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Research Article

Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable Li metal batteries

Guocheng Li1,§, Kang Liang2,§, Yuanjian Li1, Xiangrui Duan1, Lin Fu1, Zhao Cai3, Zhaofu Zhang2, Jiangnan Dai1, Yongming Sun1( )
Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
The Institute of Technological Sciences, Wuhan University, Wuhan 430074, China
Faculty of Materials Science and Chemistry, China University of Geoscience (Wuhan), Wuhan 430074, China

§ Guocheng Li and Kang Liang contributed equally to this work.

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Graphical Abstract

A new design of composite Li metal foil was proposed, which can in situ catalyze the polymerization of gel polymer electrolyte (GPE) on its surface, and synchronously eliminate the anode volume change and realize low interphase resistance between electrolyte and anode during charge/discharge cycling processes. The as-designed electrode/GPE integrity exhibited stable electrode structure and significantly improved electrochemical performance in full cells.

Abstract

Employing quasi-solid-state gel polymer electrolyte (GPE) instead of the liquid counterpart has been regarded as a promising strategy for improving the electrochemical performance of Li metal batteries. However, the poor and uneven interfacial contact between Li metal anode and GPE could cause large interfacial resistance and electrochemical Li stripping/plating inhomogeneity, deteriorating the electrochemical performance. Herein, we proposed that the functional component of composite anode could work as the catalyst to promote the in situ polymerization reaction, and we experimentally realized the integration of polymerized-dioxolane electrolyte and Li/Li22Sn5/LiF composite electrode with low interfacial resistance and good stability by in situ catalyzation polymerization. Thus, the reaction kinetics and stability of metallic Li anode were significantly enhanced. As a demonstration, symmetric cell using such a GPE-Li/Li22Sn5/LiF integration achieved stable cycling beyond 250 cycles with small potential hysteresis of 25 mV at 1 mA·cm−2 and 1 mAh·cm−2, far outperforming the counterpart regular GPE on pure Li. Paired with LiNi0.5Co0.3Mn0.2O2, the full cell with the GPE-Li/Li22Sn5/LiF integration maintained 85.7% of the original capacity after 100 cycles at 0.5 C (1 C = 200 mA·g−1). Our research provides a promising strategy for reducing the resistance between GPE and Li metal anode, and realizes Li metal batteries with enhance electrochemical performance.

Keywords

catalyzation polymerizationinterface resistanceinterfacial stabilityLi metal batterieselectrochemical performance

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Nano Research
Volume 17 Issue 6,
June 2024
Pages 5216-5223
DOI: 10.1007/s12274-024-6463-2
Cite this article:
Li G, Liang K, Li Y, et al. Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable Li metal batteries. Nano Research, 2024, 17(6): 5216-5223. https://doi.org/10.1007/s12274-024-6463-2
Topics:
Lithium batteries

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Received: 12 November 2023
Revised: 28 December 2023
Accepted: 02 January 2024
Published: 01 February 2024
© Tsinghua University Press 2024
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