Development of gold(I)-catalyzed cycloisomerizations and rearrangements

ORGN 887

Michael R. Luzung, luzung@berkeley.edu and F. Dean Toste, fdtoste@berkeley.edu. Department of Chemistry, University of California, Berkeley, 609 Latimer Hall, Berkeley, CA 94720
There have been numerous applications of transition-metal catalyzed cycloisomerization reactions involving 1,6- and 1,7-enynes for the synthesis of cyclopentyl and cyclohexyl ring systems. However, simple 1,5-enynes and other skeletal derivatives have yet to be used as viable starting materials for these rearrangements. These unsaturated systems were elaborated to give a variety of cyclic and non-cyclic products via Au-(I) catalysis. All carbon 1,5 enynes, when subjected to Au-(I) catalysis, afforded bicyclo[3.1.0]-hexenes in good yield. Subsequent 4-hydroxy-1,5-enynes undergo an oxy-Cope rearrangement to afford &alpha,&beta-unsaturated ketones. 1,5-enynes containing a silicon atom instead of carbon at the propargylic position can undergo nucleophilic attack by an external nucleophile to afford substituted vinylsilanes, which are useful cross-coupling partners.