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1
Aharon, Hannah, Omer Shavit, Matan Galanty i Adi Salomon. "Second Harmonic Generation for Moisture Monitoring in Dimethoxyethane at a Gold-Solvent Interface Using Plasmonic Structures". Nanomaterials 9, nr 12 (16.12.2019): 1788. http://dx.doi.org/10.3390/nano9121788.
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Second harmonic generation (SHG) is forbidden from most bulk metals because metals are characterized by centrosymmetric symmetry. Adsorption or desorption of molecules at the metal interface can break the symmetry and lead to SHG responses. Yet, the response is relatively low, and minute changes occurring at the interface, especially at solid/liquid interfaces, like in battery electrodes are difficult to assess. Herein, we use a plasmonic structure milled in a gold electrode to increase the overall SHG signal from the interface and gain information about small changes occurring at the interface. Using a specific homebuilt cell, we monitor changes at the liquid/electrode interface. Specifically, traces of water in dimethoxyethane (DME) have been detected following changes in the SHG responses from the plasmonic structures. We propose that by plasmonic structures this technique can be used for assessing minute changes occurring at solid/liquid interfaces such as battery electrodes.
2
Suzuki, Tatsumi, Chengchao Zhong, Keiji Shimoda, Ken'ichi Okazaki i Yuki Orikasa. "(Digital Presentation) Electrochemical Impedance Analysis of Three-Electrode Cell with Solid Electrolyte/Liquid Electrolyte Interface". ECS Meeting Abstracts MA2023-02, nr 8 (22.12.2023): 3369. http://dx.doi.org/10.1149/ma2023-0283369mtgabs.
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Mechanical contact loss at the solid electrolyte/electrode interface in all-solid-state batteries, a type of next-generation battery, has been reported as a major issue for ion transport in all-solid-state batteries[1]. To improve this contact problem, it has been proposed to add a small amount of liquid electrolyte to the solid electrolyte/electrode interface[2]. However, the reported ion transport analysis at the solid electrolyte/liquid electrolyte interface is limited in semi-solid-state system using symmetrical cells with lithium metal as the working electrode[3]. In this study, charge transfer reactions at the solid electrolyte/liquid electrolyte interface were analyzed by impedance (EIS) measurements in a three-electrode cell with a solid/liquid electrolyte interface using a composite electrode containing a cathode active material as the working electrode. A composite electrode prepared by mixing LiCoO2:acetylene black:polyvinylidene fluoride in a weight ratio of 8:1:1, coating Al foil, drying and pressing was used as the working electrode, while lithium metal was used as the counter and reference electrodes. A NASICON-type solid electrolyte Li1+x+y Al x (Ti2−y Ge y )P3−z Si z O12 was constructed between the working electrode and the counter electrode, and a three-electrode cell prepared by filling the liquid electrolyte 1 M LiClO4/PC between the solid electrolyte and both electrodes. The reference electrode was placed between the solid electrolyte and the counter electrode, as the solid electrolyte/liquid electrolyte interface charge transfer is not observed in EIS measurements when the reference electrode is placed between the working electrode and the solid electrolyte. After two cycles of constant current charge/discharge measurements (current rate: 0.1 C rate, cut-off potential: 3.2 V - 4.2 V vs. Li/Li+), the solid electrolyte/liquid electrolyte interface charge transfer was analyzed by performing EIS measurements. To identify the semicircle associated with the solid electrolyte/liquid electrolyte interface resistance, measurements were also performed in a cell without a solid electrolyte and the resistance components corresponding to each semicircle were assigned. The temperature dependence of the observed semicircles was analyzed. A comparison of the activation energies calculated from the slopes of the Arrhenius plots confirmed a particularly large activation barrier at the solid electrolyte/liquid electrolyte interface and the working electrode/liquid electrolyte interface charge transfer. [1] R. Koerver, I. Aygun, T. Leichtweiss, C. Dietrich, W. Zhang, J.O. Binder, P. Hartmann, W.G. Zeier and J. Janek, Chem. Mater., 29, 5574-5582 (2017). [2] C. Wanga, Q. Suna, Y. Liua, Y. Zhaoa, X. Lia, X. Lina, M.N. Banisa, M. Lia, W. Lia, K.R. Adaira, D. Wanga, J. Lianga, R. Lia, L. Zhangb, R. Yangb, S. Lub and X. Suna, Nano Energy, 48, 35-43 (2018). [3] T. Abe, H. Fukuda, Y. Iriyama, Z. Ogumi, J. Electrochem. Soc., 151, A1120-A1123 (2004).
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Lenser, Christian, Alexander Schwiers, Denise Ramler i Norbert H. Menzler. "Investigation of the Electrode-Electrolyte Interfaces in Solid Oxide Cells". ECS Meeting Abstracts MA2023-01, nr 54 (28.08.2023): 262. http://dx.doi.org/10.1149/ma2023-0154262mtgabs.
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The interfaces between electrodes and electrolyte are critical locations in a solid oxide cell (SOC). These interfaces originate from the chemical interaction of two different materials during processing, and are therefore very sensitive to the chemical nature of the materials, as well as the thermal history of the cell. On the air side, perovskite air electrodes tend to form insulating zirconates when sintered on stabilized zirconia, the most common electrolyte material. On the fuel side, using an ionic conductor with a different chemical composition as zirconia can lead to pronounced interdiffusion and the formation of new phases. Interlayers of doped ceria are frequently used in order to suppress these undesired chemical reactions between electrodes and stabilized zirconia electrolytes. Prior investigations have focused extensively on the chemical composition of the interface and its consequences for cell performance. The focus of this contribution is the microstructure of the interface, as well as the microstructural development during processing. On the fuel side, the interdiffusion of ceria and zirconia is known to lead to an intermixed phase with decreased conductivity. However, the reduced cell performance of anode-supported cells with Ni-GDC electrodes cannot be explained by an increase in the electrolyte resistance alone. We show that the formation of porosity due to a difference in the diffusion coefficients of ceria and zirconia leads to an increase in the fuel electrode polarization, and investigate possible countermeasures. It is shown that specifically the presence of NiO leads to the formation of porosity at the interface. On the air side, we investigate the role of a dense interdiffusion layer between ceria and zirconia on the air electrode polarization. We confirm that only a dense interdiffusion layer is necessary by using Pr-doped ceria as a barrier layer, which delaminates after sintering and leaves behind a submicron barrier layer. Finally, we investigate the hypothesis that the densification of the barrier layer during air electrode sintering is essential for electrode adhesion and performance.
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Mukhan, Orynbassar, Ji-Su Yun i Sung-soo Kim. "Investigation of Interfacial Behavior of Ni-Rich NCM Cathode Particles in Sulfide-Based Solid-State Electrolyte". ECS Meeting Abstracts MA2023-02, nr 60 (22.12.2023): 2892. http://dx.doi.org/10.1149/ma2023-02602892mtgabs.
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All-solid-state batteries (ASSBs) are currently investigated as a future battery technology with conventional layered cathode materials because they can offer benefits in the gravimetric and volumetric energy densities compared to flammable liquid electrolyte lithium-ion batteries with graphite intercalation anode. The solid electrolyte is believed to suppress dendritic growth and low Coulombic efficiency on the lithium metal anode side, which are the key issues for the use of a lithium metal electrode in conventional batteries with liquid electrolyte. Moreover, layered transition metal oxides such as LiNixCoyMnzO2 (NCM, 0 < x, y, z < 1) are one of the most promising positive electrode active material candidates being developed to increase the energy density. In particular, recent studies have shown a tendency to decrease the cobalt content and increase the nickel content to increase energy density and price competitiveness, so high-nickel NCM can be the optimal material suitable for this purpose. However, the remaining interfacial challenges of the cathode / solid electrolyte interface still need to be solved. Herein, we investigated the kinetics such as charge transfer resistance at the interface between high nickel (Ni0.94) NCM particles and argyrodite (Li6PS5Cl) solid electrolytes using the microcavity electrode with the negative and positive pulsed current measurement technique and compared with liquid electrolytes using the same manner measurement technique. The cavity-electrode system is adopted to analyze the electrochemical properties of active particles and electrolytes confined in the cavity to exclude the effects of surrounding interfaces, barriers, and side reactions caused by battery components around the electrodes and the impact of loading and current collectors of the composite electrode. Therefore, understanding the electrode-electrolyte interface between cathode active particles and solid electrolytes is crucial for theoretical studies on the interfacial phenomenon in solid electrolyte batteries.
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Marbella, Lauren, Wesley Chang, Richard May, Michael Wang, Jeff Sakamoto i Daniel A. Steingart. "Combining Operando Techniques to Probe Chemo-Mechanical Evolution at Buried Solid/Solid Interfaces". ECS Meeting Abstracts MA2022-01, nr 37 (7.07.2022): 1636. http://dx.doi.org/10.1149/ma2022-01371636mtgabs.
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Chemical and mechanical changes local to the electrode/electrolyte interface critically impact performance in all-solid-state batteries. Unfortunately, the dynamics at electrochemical interfaces are exceptionally challenging to probe in all-solid-state batteries because these changes take place across multiple length scales (from the nano- to meso-scale) and are buried within the system (at the solid/solid electrode/electrolyte interface). Here, I show our efforts to couple operando acoustic transmission measurements with nuclear magnetic resonance spectroscopy and imaging to correlate changes in interfacial mechanics with the growth of Li microstructures and the solid electrolyte interphase (SEI) in a non-invasive, multimodal fashion. Specifically, we study chemo-mechanical changes at the interface between Li metal anodes and Li7La3Zr2O12 solid electrolytes as a function of stack pressure and current density.
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Il’ina, Evgeniya, Svetlana Pershina, Boris Antonov i Alexander Pankratov. "Impact of Li3BO3 Addition on Solid Electrode-Solid Electrolyte Interface in All-Solid-State Batteries". Materials 14, nr 22 (22.11.2021): 7099. http://dx.doi.org/10.3390/ma14227099.
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All-solid-state lithium-ion batteries raise the issue of high resistance at the interface between solid electrolyte and electrode materials that needs to be addressed. The article investigates the effect of a low-melting Li3BO3 additive introduced into LiCoO2- and Li4Ti5O12-based composite electrodes on the interface resistance with a Li7La3Zr2O12 solid electrolyte. According to DSC analysis, interaction in the studied mixtures with Li3BO3 begins at 768 and 725 °C for LiCoO2 and Li4Ti5O12, respectively. The resistance of half-cells with different contents of Li3BO3 additive after heating at 700 and 720 °C was studied by impedance spectroscopy in the temperature range of 25–340 °C. It was established that the introduction of 5 wt% Li3BO3 into LiCoO2 and heat treatment at 720 °C led to the greatest decrease in the interface resistance from 260 to 40 Ω cm2 at 300 °C in comparison with pure LiCoO2. An SEM study demonstrated that the addition of the low-melting component to electrode mass gave better contact with ceramics. It was shown that an increase in the annealing temperature of unmodified cells with Li4Ti5O12 led to a decrease in the interface resistance. It was found that the interface resistance between composite anodes and solid electrolyte had lower values compared to Li4Ti5O12|Li7La3Zr2O12 half-cells. It was established that the resistance of cells with the Li4Ti5O12/Li3BO3 composite anode annealed at 720 °C decreased from 97.2 (x = 0) to 7.0 kΩ cm2 (x = 5 wt% Li3BO3) at 150 °C.
7
Lenser, Christian, Alexander Schwiers, Denise Ramler i Norbert H. Menzler. "Investigation of the Electrode-Electrolyte Interfaces in Solid Oxide Cells". ECS Transactions 111, nr 6 (19.05.2023): 1699–707. http://dx.doi.org/10.1149/11106.1699ecst.
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The interface between electrodes and electrolyte in a solid oxide cell (SOC) are critical locations for cell performance. These interfaces originate from the chemical interaction of two different materials during processing. Different mechanisms can degrade cell performance on the air and fuel side, which necessitates different approaches to mitigate these effects. Here, materials interaction during processing is discussed for selected materials on the air side of an SOC. A new approach to obtain barrier layers of doped ceria with submicron thickness is introduced, and it is confirmed that only the interdiffusion layer between ceria and zirconia is necessary to prevent the formation of SrZrO3. Furthermore, the effect of the microstructure of a GDC layer on the sintering of a perovskite air electrode in this layer is investigated. It is demonstrated that the morphology of the GDC layer has an impact on the quality of the interface between air electrode and barrier layer.
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Tan, Feihu, Hua An, Ning Li, Jun Du i Zhengchun Peng. "Stabilization of Li0.33La0.55TiO3 Solid Electrolyte Interphase Layer and Enhancement of Cycling Performance of LiNi0.5Co0.3Mn0.2O2 Battery Cathode with Buffer Layer". Nanomaterials 11, nr 4 (12.04.2021): 989. http://dx.doi.org/10.3390/nano11040989.
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All-solid-state batteries (ASSBs) are attractive for energy storage, mainly because introducing solid-state electrolytes significantly improves the battery performance in terms of safety, energy density, process compatibility, etc., compared with liquid electrolytes. However, the ionic conductivity of the solid-state electrolyte and the interface between the electrolyte and the electrode are two key factors that limit the performance of ASSBs. In this work, we investigated the structure of a Li0.33La0.55TiO3 (LLTO) thin-film solid electrolyte and the influence of different interfaces between LLTO electrolytes and electrodes on battery performance. The maximum ionic conductivity of the LLTO was 7.78 × 10−5 S/cm. Introducing a buffer layer could drastically improve the battery charging and discharging performance and cycle stability. Amorphous SiO2 allowed good physical contact with the electrode and the electrolyte, reduced the interface resistance, and improved the rate characteristics of the battery. The battery with the optimized interface could achieve 30C current output, and its capacity was 27.7% of the initial state after 1000 cycles. We achieved excellent performance and high stability by applying the dense amorphous SiO2 buffer layer, which indicates a promising strategy for the development of ASSBs.
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Crumlin, Ethan J. "(Invited) Using Ambient Pressure XPS to Probe the Solid/Gas and Solid/Liquid Interface Under in Situ and Operando Conditions". ECS Meeting Abstracts MA2022-02, nr 46 (9.10.2022): 1715. http://dx.doi.org/10.1149/ma2022-02461715mtgabs.
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Interfaces play an essential role in nearly all aspects of life and are critical for electrochemistry. Prof. Robert Savinell has played a pivotal interface to me in the role of mentorship in both life and electrochemistry, and I look to honor his contributions to both through this talk. Electrochemical systems ranging from high-temperature solid oxide fuel cells (SOFC) to batteries to capacitors have a wide range of important interfaces between solids, liquids, and gases, which play a pivotal role in how energy is stored, transferred, and converted. I will share the use of ambient pressure XPS (APXPS) to directly probe the solid/gas and solid/liquid electrochemical interface. APXPS is a photon-in/electron-out process that can provide both atomic concentration and chemical-specific information at pressures greater than 20 Torr. Using synchrotron X-rays at Lawrence Berkeley Nation Laboratory, the Advanced Light Source has several beamlines dedicated to APXPS endstations that are outfitted with various in situ/operando features such as heating to temperatures > 500 °C, pressures greater than 20 Torr to support solid/liquid experiments and electrical leads to support applying electrical potentials support the ability to collect XPS data of actual electrochemical devices while it's operating in near ambient pressures. This talk will introduce APXPS and provide several interface electrochemistry examples using in situ and operando APXPS, including the probing of Sr segregation on a SOFC electrode to a Pt metal electrode undergoing a water-splitting reaction to generate oxygen, the ability to measure the electrochemical double layer (EDL) to our most recent efforts to directly probe an ion exchange membranes Donnan potential. Gaining new insight to guide the design and control of future electrochemical interfaces and how Bob, electrochemistry, and I have interfaced over the years.
10
Hu, Jia-Mian, Linyun Liang, Yanzhou Ji, Liang Hong, Kirk Gerdes i Long-Qing Chen. "Interdiffusion across solid electrolyte-electrode interface". Applied Physics Letters 104, nr 21 (26.05.2014): 213907. http://dx.doi.org/10.1063/1.4879835.
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Kucinskis, Gints, Beate Kruze, Prasad Korde, Anatolijs Sarakovskis, Arturs Viksna, Julija Hodakovska i Gunars Bajars. "Enhanced Electrochemical Properties of Na0.67MnO2 Cathode for Na-Ion Batteries Prepared with Novel Tetrabutylammonium Alginate Binder". Batteries 8, nr 1 (14.01.2022): 6. http://dx.doi.org/10.3390/batteries8010006.
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Both the binder and solid–electrolyte interface play an important role in improving the cycling stability of electrodes for Na-ion batteries. In this study, a novel tetrabutylammonium (TBA) alginate binder is used to prepare a Na0.67MnO2 electrode for sodium-ion batteries with improved electrochemical performance. The ageing of the electrodes is characterized. TBA alginate-based electrodes are compared to polyvinylidene fluoride- (PVDF) and Na alginate-based electrodes and show favorable electrochemical performance, with gravimetric capacity values of up to 164 mAh/g, which is 6% higher than measured for the electrode prepared with PVDF binder. TBA alginate-based electrodes also display good rate capability and improved cyclability. The solid–electrolyte interface of TBA alginate-based electrodes is similar to that of PVDF-based electrodes. As the only salt of alginic acid soluble in non-aqueous solvents, TBA alginate emerges as a good alternative to PVDF binder in battery applications where the water-based processing of electrode slurries is not feasible, such as the demonstrated case with Na0.67MnO2.
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Larson, Karl, Eric A. Carmona i Paul Albertus. "High Areal Capacity Cycling of Three-Electrode Sodium/NBA/Sodium Cells". ECS Meeting Abstracts MA2023-02, nr 5 (22.12.2023): 851. http://dx.doi.org/10.1149/ma2023-025851mtgabs.
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The cycling stability of Li and Na metal electrodes is influenced by the interface with the solid electrolyte. Study of the cycling behavior at areal capacities >>0.5 mAh/cm2 are uncommon, and plating and stripping behaviors remain relatively unknown for the individual electrode/electrolyte interfaces because of the difficulty of separating the individual interfaces in a two-electrode cell configuration. Because areal capacities of practical cells target >5 mAh/cm2, it is important to cycle at much higher areal capacities than typically studied. Here, we utilize a three-electrode symmetric cell of sodium metal with sodium beta alumina (NBA) electrolyte and cycled areal capacities ranging from 0.5 to 5 mAh cm-2 and achieved current densities >10 mA cm-2 at 1.0 mAh cm-2. We find that polarization increases most at the stripping electrode, and that during current density ramps the polarizations are greatly affected by the areal capacity, affecting the maximum current density that can be reached prior to either cell shorting or impedance rise that drives the voltage magnitude to well over 1 V. Additionally, we found resistance rise occurring at the Na/NBA interface during plate (reduction) as well as strip (oxidation) for the same electrode, potentially indicating voiding on plate at sufficiently high current densities and areal capacities (5 mAh cm-2, >2 mA cm-2). For two-electrode studies, the voltage evolution on the plating electrode we observe must be considered for the assumption that the plating electrode is a pseudo reference electrode. We also use our three-electrode cell configuration to study several other experimental conditions, including cycling to failure at a fixed current density and areal capacity, as well as a uni-directional current flow experiment to determine the maximum amount of plating / stripping that can be achieved in the absence of cycling. These findings will help direct future experiments and interpretation of data to quantify the limits and improve the engineering of Li and Na metal / solid electrolytes interfaces. Jolly, D. S.; Ning, Z.; Darnbrough, J. E.; Kasemchainan, J.; Hartley, G. O.; Adamson, P.; Armstrong, D. E. J.; Marrow, J.; Bruce, P. G. Sodium/Na Β″ Alumina Interface: Effect of Pressure on Voids. ACS Appl Mater Interfaces 2019, 12 (1), 678–685. https://doi.org/10.1021/ACSAMI.9B17786. Krauskopf, T.; Hartmann, H.; Zeier, W. G.; Janek, J. Toward a Fundamental Understanding of the Lithium Metal Anode in Solid-State Batteries - An Electrochemo-Mechanical Study on the Garnet-Type Solid Electrolyte Li 6.25 Al 0.25 La 3 Zr 2 O 12. ACS Appl Mater Interfaces 2019, 11 (15), 14463–14477. https://doi.org/10.1021/ACSAMI.9B02537/SUPPL_FILE/AM9B02537_SI_001.PDF.
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Zou, Junyan, i Teng Ben. "Recent Advances in Porous Polymers for Solid-State Rechargeable Lithium Batteries". Polymers 14, nr 22 (8.11.2022): 4804. http://dx.doi.org/10.3390/polym14224804.
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The application of rechargeable lithium batteries involves all aspects of our daily life, such as new energy vehicles, computers, watches and other electronic mobile devices, so it is becoming more and more important in contemporary society. However, commercial liquid rechargeable lithium batteries have safety hazards such as leakage or explosion, all-solid-state lithium rechargeable lithium batteries will become the best alternatives. But the biggest challenge we face at present is the large solid-solid interface contact resistance between the solid electrolyte and the electrode as well as the low ionic conductivity of the solid electrolyte. Due to the large relative molecular mass, polymers usually exhibit solid or gel state with good mechanical strength. The intermolecules are connected by covalent bonds, so that the chemical and physical stability, corrosion resistance, high temperature resistance and fire resistance are good. Many researchers have found that polymers play an important role in improving the performance of all-solid-state lithium rechargeable batteries. This review mainly describes the application of polymers in the fields of electrodes, electrolytes, electrolyte-electrode contact interfaces, and electrode binders in all-solid-state lithium rechargeable batteries, and how to improve battery performance. This review mainly introduces the recent applications of polymers in solid-state lithium battery electrodes, electrolytes, electrode binders, etc., and describes the performance of emerging porous polymer materials and materials based on traditional polymers in solid-state lithium batteries. The comparative analysis shows the application advantages and disadvantages of the emerging porous polymer materials in this field which provides valuable reference information for further development.
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Cucinotta, Clotilde S. "(Invited) Towards a Realistic Modelling of Solid-Liquid Interfaces". ECS Meeting Abstracts MA2023-01, nr 30 (28.08.2023): 1806. http://dx.doi.org/10.1149/ma2023-01301806mtgabs.
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In this talk I will introduce some issues connected with the simulation of electrified interfaces at the nanoscale focusing on simulating the effect of an applied potential to an electrode, using realistic models for the charged electrode electrolyte interface. I will present some recent progress in the simulation of the double layer of fundamental solid liquid interfaces of interest for corrosion and water splitting, and its response to changes of potential applied to the cell [1]; this is obtained applying a general ab initio electrode-charging approach we developed. [1] R. Khatib, A. Kumar, S. Sanvito, M. Sulpizi and C. S. Cucinotta*, The nanoscale structure of the Pt-water double layer under applied potential revealed, 2021, 391, 138875 In this talk I will introduce some issues connected with the simulation of electrified interfaces at the nanoscale focusing on simulating the effect of an applied potential to an electrochemical (EC) cell, using realistic models for the charged electrode electrolyte interface. I will present some recent progress in the simulation of the double layer of the fundamental solid liquid interfaces of interest for corrosion and water splitting and its response to changes of potential applied to the cell [1]; this is obtained applying a general ab initio electrode-charging approach we developed. [1] R. Khatib, A. Kumar, S. Sanvito, M. Sulpizi and C. S. Cucinotta*, The nanoscale structure of the Pt-water double layer under applied potential revealed, 2021, 391, 138875
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Laguna-Bercero, Miguel A. "Degradation Issues in Solid Oxide Electrolysers". ECS Meeting Abstracts MA2023-02, nr 46 (22.12.2023): 2234. http://dx.doi.org/10.1149/ma2023-02462234mtgabs.
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One of the crucial aspects to achieving long lifetime and high-efficient SOCs (Solid oxide cells) is to enhance durability of the current devices. Degradation issues are typically associated with problems in both electrodes. For example, nickel-yttria stabilized zirconia (Ni-YSZ) hydrogen electrodes present under extreme conditions of high steam partial pressures, a low durability due to Ni oxidation resulting in lowered electronic conductivity and catalytic activity of the electrode. Ni agglomeration, depleting and micro crack in Ni-containing hydrogen electrode can also occur leading to a lower activity of the Ni-based electrodes as an SOEC fuel electrode. Furthermore, carbon deposition and sulfur poisoning on the Ni surface are also lead to cell performance degradation and poor durability. In addition, the performance of the oxygen electrode is also particularly more important in electrolysis mode than in fuel cell mode, as it is well established that electrochemically induced oxygen pressure increase at the electrolyte-oxygen electrode interface and subsequent membrane failure have been theoretically predicted and experimentally observed in SOEC mode. For example, several examples in the literature reported the presence on voids at the YSZ electrolyte, leading to delamination of the oxygen electrode. In this sense, lanthanide nickelates (Ln = La, Nd, Pr) have received considerable interest as materials for IT-SOFC electrodes and oxygen separation membranes, and they seem to be very attractive for electrolysis applications. The hyperstoichiometry of some oxygen electrode materials such as these Ruddlesden-Popper phases is believed to be favourable for effective oxygen evolution, as performance of these electrodes is enhanced in SOEC mode. Different strategies to develop optimized electrode structures as well as controlled operating conditions will be discussed in order to improve the durability of SOCs.
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Crumlin, Ethan J. "(Invited) Probing Electrolysis Interfacial Chemistry: From Well-Defined to Complex Interfaces Under in Situ and Operando Conditions Using Ambient Pressure XPS". ECS Meeting Abstracts MA2024-01, nr 35 (9.08.2024): 1978. http://dx.doi.org/10.1149/ma2024-01351978mtgabs.
Pełny tekst źródłaStreszczenie:
Interfaces play an essential role in nearly all aspects of life and are critical for electrochemistry. Electrochemical systems ranging from high-temperature solid oxide fuel cells (SOFC) to batteries to capacitors have a wide range of essential interfaces between solids, liquids, and gases, which play a pivotal role in storing, transferring, and converting energy. This talk will focus on using ambient pressure XPS (APXPS) to probe the solid/gas and solid/liquid electrochemical interface directly. APXPS is a photon-in/electron-out process that can provide both atomic concentration and chemical-specific information at pressures greater than 20 Torr. Using synchrotron X-rays at Lawrence Berkeley Nation Laboratory, the Advanced Light Source has several beamlines dedicated to APXPS endstations that are outfitted with various in situ/operando features such as heating to temperatures > 500 °C, pressures greater than 20 Torr to support solid/liquid experiments and electrical leads to support applying electrical potentials support the ability to collect XPS data of actual electrochemical devices while it's operating in near ambient pressures. This talk will introduce APXPS and provide several interface electrochemistry examples using operando APXPS, including the probing of a well-defined metal electrode to complex composite polymer/nanoparticle electrodes undergoing water-splitting or carbon dioxide reduction reactions. These studies provide new insight to guide the design and control of future electrochemical interfaces.
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Ouyang, Zhufeng, Anna Sciazko, Yosuke Komatsu, Nishimura Katsuhiko i Naoki Shikazono. "Effects of Transition Metal Elements on Ni Migration in Solid Oxide Cell Fuel Electrodes". ECS Transactions 111, nr 6 (19.05.2023): 171–79. http://dx.doi.org/10.1149/11106.0171ecst.
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In the present study, Ni-M (M = Fe, Cu) bimetallic fuel electrodes are applied to investigate the effects of transition metal elements on nickel (Ni) migration and Ni coarsening under SOFC and SOEC operations. Ni-Fe, Ni-Cu and pure Ni patterned fuel electrodes are sputtered on YSZ pellets. The electrochemical performance of these Ni-M bimetallic fuel electrodes are lower than pure Ni fuel electrode, while the degradation rate of Ni-Fe fuel electrodes is smaller than the others. The spreading of Ni film on YSZ surface is observed for all samples under anodic polarization, and such Ni migration is suppressed by Fe doping, whereas it was enhanced by Cu doping. The adhesion between the electrode/electrolyte interface is weakened for Ni-Cu and pure Ni fuel electrodes under cathodic polarization, while good adhesion at the interface is maintained for Ni-Fe, which correlates with the smaller performance degradation rate.
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Laguna-Bercero, M. A., H. Monzón, A. Larrea i V. M. Orera. "Improved stability of reversible solid oxide cells with a nickelate-based oxygen electrode". Journal of Materials Chemistry A 4, nr 4 (2016): 1446–53. http://dx.doi.org/10.1039/c5ta08531d.
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Mixed praseodymium, cerium and gadolinium oxides (PCGO) at the electrolyte–oxygen electrode interface enhance the stability and performance of nickelate based oxygen electrodes in high temperature electrolysis and fuel cell operation modes.
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Zhang, Yingjie. "(Invited) Molecular Imaging of the Local Solvation, Nucleation and Growth Processes at Electrode-Electrolyte Interfaces". ECS Meeting Abstracts MA2023-02, nr 60 (22.12.2023): 2904. http://dx.doi.org/10.1149/ma2023-02602904mtgabs.
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Electrochemical energy storage is a complex process that requires the synergistic participation of electrodes, electrolytes, and separators in the system. However, the key energy storage functions usually depend critically on the electrode-electrolyte interfaces, which include both the electrode surface and the electrical double layers (EDLs). Here I will discuss our efforts on developing and using electrochemical 3D atomic force microscopy (EC-3D-AFM) to simultaneously image the electrode and EDLs under operando conditions, with atomic-scale resolution. We study the interface between graphite electrode and various types of electrolytes. We observe rich EDL reconfiguration effects at different electrode potentials, which we find to be directly responsible for the capacitive charge storage functions. As the electrode potential goes beyond the electrochemical stability window of the electrolyte, we observe nucleation and growth processes where the EDLs and the deposited solid clusters exhibit intertwined structures. Such initial stage of electrode processes is likely connected to the long-term cycling behaviors of batteries.
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Ji, Yanzhou, Seyed Amin Nabavizadeh, Qisheng Wu, Yue Qi i Long-Qing Chen. "A Diffuse-Interface Description of Electron Tunneling across Solid Electrolyte Interphases". ECS Meeting Abstracts MA2023-01, nr 45 (28.08.2023): 2484. http://dx.doi.org/10.1149/ma2023-01452484mtgabs.
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Solid electrolyte interphase (SEI) is an electronically insulating layer on battery electrode due to electrolyte decomposition, which critically affects the battery performance. Electron tunneling is a key short-term electron transport mechanism that controls the SEI thickness and its growth behavior. The electron tunneling behavior is governed by the static Schrödinger equation and the tunneling barrier of SEIs, which shows an exponential decay of electron probability across the SEI layer. Here we develop a diffuse-interface description of electron tunneling behavior by formulating a phase-dependent tunneling barrier, so that the electrode/SEI and SEI/electrolyte interface positions do not need to be explicitly tracked when numerically solving the Schrödinger equation. We will show that this diffuse-interface description can accurately and efficiently predict the electron tunneling behaviors in 2D and 3D especially when the electrode/SEI and SEI/electrolyte interfaces are highly nonuniform. Furthermore, we will show that it can be seamlessly integrated with the phase-field simulation of electrodeposition and SEI growth in lithium-ion batteries, providing guidance for controlling the SEI morphology and improving the battery performance.
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Leskes, Michal. "(Invited) Elucidating the Structure and Function of the Electrode-Electrolyte Interface By New Solid State NMR Approaches". ECS Meeting Abstracts MA2022-01, nr 2 (7.07.2022): 369. http://dx.doi.org/10.1149/ma2022-012369mtgabs.
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The development of high-energy, long-lasting energy storage systems based on rechargeable batteries relies on our ability to control charge storage and degradation processes in the bulk of the electrode materials and at the electrode-electrolyte interface. NMR spectroscopy is exceptionally suited to follow the electrochemical and chemical processes in the bulk of the electrodes and electrolyte, providing atomic scale structural insight into the charge storage mechanisms and ion transport properties. However, interfacial properties, such as the processes governing charge transport between the electrode and the electrolyte, are much harder to study. These processes typically involve thin, heterogeneous and disordered layers that are formed chemically/electrochemically in the battery cell or artificially through coating the electrode material. While NMR is in principle an excellent approach for probing disordered phases, its low sensitivity presents an enormous challenge in the detection of interfacial processes. In this talk I will describe recent approaches to overcome the sensitivity limitation by the use of Dynamic Nuclear Polarization (DNP). In DNP, the large electron spin polarization is used to boost the sensitivity of NMR spectroscopy by orders of magnitude. I will show how we can use this approach to detect the solid-electrolyte interphase (SEI), electrode coatings as well as the electrode’s bulk, with unprecedented sensitivity. Furthermore, I will present new approaches to probe ion transport properties of various interfaces. These allow us to get insight into the functional role of interfaces, which along with the chemical and structural insight, can provide design rules for beneficial interfaces, an essential aspect for developing long-lasting energy storage systems.
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Wu, Xi, Xinghua Liang, Xiaofeng Zhang, Lingxiao Lan, Suo Li i Qixin Gai. "Structural evolution of plasma sprayed amorphous Li4Ti5O12 electrode and ceramic/polymer composite electrolyte during electrochemical cycle of quasi-solid-state lithium battery". Journal of Advanced Ceramics 10, nr 2 (6.02.2021): 347–54. http://dx.doi.org/10.1007/s40145-020-0447-9.
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AbstractA quasi-solid-state lithium battery is assembled by plasma sprayed amorphous Li4Ti5O12 (LTO) electrode and ceramic/polymer composite electrolyte with a little liquid electrolyte (10 µL/cm2) to provide the outstanding electrochemical stability and better normal interface contact. Scanning Electron Microscope (SEM), Scanning Transmission Electron Microscopy (STEM), Transmission Electron Microscopy (TEM), and Energy Dispersive Spectrometer (EDS) were used to analyze the structural evolution and performance of plasma sprayed amorphous LTO electrode and ceramic/polymer composite electrolyte before and after electrochemical experiments. By comparing the electrochemical performance of the amorphous LTO electrode and the traditional LTO electrode, the electrochemical behavior of different electrodes is studied. The results show that plasma spraying can prepare an amorphous LTO electrode coating of about 8 µm. After 200 electrochemical cycles, the structure of the electrode evolved, and the inside of the electrode fractured and cracks expanded, because of recrystallization at the interface between the rich fluorine compounds and the amorphous LTO electrode. Similarly, the ceramic/polymer composite electrolyte has undergone structural evolution after 200 test cycles. The electrochemical cycle results show that the cycle stability, capacity retention rate, coulomb efficiency, and internal impedance of amorphous LTO electrode are better than traditional LTO electrode. This innovative and facile quasi-solid-state strategy is aimed to promote the intrinsic safety and stability of working lithium battery, shedding light on the development of next-generation high-performance solid-state lithium batteries.
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Wu, Wei, Congjian Wang, Wenjuan Bian i Dong Ding. "Root Cause Analysis of Degradation in Protonic Ceramic Electrochemical Cells with Interfacial Electrical Sensors". ECS Meeting Abstracts MA2023-01, nr 54 (28.08.2023): 332. http://dx.doi.org/10.1149/ma2023-0154332mtgabs.
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Protonic ceramic electrochemical cells (PCEC), including solid oxide fuel/electrolysis cell, present promising routes to energy harvest and value-added chemical production. Despite tremendous efforts, PCEC still encounters several challenges, including poor thermal/chemical/mechanical compatibility and inferior solid-solid contact at the interfaces between electrolytes and electrodes. In this presentation, we will demonstrate in-line electrochemical characterization of interfacial electrical sensor embedded PCEC that can lead to fast identification of the failure mechanism of electrode supported PCECs. Upon the acquisition of quantitative contributions from different cell components to total degradation, data-driven machine learning is employed to further predict the long-term performance of the full cell up to 3000 hours. This presents novel insights into the degradation mechanism analysis in the solid-state electrochemical units, allowing ones to better modify the electrolyte and electrode materials and the interface between them, and develop more robust PCEC systems. The technology can be appliable to other electrochemical systems, including higher temperature counterpart (e.g., oxygen ion conducting solid oxide electrolysis cells, o-SOEC)
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Chen, Kongfa, Junji Hyodo, Aaron Dodd, Na Ai, Tatsumi Ishihara, Li Jian i San Ping Jiang. "Chromium deposition and poisoning of La0.8Sr0.2MnO3 oxygen electrodes of solid oxide electrolysis cells". Faraday Discussions 182 (2015): 457–76. http://dx.doi.org/10.1039/c5fd00010f.
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The effect of the presence of an Fe–Cr alloy metallic interconnect on the performance and stability of La0.8Sr0.2MnO3 (LSM) oxygen electrodes is studied for the first time under solid oxide electrolysis cell (SOEC) operating conditions at 800 °C. The presence of the Fe–Cr interconnect accelerates the degradation and delamination processes of the LSM oxygen electrodes. The disintegration of LSM particles and the formation of nanoparticles at the electrode/electrolyte interface are much faster as compared to that in the absence of the interconnect. Cr deposition occurs in the bulk of the LSM oxygen electrode with a high intensity on the YSZ electrolyte surface and on the LSM electrode inner surface close to the electrode/electrolyte interface. SIMS, GI-XRD, EDS and XPS analyses clearly identify the deposition and formation of chromium oxides and strontium chromate on both the electrolyte surface and electrode inner surface. The anodic polarization promotes the surface segregation of SrO and depresses the generation of manganese species such as Mn2+. This is evidently supported by the observation of the deposition of SrCrO4, rather than (Cr,Mn)3O4 spinels as in the case under the operating conditions of solid oxide fuel cells. The present results demonstrate that the Cr deposition is essentially a chemical process, initiated by the nucleation and grain growth reaction between the gaseous Cr species and segregated SrO on LSM oxygen electrodes under SOEC operating conditions.
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Chatterjee, Debanjali, Kaustubh Girish Naik, Bairav Sabarish Vishnugopi i Partha P. Mukherjee. "Mechanics-Coupled Interface Kinetics in Solid-State Batteries". ECS Meeting Abstracts MA2023-02, nr 4 (22.12.2023): 632. http://dx.doi.org/10.1149/ma2023-024632mtgabs.
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Solid-state batteries (SSBs) utilizing lithium metal anode are promising candidates for next-generation energy storage systems, offering high energy density and enhanced safety. However, imperfect electrochemical contact at the lithium-solid electrolyte (SE) interface results in transport limitations and high interfacial resistance, posing a critical bottleneck on rate performance. Solid-solid point contacts at the interface lead to stress hotspots and current-focusing, resulting in localized lithium deposition, filament growth and mechanical fracture of the SE. The application of external pressures potentially enables enhanced electrochemical contact at such solid-solid interfaces. Under these circumstances, non-uniform stresses arising due to the heterogeneous nature of interface morphology and surface defects play a critical role in the onset of interface instability. In this work, we present a mechanistic description of stress-coupled reaction kinetics governing the evolution of solid-solid interfaces in SSBs. We demonstrate how the energetic contribution of interfacial stresses alters the open circuit potential and exchange current density, which further affects the Butler-Vomer kinetics and morphological stability of the lithium-SE interface. Through our analysis, we illustrate the strong dependence of mechanical stress contributions to reaction current on the material characteristics of the electrode-SE pair and delineate interface stability regimes for different formulations of mechanics-coupled reaction kinetics interactions.
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Divya, Velpula, i M. V. Sangaranarayanan. "Electrodeposition of Polymer Nanostructures using Three Diffuse Double Layers: Polymerization beyond the Liquid/Liquid Interfaces". Electrochemical Energy Technology 4, nr 1 (28.04.2018): 6–20. http://dx.doi.org/10.1515/eetech-2018-0002.
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Abstract Nanostructured conducting polymers have received immense attention during the past few decades on account of their phenomenal usefulness in diverse contexts, while the interface between two immiscible liquids is of great interest in chemical and biological applications. Here we propose a novel Electrode(solid)/Electrolyte(aqueous)/Electrolyte(organic) Interfacial assembly for the synthesis of polymeric nanostructures using a novel concept of three diffuse double layers. There exist remarkable differences between the morphologies of the polymers synthesized using the conventional electrode/electrolyte method and that of the new approach. In contrast to the commonly employed electrodeposition at liquid/liquid interfaces, these polymer modified electrodes can be directly employed in diverse applications such as sensors, supercapacitors etc.
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Le, Jia-Bo, Qi-Yuan Fan, Jie-Qiong Li i Jun Cheng. "Molecular origin of negative component of Helmholtz capacitance at electrified Pt(111)/water interface". Science Advances 6, nr 41 (październik 2020): eabb1219. http://dx.doi.org/10.1126/sciadv.abb1219.
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Electrified solid/liquid interfaces are the key to many physicochemical processes in a myriad of areas including electrochemistry and colloid science. With tremendous efforts devoted to this topic, it is unexpected that molecular-level understanding of electric double layers is still lacking. Particularly, it is perplexing why compact Helmholtz layers often show bell-shaped differential capacitances on metal electrodes, as this would suggest a negative capacitance in some layer of interface water. Here, we report state-of-the-art ab initio molecular dynamics simulations of electrified Pt(111)/water interfaces, aiming at unraveling the structure and capacitive behavior of interface water. Our calculation reproduces the bell-shaped differential Helmholtz capacitance and shows that the interface water follows the Frumkin adsorption isotherm when varying the electrode potential, leading to a peculiar negative capacitive response. Our work provides valuable insight into the structure and capacitance of interface water, which can help understand important processes in electrocatalysis and energy storage in supercapacitors.
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Ers, Heigo, Liis Siinor i Piret Pikma. "The Puzzling Processes at Electrode | Ionic Liquid Interface". ECS Meeting Abstracts MA2022-02, nr 60 (9.10.2022): 2533. http://dx.doi.org/10.1149/ma2022-02602533mtgabs.
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J.M. Lehn stated in his Nobel prize lecture in 1988 that supramolecular chemistry is the chemistry of the intermolecular bond, covering the structure and functions of entities formed by the association of two or more chemical species [1]. The adsorption of organic molecules is the net result of the interactions between the molecules and the two phases, the metal and the electrolyte, and the interactions between the latter two. To this day, the universal understanding that the adsorption of organic molecules results in the formation of an ordered monolayer is based on the phenomenon observed in mainly aqueous solutions. However, the conception might not be straightforwardly transferrable to the organic additive + ionic liquid | electrode interface. For example, the existence of an interfacial multilayer structure of pure IL ions in contrast with an aqueous electrolyte has been previously shown in both experimental and computational studies. Furthermore, it has been shown that in ILs, if the ions form rigid layers on the electrode, it is necessary to apply an overpotential for interfacial restructuring. Therefore, studying the adsorption of organic additives in ionic liquids (IL) should contribute to a better understanding of metal | IL interfaces. In the given presentation we overview the characteristics of solid-liquid interface characteristics of various additives from ionic liquid media at different electrodes. Cyclic voltammetry, electrochemical impedance spectroscopy and in situ scanning tunnelling microscopy measurements were conducted to characterize the electrochemical behavior of the self-assembled layers of 4,4’-bipyridine (4,4’-BP) and 2,2’-bipyridine (2,2’-BP) at the Sb(111) | x-BP+1-ethyl-3-methylimidazolium tetrafluoroborate (EMImBF4) interface [2-3]. The specific adsorption of iodide ions was studied at Bi(111), Cd(0001) and pyrolytic graphite electrodes [4-6]. All the experiments were carried out in a three-electrode electrochemical cell in a glovebox. The halide ions are surface active ions with specific adsorption behavior [4-6]. The strong specific adsorption of halide ions at single crystal electrodes, as well as other electrodes, is a complicated process due to the partial charge transfer between adsorbed ions and the solid electrode surface. The properties of the adsorption layer depend on the electrode potential and the concentration of the surface-active ions in an electrolyte. The theory that the adsorption of organic molecules results in SAM formation is mainly based on the results observed in aqueous solutions. However, these findings may not be as straightforwardly linkable to the organic additive + ionic liquid | electrode interface. The analysis of cyclic voltammetry and impedance results revealed that 2,2′-BP and 4,4′-BP indeed adsorb at the Sb(111) interface, forming a thin dielectric layer at the electrode surface, confirmed by in situ STM measurements, resulting in the differential capacitance values nearly two times lower compared to EMImBF4. Acknowledgments: This work was supported by the Estonian Research Council grant PSG249, and by the EU through the European Regional Development Fund under project TK141 (2014-2020.4.01.15-0011). References: [1] Lehn, J.-M., Angew. Chem. Int. Ed. Engl. 1988, 27 (1), 89–112. [2] Pikma et al., Electrochem. Commun. 2015, 61 (Supplement C), 61–65. [3] H. Ers et al., Electrochim. Acta 2022, 421, 140468. [4] H. Ers et al., J. Electroanal. Chem. 2021, 903, 115826. [5] L. Siinor et al., Electrochem. Commun. 2013, 35, 5–7. [6] L. Siinor et al., J. Electroanal. Chem. 2014, 719, 133–137.
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Motheo, A. de J., R. M. P. Saldanha, R. de S. Neves, E. de Robertis i A. Sadkowski. "Characteristics of pyridine adsorption on Au(111) and Au(210) by EIS parameters fitting procedure". Eclética Química 28, nr 2 (2003): 29–40. http://dx.doi.org/10.1590/s0100-46702003000200004.
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Some aspects of the application of electrochemical impedance spectroscopy to studies of solid electrode / solution interface, in the absence of faradaic processes, are analysed. In order to perform this analysis, gold electrodes with (111) and (210) crystallographic orientations in an aqueous solution containing 10 mmol dm-3 KF, as supporting electrolyte, and a pyridine concentration varying from 0.01 to 4.6 mmol dm-3, were used. The experimental data was analysed by using EQUIVCRT software, which utilises non-linear least squares routines, attributing to the solid electrode / solution interface behaviour described by an equivalent circuit with a resistance in series with a constant phase element. The results of this fitting procedure were analysed by the dependence on the electrode potential on two parameters: the pre-exponential factor, Y0, and the exponent n f, related with the phase angle shift. By this analysis it was possible to observe that the pyridine adsorption is strongly affected by the crystallographic orientation of the electrode surface and that the extent of deviation from ideal capacitive behaviour is mainly of interfacial origin.
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Fan, Feng Ru. "(Invited) novel Charged Interfaces for Catalysis and Energy Conversion". ECS Meeting Abstracts MA2023-01, nr 34 (28.08.2023): 1885. http://dx.doi.org/10.1149/ma2023-01341885mtgabs.
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Charged interfaces are ubiquitous in many research fields such as electrochemistry, catalysis, and energy chemistry, and are key places where physical and chemical processes occur. The charged interface structure can also be affected by external fields such as light, electricity, and force, and becomes the key to regulating chemical reactions. It is of great significance for the development of surface and interface science, electrochemistry, catalysis and energy science to deeply understand the physical and chemical reaction process and mechanism of various charged interface systems, and to clarify the interaction between interface structure and reacting species. It is extremely challenging to rationally design, construct, and characterize various novel charged interfaces, and then comprehensively and deeply study their physical and chemical processes and mechanisms. By constructing new charged interface structures such as solid/solid triboelectric interface, micro-droplet charged liquid/gas interface, and metal/two-dimensional material charged interface, we study the reaction process and mechanism of the charged interface and develop new energy conversion pathways. A series of innovative research results: Discovered a new mechanism of triboelectric power generation, expanding the new direction of charged interface structure in energy conversion; established and developed epitaxial growth modes of various interface structures; accurately characterized the electron transport of charged interface structure and surface charge distribution and other physical and chemical properties. We have developed new systems such as solid/dielectric/liquid charged interfaces based on electrodes/dielectric layers/electrolytes and liquid/gas charged interfaces based on microdroplets, and explored new applications in energy conversion and electrocatalysis. Applying a voltage to the electrode/dielectric layer/electrolyte interface can polarize the dielectric layer and adsorb ions in the electrolyte, forming a special "sandwich" electric double layer. Different from the solid/solid charged interface formed by triboelectrification or light excitation, this is a new solid/dielectric/liquid charged interface system based on electrostatic adsorption. Based on this interface system, a new nanoscale power generation device is designed, which can effectively convert mechanical energy into electrical energy, and has high output performance. A new liquid/gas charged interface based on micro-droplets was constructed by means of electrospray, a new strategy for confining the liquid/gas charged interface was proposed, and a high-performance electrolytic water catalyst was prepared. The physical and chemical mechanism of accelerated chemical reactions at the liquid/gas charged interface is revealed, and the desolvation effect and interface confinement effect are proved to be effective ways to construct defect-rich electrocatalysts.
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Frankenberger, Martin, Madhav Singh, Alexander Dinter i Karl-Heinz Pettinger. "EIS Study on the Electrode-Separator Interface Lamination". Batteries 5, nr 4 (17.11.2019): 71. http://dx.doi.org/10.3390/batteries5040071.
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This paper presents a comprehensive study of the influences of lamination at both electrode-separator interfaces of lithium-ion batteries consisting of LiNi1/3Mn1/3Co1/3O2 cathodes and graphite anodes. Typically, electrode-separator lamination shows a reduced capacity fade at fast-charging cycles. To study this behavior in detail, the anode and cathode were laminated separately to the separator and compared to the fully laminated and non-laminated state in single-cell format. The impedance of the cells was measured at different states of charge and during the cycling test up to 1500 fast-charging cycles. Lamination on the cathode interface clearly shows an initial decrease in the surface resistance with no correlation to aging effects along cycling, while lamination on both electrode-separator interfaces reduces the growth of the surface resistance along cycling. Lamination only on the anode-separator interface shows up to be sufficient to maintain the enhanced fast-charging capability for 1500 cycles, what we prove to arise from a significant reduction in growth of the solid electrolyte interface.
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Min, Yu-Jeong, Ga-Eun Lee i Heon-Cheol Shin. "Novel Symmetric Cell Design for Analyzing All-Solid-State Battery Electrode". ECS Meeting Abstracts MA2023-01, nr 55 (28.08.2023): 2673. http://dx.doi.org/10.1149/ma2023-01552673mtgabs.
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All-solid-state lithium batteries (ASSBs) with sulfide-based solid electrolytes (SSEs) have drawn much attention recently for the next-generation batteries. But there are some obstacles to overcome for their practical use. The SSE|cathode interface with poor contact and (electro)chemical instability is the subject of special interest, since it critically aggravates the core performance of battery, including cycling stability and rate capability. In addition to the interfacial property, it has been widely known that Li+ transport characteristics inside the cathode is another key factor in terms of fast and efficient operation of all the lithium battery systems, including the ASSBs. Thus, it goes without saying that the accurate characterization of the interfacial and bulk properties of the cathode is essential to develop the ASSBs. There are limited numbers of test cells to analyze the interface and bulk properties of the battery. First, a conventional half-cell includes Li metal as a counter electrode (CE), which is assumed to have a negligible resistance compared to that of the working electrode (i.e., cathode). It has been reported, however, that the effect of Li CE on total electrochemical signal cannot be disregarded. Moreover, the relative contribution of Li CE to total signal is increasing with the use of the state-of-the-art cathode, whose resistance is getting dramatically lower with technological progress. That is, it is getting difficult to obtain a reliable cathode response by using the two-electrode half-cell configuration. Second, a three-electrode test cell provides the signal of each electrode separately and has been extensively used for the electrochemical analysis. When one uses it for the ASSBs, however, the signals can be erroneous due to the structural distortion caused by the reference electrode (RE) insertion and its own chemical instability, which is especially severe in ASSBs with SSEs. Finally, an alternative cell design to avoid the above problems is a symmetric cell including two identical electrodes facing each other. A general symmetric cell is fabricated by charging/discharging two unit-cell, disassembling them, and re-assembling the identical electrodes to face each other. Unfortunately, a series of such procedure, esp. disassembling/re-assembling, is not applicable to the ASSB systems. In this study, a novel non-destructive potential-controllable symmetric cell (PCSC) is proposed for ASSBs. It features a porous temporary CE (TCE) in parallel between two symmetric electrodes. TCE works as an acceptor or provider of Li to charge or discharge, thereby controls the electrode potential. Symmetric electrodes are then evaluated electrochemically after disconnecting the TCE. As a case study, we investigated and comparatively analyze the electrochemical characteristics of an ASSB cathode, LiNbO3-coated LiNi0.8Co0.1Mn0.1O2, obtained from the conventional test cells and PCSC. Figure presents the impedance spectra of test cells. The two-electrode half-cell impedance is noticeably affected by Li CE over a wide frequency range and the three-electrode cell impedance suffers from severe noise probably caused by RE in the low frequency region. This indicates that both test cells are not suitable for interpreting reliably the interfacial and bulk properties of the cathode. In contrast, the impedance spectra from the PCSC have similar trend to that of three-electrode cell, but provides much more stable impedance spectra, allowing more accurate estimation of interface and bulk characters. In this presentation, the results obtained from DC techniques, such as galvanostatic method, are also comparatively analyzed with conventional test cells and our PCSC. Moreover, the reliability of the estimated values from the PCSC will be discussed by the comparison with those of the previous works. Figure 1
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Park, Sangbaek. "Recent Advances in Interface Engineering for All-Solid-State Batteries". Ceramist 25, nr 1 (31.03.2022): 104–21. http://dx.doi.org/10.31613/ceramist.2022.25.1.03.
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All-solid-state batteries are attractive energy storage devices with high stability and energy density due to their non-flammable solid electrolytes that can utilize lithium and allow cells to be stacked directly in series. It is essential to develop superior solid interfaces for its commercialization by improving the interfacial stability and kinetics. However, complex interfacial phenomena in both solid electrolyte/cathode and solid electrolyte/anode make the interfacial problem of all-solid-state batteries difficult to solve. To overcome this issue, the origins of high resistance and low stability at solid interfaces have been widely explored and alternatives have been proposed accordingly. In this paper, the main methodologies and recent advances for solving the solid electrolyte/electrode interface problems will be reviewed in the chemical, electrochemical, and mechanical aspects.
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Wu, Cheng-Wei, Guo-Feng Xie i Wu-Xing Zhou. "Frontiers of investigation on thermal transport in all-solid-state lithium-ion battery". Acta Physica Sinica 71, nr 2 (2022): 026501. http://dx.doi.org/10.7498/aps.71.20211887.
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This paper briefly describes the characteristics of all-solid-state lithium-ion battery and the significance of investigation on the internal thermal transport. The related experimental and theoretical works on the thermal transport properties of cathode materials, anode materials, solid-state electrolytes, and electrode-electrolyte interfaces are introduced and summarized. In view of the unclear mechanism of the influence of lithium insertion and extraction process on the thermal conductivity of electrode materials, the challenge of solid-state amorphization to the research of thermal transport, and the limitation of models and methods in heat transport across the interface, we systematically sort out the important scientific issues of thermal transport in all-solid-state lithium-ion battery.
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Wang, Jing, Riwei Xu, Chengzhong Wang i Jinping Xiong. "Electrochemical Performance of Deposited LiPON Film/Lithium Electrode in Lithium—Sulfur Batteries". Molecules 29, nr 17 (4.09.2024): 4202. http://dx.doi.org/10.3390/molecules29174202.
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This paper presents a composed lithium phosphate (LiPON) solid electrolyte interface (SEI) film which was coated on a lithium electrode via an electrodeposit method in a lithium–sulfur battery, and the structure of the product was characterized through infrared spectrum (IR) analysis, X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), environment scanning electron microscope (ESEM), etc. Meanwhile, the electrochemical impedance spectrum and the interface stability of the lithium electrode with the LiPON film was analyzed, while the coulomb efficiency and the cycle life of the lithium electrode with the LiPON film in the lithium–sulfur battery were also studied. It was found that this kind of film can effectively inhibit the charge from transferring at the interface between the electrode and the solution, which can produce a more stable interface impedance on the electrode, thereby improving the interface contact with the electrolyte, and effectively improve the discharge performance, cycle life, and the coulomb efficiency of the lithium–sulfur battery. This is of great significance for the further development of solid electrolyte facial mask technology for lithium–sulfur batteries.
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Sharma, Shrishti, Gurpreet Kaur i Anshuman Dalvi. "Improving Interfaces in All-Solid-State Supercapacitors Using Polymer-Added Activated Carbon Electrodes". Batteries 9, nr 2 (25.01.2023): 81. http://dx.doi.org/10.3390/batteries9020081.
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Solvent-free all-solid-state supercapacitors have recently received attention. Despite their highly specific capacitance, they suffer issues related to the solid–solid interface that degrade their performance during prolonged cycling. Here, we propose a novel strategy for improving the electrode–electrolyte interface by introducing a small amount of polymer into the activated carbon-based electrode. An electrode composition of 80AC:8SA:7AB:5[PEO0.95 (LiClO4)0.05]—where AC, SA, and AB stand for activated carbon, sodium alginate binder, and acetylene black, respectively—is optimized. A composite membrane—viz., PEO-LiClO4 reinforced with 38 wt% NASICON structured nano crystallites of Li1.3Al0.3Ti1.7(PO4)3—is used as a solid electrolyte. Incorporating a small amount of salt-in-polymer (95PEO-5 LiClO4) in the electrode matrix leads to a smooth interface formation, thereby improving the performance parameters of the all-solid-state supercapacitors (ASSCs). A typical supercapacitor with a polymer-incorporated electrode exhibits a specific capacitance of ~102 Fg−1 at a discharge current of 1.5 Ag−1 and an operating voltage of 2 V near room temperature. These ASSCs also exhibit relatively better galvanostatic charge–discharge cycling, coulombic efficiency, specific energy, and power in comparison to those based on conventional activated carbon.
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Yokokawa, Harumi, Natsuko Sakai, Teruhisa Horita, Katsuhiko Yamaji i M. E. Brito. "Electrolytes for Solid-Oxide Fuel Cells". MRS Bulletin 30, nr 8 (sierpień 2005): 591–95. http://dx.doi.org/10.1557/mrs2005.166.
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AbstractThree solid-oxide fuel cell (SOFC) electrolytes, yttria-stabilized zirconia (YSZ), rare-earth–doped ceria (REDC), and lanthanum strontium gallium magnesium oxide (LSGM), are reviewed on their electrical properties, materials compatibility, and mass transport properties in relation to their use in SOFCs. For the fluorite-type oxides (zirconia and ceria), electrical properties and thermodynamic stability are discussed in relation to their valence stability and the size of the host and dopant ions. Materials compatibility with electrodes is examined in terms of physicochemical features and their relationship to the electrochemical reactions. The application of secondary ion mass spectrometry (SIMS) to detect interface reactivity is demonstrated. The usefulness of doped ceria is discussed as an interlayer to prevent chemical reactions at the electrode–electrolyte interfaces and also as an oxide component in Ni–cermet anodes to avoid carbon deposition on nickel surfaces. Finally, the importance of cation diffusivity in LSGM is discussed, with an emphasis on the grain-boundary effects.
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Lorenz, Oliver, Alexander Kühne, Martin Rudolph, Wahyu Diyatmika, Andrea Prager, Jürgen W. Gerlach, Jan Griebel i in. "Role of Reaction Intermediate Diffusion on the Performance of Platinum Electrodes in Solid Acid Fuel Cells". Catalysts 11, nr 9 (31.08.2021): 1065. http://dx.doi.org/10.3390/catal11091065.
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Understanding the reaction pathways for the hydrogen oxidation reaction (HOR) and the oxygen reduction reaction (ORR) is the key to design electrodes for solid acid fuel cells (SAFCs). In general, electrochemical reactions of a fuel cell are considered to occur at the triple-phase boundary where an electrocatalyst, electrolyte and gas phase are in contact. In this concept, diffusion processes of reaction intermediates from the catalyst to the electrolyte remain unconsidered. Here, we unravel the reaction pathways for open-structured Pt electrodes with various electrode thicknesses from 15 to 240 nm. These electrodes are characterized by a triple-phase boundary length and a thickness-depending double-phase boundary area. We reveal that the double-phase boundary is the active catalytic interface for the HOR. For Pt layers ≤ 60 nm, the HOR rate is rate-limited by the processes at the gas/catalyst and/or the catalyst/electrolyte interface while the hydrogen surface diffusion step is fast. For thicker layers (>60 nm), the diffusion of reaction intermediates on the surface of Pt becomes the limiting process. For the ORR, the predominant reaction pathway is via the triple-phase boundary. The double-phase boundary contributes additionally with a diffusion length of a few nanometers. Based on our results, we propose that the molecular reaction mechanism at the electrode interfaces based upon the triple-phase boundary concept may need to be extended to an effective area near the triple-phase boundary length to include all catalytically relevant diffusion processes of the reaction intermediates.
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Lai, Chun Yan, Jing Jing Xu i Yong Feng Wei. "Study on the Solid Electrolyte Interface at the Surface of Anode Electrode in Li4Ti5O12/LiFePO4 Battery System". Advanced Materials Research 347-353 (październik 2011): 3522–26. http://dx.doi.org/10.4028/www.scientific.net/amr.347-353.3522.
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A safe lithium-ion battery system of Li4Ti5O12/LiFePO4 was prepared, the solid electrolyte interface on the surface of Li4Ti5O12 electrode and the electrochemical performances of this lithium-ion battery system were studied. XRD、SEM and EIS texts were used to analyses the solid electrolyte interface on the surface of anode electrode. The result of XRD indicates that new material does generate at the surface of Li4Ti5O12 anode electrode. The result of EIS indicates that the SEI film increased the resistance of the battery, and the resistance will decrease as the cycle time increasing.
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Min, Jungki, Seongmin Bak, Yuxin Zhang, Mingyu Yuan, Nicholas Pietra, Joshua Russell, Dawei Xia i in. "Interfacial Phase Separation Governs the Chemomechanics of Polymer Electrolytes in High-Voltage, Solid-State Lithium Batteries". ECS Meeting Abstracts MA2024-01, nr 5 (9.08.2024): 748. http://dx.doi.org/10.1149/ma2024-015748mtgabs.
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Polymer electrolytes hold great promise for safe and high-energy solid-state batteries. Multiphase polymer electrolytes, consisting of mobile and rigid phases, exhibit fast ion conduction and desired mechanical properties. However, fundamental challenges exist in understanding and regulating intricate chemomechanical interactions at the electrode-electrolyte interface, especially when using a high-voltage layered cathode. Here, we report that depletion of the mobile conductive phase at the interface contributes to battery performance degradation. Molecular ionic composite electrolytes, composed of a rigid-rod ionic polymer with small mobile cations and anions, serve as a multiphase platform to investigate the evolution of conductive domains at the interface. Synchrotron chemical and structural analyses enable the direct visualization of concentration polarization and spatially resolve the interfacial chemical states over a statistically significant field of view for buried interfaces. We discover that concentration and chemical heterogeneities prevail at electrode-electrolyte interfaces, leading to interfacial chemomechanical degradation. We further demonstrate an interphase tailoring strategy based on electrolyte additives to mitigate such interfacial heterogeneity and improve battery stability. While polymer electrolytes have been considered “deformable” for conformal interfaces, our work shows the hidden roles of interfacial chemomechanics in polymer electrolytes and provides an effective mitigation approach.
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Inada, Ryoji, Kohei Okuno, Shunsuke Kito, Tomohiro Tojo i Yoji Sakurai. "Properties of Lithium Trivanadate Film Electrodes Formed on Garnet-Type Oxide Solid Electrolyte by Aerosol Deposition". Materials 11, nr 9 (1.09.2018): 1570. http://dx.doi.org/10.3390/ma11091570.
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We fabricated lithium trivanadate LiV3O8 (LVO) film electrodes for the first time on a garnet-type Ta-doped Li7La3Zr2O12 (LLZT) solid electrolyte using the aerosol deposition (AD) method. Ball-milled LVO powder with sizes in the range of 0.5–2 µm was used as a raw material for LVO film fabrication via impact consolidation at room temperature. LVO film (thickness = 5 µm) formed by AD has a dense structure composed of deformed and fractured LVO particles and pores were not observed at the LVO/LLZT interface. For electrochemical characterization of LVO film electrodes, lithium (Li) metal foil was attached on the other end face of a LLZT pellet to comprise a LVO/LLZT/Li all-solid-state cell. From impedance measurements, the charge transfer resistance at the LVO/LLZT interface is estimated to be around 103 Ω cm2 at room temperature, which is much higher than at the Li/LLZT interface. Reversible charge and discharge reactions in the LVO/LLZT/Li cell were demonstrated and the specific capacities were 100 and 290 mAh g−1 at 50 and 100 °C. Good cycling stability of electrode reaction indicates strong adhesion between the LVO film electrode formed via impact consolidation and LLZT.
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Yang, Guang, i Jagjit Nanda. "(Invited) Multiscale Interfacial Heterogeneity Explored by Advanced Spectroscopy and Imaging for Batteries Beyond Lithium-Ion". ECS Meeting Abstracts MA2023-01, nr 46 (28.08.2023): 2496. http://dx.doi.org/10.1149/ma2023-01462496mtgabs.
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Keywords: solid-liquid interface, solid-state battery, surface-enhanced Raman spectroscopy (SERS), tip-enhanced Raman spectroscopy (TERS), neutron tomography, sulfide solid-state electrolyte, Raman imaging The ever-growing needs for energy storage systems require batteries with even higher power and energy density with extended life and enhanced safety beyond the current Li-ion battery technologies. Fulfilling these needs requires new battery chemistries, including high-energy-density electrode materials, solid-state electrolytes, and efficient interphases to mitigate the side reactions between the electrodes and the electrolytes. Charge transport across the electrode and electrolyte interface is believed to be one of the charge/discharge rate-limiting steps. Although the composition, morphology, and structure of solid-electrolyte interphase (SEI) have been extensively studied, probing its evolution at the nanoscale is challenging to a large extent. Plasmon-enhanced Raman spectroscopy (PERS) is promising to solve this challenge. PERS is the resonant oscillation of conduction electrons at the interface between negative and positive permittivity molecules stimulated by incident light. It includes surface-enhanced Raman spectroscopy (SERS) and tip-enhanced Raman spectroscopy (TERS). In the first part of this talk, I will show that gap-mode SERS is ideal to probe salt solvation structure in the immediate vicinity (< 20 nm) of the electrode/electrolyte interface. SERS lacks the nanoscale resolution in the sample plane. This can be compensated by TERS. TERS analysis on cycled high-energy silicon anodes indicates that the nanometer scale SEI "islands" are unevenly distributed. Even for the same SEI "island", the composition is different from point to point with inter-point distance smaller than 10 nm. All-solid-state lithium metal batteries (SSBs) promise specific energy >500 Wh/kg. A solid-state electrolyte (SSE) plays an irreplaceable role in reaching such an energy-density goal. Sulfide-based SSEs have emerged as a prominent class of soft ionic conductors that have comparable room-temperature ionic conductivity to their liquid electrolyte counterparts. However, when paring with a high voltage cathode, such as lithium nickel manganese cobalt oxide (NMC), the (electro)chemical instability of the sulfide SSE at the electrode/SSE interfaces becomes a major challenge. The interfacial instability can result in >50% initial capacity loss in a Li/sulfide SSE/NMC battery, thereby keeping the sulfide SSEs from commercialization. In the second part of this talk, I will show how we synergistically use neutron computed tomography and in situ Raman imaging, with clustering analysis to track lithium displacement at the interface of a sulfide-based SSB. Acknowledgment This research was conducted at Oak Ridge National Laboratory, managed by UT Battelle, LLC, for the U.S. Department of Energy (DOE) and is supported by Asst. Secretary, Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (VTO) through the Advanced Battery Materials Research (BMR) Program. This research used resources at High Flux Isotope Reactor, a DOE Office of Science User Facilities operated by the Oak Ridge National Laboratory.
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Winterhalder, Franziska Elisabeth, Yousef Alizad Farzin, Olivier Guillon, Andre Weber i Norbert H. Menzler. "Perovskite-Based Materials As Alternative Fuel Electrodes for Solid Oxide Electrolysis Cells (SOECs)". ECS Transactions 111, nr 6 (19.05.2023): 1115–23. http://dx.doi.org/10.1149/11106.1115ecst.
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Perovskites show high potential as alternative fuel electrodes in solid oxide electrolysis cells (SOECs) due to their high chemical stability, high conductivity, good catalytic activity and cost-effectiveness. In this work, four perovskites (strontium-iron-niobate double perovskite (SFN), strontium-iron-titanate (STF), lanthanum-strontium-titanate (LST), and lanthanum-strontium-iron-manganese (LSFM)) were examined as fuel electrode materials for SOECs. First, the chemical stability of the perovskites in a reducing atmosphere and the reactivity between the electrode and electrolyte material were analyzed. Besides featuring good chemical stability under reducing conditions, SFN double perovskite and LST exhibit the lowest interaction with the electrolyte (yttria-stabilized zirconia, 8YSZ) after thermal treatment. The results indicate a need for a barrier layer between the tested electrode materials and the YSZ electrolyte to achieve sufficient cell performance throughout its operation in the electrolysis mode. After thoroughly evaluating all preliminary tests, STF was chosen for the first subsequent electrochemical tests. Initial impedance measurements of symmetrical electrolyte-supported cells consisting of pure STF-based electrodes with and without a barrier layer between the electrodes and the electrolyte were conducted to obtain a base for further optimization. For the 5STF fuel electrode, the obtained EIS data confirm the conclusion from the reactivity experiments. Applying a barrier layer at the 5STF fuel electrode/ electrolyte interface is needed to reduce the cell´s ohmic and polarization resistances.
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Nagao, Kenji, Yuka Nagata, Atsushi Sakuda, Akitoshi Hayashi, Minako Deguchi, Chie Hotehama, Hirofumi Tsukasaki i in. "A reversible oxygen redox reaction in bulk-type all-solid-state batteries". Science Advances 6, nr 25 (czerwiec 2020): eaax7236. http://dx.doi.org/10.1126/sciadv.aax7236.
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An all-solid-state lithium battery using inorganic solid electrolytes requires safety assurance and improved energy density, both of which are issues in large-scale applications of lithium-ion batteries. Utilization of high-capacity lithium-excess electrode materials is effective for the further increase in energy density. However, they have never been applied to all-solid-state batteries. Operational difficulty of all-solid-state batteries using them generally lies in the construction of the electrode-electrolyte interface. By the amorphization of Li2RuO3 as a lithium-excess model material with Li2SO4, here, we have first demonstrated a reversible oxygen redox reaction in all-solid-state batteries. Amorphous nature of the Li2RuO3-Li2SO4 matrix enables inclusion of active material with high conductivity and ductility for achieving favorable interfaces with charge transfer capabilities, leading to the stable operation of all-solid-state batteries.
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Mukherjee, Partha P., Bairav Sabarish Vishnugopi i Kaustubh Girish Naik. "(Keynote) Heterogeneities in Solid-State Battery Interfaces and Architectures". ECS Meeting Abstracts MA2023-01, nr 25 (28.08.2023): 1639. http://dx.doi.org/10.1149/ma2023-01251639mtgabs.
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While lithium-ion batteries have garnered significant success over the past decades, the development of next-generation batteries with higher energy densities is crucial for future electromobility demands such as long-range electric vehicles and electric aviation. In this context, solid-state batteries (SSBs), consisting of an inorganic solid electrolyte and lithium metal, are promising in simultaneously improving the energy density and safety. Despite their irrefutable promise, the realization of practical SSBs is predicated on overcoming important challenges pertaining to electro-chemo-mechanics, transport, and interface evolution. Myriad heterogeneities ranging from defects/voids at the lithium/solid electrolyte interface, grain boundaries in the solid electrolyte and singularities in the solid-state cathode have a pivotal influence on the onset of failure and electrochemical performance. In this presentation, the critical role of heterogeneities on the mechanistic interplay at solid-solid interfaces and the underlying failure mechanisms will be delineated. Governed by the manifestation of spatio-temporal heterogeneity at scales, the origin of solid/solid interface instability, resultant asymmetry in the plating/stripping response and electrode crosstalk implications will be discussed.
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Park, Beom-Kyeong, Qian Zhang, Peter W. Voorhees i Scott A. Barnett. "Conditions for stable operation of solid oxide electrolysis cells: oxygen electrode effects". Energy & Environmental Science 12, nr 10 (2019): 3053–62. http://dx.doi.org/10.1039/c9ee01664c.
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Guseynov, Rizvan M., Radzhab A. Radzhabov, Kheirulla M. Makhmudov i Ruslan K. Kelbikhanov. "INVESTIGATION OF ELECTROCHEMICAL CELL WITH REVERSIBLE ELECTRODE – SOL-ID ELECTROLYTE OR IONIC MELT INTERFACE BY LINEAR CURRENT AND LINEAR POTENTIAL SCANNING METHODS". IZVESTIYA VYSSHIKH UCHEBNYKH ZAVEDENIY KHIMIYA KHIMICHESKAYA TEKHNOLOGIYA 61, nr 4-5 (17.04.2018): 57. http://dx.doi.org/10.6060/tcct.20186104-05.5574.
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The main purpose of this article is a study of the kinetics of two simultaneous process: the charging of the electric double layer and discharge-ionization on the reversible silver electrode – sulfate solid electrolyte interface and its melt in two regimes: galvanodynamical and potentiodynamical. The investigation of the electrochemical kinetics was performed by operational impedance method which is based on the Laplas transformation and Ohm’s law between current, voltage and complex resistance (impedance). By corresponding mathematical computations the analytical expression of time dependence of current which passes through electrochemical cell in potentiodynamical mode were received. The analytical expression of interface potential – time dependence in galvanodynamical regime (mode) was obtained also. The electrode – solid electrolyte or its ionic melt interface potential – time dependence in galvanodynamical regime is described by exponential function. The time dependence of the current which passes through electrochemical cell in potentiodynamical regime is described by linear function. The comparative analysis of a results of two independent methods showed that for the investigation of the electrochemical systems contained the reversible metallic electrode – solid electrolyte and ionic melt interface may be used not only alternate current methods but relaxation methods also (for instance, Galvanodynamic and Potentiodynamic methods).Forcitation:Guseynov R.M.; Radzhabov R.A.; Makhmudov Kh.M.; Kelbikhanov R.K. Investigation of electrochemical cell with reversible electrode – solid electrolyte or ionic melt interface by linear current and linear potential scanning methods. Izv. Vyssh. Uchebn. Zaved. Khim. Khim. Tekhnol. 2018. V. 61. N 4-5. P. 57-63
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Allen, Jan L., Bria A. Crear, Rishav Choudhury, Michael J. Wang, Dat T. Tran, Lin Ma, Philip M. Piccoli, Jeff Sakamoto i Jeff Wolfenstine. "Fast Li-Ion Conduction in Spinel-Structured Solids". Molecules 26, nr 9 (30.04.2021): 2625. http://dx.doi.org/10.3390/molecules26092625.
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Spinel-structured solids were studied to understand if fast Li+ ion conduction can be achieved with Li occupying multiple crystallographic sites of the structure to form a “Li-stuffed” spinel, and if the concept is applicable to prepare a high mixed electronic-ionic conductive, electrochemically active solid solution of the Li+ stuffed spinel with spinel-structured Li-ion battery electrodes. This could enable a single-phase fully solid electrode eliminating multi-phase interface incompatibility and impedance commonly observed in multi-phase solid electrolyte–cathode composites. Materials of composition Li1.25M(III)0.25TiO4, M(III) = Cr or Al were prepared through solid-state methods. The room-temperature bulk Li+-ion conductivity is 1.63 × 10−4 S cm−1 for the composition Li1.25Cr0.25Ti1.5O4. Addition of Li3BO3 (LBO) increases ionic and electronic conductivity reaching a bulk Li+ ion conductivity averaging 6.8 × 10−4 S cm−1, a total Li-ion conductivity averaging 4.2 × 10−4 S cm−1, and electronic conductivity averaging 3.8 × 10−4 S cm−1 for the composition Li1.25Cr0.25Ti1.5O4 with 1 wt. % LBO. An electrochemically active solid solution of Li1.25Cr0.25Mn1.5O4 and LiNi0.5Mn1.5O4 was prepared. This work proves that Li-stuffed spinels can achieve fast Li-ion conduction and that the concept is potentially useful to enable a single-phase fully solid electrode without interphase impedance.
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Won, Eun-Seo, i Jong-Won Lee. "Biphasic Solid Electrolytes with Homogeneous Li-Ion Transport Pathway Enabled By Metal-Organic Frameworks". ECS Meeting Abstracts MA2022-01, nr 55 (7.07.2022): 2248. http://dx.doi.org/10.1149/ma2022-01552248mtgabs.
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Solid-state batteries based on nonflammable inorganic solid electrolytes provide a promising technical solution that can resolve the safety issues of current lithium-ion batteries. Biphasic solid electrolytes comprising Li7La3Zr2O12 (LLZO) garnet and polymer have been attracting significant interest for solid-state Li batteries because of their mechanical robustness and enhanced Li+ conductivity, compared to conventional polymer electrolytes. Furthermore, the hybridization allows for the fabrication of thin and large-area electrolyte membranes without the need for high-temperature sintering of LLZO. However, the non-uniform distribution of LLZO particles and polymer species in biphasic electrolytes may cause uneven Li+ conduction, which results in poor interfacial stability with electrodes during repeated charge–discharge cycling. In this study, we report a biphasic solid electrolyte with homogeneous Li+ transport pathway achieved by a metal–organic framework (MOF) layer. To regulate and homogenize the Li+ flux across the interface between the electrolyte and electrode, a free-standing, biphasic solid electrolyte membrane is integrated with the MOF nanoparticle layer. A mixture of plastic crystal (PC) and polymeric phase is infused into porous networks of the MOF-integrated electrolyte membrane, producing the percolating Li+ conduction pathways. The MOF-integrated electrolyte membrane is found to form the smooth and uniform interface with nanoporous channels in contact with the electrodes, effectively facilitating homogeneous Li+ transport. A solid-state battery with the MOF-integrated electrolyte membrane shows the enhanced rate-capability and cycling stability in comparison to the battery with the unmodified biphasic electrolyte. This study demonstrates that the proposed electrolyte design provides an effective approach to improving the interfacial stability of biphasic electrolytes with electrodes for long-cycling solid-state batteries. [1] H.-S. Shin, W. Jeong, M.-H. Ryu, S.W. Lee, K.-N. Jung, J.-W. Lee, Electrode-to-electrode monolithic integration for high-voltage bipolar solid-state batteries based on plastic-crystal polymer electrolyte, Chem. Eng. J, published online. [2] T. Jiang, P. He, G. Wang, Y. Shen, C.-W. Nan, L.-Z. Fan, Solvent-free synthesis of thin, flexible, nonflammable garnet-based composite solid electrolyte for all-solid-state lithium batteries, Adv. Energy Mater. 10 (2020) 1903376.
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Swain, Greg M., Alfred B. Anderson i John C. Angus. "Applications of Diamond Thin Films in Electrochemistry". MRS Bulletin 23, nr 9 (wrzesień 1998): 56–60. http://dx.doi.org/10.1557/s0883769400029389.
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Electrochemical reactions typically involve electron transfer between an electrode and a dissolved chemical species at a solid-electrode/liquid-electrolyte interface. Three broad classes of electrochemical applications may be identified: (1) synthesis (or destruction), in which an applied potential is used to bring about a desired chemical oxidation or reduction reaction; (2) analysis, in which the current/potential characteristics of an electrode are used to determine the type and concentration of a species; and (3) power generation. These broad types of applications require stable, conductive, chemically robust, and economical electrodes. Diamond electrodes, fabricated by chemical vapor deposition, provide electrochemists with an entirely new type of carbon electrode that meets these requirements for a wide range of applications.The first reports of electrochemical studies using diamond were in the mid-1980s. During the past several years, the field has attracted increasing attention. This review summarizes the electrochemical properties of diamond that make it a unique electrode material and that distinguish it from conventional carbon electrodes.