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  • Title: Cooperative Catalysis of an Alcohol Dehydrogenase and Rhodium-Modified Periodic Mesoporous Organosilica.
    Author: Himiyama T, Waki M, Maegawa Y, Inagaki S.
    Journal: Angew Chem Int Ed Engl; 2019 Jul 01; 58(27):9150-9154. PubMed ID: 31025503.
    Abstract:
    The combined use of a metal-complex catalyst and an enzyme is attractive, but typically results in mutual inactivation. A rhodium (Rh) complex immobilized in a bipyridine-based periodic mesoporous organosilica (BPy-PMO) shows high catalytic activity during transfer hydrogenation, even in the presence of bovine serum albumin (BSA), while a homogeneous Rh complex exhibits reduced activity due to direct interaction with BSA. The use of a smaller protein or an amino acid revealed a clear size-sieving effect of the BPy-PMO that protected the Rh catalyst from direct interactions. A combination of Rh-immobilized BPy-PMO and an enzyme (horse liver alcohol dehydrogenase; HLADH) promoted sequential reactions involving the transfer hydrogenation of NAD+ to give NADH followed by the asymmetric hydrogenation of 4-phenyl-2-butanone with high enantioselectivity. The use of BPy-PMO as a support for metal complexes could be applied to other systems consisting of a metal-complex catalyst and an enzyme.
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