期刊信息
- 刊名： 河北师范大学学报（自然科学版）Journal of Hebei Normal University (Natural Science)
- 主办： 河北师范大学
- ISSN： 1000-5854
- CN： 13-1061/N
- 中国科技核心期刊
- 中国期刊方阵入选期刊
- 中国高校优秀科技期刊
- 华北优秀期刊
- 河北省优秀科技期刊
A Theoretical Study of The Reforming Dehydrogenation Reaction's Mechanism Between Methane and Carbon Dioxide Based on Nickel
摘要/Abstract
采用密度泛函理论(DFT)及二级微扰(MP2)方法对使用镍基催化剂上甲烷的逐步脱氢后与CO2发生重整反应制合成气的机理进行了研究.计算结果表明,甲烷进行4步脱氢后生成镍基碳,同时释放出氢气,镍基碳再与CO2反应生成CO.反应分5步进行,其焓变分别为-104.310,52.501,55.135,315.602,-202.164 kJ/mol.5步反应的活化能表明第1步和第5步反应较易进行,反应的速控步骤是第4步,其正反应的活化能为577.610 kJ/mol.
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 Ni-based catalysts,the progress of methane's dehydroge had occured before the reforming reaction with CO2.The results also showed that methane had generated Ni-based carbon after the four-step 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 exothermic reaction,and the second,the third and the fourth steps were endothermic reactions.The heats of reaction of the five steps were:-104.310,52.501,55.135,315.602,-202.164 kJ/mol.The activation energy of five steps showed the first step and the fifth-step reaction were easy,the fourth step was the rate determining step,and its activation energy was 577.610 kJ/mol.