Selective Aerobic Oxidation of Alcohols over Atomically-Dispersed Non-Precious Metal Catalysts

Xie, Jiahan; Yin, Kehua; Serov, Alexey; Artyushkova, Kateryna; Pham, Hien N.; Sang, Xiahan; Unocic, Raymond R.; Atanassov, Plamen; Datye, Abhaya K.; Davis, Robert J.

doi:10.1002/cssc.201601364

Title: Selective Aerobic Oxidation of Alcohols over Atomically-Dispersed Non-Precious Metal Catalysts

Journal Article · Thu Dec 15 00:00:00 EST 2016 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.201601364· OSTI ID:1341579

Xie, Jiahan ^[1]; Yin, Kehua ^[1]; Serov, Alexey ^[2]; Artyushkova, Kateryna ^[2]; Pham, Hien N. ^[2]; Sang, Xiahan ^[3]; Unocic, Raymond R. ^[3]; Atanassov, Plamen ^[2]; Datye, Abhaya K. ^[2]; Davis, Robert J. ^[1]

Univ. of Virginia, Charlottesville, VA (United States). Dept. of Chemical Engineering
Univ. of New Mexico, Albuquerque, NM (United States). Dept. of Chemical and Biological Engineering and Center for Microengineered Materials
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science

Catalytic oxidation of alcohols often requires the presence of expensive transition metals. We show that earth-abundant Fe atoms dispersed throughout a nitrogen-containing carbon matrix catalyze the oxidation of benzyl alcohol and 5-hydroxymethylfurfural by O₂ in the aqueous phase. Furthermore, the activity of the catalyst can be regenerated by a mild treatment in H₂. An observed kinetic isotope effect indicates that β-H elimination from the alcohol is the kinetically relevant step in the mechanism, which can be accelerated by substituting Fe with Cu. Dispersed Cr, Co, and Ni also convert alcohols, demonstrating the general utility of metal–nitrogen–carbon materials for alcohol oxidation catalysis. Oxidation of aliphatic alcohols is substantially slower than that of aromatic alcohols, but adding 2,2,6,6-tetramethyl-1-piperidinyloxy as a co-catalyst with Fe can significantly improve the reaction rate.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office; National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1341579

Journal Information:: ChemSusChem, Vol. 10, Issue 2; ISSN 1864-5631

Publisher:: ChemPubSoc EuropeCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 58 works

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