Abstract
Experimental high-pressure phase equilibrium data (cloud point and coexistence data) are reported for solutions of commercial poly(ethyleneco-vinyl acetate) samples in supercritical ethylene and ethylenevinyl acetate (VA) mixtures. These data are correlated with an equation of state rooted in statistical associating fluid theory (SAFT). SAFT captures the effects of polymer MW, incorporated VA%, and free VA on the cloud point pressure, and on the size of the fluid-liquid miscibility gap, over a broad range of temperatures (50–250°C) and polymer concentrations. Free VA is found to behave as a cosolvent (lowering the cloud point pressure), except at low temperatures (< 100°C) and with low VA-containing copolymers, in which case free VA, if present in large excess (> 70 wt.%), behaves as a polar antisolvent due to favorable self-interactions among the free VA molecules. SAFT predicts a shift in the phase transition type, from upper-critical-solution-temperature (UCST), to upper-lower-critical-solution-temperature (U-LCST) with increasing free VA in the monomer mixture.
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