Theoretical study on the reaction of methane and zinc oxide in gas phase

The mechanism of the reaction between CH4 and ZnO has been studied theoretically at the CCSD(T)//B3LYP/6-311++G(2d,2p) levels. Four possible reaction pathways, yielding three products of syngas, HCHO and CH3OH, respectively, have been evaluated. All the four pathways are predicted to occur via the formation of CH4-ZnO molecular complex with two H atoms of CH4 approaching to the Zn end of ZnO. From this complex, the insertion of ZnO into the C-H bond of CH4 might proceed through two concerted manners along with charge transfer process. The pathway corresponding to the production of syngas is energetically feasible, in which the cleavage of C-H and Zn-H bonds with the formation of H-2 molecule is predicted to be the rate-limiting- step with the energy barrier of 45.4 kcal/mol. (c) 2006 Elsevier B.V. All rights reserved.