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Explicit stochastic modeling of termination chain length dependencies for all disparate radical pairs in single phase free radical induced grafting

Freddy L. Figueira (UGent) , Alessandro Trigilio (UGent) , Yi-Yang Wu, Yin-Ning Zhou, Zheng-Hong Luo, Paul Van Steenberge (UGent) and Dagmar D'hooge (UGent)
(2023) CHEMICAL ENGINEERING JOURNAL. 452(Part 3).
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Abstract
In radical (co)polymerization and polymer recycling processes with branch and crosslinking formation easily more than two macroradical types exist, defining a variety of termination reaction possibilities. However, in many kinetic modeling studies the termination of each distinct radical pair is described by the same average (apparent) rate coefficient formula, only acknowledging polymer mass fraction variations but ignoring chain length dependencies. In the present work, it is demonstrated that coupled matrix-based Monte Carlo (CMMC) simulations can reliably predict the termination behavior of distinct radical pairs. This is illustrated for freeradical induced grafting (FRIG) of polybutadiene with styrene, distinguishing six termination (by recombination) reaction channels as defined by (conventional) polystyrene radicals, polybutadiene mid-chain radicals, and grafted end-chain radicals. Model validation is uniquely performed under both free radical polymerization (FRP) and FRIG conditions, highlighting that the CMMC simulations should be applied with the so-called shooting method, in which each average apparent termination rate coefficient is updated per reaction event to capture to dynamic changes of all chain length distributions in the FRIG process. These updates should be done based on the composite kt (diffusion) model while considering better-tuned chain transfer kinetic parameters, as recommended based on recent developments in the polymer reaction engineering field. It is showcased that the FRIG reaction conditions have a clear impact on the kinetic importance of all radical types and their termination pattern determining the evolution of the bimodal log-molar mass distribution. The current work further enhances the stochastic modeling field to accurately represent (de)polymerization kinetics with several macroradical types and topological variations.
Keywords
Industrial and Manufacturing Engineering, General Chemical Engineering, Environmental Chemistry, General Chemistry, Graft copolymers, kinetic Monte Carlo, Diffusion model, Apparent, kinetics, Radical chemistry, TWIN-SCREW EXTRUDER, POLYMER-SOLVENT SYSTEMS, BULK-POLYMERIZATION, DIFFUSION-COEFFICIENTS, METHYL-METHACRYLATE, MATHEMATICAL-MODEL, MALEIC-ANHYDRIDE, INTERNAL MIXER, SELF-DIFFUSION, STYRENE

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MLA
Figueira, Freddy L., et al. “Explicit Stochastic Modeling of Termination Chain Length Dependencies for All Disparate Radical Pairs in Single Phase Free Radical Induced Grafting.” CHEMICAL ENGINEERING JOURNAL, vol. 452, no. Part 3, 2023, doi:10.1016/j.cej.2022.139389.
APA
Figueira, F. L., Trigilio, A., Wu, Y.-Y., Zhou, Y.-N., Luo, Z.-H., Van Steenberge, P., & D’hooge, D. (2023). Explicit stochastic modeling of termination chain length dependencies for all disparate radical pairs in single phase free radical induced grafting. CHEMICAL ENGINEERING JOURNAL, 452(Part 3). https://doi.org/10.1016/j.cej.2022.139389
Chicago author-date
Figueira, Freddy L., Alessandro Trigilio, Yi-Yang Wu, Yin-Ning Zhou, Zheng-Hong Luo, Paul Van Steenberge, and Dagmar D’hooge. 2023. “Explicit Stochastic Modeling of Termination Chain Length Dependencies for All Disparate Radical Pairs in Single Phase Free Radical Induced Grafting.” CHEMICAL ENGINEERING JOURNAL 452 (Part 3). https://doi.org/10.1016/j.cej.2022.139389.
Chicago author-date (all authors)
Figueira, Freddy L., Alessandro Trigilio, Yi-Yang Wu, Yin-Ning Zhou, Zheng-Hong Luo, Paul Van Steenberge, and Dagmar D’hooge. 2023. “Explicit Stochastic Modeling of Termination Chain Length Dependencies for All Disparate Radical Pairs in Single Phase Free Radical Induced Grafting.” CHEMICAL ENGINEERING JOURNAL 452 (Part 3). doi:10.1016/j.cej.2022.139389.
Vancouver
1.
Figueira FL, Trigilio A, Wu Y-Y, Zhou Y-N, Luo Z-H, Van Steenberge P, et al. Explicit stochastic modeling of termination chain length dependencies for all disparate radical pairs in single phase free radical induced grafting. CHEMICAL ENGINEERING JOURNAL. 2023;452(Part 3).
IEEE
[1]
F. L. Figueira et al., “Explicit stochastic modeling of termination chain length dependencies for all disparate radical pairs in single phase free radical induced grafting,” CHEMICAL ENGINEERING JOURNAL, vol. 452, no. Part 3, 2023.
@article{01H6EAVCQT8N88NB5J0RM9XH1Q,
  abstract     = {{In radical (co)polymerization and polymer recycling processes with branch and crosslinking formation easily more than two macroradical types exist, defining a variety of termination reaction possibilities. However, in many kinetic modeling studies the termination of each distinct radical pair is described by the same average (apparent) rate coefficient formula, only acknowledging polymer mass fraction variations but ignoring chain length dependencies. In the present work, it is demonstrated that coupled matrix-based Monte Carlo (CMMC) simulations can reliably predict the termination behavior of distinct radical pairs. This is illustrated for freeradical induced grafting (FRIG) of polybutadiene with styrene, distinguishing six termination (by recombination) reaction channels as defined by (conventional) polystyrene radicals, polybutadiene mid-chain radicals, and grafted end-chain radicals. Model validation is uniquely performed under both free radical polymerization (FRP) and FRIG conditions, highlighting that the CMMC simulations should be applied with the so-called shooting method, in which each average apparent termination rate coefficient is updated per reaction event to capture to dynamic changes of all chain length distributions in the FRIG process. These updates should be done based on the composite kt (diffusion) model while considering better-tuned chain transfer kinetic parameters, as recommended based on recent developments in the polymer reaction engineering field. It is showcased that the FRIG reaction conditions have a clear impact on the kinetic importance of all radical types and their termination pattern determining the evolution of the bimodal log-molar mass distribution. The current work further enhances the stochastic modeling field to accurately represent (de)polymerization kinetics with several macroradical types and topological variations.}},
  articleno    = {{139389}},
  author       = {{Figueira, Freddy L. and Trigilio, Alessandro and Wu, Yi-Yang and Zhou, Yin-Ning and Luo, Zheng-Hong and Van Steenberge, Paul and D'hooge, Dagmar}},
  issn         = {{1385-8947}},
  journal      = {{CHEMICAL ENGINEERING JOURNAL}},
  keywords     = {{Industrial and Manufacturing Engineering,General Chemical Engineering,Environmental Chemistry,General Chemistry,Graft copolymers,kinetic Monte Carlo,Diffusion model,Apparent,kinetics,Radical chemistry,TWIN-SCREW EXTRUDER,POLYMER-SOLVENT SYSTEMS,BULK-POLYMERIZATION,DIFFUSION-COEFFICIENTS,METHYL-METHACRYLATE,MATHEMATICAL-MODEL,MALEIC-ANHYDRIDE,INTERNAL MIXER,SELF-DIFFUSION,STYRENE}},
  language     = {{eng}},
  number       = {{Part 3}},
  pages        = {{18}},
  title        = {{Explicit stochastic modeling of termination chain length dependencies for all disparate radical pairs in single phase free radical induced grafting}},
  url          = {{http://doi.org/10.1016/j.cej.2022.139389}},
  volume       = {{452}},
  year         = {{2023}},
}
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