Simulation of polymerization induced phase separation in model thermosets

Stevens, Mark J.

doi:10.1063/5.0061654

Simulation of polymerization induced phase separation in model thermosets

Journal Article · Wed Aug 04 00:00:00 EDT 2021 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0061654· OSTI ID:1822246

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Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Polymerization induced phase separation (PIPS) in a three component thermoset is studied using molecular dynamics simulations of a new coarse-grained thermoset model. The system includes two crosslinker molecules, which differ in their glass transition temperatures (T_g) and chain length and thus have the potential for phase separation. Here, one crosslinker has a high T_g corresponding to a rubbery behavior, and simulations were performed for a short length (4 beads) and a long length (33 beads). The resin and other crosslinker have low T_g. A coarse-grained model is developed with these features and with interaction parameters determined so that for either rubbery crosslinker length, the system is in the liquid state at the cure temperature. For sufficiently slow reaction rates, the long rubbery molecule exhibits PIPS into a bicontinuous array of nanoscale domains, but the short one does not, reproducing recent experimental results. The simulations demonstrate that the reaction rates must be slow enough to allow diffusion to yield phase separation. Particularly, the reaction rate corresponding to the secondary amine must be very slow, else the structure of crosslinked clusters and the substantially increased diffusion time will prevent PIPS.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: NA0003525; AC52-06NA25396

OSTI ID:: 1822246

Report Number(s):: SAND--2021-9057J; 699849

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 5 Vol. 155; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Simulation of polymerization induced phase separation in model thermosets

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