Grain Boundary Electronic Insulation for High-Performance All-Solid-State Lithium Batteries

Xiaofei Yang; Xuejie Gao; Ming Jiang; Jing Luo; Jitong Yan; Jiamin Fu; Hui Duan; Shangqian Zhao; Yongfu Tang; Rong Yang; Ruying Li; Jiantao Wang; Huan Huang; Chandra Veer Singh; Xueliang Sun

doi:10.1002/anie.202215680

Grain Boundary Electronic Insulation for High-Performance All-Solid-State Lithium Batteries

Angew Chem Int Ed Engl. 2023 Jan 26;62(5):e202215680. doi: 10.1002/anie.202215680. Epub 2022 Dec 22.

Authors

Xiaofei Yang¹, Xuejie Gao^{1

2}, Ming Jiang³, Jing Luo¹, Jitong Yan⁴, Jiamin Fu¹, Hui Duan¹, Shangqian Zhao⁵, Yongfu Tang⁴, Rong Yang⁵, Ruying Li¹, Jiantao Wang⁵, Huan Huang⁶, Chandra Veer Singh⁷, Xueliang Sun¹

Affiliations

¹ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9, Canada.
² Liaoning Key Laboratory of Lignocellulose Chemistry and BioMaterials, College of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034, China.
³ Institute of Physical Science and Information Technology, Anhui University, Hefei, 230601, China.
⁴ Hebei Key Laboratory of Applied Chemistry, School of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China.
⁵ China Automotive Battery Research Institute, Beijing, 100088, China.
⁶ Glabat Solid-State Battery Inc., 700 Collip Circle, London, ON, N6G 4X8, Canada.
⁷ Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, M5S 3E4, Canada.

PMID: 36446742
DOI: 10.1002/anie.202215680

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.

Keywords: All-Solid-State Lithium Batteries; Grain Boundaries; Humidity Stability; Lithium Dendrite; Self-Discharging.

Abstract

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