journal article·2025-03-14

A Superionic Conductor Lithium Argyrodite Sulfide of Li7–x(GeSi)(1–x)/2SbxS5I toward All-Solid-State Lithium-Ion Batteries

Yuxin Ma, Daokuan Jin, Haodong Shi, Rui Li, Yutao Niu, Yunyun Xu, Cong Dong, Yangyang Liu, Rui Yang, Guiming Zhong, Chunyang Wang, Zhizhen Zhang, Zhangquan Peng, Zhong-Shuai Wu

ACS Energy Letters· Volume 10· Issue 3
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Abstract

Li 6 PS 5 I based solid-state electrolytes (SSEs) show promising interface compatibility for all-solid-state batteries (ASSBs), but they still suffer from limited ionic conductivity. Herein, a superionic conductor lithium argyrodite sulfide, Li 7– x (GeSi) (1– x )/2 Sb x S 5 I, was developed through multi-cation substitution of Ge, Si, and Sb for P, increasing configurational entropy of the Li 6 PS 5 I. This approach enhanced Li + content and anion site disorder, leading to a low activation energy of 0.17 eV for Li + migration, and consequently a high cold-pressed ionic conductivity of 12.7 mS cm –1, and a record value of 32.2 mS cm –1 after hot-pressing. When incorporating Li 3 InCl 6 as the catholyte and interlayer, the LiNi 0.8 Co 0.1 Mn 0.1 O 2 @Li 3 InCl 6 |Li 3 InCl 6 |Li 20/3 (GeSiSb) 1/3 S 5 I|Li-In ASSBs exhibited a high capacity of 219 mAh g –1 at 0.1 C, and a notable capacity of 135 mAh g –1 with 84.4% retention at 1 C after 550 cycles. Our ASSBs demonstrated stable cycling across −20 to 60 °C and operated well at an ultrahigh cathode loading of 100 mg cm –2 . These findings advance sulfide SSEs for high-performance and wide-temperature ASSBs.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Solid-state spectroscopy and crystallography

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Affiliations

State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, Liaoning, China

University of Chinese Academy of Sciences, 19 A Yuquan Road, Shijingshan District, Beijing 100049, China

State Key Laboratory of Heavy Oil Processing, Institute of New Energy, College of Chemistry and Chemical Engineering

China University of Petroleum (East China)

School of Materials

Sun Yat-sen University

Shenyang National Laboratory for Materials Science

Institute of Metal Research, Chinese Academy of Sciences

Dalian National Laboratory for Clean Energy, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, Liaoning, China

Funding

National Key Research and Development Program of China · Dalian Institute of Chemical Physics, Chinese Academy of Sciences · Natural Science Foundation of Liaoning Province · Dalian High-Level Talent Innovation Program · National Natural Science Foundation of China · State Key Laboratory of Catalysis · Yulin Innovation Institute of Clean Energy

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