Chemo-bio catalysis using carbon supports: application in H2-driven cofactor recycling. Issue 23 (13th May 2021)

• Record Type: Journal Article
• Authors: Zhao, Xu; Cleary, Sarah E.; Zor, Ceren; Grobert, Nicole; Reeve, Holly A.; Vincent, Kylie A.
• Is Part Of: Chemical science. Volume 12:Issue 23(2021)
• Page Start: 8105
• Page End: 8114
• Publication Date: 2021-05-13
• Subjects: Chemistry -- Periodicals; 540.5
• DOI: 10.1039/d1sc00295c
• Languages: English
• ISSNs: 2041-6520

Abstract

Abstract : Heterogeneous chemo-bio catalytic hydrogenation is an attractive strategy for clean, enantioselective CX reduction. Abstract : Heterogeneous biocatalytic hydrogenation is an attractive strategy for clean, enantioselective CX 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 H2 oxidation with electrons transferred via the 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 −1 and 2347 h −1, respectively. This method demonstrates a new way of combining chemo- and biocatalysis on carbon supports, highlighted here for selective hydrogenation reactions.