Pressure-regulated mechanochemistry at lithium metal-sulfide electrolyte interfaces
Abstract
Stack pressure is commonly treated as a means of maintaining physical contact in all-solid-state lithium-metal batteries, but it can also alter the chemistry of reactive solid-solid interfaces. Here, using pressure-aware, charge-resolved machine-learning molecular dynamics validated against DFT, we determine how pressure magnitude and loading geometry regulate interphase formation at Li||Li6PS5Cl interfaces. The response is nonmonotonic: compression at 1 kbar accelerates PS4 decomposition and Li2S-like ordering, whereas 10-100 kbar compression restricts structural rearrangement and long-range crystallization. Charge-resolved dynamics further identify sulfur-centered, lithium-rich early-interphase environments associated with subsequent Li2S-like ordering. Uniaxial loading accelerates interfacial reaction relative to isostatic loading at the same nominal pressure. Pressure also changes void closure and dead-lithium spreading in a defect-location-dependent manner. These results establish applied pressure as a mechanochemical process variable coupling interphase chemistry, ion transport and defect evolution, providing a mechanistic framework for interpreting pressure effects in sulfide solid-state batteries.
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BibTeX
@misc{jang2026pressureregulated,
title = {{Pressure-regulated mechanochemistry at lithium metal-sulfide electrolyte interfaces}},
author = {Kunik Jang and Jaehwan Choi and Jang Wook Choi and Yousung Jung},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.01088},
eprint = {2609.01088},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.01088},
}
RIS
TY - UNPB
TI - Pressure-regulated mechanochemistry at lithium metal-sulfide electrolyte interfaces
AU - Kunik Jang
AU - Jaehwan Choi
AU - Jang Wook Choi
AU - Yousung Jung
PY - 2026
DA - 2026/09/01
PB - arXiv
DO - 10.48550/arxiv.2609.01088
UR - https://arxiv.org/abs/2609.01088
AB - Stack pressure is commonly treated as a means of maintaining physical contact in all-solid-state lithium-metal batteries, but it can also alter the chemistry of reactive solid-solid interfaces. Here, using pressure-aware, charge-resolved machine-learning molecular dynamics validated against DFT, we determine how pressure magnitude and loading geometry regulate interphase formation at Li||Li6PS5Cl interfaces. The response is nonmonotonic: compression at 1 kbar accelerates PS4 decomposition and Li2S-like ordering, whereas 10-100 kbar compression restricts structural rearrangement and long-range crystallization. Charge-resolved dynamics further identify sulfur-centered, lithium-rich early-interphase environments associated with subsequent Li2S-like ordering. Uniaxial loading accelerates interfacial reaction relative to isostatic loading at the same nominal pressure. Pressure also changes void closure and dead-lithium spreading in a defect-location-dependent manner. These results establish applied pressure as a mechanochemical process variable coupling interphase chemistry, ion transport and defect evolution, providing a mechanistic framework for interpreting pressure effects in sulfide solid-state batteries.
ER -