Theoretical study of the mechanism of cationic chain decomposition of S-nitrosothiols

ORGN 25

Yilei Zhao, Dept. of Chemistry and Biochemistry, University of California, Los Angeles, 405 Hilgard Ave., Los Angeles, CA 90095-1569 and K. N. Houk, Department of Chemistry and Biochemistry, University of California Los Angeles, 405 Hilgard Ave, Los Angeles, CA 90095-1569.
S-Nitrosothiols (RSNO) have been suggested as physiologically active species in nitric oxide chemistry. However, the decompositions of nitrosothiols are faster than homolysis of the S-N bond under some conditions. We have explored a cationic chain mechanism, which is able to explain several experimental facts: 1) the decomposition is accelerated by O2, mixtures of O2 and NO, excess nitrosonium, and other oxidants; 2) the decomposition is blocked by thiols, high concentrations of NO, p-cresol, and other antioxidants; 3) RSNOs are more stable in polar solvents. We propose a cationic chain mechanism, in which a nitrosylated nitrosothiol reacts with a neutral nitrosothiol. This catalytic cycle produces disulfide and the NO dimer. The computed mechanism will be compared to the experimental data available for this reaction.