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Tuning the Solvation Structure in Aqueous Zinc Batteries to Maximize Zn-Ion Intercalation and Optimize Dendrite-Free Zinc Plating

Journal Article · · ACS Energy Letters
 [1];  [2];  [1];  [1];  [3];  [1]
  1. University of Waterloo, ON (Canada); Argonne National Laboratory (ANL), Lemont, IL (United States). Joint Center for Energy Storage Research (JCESR)
  2. Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
  3. Argonne National Laboratory (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research (JCESR); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
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Aqueous zinc batteries are recognized to suffer from H+/Zn2+ coinsertion in the cathode, but few approaches have been reported to suppress deleterious H+ intercalation. We realize this goal by tuning the solvation structure, using LiV2(PO4)3 (LVP) as a model cathode. Phase conversion of LVP induced by H+ intercalation is observed in 4 m Zn(OTf)2, whereas dominant Zn2+ insertion is confirmed in a ZnCl2 water-in-salt electrolyte (WiSE). This disparity is ascribed to the complete absence of free water and a strong Zn2+–H2O interaction in the latter that interrupts the H2O hydrogen bonding network, thus suppressing H+ intercalation. On the basis of this strategy, a novel PEG-based hybrid electrolyte is designed to replace the corrosive ZnCl2 WiSE. This system exhibits an optimized Zn2+ solvation sheath with a similar low free water content, showing not only much better suppression of H+ intercalation but also highly reversible Zn plating/stripping with a CE of ~99.7% over 150 cycles.
Research Organization:
Argonne National Laboratory (ANL), Lemont, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
Discovery Grant and Canada Research Chair; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1963433
Alternate ID(s):
OSTI ID: 1989023
Journal Information:
ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 7; ISSN 2380-8195
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

25 ENERGY STORAGE
diffraction
electrodes
electrolytes
intercalation
molecules