화학공학소재연구정보센터
Chemical Physics Letters, Vol.515, No.1-3, 13-18, 2011
Towards a converged barrier height for the entrance channel transition state of the N(D-2) + CH4 reaction and its implication for the chemistry in Titan's atmosphere
The N(D-2) + CH4 reaction appears to be a key reaction for the chemistry of Titan's atmosphere, opening the door to nitrile formation as recently observed by the Cassini-Huygens mission. Faced to the controversy concerning the existence or not of a potential barrier for this reaction, we have carried out accurate ab initio calculations by means of multi-state multi-reference configuration interaction (MS-MR-SDCI) method. These calculations have been partially corrected for the size-consistency errors (SCE) by Davidson, Pople or AQCC corrections. We suggest a barrier height of 3.86 +/- 0.84 kJ/mol, including ZPE, for the entrance transition state, in good agreement with the experimental value. Its implication in Titan's atmopsheric chemistry is discussed. (C) 2011 Elsevier B.V. All rights reserved.