caa a22 4500 477061214 CHVBK 20180405111401.0 cr unu---uuuuu 170330e19960101xx s 000 0 eng 10.1007/BF00058703 doi (NATIONALLICENCE)springer-10.1007/BF00058703 Ab initio study on carbon Kinetic Isotope Effect (KIE) in the reaction of CH4+Cl• [Elektronische Daten] [Noriyuki Tanaka, Yitian Xiao, Antonio Lasaga] Recent studies suggest that the destruction of methane by Cl• in the marine boundary layer could be accounted for as another major sink besides the methane destruction by OH•. High level ab initio molecular orbital calculations have been carried out to study the CH4+Cl• reaction, the carbon Kinetic Isotope Effect (KIE) is calculated using Conventional Transition-State Theory (CTST) plus Wigner and Eckart semiclassical tunneling corrections. The calculated KIE is around 1.026 at 300 K and has a small temperature variation. This is by far the largest KIE among different processes involving atmospheric methane destruction (e.g., OH•, soil). A calculated mass balance of atmospheric methane including the KIE for the CH4+Cl• reaction is found to favor those methane budgets with enhanced biological methane sources, which have relatively lighter carbon isotope composition. Kluwer Academic Publishers, 1996 Ab initio nationallicence methane nationallicence chlorine nationallicence kinetic isotope effect nationallicence Tanaka Noriyuki Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A. aut Xiao Yitian Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A. aut Lasaga Antonio Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A. aut Journal of Atmospheric Chemistry Kluwer Academic Publishers; gopher://gopher.wkap.nl 23/1(1996-01-01), 37-49 0167-7764 23:1<37 1996 23 10874 https://doi.org/10.1007/BF00058703 text/html Onlinezugriff via DOI 1 research-article jats NATIONALLICENCE 856 40 https://doi.org/10.1007/BF00058703 text/html Onlinezugriff via DOI NATIONALLICENCE 700 1- Tanaka Noriyuki Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A aut NATIONALLICENCE 700 1- Xiao Yitian Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A aut NATIONALLICENCE 700 1- Lasaga Antonio Center for the Study of Global Change, Yale University, P.O. Box 208109, 06511-8109, New Haven, CT, U.S.A aut NATIONALLICENCE 773 0- Journal of Atmospheric Chemistry Kluwer Academic Publishers; gopher://gopher.wkap.nl/ 23/1(1996-01-01), 37-49 0167-7764 23:1<37 1996 23 10874 Metadata rights reserved Springer special CC-BY-NC licence nationallicence BK010053 XK010053 XK010000 NATIONALLICENCE NATIONALLICENCE NL-springer