Azulene to naphthalene conversion: Generation and detection of possible radical intermediates

ORGN 15

Brett M. McCollum1, Jean-Claude Brodovitch1, Paul W. Percival, percival@sfu.ca1, and Jason A. C. Clyburne, jason.clyburne@smu.ca2. (1) Department of Chemistry, Simon Fraser University, 8888 University Drive, Burnaby, BC V5A 1S6, Canada, (2) Department of Chemistry, Saint Mary's University, 923 Robie St., Halifax, NS B3H 3C3, Canada
The conversion of azulene to naphthalene at high temperatures has captured the attention of both experimentalists and theoreticians.[1] Its importance lies not only as the first documented thermal rearrangement of an aromatic hydrocarbon, but more specifically as the reorganization of an aromatic polar nonbenzenoid to an aromatic nonpolar benzenoid structure. Various experimental and computational approaches have been made over the years to determine the reaction pathways involved. It has been argued that two radical-promoted pathways play a role in the conversion process. Both of these reactions, the spiran mechanism and the methylene-walk mechanism, involve the attack of a hydrogen atom (H•) to the azulene molecule. In addition, both pathways require the unfavorable geometry of a hydrogen or methylene bonded to one of the two bridging carbon atoms. More recently, Stirling et. al. recognize the necessity for an experimental study of the radical products of H• addition to azulene. Using the light ‘isotope' of hydrogen, muonium (Mu = µ+e-), formed by the capture of an electron by a positively charged muon, we have been able to detect the radical products formed by Mu addition to azulene. We have also been able to identify each of the detected radicals, based on our measurements of the hyperfine coupling constants of the spin active atoms in the Mu-azulyl radicals.
 

Heterocycles and Aromatics
8:00 AM-12:00 PM, Sunday, 26 March 2006 Georgia World Congress Center -- C301, Oral

Division of Organic Chemistry

The 231st ACS National Meeting, Atlanta, GA, March 26-30, 2006