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Bioinspired design of a hybrid bifunctional enzymatic/organic electrocatalyst for site selective alcohol oxidation
Louis Lancaster1, David P Hickey, Matthew S Sigman
1Department of Chemical and Environmental Engineering, University of California, Riverside, Riverside, CA 92521, USA. iwheeldon@engr.ucr.edu.
Abstract:
This work combines the thermostable alcohol dehydrogenase D (AdhD) from Pyrococcus furiosus and the organic electrocatalyst TEMPO to create a bifunctional catalyst that selectively oxidizes primary and secondary alcohols. The active sites function independently, can be switched on by changing reaction conditions, and can selectively oxidize a mixture of 1- and 2-butanol. The NAD+-dependent enzyme catalyses the secondary alcohol oxidation at a rate 3-fold faster than the primary alcohol, while the covalently attached 4-glycidyl-TEMPO oxidizes 1-butanol and has negligible activity toward 2-butanol. This hybrid catalytic approach has potential value for selective alcohol oxidations as well as other electrochemical and enzymatic multistep processes in energy conversion and chemical synthesis.
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