全固体リチウムイオン電池の性能を向上させる新固体電解質を開発（Novel Solid-state Electrolyte Developed to Enhance Performance of All-solid-state Lithium-ion Batteries）

2025-03-13 中国科学院（CAS）

＜関連情報＞

• https://english.cas.cn/newsroom/research_news/chem/202503/t20250314_903868.shtml
• https://pubs.acs.org/doi/10.1021/acsenergylett.4c03115

Li7-x(GeSi)(1-x)/2 SbxS5Iの全固体リチウムイオン電池に向けた超イオン伝導性リチウムアルグロダイト硫化物 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  Published: February 25, 2025
DOI:https://doi.org/10.1021/acsenergylett.4c03115

Abstract

Li₆PS₅I 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)/2Sb_xS₅I, was developed through multi-cation substitution of Ge, Si, and Sb for P, increasing configurational entropy of the Li₆PS₅I. 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 Li₃InCl₆ as the catholyte and interlayer, the LiNi_0.8Co_0.1Mn_0.1O₂@Li₃InCl₆|Li₃InCl₆|Li_20/3(GeSiSb)_1/3S₅I|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.