期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 11, 页码 4783-4791出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c10295
关键词
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资金
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- University of Waterloo
- Waterloo Institute for Nanotechnology
- NSERC
- Canadian Institutes of Health Research
- Province of Saskatchewan
- Western Economic Diversification Canada
- University of Saskatchewan
- National Research Council Canada
This study proposes a linker compensation strategy to enhance the catalytic performance of metal-organic frameworks. By compensating the metal nodes, the performance of zinc-air batteries can be improved, resulting in higher current density and more stable voltage gap.
Metal-organic frameworks with tailorable coordinationchemistry are propitious for regulating catalytic performance anddeciphering genuine mechanisms. Herein, a linker compensation strategyis proposed to alter the intermediate adsorption free energy on the Co-Fezeolitic imidazolate framework (CFZ). This grants zinc-air batterysuperior high current density capability with a small discharge-chargevoltage gap of 0.88 V at 35 mA cm-2and an hourly fading rate of less than0.01% for over 500 h. Systematic characterization and theoretical modelingreveal that the performance elevation is closely correlated with thecompensation of CFZ unsaturated metal nodes by S-bridging heteroge-neous linkers, which exhibit electron-withdrawing characteristic that drivesthe delocalization of d-orbital electrons. These rearrangements ofelectronic structures establish a favorable adsorption/desorption pathwayfor key intermediates (OH*) and a stable coordination environment in bifunctional oxygen electrocatalysis.
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