Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 5, Pages 1871-1877Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201911943
Keywords
antiperovskites; metal-organic frameworks (MOFs); nitrogen substitution; oxygen reduction reaction; zinc-air batteries
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Funding
- National Natural Science Foundation of China [51825201]
- National Key Research and Development Program of China [2017YFA0206701]
- National Program for Support of Topnotch Young Professionals
- Changjiang Scholar Program
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Antiperovskite Co3InC0.7N0.3 nanomaterials with highly enhanced oxygen reduction reaction (ORR) performance were prepared by tuning nitrogen contents through a metal-organic framework (MOF)-derived strategy. The nanomaterial surpasses all reported noble-metal-free antiperovskites and even most perovskites in terms of onset potential (0.957 V at J=0.1 mA cm(-2)) and half-wave potential (0.854 V). The OER and zinc-air battery performance demonstrate its multifunctional oxygen catalytic activities. DFT calculation was performed and for the first time, a 4 e(-) dissociative ORR pathway on (200) facets of antiperovskite was revealed. Free energy studies showed that nitrogen substitution could strengthen the OH desorption as well as hydrogenation that accounts for the enhanced ORR performance. This work expands the scope for material design via tailoring the nitrogen contents for optimal reaction free energy and hence performance of the antiperovskite system.
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