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

Yubin He, Chunyang Wang, Rui Zhang, Peichao Zou, Zhouyi Chen, Seong-Min Bak, Stephen E. Trask, Yonghua Du, Ruoqian Lin, Enyuan Hu and Huolin L. Xin ()
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Yubin He: University of California
Chunyang Wang: University of California
Rui Zhang: University of California
Peichao Zou: University of California
Zhouyi Chen: University of California
Seong-Min Bak: Brookhaven National Laboratory
Stephen E. Trask: Argonne National Laboratory
Yonghua Du: Brookhaven National Laboratory
Ruoqian Lin: University of California
Enyuan Hu: Brookhaven National Laboratory
Huolin L. Xin: University of California

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract Oxide ceramic electrolytes (OCEs) have great potential for solid-state lithium metal (Li0) battery applications because, in theory, their high elastic modulus provides better resistance to Li0 dendrite growth. However, in practice, OCEs can hardly survive critical current densities higher than 1 mA/cm2. Key issues that contribute to the breakdown of OCEs include Li0 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 –CH3⋯CF3 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 Li0 penetration and chemomechanical degradations, resulting in durability beyond 2000 hours in Li0-Li0 cells at 1 mA/cm2. Furthermore, by introducing a polyacrylate buffer layer between PCE and Li0-anode, long cycle life >3600 cycles was achieved when paired with a 4.2 V zero-strain cathode, all under near-zero stack pressure.

Date: 2024
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DOI: 10.1038/s41467-024-53869-z

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