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

doi:10.1016/j.cjche.2020.10.033

Chinese Journal of Chemical Engineering ›› 2021, Vol. 29 ›› Issue (3): 94-102.DOI: 10.1016/j.cjche.2020.10.033

Previous Articles Next Articles

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:2021-05-13 Published:2021-03-28
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).

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

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).

Abstract

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

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

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]. Chinese Journal of Chemical Engineering, 2021, 29(3): 94-102.

References

[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

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

References

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	Yuehua Liu, Lili Chen, Shoujun Liu, Song Yang, Ju Shangguan. Role of iron-based catalysts in reducing NO_x emissions from coal combustion [J]. Chinese Journal of Chemical Engineering, 2023, 59(7): 1-8.
[2]	Wei Wang, Romain Lemaire, Ammar Bensakhria, Denis Luart. Thermogravimetric analysis and kinetic modeling of the co-pyrolysis of a bituminous coal and poplar wood [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 53-68.
[3]	Xinyu Liu, Hongliang Sheng, Song He, Chunhua Du, Yuansheng Ma, Chichi Ruan, Chunxiang He, Huaming Dai, Yajun Huang, Yuelei Pan. Insight into pyrolysis of hydrophobic silica aerogels: Kinetics, reaction mechanism and effect on the aerogels [J]. Chinese Journal of Chemical Engineering, 2023, 58(6): 266-281.
[4]	Haodi Tan, Minjiao Yang, Yingquan Chen, Xu Chen, Francesco Fantozzi, Pietro Bartocci, Roman Tschentscher, Federica Barontini, Haiping Yang, Hanping Chen. Preparation of aromatic hydrocarbons from catalytic pyrolysis of digestate [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 1-9.
[5]	Huan-Huan Yin, Yin-Lei Han, Xiao Yan, Yi-Xin Guan. Proanthocyanidins prevent tau protein aggregation and disintegrate tau filaments [J]. Chinese Journal of Chemical Engineering, 2023, 57(5): 63-71.
[6]	Qiaoqiao Liu, Guihong Lin, Jian Zhou, Liangliang Huang, Chang Liu. Hydrogen-bond mediated and concentrate-dependent NaHCO₃ crystal morphology in NaHCO₃–Na₂CO₃ aqueous solution: Experiments and computer simulations [J]. Chinese Journal of Chemical Engineering, 2023, 55(3): 49-58.
[7]	Baodong Zhao, Yinglei Wang, Fulei Gao, Yajing Liu, Weixiao Liu, Feng Ding. Understanding the alkyl effect of geminal dinitropropyl ester energetic plasticizers on hydroxyl terminated polybutadiene (HTPB): Simultaneous tuning on low temperature behavior and processability [J]. Chinese Journal of Chemical Engineering, 2023, 54(2): 364-371.
[8]	Xueguang Li, Mengyan Yu, Changfa Zhang, Xiangtong Li, Guangqing Liu, Jianjun Dai, Chunbao Zhou, Yang Liu, Jie Fu, Yingwen Zhang, Bang Yao. Co-pyrolysis of soybean soapstock with iron slag/aluminum scrap, and characterization and analysis of their products [J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 25-36.
[9]	Peng Yang, Shengzhe Jia, Yan Wang, Zongqiu Li, Songgu Wu, Jingkang Wang, Junbo Gong. Dissolution behavior, thermodynamic and kinetic analysis of malonamide by experimental measurement and molecular simulation [J]. Chinese Journal of Chemical Engineering, 2023, 53(1): 260-269.
[10]	Linyang Wang, Qiang Wang, Yongqi Liu, Qiuxiang Yao, Ming Sun, Xiaoxun Ma. Catalytic conversion of asphaltenes to BTXN using metal-loaded modified HZSM-5 [J]. Chinese Journal of Chemical Engineering, 2022, 49(9): 253-264.
[11]	Xiaobin Chen, Yuting Tang, Chuncheng Ke, Chaoyue Zhang, Sichun Ding, Xiaoqian Ma. CO₂ capture by double metal modified CaO-based sorbents from pyrolysis gases [J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 40-49.
[12]	Hojatollah Moradi, Hedayat Azizpour, Hossein Bahmanyar, Mohammad Emamian. Molecular dynamic simulation of carbon dioxide, methane, and nitrogen adsorption on Faujasite zeolite [J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 70-76.
[13]	Shaoxiang Cai, Han Yan, Qiuyi Wang, He Han, Ru Li, Zhichao Lou. Top-down strategy for bamboo lignocellulose-derived carbon heterostructure with enhanced electromagnetic wave dissipation [J]. Chinese Journal of Chemical Engineering, 2022, 43(3): 360-369.
[14]	Tongan Yan, Minman Tong, Qingyuan Yang, Dahuan Liu, Yandong Guo, Chongli Zhong. Large-scale simulations of CO₂ diffusion in metal-organic frameworks with open Cu sites [J]. Chinese Journal of Chemical Engineering, 2022, 42(2): 1-9.
[15]	Puxu Liu, Yong Wang, Yang Chen, Xiaoqing Wang, Jiangfeng Yang, Libo Li, Jinping Li. Stable titanium metal-organic framework with strong binding affinity for ethane removal [J]. Chinese Journal of Chemical Engineering, 2022, 42(2): 35-41.