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Vulcanization Accelerators and Silica Coupling Agents in Polyisoprene Melts.

Nikolaos Patsalidis1,2, George J Papakonstantopoulos3, Jan Domurath4

  • 1Chemical and Biomolecular Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States.

The Journal of Physical Chemistry. B
|December 21, 2024
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Understanding vulcanization accelerators like CBS, DBTH, and DPG is key for advanced elastomers. DPG aggregates in polyisoprene, while CBS and DBTH do not. Accelerators strongly bind to silica surfaces, but coupling agents can displace them.

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Area of Science:

  • Polymer Science and Engineering
  • Materials Chemistry
  • Computational Materials Science

Background:

  • Effective dispersion of vulcanization accelerators is essential for optimizing cross-linked elastomer properties.
  • Current elastomer formulations utilize complex mixtures involving silica particles functionalized with coupling agents.

Purpose of the Study:

  • To investigate the molecular properties and self-association behavior of key accelerators: (N-cyclohexyl)-2-benzothiazole sulfenamide (CBS), 1,6-bis(N,N-dibenzylthiocarbamoyldithio)hexane (DBTH), and diphenyl guanidine (DPG) in polyisoprene melts.
  • To determine the affinity of these accelerators for bare and functionalized silica surfaces, considering various coupling agents like MPTES, NXT, and TESPD.
  • To explore the role of DPG in binary DPG-CBS formulations for improved CBS solubility.

Main Methods:

  • Extensive all-atom molecular dynamics simulations were employed to study accelerator behavior in polyisoprene melts.
  • Free energy calculations were used to assess accelerator-substrate affinity at infinite dilution and finite concentrations.
  • Simulations examined interactions with silica surfaces modified with different coupling agents at varying grafting densities.

Main Results:

  • CBS and DBTH exhibit low self-association in polyisoprene, while DPG forms small hydrogen-bonded aggregates.
  • All accelerators show high affinity for silica surfaces, with DPG > CBS > DBTH.
  • Coupling agents can displace accelerators from the silica surface; displacement increases with grafting density and coupling agent size.
  • In DPG-CBS mixtures, DPG acts as a covering agent, enhancing CBS solubility in the polymer matrix.

Conclusions:

  • The molecular interactions and surface affinities of vulcanization accelerators significantly influence elastomer network formation.
  • Understanding accelerator self-association and substrate interactions is crucial for designing high-performance rubber compounds.
  • DPG's ability to solubilize CBS offers a potential strategy for improved accelerator dispersion and elastomer properties.