Crystallization-Driven Supramolecular Gelation of Poly(vinyl alcohol) by a Small Catechol Derivative

BONAFÉ ALLENDE, JUAN CRUZ; SCHMARSOW, RUTH N.; MATXINANDIARENA, EIDER; GARCÍA SCHEJTMAN, SERGIO D.; CORONADO, EDUARDO A.; ALVAREZIGARZABAL, CECILIA I.; PICCHIO, MATÍAS L.; MÜLLER, ALEJANDRO J.

MACROMOLECULES

AMER CHEMICAL SOC

Año: 2022 vol. 55 p. 10870 - 10870

0024-9297

atechol-containing molecules have been recognized as versatile building blocks for polymer structures with tailor-made functional properties. While catechol chemistry via metal-ligand coordination, boronate complexation, and oxidation-driven covalent bonds has been well examined in the past, the hydrogen bonding ability of these intriguing molecules has been dismissed. In this research, we investigated the gelation of poly(vinyl alcohol) (PVA) triggered by the crystallization of a 3,4-dihydroxy-catechol in water. Strong hydrogen bond interactions between PVA and catechol groups afforded supramolecular hydrogels with near-covalent elastic moduli, yet dynamic, exhibiting reversible gel-to-sol phase transitions around 50-60 °C. We studied the impact of the catechol derivative concentration on the gelation kinetics and physicochemical properties of these dynamic materials. Isothermal experiments revealed that heterogeneous crystallization governs the gelation kinetics. Moreover, because o