Highly reversible zinc metal anode enabled by strong Brønsted acid and hydrophobic interfacial chemistry

Qingshun Nian, Xuan Luo, Digen Ruan, Yecheng Li, Bing-Qing Xiong, Zhuangzhuang Cui, Zihong Wang, Qi Dong, Jiajia Fan, Jinyu Jiang, Jun Ma, Zhihao Ma, Dazhuang Wang and Xiaodi Ren ()
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Qingshun Nian: University of Science and Technology of China
Xuan Luo: University of Science and Technology of China
Digen Ruan: University of Science and Technology of China
Yecheng Li: University of Science and Technology of China
Bing-Qing Xiong: University of Science and Technology of China
Zhuangzhuang Cui: University of Science and Technology of China
Zihong Wang: University of Science and Technology of China
Qi Dong: University of Science and Technology of China
Jiajia Fan: University of Science and Technology of China
Jinyu Jiang: University of Science and Technology of China
Jun Ma: University of Science and Technology of China
Zhihao Ma: University of Science and Technology of China
Dazhuang Wang: University of Science and Technology of China
Xiaodi Ren: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract Uncontrollable zinc (Zn) plating and hydrogen evolution greatly undermine Zn anode reversibility. Previous electrolyte designs focus on suppressing H2O reactivity, however, the accumulation of alkaline byproducts during battery calendar aging and cycling still deteriorates the battery performance. Here, we present a direct strategy to tackle such problems using a strong Brønsted acid, bis(trifluoromethanesulfonyl)imide (HTFSI), as the electrolyte additive. This approach reformulates battery interfacial chemistry on both electrodes, suppresses continuous corrosion reactions and promotes uniform Zn deposition. The enrichment of hydrophobic TFSI– anions at the Zn|electrolyte interface creates an H2O-deficient micro-environment, thus inhibiting Zn corrosion reactions and inducing a ZnS-rich interphase. This highly acidic electrolyte demonstrates high Zn plating/stripping Coulombic efficiency up to 99.7% at 1 mA cm–2 ( > 99.8% under higher current density and areal capacity). Additionally, Zn | |ZnV6O9 full cells exhibit a high capacity retention of 76.8% after 2000 cycles.

Date: 2024
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DOI: 10.1038/s41467-024-48444-5

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