Predicting Oligomer/Polymer Compatibility and its Impact on Nanoscale Segregation in Thin Films

Sabattié, Elise; Tasche, Jos; Wilson, Mark Richard; Skoda, Maximilian W.A.; Hughes, Arwel V.; Lindner, Torsten; Thompson, Richard

Abstract

Compatibility between oligomers and polymers was systematically assessed using differential scanning calorimetry (DSC) and correlated with similarity in saturation and solubility parameter. These measurements enabled validation of detailed volume of mixing calculations using Statistical Association Fluid Theory (SAFT-γ Mie) and molecular dynamics (MD) simulations, which can be used to predict behaviour beyond the experimentally accessibly conditions. These simulations confirmed that squalane is somewhat more compatible with poly(isoprene), “PI” than poly(butadiene), “PB”, and further enabled prediction of the temperature dependence of compatibility. Surface and interfacial segregation of a series of deuterated oligomers was quantified in rubbery polymer films PI, PB and hydrogenated poly(isoprene) “hPI”. A striking correlation was established between surface wetting transition and mixtures of low compatibility, such as oligo-dIB in PB or PI. Segregation was quantified normal to the surface by ion beam analysis and neutron reflectometry and in some cases lateral segregation was observable by AFM. While surface segregation is driven by disparity in molecular weight in highly compatible systems this trend reverses as critical point is approached, and surface segregation increases with increasing oligomer molecular weight.

Citation

Sabattié, E., Tasche, J., Wilson, M. R., Skoda, M. W., Hughes, A. V., Lindner, T., & Thompson, R. (2017). Predicting Oligomer/Polymer Compatibility and its Impact on Nanoscale Segregation in Thin Films. Soft Matter, 13(19), 3580-3591. https://doi.org/10.1039/c7sm00048k

• Journal Article Type: Article
• Acceptance Date: Apr 14, 2017
• Online Publication Date: Apr 18, 2017
• Publication Date: May 21, 2017
• Deposit Date: Apr 21, 2017
• Publicly Available Date: Apr 14, 2018
• Journal: Soft Matter
• Print ISSN: 1744-683X
• Electronic ISSN: 1744-6848
• Publisher: Royal Society of Chemistry
• Peer Reviewed: Peer Reviewed
• Volume: 13
• Issue: 19
• Pages: 3580-3591
• DOI: https://doi.org/10.1039/c7sm00048k
• Public URL: https://durham-repository.worktribe.com/output/1388989