正十二烷高温燃烧详细化学动力学机理的系统简化.pdf

物理化学学报( Wuli Huarue
yendo
2536
cta Phys.-Chim.Sin.2012,28(11),2536-2542
November
e」
doi:10.3866/PKU.WHXB201208201
www.whxb.pku.edu.cn
正十二烷高温燃烧详细化学动力学机理的系统简化
方亚梅1王全德1王繁1李象远2
(四川大学化学学院,成都610064;2四川大学化学工程学院,成都610065
摘要:采用详细化学反应动力学机理的系统简化方法,以典型航空燃料的替代组分正十二烷为研究对象,开
展了正十二烷高温燃烧化学动力学机理的系统简化.首先采用多步直接关系图法(DRG)和基于计算奇异值摄
动法(CSP)重要性指标的反应移除方法对由1279个组分,5056个棊元反应组成的正十二烷燃烧详细机理进行
框架简化,得到了包含59个组分,222个基元反应的框架机理;进一步采用CSP对框架机理进行时间尺度分
析,选出了10个准稳态物种,采用准稳态近似方法(QSSA)构建了包含49个组分的全局简化机理.计算结果表
明,在较宽的参数范围内,框架机理和全局简化机理均能够重现正十二烷详细机理在高温燃烧的点火延迟时
间、熄火以及物种浓度分布等方面的模拟结果
关鍵词:正十二烷;详细反应动力学机理;机理简化;直接关系图;计算奇异值摄动法;准稳态近似
中图分类号』O643
Reduction of the Detailed Kinetic Mechanism for High-temperature
Combustion of n-dodecane
FANG Ya-mei WANG Quan-de WANG Fan"LI Xiang-yuan
College of Chemisry Sichuan University, Chengdu 610064, P R. China; College of Chemical Engineering.
Sichuan University, Chengdu 610065, P R. China)
Abstract: The detailed chemical kinetic mechanism for high-temperature combustion of n-dodecane was
systematically reduced via integrated mechanism reduction methods. The skeletal mechanism, including
59 species and 222 elementary reactions, was derived using the directed relation graph method(DRG)
combined with a method based on computational singular per urbation(SP importance index from a
detailed mechanism consisting of 1279 species and 5056 elementary reactions. The skeletal mechanism
was fur er ee through tm analsis T mto was employ for e selection of quasi
steady state (@SS)species, and ten species were chosen as QSS species. Finally, based on the quasi
steady state approximation method, a 49-species reduced mechanism was derived. Both the skeletal
echanism and the 49-species reduced mechanism reproduced the ignition delay time, extinction, and
species profiles of the detailed mechanism over a wide range of simulation conditions
Key Words: n-dodecane Detailed chemical kinetic mechanism: Mechanism reduction: Directed
relation graph, Computational singular perturbation; Quasi-steady state approximation
要的燃料是碳氢燃料,研究碳氢燃料燃烧反应动力
到目前为止,人类社会使用的最普遍也是最重学机理对于发动机燃烧室的设计、污染物的形成与
Received: June 13, 2012; Revised: August 20, 2012; Published on Web: August 20, 2012.
Correspondingauthors.WANGFan,Email;wang@scu.edu.cn;Tel:+86-28-85406139,LIXiang-yuan,Email:lixy(@scu.edu.cn
The project was supported by the National Natural Science Foundation of China(1016002, 91116001/A0204)
国家自然科学基金(9101600,9110A0204)资助项目
(C Editorial office of Acta Physico-chimica Sinica