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Fluorinated interphase enables reversible aqueous zinc battery chemistries

Journal Article · · Nature Nanotechnology
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [2];  [3];  [1];  [4];  [2];  [1];  [1];  [1];  [1];  [3];  [2];  [2];  [1]
  1. Univ. of Maryland, College Park, MD (United States)
  2. US Army Research Lab., Adelphi, MD (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Univ. of Maryland, College Park, MD (United States); US Army Research Lab., Adelphi, MD (United States)

Metallic zinc is an ideal anode due to its high theoretical capacity (820 mAh g-1), low redox potential (-0.762 V versus the standard hydrogen electrode), high abundance and low toxicity. When used in aqueous electrolyte, it also brings intrinsic safety, but suffers from severe irreversibility. This is best exemplified by low coulombic efficiency, dendrite growth and water consumption. This is thought to be due to severe hydrogen evolution during zinc plating and stripping, hitherto making the in-situ formation of a solid-electrolyte interphase (SEI) impossible. Here, we report an aqueous zinc battery in which a dilute and acidic aqueous electrolyte with an alkylammonium salt additive assists the formation of a robust, Zn2+-conducting and waterproof SEI. The presence of this SEI enables excellent performance: dendrite-free zinc plating/stripping at 99.9% coulombic efficiency in a Ti||Zn asymmetric cell for 1,000 cycles; steady charge-discharge in a Zn||Zn symmetric cell for 6,000 cycles (6,000 h); and high energy densities (136 Wh kg-1 in a Zn||VOPO4 full battery with 88.7% retention for >6,000 cycles, 325 Wh kg-1 in a Zn||O2 full battery for >300 cycles and 218 Wh kg-1 in a Zn||MnO2 full battery with 88.5% retention for 1,000 cycles) using limited zinc. The SEI-forming electrolyte also allows the reversible operation of an anode-free pouch cell of Ti||ZnxVOPO4 at 100% depth of discharge for 100 cycles, thus establishing aqueous zinc batteries as viable cell systems for practical applications.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
SC0012704
OSTI ID:
1787833
Alternate ID(s):
OSTI ID: 1813008
Report Number(s):
BNL--221586-2021-JAAM
Journal Information:
Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 8 Vol. 16; ISSN 1748-3387
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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