1, 3-丁二烯热裂解的动力学计算与模型研究

doi:10.3866/PKU.WHXB201512071

Abstract

Abstract:

1, 3-Butadiene is an important product in combustion and pyrolysis of hydrocarbon fuels and it is also an important precursor to formpolycyclic aromatic hydrocarbons (PAHs). Currently, a variety of experimental and mechanism studies have been performed on 1, 3-butadiene oxidation. However, few studies about pyrolysis mechanism of 1, 3-butadiene have been done. In this work, the optimization of the geometries and the vibrational frequencies for the reactants, products, and transition states of the relevant reactions in 1, 3-butadiene pyrolysis have been performed at the B3LYP/CBSB7 level. Their single point energies and the thermodynamic parameters are also calculated by using the composite CBS-QB3 method. The high-pressure limit rate constants for tight transition state reactions and barrierless reactions are obtained by transition state theory and variable reaction coordinate transition state theory, respectively. The calculated rate constants in this work are in good agreement with those available from literature. Furthermore, the mechanism of Hidaka et al. is updated with replacing the calculated rate constants of reactions in this work to simulate the shock tube experiment results of 1, 3-butadiene pyrolysisand the updated mechanism consists of 45 species and 224 reactions. It can be seen that the updated mechanism can improve the concentration profiles of the main products, ethylene, 1-butylene-3-acetylene, and benzene in 1, 3-butadiene pyrolysis. It can also provide reliable kinetic and thermodynamic parameters to further improve the core mechanism of C₀-C₄ species.

Key words: 1, 3-Butadiene, Pyrolysis mechanism, Rate constant, Kinetic simulation

Click here to download Supporting Info material in ZIP type

Niao-Feng DU,Hong-Bo NING,Ze-Rong LI,Qi-Yi ZHANG,Xiang-Yuan LI. Kinetic Calculation and Modeling Study of 1, 3-Butadiene Pyrolysis[J]. Acta Phys. -Chim. Sin. 2016, 32(2), 453-464. doi: 10.3866/PKU.WHXB201512071

References

1	Yao T. ; Zhong B. J Acta Phys. -Chim. Sin 2013, 29 (7), 1385.
1	姚通; 钟北京. 物理化学学报, 2013, 29 (7), 1385.
2	Zeng M. R. ; Yuan W. H. ; Wang Y. Z. ; Zhou W. X. ; Zhang L.D. ; Qi F. ; Li Y. Y Combust. Flame 2014, 161, 1701.
3	Hughes K. ; Meek M. E. ; Walker M. ; Beauchamp R 1, 3-Butadiene: Human Health Aspects. In Concise International Chemical Assessment Document 30; WHO: Geneva, Switzerland 2001, pp 1-73.
4	Vaughan W. E. J Am. Chem. Soc 1932, 54, 3863.
5	Kistiakovsky G. B. ; Ransom W.W. J Chem. Phys 1939, 7, 725.
6	Harkness J. B. ; Kistiakowski G. B. ; Mears W. H. J Chem. Phys 1937, 5, 682.
7	Granata S. ; Faravelli T. ; Ranzi E. ; Olten N. ; Senkan S Combust. Flame 2002, 131, 273.
8	Dagaut P. ; Cathonnet M Combust. Sci. Technol 1998, 140, 225.
9	Hidaka, Y.; Higashihara, T.; Ninomiya, N.; Masaoka, H.; Nakamura, T.; Kawano, H. Int. J. Chem. Kinet. 1996, 28, 137.
10	Tsang, W. Chemical Activation Reactions in the HeptaneCombustion Kinetics Database. In AIAA 44th Aerospace Sciences Meeting and Exihibt, American Institute ofAeronautics and Astronautics, Reno, Nevada, January 9-12, 2006.
11	Laskin, A.; Wang, H.; Law, C. K. Int. J. Chem. Kinet. 2000, 32, 589.
12	Peukert, S.; Braun-Unkhoff, M.; Naumann, C. HighTemperature Kinetics of the Pyrolysis of 1, 3-Butadiene and 2-Butyne. In Fundamental Physical and Chemical Kinetics, Proceedings of the European Combustion Meeting, Vienna, Austria, April 14-17, 2009.
13	Montgomery J. A. ; J r. ; Frisch M. J. ; Ochterski J.W. ; Petersson G. A. J Chem. Phys 1999, 110, 2822.
14	Miller J. A. ; Klippenstein S. J. J Phys. Chem. A 2013, 117, 2718.
15	Xu C. ; Shoaibi A. S. A. ; Wang C. G. ; Carstensen H. H. ; Dean A. M. J Phys. Chem. A 2011, 115, 10470.
16	Frisch, M. J.; Trucks, G.W.; Schlegel, H. B.; et al. Gaussian 03, Revision B.05; Gaussian Inc.: Pittsburgh, PA, 2003.
17	Becke A. D. J Chem. Phys 1993, 98, 1372.
18	Lee C. ; Yang W. ; Parr R. G Phys. Rev. B 1988, 37, 785.
19	Gonzalez C. ; Schlegel H. B. J Chem. Phys 1989, 90, 2154.
20	Sirjean B. ; Fournet R. J Phys. Chem. A 2012, 116, 6675.
21	Curtiss L. A. ; Raghavachari K. ; Redfern P. C. ; Pople J. A J. Chem. Phys 1997, 106, 1063.
22	Gaithersburg, M. D. NIST Computational ChemistryComparison and Benchmark Database; National Institute ofStandards and Technology. http://webbook.nist.gov/chemistry(2003).
23	Wang, H.; You, X. Q.; Joshi, A. V.; Davis, S. G.; Laskin, A.; Egolfopoulos, F. N.; Law, C. K. USC Mech Version II. High-Temperature Combustion Reaction Model of H2/CO/C1-C4Compounds. http://ignis.usc.edu/USC_Mech_II.htm (accessed2007).
24	Klippenstein S. J. ; Wagner A. F. ; Dunbar R. C. ; Wardlaw D.M. ; RobertsonS.H. VariFlex, Version 1.0; Argonne NationalLaboratory: Argonne, IL 1999.
25	Beyer, T.; Swinehart, D. F. Comm. Assoc. Comput. Mach.1973, 16, 379.
26	Holbrook, K. A.; Pilling, M. J.; Robertson, S. H., Unimolecular Reactions, 2nd ed.; JohnWiley & Sons:Chichester, UK, 1996.
27	Miller J. A. ; Klippenstein S. J. J Phys. Chem. A 2003, 107, 2680.
28	Saito K. ; Kakumoto T. ; Murakami I. J Phys. Chem 1984, 88, 1182.
29	Welty, J. R.; Wicks, C. E.; Wilson, R. E.; Rorrer, G. L., Fundamentals of Momentum, Heat and Mass Transfer, 4th ed.; JohnWiley & Sons Ltd.: New York, 2001.
30	Metcalfe W. K. ; Burke S. M. ; Ahmed S. S. ; Curran H. J. Int. J Chem. Kinet 2013, 45, 638.
31	UCSD, The San Diego Mechanism, Version 20141004, 2014.http://maeweb.ucsd.edu/combustion/.
32	Robinson, J. C.; Harris, S. A.; Sun, W.; Sveum, N. E.; Neumark, D. M. J. Am. Chem. Soc. 2002, 124, 10211. doi: 10.1021/ja0127281
33	Dean A. M. J Phys. Chem 1985, 89, 4600.
34	Kossiakoff A. ; Rice F. O. J Am. Chem. Soc 1943, 65, 590.
35	Fabuss B. M. ; Borsanyi A. S. ; Satterfield C. N. ; Lait R. I. ; Smith J. O Ind. Eng. Chem. Process Des. Dev 1962, 1, 293.
36	Wu C. H. ; Kern R. D. J Phys. Chem 1987, 91, 6291.

[1]	Minyi Su,Huisi Liu,Haixia Lin,Renxiao Wang. Machine-Learning Model for Predicting the Rate Constant of ProteinLigand Dissociation [J]. Acta Physico-Chimica Sinica, 2020, 36(1): 1907006-.
[2]	Qian YAO,Li-Juan PENG,Ze-Rong LI,Xiang-Yuan LI. Accurate Calculation of the Energy Barriers and Rate Constants of Hydrogen Abstraction from Alkanes by Hydroperoxyl Radical [J]. Acta Phys. -Chim. Sin., 2017, 33(4): 763-768.
[3]	Hong-Jing YU,Wen-Wen XIA,Li-Guo SONG,Yang DING,Yu HAO,Li-Qiang KANG,Xin-Xiang PAN,Li YAO. Anharmonic Effect of the Decomposition Reaction in High-Temperature Combustion of Monomethylhydrazine Radicals [J]. Acta Phys. -Chim. Sin., 2017, 33(11): 2207-2218.
[4]	Tian-Lei ZHANG,Chen YANG,Xu-Kai FENG,Zhu-Qing WANG,Rui WANG,Qiu-Li LIU,Peng ZHANG,Wen-Liang WANG. Theoretical Study on the Atmospheric Reaction of HS with HO₂: Mechanism and Rate Constants of the Major Channel [J]. Acta Phys. -Chim. Sin., 2016, 32(3): 701-710.
[5]	Yang DING,Li-Guo SONG,Yi-Xuan YU,Li YAO,Sheng-Hsien LIN. Anharmonic Effect of the Decomposition Reaction of Methyl Butanoate [J]. Acta Phys. -Chim. Sin., 2016, 32(11): 2685-2692.
[6]	LI Shang-Jun, TAN Ning-Xin, YAO Qian, LI Ze-Rong, LI Xiang-Yuan. Calculation of Rate Constants for Intramolecular Hydrogen Migration Reactions of Alkylperoxy Radicals [J]. Acta Phys. -Chim. Sin., 2015, 31(5): 859-865.
[7]	GUO Jun-Jiang, HUA Xiao-Xiao, WANG Fan, TAN Ning-Xin, LI Xiang-Yuan. Systematic Approach to Automatic Construction of High-Temperature Combustion Mechanisms of Alkanes [J]. Acta Phys. -Chim. Sin., 2014, 30(6): 1027-1041.
[8]	XU Qiong, ZHANG Tian-Lei, Lü Wen-Bin, WANG Rui, WANG Zhi-Yin, WANG Wen-Liang, WANG Zhu-Qing. Theoretical Study on the effect of a Single Water Molecule on the H₂O₂+Cl Gas Reaction [J]. Acta Phys. -Chim. Sin., 2014, 30(6): 1061-1070.
[9]	HU Ren-Zhi, XIE Pin-Hua, ZHANG Qun, SI Fu-Qi, CHEN Yang. Temperature Dependence of C₂(a³П_u) Radical Reactions with Sulfur Bearing Molecules [J]. Acta Phys. -Chim. Sin., 2014, 30(5): 797-802.
[10]	ZHANG Tian-Lei, WANG Wei-Na, LIU Chang, LU Na, CHEN Miao, GUO Sha, WANG Wen-Liang. Computational Study of the Reaction Mechanism and Kinetics of CH₃CHC(CH₃)COOCH₃ Ozonolysis [J]. Acta Phys. -Chim. Sin., 2013, 29(11): 2313-2320.
[11]	CAO Jia, WANG Wen-Liang, GAO Lou-Jun, FU Feng. Mechanism and Thermodynamic Properties of CH₃SO₃ Decomposition [J]. Acta Phys. -Chim. Sin., 2013, 29(06): 1161-1167.
[12]	HU Ren-Zhi, XIE Pin-Hua, ZHANG Qun, SI Fu-Qi, CHEN Yang. Temperature Dependence of C₂(X¹Σ_g⁺) in Reactions with Unsaturated Hydrocarbons [J]. Acta Phys. -Chim. Sin., 2013, 29(04): 683-688.
[13]	WANG Bi-Yao, TAN Ning-Xin, YAO Qian, LI Ze-Rong, LI Xiang-Yuan. Accurate Calculation of the Reaction Barriers and Rate Constants of the Pyrolysis of Alkyl Radicals in the β Position Using the Isodesmic Reaction Method [J]. Acta Phys. -Chim. Sin., 2012, 28(12): 2824-2830.
[14]	FENG Li-Xia, JIN Ling-Xia, WANG Wei-Na, WANG Wen-Liang. Mechanism and Kinetics of the Hydrogen Abstraction Reaction of C₂H₃ with CH₃F [J]. Acta Phys. -Chim. Sin., 2012, 28(07): 1623-1629.
[15]	HUA Xiao-Xiao, WANG Jing-Bo, WANG Quan-De, TAN Ning-Xin, LI Xiang-Yuan. Mechanism Construction and Simulation for the High-Temperature Combustion of n-Dodecane [J]. Acta Phys. -Chim. Sin., 2011, 27(12): 2755-2761.

Kinetic Calculation and Modeling Study of 1, 3-Butadiene Pyrolysis

RichHTML

PDF

Like

Knowledge

Abstract

Supporting Info

Cite this article

share this article

References

Related Articles 15

Metrics

Recommended 0