碳烟表面生长中碳加成氢转移机理研究  

Study of Carbon-Addition-Hydrogen-Migration Mechanism in Soot Surface Growth

作　　者：侯丁钰 章竑博 何坦瑨 游小清[1,2] 

机构地区：[1]清华大学燃烧能源中心,北京100084 [2]清华大学热科学与动力工程教育部重点实验室,北京100084 [3]清华大学汽车系,北京100084

出　　处：《工程热物理学报》2016年第5期1100-1105,共6页Journal of Engineering Thermophysics

基　　金：国家自然科学基金委青年基金(No.51206090);国家重点基础研究发展计划(973)项目(No.2013CB228500)

摘　　要：为探究碳加成氢转移(CAHM)机理在碳烟表面生长的重要性并且完善表面生长模型,本文系统研究了层流预混火焰中含量较高的6种烯炔烃的CAHM反应势能面,计算了反应速率常数,进行了化学动力学模拟,然后将CAHM反应加入到已有的碳烟表面反应模型中进行动力学蒙特卡洛模拟。模拟结果表明1500 K低氢原子浓度下CAHM机理对质量增加的贡献是氢吸取乙炔加成(HACA)机理的十几倍,而且可以解释碳烟脂肪族外壳的结构,且与实验结果脂肪族是烯基相符。This work aims to explore the role of Carbon-Addition-Hydrogen-Migration（CAHM）mechanism and to improve the soot surface growth model.CAHM reactions involving six alkenes and alkynes that are relatively abundant in laminar premixed flames were investigated using both density functional theory and transition state theory.We developed a CAHM sub-model using the computed rate constants and perfomed chemical kinetics modeling and detailed kinetic Monte Carlo（KMC） simulations to predict the evolution of graphene edges at typical conditions of the post-flame region.KMC results show that mass growth contributed by CAHM mechanism is 13 times that of HACA mechanism,which also explains the aromatic-core-aliphatic-shell structures observed in soot experiments.

关 键 词：碳烟 表面生长 碳加成氢转移机理 化学动力学模拟 动力学蒙特卡洛模拟 

分 类 号：TK16[动力工程及工程热物理—热能工程]