Crosslinked solubilizer enables nitrate-enriched carbonate polymer electrolytes for stable, high-voltage lithium metal batteries

Chuyang Jing; Kuan Dai; Dong Liu; Wenran Wang; Libao Chen; Chunxiao Zhang; Weifeng Wei

doi:10.1016/j.scib.2023.11.039

Crosslinked solubilizer enables nitrate-enriched carbonate polymer electrolytes for stable, high-voltage lithium metal batteries

Sci Bull (Beijing). 2024 Jan 30;69(2):209-217. doi: 10.1016/j.scib.2023.11.039. Epub 2023 Nov 21.

Authors

Chuyang Jing¹, Kuan Dai², Dong Liu¹, Wenran Wang¹, Libao Chen¹, Chunxiao Zhang³, Weifeng Wei⁴

Affiliations

¹ State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China.
² College of Materials and Chemical Engineering, Hunan Institute of Engineering, Xiangtan 411104, China.
³ State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China. Electronic address: chunxiaozhang@csu.edu.cn.
⁴ State Key Laboratory of Powder Metallurgy, Central South University, Changsha 410083, China. Electronic address: weifengwei@csu.edu.cn.

PMID: 38007330
DOI: 10.1016/j.scib.2023.11.039

Abstract

High-voltage lithium metal batteries (LMBs) have been considered promising next-generation high-energy-density batteries. However, commercial carbonate electrolytes can scarcely be employed in LMBs owing to their poor compatibility with metallic lithium. N,N-dimethylacrylamide (DMAA)-a crosslinkable solubilizer with a high Gutmann donor number-is employed to facilitate the dissolution of insoluble lithium nitrate (LiNO₃) in carbonate-based electrolytes and to form gel polymer electrolytes (GPEs) through in situ polymerization. The Li⁺ solvation structure of the GPEs is regulated using LiNO₃ and DMAA, which suppresses the decomposition of LiPF₆ and facilitates the formation of an inorganic-rich solid electrolyte interface. Consequently, the Coulombic efficiency (CE) of the Li||Cu cell assembled with a GPE increases to 98.5% at room temperature, and the high-voltage Li||NCM622 cell achieves a capacity retention of 80.1% with a high CE of 99.5% after 400 cycles. The bifunctional polymer electrolytes are anticipated to pave the way for next-generation high-voltage LMBs.

Keywords: Carbonate electrolytes; Crosslinked solubilizer; Gel polymer electrolytes; Lithium metal batteries; Lithium nitrate.