Interfacial Catalysis Strategy for High‐Performance Solid‐State Lithium Metal Batteries

• Published in: Advanced energy materials 2024-10, Vol.14 (39), p.n/a
• Main Authors: Yang, Li, Zhang, Hong, Xu, Hantao, Peng, Wei, Wu, Lu, Cheng, Yu, Liu, Yuheng, Xu, Lin, Mai, Liqiang
• Format: Article
• Language: English
• Subjects: Catalysis; Decomposition; decomposition kinetic; Electrolytic cells; electron transformation; inorganic‐rich SEI; interfacial catalysis strategy; Lithium batteries; Molten salt electrolytes; Solid electrolytes; solid‐state lithium metal batteries
• ISSN: 1614-6832; 1614-6840
• DOI: 10.1002/aenm.202401829

Solid‐state lithium metal batteries (SSLMBs) with polymer electrolytes (SPEs) have attracted tremendous attention owing to their superior safety and high energy density. However, the unstable solid electrolyte interphase (SEI) between Lithium (Li) and SPEs hinders their practical application. Herein, an innovative interfacial catalysis strategy is applied to the in situ construction of a multifunctional inorganic‐rich SEI. The transfer of unpaired electrons adjacent to calcium vacancies (VCa) to the TFSI− anion promotes the breaking of S─N and C─F bonds during the electrochemical decomposition of TFSI−, thus enhancing its decomposition kinetics. The inorganic‐rich SEI derived from TFSI− is super‐stable and kinetically favorable for fast and homogeneous transport of Li ions, thereby hindering the growth of lithium dendrites. Consequently, the interfacial catalysis strategy endows Li||Li symmetric cells, LFP||Li and NCM811||Li full batteries with enhanced cyclability. Thus, this work expands the interfacial catalysis strategy to a platform for designing multifunctional SEI in long‐life SSLMB. The electron transfer to the TFSI‐ from the VCa of the ultrafine CHANW promotes the breakage of S─N and C─F bonds in the TFSI‐, thus inducing the formation of inorganic‐rich SEI derived from the TFSI‐. The inorganic‐rich SEI enables the rapid and uniform transport of lithium ions through the SEI, which in turn inhibits the formation and growth of lithium dendrites.