DataVXACS Applied Materials & InterfacesPaper
journal article·2023-06-28

Origin of the Seriously Limited Anionic Redox Reaction of Li-Rich Cathodes in Sulfide All-Solid-State Batteries

Yuan Yang, Naifang Hu, Yu-Han Zhang, Yue Zheng, Zhiwei Hu, Chang-Yang Kuo, Hong-Ji Lin, Chien-Te Chen, Ting-Shan Chan, Cheng-Wei Kao, Yongcheng Jin, Jun Ma, Guanglei Cui

ACS Applied Materials & Interfaces· Volume 15· Issue 25
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Source abstract

Abstract

Li-rich layered oxide (LLO) cathode materials with mixed cationic and anionic redox reactions display much higher specific capacity than other traditional layered oxide materials. However, the practical specific capacity of LLO during the first cycle in sulfide all-solid-state lithium-ion batteries (ASSLBs) is extremely low. Herein, the capacity contribution of each redox reaction in LLO during the first charging process is qualitatively and quantitatively analyzed by comprehensive electrochemical and structural measurements. The results demonstrate that the cationic redox of the LiTMO 2 (TM = Ni, Co, Mn) phase is almost complete, while the anionic redox of the Li 2 MnO 3 phase is seriously limited due to the sluggish transport kinetics and severe LLO/Li 6 PS 5 Cl interface reaction at high voltage. Therefore, the poor intrinsic conductivity and interface stability during the anionic redox jointly restrict the capacity release or delithiation/lithiation degree of LLO during the first cycle in sulfide ASSLBs. This study reveals the origin of the seriously limited anionic redox reaction in LLO, providing valuable guidance for the bulk and interface design of high-energy-density ASSLBs.
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Research context

Energy storage

OpenAlex topics: Advancements in Battery Materials · Advanced Battery Materials and Technologies · Advanced Battery Technologies Research

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Materials Science and Engineering, Ocean University of China, Qingdao 266100, P. R. China

Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, P. R. China

School of Future Technology, University of Chinese Academy of Sciences, Beijing 100049, P. R. China

Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden D-01187, Germany

National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan, Republic of China

Department of Electrophysics, National Chiao Tung University, Hsinchu 30010, Taiwan, Republic of China

Shandong Energy Institute, Qingdao 266101, P. R. China

Funding

Youth Innovation Promotion Association of the Chinese Academy of Sciences · Major Scientific and Technological Innovation Project of Shandong Province · National Natural Science Foundation of China · Natural Science Foundation of Shandong Province · Chinese Academy of Sciences · Qingdao New Energy Shandong Laboratory · Shandong Energy Institute · Max Planck-POSTECH Hsinchu Center for Complex Phase Materials

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