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

Nature Communications
Liang ZhaoChunying Duan

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.

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Citations

Jun 10, 2021·The Journal of Physical Chemistry. B·Sergi RodaVictor Guallar
Jul 10, 2021·The Journal of Chemical Physics·Matt McTaggartCecile Malardier-Jugroot
Sep 24, 2021·Journal of the American Chemical Society·Dan-Ni YanQing-Fu Sun

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Methods Mentioned

BETA
column chromatography
X-ray

Software Mentioned

SAINT
SHELXTL
SMART

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