Localized Hydrophobicity in Aqueous Zinc Electrolytes Improves Zinc Metal Reversibility

Zou, Peichao; Lin, Ruoqian; Pollard, Travis P.; Yao, Libing; Hu, Enyuan; Zhang, Rui; He, Yubin; Wang, Chunyang; West, William C.; Ma, Lu; Borodin, Oleg; Xu, Kang; Yang, Xiao-Qing; Xin, Huolin L.

doi:10.1021/acs.nanolett.2c02514

Localized Hydrophobicity in Aqueous Zinc Electrolytes Improves Zinc Metal Reversibility

Journal Article · Wed Sep 07 00:00:00 EDT 2022 · Nano Letters

DOI:https://doi.org/10.1021/acs.nanolett.2c02514· OSTI ID:1889143

^[1]; Lin, Ruoqian ^[2]; ^[3]; Yao, Libing ^[1]; ^[4]; Zhang, Rui ^[1]; He, Yubin ^[1]; ^[1]; West, William C. ^[5]; Ma, Lu ^[4]; ^[3]; Xu, Kang ^[3]; ^[4]; ^[1]

Univ. of California, Irvine, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); California Institute of Technology (CalTech), Pasadena, CA (United States)
Army Research Lab., Adelphi, MD (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
California Institute of Technology (CalTech), Pasadena, CA (United States)

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-ions scavengers and hydrophobicity localized in solvent clusters. In this work 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 cation-philic, 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 reductions; 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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: National Aeronautics and Space Administration (NASA); National Science Foundation (NSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; SC0021204

OSTI ID:: 1889143

Report Number(s):: BNL-223416-2022-JAAM

Journal Information:: Nano Letters, Journal Name: Nano Letters Journal Issue: 18 Vol. 22; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Localized Hydrophobicity in Aqueous Zinc Electrolytes Improves Zinc Metal Reversibility

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