Stereoselective formation of eight-membered rings by radical cyclization of silylenedioxy-tethered bis-methacrylate derivatives

J Org Chem. 2015 Mar 6;80(5):2869-73. doi: 10.1021/jo502947k. Epub 2015 Feb 12.

Abstract

Radical-initiated addition of CCl4, Cl3CBr, PhSH, and (TMS)3SiH to (bisisopropyl)silylenedioxy-tethered bis-methacrylate derivatives gives the corresponding eight-membered ring cyclic adducts stereoselectively. Hydrolysis of halo-substituted cyclic adducts with HCl in methanol affords the corresponding valerolactones, and the stereochemistry was determined by the X-ray crystallography on a dibromobenzoate derivative. DFT calculation on the eight-membered radical intermediate offers a plausible rationale for the stereoselectivity of the reaction.