Electrochemically-induced highly reactive PdO* interface on modulated mesoporous MOF-derived Co3O4 support for selective ethanol electro-oxidation

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.

Automated summary

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.