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Predicting oligomer/polymer compatibility and its impact on nanoscale segregation in thin films.

Sabattié, Elise and Tasche, Jos and Wilson, Mark Richard and Skoda, Maximilian W. A. and Hughes, Arwel V. and Lindner, Torsten and Thompson, Richard (2017) 'Predicting oligomer/polymer compatibility and its impact on nanoscale segregation in thin films.', Soft matter., 13 (19). pp. 3580-3591.


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.

Item Type:Article
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Date accepted:14 April 2017
Date deposited:24 April 2017
Date of first online publication:18 April 2017
Date first made open access:14 April 2018

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