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A host-guest approach to combining enzymatic and artificial catalysis for catalyzing biomimetic monooxygenation.


ABSTRACT: Direct transfer of protons and electrons between two tandem reactions is still a great challenge, because overall reaction kinetics is seriously affected by diffusion rate of the proton and electron carriers. We herein report a host-guest supramolecular strategy based on the incorporation of NADH mimics onto the surface of a metal-organic capsule to encapsulate flavin analogues for catalytic biomimetic monooxygenations in conjunction with enzymes. Coupling an artificial catalysis and a natural enzymatic catalysis in the pocket of an enzyme, this host-guest catalyst-enzyme system allows direct proton and electron transport between two catalytic processes via NADH mimics for the monooxygenation of both cyclobutanones and thioethers. This host-guest approach, which involves the direct coupling of abiotic and biotic catalysts via a NADH-containing host, is quite promising compared to normal catalyst-enzyme systems, as it offers the key advantages of supramolecular catalysis in integrated chemical and biological synthetic sequences.

SUBMITTER: Zhao L 

PROVIDER: S-EPMC7283336 | biostudies-literature | 2020 Jun

REPOSITORIES: biostudies-literature

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A host-guest approach to combining enzymatic and artificial catalysis for catalyzing biomimetic monooxygenation.

Zhao Liang L   Cai Junkai J   Li Yanan Y   Wei Jianwei J   Duan Chunying C  

Nature communications 20200609 1


Direct transfer of protons and electrons between two tandem reactions is still a great challenge, because overall reaction kinetics is seriously affected by diffusion rate of the proton and electron carriers. We herein report a host-guest supramolecular strategy based on the incorporation of NADH mimics onto the surface of a metal-organic capsule to encapsulate flavin analogues for catalytic biomimetic monooxygenations in conjunction with enzymes. Coupling an artificial catalysis and a natural e  ...[more]

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