Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 36, Pages 12469-12475Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201906289
Keywords
chromium; Fenton reaction; heterogeneous catalysis; oxygen reduction; single-atom catalysts
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Funding
- National Natural Science Foundation of China [21433003, 21633008, 21875243, 21603216, U1601211]
- National Science and Technology Major Project [2017YFB0102900]
- Jilin Province Science and Technology Development Program [20190201270JC, 20180101030JC, 20170203003SF]
- Hundred Talents Program of Chinese Academy of Sciences
- Recruitment Program of Foreign Experts [WQ20122200077]
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Single-atom catalysts (SACs) are attracting widespread interest for the catalytic oxygen reduction reaction (ORR), with Fe-N-x SACs exhibiting the most promising activity. However, Fe-based catalysts suffer serious stability issues as a result of oxidative corrosion through the Fenton reaction. Herein, using a metal-organic framework as an anchoring matrix, we for the first time obtained pyrolyzed Cr/N/C SACs for the ORR, where the atomically dispersed Cr is confirmed to have a Cr-N-4 coordination structure. The Cr/N/C catalyst exhibits excellent ORR activity with an optimal half-wave potential of 0.773 V versus RHE. More excitingly, the Fenton reaction is substantially reduced and, thus, the final catalysts show superb stability. The innovative and robust active site for the ORR opens a new possibility to circumvent the stability issue of the non-noble metal ORR catalysts.
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