journal article·2022-08-12

Local Li+ Framework Regulation of a Garnet-Type Solid-State Electrolyte

Furong Sun, Yubo Yang, Shu Zhao, Yongtao Wang, Mingxue Tang, Qingzhen Huang, Yang Ren, Heng Su, Boya Wang, Ning Zhao, Xiangxin Guo, Haijun Yu

ACS Energy Letters· Volume 7· Issue 8
Publisher page

Abstract

Garnet-type solid-state electrolytes Li7La3Zr2O12 (LLZO) for high-energy-density batteries have attracted extensive attention. However, stabilizing the high-conductive cubic phase and improving its ionic conductivity remain challenges of current research. Here, a Ca–W dual-substitution strategy has been designed, and the effect of doping on cubic phase formation and Li+ mobility has been investigated thoroughly. The results indicated that the partial substitution of Ca2+ at the La3+ site and W6+ at the Zr4+ site can effectively stabilize the cubic phase while reducing the endothermic enthalpy during the synthesis. Moreover, Ca–W dual substitution regulates the local Li+ framework by increasing Li+ occupancy at the 96h site, which can significantly lower the Li+ migration barrier and thus improve the ionic conductivity by two orders of magnitude. This work addresses the challenge of stabilizing a highly conductive cubic phase with low-energy consumption and represents a major breakthrough in understanding how to improve the ionic conductivity by regulating local structures.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced battery technologies research

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

Affiliations

Institute of Advanced Battery Materials and Devices, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, P. R. China

Key Laboratory of Advanced Functional Materials, Ministry of Education, Beijing University of Technology, Beijing 100124, P. R. China

Center for High Pressure Science & Technology Advanced Research, Beijing 100094, P. R. China

NIST Center for Neutron Research, National Institute of Standards and Technology, Gaithersburg, Maryland 20899, United States

X-ray Science Division, Argonne National Laboratory, 9700 S. Cass Avenue, Lemont, Illinois 60439, United States

Department of Physics, City University of Hong Kong, Kowloon, Hong Kong, P. R. China

College of Physics, Qingdao University, Qingdao 266071, P. R. China

Funding

Natural Science Foundation of Beijing Municipality · National Natural Science Foundation of China

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