Interfacial Speciation Determines Interfacial Chemistry: X-ray-Induced Lithium Fluoride Formation from Water-in-salt Electrolytes on Solid Surfaces

Steinrück, Hans‐Georg; Cao, Chuntian; Lukatskaya, Maria R.; Takacs, Christopher J.; Wan, Gang; Mackanic, David G.; Tsao, Yuchi; Zhao, Jingbo; Helms, Brett A.; Xu, Kang; Borodin, Oleg; Wishart, James F.; Toney, Michael F.

doi:10.1002/ange.202007745

Title: Interfacial Speciation Determines Interfacial Chemistry: X-ray-Induced Lithium Fluoride Formation from Water-in-salt Electrolytes on Solid Surfaces

Journal Article · Thu Sep 03 00:00:00 EDT 2020 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202007745· OSTI ID:1670505

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SSRL Materials Science Division SLAC National Accelerator Laboratory Menlo Park CA 94025 USA;SLAC National Accelerator Laboratory Joint Center for Energy Storage Research (JCESR) Lemont IL 60439 USA;Department Chemie Universität Paderborn 33098 Paderborn Germany
SSRL Materials Science Division SLAC National Accelerator Laboratory Menlo Park CA 94025 USA
SSRL Materials Science Division SLAC National Accelerator Laboratory Menlo Park CA 94025 USA;SLAC National Accelerator Laboratory Joint Center for Energy Storage Research (JCESR) Lemont IL 60439 USA;Laboratory for Electrochemical Energy Systems Department of Mechanical and Process Engineering ETH Zürich 8092 Zürich Switzerland
SSRL Materials Science Division SLAC National Accelerator Laboratory Menlo Park CA 94025 USA;SLAC National Accelerator Laboratory Joint Center for Energy Storage Research (JCESR) Lemont IL 60439 USA
Department of Chemical Engineering Stanford University Stanford USA
Department of Chemistry Stanford University Stanford USA
Joint Center for Energy Storage Research Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
Joint Center for Energy Storage Research Lawrence Berkeley National Laboratory Berkeley CA 94720 USA;The Molecular Foundry Lawrence Berkeley National Laboratory Berkeley CA 94720 USA
Energy Storage Branch Sensor and Electron Devices Directorate U.S. Army Research Laboratory Adelphi 20783 USA
Chemistry Division Brookhaven National Laboratory Upton NY 11973 USA
SSRL Materials Science Division SLAC National Accelerator Laboratory Menlo Park CA 94025 USA;SLAC National Accelerator Laboratory Joint Center for Energy Storage Research (JCESR) Lemont IL 60439 USA;Department of Chemical and Biological Engineering University of Colorado Boulder CO 80309 USA

Using synchrotron X-rays the LiTFSI/H₂O electrolyte interfacial decomposition pathways in the „water-in-salt“ and „salt-in-water“ regimes are investigated. The resultant photoelectron-induced reduction was revealed to be concentration-dependent interfacial chemistry that only occurs among closely contact ion-pairs, which constitutes the rationale behind the „water-in-salt“ concept.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; SN2020957; AC02‐76SF00515; AC02‐05CH11231; ECCS‐2026822

OSTI ID:: 1670505

Alternate ID(s):: OSTI ID: 1670508; OSTI ID: 1706596

Report Number(s):: BNL-220566-2020-JAAM

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Vol. 132 Journal Issue: 51; ISSN 0044-8249

Publisher:: German Chemical SocietyCopyright Statement

Country of Publication:: Germany

Language:: English

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