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Catalytic Synthesis of Cyclic Guanidines via Hydrogen Atom Transfer and Radical-Polar Crossover

Shunya Ohuchi, Hiroki Koyama, Hiroki Shigehisa

2021ACS Catalysis57 citationsDOI

Abstract

Cyclic guanidines are found in many biologically active compounds and natural products. Further, the formation of the atypical seven-membered ring of cyclic guanidine remains challenging because of a lack of efficient preparation strategies and low yield. Herein, a catalytic synthetic method for cyclic guanidines was developed via transition-metal hydrogen atom transfer and radical-polar crossover. This mild and functional-group-tolerant process enabled the cyclization of alkenyl guanidines bearing common protective groups, such as Cbz and Boc groups. This powerful method provided not only typical five- and six-membered rings but also the atypical seven-membered ring. The derivatization of the products afforded various heterocycles. We also investigated the selective cyclization of monoprotected or heteroprotected (TFA and Boc) alkenyl guanidines and their further derivatizations.

Topics & Concepts

ChemistryGuanidineCatalysisRing (chemistry)Yield (engineering)DerivatizationCombinatorial chemistryFunctional group2-PyridoneHydrogen atomOrganic chemistryGroup (periodic table)High-performance liquid chromatographyPolymerMaterials scienceMetallurgyRadical Photochemical ReactionsCatalytic C–H Functionalization MethodsSynthesis and Catalytic Reactions
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