Reprocessable and Recyclable Polymer Network Electrolytes via Incorporation of Dynamic Covalent Bonds

Lin, Yangju; Chen, Yuelang; Yu, Zhiao; Huang, Zhuojun; Lai, Jian-Cheng; Tok, Jeffrey B.-H.; Cui, Yi; Bao, Zhenan

doi:10.1021/acs.chemmater.1c04396

Title: Reprocessable and Recyclable Polymer Network Electrolytes via Incorporation of Dynamic Covalent Bonds

Journal Article · 22 February 2022 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c04396 · OSTI ID:1875429

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Stanford Univ., CA (United States)
Stanford Univ., CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES)

Mechanically durable polymer network electrolytes are desirable for batteries; however, covalent cross-linking adversely affects their large-scale manufacturing, and they are difficult to recycle post-lifespan. In this work, we address the electrolyte reprocessability and recyclability challenges through the use of dynamic covalent bonds for polymer network solid electrolytes. Specifically, the associative dynamic vinylogous urethane motif is incorporated into a poly(ethylene oxide) network electrolyte containing lithium bis(fluorosulfonyl)imide (LiFSI) salt. The resulting dynamic covalent network electrolyte possesses a modest ion conductivity (~10–5 S/cm at room temperature) and good reprocessability. Stress–relaxation studies indicate that the LiFSI salt can catalyze the bond exchange and enhance the network dynamics. Furthermore, the reprocessability associated with bond exchange can be tuned by simply adjusting the formulation of reagent compositions, in which increasing the amount of excess amine or using a shorter chain of PEO prepolymer can further enhance the network dynamics and corresponding reprocessability.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1875429

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 5 Vol. 34; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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