Tuneable phase behaviour and glass transition via polymerization-induced phase separation in crosslinked step-growth polymers

Leguizamon, Samuel C.; Ahn, Juhong; Lee, Sangwoo; Jones, Brad H.

doi:10.1039/d2sm00485b

Tuneable phase behaviour and glass transition via polymerization-induced phase separation in crosslinked step-growth polymers

Journal Article · Mon Jun 06 00:00:00 EDT 2022 · Soft Matter

DOI:https://doi.org/10.1039/d2sm00485b· OSTI ID:1872053

^[1]; Ahn, Juhong ^[2]; ^[2]; ^[1]

Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Rensselaer Polytechnic Institute, Troy, NY (United States)

We report once limited to chain-growth polymerizations, fine control over polymerization-induced phase separation (PIPS) has recently been demonstrated in rubber-toughened thermoset materials formed through step-growth polymerizations. The domain length scales of these thermoset materials can be elegantly tuned by utilizing a binary mixture of curing agents (CAs) that individually yield disparate morphologies. Importantly, varying the composition of the binary mixture affects characteristics of the materials such as glass transition temperature and tensile behavior. Here, we establish a full phase diagram of PIPS in a rubber-toughened epoxy system tuned by a binary CA mixture to provide a robust framework of phase behaviour. X-Ray scattering in situ and post-PIPS is employed to elucidate the PIPS mechanism whereby an initial polymerization-induced compositional fluctuation causes nanoscale phase separation of rubber and epoxy components prior to local chain crosslinking and potential macrophase separation. We further demonstrate the universality of this approach by alternatively employing binary epoxy or binary rubber mixtures to achieve broad variations in morphology and glass transitions.

View Accepted Manuscript (DOE)

Research Organization:: Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)

Grant/Contract Number:: NA0003525; SC0012704; AC02-06CH11357

OSTI ID:: 1872053

Alternate ID(s):: OSTI ID: 1871237

Report Number(s):: SAND2022-7270J; 706848

Journal Information:: Soft Matter, Journal Name: Soft Matter Journal Issue: 23 Vol. 18; ISSN 1744-683X

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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