Surface molecular engineering to enable processing of sulfide solid electrolytes in humid ambient air

Mengchen Liu, Jessica J. Hong, Elias Sebti, Ke Zhou, Shen Wang, Shijie Feng, Tyler Pennebaker, Zeyu Hui, Qiushi Miao, Ershuang Lu, Nimrod Harpak, Sicen Yu, Jianbin Zhou, Jeong Woo Oh, Min-Sang Song, Jian Luo, Raphaële J. Clément () and Ping Liu ()
Additional contact information
Mengchen Liu: University of California San Diego
Jessica J. Hong: University of California San Diego
Elias Sebti: University of California Santa Barbara
Ke Zhou: University of California San Diego
Shen Wang: University of California San Diego
Shijie Feng: University of California San Diego
Tyler Pennebaker: University of California Santa Barbara
Zeyu Hui: University of California San Diego
Qiushi Miao: University of California San Diego
Ershuang Lu: San Diego
Nimrod Harpak: University of California San Diego
Sicen Yu: University of California San Diego
Jianbin Zhou: University of California San Diego
Jeong Woo Oh: Gangseo-gu
Min-Sang Song: Gangseo-gu
Jian Luo: University of California San Diego
Raphaële J. Clément: University of California Santa Barbara
Ping Liu: University of California San Diego

Nature Communications, 2025, vol. 16, issue 1, 1-12

Abstract: Abstract Sulfide solid-state electrolytes (SSEs) are promising candidates to realize all solid-state batteries (ASSBs) due to their superior ionic conductivity and excellent ductility. However, their hypersensitivity to moisture requires processing environments that are not compatible with today’s lithium-ion battery manufacturing infrastructure. Herein, we present a reversible surface modification strategy that enables the processability of sulfide SSEs (e. g., Li6PS5Cl) under humid ambient air. We demonstrate that a long chain alkyl thiol, 1-undecanethiol, is chemically compatible with the electrolyte with negligible impact on its ion conductivity. Importantly, the thiol modification extends the amount of time that the sulfide SSE can be exposed to air with 33% relative humidity (33% RH) with limited degradation of its structure while retaining a conductivity of above 1 mS cm-1 for up to 2 days, a more than 100-fold improvement in protection time over competing approaches. Experimental and computational results reveal that the thiol group anchors to the SSE surface, while the hydrophobic hydrocarbon tail provides protection by repelling water. The modified Li6PS5Cl SSE maintains its function after exposure to ambient humidity when implemented in a Li0.5In | |LiNi0.8Co0.1Mn0.1O2 ASSB. The proposed protection strategy based on surface molecular interactions represents a major step forward towards cost-competitive and energy-efficient sulfide SSE manufacturing for ASSB applications.

Date: 2025
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DOI: 10.1038/s41467-024-55634-8

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