Bayesian tuned kinetic Monte Carlo modeling of polystyrene pyrolysis : unraveling the pathways to its monomer, dimers, and trimers formation
| العنوان: | Bayesian tuned kinetic Monte Carlo modeling of polystyrene pyrolysis : unraveling the pathways to its monomer, dimers, and trimers formation |
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| المؤلفون: | Onur Dogu, Andreas Eschenbacher, Robin John Varghese, Maarten Dobbelaere, Dagmar R. D'hooge, Paul H.M. Van Steenberge, Kevin M. Van Geem |
| المصدر: | CHEMICAL ENGINEERING JOURNAL |
| بيانات النشر: | Elsevier BV, 2023. |
| سنة النشر: | 2023 |
| مصطلحات موضوعية: | Chemistry, Chemical recycling, Kinetic modeling, General Chemical Engineering, Thermal degradation, Environmental Chemistry, General Chemistry, Diels-Alder dimerization, Polystyrene, Industrial and Manufacturing Engineering, Bayesian optimization |
| الوصف: | The current kinetic models for polystyrene (PS) pyrolysis contain many simplifications to reduce their size and the corresponding simulation time. Moreover, they are often based on rate coefficients determined using non -ideal experimental data featuring ambiguous process conditions with respect to mixing and temperature uni-formity. The practical interest of PS pyrolysis is the production of styrene monomer to be reused as a feedstock in the polymerization of styrene. In the present work, a lab-scale tree-based kinetic Monte Carlo (kMC) model is presented that differentiates between 18 reaction families and 26 end-group pairs to study the product yield variations for thermal degradation of PS. Model parameters follow from Bayesian optimization to experimental data recorded with an in-house micro-pyrolysis unit coupled with comprehensive two-dimensional gas chro-matography. Low chain length (CL) anionic-made PS is specifically considered to gain an understanding of the role of specific end-groups. The experimental yields of the major products (monomer: 74.7-80.8 wt%, dimer: 5.1-5.5 wt%, trimer: 1.6-7.7 wt%) are well-predicted with the fine-tuned parameters. The main reaction pathway in the formation of styrene monomer is end-chain beta-scission, while mid-chain beta-scission is primarily involved in the formation of the styrene dimer and trimer. Our model shows that the pyrolysis of low CL anionic-made PS leads to better rate coefficients than those obtained from state-of-the-art pyrolysis of long CL PS, in which end-groups play a much smaller role. |
| وصف الملف: | application/pdf |
| اللغة: | English |
| تدمد: | 1385-8947 1873-3212 |
| URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::8de8a696bb16caef34669d45d6140b11 https://hdl.handle.net/1854/LU-01GPE3CXP8D50YERZKH8SCZN3M |
| حقوق: | RESTRICTED |
| رقم الأكسشن: | edsair.doi.dedup.....8de8a696bb16caef34669d45d6140b11 |
| قاعدة البيانات: | OpenAIRE |
| تدمد: | 13858947 18733212 |
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