Review
Chemistry, Multidisciplinary
Jinghua Wu, Sufu Liu, Fudong Han, Xiayin Yao, Chunsheng Wang
Summary: All-solid-state lithium batteries (ASSLBs) are considered the next generation electrochemical energy storage devices due to their high safety and energy density, along with simple packaging and wide operable temperature range. The sulfide electrolytes, with the highest ionic conductivity among solid-state electrolytes, face challenges such as narrow electrochemical stability window, unstable electrode/electrolyte interfaces, and lithium dendrite formation. Research on emerging sulfide electrolytes and preparation methods is ongoing, focusing on achieving required properties for stable electrochemical performance and compatible interfaces in ASSLBs.
ADVANCED MATERIALS
(2021)
Review
Chemistry, Multidisciplinary
Boran Tao, Chaojun Ren, Hongda Li, Baosheng Liu, Xiaobo Jia, Xinwei Dong, Shaohui Zhang, Haixin Chang
Summary: This review presents the research progress on solid-state electrolytes in all-solid-state lithium batteries, analyzes the ion transport mechanism, and summarizes effective strategies for improving ionic conductivity and interface stability.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Review
Electrochemistry
Zhan Wu, Xiaohan Li, Chao Zheng, Zheng Fan, Wenkui Zhang, Hui Huang, Yongping Gan, Yang Xia, Xinping He, Xinyong Tao, Jun Zhang
Summary: Due to their high energy density and environmental friendliness, lithium-ion batteries (LIBs) have been widely used in electric vehicles, energy storage systems, and other devices. However, the traditional LIBs with liquid electrolytes (LEs) pose safety hazards. In order to achieve higher safety and energy density, researchers are exploring the use of solid-state electrolytes (SSEs) instead. This review comprehensively summarizes the behaviors, properties, and mechanisms of interfaces in all-solid-state lithium batteries with various sulfide SSEs, as well as recent research progress on characterization methods and designs to stabilize interfaces. Outlooks, challenges, and possible interface engineering strategies are also discussed.
ELECTROCHEMICAL ENERGY REVIEWS
(2023)
Article
Chemistry, Physical
Yaqi Hu, Zhen Sun, Zongliang Zhang, Siliang Liu, Fangbo He, Yang Liu, Zhi Zhuang, Fangyang Liu
Summary: This study investigates the use of a sulfide cathode active material Li2TiS3 that is chemically compatible with sulfide solid electrolytes in all-solid-state lithium batteries. The batteries show high discharge capacity and good capacity retention at room temperature, and the Li6PS5Cl electrolyte also contributes to additional capacity. The potential of Li2TiS3 material for practical applications is explored.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Xinxin Zhu, Wei Jiang, Shu Zhao, Renzhi Huang, Min Ling, Chengdu Liang, Liguang Wang
Summary: The design of composite sulfur cathode is crucial for determining the physical and chemical properties of all-solid-state lithium-sulfur batteries (ASSLSBs), and the selection of solid-state electrolyte in the composite sulfur cathode is rarely studied. By comparing three typical sulfide solid-state electrolytes, the excellent compatibility between Li7P(3)S(11) electrolyte and sulfur cathode is revealed. The ASSLSBs based on Li7P(3)S(11) electrolytes exhibit fast reaction kinetics and high electrochemical stability, contributing to chemical congruency. These findings provide guidance for developing high-energy-density ASSLSBs.
Review
Electrochemistry
Jinghua Wu, Lin Shen, Zhihua Zhang, Gaozhan Liu, Zhiyan Wang, Dong Zhou, Hongli Wan, Xiaoxiong Xu, Xiayin Yao
Summary: All-solid-state lithium batteries (ASSLBs) based on sulfide electrolytes and oxide cathodes have high safety and energy density, but face challenges such as stability of electrolytes, complex interfacial issues, and unstable electrode interfaces. Despite oxide cathodes being stable and industrialized, their compatibility with sulfide electrolytes presents a challenge for commercial use in ASSLBs.
ELECTROCHEMICAL ENERGY REVIEWS
(2021)
Article
Chemistry, Physical
Jong Seok Kim, Seungwon Jung, Hiram Kwak, Yoonjae Han, Suhwan Kim, Jongwoo Lim, Yong Min Lee, Yoon Seok Jung
Summary: A novel halide-sulfide hybrid catholyte design is reported for Ni-rich layered oxide cathodes in all-solid-state Li batteries. The hybrid catholyte consists of Li3YCl6 coatings for protection and Li6PS5Cl as a Li+conductor, which significantly improves the performance of the Li[Ni0.88Co0.11Al0.01]O2 cathodes.
ENERGY STORAGE MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Xin Lu, Chih-Long Tsai, Shicheng Yu, Hongying He, Osmane Camara, Hermann Tempel, Zigeng Liu, Anna Windmueller, Evgeny Alekseev, Simone Koecher, Shibabrata Basak, Li Lu, Ruediger A. Eichel, Hans Kungl
Summary: This review focuses on the importance of phosphosulfide electrolytes in solid-state lithium-ion batteries. The author introduces different types of phosphosulfide electrolytes and discusses their Li-ion conductivity and electrochemical stability vs. metallic lithium. By comparing the chemistry and structure of different electrolytes, the author summarizes the current status and future perspectives of research on Li-ion conducting phosphosulfide electrolytes.
FUNCTIONAL MATERIALS LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Yushi Fujita, Atsushi Sakuda, Yuki Hasegawa, Minako Deguchi, Kota Motohashi, Ding Jiong, Hirofumi Tsukasaki, Shigeo Mori, Masahiro Tatsumisago, Akitoshi Hayashi
Summary: All-solid-state lithium-sulfur (Li/S) batteries show high capacities and long cycle lives. This study develops a Li2S-Li2O-LiI positive electrode with an active material dispersed in an amorphous matrix. The electrode exhibits high charge-discharge capacities and a high specific capacity at a 2 C rate and 25 degrees C, with nanoscale ion-conduction pathways provided by Li2O-LiI. Furthermore, a cell with a high areal capacity is successfully operated using this positive electrode.
Review
Chemistry, Physical
Tianwei Yu, Xiaofei Yang, Rong Yang, Xiangtao Bai, Guofeng Xu, Shangqian Zhao, Yi Duan, Yanlong Wu, Jiantao Wang
Summary: All-solid-state lithium batteries (ASSLBs) have gained increasing attention for their safety and energy density advantages. Inorganic solid-state electrolytes (SSE5) have shown progress, with systems including oxide, sulfide, and halide SSE5. These inorganic SSE5 typically exhibit an ionic conductivity close to liquid electrolytes at around 10(-3) S/cm at room temperature.
JOURNAL OF ALLOYS AND COMPOUNDS
(2021)
Review
Chemistry, Multidisciplinary
Ping Li, Zhihui Ma, Jie Shi, Kun Han, Qi Wan, Yongchang Liu, Xuanhui Qu
Summary: This review provides an overview of several promising sulfide solid electrolytes and discusses the strategies for improving their resistance against oxidation. The major challenges for practical applications of all-solid-state batteries and different types of sulfide electrolytes are also pointed out.
Review
Electrochemistry
Xiaotang Gan, Zihao Yang, Zhiping Song
Summary: Organic cathode materials (OCMs) have high resource sustainability, structural diversity, theoretical energy density, and potentially low cost, but suffer from dissolution in liquid non-aqueous electrolyte. Solid-state batteries (SSBs) are considered the final solution to Li and Na metal batteries due to their safety, but face challenges in contacting with inorganic cathode materials. Therefore, combining OCMs and SSBs could compensate for their respective deficiencies and bring new challenges and opportunities for practical applications.
BATTERIES & SUPERCAPS
(2023)
Review
Electrochemistry
Xiaotang Gan, Zihao Yang, Zhiping Song
Summary: This review briefly introduces the fundamental knowledge of organic cathode materials (OCMs) and solid-state batteries (SSBs), with emphasis on different types of solid-state electrolytes (SSEs). The reported works on OCM-based SSBs are summarized, classified into non-ceramic, semi-ceramic, and all-ceramic ones. Finally, the main scientific issues and possible solutions are concluded.
BATTERIES & SUPERCAPS
(2023)
Letter
Chemistry, Multidisciplinary
Xiaolei Zhao, Pan Xiang, Jinghua Wu, Ziqiang Liu, Lin Shen, Gaozhan Liu, Ziqi Tian, Liang Chen, Xiayin Yao
Summary: In this study, a Li9.88GeP1.96Sb0.04S11.88Cl0.12 solid electrolyte was synthesized, which exhibited excellent tolerance and stability to toluene. The ultrathin membranes of this electrolyte were successfully prepared with adjustable thickness and showed good ionic conductivity. The fabricated all-solid-state lithium battery with this membrane showed high capacity retention.
Article
Nanoscience & Nanotechnology
Hany El-Shinawi, Ed Darnbrough, Johann Perera, Innes McClelland, David E. J. Armstrong, Edmund J. Cussen, Serena A. Cussen
Summary: Deformable, fast-ion conducting sulfides make it possible to create bulk-type solid-state batteries that can rival current Li-ion batteries in terms of energy density and scalability. One way to optimize the energy density of these batteries is to minimize the size of the electrolyte layer by integrating the solid electrolyte into thin membranes. However, it is difficult to prepare or integrate additive-free thin membranes or membranes based on preprepared scaffolds on a large scale. In this study, a scalable solution-based approach is proposed to produce glass microfiber-reinforced composites that restore the deformability of sulfide electrolytes and can easily be shaped into thin membranes through cold pressing. This approach enables easy preparation and enhances the energy density of sulfide-based solid-state batteries.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Materials Science, Multidisciplinary
Gabriel L. Murphy, Zhaoming Zhang, Helen E. Maynard-Casely, Joshua Stackhouse, Piotr M. Kowalski, Thomas Vogt, Evgeny Alekseev, Brendan J. Kennedy
Summary: A combined experimental and theoretical investigation was conducted to study the compressibility of two SrUO4-x polymorphs (alpha and fi) under hydrostatic conditions. The study explains the contrasting chemical and mechanical behaviors of these polymorphs by differences in oxygen defect formation chemistry. The experimental data and ab initio calculations revealed that the expansion of the uranyl bonds in alpha-SrUO4 and fi-SrUO4 under hydrostatic pressures is due to the reduction of uranium formal oxidation state and the formation of oxygen vacancies. The difference in preferred lattice sites for oxygen defect formation leads to the significant difference in apparent bulk moduli between the two polymorphs.
Article
Chemistry, Multidisciplinary
An-Yuan Hou, Chih-Yang Huang, Chih-Long Tsai, Chun-Wei Huang, Roland Schierholz, Hung-Yang Lo, Hermann Tempel, Hans Kungl, Ruediger-A. Eichel, Jeng-Kuei Chang, Wen-Wei Wu
Summary: LLZO-based all-solid-state Li batteries (SSLBs) have the potential for enhanced safety and improved energy density, but the rigid nature of ceramics poses challenges in the SSLB fabrication and interfacial stability during electrochemical cycling. This study demonstrates a promising LLZO-based SSLB with high areal capacity and stable cycle performance. In operando TEM is used to investigate the delithiation/lithiation process and capacity degradation mechanism on an atomic scale. The capacity degradation is attributed to interfacial delamination and the oxygen deficiency of LiCoO2.
Article
Chemistry, Multidisciplinary
Xin Lu, Anna Windmueller, Dana Schmidt, Sandro Schoener, Roland Schierholz, Chih-Long Tsai, Hans Kungl, Xunfan Liao, Shicheng Yu, Hermann Tempel, Yiwang Chen, Rudiger-A. Eichel
Summary: The structural and morphological changes of Li10GeP2S12 were studied over a comprehensive heat treatment range (50 - 700 degrees C) using a ball milling-heating method. The formation process was divided into four zones based on phase composition: Educt, Intermediary, Formation, and Decomposition zones. Diversified intermediate phases and multi-phasic lithium phosphosulfides were found to be involved in the formation and decomposition of Li10GeP2S12. The phase composition exhibited deviations around the transition temperatures of different formation zones, with the sample decomposing into complex phases at 650 degrees C.
Article
Chemistry, Multidisciplinary
Ifeanyichukwu D. Unachukwu, Vaibhav Vibhu, Jan Uecker, Izaak C. Vinke, Ruediger-A. Eichel, L. G. J. (Bert) de Haart
Summary: In this study, the performance and electrochemical behavior of the Ni-GDC fuel electrode under CO2 electrolysis were investigated. The long-term stability test results showed a low degradation rate under the operating conditions of 900 degrees C and 0.5 A/cm2. SEM analysis revealed the agglomeration of Ni particles, an increase in electrode porosity, and Ni migration away from the electrode/electrolyte interface.
JOURNAL OF CO2 UTILIZATION
(2023)
Article
Chemistry, Multidisciplinary
Yucheng Hao, Eike M. Langer, Bin Xiao, Philip Kegler, Xin Cao, Kunhong Hu, Ruediger-A. Eichel, Shuao Wang, Evgeny V. Alekseev
Summary: The study investigated the phase formation in the U-Te-O systems under high-temperature high-pressure conditions and discovered four new inorganic compounds. These compounds demonstrate the high chemical flexibility of the system with different oxidation states of Tellurium and Uranium. The crystal structures of these compounds were discussed, along with the synthetic conditions for preparing single crystalline samples.
FRONTIERS IN CHEMISTRY
(2023)
Review
Chemistry, Physical
Baolin Wu, Chunguang Chen, Luc H. J. Raijmakers, Jin Liu, Dmitri L. Danilov, Peter H. L. Notten
Summary: Li-metal battery systems are attractive for high-energy batteries due to their high theoretical specific capacity and low redox potential. Anode-free Li-metal batteries (AFLBs) have higher energy density and lower production costs. However, challenges in Li-metal reactivity and dendrite-growth prevent commercialization. Homogeneous Li-metal growth and stable SEI are crucial for addressing these issues. Approaches such as electrolyte optimization and artificial layers design have been developed to enhance Li-ion transport and suppress dendrite growth. This review provides an overview of these developments and insights into battery performance mechanisms.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Physical
Katherine E. MacArthur, Shlomi Polani, Malte Klingenhof, Nina Gumbiowski, Tim Moller, Paul Paciok, Jiaqi Kang, Matthias Epple, Shibabrata Basak, Ruediger-A. Eichel, Peter Strasser, Rafal E. Dunin-Borkowski, Marc Heggen
Summary: This study provides a detailed characterization of the morphological and compositional changes of octahedral-shaped PtNi catalysts and doped octahedral PtNi-(Mo) and PtNi-(MoRh) catalysts during thermal annealing. The results show that the octahedral shape of PtNi catalysts gradually changes and undergoes alloying upon heating. However, doping with Mo or Mo/Rh stabilizes the structure and maintains a truncated octahedral shape during heat treatments.
ACS APPLIED ENERGY MATERIALS
(2023)
Review
Electrochemistry
Baolin Wu, Chunguang Chen, Dmitri L. Danilov, Ruediger-A. Eichel, Peter H. L. Notten
Summary: All-solid-state thin film Li-ion batteries (TFLIBs) with extended cycle life, broad temperature operation range, and minimal self-discharge rate are superior to conventional batteries, but face challenges such as interfacial instability, low energy density, and high manufacturing cost.
Article
Nanoscience & Nanotechnology
Xin Lu, Anna Windmueller, Dana Schmidt, Sandro Schoener, Chih-Long Tsai, Hans Kungl, Xunfan Liao, Yiwang Chen, Shicheng Yu, Hermann Tempel, Ruediger-A. Eichel
Summary: A glassy-ceramic Li10GeP2S12 solid electrolyte with high Li-ion conductivity can be produced through a single-step high-energy ball milling method. The as-milled sample exhibits high ionic conductivity at room temperature, and heat treatment can further improve its crystallinity and ionic conductivity.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Verena Theussl, Henning Weinrich, Christine Heume, Krzysztof Dzieciol, Bernhard Schmid, Hans Kungl, Hermann Tempel, Ruediger-A. Eichel
Summary: In order to improve the technical maturity of CO2 electrolysis to formic acid, various gas diffusion layers (GDLs) were investigated for their suitability as a carbon-based substrate for gas diffusion electrodes (GDEs) and their effect on the electroreduction of CO2 to formate. The thickness, hydrophobic treatment, and presence of a microporous layer (MPL) in the GDL were examined for their impact on the Faradaic efficiency of the GDE. The results showed that the GDL thickness had no noticeable effect on the Faradaic efficiency, while a GDE with 10% PTFE hydrophobic treatment performed better than a GDE based on a GDL with 30% PTFE. Furthermore, the presence of an MPL was found to be significantly important in achieving relevant current densities through its effects on catalyst layer focus, wetting, and electrical conductivity on the GDE surface after spray coating.
Review
Chemistry, Physical
Stephanie E. E. Wolf, Franziska E. E. Winterhalder, Vaibhav Vibhu, L. G. J. (Bert) de Haart, Olivier Guillon, Ruediger-A. Eichel, Norbert H. H. Menzler
Summary: Solid Oxide Electrolysis Cells (SOECs) are highly efficient in producing chemicals and fuels from renewable electricity at high temperatures. However, the materials currently used for SOEC systems have been optimized for fuel cell operation, which slows down the technology development. This review discusses the state-of-the-art materials for SOECs, challenges in materials design and degradation, and recent advances in material compositions.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Correction
Chemistry, Physical
Elisabeth Robens, Burkhard Hecker, Hans Kungl, Hermann Tempel, Rudiger A. Eichel
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Sven Jovanovic, Peter Jakes, Steffen Merz, Davis Thomas Daniel, Ruediger-A. Eichel, Josef Granwehr
Summary: The electrolytic reduction of CO2 in aqueous media is a promising method for converting greenhouse gas into base chemicals. Current research is focusing on the importance of the local environment and reactions at the electrodes. In this study, in operando NMR techniques were used to investigate changes in the electrolyte chemistry during CO2 electrolysis. It was found that the dynamic equilibrium of the electrolyte salt affects the resupply rate of CO2 to the reaction. Stable ion pairs in solution were proposed to catalyze the bicarbonate dehydration reaction, potentially providing a new pathway for improving educt resupply during CO2 electrolysis.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Electrochemistry
Shidong Zhang, Shangzhe Yu, Roland Peters, Steven B. Beale, Holger Marschall, Felix Kunz, Ruediger-A. Eichel
Summary: This paper presents a novel coupled region-to-region numerical procedure for electric field potential calculations. It compares the performance of the coupled method with a conventional segregated scheme for simulations of a solid oxide cell. The results show that the coupled method outperforms the segregated scheme, reducing convergence times and improving stability. It can also be applied to heat transfer problems between multiple phases and regions.
ELECTROCHIMICA ACTA
(2023)