Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphase

Hao, Hongchang; Liu, Yijie; Greene, Samuel M.; Yang, Guang; Naik, Kaustubh G.; Vishnugopi, Bairav S.; Wang, Yixian; Celio, Hugo; Dolocan, Andrei; Tsai, Wan‐Yu; Fang, Ruyi; Watt, John; Mukherjee, Partha P.; Siegel, Donald J.; Mitlin, David

doi:10.1002/aenm.202301338

Tuned Reactivity at the Lithium Metal–Argyrodite Solid State Electrolyte Interphase

Journal Article · Wed Sep 27 00:00:00 EDT 2023 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202301338· OSTI ID:2007379

^[1]; Liu, Yijie ^[1]; Greene, Samuel M. ^[1]; Yang, Guang ^[2]; Naik, Kaustubh G. ^[3]; Vishnugopi, Bairav S. ^[3]; Wang, Yixian ^[1]; Celio, Hugo ^[1]; Dolocan, Andrei ^[1]; Tsai, Wan‐Yu ^[2]; Fang, Ruyi ^[1]; ^[4]; Mukherjee, Partha P. ^[3]; Siegel, Donald J. ^[1]; ^[1]

University of Texas, Austin, TX (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Purdue University, West Lafayette, IN (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Thin intermetallic Li₂Te–LiTe₃ bilayer (0.75 µm) derived from 2D tellurene stabilizes the solid electrolyte interphase (SEI) of lithium metal and argyrodite (LPSCl, Li₆PS₅Cl) solid-state electrolyte (SSE). Tellurene is loaded onto a standard battery separator and reacted with lithium through single-pass mechanical rolling or transferred directly to SSE surface by pressing. State-of-the-art electrochemical performance is achieved, e.g., symmetric cell stable for 300 cycles (1800 h) at 1 mA cm^-2 and 3 mAh cm^-2 (25% DOD, 60 µm foil). Cryo-stage focused ion beam (Cryo-FIB) sectioning and Raman mapping demonstrate that the Li₂Te–LiTe₃ bilayer impedes SSE decomposition. The unmodified Li–LPSCl interphase is electrochemically unstable with a geometrically heterogeneous reduction decomposition reaction front that extends deep into the SSE. Decomposition drives voiding in Li metal due to its high flux to the reaction front, as well as voiding in the SSE due to the associated volume changes. Analysis of cycled SSE found no evidence for pristine (unreacted) lithium metal filaments/dendrites, implying failure driven by decomposition phases with sufficient electrical conductivity that span electrolyte thickness. In conclusion, DFT calculations clarify thermodynamic stability, interfacial adhesion, and electronic transport properties of interphases, while mesoscale modeling examines interrelations between reaction front heterogeneity (SEI heterogeneity), current distribution, and localized chemo-mechanical stresses.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: 89233218CNA000001; SC0023438

OSTI ID:: 2007379

Alternate ID(s):: OSTI ID: 2007709
OSTI ID: 2229178

Report Number(s):: LA-UR--23-30506

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 46 Vol. 13; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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All-solid-state lithium batteries enabled by sulfide electrolytes: from fundamental research to practical engineering design Wang, Changhong; Liang, Jianwen; Zhao, Yang Energy & Environmental Science, Vol. 14, Issue 5 https://doi.org/10.1039/D1EE00551K	journal	January 2021
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Commentary: The Materials Project: A materials genome approach to accelerating materials innovation Jain, Anubhav; Ong, Shyue Ping; Hautier, Geoffroy APL Materials, Vol. 1, Issue 1 https://doi.org/10.1063/1.4812323	journal	July 2013
Carbon-free high-loading silicon anodes enabled by sulfide solid electrolytes Tan, Darren H. S.; Chen, Yu-Ting; Yang, Hedi Science, Vol. 373, Issue 6562 https://doi.org/10.1126/science.abg7217	journal	September 2021
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