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

Author

Listed:
  • Yi Jiang

    (University of Waterloo)

  • Ya-Ping Deng

    (University of Waterloo)

  • Ruilin Liang

    (University of Waterloo)

  • Jing Fu

    (University of Waterloo
    Tongji University Shanghai)

  • 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)

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.

Suggested Citation

  • Yi Jiang & Ya-Ping Deng & Ruilin Liang & Jing Fu & Rui Gao & Dan Luo & Zhengyu Bai & Yongfeng Hu & Aiping Yu & Zhongwei Chen, 2020. "d-Orbital steered active sites through ligand editing on heterometal imidazole frameworks for rechargeable zinc-air battery," Nature Communications, Nature, vol. 11(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-19709-6
    DOI: 10.1038/s41467-020-19709-6
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