Hybrid Dynamic Covalent Network as a Protective Layer and Solid-State Electrolyte for Stable Lithium-Metal Batteries

Author:Date:2023-05-11Views:11

论文题目:Hybrid Dynamic Covalent Network as a Protective Layer and Solid-State Electrolyte for Stable Lithium-Metal Batteries

论文作者:Yayue He, Mengxiang Ma, Lin Li, Zhenxi Li, Sheng Zhao, Xiao Zhao, Rigoberto Advincula, Ming Tian, Shilun Gao, Huabin Yang*, and Peng-Fei Cao*

发表期刊:ACS Appl. Mater. Interfaces 2023



Abstract

Lithium  (Li) metal is a highly promising anode material for next-generation  high-energy-density batteries, while Li dendrite growth and the unstable  solid electrolyte interphase layer inhibit its commercialization.  Herein, a chemically grafted hybrid dynamic network (CHDN) is rationally  designed and synthesized by the 4,4′-thiobisbenzenamine cross-linked  poly(poly(ethylene glycol) methyl ether methacrylate-r-glycidyl methacrylate) and (3-glycidyloxypropyl) trimethoxysilane-functionalized SiO2  nanoparticles, which is utilized as a protective layer and hybrid  solid-state electrolyte (HSE) for stable Li-metal batteries. The  presence of a dynamic exchangeable disulfide affords self-heability and  recyclability, and the chemical attachment between SiO2  nanoparticles and the polymer matrix enables the homogeneous  distribution of inorganic fillers and mechanical robustness. With  integrated flexibility, fast segmental dynamics, and autonomous  adaptability, the as-prepared CHDN-based protective layer enables  superior electrochemical performance in half cells and full cells  (capacity retention of 83.7% over 400 cycles for the CHDN@Li/LiFePO4  cell at 1 C). Furthermore, benefiting from intimate  electrode/electrolyte interfacial contact, CHDN-based solid-state cells  deliver excellent electrochemical performance (capacity retention of  89.5% over 500 cycles for the Li/HSE/LiFePO4 cell at 0.5 C). In addition, the Li/HSE/LiFePO4  pouch cell exhibits superior safety, even exposing various physical  damage conditions. This work thereby provides a fresh insight into a  rational design principle for dynamic network-based protective layers  and solid-state electrolytes for battery applications.