Abstract
The application of biocatalysts in the synthesis of fine chemicals and medicinal compounds has grown significantly in recent years. Particularly, there is a growing interest in the development of one-pot tandem catalytic systems combining the reactivity of a chemical catalyst with the selectivity engendered by the active site of an enzyme. Such tandem catalytic systems can achieve levels of chemo-, regio-, and stereo-selectivities that are unattainable with a small molecule catalyst. In addition, artificial metalloenzymes widen the range of reactivities and catalyzed reactions that are potentially employable. This review highlights some of the recent examples in the past three years that combined transition metal catalysis with enzymatic catalysis. This field is still in its infancy. However, with recent advances in protein engineering, catalyst synthesis, artificial metalloenzymes and supramolecular assembly, there is great potential to develop more sophisticated tandem chemoenzymatic processes for the synthesis of structurally complex chemicals.
Highlights
Living beings do not use enzymes in isolation
Recently,for photoredox photoredox has enteredwith the realm of biocatalysis to formora electrocatalysis more synergistic framework catalysis photoredox hasrealm entered the realm oftobiocatalysis tosynergistic form a more synergistic framework for catalysis has entered the of biocatalysis form a more framework for catalysis of challenging of challenging reactions under mild conditions
Were successfully applied as photosensitizers for regeneration of nicotinamide adenine dinucleotide were successfully applied as photosensitizers for regeneration of nicotinamide adenine dinucleotide phosphate (NADPH) in old yellowold enzyme (OYE) catalytic cycles
Summary
Living beings do not use enzymes in isolation. they build up the living system by applying multi-step synthesis strategies catalyzed by enzymes acting cooperatively. Reaction systems with maximized energy utilization efficiency and minimal waste generation Such synergy inspires biochemists to mimic nature to develop multi-step catalysis for selective synthesis, termed tandem catalysis. Biocatalysts typically have high regio-, stereo- and enantio-selectivity, but low productivity Considering those factors, combining the two technologies into a tandem one-pot reaction would allow access to more enantiopure compounds. Several strategies have been developed to overcome these obstacles, including using biphasic systems, the development of supramolecular hosts and the development of artificial metalloenzymes to compartmentalize the chemical catalysts Both metal catalysts and biocatalysts have been engineered to show higher activity in aqueous solutions or organic solvents with the utilization of catalyst immobilization and protein engineering respectively. We will cover major accomplishments in one-pot chemoenzymatic reactions within the last three years, including dynamic kinetic resolution, one-pot concurrent transformations in aqueous solutions, and interfacing transition-metal complexes with living cells
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