Long-cycling lithium-metal batteries via an integrated solid–electrolyte interphase promoted by a progressive dual-passivation coating

Guo-Xing Li, Rong Kou, Au Nguyen, Ke Wang, Yu-Sheng Li, Jongcheol Lee, Seong H. Kim and Donghai Wang ()
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Guo-Xing Li: The Pennsylvania State University
Rong Kou: Southern Methodist University
Au Nguyen: The Pennsylvania State University
Ke Wang: The Pennsylvania State University
Yu-Sheng Li: The Pennsylvania State University
Jongcheol Lee: The Pennsylvania State University
Seong H. Kim: The Pennsylvania State University
Donghai Wang: The Pennsylvania State University

Nature Energy, 2025, vol. 10, issue 8, 941-950

Abstract: Abstract Stabilizing lithium (Li) metal anodes has long been hindered by the challenge of forming a stable solid–electrolyte interphase, stemming from the inherently high reactivity of Li metal with liquid electrolytes. Here we developed a progressive dual-passivation polymer coating strategy to stabilize Li-metal anodes, achieving exceptional cycle life of Li-metal batteries in carbonate electrolyte. Unlike current approaches, the synthesized copolymer coating passivates the Li-metal anode while also tailoring the Li-ion solvation structure by facilitating selective anion decoordination in a binary salt carbonate electrolyte. This process leads to the formation of an integrated solid–electrolyte interphase, featuring a chemical passivation outer layer predominant in LiF generated by the polymer coating and an anion-derived Li2O-prevalent inner layer from the electrolyte decomposition. Consequently, this coating strategy remarkably enhances the stability of Li-metal anodes, enabling double-layer Li||NMC811 pouch cells to maintain 80% of their initial capacity up to 611 cycles under a low electrolyte/capacity (E/C) ratio of 2.0 g Ah−1.

Date: 2025
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DOI: 10.1038/s41560-025-01803-y

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