环戊二烯到萘生长路径的密度泛函研究
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- 英文论文题名：DFT Studies on the Reaction Mechanism of PAHs Growth from Cyclopentadiene to Naphthalene
- 论文作者：魏明锐 ; 张婷婷 ; 郭冠伦
- 英文论文作者：Mingrui Wei ; Tingting Zhang ; Guanlun Guo ; Hubei Key Laboratory of Advanced Technology for Automotive Components ; Wuhan University of Technology ; Hubei Collaborative Innovation Center for Automotive Components Technology ; Wuhan University of Technology
- 年：2016
- 作者机构：武汉理工大学现代汽车零部件技术湖北省重点实验室;武汉理工大学汽车零部件技术湖北省协同创新中心;
- 论文关键词：碳烟 ; PAH生长 ; 环戊二烯 ; 密度泛函理论
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第四十六分会：燃烧化学
- 语种：中文
- 分类号：O641.1;O625.151
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第四十六分会 ; 燃烧化学
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：268k
- 原文格式：D
- 会议级别：全国
摘要
多环芳香烃作为碳烟形成的重要前驱物,其生长过程引起了广泛关注。目前使用最广泛的PAH生长机理,HACA机理,在预测PAH和碳烟生成速率及浓度方面与实验结果相比偏低[1]。环戊二烯作为重要PAH生长组分,其重要性已被众多学者进行了理论与实验验证[2-4]。本文使用密度泛函方法研究了两条PAH生长的路径,两个环戊二烯反应生长到萘环或中间产物CS9。首先用DFT方法进行构型优化,然后提高水平用MP2方法计算单点能。该路径可添加到现有机理中,并一起用于PAH生长模拟。
PAHs growth process attracted much attention for it plays the key role for soot formation. Recently, H-abstraction-C_2H_2-addition(HACA), the most popular mechanism of PAHs growth, was found to predict lower concentrations and formation rates of PAHs and soot in comparison with the experiment results [1]. Cyclopentadiene was studied experimentally and theoretically for its importance to PAHs growth [2-4]. With density functional method, we studied two PAH growth routes from cyclopentadiene to naphthalene or intermediate CS9. All geometries were optimized with DFT, and single point energies were recalculated at the MP2/6-311G++(d,p) level. These routes could be added to the existing PAHs growth mechanism for further simulation.
PAHs growth process attracted much attention for it plays the key role for soot formation. Recently, H-abstraction-C_2H_2-addition(HACA), the most popular mechanism of PAHs growth, was found to predict lower concentrations and formation rates of PAHs and soot in comparison with the experiment results [1]. Cyclopentadiene was studied experimentally and theoretically for its importance to PAHs growth [2-4]. With density functional method, we studied two PAH growth routes from cyclopentadiene to naphthalene or intermediate CS9. All geometries were optimized with DFT, and single point energies were recalculated at the MP2/6-311G++(d,p) level. These routes could be added to the existing PAHs growth mechanism for further simulation.
引文
[1]Violi,A.;D’Anna,A.;D’Alessio,A.Chem.Eng.Sci.1999,54:3433.
[2]Dijokic,M.R.;Geem,K.M.V.;Cavallotti,C.;Frassoldati,A.;Ranzi,E.Combust.Flame.2014,161:2739.
[3]Wang,D.;Violi,A.;Kim,D.H.;Mullholland,J.A.J.Phys.Chem.A.2006,110:4719.
[4]Mullholland,J.A.;Lu,M.;Kim,D.H.Proc.Combust.Inst.2000,28:2593.
[2]Dijokic,M.R.;Geem,K.M.V.;Cavallotti,C.;Frassoldati,A.;Ranzi,E.Combust.Flame.2014,161:2739.
[3]Wang,D.;Violi,A.;Kim,D.H.;Mullholland,J.A.J.Phys.Chem.A.2006,110:4719.
[4]Mullholland,J.A.;Lu,M.;Kim,D.H.Proc.Combust.Inst.2000,28:2593.