Ambient-stable cathode-level solid electrolyte via wetting-controlled surface molecular modification

doi:10.1016/j.jechem.2026.04.054

Ambient-stable cathode-level solid electrolyte via wetting-controlled surface molecular modification

2026-04-29

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DOI：10.1016/j.jechem.2026.04.054

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Sulfide solid electrolytes offer high ionic conductivity and favorable processability for all-solid-state batteries, yet their air instability remains a critical challenge, particularly for cathode-grade fine particles required in composite cathodes. In this work, we introduce an ultra-low surface energy molecular passivation (SEMP) strategy based on perfluorodecanethiol to stabilize argyrodite solid electrolytes under practically relevant ambient conditions (31% RH, 22 °C). Particle-size-dependent spectroscopic analyses reveal that cathode-grade electrolytes experience accelerated surface degradation driven by increased surface-to-volume ratios and diffusion kinetics. These degradation pathways are effectively suppressed by SEMP through chemically robust thiol anchoring and an ultralow-surface-energy perfluorinated tail. As a result, SEMP-treated cathode-grade electrolytes exhibit a slow ionic conductivity degradation rate and retain stable conductivity after 100 h of air exposure. Cell-level evaluations further demonstrate that, unlike pristine cathode-grade electrolytes that fail within 20 cycles after air exposure, SEMP-treated catholytes maintain stable interfacial behavior and prolonged cycling performance.

Keywords:

Sulfide solid electrolytes

Surface passivation

Argyrodite

Air stability

Ionic conductivity

Ambient-stable cathode-level solid electrolyte via wetting-controlled surface molecular modification

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