Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 34, Pages 14373-14377Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202006422
Keywords
electrocatalysis; hydrogen peroxide; metal-organic frameworks; oxygen reduction reaction; pyrolysis
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Funding
- Ministry of Science and Technology of China [2016YFA0204100, 2017YFA0208200]
- National Natural Science Foundation of China [21571135]
- Young Thousand Talented Program
- Natural Science Foundation of Jiangsu Higher Education Institutions [17KJB150032]
- project of scientific and technologic infrastructure of Suzhou [SZS201708]
- Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
- Soochow University
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Herein, we developed a partially controlled pyrolysis strategy to create evenly distributed NiO nanoparticles within NiFe-MOF nanosheets (MOF NSs) for electrochemical synthesis of H(2)O(2)by a two-electron oxygen reduction reaction (ORR). The elemental Ni can be partially transformed to NiO and uniformly distributed on the surface of the MOF NSs, which is crucial for the formation of the particular structure. The optimized MOF NSs-300 exhibits the highest activity for ORR with near-zero overpotential and excellent H(2)O(2)selectivity (ca. 99 %) in 0.1 mKOH solution. A high-yield H(2)O(2)production rate of 6.5 mol g(cat)(-1) h(-1)has also been achieved by MOF NSs-300 in 0.1 mKOH and at 0.6 V (vs. RHE). In contrast to completely pyrolyzed products, the enhanced catalytic activities of partially pyrolyzed MOF NSs-300 originates mainly from the retained MOF structure and the newly generated NiO nanoparticles, forming the coordinatively unsaturated Ni atoms and tuning the performance towards electrochemical H(2)O(2)synthesis.
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