西安交通大学动力工程多相流国家重点实验室
纸质出版:2023
移动端阅览
殷阁媛, 肖波, 胡二江, 等. 乙酸基+O2及其分解异构化反应速率常数计算和不确定度分析[J]. 西安交通大学学报, 2023,(5):109-117.
为了构建准确乙酸燃烧化学反应动力学模型,进行了乙酸基与O
2
及其分解异构化高精度的量子计算。利用CCSD(T)-F12/cc-pVTZ-F12//B2PLYPD3/cc-pVTZ算法,得到了反应体系势能面,并基于多参考态方法CASPT2/CBS//CASPT2/cc-pVTZ
获得无势垒反应势能面。通过气相单分子反应理论(RRKM)和主方程理论求解了温度和压力相关的速率常数,利用可变反应坐标过渡态理论求解无势垒反应乙酸基与O
2
加成反应的速率常数。结果表明:在低压或者高温条件下,超过99%的化学活化的O
2
CH
2
CO
2
H自由基直接分解为CH
2
O
2
H+CO
2
。随着压力升高,化学活化的O
2
CH
2
CO
2
H碰撞稳定后生成O
2
CH
2
CO
2
H
O
2
CH
2
CO
2
H则在后续反应中分解为CH
2
O
2
H+CO
2
。乙酸自由基在分解时,CO
2
+CH
3
产物通道占据主导地位。基于计算结果改进了原有乙酸模型,改进后的模型能够更好地预测层流燃烧速度,并且乙酸基存在更多的消耗路径,与量化计算结果一致。
张烨苗,李倩倩,闫治宇,黄佐华.异辛烷掺混乙醇在高温下层流预混燃烧特性的研究[J].西安交通大学学报,2018(07).
李小东,徐哲,燕翔,刘磊,王恒,王晶禹.FOX-7团簇中分子间相互作用对其裂解影响的量子化学研究[J].含能材料,2018(03).
潘伦,张英佳,黄佐华.C_2H_6/H_2混合气着火特性的实验与化学动力学研究[J].西安交通大学学报,2014(09).
郑爱军,仲兆平,戴佳佳,王春华.生物油催化酯化过程中乙酸转化率的智能预测[J].西安交通大学学报,2011(07).
Geyuan Yin,Zhenhua Gao,Erjiang Hu,Zhaohua Xu,Zuohua Huang.Comprehensive experimental and kinetic study of 2,4,4-trimethyl-1-pentene oxidation[J].Combustion and Flame,2019.
Xi Chen,Mark E. Fuller,C. Franklin Goldsmith.Decomposition kinetics for HONO and HNO2[J].Reaction Chemistry & Engineering,2019.
Chen Xi,Goldsmith C Franklin.A Theoretical and Computational Analysis of the Methyl-Vinyl + O2 Reaction and Its Effects on Propene Combustion.[J].The journal of physical chemistry. A,2017.
Moah Christensen,Alexander A. Konnov.Laminar burning velocity of acetic acid + air flames[J].Combustion and Flame,2016.
Goldsmith C Franklin,Harding Lawrence B,Georgievskii Yuri,Miller James A,Klippenstein Stephen J.Temperature and Pressure-Dependent Rate Coefficients for the Reaction of Vinyl Radical with Molecular Oxygen.[J].The journal of physical chemistry. A,2015.
Sinéad M. Burke,Ultan Burke,Reuben Mc Donagh,Olivier Mathieu,Irmis Osorio,Charles Keesee,Anibal Morones,Eric L. Petersen,Weijing Wang,Trent A. DeVerter,Matthew A. Oehlschlaeger,Brandie Rhodes,Ronald K. Hanson,David F. Davidson,Bryan W. Weber,Chih-Jen Sung,Jeffrey Santner,Yiguang Ju,Francis M. Haas,Frederick L. Dryer,Evgeniy N. Volkov,Elna J.K. Nilsson,Alexander A. Konnov,Majed Alrefae,Fethi Khaled,Aamir Farooq,Patricia Dirrenberger,Pierre-Alexandre Glaude,Frédérique Battin-Lecler.An experimental and modeling study of propene oxidation. Part 2: Ignition delay time and flame speed measurements[J].Combustion and Flame,2015.
Jiaxiang Zhang,Lun Pan,Jun Mo,Jing Gong,Zuohua Huang,Chung K. Law.A shock tube and kinetic modeling study of n -butanal oxidation[J].Combustion and Flame,2013.
Nicolas Leplat,Jaques Vandooren.Numerical and experimental study of the combustion of acetic acid in laminar premixed flames[J].Combustion and Flame,2011.
Anja Oasmaa,Yrjö Solantausta,Vesa Arpiainen,Eeva Kuoppala,Kai Sipilä.Fast Pyrolysis Bio-Oils from Wood and Agricultural Residues[J].Energy Fuels,2009.
Knizia Gerald,Werner Hans-Joachim.Explicitly correlated RMP2 for high-spin open-shell reference states.[J].The Journal of chemical physics,2008.
Grimme Stefan.Semiempirical hybrid density functional with perturbative second-order correlation.[J].The Journal of chemical physics,2006.
L. Gasnot,V. Decottignies,J.F. Pauwels.Kinetics modelling of ethyl acetate oxidation in flame conditions[J].Fuel,2004.
Juan P. Senosiain,Stephen J. Klippenstein,James A. Miller.A complete statistical analysis of the reaction between OH and CO[J].Proceedings of the Combustion Institute,2004.
Yuri Georgievskii,Stephen J. Klippenstein.Variable reaction coordinate transition state theory: Analytic results and application to the C2H3+H-C2H4 reaction[J].The Journal of Chemical Physics,2003.
Jan M.L. Martin,Jamal El-Yazal,Jean-Pierre Fran?ois.Structure and relative energetics of C 2 n +1 ( n = 2?7) carbon clusters using coupled cluster and hybrid density functional methods[J].Chemical Physics Letters,1996(1).
Lawrence J E,Koutrakis P.Measurement of atmospheric formic and acetic acids: methods evaluation and results from field studies.[J].Environmental science & technology,1994(5).
Kawamura K,Ng L L,Kaplan I R.Determination of organic acids (C1-C10) in the atmosphere, motor exhausts, and engine oils.[J].Environmental science & technology,1985(11).
0
浏览量
17
下载量
2
CSCD
关联资源
相关文章
相关作者
相关机构
京公网安备11010802024621