期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 51, 页码 23180-23187出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007745
关键词
aqueous lithium-ion batteries; interfaces; interphases; water-in-salt electrolyte; X-ray chemistry
资金
- Joint Center for Energy Storage Research (JCESR)
- DOE Office of Science via JCESR [IAA SN2020957]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-76SF00515]
- National Science Foundation [ECCS-2026822]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- U.S. DOE Office of Science, Division of Chemical Sciences, Geosciences and Biosciences [DE-SC0012704]
- Projekt DEAL
Super-concentrated water-in-salt electrolytes recently spurred resurgent interest for high energy density aqueous lithium-ion batteries. Thermodynamic stabilization at high concentrations and kinetic barriers towards interfacial water electrolysis significantly expand the electrochemical stability window, facilitating high voltage aqueous cells. Herein we investigated LiTFSI/H2O electrolyte interfacial decomposition pathways in the water-in-salt and salt-in-water regimes using synchrotron X-rays, which produce electrons at the solid/electrolyte interface to mimic reductive environments, and simultaneously probe the structure of surface films using X-ray diffraction. We observed the surface-reduction of TFSI(-)at super-concentration, leading to lithium fluoride interphase formation, while precipitation of the lithium hydroxide was not observed. The mechanism behind this 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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