Journal
NANO LETTERS
Volume 22, Issue 18, Pages 7535-7544Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c02514
Keywords
Aqueous electrolytes; zinc metal batteries; localized hydrophobicity; alkalinity scavenging; anion-phobic diluent
Categories
Funding
- National Science Foundation [CHE-1900401]
- UCI
- Office of Basic Energy Sciences of the U.S. Department of Energy [DE-SC0021204]
- National Science Foundation through the UC Irvine Materials Research Science and Engineering Center [DMR-2011967]
- National Science Foundation Major Research Instrumentation Program [CHE-1338173]
- Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office of the U.S. Department of Energy through the Advanced Battery Materials Research (BMR) Program [DE-SC0012704]
- Joint Center of Energy Storage Research (JCESR) - DOE Office of Science
- Jet Propulsion Laboratory, California Institute of Technology
- National Aeronautics and Space Administration
- DOE Office of Science by Brookhaven National Laboratory [DE-SC0012704]
- U.S. Department of Energy (DOE) [DE-SC0021204] Funding Source: U.S. Department of Energy (DOE)
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In this study, a new solution structure of aqueous electrolyte was reported, which achieved a hydrophobic anode-electrolyte interface by adding a suitable diluent, and reduced passivation layer formation through the hydroxyl-ion-scavenging functionality, improving the reversibility and lifetime of zinc metal batteries.
The rechargeability of aqueous zinc metal batteries is plagued by parasitic reactions of the zinc metal anode and detrimental morphologies such as dendritic or dead zinc. To improve the zinc metal reversibility, hereby we report a new solution structure of aqueous electrolyte with hydroxyl-ion scavengers and hydrophobicity localized in solvent clusters. We show that although hydrophobicity sounds counterintuitive for an aqueous system, hydrophilic pockets may be encapsulated inside a hydrophobic outer layer, and a hydrophobic anode-electrolyte interface can be generated through the addition of a cationphilic, strongly anion-phobic, and OH--reactive diluent. The localized hydrophobicity enables less active water and less absorbed water on the Zn anode surface, which suppresses the parasitic water reduction; while the hydroxyl-ion-scavenging functionality further minimizes undesired passivation layer formation, thus leading to superior reversibility (an average Zn plating/stripping efficiency of 99.72% for 1000 cycles) and lifetime (80.6% capacity retention after 5000 cycles) of zinc batteries.
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