Anomalous C−C Bond Cleavage in Sulfur-Centered Cation Radicals Containing a Vicinal Hydroxy Group

Abstract
1,3-Dithianyl cation radicals having α-hydroxy-neopentyl or similar groups in position 2, which are generated via oxidative photoinduced electron transfer, undergo anomalous fragmentation necessitating refinement of the accepted mechanism. Experimental and computational data support a rationale in which proton abstraction from the hydroxy group in the initial cation radical does not cause a Grob-like fragmentation, but rather produces a neutral radical species, the alkoxy radical, that undergoes fragmentation in either direction, i.e., cleaving the C−C bond to dithiane or to the tertiary alkyl group.

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