Chemical Science p. 8105 - 8114 (2021)
Update date:2022-08-02
Topics:
Cleary, Sarah E.
Grobert, Nicole
Reeve, Holly A.
Vincent, Kylie A.
Zhao, Xu
Zor, Ceren
Heterogeneous biocatalytic hydrogenation is an attractive strategy for clean, enantioselective CX reduction. This approach relies on enzymes powered by H2-driven NADH recycling. Commercially available carbon-supported metal (metal/C) catalysts are investigated here for direct H2-driven NAD+reduction. Selected metal/C catalysts are then used for H2oxidation with electrons transferredviathe conductive carbon support material to an adsorbed enzyme for NAD+reduction. These chemo-bio catalysts show improved activity and selectivity for generating bioactive NADH under ambient reaction conditions compared to metal/C catalysts. The metal/C catalysts and carbon support materials (all activated carbon or carbon black) are characterised to probe which properties potentially influence catalyst activity. The optimised chemo-bio catalysts are then used to supply NADH to an alcohol dehydrogenase for enantioselective (>99% ee) ketone reductions, leading to high cofactor turnover numbers and Pd and NAD+reductase activities of 441 h?1and 2347 h?1, respectively. This method demonstrates a new way of combining chemo- and biocatalysis on carbon supports, highlighted here for selective hydrogenation reactions.
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