期刊
JOURNAL OF CATALYSIS
卷 377, 期 -, 页码 283-292出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.06.047
关键词
Co-N-C; Single-atom catalyst; Benzyl alcohol oxidation; Kinetics; DFT calculation
资金
- National Natural Science Foundation of China (NSFC) [21676100, 21872041]
- Guangdong Natural Science Foundation [2017A030312005]
- Science and Technology Program of Guangzhou City [201707010058]
- NSFC [21773269]
- Youth INnuovation Promotion Association CAS [20151521]
Me-N-C catalysts have received intensive scientific interest as non-noble-metal single-atom catalysts (SAC) for electrochemical- and thermocatalytic reactions. However, the lack of understanding of its properties hinders further improvement of the catalytic performance. An interesting issue is the molecular details of the reaction involving more than one reactant, since the activation of the second reactant is inevitably affected by the first one on SAC. Here, we synthesized Co-N-C SACs for the aerobic oxidation of benzyl alcohol (BA) to benzaldehyde. The catalyst exhibited excellent activity for this reaction, among the most active non-noble-metal catalysts. Differently from particulate metal or metal oxide catalysts, the Co-N-C SAC displayed self-poisoning due to the strong competitive adsorption of BA to O-2, as revealed by kinetics experiments and density functional theory calculations. Moreover, we rationalized the poisoning effect of polar moieties, including organic solvents and aqueous solutions, on the SAC. These results shed light on the catalytic behavior of aerobic oxidation of BA on the molecular level and enable the rational design of catalytic organic synthesis over Co-N-C SACs. (C) 2019 Elsevier Inc. All rights reserved.
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