Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation

doi:10.1016/j.cjche.2020.10.033

中国化学工程学报 ›› 2021, Vol. 29 ›› Issue (3): 94-102.DOI: 10.1016/j.cjche.2020.10.033

• Special Issue on Frontiers of Chemical Engineering Thermodynamics • 上一篇下一篇

Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation

Yinbin Wang¹, Senjun Yao², Wei Wang¹, Chenglong Qiu¹, Jing Zhang¹, Shengwei Deng¹, Hong Dong³, Chuan Wu³, Jianguo Wang¹

1 Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China;
2 College of Computer Science and Technology, Zhejiang University of Technology, 310014, China;
3 Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Hangzhou Normal University, 310012, China

收稿日期:2020-09-14 修回日期:2020-10-22 出版日期:2021-03-28 发布日期:2021-05-13
通讯作者: Shengwei Deng, Hong Dong, Jianguo Wang
基金资助:
The authors would like to express appreciation for the support of National Key Research and Development Program of China (Grant No. 2018YFC1902601).

Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation

Yinbin Wang¹, Senjun Yao², Wei Wang¹, Chenglong Qiu¹, Jing Zhang¹, Shengwei Deng¹, Hong Dong³, Chuan Wu³, Jianguo Wang¹

1 Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China;
2 College of Computer Science and Technology, Zhejiang University of Technology, 310014, China;
3 Key Laboratory of Organosilicon Chemistry and Material Technology, Ministry of Education, Hangzhou Normal University, 310012, China

Received:2020-09-14 Revised:2020-10-22 Online:2021-03-28 Published:2021-05-13
Contact: Shengwei Deng, Hong Dong, Jianguo Wang
Supported by:
The authors would like to express appreciation for the support of National Key Research and Development Program of China (Grant No. 2018YFC1902601).

摘要/Abstract

摘要： Styrene-butadiene rubber (SBR) is widely used in tires in the automotive segment and vulcanization using sulfur is a common process to enhance its mechanical properties. However, the addition of sulfur as the cross-linking agent usually results in impurities in pyrolysis products during rubber recycling, and thus the desulfurization during tire pyrolysis attracts much attention. In this work, the pyrolysis of vulcanized SBR is studied in detail with the help of ReaxFF molecular dynamics simulation. A series of crosslinked SBR models were built with different sulfur contents and densities. The following ReaxFF MD simulations were performed to show products distributions at different pyrolysis conditions. The simulation results show that sulfur products distribution is mainly controlled by sulfur contents and temperatures. The reaction mechanism is proposed based on the analysis of sulfur products conversion pathway, where most sulfur atoms are bonded with hydrocarbon radicals and the rest transfer to H₂S. High sulfur contents tend to the formation of elemental sulfur intermediate, and temperature increase facilitates the release of H₂S.

关键词: Pyrolysis, ReaxFF, Molecular simulation, Vulcanized, Styrene-butadiene rubber, Sulfur products

Abstract: Styrene-butadiene rubber (SBR) is widely used in tires in the automotive segment and vulcanization using sulfur is a common process to enhance its mechanical properties. However, the addition of sulfur as the cross-linking agent usually results in impurities in pyrolysis products during rubber recycling, and thus the desulfurization during tire pyrolysis attracts much attention. In this work, the pyrolysis of vulcanized SBR is studied in detail with the help of ReaxFF molecular dynamics simulation. A series of crosslinked SBR models were built with different sulfur contents and densities. The following ReaxFF MD simulations were performed to show products distributions at different pyrolysis conditions. The simulation results show that sulfur products distribution is mainly controlled by sulfur contents and temperatures. The reaction mechanism is proposed based on the analysis of sulfur products conversion pathway, where most sulfur atoms are bonded with hydrocarbon radicals and the rest transfer to H₂S. High sulfur contents tend to the formation of elemental sulfur intermediate, and temperature increase facilitates the release of H₂S.

Key words: Pyrolysis, ReaxFF, Molecular simulation, Vulcanized, Styrene-butadiene rubber, Sulfur products

Yinbin Wang, Senjun Yao, Wei Wang, Chenglong Qiu, Jing Zhang, Shengwei Deng, Hong Dong, Chuan Wu, Jianguo Wang. Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation[J]. 中国化学工程学报, 2021, 29(3): 94-102.

参考文献

[1] J.D. Martínez, N. Puy, R. Murillo, T. García, M.V. Navarro, A.M. Mastral, Waste tyre pyrolysis -A review, Renew. Sustain. Energy Rev. 23 (2013) 179-213.
[2] J.D. Martinez, N. Cardona-Uribe, R. Murillo, T. Garcia, J.M. Lopez, Carbon black recovery from waste tire pyrolysis by demineralization: Production and application in rubber compounding, Waste Manage. 85 (2019) 574-584.
[3] A.M. Cunliffe, P.T. Williams, Composition of oils derived from the batch pyrolysis of tyres, J. Anal. Appl. Pyrolysis. 44 (1998) 131-152.
[4] S.Y. Luo, Y. Feng, The production of fuel oil and combustible gas by catalytic pyrolysis of waste tire using waste heat of blast-furnace slag, Energy Convers. Manage. 136 (2017) 27-35.
[5] T. Kan, V. Strezov, T. Evans, Fuel production from pyrolysis of natural and synthetic rubbers, Fuel 191 (2017) 403-410.
[6] M. Arabiourrutia, G. Lopez, M. Artetxe, J. Alvarez, J. Bilbao, M. Olazar, Waste tyre valorization by catalytic pyrolysis -A review, Renew. Sustain. Energy Rev. 129 (2020) 109932-109955.
[7] L. Asaro, M. Gratton, S. Seghar, N. Aït Hocine, Recycling of rubber wastes by devulcanization, Resour., Conserv. Recycl. 133 (2018) 250-262.
[8] J.-R. Lanteigne, J.-P. Laviolette, J. Chaouki, Behavior of sulfur during the pyrolysis of tires, Energy Fuels 29 (2) (2015) 763-774.
[9] Y.H. Pan, D.C. Yang, K. Sun, X.W. Wang, Y.G. Zhou, Q.X. Huang, Pyrolytic transformation behavior of hydrocarbons and heteroatom compounds of scrap tire volatiles, Fuel 276 (2020) 118095-118105.
[10] F. Murena, Kinetics of sulphur compounds in waste tyres pyrolysis, J. Anal. Appl. Pyrol. 56 (2000) 195-205.
[11] G.-G. Choi, S.-J. Oh, J.-S. Kim, Clean pyrolysis oil from a continuous two-stage pyrolysis of scrap tires using in-situ and ex-situ desulfurization, Energy 141 (2017) 2234-2241.
[12] J. Yu, S. Liu, A. Cardoso, Y. Han, K. Bikane, L.S. Sun, Catalytic pyrolysis of rubbers and vulcanized rubbers using modified zeolites and mesoporous catalysts with Zn and Cu, Energy 188 (2019) 116117-116127.
[13] F. Xu, B. Wang, D. Yang, X. Ming, Y. Jiang, J.H. Hao, Y.Y. Qiao, Y.Y. Tian, TG-FTIR and Py-GC/MS study on pyrolysis mechanism and products distribution of waste bicycle tire, Energy Convers. Manage. 175 (2018) 288-297.
[14] A.C.T. van Duin, S. Dasgupta, F. Lorant, W.A. Goddard III, ReaxFF: A reactive force field for hydrocarbons, J. Phys. Chem. A 9396-9409 (2001).
[15] K. Chenoweth, A.C.T. van Duin, W.A. Goddard III, ReaxFF reactive force field for molecular dynamics simulations of hydrocarbon oxidation, J. Phys. Chem. A 1040-1053 (2008).
[16] T.T. Qi, C.W. Bauschlicher Jr., J.W. Lawson, T.G. Desai, E.J. Reed, Comparison of ReaxFF, DFTB, and DFT for phenolic pyrolysis. 1. Molecular dynamics simulations, J. Phys. Chem. A. 117 (44) (2013) 11115-11125.
[17] G.-Y. Li, F. Wang, J.-P. Wang, Y.-Y. Li, A.-Q. Li, Y.-H. Liang, ReaxFF and DFT study on the sulfur transformation mechanism during the oxidation process of lignite, Fuel 181 (2016) 238-247.
[18] S. Bhoi, T. Banerjee, K. Mohanty, Insights on the combustion and pyrolysis behavior of three different ranks of coals using reactive molecular dynamics simulation, RSC. Adv. 6 (4) (2016) 2559-2570.
[19] F. Castro-Marcano, A.M. Kamat, M.F. Russo, A.C.T. van Duin, J.P. Mathews, Combustion of an Illinois No. 6 coal char simulated using an atomistic char representation and the ReaxFF reactive force field, Combust. Flame 159 (3) (2012) 1272-1285.
[20] C. Chen, L.L. Zhao, J.F. Wang, S.C. Lin, Reactive molecular dynamics simulations of biomass pyrolysis and combustion under various oxidative and humidity environments, Ind. Eng. Chem. Res. 56 (43) (2017) 12276-12288.
[21] X. Wei, H.W. Zhong, Q.R. Yang, E. Yao, Y. Zhang, H.S. Zou, Studying the mechanisms of natural rubber pyrolysis gas generation using RMD simulations and TG-FTIR experiments, Energy Convers. Manage. 189 (2019) 143-152.
[22] S. Deng, H. Zhuo, Y. Wang, S. Leng, G. Zhuang, X. Zhong, Z. Wei, Z. Yao, A.J. Wang, Multiscale simulation on product distribution from pyrolysis of styrene-butadiene rubber, Polymers (Basel). 11 (12) (2019) 1967-1980.
[23] M.J. Frisch, G.W. Trucks, H.B. Schlegel, G.E. Scuseria, M.A. Robb, J.R. Cheeseman, G. Scalmani, V. Barone, B. Mennucci, G.A. Petersson, Gaussian 09, Revision D.01. Gaussian, Inc: Wallingford, CT, 2009.
[24] A. Paajanen, J. Vaari, T. Verho, Crystallization of cross-linked polyethylene by molecular dynamics simulation, Polymer 171 (2019) 80-86.
[25] A. Torres-Knoop, I. Kryven, V. Schamboeck, P.D. Iedema, Modeling the freeradical polymerization of hexanediol diacrylate (HDDA): A molecular dynamics and graph theory approach, Soft Matter 14 (17) (2018) 3404-3414.
[26] H.J. Wang, Y.H. Feng, X.X. Zhang, W. Lin, Y.L. Zhao, Study of coal hydropyrolysis and desulfurization by ReaxFF molecular dynamics simulation, Fuel 145 (2015) 241-248.
[27] C. Ashraf, A. Jain, Y. Xuan, A.C. van Duin, ReaxFF based molecular dynamics simulations of ignition front propagation in hydrocarbon/oxygen mixtures under high temperature and pressure conditions, Phys. Chem. Chem. Phys. 19 (7) (2017) 5004-5017.
[28] M.J. Gao, X.X. Li, L. Guo, Pyrolysis simulations of Fugu coal by large-scale ReaxFF molecular dynamics, Fuel Process. Technol. 178 (2018) 197-205.
[29] A.C. Van Duin, S. Dasgupta, F. Lorant, W.A. Goddard, ReaxFF: A reactive force field for hydrocarbons, J. Phys. Chem. A. 105 (41) (2001) 9396-9409.
[30] R. Chaudret, A. Bick, X. Krokidis, Theoretical modeling of thermal decomposition of methylnaphthalene derivatives: Influence of substituents, Energy Fuels 30 (8) (2016) 6817-6821.
[31] J.P. Larentzos, B.M. Rice, Transferable reactive force fields: Extensions of ReaxFF-lg to nitromethane, J. Phys. Chem. A 121 (9) (2017) 2001-2013.
[32] F. Yin, C. Tang, Y. Tang, Y. Gui, Z. Zhao, Reactive molecular dynamics study of effects of small-molecule organic acids on PMIA thermal decomposition, J. Phys. Chem. B 122 (45) (2018) 10384-10392.
[33] L.Z. Zhang, S.V. Zybin, A.C.T. van Duin, S. Dasgupta, W.A. Goddard III, Carbon cluster formation during thermal decomposition of octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine and 1,3,5-triamino-2,4,6-trinitrobenzene high explosives from ReaxFF reactive molecular dynamics simulations, J. Phys. Chem. A. 113 (2009) 10619-10640.
[34] A. Stukowski, Visualization and analysis of atomistic simulation data with OVITO-the Open Visualization Tool, Modell. Simul. Mater. Sci. Eng. 18 (1) (2010) 015012-015018.
[35] B. Danon, P. van der Gryp, C.E. Schwarz, J.F. Görgens, A review of dipentene (dllimonene) production from waste tire pyrolysis, J. Anal. Appl. Pyrolysis. 112 (2015) 1-13.
[36] J.B. Zhou, Y. Qiao, W.X. Wang, E.W. Leng, J.C. Huang, Y. Yu, M.H. Xu, Formation of styrene monomer, dimer and trimer in the primary volatiles produced from polystyrene pyrolysis in a wire-mesh reactor, Fuel 182 (2016) 333-339.
[37] F.Z. Chen, J.L. Qian, Studies on the thermal degradation of cis-1,4-polyisoprene, Fuel 81 (16) (2002) 2071-2077.

Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation

Pyrolysis of vulcanized styrene-butadiene rubber via ReaxFF molecular dynamics simulation

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