations.

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18

Du, Juan [Verfasser]. "Electrochemical deposition of dye-modified ZnO hybrid thin films and their application to flexible dye-sensitized solar cells / Juan Du." Hannover : Technische Informationsbibliothek und Universitätsbibliothek Hannover (TIB), 2013. http://d-nb.info/1032724811/34.

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19

Pham, Truong Thuan Nguyen. "Multifunctional materials based on task-specific ionic liquids : from fundamental to next generation of hybrid electrochemical devices and artifical skin." Thesis, Sorbonne Paris Cité, 2018. http://www.theses.fr/2018USPCC218/document.

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Le développement durable nécessite des investissements massifs pour l'exploration et l'utilisation des sources d'énergie renouvelables dans le bilan énergétique. Parmi diverses formes de l’énergie, l'électricité est sans doute la forme la plus souhaitable pour les usages quotidiens. Cependant, en raison de l'intermittence des sources d’énergie renouvelables, l'électricité doit être stockée sous d'autres formes afin de corréler la production éphémère et la consommation en continue. Malgré la présence des systèmes commerciaux de stockage d'énergie, la recherche de nouveaux matériaux et de nouvelles approches pour résoudre ce problème est toujours en cours et attire également une grande attention. Les récents progrès ont poussé la communauté scientifique vers l'utilisation de matériaux à l'échelle nanométrique pour des systèmes de stockage et de conversion de l'énergie. Bien que ces derniers offrent des avantages pour réduire les émissions de gaz à effet de serre, leurs performances sont encore inférieures aux valeurs théoriques. Dans ce contexte, l’ingénierie à l'échelle moléculaire devient cruciale non seulement pour créer un nouveau type d'entités moléculaires mais aussi pour augmenter les performances des matériaux existants. Dans ce contexte, nous proposons d’utiliser une nouvelle famille de matériaux à base de liquides ioniques pour diverses d’applications, comprenant celles dans le domaine énergétique et pour le long terme, dans la fabrication de la peau artificielle, ces objectifs font l’objet de ces travaux de thèse. Cette dissertation est composée de cinq chapitres. Le chapitre 1 présente différents aspects des liquides ioniques (LIs) et des polymères à base de LI décrites dans la littérature. Via ce chapitre, nous envisageons d’atteindre les points suivants : (1) Décrire les utilisations possibles des liquides ioniques en électrochimie ; (2) Discuter des comportements physico-chimiques de ces composés en solution, (3) Montrer l'immobilisation de liquides ioniques (Redox-actifs) sur différents substrats : de couches minces aux polymères et (4) Mettre en évidence les travaux marquant portant sur l’utilisation des polymères ioniques liquides dans diverses applications. Le chapitre 2 présente différentes approches électrochimiques pour l'immobilisation de liquides ioniques rédox à la surface de l'électrode. De plus, les différentes caractéristiques des nouvelles interfaces seront reportées. Le chapitre 3 se concentre sur l'utilisation des polymères LIs comme catalyseurs émergents et comme matrices pour la génération de matériaux hybrides vers l'activation de petites molécules (ORR, OER, HER). Le chapitre 4 étudie la réactivité à l'échelle micro / nanométrique de divers matériaux, y compris les polymères liquides ioniques électro-actifs, en utilisant la microscopie électrochimique à balayage (SECM). Le chapitre 5 présente les résultats préliminaires de la fabrication de substrats flexibles avec des fonctionnalités intéressantes : possibilité de convertir le frottement en électricité et stockage d'énergie en utilisant des liquides ioniques redox polymériques. Ces études ouvrent de nouvelles opportunités pour élaborer des dispositifs flexibles, portables et implantables
Increasing demand of energy requires massive investment for exploration and utilization of renewable energy sources in the energy balance. However, due to the intermittence of the current renewable sources, the generated electricity must be stored under other forms to correlate the fleeting production and the continuous consumption. Despite available commercialized systems, seeking for new materials and new approaches for resolving this problem is still matter of interest for scientific researches. Highlighted advancements have recently oriented the community towards the utilization of nanoscale materials for efficient energy storage and conversion. Although the advantages given by existing nanomaterials for diverse applications, especially in the energy field, their performance is still lower than theoretical purposes. Consequently, tailoring the physical-chemical properties at the molecular scale becomes crucial not only for boosting the activities of the existed materials but also for creating a new type of molecular entities for storing and releasing the energy. Accordingly, this PhD work aim to develop new family of materials based on ionic liquid that exhibits a multifunctionality towards energy applications. Our work is based on the knowhow in surface functionalization and material preparation by simple methods to build up electrochemical systems that can be utilized in various applications. Thus, this thesis will report different results obtained by following this direction and is composed of six chapters: Chapter 1 reports an overview of ionic liquid and polymeric ionic liquid. We propose to review the available literature on the redox-IL from solution to immobilized substrates. Through this chapter, we will achieve the following points: (1) Report the possible uses of ionic liquids in electrochemistry; (2) Discuss about the physical-chemical behaviors of these compounds in solution, (3) Show the immobilization of (Redox-active)–ionic liquids onto different substrates: from thin layer to polymer and (4) Highlight recent advances using polymeric ionic liquids for diverse applications. Chapter 2 will be devoted to different electrochemical assisted approaches for the immobilization of (redox)-ionic liquids to the electrode surface. We will focus on generating a thin layer and polymeric film based ionic liquid. Furthermore, the different characteristics of the new interfaces will be reported. Chapter 3 concentrates on the use of the polymer ionic liquid modified electrodes as emerging catalyst and as template for the generation of hybrid materials towards activation of small molecules. Chapter 4 studies the reactivity at micro/nanometer scale of diverse materials, including single layer graphene, polymeric redox – ionic liquid, using the scanning electrochemical microscopy (SECM). Chapter 5 reports the potential applications of redox ionic liquid and focus on providing the preliminary results towards the fabrication of flexible substrates with interesting functionalities: possibility to convert the friction to electricity and energy storage by using polymeric redox ionic liquids. These studies open a new opportunity to elaborate flexible, wearable and implantable devices. Finally, some concluding remarks are given to summarize different results obtained in the previous chapters. Besides, different perspectives will be given by using ionic liquid as main material for developing different energy storage and conversion systems

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20

Sánchez, Molas David. "Hybrid integration of MEMS technology and rapid - prototyping techniques: Design, fabrication and characterization of electrochemical devices and miniaturized microbial fuel cells." Doctoral thesis, Universitat Autònoma de Barcelona, 2013. http://hdl.handle.net/10803/129392.

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El objetivo de esta tesis es el de la mejora del rendimiento de dispositivos electroquímcos miniaturizados, con énfasis en pilas de combustible microbianas y sensores electroquímicos. Para conseguir este objetivo, está tesis está centrada en el desarrollo de nuevos materiales para electrodos, nuevas geometrías para microelectrodos y mejor fabricación y procesos de encapsulado. Un inconveniente muy importante en la miniaturización de dispositivos electroquímicos está en la reducción de al superficie activa de los electrodos resultado en señales más pequeñas. Sin embargo, la introducción de técnicas de micromecanizado de silicio como pueden ser fotolitografía grabados seco y húmedo, deposición de metales o dieléctricos por métodos físicos o químicos o procesos térmicos rápidos se han convertido en una vía real para solventar todos los problemas relacionados la manufacturación de dispositivos electroquímicos miniaturizados. Además el uso de herramientas computacionales basadas en métodos de elementos finitos ha ayudado extraordinariamente al diseño de estos dispositivos porque la quinética del electrodo y el transporte de masa pueden ser simulados y estudiados antes de su fabricación. El primer capítulo es una introducción a los fundamentos de la electroquímica, al diseño, a la fabricación y a las aplicaciones desarrolladas en esta tesis. La primera sección se centra en explicar los aspectos fundamentales de la electroquímica. La segunda sección introduce las pilas de combustible, porque estos son los dispositivos electroquímicos desarrollados en el capítulo 4. Finalmente la última sección cubre los materiales y métodos utilizados, incluyendo la microfabricación de los electrodos y las técnicas de prototipaje utilizadas para fabricar las pilas de combustible microbianas. El segundo capítulo comienza con la teoría del transporte de masa en micropilares totalmente conductores. A continuación, el modelo computacional de un único dominio de un micropilar es desarrollado utilizando COMSOL. La fabricación de electrodos con arrays de micropilares totalmente conductores fue conseguida por electrodeposición de oro y también por la combinación de grabado seco y metalización por deposición de oro mediante sputtering. El capítulo cierra con la caracterización electroquímica de los dos arrays, lo que permitió comparar su respuesta y averiguar que ruta era la mejor. El capítulo tres se dirige a la síntesis y fabricación de discos de electrodos de carbón para detectar mercurio en muestras acuosas. Estos electrodos de carbón están basados en la pirólisis de fotoresina. Esta técnica combina fotolitografía y procesos térmicos rápidos. Además las ventanas activas de esos electrodos fueron definidas por deposición química de dieléctricos, también los electrodos fueron físicamente y electroquímicamente caracterizados. Una vez estos electrodos fueron completamente estudiados se utilizaron para detectar mercurio en soluciones. El último capítulo se centra en encontrar una aplicación a los electrodos de arrays de micropilares totalmente conductores. La aplicación escogida fue una pila de combustible microbiana miniaturizada fabricada mediante técnicas de prototipaje rápido, donde en cada caso una geometría diferente con el objeto de averiguar si los arrays de micropilares ayudan a mejorar el rendimiento eléctrico de las pilas de combustible microbianas.
The aim of this thesis is to improve the performance of miniaturized electrochemical devices, with emphasis in microbial fuel cells and electrochemical sensors. To achieve this goal, this thesis focuses on the development of new electrode materials, new microelectrode geometries, and better fabrication and packaging processes. An important drawback in the miniaturization of electrochemical devices lies in that the reduction of the active area of the electrodes results in smaller signals. However, the introduction of silicon micromachining techniques such as photolithography, wet and dry etching, metal or dielectric coating by physical and chemical deposition or rapid thermal processes has become a realistic way to solve all the problems regarding the manufacturing of miniaturized electrochemical devices. In addition the use of computational tools based on finite element methods has helped extraordinarily in the design of these devices because both electrode kinetics and mass transport can be simulated and studied prior to fabrication. The first chapter is an introduction of the fundamentals of electrochemistry, design, fabrication and applications to develop the work described in this thesis. The first section focuses on explaining the fundamental aspects of electrochemistry. The second section fuel cells are introduced because it is the electrochemical device developed in chapter 4. Finally the last section covers the materials and methods used, including the microfabrication of the electrodes and the prototyping techniques used to fabricate the miniaturized microbial fuel cells. The second chapter begins with the theory of mass transport at fully-conducting micropillars. Following this, the computational model of a single domain is developed using COMSOL. The fabrication of fully-conducting micropillar array electrodes was achieved by gold electrodeposition and also by a combination of dry etching and sputtered gold deposition. The chapter closes with the electrochemical characterization of both arrays, which allowed to compare their response and found out which route was better. Chapter three addresses the synthesis and fabrication of carbon disk electrodes to detect mercury in aqueous samples. These carbon electrodes are based on the pyrolysis of photoresist. This technique combines photolithograpy and a rapid thermal process. Besides the active window of these electrodes was defined by the chemical deposition of dielectric layers, also the electrodes were physically and electrochemically characterized. Once these electrodes were completely studied they were used to detect mercury in a stagnant solution. The last chapter focuses on finding an application for the fully-conducting micropillar array electrodes. The application chosen was a miniaturized microbial fuel cell fabricated by rapid-prototyping techniqueswhere in each case a different geometry with the aim of find out if the use of micropillar array helps to improve the electrical performance of microbial fuel cells.

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21

Faber, Erik Jouwert. "Towards the hybrid organic semiconductor fet (hosfet) electrical and electrochemical characterization of functionalized and unfunctionalized, covalently bound organic monolayers on silicon surfaces /." Enschede : University of Twente [Host], 2006. http://doc.utwente.nl/55446.

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22

Fleischmann, Simon [Verfasser], and Volker [Akademischer Betreuer] Presser. "Hybridization of electrochemical energy storage : nanohybrid materials and hybrid cell architectures for high energy, power and stability / Simon Fleischmann ; Betreuer: Volker Presser." Saarbrücken : Saarländische Universitäts- und Landesbibliothek, 2018. http://d-nb.info/1175950122/34.

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23

Fleischmann, Simon Verfasser], and Volker [Akademischer Betreuer] [Presser. "Hybridization of electrochemical energy storage : nanohybrid materials and hybrid cell architectures for high energy, power and stability / Simon Fleischmann ; Betreuer: Volker Presser." Saarbrücken : Saarländische Universitäts- und Landesbibliothek, 2018. http://nbn-resolving.de/urn:nbn:de:bsz:291--ds-275606.

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24

Hughes, Dimitri O. "A hardware-based transient characterization of electrochemical start-up in an SOFC/gas turbine hybrid environment using a 1-D real time SOFC model." Diss., Georgia Institute of Technology, 2011. http://hdl.handle.net/1853/41229.

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Solid oxide fuel cell/gas turbine (SOFC/GT) hybrid systems harness the capability to operate nearly 15 to 20 percentage points more efficiently than standard natural gas or pulverized coal power plants. Though the performance of these systems is quite promising, a number of system integration challenges, primarily with regards to thermal transport, still remain. It is for that reason that the Hybrid Performance Project (HyPer) facility, a Hardware-in-the-Loop SOFC/GT hybrid simulator, was built at the National Energy Technology Laboratory in Morgantown, WV. The HyPer facility couples an actual gas turbine with a combination of hardware and software that are used to simulate an actual SOFC. The facility is used to empirically address the system integration issues associated with fuel cell/gas turbine hybrids. Through this dissertation project, the software component of the SOFC simulator was upgraded from a 0-D lumped SOFC model to a 1-D, distributed, real-time operating SOFC model capable of spatio-temporal characterization of a fuel cell operating with a gas turbine in a hybrid arrangement. Once completed and verified, the upgraded HyPer facility was used to characterize the impact of cold air by-pass and initial fuel cell load on electrochemical start-up in an SOFC/GT hybrid environment. The impact of start-up on fuel cell inlet process parameters, SOFC performance and SOFC distributed behavior are presented and analyzed in comparative manner. This study represents the first time that an empirical parametric study, characterizing system operation during electrochemical start-up has been conducted.

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25

Chamaani, Amir. "Hybrid Polymer Electrolyte for Lithium-Oxygen Battery Application." FIU Digital Commons, 2017. https://digitalcommons.fiu.edu/etd/3562.

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The transition from fossil fuels to renewable resources has created more demand for energy storage devices. Lithium-oxygen (Li-O2) batteries have attracted much attention due to their high theoretical energy densities. They, however, are still in their infancy and several fundamental challenges remain to be addressed. Advanced analytical techniques have revealed that all components of a Li-O2 battery undergo undesirable degradation during discharge/charge cycling, contributing to reduced cyclability. Despite many attempts to minimize the anode and cathode degradation, the electrolyte remains as the leading cause for rapid capacity fading and poor cyclability in Li-O2 batteries. In this dissertation, composite gel polymer electrolytes (cGPEs) consisting of a UV-curable polymer, tetragylme based electrolyte, and glass microfibers with a diameter of ~1 µm and an aspect ratio of >100 have been developed for their use in Li-O2 battery application. The Li-O2 batteries containing cGPEs showed superior charge/discharge cycling for 500 mAh.g-1 cycle capacity with as high as 400% increase in cycles for cGPE over gel polymer electrolytes (GPEs). Results using in-situ electrochemical impedance spectroscopy (EIS), Raman spectroscopy, and scanning electron microscopy revealed that the source of the improvement was the reduction of the rate of lithium carbonates formation on the surface of the cathode. This decrease in formation rate afforded by cGPE-containing batteries was possible due to the decrease of the rate of electrolyte decomposition. The increase in solvated to the paired Li+ ratio at the cathode, afforded by increased lithium transference number, helped lessen the probability of superoxide radicals reacting with the tetraglyme solvent. This stabilization during cycling helped prolong the cycling life of the batteries. The effect of ion complexes on the stability of liquid glyme based electrolytes with various lithium salt concentrations has also been investigated for Li-O2 batteries. Charge/discharge cycling with a cycle capacity of 500 mAh·g-1 showed an improvement as high as 300% for electrolytes containing higher lithium salt concentrations. Analysis of the Raman spectroscopy data of the electrolytes suggested that the increase in lithium salt concentration afforded the formation of cation-solvent complexes, which in turn, mitigated the tetragylme degradation.

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26

Brevnov, Dmitri A. "Development and application electrochemical and spectrophotometric methods based upon AC potential modulation for characterization of hybrid bilayer membranes and electroactive self-assembled monolayers supported on gold electrodes." Morgantown, W. Va. : [West Virginia University Libraries], 2000. http://etd.wvu.edu/templates/showETD.cfm?recnum=1462.

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27

Peng, Chunqing. "Electrostatic layer-by-layer assembly of hybrid thin films using polyelectrolytes and inorganic nanoparticles." Diss., Georgia Institute of Technology, 2011. http://hdl.handle.net/1853/43684.

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Polymer/inorganic nanoparticle hybrid thin films, primarily composed of functional inorganic nanoparticles, are of great interest to researchers because of their interesting electronic, photonic, and optical properties. In the past two decades, layer-by-layer (LbL) assembly has become one of the most powerful techniques to fabricate such hybrid thin films. This method offers an easy, inexpensive, versatile, and robust fabrication technique for multilayer formation, with precisely controllable nanostructure and tunable properties. In this thesis, various ways to control the structure of hybrid thin films, primarily composed of polyelectrolytes and indium tin oxide (ITO), are the main topics of study. ITO is one of the most widely used conductive transparent oxides (TCOs) for applications such as flat panel displays, photovoltaic cells, and functional windows. In this work, polyethyleneimine (PEI) was used to stabilize the ITO suspensions and improve the film buildup rate during the LbL assembly of poly(sodium 4-styrenesulfonate) (PSS) and ITO. The growth rate was doubled due to the stronger interaction forces between the PSS and PEI-modified ITO layer. The assembly of hybrid films was often initiated by a polyelectrolyte precursor layer, and the characteristics of the precursor layer were found to significantly affect the assembly of the hybrid thin films. The LbL assembly of ITO nanoparticles was realized on several substrates, including cellulose fibers, write-on transparencies, silicon wafers, quartz crystals, and glasses. By coating the cellulose fibers with ITO nanoparticles, a new type of conductive paper was manufactured. By LbL assembly of ITO on write-on transparencies, transparent conductive thin films with conductivity of 10⁻⁴ S/cm and transparency of over 80 % in the visible range were also prepared. As a result of this work on the mechanisms and applications of LbL grown films, the understanding of the LbL assembly of polyelectrolytes and inorganic nanoparticles was significantly extended. In addition to working with ITO nanoparticles, this thesis also demonstrated the ability to grow bicomponent [PEI/SiO₂]n thin films. It was further demonstrated that under the right pH conditions, these films can be grown exponentially (e-LbL), resulting in much thicker films, consisting of mostly the inorganic nanoparticles, in much fewer assembly steps than traditional linearly grown films (l-LbL). These results open the door to new research opportunities for achieving structured nanoparticle thin films, whose functionality depends primarily on the properties of the nanoparticles.

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28

Řihák, Pavel. "Zkoumání vlivu oxidu titaničitého na životnost olověných akumulátorů s aplikovaným přítlakem." Master's thesis, Vysoké učení technické v Brně. Fakulta elektrotechniky a komunikačních technologií, 2013. http://www.nusl.cz/ntk/nusl-220183.

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Hybrid electric vehicles use lead acid batteries operating under partial charge. Battery life of these batteries is dependent on the speed of development of lead sulphate (PbSO4) to the negative electrodes. Different admixtures are affected battery life. This work deals with the influence of titanium dioxide on the negative active material in lead battery. Mainly devoted to the influence of the applied pressure.

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29

Oliveira, Elton Inacio de. "Avaliação do desempenho de revestimentos híbridos modificados com inibidores no combate à corrosão de ligas de alumínio." Universidade de São Paulo, 2014. http://www.teses.usp.br/teses/disponiveis/3/3137/tde-29122015-161538/.

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Tratamentos de metais contra a corrosão usando formulações contendo derivados de cromo hexavalente (Cr6+) tem sido padrão na indústria de tratamento de superfície durante muitas décadas. Esses tratamentos oferecem excelente proteção contra a corrosão, fornecem boa base para pinturas, são baratos e relativamente fáceis de aplicar. Além do mais oferecem proteção ativa ao substrato devido à capacidade de autorregeneração. Porém, restrições ambientais e de saúde, tornadas mais severas a partir das últimas décadas, requerem a substituição destes tratamentos por processos que sejam ambientalmente corretos e não agressivos à saúde humana. Neste contexto, a indústria aeroespacial, amplamente dependente de ligas de alumínio com elevada resistência mecânica para a construção das aeronaves, é uma das mais atingidas, visto que várias das etapas do tratamento superficial e dos processos de proteção contra a corrosão destas ligas utilizam compostos de Cr6+. Dentro dessa nova realidade, a utilização de revestimentos híbridos derivados de silanos, obtidos pelo processo sol-gel, tem se apresentado como uma das alternativas mais investigadas para a substituição dos pré-tratamentos à base de cromato. Estes revestimentos formam uma cadeia polimérica compacta sobre a superfície do metal constituindo uma barreira efetiva contra espécies agressivas, podendo também ser funcionalizados para apresentarem compatibilidade com revestimentos orgânicos. Entretanto os mesmos não exibem proteção ativa contra a corrosão. Nesse trabalho o comportamento anticorrosivo, em solução de NaCl 0,1 M, de um revestimento híbrido produzido pela hidrólise e condensação do 3-glicidóxipropiltrimetóxisilano (GPTMS) e do tetraetil ortosilicato (TEOS) aplicado sobre a liga AA2024-T3 foi investigado por espectroscopia de impedância eletroquímica (EIS) e analisado por SEM/EDX. Com a finalidade de melhorar o desempenho dos revestimentos, as soluções de hidrólise foram modificadas pela introdução de 0,005 M de inibidores de corrosão derivados de triazol (benzotriazol (BTAH) e toliltriazol (TTA)) ou de organofosfonatos (ácido trimetileno fosfônico (ATMP) e ácido 1-hidróxietileno 1,1-difosfônico (HEDP)). Os resultados dos ensaios eletroquímicos mostraram que, apesar de eficientes para a proteção contra a corrosão da liga, o BTAH e o TTA interferem negativamente nas propriedades anticorrosivas do revestimento híbrido. Por sua vez, a modificação do híbrido com o ATMP ou HEDP melhorou a resposta de impedância do revestimento e aumentou sua estabilidade, se mostrando como um enfoque promissor para aumentar o desempenho do revestimento. A espectroscopia por emissão de fotoelétrons (XPS) e a espectroscopia Raman foram utilizadas para caracterizar o híbrido modificado com os organofosfonatos. Através da primeira técnica foi possível evidenciar a interação das moléculas de inibidor com a superfície metálica. Já os resultados de espectroscopia Raman indicaram a incorporação dos inibidores no revestimento, tendo sido mais eficaz para esta finalidade que as análises por XPS. Entretanto, para evidenciar esse processo, foi necessário aumentar a concentração dos inibidores em 10 vezes com relação à quantidade empregada nos ensaios eletroquímicos.
Anticorrosion metals treatments using formulations containing derivatives of hexavalent chromium (Cr6+) have been standard in the surface treatment industry for many decades. These treatments afford excellent corrosion protection, offer good base for paintings, are inexpensive and relatively easy to apply. Besides, they provide active protection to the substrate due to their selfhealing abilities. However, environmental and health restrictions, made more severe from the end of the eighties, require replacement of these treatments by processes that are environmentally friendly and not aggressive to human health. In this context, the aerospace industry, which is strongly dependent on high strength aluminium alloys, is one of the most heavily affected, as (Cr6+) compounds are used in several steps of the surface treatment and corrosion protection processes. Within this new reality, the use of hybrid coatings derived from silanes and obtained by the sol-gel process, has emerged as one of the most investigated alternatives to replace the chromate based pre-treatments. These coatings form a compact polymer network on the metal surface providing an effective barrier against aggressive species, they may also be tailored to present compatibility with organic coatings. However they do not exhibit active corrosion protection. In this study the corrosion behavior, in 0.1 M NaCl, of a hybrid coating produced by hydrolysis and condensation of 3glycidoxypropyltrimethoxysilane (GPTMS) and tetraethyl orthosilicate (TEOS) applied on AA2024-T3 alloy was investigated by means of electrochemical impedance spectroscopy (EIS) and analysed by SEM/EDX. Aiming to improve the coatings performances, the hydrolysis solutions were modified by the addition of 0.005 M of triazoles (benzotriazole (BTAH) and tolyltriazole (TTA)) or organophosphates (trimethylene phosphonic acid (ATMP) and 1hydroxyethylidene-1 1-diphosphonic acid (HEDP)) based corrosion inhibitors. The results of the electrochemical tests showed that, although effective for corrosion protection of the alloy, BTAH and TTA adversely impacted the anticorrosive properties of the hybrid coating. In turn, the modification of the hybrid with ATMP or HEDP improved the impedance response of the coating and increased its stability, proving to be a promising approach to enhance the coating performance. X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy were used to characterize the hybrid modified with organophosphates. With the first technique it was possible to demonstrate the interaction of the inhibitor molecules with the metal surface. Raman spectroscopy results indicated the incorporation of the inhibitors in the coating, being more effective for this purpose than the XPS analysis. However, to demonstrate this process, it was necessary use the concentration of the inhibitors 10 times more than the amount employed in the electrochemical tests.

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30

Tošer, Pavel. "Zkoumání teplotních změn vlastností olověného akumulátoru v režimu hybridních vozidel." Master's thesis, Vysoké učení technické v Brně. Fakulta elektrotechniky a komunikačních technologií, 2010. http://www.nusl.cz/ntk/nusl-218567.

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The oldest and also most used type of secondary cells is lead-acid accumulator. Basic functional principle stayed same as in foundation time, only operation parameters are still improving (for example one of the most important is lifetime). Significant technical problem is temperature of lead-acid battery and her influence on functionality and running reactions. Master thesis is focused on this section, when is necessary to evaluate new pieces of knowledge in development. The work deals with description existing types of accumulators, further deals with theory of temperature balance and in the end by measured datas and theirs analyzing.

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Hibino, Takashi, Atsuko Tomita, Mitsuru Sano, Toshio Kamiya, Masahiro Nagao, and Pilwon Heo. "Sn0.9In0.1P2O7-Based Organic/Inorganic Composite Membranes : Application to Intermediate-Temperature Fuel Cells." The Electrochemical Society, 2007. http://hdl.handle.net/2237/18430.

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32

Medina, Elise. "Synthèse de revêtements anticorrosion par voie sol-gel pour la protection de l’alliage 2024 T3. Caractérisation par spectroscopie d’impédance électrochimique et ellipsométrie in situ." Electronic Thesis or Diss., Sorbonne université, 2019. http://www.theses.fr/2019SORUS673.

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L’alliage d’aluminium 2024 T3 est utilisé dans l’aéronautique pour sa légèreté et ses bonnes propriétés mécaniques. Il présente cependant une microstructure hétérogène le rendant particulièrement sensible à la corrosion. La stratégie de protection actuelle consiste à incorporer des composés à base de CrVI dans les revêtements ; à cause de leur toxicité, il devient cependant de plus en plus urgent de les remplacer. C’est dans ce contexte que s’inscrit cette thèse qui a pour objectif d’étudier l’évolution des matériaux et les phénomènes de corrosion en combinant une technique d’analyse de surface (l’ellipsométrie in situ) et la spectroscopie d’impédance électrochimique. Ce couplage étant une avancée significative dans la compréhension des relations entre le mode de synthèse, la microstructure, la durabilité et les propriétés anticorrosion, permet l’élaboration de revêtements plus performants. Une partie de l’étude a été consacrée à la synthèse de revêtements denses hydrophobes par voie sol gel pour améliorer les propriétés barrières. D’autre part, des films mésostructurés, susceptible d’accueillir et de faciliter la diffusion d’inhibiteurs de corrosion ont été étudiés. Le but final étant de mettre au point un système bicouches pour optimiser les propriétés anticorrosion
Aluminum alloy 2024 T3 is widely used in the aeronautical field due to its high weight-to-strength ratio. However, such material is particularly sensitive to corrosion because of its heterogeneous structure. To protect these alloys, the current strategy is to use a three layer stack doped with CrVI based corrosion inhibitors. Nevertheless, those substances are highly toxic. Therefore, their replacement has become a critical issue for the aircraft industry. In this context, synthesis and characterization of new protective coatings are particularly important. The objective of this work is thus to study materials evolution and corrosion phenomena using in situ ellipsometry and electrochemical impedance spectroscopy. Coupling those tow techniques provides new insights to understand the relationship between coating synthesis, microstructure, durability and anticorrosion properties. On one hand, a study has been done on hybrid hydrophobic layers to enhance barrier properties. On the other hand, mesostructured layers, potential matrix for anticorrosion inhibitors have been studied. The final goal is to couple those two materials in a multi-layer system in order to optimize anticorrosion properties

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Konečný, Zdeněk. "Vliv oxidu titaničitého na vlastnosti olověných akumulátorů pracujících v režimu hybridních vozidel." Master's thesis, Vysoké učení technické v Brně. Fakulta elektrotechniky a komunikačních technologií, 2012. http://www.nusl.cz/ntk/nusl-219871.

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This work deals with lead-acid batteries operating in hybrid electric vehicles mode, i.e. in a partial state of charge. The adverse effects such as premature capacity loss and large internal resistance can markedly affect the life of a lead battery. The experiment described in this work aims to clarify the influence of the titanium dioxide in the active mass of negative electrodes especially in the life of lead acid batteries.

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34

Haaken, Daniela. "Innovative Desinfektionsverfahren zur Brauchwassergewinnung in der dezentralen Abwasserbehandlung - Elektrolyse und UV/Elektrolyse-Hybridtechnik." Doctoral thesis, Saechsische Landesbibliothek- Staats- und Universitaetsbibliothek Dresden, 2015. http://nbn-resolving.de/urn:nbn:de:bsz:14-qucosa-166834.

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According to estimates of the United Nations Environment Programme (UNEP), more than 1.8 billion people will be living in countries or regions with absolute water scarcity by 2025. The pressure on water resources is increased not only in arid and semiarid regions, but also in fast growing megacities around the world as a result of, amongst other factors, the changing nutritional and consumer behavior (rising living standards). Over 90 % of the annual water consumption of the newly industrializing and developing countries in the arid and semiarid climate zone is used for agricultural irrigation to ensure the nutrition of the population. Thus, since the beginning of the 20th century, the planned/controlled reuse of wastewater has developed into a central task of the sustainable water resources management. Wastewater represents a valuable resource in view of its composition (e. g. nutrients P, N for soil fertilizing) and its reliable, weather-independent availability in every household. The establishment of a closed-loop water management can enhance the efficiency of water usage. Therefore, activities in research and development are currently focused on decentralized and semi-centralized concepts, since their structures offer better conditions for the establishment of closed-loop systems and innovations in wastewater technology can be implemented more easily. In general, the hygienic quality requirements for wastewater reuse are predominantly oriented towards the planned usage. These are, in turn, regulated by thresholds and guidance values, e. g. for faecal indicator bacteria (e. g. faecal coliforms: E. coli), in widely differing norms and legal provisions specific to the respective countries. In Germany since 2005, small wastewater treatment plants can obtain the discharge class +H by the German Institute for Civil Engineering (DIBt: Deutsches Institut für Bautechnik) if secondary effluents contain less than 100 faecal coliforms (E. coli) per 100 mL. This ensures a safe effluent seepage in karst and water protection areas. Due to the infectious risk caused by a multitude of pathogens (bacteria, viruses, worm eggs, protozoa) which are still contained in wastewater after mechanical-biological treatment, specific disinfection methods are indispensable for their satisfactory reduction. Demands on disinfection methods for wastewater reclamation are quite complex. They should be characterized by a high and constant disinfection efficiency at low or moderate formation of disinfection by-products. The reclaimed wastewater should be able to be stored safely. Moreover, the disinfection method should be technically simple, scaleable, space-saving, subjected to low maintenance and realized at moderate investment and operating costs without applying external toxic chemicals. Established methods in decentralized wastewater disinfection are mainly based on membrane and UV technologies. However, these methods are currently working under high operating costs (high maintenance and cleaning efforts). Furthermore, the high investment costs of the membrane filtration are disadvantageous. In addition, both methods do not provide a disinfection residual. Thus, further research is required for the development and testing of alternative disinfection technologies. Against this background, the applicability of the electrolysis and UV/electrolysis hybrid technology for the decentralized wastewater reclamation was investigated and assessed in this dissertation. Results have shown that the electrochemical disinfection of biologically treated wastewater represents an efficient method at temperatures of > 6 °C, pH values of < 8.5 and DOC con-centrations of < 22 mg L-1. Under these conditions, an E. coli reduction of four log levels was achieved at a concentration of free chlorine ranging from 0.4 mg L-1 to 0.6 mg L-1 and at an after-reaction time of 15...20 min. However, it becomes simultaneously apparent that low temperatures, high pH values and high DOC concentrations are limiting parameters for this disinfection method to reclaim biologically treated wastewater. A high energy consumption of the electrolysis cell equipped with boron-doped diamond (BDD) electrodes (2...2.6 kWh m-3) represents a further unfavourable effect. Moreover, the undesired formation of chlorate (c = 1.3 mg L-1) and perchlorate (c = 18 mg L-1) at BDD electrodes can be considered as critical, since these disinfection by-products are, amongst others, human-toxicologically relevant. The concentration of adsorbable organically bound halogens (AOX) and trihalomethanes (THMs) proved to be marginal to moderate. Due to the synergistic effect of the combined application of UV irradiation (primary disinfection method) and electrolysis, the disadvantages of the single methods can be compensated. Decisive drawbacks of UV irradiation are photo and dark repair mechanisms of reversibly damaged bacteria. It was observed that the reactivation of reversibly UV-damaged E. coli even occurs at low temperatures (T = 10 °C) and strongly differing pH values (pH = 5.7...8.1) as well as at low light intensities and in darkness to an extent excluding a safe usage and storage of the reclaimed wastewater. The reactivation processes might be lowered by increased UV fluences. However, this is limited by high concentrations of total suspended solids (TSS). In spite of high UV fluences of > 400 J m-1, no complete removal of E. coli bacteria can be achieved at TSS concentrations of > 17 mg L-1. Therefore, it is indispensable to prevent bacterial reactivation caused by photo and dark repair processes. This topic was studied in the current work by electrochemically produced oxidants using an electrolysis cell positioned downstream of the UV unit. Results have shown that photo and dark reactivation were completely prevented by oxidants in a total concentration of 0.5...0.6 mg L-1 at a TSS concentration of 8...11 mg L-1, at pH values ranging from 5.7 to 8.1 and at temperatures ranging from 10 °C to 30 °C (t = 24....72 h). Even at a high TSS concentration of 75 mg L-1, the reactivation of E. coli (ctotal oxidants = 1.8 mg L-1) and, up to a TSS concentration of 32 mg L-1, the reactivation of total coliforms (except E. coli, ctotal oxidants = 1.0 mg L-1) can be prevented at a high initial germ concentration of 2…3 105 per 100 mL. The lowest energy consumption could be observed when mixed oxide electrodes (MOX electrodes) were applied. This result and the fact that no chlorate and perchlorate were observed at MOX electrodes argue for the application of these electrodes in practice. All in all, the UV/electrolysis hybrid technology represents an energy-efficient method for reclamation of biologically treated wastewater with TSS concentrations ranging from < 11 to 32 mg L-1 (E = 0.17…0.24 kWh m-3, MOX electrodes). Thereby, the reclaimed wastewater meet the hygienic quality requirements for a multitude of reuse categories starting from agricultural irrigation to urban and recreational reuse. Moreover, the requirements of the discharge class +H (100 faecal coliforms (E. coli) per 100 mL) are complied with reliably. The operational stability of the UV/electrolysis hybrid technology should also be ensured within the required maintenance intervals (t > 6 months). The undesired formation of coverings caused by biofouling processes on quartz glass surfaces could be prevented by electrochemically produced oxidants in a total concentration of 1 mg L-1 within an experimental duration of 5.5 months. However, the application of the UV/electrolysis hybrid technology is limited by increased particle concentrations and faecal loadings (initial E. coli concentration). The resulting enhanced demand of electrochemically produced oxidants for the prevention of bacterial reactivation results in a considerable increase of the electric charge input and energy consumption.

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Cabo, Fernández Laura. "Electrochemical properties of redox centres in coordination compounds and in gold nanocluster hybrids." Thesis, University of Liverpool, 2011. http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.569515.

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In the present work the properties of compounds that can display conformational switching and Coulomb blockade features as a result of electron transfer reactions have been investigated with a view to observing possible Negative Differential Resistance behaviour. This phenomenon is sometimes associated with oscillatory processes and could broaden the field of applications of nanoparticles such as for electronic devices and storage memories. Copper coordination compounds with macro cyclic ligands change their geometry from a distorted octahedral conformation, for Cu(II), to a tetrahedral geometry, for Cu(I), upon reduction of the metal centre. In the research described in this Thesis, copper was coordinated to tetradentante macrocycles with two types of donor sets, tetra-amine (i.e., N4) and macrocycles containing sulfur and nitrogen atoms (i.e., N2S2). It was found that increasing the cavity dimensions of the ligand, the copper(II) complexes were destabilised leading to a shift in the reduction potential to more positive values. The presence of tertiary amines and soft electron-donating atoms such as sulfur in the structure of the ligands favours the formation of Cu(I) intermediates in comparison with Cu(II) species. Rate constants for the electron transfer reactions and chemical steps for these reactions were estimated using computer simulations. Hexanethiolate gold clusters with an average core diameter of 1.8 nm and a calculated capacitance of 0.6 aF were synthesised using a two-phase method. These clusters presented Coulomb blockade responses due to Quantised Double-Layer charging (QDL) events in voltammetric studies. These nanoparticles were functionalised by a place-exchange reaction and terminal bromine groups were introduced by reaction with l l-bromo-l-undecanethiol. The clusters thus synthesised preserved the core single-charging events and served as precursors for the synthesis of hybrids with copper complexes via a nucleophilic substitution reaction. Place-exchange with 6-(ferrocenyl)-1-hexanethiol was also carried out to incorporate ferrocene centres on the cluster surface. Voltammetric measurements showed the redox response of the F c +/F c couple and the charging events of the gold core. A transition in the behaviour from single to multiple electron transfer response for the redox couple was observed as the number of ferrocene units per cluster was increased. For multiple electron transfer processes, a mechanism in which the core acts as a mediator has been proposed involving electron tunnelling through the chains linking the redox centre to the gold core.

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Cakici, Murat. "Highly flexible carbon fibre fabric based nanostructured hybrids for high performance energy storage systems." Thesis, The University of Sydney, 2017. http://hdl.handle.net/2123/18123.

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Electrochemical supercapacitors (ES), or ultracapacitors, store energy using either reversible adsorption of electrolyte ions (electrochemical double layer capacitors) or fast surface redox reactions on its electrodes (pseuodocapacitors). Currently, they are used together with batteries or fuel cells when high-power delivery or uptake is required. They have exceptional features such as high power density, high cycle efficiency, fast charging-discharging rate, long lifecycle, and safe operation. Therefore, they have attracted tremendous interest as next generation energy conversion and storage systems, ranging from portable wearable electronics to hybrid electric vehicles. However, low energy density is the main drawback to use ES as a stand-alone energy storage system. Thus, their performance should be improved to fulfil the requirements of ever-growing energy demands of progressing global economy and industry. In addition, most of the ES electrodes are fabricated from powders which makes them unsuitable for their potential use as wearable lightweight flexible devices in the future. Considering the requirements of future industrial applications of ES, this thesis focuses on synthesizing high performance, flexible, mechanically stable, lightweight, eco-friendly, and low cost ES electrodes using green, scalable, and inexpensive fabrication methods. To develop highly efficient electrode materials suitable for practical applications in a flexible design, novel synthesis procedures were explored to incorporate pseudocapacitive materials (metal oxides and electrically conductive polymers) into three-dimensional and flexible conductive carbon materials to obtain multicomponent hybrid materials. Therefore, hybrid materials reported in this thesis are binder-/conductive agent-free and also have enhanced three-dimensional nanostructures which promote energy storage. Simplicity of the fabrication methods also enable large scale and economical production of flexible and mechanically stable materials which can be directly used as ES electrodes. First, electrode materials with a unique nanostructure was developed for supercapacitor applications based on carbon fibre fabric (CFF) / MnO2 hybrid materials, in which MnO2 was uniformly coated on the surface of CFF. A green hydrothermal method was used to functionalize CFF with coral-like MnO2 nanostructures to improve the electrochemical performance of the hybrid composites. The morphological, structural, and crystalline properties of composites were analysed by using various techniques to confirm the deposition of coral-like MnO2 on CFF. The electrochemical performance was examined in a three-electrode system and cyclic voltammetry results reveal the superior specific capacitance of 467 F g-1 at a scan rate of 5 mV s-1. The cycling performance test revealed that the capacitance retention was 99.7% and the coulombic efficiency remained as high as 99.3% after 5000 cycles, demonstrating an outstanding electrochemical stability of the coral-like MnO2/CFF composite electrode. Second, synthesis method used in the first study was optimised to obtain three novel nanostructured MnO2 layers on flexible CFF substrates. It was observed that different morphologies of MnO2 could be grown on carbon fibres by adjusting the concentration of precursor solution. The morphological, structural, and crystalline properties of the composites were analysed by using various techniques to confirm that MnO2 nanostructures were successfully anchored on CFF. The electrochemical performances of the nanostructured MnO2/CFF composites were examined in two-electrode symmetric cell configuration in 1 M Na2SO4 electrolyte. Among three different morphologies, nanoplate type MnO2/CFF electrode had the best electrochemical performance (528 F g-1 at 0.5 A g-1 current density). In addition, binder and conductive agent free, flexible MnO2/CFF composite electrode had excellent cycling stability and coulombic efficiency. Finally, activated CFF (ACFF) / reduced graphene oxide (RGO)/polyaniline (PANI) composite flexible electrodes were prepared by in-situ polymerization method. Polymerization of aniline was optimized by adjusting aniline concentration to obtain PANI nanowire arrays on the three-dimensional flexible carbon based substrate. Electrochemical performance of ACFF/RGO/PANI composite was compared with ACFF and ACFF/RGO electrodes in two-electrode symmetrical cell configuration in 1 M H2SO4 electrolyte. The results indicated that ACFF/RGO/PANI exhibited outstanding area normalized capacitance due to synergistic effect between ACFF, RGO, and PANI. The facile synthesis method of the composite electrode using textile based substrate enables the possibility for fabrication of high-performance flexible energy storage devices.

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Zinovyeva, Veronika. "Matériaux composés (polymères électroactif - nanoparticules de métal) et liquides ioniques." Thesis, Dijon, 2010. http://www.theses.fr/2010DIJOS056.

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La thèse de doctorat est consacrée aux synthèses de matériaux composites combinant des polymères conducteurs avec des métaux de transition, leur caractérisation par l'utilisation d'un ensemble des méthodes physiques, chimiques et électrochimiques et leur application catalytique. Ces processus ont été réalisés en milieu conventionnel (aqueux et organique) et dans les liquides ioniques à température ambiante. En tant qu’approche de synthèse, nous proposons une méthode simple qui consiste en la réduction chimique de sels inorganiques au moyen de l’oxydation du monomère en milieux variés. La polymérisation du pyrrole en utilisant des sels de Fe(III), Cu(II) et Pd(II) comme oxydants a été réalisée dans une large gamme de conditions de réaction. La cinétique du processus de polymérisation a été étudiée par spectrophotométrie UV-visible et DLS. Les matériaux obtenus ont été caractérisés par les méthodes de voltammétrie cyclique, analyse élémentaire, ICP-AES, AFM, SEM, EDX, TEM, XRD, XPS, XAS, IR. Les propriétés catalytiques et électrocatalytiques des matériaux nanocomposites Pd/polypyrrole ont été analysées pour des réactions du couplage direct hétéroaryle-aryle et l’électrooxidation de l’acide ascorbique. Les procédures alternatives de préparation de polymères conducteurs dans les liquides ioniques, en comparaison avec celles dans les solvents conventionnels, ont été décrites. L’influence des conditions de synthèse sur les propriétés électrochimiques et sur la morphologie des polymères conducteurs a été discutée. L’électrooxidation du ferrocène dans les liquides ioniques a été étudiée en détail, et le modèle du transport diffusionnel dans ces milieux visqueux a été proposé
The actual PhD thesis is devoted to syntheses of composite materials combining conducting polymers with transition metals, their characterization with the use of a large set of modern physical, chemical and electrochemical methods and initial studies of their catalytic applications. These processes were realized both in conventional (aqueous and organic) media and in room-temperature ionic liquids. As an approach for the chemical synthesis, a simple one-pot non-template method, consisting in the chemical reduction of various inorganic salts by pyrrole monomer in a set of solvents, was applied. Polymerization of pyrrole with the use of Fe(III), Cu(II) and Pd(II) salts as oxidants was carried out in a wide range of reaction conditions. The kinetics of the polymerization process was studied by UV-visible spectroscopy and DLS. The obtained materials were characterized by means of cyclic voltammetry, elemental CHNS analysis, ICP-AES, AFM, SEM, EDX, TEM, XRD, XPS, XAS, IR techniques. Catalytic and electrocatalytic properties of the synthesized Pd/polypyrrole nanocomposites were analyzed for the direct catalytic arylation of heteroaromatics and electrooxidation of ascorbic acid. Alternative ways to conducting polymer preparation in the form of films and powders inside ionic liquids, in comparison to those in conventional media, were described. The influence of the synthesis conditions and of the solvent nature on electrochemical properties and morphology of conducting polymers was discussed. The electrooxidation of ferrocene in ionic liquids was investigated in details, and a model for the diffusional transport in these viscous media was proposed

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Van, Meveren Mayme Marie. "Graphene-Based ‘Hybrids’ as High-Performance Electrodes with Tailored Interfaces for Alternative Energy Applications: Synthesis, Structure and Electrochemical Properties." TopSCHOLAR®, 2017. https://digitalcommons.wku.edu/theses/2048.

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Technological progress is determined to a great extent by developments of novel materials from new combinations of known substances with different dimensionality and functionality. We investigate the development of 3D ‘hybrid’ nanomaterials by utilizing graphene based systems coupled with transition metal oxides (e.g. manganese oxides MnO2 and Mn3O4). This lays the groundwork for high performance electrochemical electrodes for alternative energy owing to their higher specific capacitance, wide operational window and stability through charge-discharge cycling, environmental benignity, cost effective, easily processed, and reproducible in a larger scale. Thus far, very few people have investigated the potential of combining carbon sheets that can function as a supercapacitor in certain systems with transition metals that have faradaic properties to create electrochemical capacitors. Previous work by Wang et al. has focused on the structural combination of Mn3O4 and graphene based materials,1 and research by Jafta et al. studied the electrochemical properties of MnO2 with GO.2 We find that both physical and chemical attachment of manganese oxide on graphene allows for electrical interplay of the materials as indicated in electrochemical analysis and Raman spectroscopy. Attachment of the two materials is also characterized by scanning electron microscopy and X-ray diffraction.

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Pinto, Jonathan Hunder Dutra Gherard. "Conversor modular multinível aplicado a sistema híbrido de armazenamento de energia." Universidade Federal de Juiz de Fora (UFJF), 2018. https://repositorio.ufjf.br/jspui/handle/ufjf/6501.

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Este trabalho tem como contribuição o desenvolvimento de uma estratégia de equa-lização das tensões em um conversor multinível modular, como parte integrante de um sistema híbrido de armazenamento de energia. O conversor modular multinível realiza a conexão em série de módulos supercapacitores, o que possibilita aumentar a ten-são sem prejudicar a transferência rápida de energia. Em relação à outras topologias, este trabalho permite reduzir a quantidade, volume e massa do elemento magnético da estrutura do conversor. Um banco de baterias de íons de lítio também integra o sistema por intermédio de um conversor estático. Como é a fonte de maior densidade de energia, fornece a potência média requerida pelo carga. A associação com uma fonte de transferência rápida de energia permite aumentar o desempenho dinâmico, a eficiência energética e a vida útil da bateria. Com efeito, tem-se um sistema híbrido de armazenamento de energia que requer estratégias de gestão para múltiplas fontes de suprimento. Os resultados simulados considerando a estimativa da demanda de po-tência de um protótipo de veículo elétrico, são adequados e propiciam os fundamentos necessários para a construção de um protótipo.
This work is a contribution to develop a strategy equalization of tensions in a mo-dular multilevel converter as part of a hybrid system energy storage. The multilevel modular converter realizes the series connection of supercapacitor modules, which al-lows to increase the voltage without cause damages to the quick energy transfer. In relation to other topologies, it allows reduction of the quantity, volume and mass of the magnetic element of the converter structure. A lithium-ion battery bank also integrates the system via a voltage boost converter. This battery is the source of high energy density, which provides the average power required by the load. The association with a fast transfer power source allows for increased dynamic performance, energy efficiency and service life. In fact, there is a hybrid energy storage system that requires mana-gement strategies for multiple sources of supply. The simulated results were obtained considering the power demand estimation of an electric vehicle prototype.

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Callera, Welder Franzini Amaral [UNESP]. "Estudos de mecanismos redox enzimáticos por eletroquímica e modelagem computacional." Universidade Estadual Paulista (UNESP), 2017. http://hdl.handle.net/11449/151472.

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Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES)
Esta tese de doutoramento apresentou o entendimento de processos redox enzimáticos, detalhando o mecanismo envolvido na troca eletrônica, a qual resulta na formação de um produto, por catálise enzimática. Observou-se a influência de um eletrodo sob a ação de um potencial estacionário aplicado (E) na reação enzima/substrato. Realizou-se eletroanálises, como: Voltametria Cíclica (VC) e Espectroscopia de Impedância Eletroquímica (EIE), para a penicilinase. Os resultados obtidos dão indícios de que a reação enzimática se beneficia de determinados potenciais, pois o parâmetro utilizado, Rct, resistência à transferência de cargas, sugere que ocorre maior troca eletrônica em alguns potenciais ótimos (faixa de -0,3 a -0,5 V). A Simulação Molecular serviu para estudar o comportamento atomístico por métodos clássicos (Dinâmica Molecular – DM) para as condições impostas experimentalmente, esclarecendo o mecanismo de reação enzimática por métodos quânticos (DFT – Teoria do Funcional de Densidade) e híbridos (QM/MM), cabendo salientar que a penicilinase não pertence à classe das enzimas oxirredutivas.
This doctoral thesis presented the understanding of enzymatic redox processes, detailing the mechanism involved in the electronic exchange, which results in the formation of a product by enzymatic catalysis. The influence of an electrode under the action of an applied stationary potential (E) on the enzyme/substrate reaction was observed. Electroanalysis was performed, such as: Cyclic Voltammetry (VC) and Electrochemical Impedance Spectroscopy (EIS), for the penicilinase. The results obtained indicate that the enzymatic reaction benefits from certain potentials, since the parameter used, Rct, resistance to the transfer of charges, suggests that there is greater electronic exchange in some optimal potentials (range the -0.3 to -0.5 V). The Molecular Simulation was used to study the atomistic behavior by classical methods (Molecular Dynamics - DM) for experimentally imposed conditions, clarifying the mechanism of enzymatic reaction by quantum methods (DFT) and hybrids (QM/MM). That penicillinase does not belong to the class of oxidoreductive enzymes.

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Botero, Carrizosa Sara C. "Synthesis, Characterization, and Properties of Graphene-Based Hybrids with Cobalt Oxides for Electrochemical Energy Storage and Electrocatalytic Glucose Sensing." TopSCHOLAR®, 2017. http://digitalcommons.wku.edu/theses/1941.

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A library of graphene-based hybrid materials was synthesized as novel hybrid electrochemical electrodes for electrochemical energy conversion and storage devices and electrocatalytical sensing namely enzymeless glucose sensing. The materials used were supercapacitive graphene-family nanomaterials (multilayer graphene-MLG; graphene oxide-GO, chemically reduced GO-rGO and electrochemical reduced GOErGO) and pseudocapacitive nanostructured transition metal oxides including cobalt oxide polymorphs (CoO and Co3O4) and cobalt nanoparticles (CoNP). These were combined through physisorption, electrodeposition, and hydrothermal syntheses approaches. This project was carried out to enhance electrochemical performance and to develop electrocatalytic platforms by tailoring structural properties and desired interfaces. Particularly, electrodeposition and hydrothermal synthesis facilitate chemically-bridged (covalently- and electrostatically- anchored) interfaces and molecular anchoring of the constituents with tunable properties, allowing faster ion transport and increased accessible surface area for ion adsorption. The surface morphology, structure, crystallinity, and lattice vibrations of the hybrid materials were assessed using electron microscopy (scanning and transmission) combined with energy dispersive spectroscopy and selected-area electron diffraction, X-ray diffraction, and micro-Raman Spectroscopy. The electrochemical properties of these electrodes were evaluated in terms of supercapacitor cathodes and enzymeless glucose sensing platforms in various operating modes. They include cyclic voltammetry (CV), ac electrochemical impedance spectroscopy, charging-discharging, and scanning electrochemical microscopy (SECM). These hybrid samples showed heterogeneous transport behavior determining diffusion coefficient (4⨯10-8 – 6⨯10-6 m2/s) following an increasing order of CoO/MLG < Co3O4/MLG < Co3O4/rGOHT < CoO/ErGO < CoNP/MLG and delivering the maximum specific capacitance 450 F/g for CoO/ErGO and Co3O4/ rGOHT. In agreement with CV properties, these electrodes showed the highest values of low-frequency capacitance and lowest charge-discharge response (0.38 s – 4 s), which were determined from impedance spectroscopy. Additionally, through circuit simulation of experimental impedance data, RC circuit elements were derived. SECM served to investigate electrode/electrolyte interfaces occurring at the solid/liquid interface operating in feedback probe approach and imaging modes while monitoring and mapping the redox probe (re)activity behavior. As expected, the hybrids showed an improved electroactivity as compared to the cobalt oxides by themselves, highlighting the importance of the graphene support. These improvements are facilitated through molecular/chemical bridges obtained by electrodeposition as compared with the physical deposition.

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Santos, Diógenes Meneses dos. "Microssistemas eletroforéticos em materiais poliméricos de duplo canal com detecção amperométrica." Universidade Federal de Alagoas, 2014. http://www.repositorio.ufal.br/handle/riufal/1919.

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Electrophoretic microsystems (EM) are powerful tools for the separation of species of microsystems analyzes which can easily be combined with electrochemical detection (ECD) and therefore making it ideal for a method of detection. However, the influence of high voltage at the working electrode used for the separation is a problem to be overcome due to the increased signal/noise ratio and possible damage of the electrode and/or the potentiostat. Thus, it was proposed in this thesis one EM hybrid PDMS / glass configuration with dual-channel potentiostat coupled to an electrically isolated in order to minimize the influence of high potential in the separation channel and improve the separation efficiency of the species and subsequently, improve detection limits. The EM contains two separate parallel channels 200 microns and a channel separation and another reference, and each containing a platinum electrode 15 or 50 μm placed about 1 to 4 μm in the channel. An electrode served as the working electrode, positioned in the separation channel, and another electrode as reference electrode, placed in the reference channel. This configuration associated with the electrically isolated potentiostat allowed the amperometric signals were measured without any change or potential interference arising from the high voltage applied separation. Aiming to evaluate the effectiveness of the methodology proposed in this thesis, samples nitrite, tyrosine and peroxynitrite (reactive nitrogen species – RNS), hydrogen peroxide (reactive oxygen species – ROS), ascorbic acid, glutathione and cysteine were injected into the channel containing the working electrode, while simultaneously boric acid buffer pH 11 containing TTAB was injected into the reference channel containing the reference electrode. From this configuration, we obtained a significant reduction in noise level (about 0.94 pA) and a relative improvement in the resolution ratified by electropherograms, compared with using single channel configuration. The limits of detection (LOD) for the chemical species mentioned above were 0.58 μM, 0.14 μM, 0.75 μM, 0.21 μM, 0.82 μM, was not obtained for cysteine and 1.63 μM, respectively. The efficiency can also be seen by analyzing nitrite performed on samples of perfusate blood of sheeps and rats, where have been detected a concentration of 68.05 μM and 22.04 μM, respectively, by the proposed method. It was also proposed in this thesis, microfabrication and evaluation of a PMMA electrophoretic microsystem with single channel configuration coupled to a base made of the same material to fix the microchip with electrochemical detection using a carbon paste electrode. The purpose of the construction of the base was to obtain, by fixing, reproducibility of events. And the microfabrication of PMMA EM aimed the viability of its use in analysis perspective as having the lowest cost per unit made due to the use of CO2 laser for microfabrication, which has a value considerably lower, compared with photolithographic processes. The evaluation of this system was performed through the analysis standards of serotonin and acetaminophen, which proved that the microfabrication of this system showed good reproducibility and repeatability of events, making it viable processing.
Coordenação de Aperfeiçoamento de Pessoal de Nível Superior
Os microssistemas eletroforéticos (MSE) são ferramentas poderosas para a separação de espécies em microssistemas de análises, onde pode ser facilmente combinada com detecção eletroquímica (DEQ) e tornando-se, portanto, um método de detecção ideal. No entanto, a influência da alta tensão no eletrodo de trabalho utilizada para a separação é um problema a ser contornado devido o aumento da relação sinal/ruído e possíveis danificações do eletrodo e/ou do potenciostato. Assim, foi proposto nesta tese um MSE híbrido de PDMS/vidro com configuração de duplo-canal acoplado a um potenciostato eletricamente isolado com objetivo de minimizar a influência do elevado potencial no canal de separação e melhorar a eficiência de separação das espécies e, subsequentemente, melhorar os limites de detecção. O MSE contém dois canais paralelos separados 200 μm, sendo um canal de separação e outro de referência, e cada um deles contendo um eletrodo de platina de 15 ou 50 μm colocados cerca de 1 a 4 μm dentro do canal. Um eletrodo serviu como eletrodo de trabalho, posicionado no canal de separação, e o outro eletrodo como eletrodo de referência, posicionado no canal de referência. Essa configuração associado ao potenciostato eletricamente isolado permitiu que os sinais amperométricos fossem medidos sem qualquer mudança de potencial ou de interferência oriunda da alta tensão de separação aplicada. Objetivando avaliar a eficiência da metodologia proposta nessa tese, amostras de nitrito e peroxinitrito (espécies reativas de nitrogênio – ERN), tirosina, peróxido de hidrogênio (espécie reativa de oxigênio – ERO), ácido ascórbico, glutationa e cisteína foram injetadas no canal contendo o eletrodo de trabalho, enquanto que simultaneamente o tampão de ácido bórico contendo TTAB pH 11 foi injetado no canal de referência contendo o eletrodo de referência. A partir desta configuração, obteve-se uma significativa diminuição no nível de ruído (cerca de 0,94 pA) e uma relativa melhora na resolução ratificadas pelos eletroferogramas, se comparado com a configuração que utiliza canal único. Os limites de detecção (LOD) para as espécies químicas supracitados foram de 0,58 μM, 0,14 μM, 0,75 μM, 0,21 μM, 0,82 μM, não foi obtida para a cisteína, e 1,63 μM, respectivamente. A eficiência também pode ser vista através das análises de nitrito realizadas em amostras de perfusato de sangue de ovelhas e ratos, onde foram detectados uma concentração de 68,05 μM e 22,04 μM, respectivamente, através da metodologia proposta. Foi proposto também nessa tese, a microfabricação e avaliação de um microssistema eletroforético de PMMA com configuração de canal único acoplado a uma base feita do mesmo material para fixar o microchip, com detecção eletroquímica usando eletrodo de pasta de carbono. O objetivo da construção da base foi obter, através da fixação, reprodutibilidade de eventos. E a microfabricação do MSE de PMMA objetivou a viabilidade do seu uso em análises tendo como perspectiva o baixo custo por unidade confeccionada devido ao uso de laser de CO2 para a microfabricação, o qual possui um valor agregado consideravelmente menor, se comparado com os processos fotolitográficos. A avaliação desse sistema foi feita através das análises de padrões de serotonina e acetaminofeno, onde comprovou-se que a microfabricação desse sistema apresentou boa reprodutibilidade e repetitividade de eventos, tornando-se viável o seu processamento.

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Sapountzi, Eleni. "Développement de nouveaux supports basés sur des nanofibres de matériaux hybrides électrofilées pour le développement de biocapteurs électrochimiques." Thesis, Lyon 1, 2015. http://www.theses.fr/2015LYO10122/document.

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Les travaux présentés dans ce manuscrit décrivent le développement de trois supports innovants basés sur des nanofibres de matériaux hybrides obtenus par électrofilage pour la réalisation de biocapteur électrochimiques. La performance des biocapteurs est fortement améliorée du fait de l'utilisation de matériaux nanostructurés qui leurs confèrent des propriétés uniques. Les fibres obtenues par électrofilage trouvent des applications dans de nombreux domaines, mais leur utilisation pour l'élaboration de biocapteurs, bien que très prometteuse, est encore très peu abordée. Dans ce travail, différentes nanofibres polymériques contenant des nanotubes de carbone ou recouvertes de nanoparticules d'or ou d'un film de copolymère polypyrolle / poly(pyrolle-3-carboxylique acide) ont été utilisées comme support pour le développement de biocapteurs. La glucose oxydase a été utilisée comme enzyme modèle pour valider les performances des biocapteurs réalisés. Cette enzyme a été incorporée directement dans les nanofibres ou fixée de façon covalente à leur surface. Les biocapteurs ainsi obtenus, caractérisés par différentes techniques microscopiques et électrochimiques, ont permis la détection du glucose avec succès, en utilisant la voltammétrie cyclique et la spectroscopie d'impédance électrochimique, tout en montrant des performances (sensibilité, reproductibilité, stabilité) supérieures à celles des biocapteurs conventionnels
The work detailed within this manuscript describes the development of three novel efficient electroactive platforms based on electrospun nanofibrous hybrid materials for further application to electrochemical biosensors elaboration. The performance of biosensors is enhanced by their coupling with nanoscale materials, due to the unique properties that the latter exhibit. Although electroctrospun fibers find applications in various fields, their exploitation for biosensing is still in an early but promising stage. Herein, different polymeric nanofibers incorporating carbon nanotubes, decorated with gold nanoparticles or coated with conducting polypyrrole/poly(pyrrole-3-carboxylic acid) films were used as platforms for the development of biosensors. Glucose oxidase was used as a model enzyme to validate the performance of the developed biosensors. The enzyme was either incorporated into the nanofibers or covalently immobilized onto their surface. These innovative biosensors, characterized by different microscopic and electrochemical techniques, enabled successful detection of glucose by employing cyclic voltammetry and electrochemical impedance spectroscopy, whilst demonstrating enhanced performances over conventional biosensors in terms of sensitivity, reproducibility and stability

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Touati, Souad. "Elaboration d'aérogels d'hydroxydes doubles lamellaires et de bionanocomposites à base d'alginate." Phd thesis, Université Blaise Pascal - Clermont-Ferrand II, 2013. http://tel.archives-ouvertes.fr/tel-00975932.

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Cette thèse présente un travail sur l'obtention d'aérogels d'HDL par séchage en conditions CO2 supercritique et l'élaboration de nouveaux bionanocomposites formés par la coprécipitation d'hydroxydes doubles lamellaire (HDL) dans l'espace confiné des billes d'alginate. Grâce à la combinaison d'une synthèse par coprécipitation Flash et d'un séchage en conditions supercritiques au CO2, des aérogels d'HDL possédant des surfaces spécifiques élevées sont élaborés. Parallèlement, l'alginate est utilisé comme une matrice de confinement pour la précipitation inorganique d'HDL. D'une part, les billes d'alginate sont synthétisées par complexation des ions Ca2+ et la coprécipitation des phases HDL s'effectue en réalisant des imprégnations successives de réactifs. D'autre part, des billes d'alginate sont formées directement en présence des cations divalents (Mg2+, Ni2++, Co2+, ...) et des cations des métaux trivalents (Al3+), précurseurs des composés inorganiques. La coprécipitation des HDL se produit dans ce cas lors d'une étape d'imprégnation dans une solution d'hydroxyde de sodium. Tous les composés HDL, aérogels ou encore bionanocomposites sont caractérisés en détail par DRX, spectroscopie IR, MEB/MET, adsorption/désorption d'azote et ATG/DTG, pour obtenir un meilleur aperçu de la structure des particules, de leur taille et de leur morphologie. Des études menées sur l'adsorption de la trypsine pour les aérogels ou encore sur les performances d'électrodes modifiées HDL-alginate ont permis de montrer qu'il était possible d'améliorer les performances des HDL en augmenter leur porosité et en élaborant des bionanocomposites.

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Hung, Kai-Hsuan, and 洪凱炫. "Synthesis of Hybrid Carbon Nanostructures and Their Electrochemical Applications." Thesis, 2009. http://ndltd.ncl.edu.tw/handle/97031525064021226988.

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博士
逢甲大學
材料科學所
97
A pulse electrodeposition technique was utilized to deposit nanometric (10 nm) Ni catalysts on a carbon fabric (CF). Using this technique, the morphology and loading of the Ni catalysts can be controlled by changing the duration, overpotential, and cycle numbers. After the pulse electrodeposition, the growth of carbon nanofibers (CNFs) on catalytic Ni/carbon fabric was carried out in a thermal chemical vapor deposition system with the optimum Ni loading from 20 to 320 cycles of the pulse electrodeposition. Confirmed by the transmission electron microscopy images, the structure of CNFs was transformed from solid wire at 540oC to a bamboo-like structure at temperature beyond 800oC. 　The CNFs grown on carbon fabric, termed carpet-like CF, were hydrophobic and were used as a cathode electrode of fuel cells. A thermal impregnation method was adopted to achieve highly dispersion of Pd catalysts with a small dimension on the CNFs. In cyclic voltammograms, the Pd-supported carpet-like CF electrode exhibited an electrocatalytic activity for the O2 reduction in the 0.5 M sulfuric acid electrolyte. The polarization characteristic of Pd-supported carpet-like CF cathode single cell showed a maximum power density of 500 mW/cm2 and a current density of 173 mA/cm2 at 0.8 V, without additional gas diffusion backing. 　Examined in this work was another type of carpet-like CF, using the activated carbon fabric as the substrate for CNFs growth. The fabric was used as an electrode of supercapacitors to evaluate the efficiency of mass capacitance (F/g) and electrical-double layer capacitance (μF/cm2) in both aqueous and organic electrolytes. The hydrophilic carpet-like CF has a network structure of CNFs. For electrolyte molecules, the CNF network structure is much easier to access. Compared with the activated carbon fabric, the carpet-like CF electrode has a better performance in electrical-double layer capacitance. Results of AC impedance showed that electrolyte molecules exhibited a quick capacitance to frequencies under alternating potential when using the carpet-like CF electrode. 　As an electrode of supercapacitors, the activated carbon fabric has demonstrated a wide-temperature tolerance from 100oC to -40oC within a voltage window from -2 V to 2 V. In cyclic voltammograms, the coin cell assembly of activated carbon fabric electrodes in an organic electrolyte has yielded ideal rectangular shapes from 0oC to 100oC with an average mass capacitance of 90 F/g and, 60 F/g at -25oC. At an extremely low temperature of -40oC, the capacitance was still over 20 F/g. Another exciting feature of the activated carbon fabric supercapacitors was that they resumed their room temperature capacitance when cooled from 100oC and defrosted from -40oC, demonstrating an excellent repeatability and stability. The charge-discharge behavior of the activated carbon fabric supercapacitors showed long-cycle stability at extreme temperatures. The high electrochemical performance makes this type of supercapacitors very promising in many practical applications.

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46

Lin, Yu-Cheng, and 林育成. "A Hybrid Electrochemical Micro-Machining Method of Tungsten Microprobe." Thesis, 2012. http://ndltd.ncl.edu.tw/handle/e3w3c2.

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碩士
國立虎尾科技大學
機械與機電工程研究所
100
Microprobes are a component which can be used to measure the features of objects. It was applied to manufacturing widely. For example, it can be used to measure surface roughness, electricity, integrated circuit yield and so on. There are different kinds of tungsten microprobe machine technologies. They are Electrical Discharge Machining (EDM), Electrochemical Machining (ECM), Grinding Machining, etc. However, each of them has their own obvious advantages and disadvantages. The disadvantages of producing tungsten microprobes by electrolytic machines are long waiting time and inaccuracies. Otherwise, using grinding machines can form tungsten microprobes quickly, but it lowers the quality of surface roughness. Therefore, in this research, the researcher employs several methods to manufacture the tungsten microprobe, and then discuss about the probe features which was produced under the different electrolysis parameters. First, the researcher grinded the model of tungsten microprobe rapidly by mechanical grinding method; afterwards, leveled the surface of the tungsten microprobe by electrochemical machining, while also electrolyzing the original flat head of probe into a round head. The experiment attests that the new process of combining grinding machines and electrolytic machines can efficiently reduce machining time. For each product of one tungsten microprobe, machining time of grinding hybrid electrolysis process is only 110 seconds. Compared with pure grinding process, which takes 210 seconds, the time is reduced by 48%. Moreover, it reduces the time of electrolysis process by 94%, which takes 1800 seconds. Also, its surface roughness degree is better than the tungsten microprobe produced by pure grinding process. Using the new process to produce the tungsten microprobe can get less contact resistance under the same probing force, than even the ones produced by pure grinding machining method or the commercial ones. Keywords: grinding, electrolysis, tungsten microprobe, contact resistance

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47

"Graphene and Hybrid Perovskite Materials for Electronic and Electrochemical Devices." 2016. http://repository.lib.cuhk.edu.hk/en/item/cuhk-1292434.

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為了滿足全球對可持續能源和清潔環境日益增長的需求，發展新材料和有實際應用價值的能源器件是非常意義深遠的。在眾多新興的能源材料中，基於石墨烯的二維（2D）材料以及雜化鈣鈦礦材料在全世界範圍內獲得了廣泛的關注和研究興趣。本博士畢業論文詳細闡述了我在開發新材料的製備方法和基於合成的材料所開拓的電子和電化學器件方面的研究成果。
首先，我們使用常壓化學氣相沉積法（APCVD）在銅箔上合成了高質量的二維石墨烯。并展示了利用十八烷基磷酸單分子層修飾的溶液法所製備的雙層金屬氧化物（Al2Oy/TiOx,縮寫為ATO）作為高介電常數的介電層所裝配的低電壓背柵石墨烯場效應晶體管（GFETs）。得益于高質量的介電層和高質量的石墨烯層，器件在一個很小的柵電壓範圍內（-3.0伏到3.0伏）表現出來的空穴載流子遷移率在室溫下可以高達5805 cm2 V-1 s-1,電子遷移率可以達到3232 cm2 V-1 s-1。該研究提出了用一種有效的辦法可以在室溫下實現低電壓高遷移率的石墨烯場效應晶體管器件。此外，基於該器件結構，我們開發了一個策略，通過使用聚乙烯乙胺（PEI）來修飾器件界面以提高電子遷移率。修飾之後的器件顯示出了增強的器件性能，其中電子遷移率已高達6814 cm2 V-1 s-1,同時接觸電阻也降低至45歐姆。根據對比試驗研究，我們發現提高的電子遷移率主要是由PEI對金屬和石墨烯接觸界面的修飾作用決定的。
虽然二维石墨烯有很多优势，并能很好的用于电子器件中，但是仍有一应用是需要石墨烯的三维结构的性质。在这一部分，為了實現多孔三維（3D）石墨烯結構，以降低劇烈的層間團聚，我們闡示了一種低溫（650oC）APCVD生長方法，可以在微米級的鎳顆粒上合成高質量的彎曲石墨烯。同時系統地研究了生長溫度和顆粒尺寸對彎曲石墨烯形貌的影響，并可以將實驗結果與之前的石墨烯生長理論模型關聯起來，表明在鎳顆粒上呈現的大量原子級別的台階邊緣可以有效的促進甲烷分解，石墨烯形成和缺陷愈合。得益于彎曲的幾何結構，彎曲石墨烯在用作電極材料時，在KOH電解液中有203.4 F g1的比電容。兩電極測試表現出了出色的電化學性質，其中能量密度高達40.9 Wh kg-1，功率密度高達70 W kg-1，以及擁有長期的穩定性。與此同時，我通過探究彎曲石墨烯在其他過渡金屬顆粒上的生長，指出了另外一個不同的生長機理，以及表明了該生長方法可以用于生長不同3D石墨烯材料的通用性。
在第二部分展示的电化学电容器，是一种电化学器件，可以有效的分离离子导电性和电子导电性。所以在本毕业论文的第三部分，我還探究了另外一種新興的能源材料，有機金屬鹵化鈣鈦礦的電化學性質。一種基於有機鉛三碘化鈣鈦礦的薄膜電化學電容器（EC）被展示具有優良的循環性能。通過系統的對不同電解液和不同厚度的鈣鈦礦薄膜的電化學測試研究，鈣鈦礦的雙重傳導（電子傳導和離子傳導）過程被鑒定，并闡釋了鈣鈦礦層不僅能作為電極材料也可以作為一種固體電解液。通過對電化學阻抗譜（EIS）的結果進行電路模擬，鈣鈦礦薄膜中的可移動離子（即離子天然缺陷）密度可以被提取，而該數值比從一般鈣鈦礦電子器件，如太陽能電池估計出來的數值低。該結果表明有機金屬鹵化鈣鈦礦材料中的離子形成和傳輸過程可能更大程度的被自由載流子的流動所激活。
本文的最後部分呈現了本博士論文在研究成果和貢獻上的全面總結，并提出了基於二維材料和雜化材料的更多有能源器件的應用方向。
To fulfill the increasing global demand for sustainable energy and clean environment, it is of great significance to develop not only new materials but also practical energy devices. Among the emerging energy materials, graphene based two-dimensional (2D) materials and hybrid perovskite materials have drawn tremendous attention and research interest around the world. This thesis describes my research efforts in developing new material preparation methods and exploiting the electronic and electrochemical devices based on these materials.
In the first part, high-quality 2D graphene is grown on Cu foil by atmospheric pressure chemical vapor deposition (APCVD) method. A low-voltage back-gated graphene field-effect transistor (GFET) is demonstrated, which employs an octadecylphosphonic acid self-assembled monolayer modified solution-processed bilayer metal oxide (Al2Oy/TiOx, abbrev. as ATO) as the high-k gate dielectric. Owing to the high quality of the gate dielectric as well as the graphene layer, outstanding room-temperature hole mobility up to 5805 cm2 V-1 s-1 and electron mobility of 3232 cm2 V-1 s-1 are obtained in a small gate voltage range from -3.0 V to 3.0 V under vacuum. This study suggests an effective way to realize low-voltage high mobility GFETs at room temperature. Furthermore, based on the device structure, a strategy is developed to enhance the electron mobility with interface modification by poly (ethylene imine) (PEI). The modified device shows an enhanced performance with a high electron mobility (~ 6814 cm2 V-1 s-1) and a low contact resistance (~ 45 ohm). Upon a comparative study, it is found that the high electron mobility is mainly determined by the interface modification at the metal/graphene contact.
Although 2D graphene has a lot of advantages and can be well applied in the electronic devices, there are still some applications that need the three-dimensional (3D) response of graphene based materials. Thus in this part, to achieve porous and 3D graphene structure without severe aggregation, a low-temperature (650 oC) APCVD growth method is demonstrated to synthesize high-quality curved graphene on micron-sized Ni particles. The effects of growth temperature and particle size are systematically studied and the experimental observations can be well correlated with previous theoretical models on graphene growth, suggesting that a large amount of atomic step edges is presented at the Ni particle surface, which facilitate methane decomposition, graphene formation and defect healing. Due to the advantages of curved geometry, the curved graphene used as an electrode material reveals a specific capacitance of 203.4 F g-1 in aqueous KOH electrolyte. Two-electrode supercapacitors (or electrochemical capacitors) constructed with the curved graphene also show outstanding electrochemical properties, such as high energy density (40.9 Wh kg-1) and power density (70 kW kg-1), as well as long-term stability. In addition, other transition metal particles are also explored as the catalysts for the curved graphene growth, and the results indicate a different growth mechanism and the versatility of the present method in producing different kinds of 3D graphene materials.
Electrochemical capacitor, as demonstrated in the second part, is a kind of electrochemical devices, which can effectively decouple the ionic and electronic conduction. Thus in the third part of this thesis, I would like to explore the possibility of such device in the investigation of the ionic properties of an emerging photovoltaic material - organometal halide perovskite. A thin film electrochemical capacitor with excellent cyclability is demonstrated based on organolead triiodide perovskite. With systematical electrochemical characterizations on the cells with different electrolytes and perovskite thickness, dual conduction (electronic and ionic conduction) processes are identified in the perovskite films, revealing that the perovskite serves not only as an electrode but also a solid electrolyte. Through circuit modeling of the electrochemical impedance spectroscopy (EIS) characteristics, the density of mobile ions (i.e. ionic native defects) in the perovskite films is extracted and found lower than those estimated from perovskite electronic devices, e.g., solar cells. The result suggests that the ion formation and transport processes in organometal halide perovskites may largely be activated by the flow of free charge carriers.
In the last part, an overall summary on the findings and contributions of this thesis is present and the future research directions based on graphene and hybrid perovskite materials for electronic and electrochemical devices are proposed.
Zhou, Shuang.
Thesis Ph.D. Chinese University of Hong Kong 2016.
Includes bibliographical references (leaves ).
Abstracts also in Chinese.
Title from PDF title page (viewed on …).
Detailed summary in vernacular field only.
Detailed summary in vernacular field only.
Detailed summary in vernacular field only.
Detailed summary in vernacular field only.
Detailed summary in vernacular field only.

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48

Lan, Pei-Yu, and 藍珮瑜. "Poly(2,2-bithiophene)/titania Hybrid Solar Cells Prepared by Electrochemical Polymerization." Thesis, 2008. http://ndltd.ncl.edu.tw/handle/41631189290868076948.

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Анотація:

碩士
國立臺灣大學
高分子科學與工程學研究所
96
A series of novel organic/inorganic hybrids solar cells were fabricated and investigated. Various thicknesses of TiO2 films were coated on top of FTO glass by spin-casting using different concentrations of TiO2 colloids that synthesized by sol-gel method. This study developed an electrochemical polymerization route for preparing organic/inorganic hybrids for use as photoactive materials in photovoltaic devices. This new technique was benefited from the ability of using non-soluble conjugated polymers as major photoactive component in solar cells. Moreover, the monomer can be polymerized from the interstices of TiO2 matrices due to their much smaller size in comparison to the corresponding polymer, thus substantially increasing the donor-acceptor interface for exciton dissociation. The effect of titania film thickness on the performance of the photovoltaic cells constructed from these materials was examined. An approximate thickness of 165 nm of TiO2 exhibited an optimal cell performance with a short-circuit current, an open-circuit voltage, a fill factor and a power conversion efficiency of 0.171 mA/cm2, 0.42 V, 0.48 and 3.44E-2 %, respectively. Additionally, 2-thiophenecarboxylic acid was employed as a surface modifier to alter the TiO2 surface from hydrophilic to hydrophobic. The devices with 2-thiophenecarboxylic acid had an optimal short-circuit current, open-circuit voltage, fill factor and power conversion efficiency of 0.09 mA/cm2, 0.47 V, 0.48 and 2.02E-2 %, respectively. Although the cell performance was not improved, the Voc was slightly increased, revealing that surface modifier certainly ameliorated the interface properties of organic/inorganic.

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49

張聖章. "Preparation of high-quality graphene sheets under electrochemical/mechanical hybrid exfoliation." Thesis, 2014. http://ndltd.ncl.edu.tw/handle/43939312664094780277.

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碩士
國立臺灣師範大學
工業科技教育學系
102
In this study, using the liquid phase electrochemical/mechanical hybrid process for exfoliating a lot of few-layer graphene, after heating to 800 ℃ for two hours under argon/hydrogen (90/10) atmosphere controlled, producing high quality graphene sheet powder. First, natural graphite powder for the experimental circulation of the positive electrode or the negative electrode in an electrochemical intercalation ion solution, the use of intercalation ions and gas to form an expanded graphite, and then homogenized using a high speed clarifixator, a rotary-type cyclic mechanical agitation to generate shear force for expanded graphite, interrupted the van der Waals bonding between the graphite layers caused graphene delamination peel. Of course, during the mechanical exfoliation, simultaneously electrochemical exfoliated can be conducted, both of two mechanisms , in order to achieve fast, high-quality preparation of graphene sheets. Expected by the ion concentration in the solution, the positive and negative intercalation effects, intercalation voltage, intercalation speed, exfoliation parameters such as speed control, voltage and time can be achieved in high throughput, high quality graphene sheets purpose of production. The experimental results showed that the optimum conditions for the exfoliation time of 1 hour under the intercalation speed 2000 rpm, intercalation voltage 4 V, 1 hour intercalation speed of 10000 rpm, the average thickness of the graphene sheet is 2.2 nm the average size of 1 ~ 1.5 μm2, by the wavelength of 521 nm green laser Raman spectroscopy measurements show its 2D-band and G-band of the intensity ratio of 0.93 (I2D / IG = 0.93), half-height width is 67.53 (FWHM = 67.53), so the judgment of graphene sheets prepared by this method is few-layer graphene. Further, by evaluation of the weight of the throughput for this method is proved few-layer of graphene sheets reach to 20 wt.%, the throughput more than pure electrochemical method at least 2 times. This study also be exfoliation the graphene sheet transferred to the 300 nm SiO2 / Si substrate through an optical microscope (OM), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and atomic force microscopy (AFM) and other equipment, to evaluated the size of the graphene sheet, the surface morphology, thickness uniformity and quality of the crystal lattice. This study has confirmed that electrochemical/mechanical hybrid method, graphene sheets prepared for rapid, low cost, high quality, high yields and no oxidation of advantages for development into industrial mass production technology, and high-quality few-layer graphene of the conductive layer applied to the transparent conductive layer eventhough in the development of a super capacitor.

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50

"Detection of Nitroaromatic Explosives Using an Electrical- Electrochemical and Optical Hybrid Sensor." Doctoral diss., 2012. http://hdl.handle.net/2286/R.I.14563.

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abstract: In today's world there is a great need for sensing methods as tools to provide critical information to solve today's problems in security applications. Real time detection of trace chemicals, such as explosives, in a complex environment containing various interferents using a portable device that can be reliably deployed in a field has been a difficult challenge. A hybrid nanosensor based on the electrochemical reduction of trinitrotoluene (TNT) and the interaction of the reduction products with conducting polymer nanojunctions in an ionic liquid was fabricated. The sensor simultaneously measures the electrochemical current from the reduction of TNT and the conductance change of the polymer nanojunction caused from the reduction product. The hybrid detection mechanism, together with the unique selective preconcentration capability of the ionic liquid, provides a selective, fast, and sensitive detection of TNT. The sensor, in its current form, is capable of detecting parts per trillion level TNT in the presence of various interferents within a few minutes. A novel hybrid electrochemical-colorimetric (EC-C) sensing platform was also designed and fabricated to meet these challenges. The hybrid sensor is based on electrochemical reactions of trace explosives, colorimetric detection of the reaction products, and unique properties of the explosives in an ionic liquid (IL). This approach affords not only increased sensitivity but also selectivity as evident from the demonstrated null rate of false positives and low detection limits. Using an inexpensive webcam a detection limit of part per billion in volume (ppbV) has been achieved and demonstrated selective detection of explosives in the presence of common interferences (perfumes, mouth wash, cleaners, petroleum products, etc.). The works presented in this dissertation, were published in the Journal of the American Chemical Society (JACS, 2009) and Nano Letters (2010), won first place in the National Defense Research contest in (2009) and has been granted a patent (WO 2010/030874 A1). In addition, other work related to conductive polymer junctions and their sensing capabilities has been published in Applied Physics Letters (2005) and IEEE sensors journal (2008).
Dissertation/Thesis
Ph.D. Electrical Engineering 2012

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Дисертації з теми "HYBRID ELECTROCHEMICAL"

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