半焦对富含甲烷气体转化制备合成气的作用(Ⅳ)理论分析半焦表面含氧官能团的催化机理  被引量:4

EFFECT OF CHAR ON THE CONVERSION OF METHANE TO PRODUCE SYNGAS PART Ⅳ THE THEORETICAL STUDIES ON CATALYSIS MECHANISM OF OXYGEN-CONTAINING GROUPS IN CHAR

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作  者:孟华平[1] 赵炜[1] 章日光[1] 王宝俊[1] 

机构地区:[1]煤科学与技术教育部和山西省重点实验室,太原理工大学,太原030024

出  处:《煤炭转化》2008年第3期31-35,共5页Coal Conversion

基  金:国家重点基础研究发展规划(973)项目(2005CB221202,2005CB221203);国家自然科学基金资助项目(20676090,20576087,20776093);长江学者和创新团队发展计划项目(IRT0517)

摘  要:运用密度泛函理论方法研究了煤焦表面典型含氧官能团与甲烷的作用机理,分析了煤焦含氧官能团上氧的电荷分布、Fukui指数和变形密度等参数.结果表明,煤焦表面含氧官能团中,内酯和酸酐中C=O结构上氧的电荷相对较大,为化学反应的活性位点.在煤焦与甲烷的反应中,内酯和酸酐中C=O上的氧为甲烷活化脱氢的活性位置.甲烷进攻内酯氧反应的动力学计算显示,反应活化能为94.50kJ/mol,与实验值96kJ/mol吻合.The reaction mechanism of typical oxygen-containing functional groups on char surface with methane was studied by using density functional theory (DFT) method. The charge distribution of oxygen-containing functional groups, Fukui index and deformation density were calculated. The results show that in oxygen-containing functional groups of char surface,the oxygen charge of C=O structure in the lactone and anhydride were relatively large, which is thought to be the activity site of chemical reaction. In the reaction of the chars with methane,the oxygen for the C=O in lactones and anhydride was the activity position of methane activation dehydrogenation. The dynamics results show that in the reaction of methane attacking the oxygen of lactone, the activation energy is 94. 50 kJ/mol, which is in agreement with the experimental values 96 kJ/mol.

关 键 词:煤焦 含氧官能团 甲烷 密度泛函理论 

分 类 号:TQ520[化学工程—煤化学工程] TQ517.5

 

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