A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries

He, Yubin; Wang, Chunyang; Zhang, Rui; Zou, Peichao; Chen, Zhouyi; Bak, Seong-Min; Trask, Stephen E.; Du, Yonghua; Lin, Ruoqian; Hu, Enyuan; Xin, Huolin L.

doi:10.1038/s41467-024-53869-z

Title: A self-healing plastic ceramic electrolyte by an aprotic dynamic polymer network for lithium metal batteries

Journal Article · 19 November 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-53869-z · OSTI ID:2477877

He, Yubin;

; Zhang, Rui; Zou, Peichao; Chen, Zhouyi; Bak, Seong-Min;

;

; Lin, Ruoqian;

;

Abstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li ⁰ ) battery applications because, in theory, their high elastic modulus provides better resistance to Li ⁰ dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm ² . Key issues that contribute to the breakdown of OCEs include Li ⁰ penetration promoted by grain boundaries (GBs), uncontrolled side reactions at electrode-OCE interfaces, and, equally importantly, defects evolution (e.g., void growth and crack propagation) that leads to local current concentration and mechanical failure inside and on OCEs. Here, taking advantage of a dynamically crosslinked aprotic polymer with non-covalent –CH ₃ ⋯CF ₃ bonds, we developed a plastic ceramic electrolyte (PCE) by hybridizing the polymer framework with ionically conductive ceramics. Using in-situ synchrotron X-ray technique and Cryogenic transmission electron microscopy (Cryo-TEM), we uncover that the PCE exhibits self-healing/repairing capability through a two-step dynamic defects removal mechanism. This significantly suppresses the generation of hotspots for Li ⁰ penetration and chemomechanical degradations, resulting in durability beyond 2000 hours in Li ⁰ -Li ⁰ cells at 1 mA/cm ² . Furthermore, by introducing a polyacrylate buffer layer between PCE and Li ⁰ -anode, long cycle life >3600 cycles was achieved when paired with a 4.2 V zero-strain cathode, all under near-zero stack pressure.

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Sponsoring Organization:: USDOE

OSTI ID:: 2477877

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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