Li-Rich Antiperovskite/Nitrile Butadiene Rubber Composite Electrolyte for Sheet-Type Solid-State Lithium Metal Battery

Juncao Bian; Huimin Yuan; Muqing Li; Sifan Ling; Bei Deng; Wen Luo; Xuedan Chen; Lihong Yin; Shuai Li; Long Kong; Ruo Zhao; Haibin Lin; Wei Xia; Yusheng Zhao; Zhouguang Lu

doi:10.3389/fchem.2021.744417

Li-Rich Antiperovskite/Nitrile Butadiene Rubber Composite Electrolyte for Sheet-Type Solid-State Lithium Metal Battery

Front Chem. 2021 Nov 15:9:744417. doi: 10.3389/fchem.2021.744417. eCollection 2021.

Authors

Juncao Bian^{1

2

3}, Huimin Yuan⁴, Muqing Li⁴, Sifan Ling⁵, Bei Deng⁵, Wen Luo⁴, Xuedan Chen^{1

2

3

5}, Lihong Yin^{1

2

3

5}, Shuai Li^{1

2

3

5}, Long Kong^{1

2

3}, Ruo Zhao^{1

2

3}, Haibin Lin^{1

2

3}, Wei Xia^{1

2

3}, Yusheng Zhao^{1

2

3

5}, Zhouguang Lu⁴

Affiliations

¹ Shenzhen Key Laboratory of Solid State Batteries, Academy for Advanced Interdisciplinary Studies, Southern University of Science and Technology (SUSTech), Shenzhen, China.
² Guangdong Provincial Key Laboratory of Energy Materials for Electric Power, Academy for Advanced Interdisciplinary Studies, SUSTech, Shenzhen, China.
³ Guangdong-Hong Kong-Macao Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Academy for Advanced Interdisciplinary Studies, SUSTech, Shenzhen, China.
⁴ Department of Materials Science and Engineering, SUSTech, Shenzhen, China.
⁵ Department of Physics, SUSTech, Shenzhen, China.

Abstract

Lithium-rich antiperovskites (LiRAPs) hold great promise to be the choice of solid-state electrolytes (SSEs) owing to their high ionic conductivity, low activation energy, and low cost. However, processing sheet-type solid-state Li metal batteries (SSLiB) with LiRAPs remains challenging due to the lack of robust techniques for battery processing. Herein, we propose a scalable slurry-based procedure to prepare a flexible composite electrolyte (CPE), in which LiRAP (e.g., Li₂OHCl_0.5Br_0.5, LOCB) and nitrile butadiene rubber (NBR) serve as an active filler and as a polymer scaffold, respectively. The low-polar solvent helps to stabilize the LiRAP phase during slurry processing. It is found that the addition of LOCB into the NBR polymer enhances the Li ion conductivity for 2.3 times at 60°C and reduces the activation energy (max. 0.07 eV). The as-prepared LOCB/NBR CPE film exhibits an improved critical current of 0.4 mA cm^-2 and can stably cycle for over 1000 h at 0.04 mA cm^-2 under 60°C. In the SSLiB with the sheet-type configuration of LiFePO₄(LFP)||LOCB/NBR CPE||Li, LFP exhibits a capacity of 137 mAh/g under 60 at 0.1°C. This work delivers an effective strategy for fabrication of LiRAP-based CPE film, advancing the LiRAP-family SSEs toward practical applications.

Keywords: anti-perovskite; composite electrolyte; sheet-type; solid-state batteries; solid-state electrolyte.