Molecular and structural insights into the thermoresponsive behavior of pyrrolidone-based LCST polymers in aqueous solution
Dergunov S.A. Mun G.A. Yermukhambetova B.B. Alikulov A.Z.
19 November 2025Elsevier Ltd
European Polymer Journal
2025#240
Amphiphilic poly(N-vinylpyrrolidone-stat-vinyl phenyl ether) [poly(NVP-stat-VPE)] copolymers were synthesized via microwave-assisted radical polymerization. Copolymers with more than 13 mol% VPE exhibited tunable LCST behavior, with the phase transition temperature decreasing from 55 °C to 27 °C as the hydrophobic content increased. Structural analysis confirmed preferential NVP incorporation and statistical monomer distribution. Combined UV–Vis, DLS, SAXS, and EPR analyses provided a comprehensive understanding of poly(NVP-stat-VPE) copolymers in aqueous solutions, detailing the size and internal composition of intramolecular micelles and aggregates. Reichardts dye probing revealed hydrophobic domain formation, with polarity shifts scaling with VPE content, demonstrating the hydrophobic nature of the VPE core of the self-assembled structures. Spin-probe EPR provided nanoscale insights into local hydration and mobility, indicating gradual dehydration and microviscosity changes above LCST. These results establish poly(NVP-stat-VPE) as a versatile platform for designing thermoresponsive materials with tunable phase behavior and microenvironmental polarity, relevant for applications in soft matter, nanocarriers, and stimuli-responsive systems.
Amphiphilic copolymers , EPR , Microwave-assisted polymerization , Reichardts dye , SAXS , Self-assembly micelles , TEMPO spin probe , Thermoresponsive behavior
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Department of Chemistry, University of Connecticut, 55 North Eagleville Rd, Storrs, 06269-3060, CT, United States
National Engineering Academy of the Republic of Kazakhstan, Almaty, 050010, Kazakhstan
Faculty of Chemistry and Chemical Technology, al-Farabi Kazakh National University, Almaty, 050040, Kazakhstan
Department of Chemistry
National Engineering Academy of the Republic of Kazakhstan
Faculty of Chemistry and Chemical Technology
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