Journal articles on the topic 'Electrolyte solvent'
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1
Lu, Xuejun, María C. Gutiérrez, M. Luisa Ferrer, Xuejun Lu, and Jian Liu. "“Tri-Solvent-in-Salt” Electrolytes for High-Performance Supercapacitors." ECS Meeting Abstracts MA2022-01, no. 35 (July 7, 2022): 1412. http://dx.doi.org/10.1149/ma2022-01351412mtgabs.
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Electrolytes chemistry for high-performance supercapacitors (SCs) has been addressed recently, where solvents included in electrolyte composition dissolving or mixing the electrochemically active salts or ILs have been typically seen as a mere medium.[1] Specifically, attention regarding the achievement of high-performacne SCs has also been paid to, e.g., water-in-salt (WIS), solvent-in-salt (SIS), and bi-solvent-in-salt (BSIS) electrolytes, demonstrating that solvent molecules may indeed play a more active role.[2 - 4] In this presentation, we will talk about the design of a tri-solvent-in-salt (TSIS) electrolyte where every solvent contributed (with an IL, i.e., EMIMBF4) to the formation of an electrochemically active hydrogen bond (HB) complex structure. Raman and NMR spectroscopies, as well as molecular dynamic (MD) simulations, helped elucidate the ratio among all compounds (e.g., solvents and IL) in the HB complex structure that best works as an electrolyte. For instance, the eutectic mixture of H2O and dimethylsulfoxide (DMSO) in a 2 to 1 molar ratio primary HB complex structures with mixed EMIMBF4 offers a low melting point and low flammability, then add acetonitrile (CH3CN) in different molar ratios providing an improvement of the rate capability to the resulting electrolyte. As compared to other electrolytes, the TSIS electrolyte composed in a molality of 5.8 m (TSIS-5.8) showed the cost efficiency and exhibited a low self-extinction rate. Moreover, SCs operating with TSIS-5.8, at -70 °C and up to 2.7 V provided energy densities of ca. 49 and 18 Wh kg-1, respectively, power densities of 10,000 and 17,000 W kg-1, the capacitance retention of ca. 82% after 15,000 cycles at 4 A g-1 and a self-discharge as low as 22%. The use of ternary solvent mixtures combining different solvents in the proper molar ratios opens up an easy and low-cost path to design many new electrolytes in terms of non-flammability, non-toxicity, high electrical conductivity, and wide electrochemical stability window (ESW). Forthcoming research could use the knowledge provided by this work in terms of ions solvation and transport in TSIS electrolytes and explore the interfacial interactions between electrolyte and electrode material to determine their respective relevance in the performance of SCs. Keywords: tri-solvent-in-salt (TSIS), hydrogen bond, eutectic mixtures, supercapacitors Reference ： [1] F. Béguin, et al. Carbons and electrolytes for advanced supercapacitors. Adv. Mater., 26 (2014), 2219-2251. [2] Q. Dou, et al. Safe and high-rate supercapacitors based on an ‘‘Acetonitrile/Water in Salt’’ hybrid electrolyte. Energy Environ. Sci, 11 (2018), 3212-3219. [3] X. Lu, et al. Aqueous-Eutectic-in-Salt Electrolytes for High-Energy-Density Supercapacitors with an Operational Temperature Window of 100 °C, from −35 to +65 °C. ACS Appl. Mater. Interfaces 2020, 12, 26, 29181–29193. [4] X. Lu, et al. Aqueous Co-Solvent in Zwitterionic-based Protic Ionic Liquids as Electrolytes in 2.0 V Supercapacitors. ChemSusChem 2020, 13, 5983. [5] X. Lu, et al. EMIMBF4 in ternary liquid mixtures of water, dimethyl sulfoxide and acetonitrile as “tri-solvent-in-salt” electrolytes for high-performance supercapacitors operating at -70 °C. Energy Storage Mater., 40, (2021), 368-385.
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Ashraf, Juveiriah M., Myriam Ghodhbane, and Chiara Busa. "The Effect of Ionic Carriers and Degree of Solidification on the Solid-State Electrolyte Performance for Free-Standing Carbon Nanotube Supercapacitor." ECS Meeting Abstracts MA2022-02, no. 7 (October 9, 2022): 2490. http://dx.doi.org/10.1149/ma2022-0272490mtgabs.
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To eliminate electrolyte leakage, the development of safe and flexible supercapacitors necessitates solid-state electrolytes which integrate both high mechanical and electrochemical capabilities. Quasi-solid-state electrolytes, which constitute a polymer matrix along with an aqueous electrolytic phase, are a viable answer to this problem. Recently, gel electrolytes have gained a lot of attention in flexible and wearable electronic devices due to their remarkable advancements. However, the limitation in the multi-functional abilities and high-performance in such gels hinders the practical usage of such devices. On the electrochemical perspective, the performance of the gel electrolyte depends on the type of ionic carrier (acidic, alkaline, or salt-based), size of the ion, solvent concentration, type of polymer, as well as the interaction between the polymer and other components. Moreover, the performance of the electrolyte differs with the electrode-electrolyte interface and thus is highly dependent on the electrode material. For this reason, it is vital to carry a parametric study to evaluate the effect of the above stated. The aim of this study is to investigate the effect of changing the ionic carrier (namely H3PO4, KOH and LiCl) as well as the solvent concentration on architecturally engineered PVA-based electrolytes’ performance in free-standing CNT supercapacitor using a bio-based compound, cellulose as a binder. The dependence of the electrolyte’s mechanical structure for long term stability is further evaluated by using the optimized concentration of each (H3PO4, KOH and LiCl) by freezing and de-freezing the gel to form membrane-like films, as a result of the increased physical cross-linking. The supercapacitors are studied for their capacitance, charge/discharge capabilities as well their long-term stability and also compared with aqueous electrolyte for the three aforementioned ionic carriers.
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Wang, Jianji, Yang Zhao, Kelei Zhuo, and Ruisen Lin. "A partial-molar volume study of electrolytes in propylene carbonate-based lithium battery electrolyte solutions at 298.15 K." Canadian Journal of Chemistry 80, no. 7 (July 1, 2002): 753–60. http://dx.doi.org/10.1139/v02-092.
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Apparent molar volumes (V2, ϕ ) and standard partial-molar volumes (V20, ϕ ) of LiClO4 and LiBr at 298.15 K have been determined from precise density measurements in solvent mixtures of propylene carbonate (PC) with dimethylformamide (DMF), tetrahydrofuran (THF), acetonitrile (AN), and methyl formate (MF). The scaled particle theory is used to calculate the contributions of the cavity formation and the electrolyte-solvent interactions to the standard partial-molar volumes. It is shown that V20, ϕ is strongly dependent on the nature of the solvents, and the trends in V20, ϕ with composition of the solvent mixtures are determined by the interaction volumes of electrolytes with solvents. The results are discussed in terms of ionic preferential solvation, packing effect of solvents in the solvation shell, and electrostriction of solvents by ion.Key words: partial-molar volume, scaled particle theory, lithium salts, propylene carbonate, solvent mixtures, lithium battery electrolytes.
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Kadam, V. V., A. B. Nikumbh, T. B. Pawar, and V. A. Adole. "Density and Viscosity of LiCl, LiBr, LiI and Kcl in Aqueous Methanol at 313.15K." Oriental Journal Of Chemistry 37, no. 5 (October 30, 2021): 1083–90. http://dx.doi.org/10.13005/ojc/370510.
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The densities and viscosities of electrolytes are essential to understand many physicochemical processes that are taking place in the solution. In the present research, the densities and viscosities of lithium halides, LiX (X = Cl, Br, I ) and KCl in (0, 20, 40, 50, 60, 80 and 100) mass % of methanol + water at 313.15K were calculated employing experimental densities (ρ), the apparent molar volumes( ϕv) and limiting apparent molar volumes (0v) of the electrolytes. The (0v) of electrolyte offer insights into solute-solution interactions. In terms of the Jones-Dole equation for strong electrolyte solution, the experimental data of viscosity were explored. Viscosity coefficients A and B have been interpreted and discussed. The B-coefficient values in these systems increase with increase of methanol in the solvents mixtures. This implied that when the dielectric constant of the solvent decreases, so do the solvent-solvent interactions in these systems.
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Wang, Jianji, Yang Zhao, Kelei Zhuo, and Ruisen Lin. "Viscosity Properties of Electrolytes in Propylene Carbonate Based Lithium Battery Electrolyte Solutions." Zeitschrift für Physikalische Chemie 217, no. 6 (June 1, 2003): 637–52. http://dx.doi.org/10.1524/zpch.217.6.637.20445.
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AbstractViscosities of LiClO4 and LiBr have been measured in solvent mixtures of propylene carbonate (PC) with dimethylformamide (DMF), tetrahydrofuran (THF), acetonitrile (AN) and methyl formate (MF) at 298.15K. The dependence of viscosity on the composition of the mixed solvents was fitted with an equation without adjustable parameter. Viscosity B-coefficients for lithium salts and the corresponding activation free energies (Δμ0,≠) for viscous flow have been evaluated. At the same time, viscosity B-coefficients were predicted by the dielectric friction theory. The unsuccessful prediction of the composition dependence of the B-coefficients indicates that improvements will be necessary on the theory with taking account of the short-range interaction and molecular nature of the solvents. Furthermore, solute–solvent interactions in these mixed solvents are discussed in terms of the B-coefficients and activation parameters.
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Ren, Xiaodi, Peiyuan Gao, Lianfeng Zou, Shuhong Jiao, Xia Cao, Xianhui Zhang, Hao Jia, et al. "Role of inner solvation sheath within salt–solvent complexes in tailoring electrode/electrolyte interphases for lithium metal batteries." Proceedings of the National Academy of Sciences 117, no. 46 (November 3, 2020): 28603–13. http://dx.doi.org/10.1073/pnas.2010852117.
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Functional electrolyte is the key to stabilize the highly reductive lithium (Li) metal anode and the high-voltage cathode for long-life, high-energy-density rechargeable Li metal batteries (LMBs). However, fundamental mechanisms on the interactions between reactive electrodes and electrolytes are still not well understood. Recently localized high-concentration electrolytes (LHCEs) are emerging as a promising electrolyte design strategy for LMBs. Here, we use LHCEs as an ideal platform to investigate the fundamental correlation between the reactive characteristics of the inner solvation sheath on electrode surfaces due to their unique solvation structures. The effects of a series of LHCEs with model electrolyte solvents (carbonate, sulfone, phosphate, and ether) on the stability of high-voltage LMBs are systematically studied. The stabilities of electrodes in different LHCEs indicate the intrinsic synergistic effects between the salt and the solvent when they coexist on electrode surfaces. Experimental and theoretical analyses reveal an intriguing general rule that the strong interactions between the salt and the solvent in the inner solvation sheath promote their intermolecular proton/charge transfer reactions, which dictates the properties of the electrode/electrolyte interphases and thus the battery performances.
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Nguyen, Thuy-Duy Thi, Phuong Tuyet Nguyen, and Phuong Hoang Tran. "Dye-sensitized solar cells using deep eutectic solvents mixed with ethanol as an effective electrolyte medium." Science and Technology Development Journal 21, no. 1 (June 8, 2018): 15–23. http://dx.doi.org/10.32508/stdj.v21i1.424.
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This research aims to develop a new type of electrolyte for dye-sensitized solar cells (DSCs) which can be produced in cost-effective and large scale. DSCs using deep eutectic solvents (DESs) mixed with ethanol (50% w/w DES content), as an electrolyte medium, was studied herein for the first time. Ten types of DESs were synthesized and three among them were potential candidates for DSC electrolytes. Compared to toxic and volatile organic solvents, this mixed solvent is more eco-friendly and inexpensive. According to J-V curve measurements, DSCs that used DES-ethanol medium showed promising photovoltaic performance.
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Apolinário, Arlete, Célia T. Sousa, Gonçalo N. P. Oliveira, Armandina M. L. Lopes, João Ventura, Luísa Andrade, Adélio Mendes, and João P. Araújo. "Tailoring the Anodic Hafnium Oxide Morphology Using Different Organic Solvent Electrolytes." Nanomaterials 10, no. 2 (February 22, 2020): 382. http://dx.doi.org/10.3390/nano10020382.
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Highly ordered anodic hafnium oxide (AHO) nanoporous or nanotubes were synthesized by electrochemical anodization of Hf foils. The growth of self-ordered AHO was investigated by optimizing a key electrochemical anodization parameter, the solvent-based electrolyte using: Ethylene glycol, dimethyl sulfoxide, formamide and N-methylformamide organic solvents. The electrolyte solvent is here shown to highly affect the morphological properties of the AHO, namely the self-ordering, growth rate and length. As a result, AHO nanoporous and nanotubes arrays were obtained, as well as other different shapes and morphologies, such as nanoneedles, nanoflakes and nanowires-agglomerations. The intrinsic chemical-physical properties of the electrolyte solvents (solvent type, dielectric constant and viscosity) are at the base of the properties that mainly affect the AHO morphology shape, growth rate, final thickness and porosity, for the same anodization voltage and time. We found that the interplay between the dielectric and viscosity constants of the solvent electrolyte is able to tailor the anodic oxide growth from continuous-to-nanoporous-to-nanotubes.
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Sedlak, Petr, Pavel Kaspar, Dinara Sobola, Adam Gajdos, Jiri Majzner, Vlasta Sedlakova, and Petr Kubersky. "Solvent Evaporation Rate as a Tool for Tuning the Performance of a Solid Polymer Electrolyte Gas Sensor." Polymers 14, no. 21 (November 6, 2022): 4758. http://dx.doi.org/10.3390/polym14214758.
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Solid polymer electrolytes show their potential to partially replace conventional electrolytes in electrochemical devices. The solvent evaporation rate represents one of many options for modifying the electrode–electrolyte interface by affecting the structural and electrical properties of polymer electrolytes used in batteries. This paper evaluates the effect of solvent evaporation during the preparation of solid polymer electrolytes on the overall performance of an amperometric gas sensor. A mixture of the polymer host, solvent and an ionic liquid was thermally treated under different evaporation rates to prepare four polymer electrolytes. A carbon nanotube-based working electrode deposited by spray-coating the polymer electrolyte layer allowed the preparation of the electrode–electrolyte interface with different morphologies, which were then investigated using scanning electron microscopy and Raman spectroscopy. All prepared sensors were exposed to nitrogen dioxide concentration of 0–10 ppm, and the current responses and their fluctuations were analyzed. Electrochemical impedance spectroscopy was used to describe the sensor with an equivalent electric circuit. Experimental results showed that a higher solvent evaporation rate leads to lower sensor sensitivity, affects associated parameters (such as the detection/quantification limit) and increases the limit of the maximum current flowing through the sensor, while the other properties (hysteresis, repeatability, response time, recovery time) change insignificantly.
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Tang, Lufan, Qiang Wei, Jiawei Yan, Yudi Hu, Xuncai Chen, Guannan Wang, Su Htike Aung, Than Zaw Oo, Dongliang Yan, and Fuming Chen. "Redox Flow Capacitive Deionization in a Mixed Electrode Solvent of Water and Ethanol." Journal of The Electrochemical Society 169, no. 1 (January 1, 2022): 013501. http://dx.doi.org/10.1149/1945-7111/ac47e9.
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In redox flow electrode capacitive deionization (FCDI), the solubility of the redox electrolyte and flowability of the carbon slurry have a great influence on the salt removal rate and energy consumption. In this work, a mixed solvent electrolyte is proposed for FCDI, which consists of iodide/triiodide redox couples and a carbon slurry in a mixed solvent of water and ethanol (1:1). At a current density of 5 mA cm−2, the salt removal rate in the mixed solvent can reach up to 2.72 μg cm−2 s−1, which is much higher than the value of 1.74 μg cm−2 s−1 and 2.37 μg cm−2 s−1 obtained in aqueous and ethanol solutions, respectively. This is attributed to the fast transport of ions during the redox reaction in organic solvents and the excellent flowability of the carbon slurry under aqueous conditions, which can provide more reaction sites for iodide/triiodide redox reactions and faster electron transportation. This unique FCDI with organic and aqueous mixed solvent electrolytes provides a new perspective for the development of redox flow electrochemical desalination.
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Jun, H. K., M. A. Careem, and A. K. Arof. "A Suitable Polysulfide Electrolyte for CdSe Quantum Dot-Sensitized Solar Cells." International Journal of Photoenergy 2013 (2013): 1–10. http://dx.doi.org/10.1155/2013/942139.
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A polysulfide liquid electrolyte is developed for the application in CdSe quantum dot-sensitized solar cells (QDSSCs). A solvent consisting of ethanol and water in the ratio of 8 : 2 by volume has been found as the optimum solvent for preparing the liquid electrolytes. This solvent ratio appears to give higher cell efficiency compared to pure ethanol or water as a solvent. Na2S and S give rise to a good redox couple in the electrolyte for QDSSC operation, and the optimum concentrations required are 0.5 M and 0.1 M, respectively. Addition of guanidine thiocyanate (GuSCN) to the electrolyte further enhances the performance. The QDSSC with CdSe sensitized electrode prepared using 7 cycles of successive ionic layer adsorption and reaction (SILAR) produces an efficiency of 1.41% with a fill factor of 44% on using a polysulfide electrolyte of 0.5 M Na2S, 0.1 M S, and 0.05 M GuSCN in ethanol/water (8 : 2 by volume) under the illumination of 100 mW/cm2white light. Inclusion of small amount of TiO2nanoparticles into the electrolyte helps to stabilize the polysulfide electrolyte and thereby improve the stability of the CdSe QDSSC. The CdSe QDs are also found to be stable in the optimized polysulfide liquid electrolyte.
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Kim, Sang Cheol, and Yi Cui. "Probing Solvation Thermodynamics of Lithium Battery Electrolytes through Potentiometric Methods." ECS Meeting Abstracts MA2022-02, no. 2 (October 9, 2022): 164. http://dx.doi.org/10.1149/ma2022-022164mtgabs.
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The electrolyte is a principal component of a lithium battery that impacts almost every facet of the battery’s performance. Solvation of lithium ions in electrolyte solution is key to understanding the electrolyte, but our understanding of solvation lags behind its significance. Particularly, estimating solvation free energy has been largely limited to computational simulations. Despite their versatility, simulations can be computationally expensive, and experimental methods to complement simulations are desired. We have recently introduced a potentiometric technique to probe the relative solvation free energy of lithium ions in battery electrolytes. We devised an electrochemical cell composed of two half-cells, with symmetric electrodes but asymmetric electrolytes. Whereas the open circuit potential of a conventional lithium-ion battery measures the free energy differences of lithium ions in the two electrodes, our experimental setup measures the energy differences of the lithium ions in two different electrolytes. By measuring the cell potential with a reference electrolyte, we can quantitatively characterize lithium ion solvation energy of an electrolyte of interest. The effects of concentration, anion and solvent on solvation energy are explored and verified with simulations. Particularly, we establish a correlation between cell potential (Ecell) and cyclability of high-performance electrolytes for lithium metal anodes. We find that solvents with more negative cell potentials and positive solvation energies—those weakly binding to Li+—lead to improved cycling stability. Weaker solvents are conjectured to have more anion-rich solvation structures that lead to anion-derived solid-electrolyte interphases, a hypothesis supported by cryogenic electron microscopy. It reveals that weaker solvation is correlated to an inorganic anion-derived solid-electrolyte interphase that stabilizes cycling.
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Smiatek, Jens, Andreas Heuer, and Martin Winter. "Properties of Ion Complexes and Their Impact on Charge Transport in Organic Solvent-Based Electrolyte Solutions for Lithium Batteries: Insights from a Theoretical Perspective." Batteries 4, no. 4 (December 3, 2018): 62. http://dx.doi.org/10.3390/batteries4040062.
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Electrolyte formulations in standard lithium ion and lithium metal batteries are complex mixtures of various components. In this article, we review molecular key principles of ion complexes in multicomponent electrolyte solutions in regards of their influence on charge transport mechanisms. We outline basic concepts for the description of ion–solvent and ion–ion interactions, which can be used to rationalize recent experimental and numerical findings concerning modern electrolyte formulations. Furthermore, we discuss benefits and drawbacks of empirical concepts in comparison to molecular theories of solution for a more refined understanding of ion behavior in organic solvents. The outcomes of our discussion provide a rational for beneficial properties of ions, solvent, co-solvent and additive molecules, and highlight possible routes for further improvement of novel electrolyte solutions.
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Astakhov, Mikhail V., Ludmila A. Puntusova, Ruslan R. Galymzyanov, Ilya S. Krechetov, Alexey V. Lisitsyn, Svetlana V. Stakhanova, and Natalia V. Sviridenkova. "Multicomponent non-aqueous electrolytes for high temperature operation of supercapacitors." Butlerov Communications 61, no. 1 (January 31, 2020): 67–75. http://dx.doi.org/10.37952/roi-jbc-01/20-61-1-67.
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Multicomponent non-aqueous electrolytes based on cyclic carbonates and tetraethylammonium tetrafluoroborate have been developed for the operation of supercapacitors at elevated temperatures. Propylene carbonate, which has a high dielectric constant and a high boiling point, was used as the main solvent of electrolytes. However, a significant drawback of propylene carbonate is its high viscosity, which leads to decrease in the electrical conductivity of electrolytes based on it compared to electrolytes based on acetonitrile. To increase the electrical conductivity, an additional component was introduced into the electrolyte – a cosolvent with the necessary set of properties. When choosing cosolvents, two approaches were used. In the first case, to increase the dielectric permittivity of the liquid phase, ethylene carbonate having a higher dielectric constant than propylene carbonate was introduced into the electrolyte. This approach made it possible to significantly increase the electrical conductivity of the electrolyte and to achieve high resource stability of the supercapacitor. The values of the specific capacitance and energy of the supercapacitor with the introduction of ethylene carbonate in the electrolyte practically did not change. In the second case, butyl acetate, which has a low viscosity but has a moderate polarity and a sufficiently high boiling point, was used as a co-solvent. In this case, not only an increase in the electrical conductivity of the electrolyte was observed, but also a significant increase in the capacitive characteristics of the supercapacitor. It is shown that the use of a mixture of cyclic carbonates and esters as a solvent in the composition of the electrolyte can increase its specific conductivity by 40%, and the specific energy consumption of a supercapacitor by 20%. The developed electrolytes provide long-term operation of supercapacitors both at room temperature and at elevated temperatures up to 80 °С.
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Cao, Xia, Peiyuan Gao, Xiaodi Ren, Lianfeng Zou, Mark H. Engelhard, Bethany E. Matthews, Jiangtao Hu, et al. "Effects of fluorinated solvents on electrolyte solvation structures and electrode/electrolyte interphases for lithium metal batteries." Proceedings of the National Academy of Sciences 118, no. 9 (February 25, 2021): e2020357118. http://dx.doi.org/10.1073/pnas.2020357118.
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Electrolyte is very critical to the performance of the high-voltage lithium (Li) metal battery (LMB), which is one of the most attractive candidates for the next-generation high-density energy-storage systems. Electrolyte formulation and structure determine the physical properties of the electrolytes and their interfacial chemistries on the electrode surfaces. Localized high-concentration electrolytes (LHCEs) outperform state-of-the-art carbonate electrolytes in many aspects in LMBs due to their unique solvation structures. Types of fluorinated cosolvents used in LHCEs are investigated here in searching for the most suitable diluent for high-concentration electrolytes (HCEs). Nonsolvating solvents (including fluorinated ethers, fluorinated borate, and fluorinated orthoformate) added in HCEs enable the formation of LHCEs with high-concentration solvation structures. However, low-solvating fluorinated carbonate will coordinate with Li+ ions and form a second solvation shell or a pseudo-LHCE which diminishes the benefits of LHCE. In addition, it is evident that the diluent has significant influence on the electrode/electrolyte interphases (EEIs) beyond retaining the high-concentration solvation structures. Diluent molecules surrounding the high-concentration clusters could accelerate or decelerate the anion decomposition through coparticipation of diluent decomposition in the EEI formation. The varied interphase features lead to significantly different battery performance. This study points out the importance of diluents and their synergetic effects with the conductive salt and the solvating solvent in designing LHCEs. These systematic comparisons and fundamental insights into LHCEs using different types of fluorinated solvents can guide further development of advanced electrolytes for high-voltage LMBs.
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Storck, Jan Lukas, Marius Dotter, Sonia Adabra, Michelle Surjawidjaja, Bennet Brockhagen, and Timo Grothe. "Long-Term Stability Improvement of Non-Toxic Dye-Sensitized Solar Cells via Poly(ethylene oxide) Gel Electrolytes for Future Textile-Based Solar Cells." Polymers 12, no. 12 (December 18, 2020): 3035. http://dx.doi.org/10.3390/polym12123035.
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To overcome the long-term stability problems of dye-sensitized solar cells (DSSC) due to solvent evaporation and leakage, gelling the electrolyte with polymers is an appropriate option. Especially for future applications of textile-based DSSCs, which require cost-effective and environmentally friendly materials, such an improvement of the electrolyte is necessary. Therefore, the temporal progressions of efficiencies and fill factors of non-toxic glass-based DSSCs resulting from different gel electrolytes with poly(ethylene oxide) (PEO) are investigated over 52 days comparatively. Dimethyl sulfoxide (DMSO) proved to be a suitable non-toxic solvent for the proposed gel electrolyte without ionic liquids. A PEO concentration of 17.4 wt% resulted in an optimal compromise with a relatively high efficiency over the entire period. Lower concentrations resulted in higher efficiencies during the first days but in a poorer long-term stability, whereas a higher PEO concentration resulted in an overall lower efficiency. Solvent remaining in the gel electrolyte during application was found advantageous compared to previous solvent evaporation. In contrast to a commercial liquid electrolyte, the long-term stability regarding the efficiency was improved successfully with a similar fill factor and thus equal quality.
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Zhang, Huang, Thomas Diemant, Bingsheng Qin, Huihua Li, R. Jürgen Behm, and Stefano Passerini. "Solvent-Dictated Sodium Sulfur Redox Reactions: Investigation of Carbonate and Ether Electrolytes." Energies 13, no. 4 (February 14, 2020): 836. http://dx.doi.org/10.3390/en13040836.
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Sulfur-based cathode chemistries are essential for the development of high energy density alkali-ion batteries. Here, we elucidate the redox kinetics of sulfur confined on carbon nanotubes, comparing its performance in ether-based and carbonate-based electrolytes at room temperature. The solvent is found to play a key role for the electrochemical reactivity of the sulfur cathode in sodium–sulfur (Na–S) batteries. Ether-based electrolytes contribute to a more complete reduction of sulfur and enable a higher electrochemical reversibility. On the other hand, an irreversible solution-phase reaction is observed in carbonate solvents. This study clearly reveals the solvent-dependent Na–S reaction pathways in room temperature Na–S batteries and provides an insight into realizing their high energy potential, via electrolyte formulation design.
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Drvarič Talian, Sara, and Robert Dominko. "Changes in internal resistance of lithium-sulfur batteries when using electrolytes based on ionic liquid [DEME][TFSI], sulfolane or TEGDME solvent." Anali PAZU 11, no. 1-2 (May 9, 2022): 64–71. http://dx.doi.org/10.18690/analipazu.11.1-2.64-71.2021.
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Internal resistance of lithium-sulfur batteries was investigated with impedance spectroscopy. In order to understand the effect of various common solvents for Li-S battery preparation, the electrolyte in the cells was varied (ionic liquid [DEME][TFSI], sulfolane or TEGDME solvent). The impedance changes were followed at several points during discharge and charge of the batteries and through 50 cycles of their use. The resulting spectra were analyzed and fitted, extracting information on four different impedance contribution. The contributions were assigned to the electrolyte, anode or cathode. Their change through a single cycle and through multiples cycles of battery use was evaluated as well as compared between cells employing different electrolytes.
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Kumar, Suresh, and Hardeep Anand. "Ionic Association of Potassium and Tetrabutylammonium Thiocyanate Salts in Binary Mixtures of γ-Butyrolactone and N,N-Dimethylacetamide at 298.15 K and 308.15 K." Asian Journal of Chemistry 34, no. 10 (2022): 2749–56. http://dx.doi.org/10.14233/ajchem.2022.23856.
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Solvation consequences of potassium thiocyanate (KSCN) and tetrabutylammonium thiocyanate (Bu4NSCN) in γ-butyrolactone (GBL), N,N-dimethylacetamide (DMA) and their binary mixtures in concentration range (0.01-0.001) mol Kg–1 of 0, 25, 50, 60, 80 and 100 mol% DMA at T = 298.15 K and 308.15 K have been studied using conductometric study and some samples of KSCN in GBL + DMA binary mixtures of different electrolytic concentrations at ambient conditions studied by FTIR spectroscopic methods. The Shedlovsky equation has been used to elucidate the data in terms of the limiting molar conductances (Λo), ion-pair association constants (KA). The Walden products (Λoηo), solvated radii (ri) and standard free energies of association (ΔGºA) were further evaluated in terms of solvation of ions. The reference electrolyte tetrabutylammonium tetraphenylborate (Bu4NBPh4) was used to determine the limiting molar ionic conductances. In pure solvents and their binary mixtures, electrolytes showed a strong association. The K+ ions have greater solvation in GBL than in DMA observed on basis of solvated radii in GBL + DMA binary solvent mixtures at both experimental temperatures. The study demonstrates that the ion-solvent interactions decrease on enhancing the temperature. The FTIR analysis was applied to obtain information about molecular as well as ionic association of KSCN in GBL + DMA binary mixtures at the ambient conditions, which has provided the information on structuring infrared modes of vibrational stretching frequencies according to the nature of the solvents or the cations. Shifting of vibrational frequencies of several functional groups of DMA and GBL in binary mixed solvents has been observed in terms of ion-ion, ion-solvent and solvent-solvent interactions.
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Ravindran, D., P. Vickraman, and N. Sankarasubramanian. "Conductivity Studies on Nano ZnO Incorporated PVC-PVdF Gel Electrolytes for Li+ Ion Battery Application." Applied Mechanics and Materials 787 (August 2015): 563–67. http://dx.doi.org/10.4028/www.scientific.net/amm.787.563.
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Polymer electrolytes with poly(vinyl chloride) (PVC) and poly(vinylidene fluoride)(PVdF) blend as matrix and lithium perchlorate (LiClO4) as dopant salt were prepared by solvent casting technique. Propylene carbonate was used as plasticizer and tetrahydrofuran (THF) as common solvent. Zinc oxide nano particles were synthesized through novel solid-state milling method and incorporated as filler. The content (wt%) of nano filler in the polymer electrolyte was systematically varied to study its influence on the conductivity of the electrolyte membranes. The films were subjected to complex impedance analysis in the frequency range 50 – 100 KHz. The analysis reveals the strong influence of filler particles on the conductivity profile of the electrolytes.
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Huynh, Tuyên Thi Kim, Thai Thị A. Đinh, Phuong Hoang Tran, Thanh Duy VO, Man Van Tran, and Phung My Loan Le. "Physical and electrochemical properties of DES solvents based on 2,2,2-trifluorocetamide and LiTFSI salt for Li-ion batteries." Science and Technology Development Journal - Natural Sciences 4, no. 2 (May 6, 2020): First. http://dx.doi.org/10.32508/stdjns.v4i2.872.
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The liquid electrolyte transports lithium ions from anode to cathode during charging, and vice versa. The choice of electrolyte is also important since high ionic conductivity between electrodes is essential for high-performance batteries. Liquid electrolytes with lithium salt dissolved in an organic solvent have been widely used since the 1970s when lithium primary batteries were first developed. Most lithium secondary batteries available today use organic electrolytes. Ionic liquids consist of organic cations and inorganic anions, due to the absence of a combustible and flammable organic solvent, they are known to produce safer batteries. Furthermore, they have a high polarity that allows dissolution of inorganic and organic metal compounds, and they can exist in a liquid state over a wide temperature range. Another type of solvent with similar physical properties and phase behavior to ILs is deep eutectic solvents (DESs) about which the first paper was recently published in 2001. These solvents are mixtures that have a much lower melting point than that of any of their individual components, mainly due to the charge delocalization occurring through hydrogen bonds between them. DESs are generally favored over ILs because they are cheaper and easier to prepare with high purity. In this work, Deep Eutectic Solvents (DESs) were prepared by simple mixing Lithium bis[(trifluoromethane)sulfonyl] imide (LiTFSI) salt and 2,2,2-trifluoroacetamide TFA at various ratios ranging from 1:1.5 to 1:4, respectively. The formation of DESs was characterized by Infrared Spectroscopy (IR) and Thermogravimetric analysis (TGA). Their physical and electrochemical properties were also evaluated based on their viscosity, conductivity, and oxidation stability window. Amongst our systems of interest, DES with LiTFSI: FAc ratio of 1:4 is the most promising as the electrolyte for Li-ion batteries, because it exhibited the lowest viscosity (42.2 mPa.s), the highest ionic conductivity (1.53 mS.cm-1 at 30oC) and relatively good anodic stability (5.2 V vs. Li+/Li).
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Ghorbanzade, Pedram, Laura C. Loaiza, and Patrik Johansson. "Plasticized and salt-doped single-ion conducting polymer electrolytes for lithium batteries." RSC Advances 12, no. 28 (2022): 18164–67. http://dx.doi.org/10.1039/d2ra03249j.
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Azeez, Fadhel, and Abdelrahman Refaie. "Integration of Semi-Empirical and Artificial Neural Network (ANN) for Modeling Lithium-Ion Electrolyte Systems Dynamic Viscosity." Journal of The Electrochemical Society 169, no. 2 (February 1, 2022): 020527. http://dx.doi.org/10.1149/1945-7111/ac4840.
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The dynamic viscosity is a key characteristic of electrolyte performance in a Lithium-ion (Li-ion) battery. This study introduces a one-parameter semi-empirical model and artificial neural network (ANN) to predict the viscosity of salt-free solvent mixtures and relative viscosity of Li-ion electrolyte solutions (lithium salt + solvent mixture), respectively. Data used in this study were obtained experimentally, in addition to data extracted from literature. The ANN model has seven inputs: salt concentration, electrolyte temperature, salt-anion size, solvent melting, boiling temperatures, solvent dielectric constant, and solvent dipole moment. Different configurations of the ANN model were tested, and the configuration with the least error was chosen. The results show the capability of the semi-empirical model in predicting the viscosity with an overall mean absolute percentage error (MAPE) of 2.05% and 3.17% for binary and tertiary mixtures, respectively. The ANN model predicted the relative viscosity of electrolyte solutions with MAPE of 4.86%. The application of both models in series predicted the viscosity with MAPE of 2.3%; however, the ANN MAPE alone is higher than this value. Thus, this study highlights the promise of using predictive models to complement physical approaches and effectively perform initial screening on Li-ion electrolytes.
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Subramani, Ramesh, Yu-Hsien Tseng, Yuh-Lang Lee, Chi-Cheng Chiu, Sheng-Shu Hou, and Hsisheng Teng. "High Li+ transference gel interface between solid-oxide electrolyte and cathode for quasi-solid lithium-ion batteries." Journal of Materials Chemistry A 7, no. 19 (2019): 12244–52. http://dx.doi.org/10.1039/c9ta02515d.
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Protsenko, Vyacheslav, Lina Bobrova, and Felix Danilov. "Trivalent chromium electrodeposition using a deep eutectic solvent." Anti-Corrosion Methods and Materials 65, no. 5 (September 3, 2018): 499–505. http://dx.doi.org/10.1108/acmm-05-2018-1946.
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Purpose This paper aims to investigate the electrolytic deposition of corrosion-resistant chromium coatings from a trivalent chromium plating bath based on deep eutectic solvent, a new generation of room temperature ionic liquids. Design/methodology/approach The electrolyte contained chromium (III) chloride, choline chloride and the additive of extra water. The surface morphology was estimated by means of SEM technique. The microstructure of as-deposited and annealed coatings was studied using X-ray diffraction method. The kinetics of the chromium electrodeposition and the corrosion electrochemical behavior of the coatings were investigated by cyclic voltammetry technique. Findings Chromium coatings with an amorphous type of microstructure are electroplated from this bath. Some carbon and oxygen are included in deposits obtained. The step-wise mechanism of the electrochemical reduction of Cr(III) ions to Cr(0) is detected. The current efficiency in this system sufficiently exceeds that typical of usual aqueous electrolytes. The coatings fabricated using plating bath based on deep eutectic solvent showed enhanced corrosion resistance in an acidic medium: there is no current peak of active dissolution in polarization curve and the corrosion potential shifts to more positive values as compared with “usual” chromium. Originality/value The electrodeposition of chromium coatings from an environmentally acceptable trivalent chromium electrolyte, a deep eutectic solvent containing chloride choline and extra water additive has been investigated for the first time.
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Self, Julian, Helen K. Bergstrom, Kara D. Fong, Bryan D. McCloskey, and Kristin A. Persson. "Theoretical Prediction of Freezing Point Depression of Lithium-Ion Battery Electrolytes." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 194. http://dx.doi.org/10.1149/ma2022-012194mtgabs.
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Understanding and predicting the freezing point depression of liquid electrolytes is of interest particularly for low-temperature battery applications. We will present a computational methodology to calculate activity coefficients and the freezing point depression of liquid electrolytes relevant to Li-ion batteries. Theoretical expressions for Born solvation, Debye-Huckel ion atmosphere effects and solvent entropy are used with results from classical molecular dynamics simulations and electronic structure methods to calculate the activity coefficients of liquid electrolytes. Using the calculated activity coefficients as well as neat solvent properties, liquidus lines of the studied electrolytes are obtained up to 1 molal. The liquid electrolytes studied include LiPF6 in dimethyl carbonate and LiPF6 in propylene carbonate. It is found that the more significant freezing point depression of the propylene carbonate-based electrolyte versus dimethyl carbonate-based electrolyte originates in large part from the much higher dielectric constant of propylene carbonate versus dimethyl carbonate.
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Ren, Yong Huan, Chun Wei Yang, Bo Rong Wu, Cun Zhong Zhang, Shi Chen, and Feng Wu. "Novel Low-Temperature Electrolyte for Li-Ion Battery." Advanced Materials Research 287-290 (July 2011): 1283–89. http://dx.doi.org/10.4028/www.scientific.net/amr.287-290.1283.
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In order to overcome the limitation of Li-ion batteries at low temperature, series of electrolytes are prepared. Specially，FEC is chose to work as electrolyte solvent to enhance its poor performance. Electrolytes are composed of EC, PC, EMC and FEC, while VC is added as additive. Electrolytes with different ratio are examined, then the electrolyte with the best conductivity is studied in detail. Its characters are evaluated by CV, EIS and charge/discharge tests et al. The discharge curves of LiCo1/3Ni1/3Mn1/3O2/Li show that battery with this FEC-based electrolyte at 233K could yield 51% of room temperature capacity. Most obviously, MCMB/Li half cell with this electrolyte could fill 91% of its normal capacity at 233K while batteries barely charge any with traditional electrolyte（LiPF6/EC+DMC(1:1 in volume)）. This nice charge behavior won’t emerge unless the conductivity could basically meet the demand at 233K. The property of FEC-based electrolyte outweighs commercialized electrolyte as this article confirms.
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Savadogo, O., and A. Yelon. "Photocorrosion of hydrogenated amorphous silicon: effect of the solvent." Canadian Journal of Physics 67, no. 10 (October 1, 1989): 980–83. http://dx.doi.org/10.1139/p89-171.
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The photocorrosion of amorphous hydrogenated silicon (a-Si:H) in different solvents was studied. Impedance measurements were performed under potentiostatic conditions. At each potential, the impedance Z(ω, V) was determined in the frequency range 5 Hz–100 kHz. The Z(ω, V) diagrams were analyzed and the corrosion sensitivity of the material in different electrolytes was determined. A correlation between electroactivity domain and ac impedance curves is proposed. A relationship is used to describe the anodic corrosion process in different solvents. The electrolyte that shows no oxide growth at the semiconductor – electrolyte interface was deduced.
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Joraleechanchai, Nattanon, and Montree Sawangphruk. "(Digital Presentation) Free Solvent Molecules in the Electrolyte Leading to Severe Safety Concern of Ni-Rich Li-Ion Batteries." ECS Meeting Abstracts MA2022-01, no. 2 (July 7, 2022): 239. http://dx.doi.org/10.1149/ma2022-012239mtgabs.
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The safety of Li-ion batteries is one of the most important factors, if not the most, determining their practical applications. We have found that free carbonate-based solvent molecules in the hybrid electrolyte system can cause severe safety concerns. The 18650 battery cells using the 50% varied-alkyl chain piperidinium-based TFSI result in an immediate and aggressive explosion after applying the impact test (UN38.3) compared with the cell using the conventional electrolyte, having a mild explosion after applying the impact force with 16 s-delayed time. Furthermore, the greater concentration of gases especially C2H4 and CO in the hybrid electrolyte system compared with the conventional electrolyte system was observed by online in situ DEMS, which is evidence for the aggressive explosion of the cell using the hybrid electrolyte. In additionally, the classical MD investigation is suggested that hybrid electrolytes have a high AGG concentration of Li+ and TFSI−, producing a high concentration of the isolated EC or free solvent, which could generate more gases in the fully charged battery cell. Mixing ionic liquids with a carbonate-based solvent as the co-solvent at a fixed salt concentration of 1 M LiPF6 can lead to free carbonate-based molecules causing poor charge storage performance and safety concerns. Keywords: Ni-rich Li-ion bateriesIonic liquids; Safety; Battery explosion; Mismatch electronic properties; 1865 cylindrical cells
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Chen, Chenglong, Fubin Pei, Shasha Feng, Mingzhu Xia, Fengyun Wang, Qingli Hao, and Wu Lei. "Molecular Dynamics Simulation of Solvation Nanostructure in Carbonate-Based Electrolyte of Lithium–Sulfur Battery." Nano 16, no. 08 (July 2021): 2150092. http://dx.doi.org/10.1142/s1793292021500922.
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Lithium–sulfur (Li–S) batteries are widely regarded as the most promising batteries for the future due to their higher specific capacity and lower prices. Various strategies are utilized to alleviate the shortcomings of Li–S batteries failing to reach theoretical capacity. However, basic research at the molecular level continues to be lacking. Therefore, we use molecular dynamics to study the details of the solvated structure of Li–S batteries electrolyte and the nature of the transport process, revealing the relationship between the solvated structure of the electrolyte of LiPF6 and the organic solvent ethylene carbonate/dimethyl carbonate (EC/DMC). The electrolyte of Li2S4 was first simulated in a pure solvent environment. Then the LiPF6 salt was added to the model to simulate a typical electrolyte for a working Li–S battery. Regarding the rationality of the solvent system, various reference systems such as density, dielectric constant, viscosity and diffusion coefficient of the solvent were used for verification. And the detailed composition of the first solvation shell of the polysulfate ion and the coordination number of the ions are discussed. These results provide new insights into the use of EC/DMC electrolytes in Li–S batteries, while at the same time providing a basis for efficient future predictions of electrolyte structure and transport in complex electrode confinements.
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Gill, Dip Singh, and Dilbag Rana. "Preparation of Some Novel Copper(I) Complexes and their Molar Conductances in Organic Solvents." Zeitschrift für Naturforschung A 64, no. 3-4 (April 1, 2009): 269–72. http://dx.doi.org/10.1515/zna-2009-3-416.
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Abstract Attempts have been made to prepare some novel copper(I) nitrate, sulfate, and perchlorate complexes. Molar conductances of these complexes have been measured in organic solvents like acetonitrile (AN), acetone (AC), methanol (MeOH), N,N-dimethylformamide (DMF), N,Ndimethylacetamide (DMA), and dimethylsulfoxide (DMSO) at 298 K. The molar conductance data have been analyzed to obtain limiting molar conductances (λ0) and ion association constants (KA) of the electrolytes. The results showed that all these complexes are strong electrolytes in all organic solvents. The limiting ionic molar conductances (λo± ) for various ions have been calculated using Bu4NBPh4 as reference electrolyte. The actual radii for copper(I) complex ions are very large and different in different solvents and indicate some solvation effects in each solvent system
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Mohammad, Irshad, Lucie Blondeau, Jocelyne Leroy, Hicham Khodja, and Magali Gauthier. "Influence of Electrolyte on the Electrode/Electrolyte Interface Formation on InSb Electrode in Mg-Ion Batteries." Molecules 26, no. 18 (September 21, 2021): 5721. http://dx.doi.org/10.3390/molecules26185721.
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Achieving the full potential of magnesium-ion batteries (MIBs) is still a challenge due to the lack of adequate electrodes or electrolytes. Grignard-based electrolytes show excellent Mg plating/stripping, but their incompatibility with oxide cathodes restricts their use. Conventional electrolytes like bis(trifluoromethanesulfonyl)imide ((Mg(TFSI)2) solutions are incompatible with Mg metal, which hinders their application in high-energy Mg batteries. In this regard, alloys can be game changers. The insertion/extraction of Mg2+ in alloys is possible in conventional electrolytes, suggesting the absence of a passivation layer or the formation of a conductive surface layer. Yet, the role and influence of this layer on the alloys performance have been studied only scarcely. To evaluate the reactivity of alloys, we studied InSb as a model material. Ex situ X-ray photoelectron spectroscopy (XPS) and electrochemical impedance spectroscopy were used to investigate the surface behavior of InSb in both Grignard and conventional Mg(TFSI)2/DME electrolytes. For the Grignard electrolyte, we discovered an intrinsic instability of both solvent and salt against InSb. XPS showed the formation of a thick surface layer consisting of hydrocarbon species and degradation products from the solvent (THF) and salt (C2H5MgCl−(C2H5)2AlCl). On the contrary, this study highlighted the stability of InSb in Mg(TFSI)2 electrolyte.
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Le, Phung My Loan, Khanh Hoang Phuong Ngo, Thanh Duy Vo, and Man Van Tran. "Physical chemical and electrochemical study of the electrolyte based on bis(trifluoromethanesulfonyl)imidur 1-(2,2,2-trifluoroethyl)-3-methylimidazolium." Science and Technology Development Journal 19, no. 4 (December 31, 2016): 167–76. http://dx.doi.org/10.32508/stdj.v19i4.626.
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In seeking the electrolyte replacing the conventional electrolyte based on organic solvent, bis(trifluoromethanesulfonyl)imidur-1-(2,2,2-trifluoroethyl)-3-methylimidazolium ionic liquid was studied for using as electrolyte in lithium batteries. Bis(trifluoromethanesulfonyl)-imidur-1-(2,2,2-trifluoroethyl)-3-methylimidazo-lium was synthesized via tosylate 2,2,2-trifluoroethyl by using microwave or ultrasound irradiation. The physico-chemical and electrochemical properties including melting temperature (Tm), degradation temperature (Td), density, viscosity, ionic conductivity and electrochemical window of synthesized ILs were characterized and compared to those of commercial electrolyte and electrolytes based on imidazolium and ammonium cations. Bis(trifluoromethanesulfonyl)imidur-1-(2,2,2-trifluoroethyl)-3-methylimidazolium exhibited good thermal stability, excellent electrochemical stability in comparing to the commercial electrolyte and ammonium cation based ILs. However, the high viscosity of ILs is still an obstacle for lithium-ion batteries application. Thus, the addition with small amount of organic solvent is able to improve the viscosity, the cycling behavior without destroying the non-volatility and thermal stability of the ionic liquid.
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Man, Tran Van. "EFFECT OF SOLVENT COMPOSITION ON THE ELECTROCHEMICAL PERFORMANCE OF HIGH-VOLTAGE CATHODE LiNi0.5Mn1.5O4." Vietnam Journal of Science and Technology 56, no. 2A (June 21, 2018): 69–74. http://dx.doi.org/10.15625/2525-2518/56/2a/12631.
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The spinel LiNi0.5Mn1.5O4 (LNMO) is considered as an accurate cathode material for high-voltage Li-ions batteries above 4.5 V due to its high energy density, safety and eco-friendly. The electrochemical performance of spinel LNMO depends on the combability between electrode material and electrolyte. In this work, we reported the essential role of solvent compositions–carbonate solvents such as ethylene carbonate (EC), dimethyl carbonate (DMC), ethylene methyl carbonate (EMC)–in 1 M LiPF6 electrolytes on the long-term cycling test. The volumetric ratios in which the solvent compositions were varied were as follows: EC-EMC (7:3), EC-EMC (1:1), EC-DMC (1:1), EC-DMC (1:2). Result of cycling test in the solvent EC-EMC (7:3) leads to a discharge capacity of 140 mAh/g and a retention of 85 % initial capacity after 50 cycles.
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Wanninayake, W. M. N. M. B., K. Premaratne, and R. M. G. Rajapakse. "High Efficient Dye-Sensitized Solar Cells Based on Synthesized SnO2 Nanoparticles." Journal of Nanomaterials 2016 (2016): 1–8. http://dx.doi.org/10.1155/2016/5203068.
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In this study, SnO2 semiconductor nanoparticles were synthesized for DSC applications via acid route using tin(ii) chloride as a starting material and hydrothermal method through the use of tin(iv) chloride. Powder X-ray diffraction studies confirmed the formation of the rutile phase of SnO2 with nanoranged particle sizes. A quasi-solid-state electrolyte was employed instead of a conventional liquid electrolyte in order to overcome the practical limitations such as electrolyte leakage, solvent evaporation, and sealing imperfections associated with liquid electrolytes. The gel electrolytes were prepared incorporating lithium iodide (LiI) and tetrapropylammonium iodide (Pr4N+I−) salts, separately, into the mixture which contains polyacrylonitrile as a polymer, propylene carbonate and ethylene carbonate as plasticizers, iodide/triiodide as the redox couple, acetonitrile as the solvent, and 4-tertiary butylpyridine as an electrolyte additive. In order to overcome the recombination problem associated with the SnO2 due to its higher electron mobility, ultrathin layer of CaCO3 coating was used to cover the surface recombination sites of SnO2 nanoparticles. Maximum energy conversion efficiency of 5.04% is obtained for the device containing gel electrolyte incorporating LiI as the salt. For the same gel electrolyte, the ionic conductivity and the diffusion coefficient of the triiodide ions are 4.70 × 10−3 S cm−1 and 4.31 × 10−7 cm2 s−1, respectively.
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PROTSENKO, Vyacheslav, Larysa PAVLENKO, Olexandr SUKHATSKYI, Tetyana BUTYRINA, and Felix DANILOV. "ELECTRODEPOSITION OF NANOCRYSTALLINE NICKEL-IRON ALLOY FROM AN ELECTROLYTE BASED ON A NEW TYPE OF IONIC LIQUIDS – DEEP EUTECTIC SOLVENT." Proceedings of the Shevchenko Scientific Society. Series Сhemical Sciences 2022, no. 70 (September 30, 2022): 119–27. http://dx.doi.org/10.37827/ntsh.chem.2022.70.119.
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The paper reports the main features of electrochemical deposition of nickel-iron alloy from electrolyte based on the eutectic mixture of choline chloride and ethylene glycol, which is a typical representative of a new type of ionic liquids, deep eutectic solvents (DES). It is found that the iron content in the deposited alloy increases with both increasing the applied cathode current density and increasing the concentration of iron ions in the electrolyte and the introduction of water additives. Thus, variation in the current density and the concentration of water additive in electrolytes based on DES is the factor of influence on the kinetics of partial electrode reactions, and hence on the composition and properties of the coating. It is shown that it is possible to deposit uniform coatings with iron content up to 10–13% from the investigated electrolyte containing water additive (up to 10 wt.%) at the deposition current density not exceeding 1–1.2 A/dm2. The current efficiency of the alloy deposition is close to the theoretical value (97–99%), i.e. the electrodeposition is practically not complicated by electrochemical processes involving components of a deep eutectic solvent. The surface of pure nickel deposited from an electrolyte based on DES without additional water is quite uniform with a small number of defects, pitting and small pores, while coatings deposited from the electrolyte containing water additives are characterized by granular surface morphology with many asymmetric spheroidal crystallites. The electrodeposition of a nickel-iron alloy yields the surface built of irregular spheroids that overlap and form a scaly-like type of surface morphology. Nickel-iron electrolytic coatings containing up to ~7% Fe, formed from the ethaline-based electrolyte, are nanocrystalline solutions of iron in nickel with a face-centered cubic nickel lattice and an average nanocrystallite size of about 6–15 nm. Nickel-iron alloy coatings electrochemically deposited under the conditions established in this work may be considered as promising electrode materials for the creation of new cheap and highly efficient electrocatalysts for water electrolysis in hydrogen energy.
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Ivol, Flavien, Marina Porcher, Arunabh Ghosh, Johan Jacquemin, and Fouad Ghamouss. "Phenylacetonitrile (C6H5CH2CN) Ionic Liquid Blends as Alternative Electrolytes for Safe and High-Performance Supercapacitors." Molecules 25, no. 11 (June 10, 2020): 2697. http://dx.doi.org/10.3390/molecules25112697.
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The increasing need in the development of storage devices is calling for the formulation of alternative electrolytes, electrochemically stable and safe over a wide range of conditions. To achieve this goal, electrolyte chemistry must be explored to propose alternative solvents and salts to the current acetonitrile (ACN) and tetraethylammonium tetrafluoroborate (Et4NBF4) benchmarks, respectively. Herein, phenylacetonitrile (Ph-ACN) has been proposed as a novel alternative solvent to ACN in supercapacitors. To establish the main advantages and drawbacks of such a substitution, Ph-ACN + Et4NBF4 blends were formulated and characterized prior to being compared with the benchmark electrolyte and another alternative electrolyte based on adiponitrile (ADN). While promising results were obtained, the low Et4NBF4 solubility in Ph-ACN seems to be the main limiting factor. To solve such an issue, an ionic liquid (IL), namely 1-ethyl-3-methylimidazolium bis [(trifluoromethyl)sulfonyl] imide (EmimTFSI), was proposed to replace Et4NBF4. Unsurprisingly, the Ph-ACN + EmimTFSI blend was found to be fully miscible over the whole range of composition giving thus the flexibility to optimize the electrolyte formulation over a large range of IL concentrations up to 4.0 M. The electrolyte containing 2.7 M of EmimTFSI in Ph-ACN was identified as the optimized blend thanks to its interesting transport properties. Furthermore, this blend possesses also the prerequisites of a safe electrolyte, with an operating liquid range from at least −60 °C to +130 °C, and operating window of 3.0 V and more importantly, a flash point of 125 °C. Finally, excellent electrochemical performances were observed by using this electrolyte in a symmetric supercapacitor configuration, showing another advantage of mixing an ionic liquid with Ph-ACN. We also supported key structural descriptors by density functional theory (DFT) and COnductor-like Screening Model for Real Solvents (COSMO-RS) calculations, which can be associated to physical and electrochemical properties of the resultant electrolytes.
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Genereux, Simon, and Dominic Rochefort. "Voltammetric Analysis of the Ferrocenium/Ferrocene Redox Couple in Litfsi-Acetonitrile Highly Concentrated Electrolyte." ECS Meeting Abstracts MA2022-01, no. 1 (July 7, 2022): 120. http://dx.doi.org/10.1149/ma2022-011120mtgabs.
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Research on electrolytes have a defining role for the progression of current energy storage device and electrocatalysis. For instance, the electrolyte is often a limiting factor in the life span of Li-ions batteries due to slow decomposition at electrodes. Intensive research is therefore ongoing to increase the stability of the electrolyte. One example of such research is on highly concentrated electrolyte (HCE) which are obtained when the number of ions of a salt nears or equals that of the solvent molecules, while maintaining a liquid state. These highly concentrated electrolytes (HCE) or "solvent-in-salt" solutions differ in properties from conventional ones because all solvent molecules are occupying the ion solvation sphere where they are strongly coordinated to the cation. While on the application side, the attention is directed towards their use in batteries or supercapacitors, current research on HCE aims at increasing the fundamental understanding of their properties mostly the transport properties of the Li+ or the formation of the solid electrolyte interface (SEI). Interestingly, there are no reports on the study of heterogeneous electron transfer (ET) in HCE, yet the absence of "free" solvent molecule suggests that ET in HCE might be different from conventional electrolytes because of the importance of solvent reorganization during ET. We therefore investigate the mass transport and ET of dissolved ferrocene (Fc) and with ferrocene terminated self-assemble monolayer, (Fc-SAM). Ferrocene was selected as the redox center for its "ideal" outer shell electron transfer mechanism and well-defined electrochemical properties. To establish the effect of salt concentration, the electrochemical measurements were done in a series of electrolytes composed of Lithium bis(trifluoromethanesulfonyl)imide in acetonitrile with concentrations spanning from diluted (0.3 M) to highly concentrated (4.1 M) solutions. The diffusivity of Fc (Shoup-Szabo) is found to follow the trend with viscosity (η) expected from the Stokes-Einstein relation over the entire concentration range. The ET rate constant k0 variation with η on the other hand diverges from what is expected from a purely adiabatic ET. Possible explanations for deviation involve different dielectric properties, strong coordination of the solvent and particular double-layer structure of HCE, properties that are not fully established. This lack of knowledge highlights the importance of increasing fundamental research on the topic of electrochemistry in HCE.
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Gu, Sichen, Yang Haoyi, Yanxia Yuan, Yaning Gao, Na Zhu, Feng Wu, Ying Bai, and Chuan Wu. "Solvent Effects on Kinetics and Electrochemical Performances of Rechargeable Aluminum Batteries." Energy Material Advances 2022 (May 25, 2022): 1–10. http://dx.doi.org/10.34133/2022/9790472.
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The rechargeable aluminum batteries (RAB) have shown great potential for energy storage applications due to their low-cost and superior volumetric capacity. However, the battery performances are far from satisfactory owing to the poor kinetics of electrode reactions, including the solid-state ionic diffusion and interfacial charge transfer. The charge transfer reaction, typically the cation desolvation at the interface (Helmholtz plane), is crucial for determining the interfacial charge transfer, which induces the solvent effect in batteries but has not been explored in RABs. Herein, we provide a comprehensive understanding of solvent effects on interface kinetics and electrochemical performance of RAB by analyzing the desolvation process and charge transfer energy barrier. The pivotal role of solvent effects is confirmed by the successful application of Al(OTF)3-H2O electrolyte, which displays easy desolvation, low charge transfer resistance, and thus superior Al-ion storage performance over other electrolytes in our studies. In addition, based on the strong correlation between the calculated desolvation energy and charge transfer energy barrier, the calculation of dissociation energy of ion-solvent complex is demonstrated as an efficient index for designing electrolytes. The in-depth understanding of solvent effects provides rational guidance for new electrolyte and RAB design.
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Wang, Yamin, Xiaoying Yu, Yingchun Liu, and Qi Wang. "Interfacial structure and electrochemical stability of electrolytes: methylene methanedisulfonate as an additive." Physical Chemistry Chemical Physics 21, no. 1 (2019): 217–23. http://dx.doi.org/10.1039/c8cp06548a.
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Green, Matthew, Hovnan Simonyan, Katty Kaydanik, and Joseph A. Teprovich. "Influence of Solvent System on the Electrochemical Properties of a closo-Borate Electrolyte Salt." Applied Sciences 12, no. 5 (February 22, 2022): 2273. http://dx.doi.org/10.3390/app12052273.
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In this study, the use of a closo-borate salt as an electrolyte for lithium-ion batteries (LIB) was evaluated in a series of solvent systems. The lithium closo-borate salts are a unique class of halogen-free salts that have the potential to offer some advantages over the halogenated salts currently employed in commercially available LIB due to their chemical and thermal stability. To evaluate this concept, three different solvent systems were prepared with a lithium closo-borate salt to make a liquid electrolyte (propylene carbonate, ethylene carbonate:dimethyl carbonate, and 1-Butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide). The closo-borate containing electrolytes were then compared by utilizing them with three different electroactive electrode materials. Their cycle stability and performance at various charge/discharge rates was also investigated. Based on the symmetrical cell and galvanostaic cycling studies it was determined that the carbonate based liquid electrolytes performed better than the ionic liquid electrolyte. This work demonstrates that halogen free closo-borate salts are interesting candidates and worthy of further investigation as lithium salts for LIB.
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Zhao, Yang, Jianji Wang, Xiaopeng Xuan, and Ruisen Lin. "Volumetric studies of ion solvation in propylene carbonate + N,N-dimethylformamide electrolyte solutions." Canadian Journal of Chemistry 81, no. 4 (April 1, 2003): 307–14. http://dx.doi.org/10.1139/v03-061.
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Apparent molar volumes V2,ϕ and standard partial molar volumes V°2,ϕ for tetraethylammonium bromide (Et4NBr), tetrapropylammonium bromide (Pr4NBr), tetrabutylammonium bromide (Bu4NBr), and tetrahexylammonium bromide (Hex4NBr) have been determined at 298.15 K from precise density measurements in solvent mixtures of propylene carbonate (PC) with N,N-dimethylformamide (DMF). Combined with our previous data for LiClO4 and LiBr in the same solvents, ionic molar volumes of Li+, Et4N+, Pr4N+, Bu4N+, Hex4N+, and related anions have been deduced from the extrapolation method suggested by Conway and co-workers. It is shown that the molar volumes of these cations are quite independent of the nature of the solvent and the composition of the solvent mixtures, in contrast to those of ClO4 and Br anions. This suggests that the Lewis-base-type solvents with similar molecular volumes have similar interactions with Li+. The constancy in partial molar volume for tetraalkylammonium ions provides helpful evidence for the lack of solvation of large tetraalkylammonium cations in organic solvents. These findings have been interpreted using scaled-particle theory. The results are discussed in terms of ion solvation, packing effects of solvent molecules in the solvation shell, and the electrostriction of solvents.Key words: ionic volumes, propylene carbonate, N,N-dimethylformamide, solvent mixtures, solvation, lithium batteries.
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Holoubek, John, Artem Baskin, Haodong Liu, Kangwoon Kim, Yijie Yin, Zhaohui Wu, John Lawson, Tod A. Pascal, Ping Liu, and Zheng Chen. "Impact of Electrolyte Chemistry and Solvation on Interphasial Ion Dynamics for Low-Temperature Li Metal Batteries." ECS Meeting Abstracts MA2022-02, no. 5 (October 9, 2022): 576. http://dx.doi.org/10.1149/ma2022-025576mtgabs.
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The influence of electrolyte chemistry on the ion-desolvation process of charge-transfer in Li-based batteries is a crucial, yet murky aspect of their design and operation. This desolvation process has been shown to be a dominant factor for the low-temperature operation of batteries, where high energy density is necessary, but difficult to achieve. We have applied Li metal batteries in an attempt to provide such metrics, which show extremely disparate performance depending on the electrolyte applied in each cell. Specifically, we have found that the induction of ion-pairing and the inclusion of weakly-bound solvents results in a substantial improvement in both the reversibility and shorting behavior when plating Li at low-temperature, despite significant loss in the bulk ionic conductivity of the solution. To provide a deeper understanding of these experimental observations, we also apply free-energy sampling techniques at 298 and 213 K to simulations involving diethyl ether (DEE) and 1,3-dioxoloane/1,2-dimethoxyethane (DOL/DME) electrolytes, which display bulk solvation structures dominated by ion-pairing and solvent coordination, respectively. We find that the degree of ion-pairing in the electrolyte bulk and at the interphase plays a vital role in assisting the delivery of Li+ to the inner Helmholtz layer, and that the sterics of DME are prone to Li+ over-coordination in solution. This mechanistic reliance of ion-pairing at the interphase conflicts with the preferred solvent-dominated structure of the DOL/DME system, which is further emphasized at 213 K, where simulations predict that the balance between solvent and anion coordination is shifted significantly in favor of solvent. This work endeavors to provide unambiguous evidence of the importance of the solvation structure for interphasial charge-transfer kinetics as well as a mechanistic understanding of the phenomena at the interphase. Figure 1
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Maribo-Mogensen, Bjørn, Kaj Thomsen, and Georgios M. Kontogeorgis. "An electrolyte CPA equation of state for mixed solvent electrolytes." AIChE Journal 61, no. 9 (August 7, 2015): 2933–50. http://dx.doi.org/10.1002/aic.14829.
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Tran, Kieu T., Tuyen T. T. Truong, Hoang V. Nguyen, Quan D. Nguyen, Quan Phung, Phung M. L. Le, and Man V. Tran. "Hybrid Deep Eutectic Solvent of LiTFSI-Ethylene Glycol Organic Electrolyte for Activated Carbon-Based Supercapacitors." Journal of Chemistry 2021 (October 5, 2021): 1–13. http://dx.doi.org/10.1155/2021/9940750.
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This research work demonstrates a novel hybrid electrolyte based on a deep eutectic solvent (DES) combined with organic solvents for high-performance supercapacitors. DES was formed between ethylene glycol (EG) and lithium bis((trifluoromethyl)sulfonyl) imide (LiTFSI) and diluted by ethylene carbonate (EC) or acetonitrile (AN) with different amounts (10–50% wt.). Such a combination gives superior properties for hybrid electrolytes compared to pure DESs and reduces the volatility of mixed organic solvents. Regarding the electrochemical properties, DES-AN mixtures exhibited a better performance under high applied voltage and more reversible behavior than DES-EC ones, which suffered from the increasing distance in the electrical double layer. DES 1 : 4 + 20% wt. AN exhibited favorable electrolyte properties such as high ionic conductivity (3.1 mS·cm−1 at 30oC), relatively lower viscosity (14.28 mPa s at 30oC, approximately 2 times lower thanDES pure), and quite large electrochemical stability window up to 3.4 V (at 20–30% wt. AN) compared to the baseline electrolyte (LiTFSI/TBABF4 in AN). With these interesting properties, selected hybrid electrolyte (DES 1 : 4 + 20% wt. AN) tested in the symmetric capacitor using the activated carbon offered decent capacitance (15 F·g−1 at 3.4 V with a scanning rate of 1 A·g−1 and remains around 95% after 100 cycles) and good charge-discharge durability (>80% retention after 2000 cycles), especially the EDLC with DES 1 : 4 + 20% wt. AN shows good rate capacity (13.2 F·g−1 at 2 A·g−1, remaining 6 F·g−1 at 10 A·g−1).
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Kuribayashi, Shunsuke, Tomoyuki Kurioka, Shinsuke Inagi, Ho-Jung Lu, Biing-Jiun Uang, and Toshio Fuchigami. "The selective electrochemical fluorination of S-alkyl benzothioate and its derivatives." Beilstein Journal of Organic Chemistry 14 (February 12, 2018): 389–96. http://dx.doi.org/10.3762/bjoc.14.27.
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We herein report that the regioselective anodic fluorination of S-alkyl benzothioate and its derivatives in various aprotic solvents using Et3N·nHF (n = 3–5) and Et4NF·nHF (n = 3–5) as supporting electrolyte and a fluorine source successfully provided the corresponding α-fluorinated products in moderate yields. Dichloromethane containing Et4NF·4HF was found to be the most suitable combination as electrolytic solvent and supporting salt as well as fluorine source for the anodic fluorination. The electrochemical fluorination of cyclic benzothioates such as benzothiophenone was also achieved.
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Lu, Ping, Peizhuo Sun, Qiang Ma, Huaneng Su, Puiki Leung, Weiwei Yang, and Qian Xu. "Rationally Designed Ternary Deep Eutectic Solvent Enabling Higher Performance for Non-Aqueous Redox Flow Batteries." Processes 10, no. 4 (March 26, 2022): 649. http://dx.doi.org/10.3390/pr10040649.
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Redox flow batteries hold promise as large-scale energy storage systems for off-grid electrification. The electrolyte is one of the key components of redox batteries. Inspired by the mechanism involved in solvents for extraction, a ternary deep eutectic solvent (DES) is demonstrated, in which glycerol is introduced into the original binary ethaline DES. Redox pairs (active substance) dissolved in the solvent have low charge transfer resistance. The results show that the viscosity of the solvent with the ratio of choline chloride to ethylene glycol to glycerol of 1:2:0.5 decreases from 51.2 mPa·s to 40.3 mPa·s after adding the redox pair, implying that the mass transfer resistance of redox pairs in this solvent is reduced. Subsequent cyclic voltammetry and impedance tests show that the electrochemical performance with the ternary DES as the electrolyte in redox flow batteries is improved. When the ratio of 1:2:0.5 ternary DES is used as the electrolyte, the power density of the battery (9.01 mW·cm−2) is 38.2% higher than that of the binary one (6.52 mW·cm−2). Fourier transform infrared spectroscopy further indicates that the introduction of glycerol breaks the hydrogen bond network of the solvent environment where the redox pair is located, unraveling the hydrogen bond supramolecular complex. Rational solvent design is an effective strategy to enhance the electrochemical performance of redox batteries.
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Clough, Matthew T. "Organic electrolyte solutions as versatile media for the dissolution and regeneration of cellulose." Green Chemistry 19, no. 20 (2017): 4754–68. http://dx.doi.org/10.1039/c7gc01776f.
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Organic electrolyte solutions – mixtures of a (room-temperature) ionic liquid with a neutral, organic, polar co-solvent – are attracting increasing attention as solvents for the regeneration and derivatisation of cellulose.
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Saitoh, Ken-ichi, Yoshihiro Takai, Tomohiro Sato, Masanori Takuma, and Yoshimasa Takahashi. "Optimization of LIB Electrolyte and Exploration of Novel Compounds via the Molecular Dynamics Method." Batteries 8, no. 3 (March 21, 2022): 27. http://dx.doi.org/10.3390/batteries8030027.
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Due to great interest in the development of electric vehicles and other applications, improving the performances of lithium-ion batteries (LIBs) is crucial. Specifically, components of electrolytes for LIBs should be adequately chosen from hundreds of thousands of candidate compounds. In this study, we aimed to evaluate some physical properties expected for combinations of molecules for electrolytes by microscopic simulations. That is, the viscosity, ionic conductivity, degree of dissociation, diffusion coefficient, and conformation of each molecule were analyzed via molecular dynamics (MD) simulations. We aimed to understand how molecular-sized structures and properties collaboratively affect the behavior of electrolytes. The practical models of molecules we used were ethylene carbonate (EC), fluoroethylene carbonate (FEC), propylene carbonate (PC), butylene carbonate (BC), γ-butyrolactone (GBL), γ-valerolactone (GVL), dimethyl carbonate (DMC), ethyl-methyl carbonate (EMC), diethyl carbonate (DEC), and lithium hexafluorophosphate (LiPF6). Many molecular systems of electrolytes were simulated, in which one molar LiPF6 was mixed into a single or combined solvent. It was found that small solvent molecules diffused with relative ease, and they contributed to the higher ionic conductivity of electrolytes. It was clarified that the diffusion coefficient of lithium (Li) ions is greatly affected by the surrounding solvent molecules. We can conclude that high-permittivity solvents can be selectively coordinated around Li ions, and Li salts are sufficiently dissociated, even when there is only a small content of high-permittivity solvent. Thus, we can confirm solely by MD simulation that one of the better candidates for solvent molecules, formamide (F), will exhibit higher performance than the current solvents.
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Dobrovolsky, Yuri A., Margarita G. Ilyina, Elizaveta Y. Evshchik, Edward M. Khamitov, Alexander V. Chernyak, Anna V. Shikhovtseva, Tatiana I. Melnikova, Olga V. Bushkova, and Sophia S. Borisevich. "QC and MD Modelling for Predicting the Electrochemical Stability Window of Electrolytes: New Estimating Algorithm." Batteries 8, no. 12 (December 18, 2022): 292. http://dx.doi.org/10.3390/batteries8120292.
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The electrolyte is an important component of lithium-ion batteries, especially when it comes to cycling high-voltage cathode materials. In this paper, we propose an algorithm for estimating both the oxidising and reducing potential of electrolytes using molecular dynamics and quantum chemistry techniques. This algorithm can help to determine the composition and structure of the solvate complexes formed when a salt is dissolved in a mixture of solvents. To develop and confirm the efficiency of the algorithm, LiBF4 solutions in binary mixtures of ethylene carbonate (EC)/dimethyl carbonate (DMC) and sulfolane (SL)/dimethyl carbonate (DMC) were studied. The structure and composition of the complexes formed in these systems were determined according to molecular dynamics. Quantum chemical estimation of the thermodynamic and oxidative stability of solvate complexes made it possible to establish which complexes make the most significant contribution to the electrochemical stability of the electrolyte system. This method can also be used to determine the additive value of the oxidation and reduction potentials of the electrolyte, along with the contribution of each complex to the overall stability of the electrolyte. Theoretical calculations were confirmed experimentally in the course of studying electrolytes by step-by-step polarisation using inert electrodes. Thus, the main aim of the study is to demonstrate the possibility of using the developed algorithm to select the optimal composition and solvent ratio to achieve predicted redox stability.