Constructing a multi-functional polymer network for ultra-stable and safe Li-metal batteries

Shilun Gao, Zhenxi Li, Zhen Zhang, Bingrui Li, Xi Chelsea Chen, Guang Yang, Tomonori Saito, Ming Tian, Huabin Yang, Peng Fei Cao

Research output: Contribution to journalArticlepeer-review

25 Scopus citations

Abstract

The practical application of lithium (Li) metal electrodes is impeded by Li dendrite growth and unstable solid electrolyte interphase (SEI). Herein, a multi-grafting polymer network, poly(dimethyl siloxane)-g-[poly(poly(ethylene glycol) methyl ether methacrylate)-r-sodium poly(p-styrene sulfonate)] (PPS), is chemically synthesized from reversible addition-fragmentation chain transfer (RAFT) polymerization. With integrated stretchability, ionic conductivity, and mechanical robustness, it serves a dual role to stabilize the Li electrode. As artificial SEI layer, the PPS enables superior electrochemical performance in half cells, symmetric cells, and full cells (PPS@Li/LiFePO4, capacity retention of >70% after 600 cycles). Utilized as solid polymer electrolyte (SPE), the all-solid-state Li/SPE/LiFePO4 full cell delivers excellent cycling performance with an unprecedented capacity retention of 90% over 1,700 cycles at 0.5 C and 81% over 1,000 cycles at 1.0 C. With high-voltage LiNi0.8Mn0.1Co0.1O2 (NMC811) as cathode, the Li/SPE/NMC811 cell exhibits an initial discharge capacity of 162.2 mAh g−1 with a capacity retention of 72% after 200 cycles. The assembled solid-state Li/SPE/LiFePO4 pouch cell with SPE exhibits stable cycling performance over 200 cycles with a capacity retention of 75% and still operates well even after curling, folding, and cutting, demonstrating great potential for achieving ultra-safe and high energy density batteries.

Original languageEnglish
Pages (from-to)214-224
Number of pages11
JournalEnergy Storage Materials
Volume55
DOIs
StatePublished - Jan 2023

Funding

S. Gao and Z. Li are supported by the Natural Science Foundation of China ( 21421001 ), China Postdoctoral Science Foundation ( 2021M701769 ), the Natural Science Foundation of Tianjin , China ( 18JCZDJC31400 ), and the MOE Innovation Team ( IRT13022 ). P.-F. Cao acknowledges financial support by Fundamental Research Funds for the Central Universities ( buctrc202222 ). The FT-IR and mechanical characterization of polymer electrolytes were supported as part of the Fast and Cooperative Ion Transport in Polymer-Based Materials (FaCT), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences at Oak Ridge National Laboratory.

Keywords

  • Artificial solid electrolyte interphase
  • Elastic polymer network
  • Lithium-metal batteries
  • Solid polymer electrolyte

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