Journal
ACS NANO
Volume 16, Issue 6, Pages 9667-9678Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.2c02996
Keywords
zinc metal anode; hydrophobic carbonate cosolvent; interface chemistry; aqueous battery; energy storage
Categories
Funding
- National Natural Science Foundation of China [22075067, 51804199]
- Natural Science Foundation of Hebei Province [B2020201001]
- Science and Technology Innovation Commission of Shenzhen [JCYJ20180507181858539, JCYJ20190808173815205]
- Young Elite Scientists Sponsorship Program by CAST [2021QNRC001]
- Guangdong Basic and Applied Basic Research Foundation [2019A1515012111]
- National Key R&D Program of China [2019YFB2204500]
- Shenzhen Science and Technology Program [KQTD20180412181422399]
- Research Innovation Team of College of Chemistry and Environmental Science of Hebei University [hxkytd2102]
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The introduction of a hydrophobic carbonate cosolvent in rechargeable aqueous zinc batteries can address the irreversible issues of Zn metal anodes by breaking the water's H-bond network, replacing solvating H2O, and creating a dendrite-free Zn2+-plating behavior. This efficient strategy with a hydrophobic cosolvent offers a promising direction for designing aqueous battery chemistries.
Rechargeable aqueous zinc (Zn) batteries are promising for large-energy storage because of their low cost, high safety, and environmental compatibility, but their implementation is hindered by the severe irreversibility of Zn metal anodes as exemplified by water-induced side reactions (H-2 evolution and Zn corrosion) and dendrite growth. Here, we find that the introduction of a hydrophobic carbonate cosolvent into a dilute aqueous electrolyte exhibits a much stronger ability to address the reversible issues facing Zn anodes than that with hydrophilic ones. Among the typical carbonates (ethylene carbonate, propylene carbonate, dimethyl carbonate, and diethyl carbonate (DEC)), DEC as the most hydrophobic additive enables the strongest breaking of water's H-bond network and replaces the solvating H2O in a Zn2+-solvation sheath, which significantly reduces the water activity and its decomposition. Additionally, DEC molecules preferentially adsorb onto the Zn surface to create an H2O-poor electrical double layer and render a dendrite-free Zn2+-plating behavior. The formulated hybrid 2 m Zn(OTf)(2) + 7 m DEC electrolyte endows the Zn electrode with an ability to achieve high cycling stability (over 3500 h at 5 mA cm(-2) with 2.5 mA h cm(-2)) and supports the stable operation of Zn parallel to V2O5 center dot nH(2)O full battery. This efficient strategy with hydrophobic cosolvent suggests a promising direction for designing aqueous battery chemistries.
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