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A Photoenzymatic Strategy for Radical‐Mediated Stereoselective Hydroalkylation with Diazo Compounds

Xinyu Duan, Dong Cui, Zhiguo Wang, Dannan Zheng, Linye Jiang, Wenyu Huang, Yi‐Xia Jia, Jian Xu

2022Angewandte Chemie International Edition55 citationsDOI

Abstract

Carbene insertion reactions initiated with diazo compounds have been widely used to develop unnatural enzymatic reactions. However, alternative functionalization of diazo compounds in enzymatic processes has been unexploited. Herein, we describe a photoenzymatic strategy for radical-mediated stereoselective hydroalkylation with diazo compounds. This method generates carbon-centered radicals through an ene reductase catalyzed photoinduced electron transfer process from diazo compounds, enabling the synthesis of γ-stereogenic carbonyl compounds in good yields and stereoselectivities. This study further expands the possible reaction patterns in photo-biocatalysis and offers a new approach to solving the selectivity challenges of radical-mediated reactions.

Topics & Concepts

DiazoStereoselectivityStereocenterChemistryBiocatalysisRadicalCarbeneCombinatorial chemistryOrganic chemistryCatalysisEnantioselective synthesisReaction mechanismCyclopropane Reaction MechanismsCatalytic C–H Functionalization MethodsSynthesis and Catalytic Reactions