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C–H Functionalization of Pyridines via Oxazino Pyridine Intermediates: Switching to <i>para</i>-Selectivity under Acidic Conditions

Hui Cao, Debkanta Bhattacharya, Qiang Cheng, Armido Studer

2023Journal of the American Chemical Society58 citationsDOI

Abstract

para -Selective C–H functionalization of pyridines holds a significant value but remains underdeveloped. Site-switchable C–H functionalization of pyridines under easily tunable conditions expedites drug development. We recently reported a redox-neutral dearomatization–rearomatization strategy for meta -C–H functionalization of pyridines via oxazino pyridine intermediates. Here, we demonstrate that these oxazino pyridine intermediates undergo highly para -selective functionalization simply by switching to acidic conditions. A broad scope of para -alkylated and arylated pyridines is prepared through radical as well as ionic pathways. These mild and catalyst-free methods are applied to the late-stage para -functionalization of drugs using pyridines as the limiting reagents. Consecutive meta,para -difunctionalization of pyridines is also achieved with complete regiocontrol relying on the pH-dependent reactivity of oxazino pyridines.

Topics & Concepts

ChemistrySelectivitySurface modificationPyridineOrganic chemistryMedicinal chemistryStereochemistryCatalysisPhysical chemistryCatalytic C–H Functionalization MethodsSynthesis and Catalytic ReactionsFluorine in Organic Chemistry
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