Single-Ion Conducting Polymeric Protective Interlayer for Stable Solid Lithium-Metal Batteries

Xinyuan Shan; Sheng Zhao; Mengxiang Ma; Yiyang Pan; Zhenxue Xiao; Bingrui Li; Alexei P Sokolov; Ming Tian; Huabin Yang; Peng-Fei Cao

doi:10.1021/acsami.2c17547

Single-Ion Conducting Polymeric Protective Interlayer for Stable Solid Lithium-Metal Batteries

ACS Appl Mater Interfaces. 2022 Dec 21;14(50):56110-56119. doi: 10.1021/acsami.2c17547. Epub 2022 Dec 9.

Authors

Xinyuan Shan¹, Sheng Zhao², Mengxiang Ma¹, Yiyang Pan³, Zhenxue Xiao¹, Bingrui Li⁴, Alexei P Sokolov^{2

5}, Ming Tian⁶, Huabin Yang^{1

7}, Peng-Fei Cao⁶

Affiliations

¹ Institute of New Energy Material Chemistry, School of Materials Science and Engineering, Nankai University, Tianjin 300350, China.
² Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, United States.
³ School of Chemistry, Beihang University, Beijing 10019, China.
⁴ The Bredesen Center for Interdisciplinary Research and Graduate Education, University of Tennessee, Knoxville, Tennessee 37996, United States.
⁵ Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States.
⁶ State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China.
⁷ Tianjin Key Laboratory of Metal and Molecule Based Material Chemistry, Nankai University, Tianjin 300350, China.

PMID: 36490324
DOI: 10.1021/acsami.2c17547

Abstract

With many reported attempts on fabricating single-ion conducting polymer electrolytes, they still suffer from low ionic conductivity, narrow voltage window, and high cost. Herein, we report an unprecedented approach on improving the cationic transport number (t_Li⁺) of the polymer electrolyte, i.e., single-ion conducting polymeric protective interlayer (SIPPI), which is designed between the conventional polymer electrolyte (PVEC) and Li-metal electrode. Satisfied ionic conductivity (1 mS cm^-1, 30 °C), high t_Li⁺ (0.79), and wide-area voltage stability are realized by coupling the SIPPI with the PVEC electrolyte. Benefiting from this unique design, the Li symmetrical cell with the SIPPI shows stable cycling over 6000 h at 3 mA cm^-2, and the full cell with the SIPPI exhibits stable cycling performance with a capacity retention of 86% over 1000 cycles at 1 C and 25 °C. This incorporated SIPPI on the Li anode presents an alternative strategy for enabling high-energy density, long cycling lifetime, and safe and cost-effective solid-state batteries.

Keywords: Li-metal batteries; polymer electrolyte; polymeric protective interlayer; single-ion conducting; solid-state battery.