期刊
JOURNAL OF ENERGY CHEMISTRY
卷 86, 期 -, 页码 609-619出版社
ELSEVIER
DOI: 10.1016/j.jechem.2023.08.012
关键词
Reactive PdO* species; Mesoporous hollow structure; Ethanol electro-oxidation; Acetaldehyde electro-oxidation
Pd nanoparticles loaded Co3O4 catalysts (Pd@Co3O4) constructed from zeolitic imidazolate framework-67 (ZIF-67) demonstrate excellent performance and mechanism for the ethanol oxidation reaction, which can provide valuable inspiration for the design of high-performing catalysts.
Herein, Pd nanoparticles loaded Co3O4 catalysts (Pd@Co3O4) are constructed from zeolitic imidazolate framework-67 (ZIF-67) for the ethanol oxidation reaction (EOR). It is demonstrated for the first time that the electrochemical conversion of Co3O4 support would result in the charge distribution alignment at the Pd/Co3O4 interface and induce the formation of highly reactive Pd-O species (PdO*), which can further catalyze the consequent reactions of the intermediates of the ethanol oxidation. The catalyst, Pd@Co3O4-450, obtained under the optimized conditions exhibits excellent EOR performance with a high mass activity of 590 mA mg-1, prominent operational stability, and extraordinary capability for the electro-oxidation of acetaldehyde intermediates. Importantly, the detailed mechanism investigation reveals that Pd@Co3O4-450 could be benefit to the C-C bond cleavage to promote the desirable C1 pathway for the ethanol oxidation reaction. The present strategy based on the metal-support interaction of the catalyst might provide valuable inspiration for the design of high-performing catalysts for the ethanol oxidation reaction.(c) 2023 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.
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