Journal
CHEMSUSCHEM
Volume 10, Issue 2, Pages 359-362Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.201601364
Keywords
heterogeneous catalyst; N-doped carbon; non-precious metal; oxidation; reaction mechanism
Funding
- US NSF [EEC-0813570, CBET-1157829]
- US DOE-EERE Fuel Cell Technology Program
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Catalytic oxidation of alcohols often requires the presence of expensive transition metals. Herein, it is shown that earth-abundant Fe atoms dispersed throughout a nitrogen-containing carbon matrix catalyze the oxidation of benzyl alcohol and 5-hydroxymethylfurfural by O-2 in the aqueous phase. The activity of the catalyst can be regenerated by a mild treatment in H-2. An observed kinetic isotope effect indicates that beta-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 addition of 2,2,6,6-tetramethyl-1-piperidinyloxy as a co-catalyst with Fe can significantly improve the reaction rate.
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