Litcius/Paper detail

Gadolinium Photocatalysis: Dearomative [2+2] Cycloaddition/Ring‐Expansion Sequence with Indoles

Jiajia Ma, Felix Schäfers, Constantin G. Daniliuc, Klaus Bergander, Cristian A. Strassert, Frank Glorius

2020Angewandte Chemie22 citationsDOI

Abstract

Abstract Lanthanide photocatalysts are much less investigated in synthetic chemistry than rare and expensive late transition metals. We herein introduce Gd III photocatalysis of a highly regioselective, intermolecular [2+2] photocycloaddition/ring‐expansion sequence with indoles, which could provide divergent access to cyclopenta[ b ]indoles and indolines. A simple and commercially available Gd(OTf) 3 salt is sufficient for this visible‐violet‐light‐induced transformation. The reaction proceeds either through a transient or start‐to‐end dearomatization cascade and shows excellent regioselectivity (usually >95:5 r.r.), broad scope (59 examples), good functional group tolerance and facile scale‐up under mild, direct visible‐light‐excitation conditions. Mechanistic investigations reveal that direct excitation of the Gd(OTf) 3 /indole mixture gives an excited state intermediate, which undergoes the subsequent [2+2] cycloaddition and cyclobutane‐expansion cascade.

Topics & Concepts

CycloadditionRegioselectivityChemistryCyclobutaneIndole testPhotocatalysisRing (chemistry)PhotochemistryLanthanideExcited stateCombinatorial chemistryStereochemistryOrganic chemistryCatalysisNuclear physicsPhysicsIonRadical Photochemical ReactionsCatalytic C–H Functionalization MethodsOxidative Organic Chemistry Reactions