Understanding the active site in chameleon-like bifunctional catalyst for practical rechargeable zinc-air batteries

Xiongwei Zhong (), Xiao Xiao, Qizhen Li, Mengtian Zhang, Zhitong Li, Leyi Gao, Biao Chen, Zhiyang Zheng, Qingjin Fu, Xingzhu Wang, Guangmin Zhou () and Baomin Xu ()
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Xiongwei Zhong: Southern University of Science and Technology
Xiao Xiao: Tsinghua University
Qizhen Li: University of Manchester
Mengtian Zhang: Tsinghua University
Zhitong Li: Southern University of Science and Technology
Leyi Gao: Southern University of Science and Technology
Biao Chen: Tianjin University
Zhiyang Zheng: Tsinghua University
Qingjin Fu: Tsinghua University
Xingzhu Wang: Southern University of Science and Technology
Guangmin Zhou: Tsinghua University
Baomin Xu: Southern University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-17

Abstract: Abstract The practical application of rechargeable zinc-air batteries faces challenges stemming from inadequate bifunctional catalysts, contradictory gas-liquid-solid three-phase interfaces, and an ambiguous fundamental understanding. Herein, we propose a chameleon-like bifunctional catalyst comprising ruthenium single-atoms grafted onto nickel-iron layer double hydroxide (RuSA-NiFe LDH). The adaptive oxidation of RuSA-NiFe LDH to oxyhydroxide species (RuSA-NiFeOOH) during charging exposes active sites for the oxygen evolution reaction, while reversible reduction to NiFe LDH during discharge exposes active sites for the oxygen reduction reaction. Additionally, a hierarchical air cathode featuring hydrophilic and hydrophobic layers facilitates the reversible conversion between RuSA-NiFe LDH and RuSA-NiFeOOH, expedites oxygen bubble desorption, and suppresses carbon corrosion. Consequently, our zinc-air batteries demonstrate a high charge/discharge capacity of 100 mAh cm−2 per cycle, a voltage gap of 0.67 V, and an extended cycle life of 2400 h at 10 mA cm−2. We comprehensively elucidate the catalytic reaction thermodynamics and kinetics for the air cathode through electrode potential decoupling monitoring, oxygen bubble desorption tracking, and carbon content quantification.

Date: 2024
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DOI: 10.1038/s41467-024-54019-1

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