Litcius/Paper detail

Unlocking Epoxide Radical Anion Reactivity for Asymmetric Cross-Coupling by Copper Metallaphotoredox

Fan Teng, Ziqing Li, Zhi-Cheng Mao, Zhihan Zhang, Min Jiang, Wen‐Jing Xiao, Jia‐Rong Chen

2025Journal of the American Chemical Society15 citationsDOI

Abstract

The ability to tame radical anions that feature both an unpaired spin and a charge is critical for synthetic chemistry, enabling the construction of diverse chemical bonds via unique reaction pathways and promoting advances in the area of synthesis. In this regard, C(sp 3 )-rich epoxide radical anions are particularly attractive but often elusive, highly reactive intermediates. Classic methods to access epoxide radical anions exploit single-electron chemistry by using dissolving alkali, sacrificial electrodes, or redox metals. However, these methods are often prohibitive because of reagent safety issues and over-reduction, limiting their wide implementation, especially in asymmetric synthesis. Herein, we realize a copper metallaphotoredox platform to unlock epoxide radical anion reactivity, allowing the controlled generation of epoxide radical anions and their enantioconvergent cross-coupling with diverse, readily available partners via distonic radical anion intermediates. These discoveries permit highly regio-, chemo-, and enantioselective hydrocyanation and hydroalkynylation, thereby providing a general solution to the challenge of epoxide radical anion-mediated enantioselective chemical diversification.

Topics & Concepts

ChemistryEpoxideCopperReactivity (psychology)IonCoupling (piping)Polymer chemistryPhotochemistryStereochemistryCombinatorial chemistryComputational chemistryOrganic chemistryCatalysisMetallurgyPathologyMaterials scienceMedicineAlternative medicineRadical Photochemical ReactionsOxidative Organic Chemistry ReactionsCatalytic C–H Functionalization Methods