Activation of Molecular Oxygen for Alcohol Oxidation over Vanadium Carbon Catalysts Synthesized via the Heterogeneous Ligand Strategy

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Author(s)Zhao, Li
Author(s)Yang, Piaoping
Author(s)Shi, Song
Author(s)Zhu, Guozhi
Author(s)Feng, Xiao
Author(s)Zheng, Weiqing
Author(s)Vlachos, Dionisios G.
Author(s)Xu, Jie
Date Accessioned2023-02-15T15:36:33Z
Date Available2023-02-15T15:36:33Z
Publication Date2022-12-16
DescriptionThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © 2022 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acscatal.2c04601. This article will be embargoed until 12/16/2023.
AbstractActivation of molecular oxygen to realize selective oxidation is challenging. We employ a heterogeneous ligand method to prepare a vanadium carbon catalyst (V–C catalyst) of high efficiency in alcohol oxidation via oxygen activation. Principal component analysis revealed that the chemisorbed oxygen and pentavalent vanadium oxide are crucial in catalyst performance. Isotopic labeling, electron paramagnetic resonance, and control experiments confirmed that the V–C catalyst activates molecular oxygen to singlet oxygen or its analogue and carries out the reaction. A kinetic study and in situ React-IR spectra illustrated that the main reaction route is the O2 activation to 1O2 or its analogue and oxidizes the substrate through C–H bond activation. We demonstrate the efficiency of the V–C catalyst in selectively oxidizing the hydroxyl group in other substrates, including benzyl alcohols, methyl lactate, and ethyl lactate biomass-based alcohols. This will guide the development of highly active nonprecious metal catalysts for activating O2 for aerobic oxidation.
SponsorThis work was supported by the National Natural Science Foundation of China (grant nos. 21790331 and 22072147), the Strategic Priority Research Program of Chinese Academy of Sciences (XDA21030400), the Youth Innovation Promotion Association, the Chinese Academy of Sciences (2021178). S.S. thanks the support of the “International Talent Program” from the Dalian Institute of Chemical Physics. P.Y., W.Z., and D.G.V.’s work was supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the US Dept. of Energy, Office of Science, Office of Basic Energy Sciences under award number DE-SC0001004.
CitationZhao, Li, Piaoping Yang, Song Shi, Guozhi Zhu, Xiao Feng, Weiqing Zheng, Dionisios G. Vlachos, and Jie Xu. “Activation of Molecular Oxygen for Alcohol Oxidation over Vanadium Carbon Catalysts Synthesized via the Heterogeneous Ligand Strategy.” ACS Catalysis 12, no. 24 (December 16, 2022): 15249–58. https://doi.org/10.1021/acscatal.2c04601.
ISSN2155-5435
URLhttps://udspace.udel.edu/handle/19716/32287
Languageen_US
PublisherACS Catalysis
Keywordsoxygen activation
Keywordsvanadium carbon catalyst
Keywordsalcohol oxidation
Keywordsheterogeneous ligand
Keywords1O2 or its analogue
TitleActivation of Molecular Oxygen for Alcohol Oxidation over Vanadium Carbon Catalysts Synthesized via the Heterogeneous Ligand Strategy
TypeArticle
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