journal article·2024-03-08

Superionic Conductivity Invoked by Enhanced Correlation Migration in Lithium Halides Solid Electrolytes

Rui Li, Pushun Lu, Xinmiao Liang, Liwei Liu, Maxim Avdeev, Zhi Deng, Shuai Li, Kaiqi Xu, Jiwen Feng, Rui Si, Fan Wu, Zhizhen Zhang, Yong-Sheng Hu

ACS Energy Letters· Volume 9· Issue 3
Publisher page

Abstract

Lithium halides are experiencing reflorescence as a promising solid electrolyte in all-solid-state batteries (ASSBs) owing to their moderate conductivities and high oxidation potential. Herein we report new lithium-superionic chlorides, Li 3– x Sc 1– x Zr x Cl 6 and Li 3– x Sc 1– x Hf x Cl 6 ( x = 0.25, 0.50, 0.625, 0.75), that demonstrate high ionic conductivities up to 2.2 mS cm –1 at room temperature coupled with low activation energy barriers (0.31 and 0.33 eV for Zr and Hf-analogy, respectively). This notably improved conductivity upon Zr 4+ /Hf 4+ substitution is ascribed to the decreased energy barrier along the c axis and enhanced correlated migration invoked by the tuned Li + /vacancy concentration. Evaluation in solid-state cells further confirmed the potential of this electrolyte to be used in high voltage ASSBs. Our work elucidates the impact of tuned cationic/vacancy concentration and consequently enhanced correlated migration on cationic conductivity. This strategy can be extended to other systems and serve as a guideline for the design of fast ion conductors.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Thermal Expansion and Ionic Conductivity · Advancements in Battery Materials

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

Affiliations

School of Materials, Shenzhen Campus of Sun Yat-Sen University, Shenzhen 518107, Guangdong, P. R. China

School of Materials, Sun Yat-Sen University, Guangzhou 510006, P. R. China

Beijing Advanced Innovation Center for Materials Genome Engineering, Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, P. R. China

School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100190, P. R. China

Innovation Academy for Precision Measurement Science and Technology, Wuhan Institute of Physics and Mathematics, Chinese Academy of Sciences, Wuhan 430071, P. R. China

Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC, NSW 2232, Australia

Department of Physics and Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology, Shenzhen 518055, P. R. China

China Southern Power Grid Technology Co. Ltd., Guangzhou 510080, P. R. China

Yangtze River Delta Physics Research Center, Liyang, Jiangsu 213300, P. R. China

Nano Science and Technology Institute, University of Science and Technology of China, Suzhou 215123, P. R. China

CASOL Energy Co Ltd., Liyang, Jiangsu 213300, China

21C Innovation Laboratory, Contemporary Amperex Technology Ltd. (21C LAB), Ningde, Fujian 352100, P. R. China

Funding

Guangdong Provincial Department of Science and Technology · Contemporary Amperex Technology · National Key Research and Development Program of China · Science and Technology Foundation of Shenzhen City · Shenzhen Fundamental Research Program

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