镍基上甲烷与二氧化碳脱氢重整机理的理论研究.pdf

35 / 1 / 河北师范大学学报/ / Vol. 35 No. 1 2011 1 JOURNAL OF HEBEI NORMAL UNIVERSITY/ Natural Science Edition/ Ja n. 2011 镍基上甲烷与二氧化碳脱氢重整机理的理论研究 徐文媛, 龙 威 ( , 330013) : ( DFT) (MP2) CO 2 ., 4 ,, CO CO.5 , - 104.310,52.501,55. 135,315.602,- 202. 164kJ/mol.5 2 1 5,4, 577.610kJ/mol. : ; ; :O 64. 12 :A :2011) A Theoretical Study of The Reforming Dehydrogenation Reactions Mechanism Between Methane and Carbon Dioxide Based on Nickel X Wenyuan, LONG Wei ( School of Chemistry and Chemical Engineering, East China Jiaotong niversity,Jiangxi Nanchang 330013, China) Abstract:The mechanism of the decomposition reforming between methane and carbon dioxide based on nickel was investigated by DFT and MP2 methods. The research showed that on Nibased catalysts,the progress of methane s dehydroge had occured before the reforming reaction with CO . T he results also showed that 2 methane had generated Nibased carbon after the fourstep dehydrogenation while releasing the hydrogen. Ni based carbon continued to react with CO2 that could produce CO.The total reaction included five steps,the first step and the fifth step were exothermicreaction,and the second,the third and thefourth steps were endothermic reactions.The heats of reaction of the five steps were:- 104.310, 52.501,55. 135,315. 602, - 202. 164kJ/ mol.T he activation energy of five steps showed the first step and the fifthstep reaction were easy,the fourth step was the rate determining step,and its activation e