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

Nature Communications
Yi JiangZhongwei Chen

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.

References

Mar 17, 2006·The Journal of Physical Chemistry. B·Frédéric JaouenMei Cai
Oct 4, 2007·Inorganic Chemistry·Rodrigo PatiñoLuis Alfonso Torres
Jun 29, 2013·Journal of the American Chemical Society·Lei ZhangXiong Wen David Lou
May 10, 2017·Materials Science & Engineering. C, Materials for Biological Applications·Ai-Nhan Au-Duong, Cheng-Kang Lee
Feb 1, 2018·Accounts of Chemical Research·Cheng TangQiang Zhang
May 24, 2019·Angewandte Chemie·Meiling XiaoZhongwei Chen
Sep 19, 2019·Angewandte Chemie·Xue Feng LuXiong Wen David Lou

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Methods Mentioned

BETA
AFM
light scattering
transmission electron microscopy
atomic force microscopy
X-ray
electron-paramagnetic resonance

Software Mentioned

Artemis
Athena
ray Microdiffraction Analysis
Vienna ab initio simulation package ( VASP )

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