Citation: XIA Wen-Sheng, CHANG Gang, HOU Yu-Hui, WENG Wei-Zheng, WAN Hui-Lin. Influence of Ni Chemical States on the Partial Oxidation Mechanism of Methane: An Energetics Analysis[J]. Acta Physico-Chimica Sinica, ;2011, 27(07): 1567-1573. doi: 10.3866/PKU.WHXB20110627 shu

Influence of Ni Chemical States on the Partial Oxidation Mechanism of Methane: An Energetics Analysis

1.
State Key Laboratory of Physical Chemistry for Solid State Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Fujian Province Key Laboratory of Theoretical and Computational Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China

Received Date: 1 April 2011
Available Online: 6 May 2011
Fund Project: 国家自然科学基金(21033006, 20923004) (21033006, 20923004) 福建省自然科学基金(2007J0168) (2007J0168)国家重点基础研究发展规划项目(973) (2010CB732303)资助 (973) (2010CB732303)

An energetics analysis of the possible elementary steps involved in the partial oxidation of methane (POM) over different chemical states of Ni was carried out using the unity bond index-quadratic exponential potential (UBI-QEP) method. The results show that the rate determining step for the partial oxidation mechanism of methane is related to the chemical state of the Ni. Over reduced Ni the rate determining step for CO formation is the association of surface CH₃ species with surface O species. Over a partial positive charged Ni surface the rate determining step is that methane dissociates into the CH_xO species with the assistance of oxygen. Over the reduced and partial positive charged Ni sites in coexistence, however, the rate determining step depends on the competition between the formation of surface CH₃ species and the recombination of surface CH₃ species with surface O species. This competition is related to the chemical states of the Ni sites. If the partial positive charged Ni sites are predominant on the surface, the recombination of surface C species with surface O species and the recombination of surface H atom species favor CO and H₂ formation because of decreasing barriers. The surface CHx species does not dissociate easily and surface carbon deposition is significantly inhibited.
- Partial oxidation of methane,
- Nickel,
- Chemical state,
- Rate determining step,
- Mechanism,
- Energetics
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沈阳化工大学材料科学与工程学院沈阳 110142