Grain Boundary Electronic Insulation for High‐Performance All‐Solid‐State Lithium Batteries. Issue 5 (22nd December 2022)

• Record Type: Journal Article
• Authors: Yang, Xiaofei; Gao, Xuejie; Jiang, Ming; Luo, Jing; Yan, Jitong; Fu, Jiamin; Duan, Hui; Zhao, Shangqian; Tang, Yongfu; Yang, Rong; Li, Ruying; Wang, Jiantao; Huang, Huan; Veer Singh, Chandra; Sun, Xueliang
• Is Part Of: Angewandte Chemie international edition. Volume 62:Issue 5(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2022-12-22
• Subjects: All-Solid-State Lithium Batteries -- Grain Boundaries -- Humidity Stability -- Lithium Dendrite -- Self-Discharging; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202215680
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Sulfide electrolytes with high ionic conductivities are one of the most highly sought for all‐solid‐state lithium batteries (ASSLBs). However, the non‐negligible electronic conductivities of sulfide electrolytes (≈10 −8 S cm −1 ) lead to electron smooth transport through the sulfide electrolyte pellets, resulting in Li dendrite directly depositing at the grain boundaries (GBs) and serious self‐discharge. Here, a grain‐boundary electronic insulation (GBEI) strategy is proposed to block electron transport across the GBs, enabling Li−Li symmetric cells with 30 times longer cycling life and Li−LiCoO2 full cells with three times lower self‐discharging rate than pristine sulfide electrolytes. The Li−LiCoO2 ASSLBs deliver high capacity retention of 80 % at 650 cycles and stable cycling performance for over 2600 cycles at 0.5 mA cm −2 . The innovation of the GBEI strategy provides a new direction to pursue high‐performance ASSLBs via tailoring the electronic conductivity. Abstract : A grain boundary electronic insulation strategy is proposed to tolerate the electronic conductivity of sulfide electrodes at the grain boundaries, which realizes dendrite‐ and self‐discharge‐free and humidity‐stable all‐solid‐state lithium batteries.