Article
Chemistry, Physical
Taotao Cai, Zijun Hu, Yingjie Gao, Gaofeng Li, Zhiping Song
Summary: A novel and low-cost MOF based on the coordination between Fe3+ and 2,5-dihydroxybenzoquinone (DHBQ) ligand was successfully synthesized, which exhibited high energy density, outstanding electronic conductivity, and applicability to both Li and Na batteries.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Atin Pramanik, Alexis G. Manche, Moulay Tahar Sougrati, Alan V. Chadwick, Philip Lightfoot, A. Rober t Armstrong
Summary: Developing multielectron redox-active cathode materials is crucial for achieving high energy density and long cycle life in next-generation secondary battery applications. Triggering anion redox activity is a promising strategy to enhance the energy density of polyanionic cathodes for Li/Na-ion batteries. In this study, K2Fe(C2O4)2 is identified as a promising cathode material that combines metal redox activity with oxalate anion (C2O42-) redox. It exhibits specific discharge capacities of 116 and 60 mAh g-1 for sodium-ion batteries (NIB) and lithium-ion batteries (LIB) cathode applications, respectively, at a rate of 10 mA g-1, with excellent cycling stability. The experimental results are supported by density functional theory (DFT) calculations of the average atomic charges.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Analytical
Xishan Zhao, De-An Zhang, Chuxiao Sun, Jiajun Liu, Tianming Zhao, Meng Wang, Yutong Song, Haowen Xu, Qi Wang
Summary: In this study, hollow S/FeS2@CNTs microspheres were synthesized by loading sulfur into hollow FeS2 microspheres with carbon nanotubes. The resulting cathode material for lithium-sulfur batteries exhibited high initial discharge capacity and excellent long-term cycling performance.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Jiuli Chang, Wenfang Liang, Wenyu Wang, Dapeng Wu, Kai Jiang, Gongke Wang, Fang Xu, Zhiyong Gao
Summary: In this study, oxygen vacancy-enriched Bi2O3 was prepared as the negative material for aqueous alkaline batteries, improving the energy and power densities of the batteries and demonstrating the potential of oxygen vacancy-enriched Bi2O3 in battery-type energy storage.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Qianqian Fan, Yubing Si, Fulong Zhu, Wei Guo, Yongzhu Fu
Summary: A study shows that the activation of lithium sulfide (Li2S) can be improved by using organochalcogenide-based redox mediators, such as phenyl ditelluride (PDTe), which reduces the activation energy barrier and enhances the charge-discharge performance of Li2S in batteries, making it more suitable for commercialization.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Electrochemistry
Florent Mohimont, Ronan Le Ruyet, Reza Younesi, Andrew J. J. Naylor
Summary: Alloy electrodes with high energy density are gaining interest in the field of Li-ion batteries, but they suffer from rapid pulverization and disconnection due to large volume changes. Ga-based liquid alloys, such as galinstan, have been studied as self-healing electrodes due to their ability to store Li and remain in a liquid state at room temperature. However, the lithiation mechanism and practical capacity of galinstan are still unknown. This study used electrochemical measurements, XRD, and SEM analyses to investigate the redox processes and structural properties of galinstan as an electrode material.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Alice J. Merryweather, Quentin Jacquet, Steffen P. Emge, Christoph Schnedermann, Akshay Rao, Clare P. Grey
Summary: Understanding the ion intercalation and degradation mechanisms is crucial for developing high-rate battery electrodes. Operando optical scattering microscopy is used to study single-particle kinetic state-of-charge heterogeneities and cracking in high-rate Li-ion anode materials. This study demonstrates the power of optical scattering microscopy in tracking rapid non-equilibrium processes that would be inaccessible with established characterization techniques.
Article
Nanoscience & Nanotechnology
Ji Hyun Han, Kyu Hang Shin, Yun Jung Lee
Summary: A freestanding cellulose acetate-carbon nanotube (CA-CNT) film electrode was introduced for highly flexible, high-energy lithium-ion batteries (LIBs), with straightforward washing removing CA while sustaining the fibrous CNT network. The large-scale production potential of the film electrode was highlighted, along with the superior electrochemical performance and high flexibility achieved even at high active material loading. By stacking six sheets of the freestanding film electrode, a high capacity of 5.4 mA h cm(-2) was demonstrated, showcasing stable operation under extreme deformation and the potential for wearable gear applications.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Physical
Jia-Jun Han, Ao-Ran Guo, Yan-Fang Wang
Summary: PANI/LFP composites were successfully prepared through synthesis and structural control, exhibiting excellent electrochemical performance and higher energy storage capacity compared to pure LFP materials. This is of great significance for the development of battery technology.
Article
Chemistry, Physical
Hongmin Wang, Shuting Fu, Chungseok Choi, Yiren Zhong, Samuel Schaefer
Summary: This study explores the potential of directly utilizing electrochemically active natural mineral pyrrhotite as electrode materials for energy storage. The cycling-instability mechanism of pyrrhotite is discovered, and by controlling carbon addition and voltage window, the stability is improved, overcoming rapid capacity fading. The optimized pyrrhotite/C electrode shows promising initial capacity and retains a high percentage of capacity after 100 cycles.
ENERGY STORAGE MATERIALS
(2023)
Article
Green & Sustainable Science & Technology
Dan Zhan, Xiaoqing Yuan, Cuili Xiang, Jun Lu, Gaopeng Dai, Ruofei Hu, Zuoan Xiao, Haiyan Mao, Marcus Fehse, Andre J. Simpson, Bing Wu
Summary: The study successfully prepared a carbon fiber/MnO/C composite material using cotton and pyrrole as raw materials, demonstrating excellent electrochemical performance attributed to its unique structure. The composite material maintained high discharge capacity, exhibited superior rate capability and long-term cycle stability compared to MnO/C and MnO.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2021)
Article
Materials Science, Multidisciplinary
Eva Gerold, Reinhard Lerchbammer, Helmut Antrekowitsch
Summary: The need to recover critical elements from lithium-ion batteries is crucial, and adapting the hydrometallurgical recycling processes is necessary due to the development of cathode materials and the search for cheaper alternatives. By optimizing the leaching process, an effective way of recovering lithium from different cathode materials has been identified.
Article
Chemistry, Physical
Jiahui Xu, Alain C. Ngandjong, Chaoyue Liu, Franco M. Zanotto, Oier Arcelus, Arnaud Demortiere, Alejandro A. Franco
Summary: The demand for lithium ion batteries (LIBs) is increasing and the development of digital twins to optimize LIB manufacturing processes is essential. A new three-dimensional physics-based modeling workflow is able to predict the influence of manufacturing parameters on electrode microstructure, providing more accurate simulation results through the use of Coarse-Grained Molecular Dynamics.
JOURNAL OF POWER SOURCES
(2023)
Article
Energy & Fuels
Jintao Jia, Longping Deng, Huajian Shentu, Mengmeng Wang, Ya-Jun Cheng, Xiuxia Zuo, Jie Gao, Yonggao Xia
Summary: This research proposes a new, sustainable, and easy-to-implement process for the recycling of spent LiFePO4 cathode powder. The 732 cation exchange resin is used as a leaching agent and an adsorbent to recover Li and Fe from the waste powder. The results show that it is technically and economically feasible to use the 732 cation exchange resin for recovery, and high-purity products can be obtained.
Article
Engineering, Mechanical
R. Vijay, B. Surya Rajan, K. Sathickbasha, P. Hariharasakthisudhan, D. Lenin Singaravelu, S. Manoharan, P. Balaji, A. B. Mohamed Ashfaq Ahmed, P. Baskara Sethupathi
Summary: The use of metal sulfide coated steel fibers can improve the wear resistance of brake pads and create a mixed mode of wear mechanism.
TRIBOLOGY INTERNATIONAL
(2022)
Article
Chemistry, Physical
Takuya Kimura, Takumi Nakano, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi
Summary: All-solid-state batteries have potential as energy storage devices due to their high safety and energy density. Sulfide-based solid electrolytes, although they have high ionic conductivities and ductility, are sensitive to moisture. Li4SnS4 electrolytes can mitigate these weaknesses by suppressing the evolution of H2S gas in a humid environment. The mechanism behind this suppression was investigated and it was found that the formation of stable hydrates plays a role. These findings will contribute to the design of moisture-resistant sulfide materials.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Nanoscience & Nanotechnology
Taichi Asakura, Takeaki Inaoka, Chie Hotehama, Hiroe Kowada, Kota Motohashi, Atsushi Sakuda, Masahiro Tatsumisago, Akitoshi Hayashi
Summary: The operating conditions of sulfide-based all-solid-state Li/S batteries were studied to suppress the formation of voids. It was found that using Li-Mg alloy electrodes can improve the cycling stability of the batteries and allow them to operate at high current densities.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Yusuke Morino, Hikaru Sano, Akihiro Shiota, Koji Kawamoto, Tsukasa Takahashi, Norihiko Miyashita, Atsushi Sakuda, Akitoshi Hayashi
Summary: All-solid-state batteries (ASSBs) using sulfide solid electrolytes (SEs) have longer lifetimes than liquid-type lithium-ion batteries (LIBs) using organic solvents. However, the influence of exposure to moisture on the durability of ASSB cell performance is not fully understood. In this study, the investigation of moisture's influence on the durability of an ASSB positive electrode with sulfide SE exposed to dry-room-simulated air was conducted, and a characteristic degradation mode was observed.
Article
Electrochemistry
Hikaru Sano, Yusuke Morino, Yasuyuki Matsumura, Koji Kawamoto, Hiroyuki Higuchi, Noriyuki Yamamoto, Atsunori Matsuda, Hirofumi Tsukasaki, Shigeo Mori, Atsush Sakuda, Akitoshi Hayashi
Summary: This study examines the stability of Li3PS4-LiI glass ceramic (LPSI) under low-humidity conditions and found that exposure to dry air at -20 degrees C resulted in low H2S gas generation and reduced ionic conductivity. Vacuum heating can recover most of the conductivity, indicating that H2S generation is not the main reason for the conductivity reduction. It is suggested that water molecules on the LPSI powder particles after dry-air exposure lead to the formation of a degraded LPSI layer and low ionic conductivity.
Article
Chemistry, Inorganic & Nuclear
Hamdi Ben Yahia, Kota Motohashi, Atsushi Sakuda, Akitoshi Hayashi
Summary: A new binary sodium magnesium sulfide (Na6MgS4) was synthesized by mechanochemical synthesis from Na2S and MgS. Na6MgS4 is highly sensitive to oxygen traces and partially decomposes. Excess MgS was used in the milling process to successfully reduce the impurity ratio from 38% (Na2S + MgO) to 13% MgO. The crystal structure and properties of Na6MgS4 were characterized by various techniques, and it was found to be isostructural to Na6ZnO4. Additionally, indium-doped samples (Na6-x Mg1-x In x S4) with improved ionic conductivities were prepared.
INORGANIC CHEMISTRY
(2023)
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.
Article
Chemistry, Physical
Yusuke Morino, Hikaru Sano, Koji Kawamoto, Ken-ichi Fukui, Masato Takeuchi, Atsushi Sakuda, Akitoshi Hayashi
Summary: Sulfide-based solid electrolytes are promising for solid-state lithium batteries due to their high ionic conductivities, suitable mechanical properties, and wide electrochemical windows. However, the hygroscopic nature of sulfide in these materials leads to the generation of toxic H2S gas upon reacting with water, which reduces the lithium-ion conductivity. On the other hand, it has been observed that conducting performance can be partially recovered through suitable heat treatment. This study employed multiple spectroscopic analyses to investigate the degradation and recovery mechanisms of a sulfide solid electrolyte under moisture exposure and vacuum heat treatment.
SOLID STATE IONICS
(2023)
Article
Materials Science, Multidisciplinary
Hiroki Yamada, Koji Ohara, Satoshi Hiroi, Atsushi Sakuda, Kazutaka Ikeda, Takahiro Ohkubo, Kengo Nakada, Hirofumi Tsukasaki, Hiroshi Nakajima, Laszlo Temleitner, Laszlo Pusztai, Shunsuke Ariga, Aoto Matsuo, Jiong Ding, Takumi Nakano, Takuya Kimura, Ryo Kobayashi, Takeshi Usuki, Shuta Tahara, Koji Amezawa, Yoshitaka Tateyama, Shigeo Mori, Akitoshi Hayashi
Summary: Controlling Li ion transport in glasses is crucial for developing all-solid-state batteries. Li3PS4 glass, a solid electrolyte candidate, shows a dynamic coupling effect between Li+ cation mobility and PS43- anion libration, known as the paddlewheel effect. Additionally, it exhibits a coordinated cation diffusion effect (cation-cation interactions) that enhances Li ion transport. The correlation between Li+ ions in the glass structure can be determined by evaluating their valence oscillations, providing insights for the development of new solid electrolytes.
ENERGY & ENVIRONMENTAL MATERIALS
(2023)
Article
Electrochemistry
Atsushi Sakuda
Summary: Lithium/transition-metal polysulfide batteries are promising candidates for next-generation high-energy density batteries, with large reversible capacities and multi-electron reaction characteristics. This comprehensive paper introduces the concept, research, and development of transition metal polysulfide electrode active materials, and summarizes the author's perspectives on this concept. Additionally, the diversity of coordination structures and unique structural changes during charging and discharging are discussed.
Article
Chemistry, Physical
Yusuke Morino, Hikaru Sano, Shunsuke Kawaguchi, Satoshi Hori, Atsushi Sakuda, Tsukasa Takahashi, Norihiko Miyashita, Akitoshi Hayashi, Ryoji Kanno
Summary: Sulfide-based solid electrolytes have attracted attention for solid-state lithium batteries due to their high ionic conductivities and suitable mechanical properties. However, sulfides react with moisture to generate toxic gas, which leads to the degradation of lithium ionic conductivity. In this study, impedance spectroscopy measurements were conducted to investigate the effect of moisture degradation on solid electrolyte particles. It was found that the impedance and activation energy of the grain boundaries between the particles increased, which inhibited lithium ionic conduction.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yushi Fujita, Takuya Kimura, Minako Deguchi, Kota Motohashi, Atsushi Sakuda, Masahiro Tatsumisago, Hirofumi Tsukasaki, Shigeo Mori, Kazutaka Ikeda, Koji Ohara, Naoaki Kuwata, Koji Amezawa, Akitoshi Hayashi
Summary: All-solid-state lithium-ion batteries with flame-retardant inorganic solid electrolytes have great potential due to their high safety. Oxide-based solid electrolytes with high chemical stability and lithium-ion conductivity are attractive, and the development of new oxide-based solid electrolytes with high ionic conductivity and ductility is crucial for improving the overall performance of all-solid-state batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Kentaro Yamamoto, Yao Xiao, Toshiki Watanabe, Atsushi Sakuda, Masakuni Takahashi, Wenli Pan, Koji Nakanishi, Toshiyuki Matsunaga, Masayuki Uesugi, Akihisa Takeuchi, Kentaro Uesugi, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto
Summary: The Li2S-V2S3-LiI cathode materials doped with different amounts of LiI showed high charge/discharge capacity without solid electrolyte and carbon in the composite electrode. The ionic conductivity of the Li2S-V2S3-LiI cathodes during charging was significantly increased with LiI doping amounts above 10 mol %. The formation of a LiI-rich domain during charging improved the electrochemical performance of the cathode materials. This material design strategy is useful for designing high packing density electrodes for all-solid-state batteries.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Yusuke Morino, Hikaru Sano, Tsukasa Takahashi, Norihiko Miyashita, Atsushi Sakuda, Akitoshi Hayashi
Summary: Sulfide-based solid electrolytes (SEs) in all-solid-state lithium-ion batteries have attracted much attention due to their high lithium ionic conductivity, plasticity, and thermal stability. However, the generation of toxic hydrogen sulfide (H2S) gas upon moisture exposure is a major issue with SEs. This study investigated the degradation mechanism and surface state of moisture-exposed sulfide-based SEs at the molecular and atomic levels. The results revealed the presence of surface hydrogen components such as LiOH, LiOH·xH2O, thiol groups, and unreacted H2O cluster adsorbates.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jiong Ding, Yushi Fujita, Hirofumi Tsukasaki, Hiroshi Nakajima, Atsushi Sakuda, Akitoshi Hayashi, Shigeo Mori
Summary: All-solid-state rechargeable batteries with Li2S-based positive electrode active materials have attracted much attention. The microstructural changes of Li2S-based positive electrode were investigated using transmission electron microscopy, and reversible structural changes and the role of nanocrystals were discovered.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Wenli Pan, Kentaro Yamamoto, Nobuya Machida, Toshiyuki Matsunaga, Mukesh Kumar, Neha Thakur, Toshiki Watanabe, Atsushi Sakuda, Akitoshi Hayashi, Masahiro Tatsumisago, Yoshiharu Uchimoto
Summary: Li2S is a promising cathode candidate for solid-state batteries, but its ionically insulating nature poses challenges. This study improves the intrinsic conductivity of Li2S by doping with PI3, resulting in a cathode material with high energy density and good rate performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
