d-Orbital steered active sites through ligand editing on heterometal imidazole frameworks for rechargeable zinc-air battery

Yi Jiang, Ya-Ping Deng, Ruilin Liang, Jing Fu, Rui Gao, Dan Luo, Zhengyu Bai, Yongfeng Hu, Aiping Yu and Zhongwei Chen ()
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Yi Jiang: University of Waterloo
Ya-Ping Deng: University of Waterloo
Ruilin Liang: University of Waterloo
Jing Fu: University of Waterloo
Rui Gao: University of Waterloo
Dan Luo: University of Waterloo
Zhengyu Bai: Henan Normal University
Yongfeng Hu: University of Saskatchewan
Aiping Yu: University of Waterloo
Zhongwei Chen: University of Waterloo

Nature Communications, 2020, vol. 11, issue 1, 1-11

Abstract: Abstract The implementation of pristine metal-organic frameworks as air electrode may spark fresh vitality to rechargeable zinc-air batteries, but successful employment is rare due to the challenges in regulating their electronic states and structural porosity. Here we conquer these issues by incorporating ligand vacancies and hierarchical pores into cobalt-zinc heterometal imidazole frameworks. Systematic characterization and theoretical modeling disclose that the ligand editing eases surmountable energy barrier for *OH deprotonation by its efficacy to steer metal d-orbital electron occupancy. As a stride forward, the selected cobalt-zinc heterometallic alliance lifts the energy level of unsaturated d-orbitals and optimizes their adsorption/desorption process with oxygenated intermediates. With these merits, cobalt-zinc heterometal imidazole frameworks, as a conceptually unique electrode, empowers zinc-air battery with a discharge-charge voltage gap of 0.8 V and a cyclability of 1250 h at 15 mA cm–2, outperforming the noble-metal benchmarks.

Date: 2020
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DOI: 10.1038/s41467-020-19709-6

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