RT journal article T1 Multifunctional Protein Eutectogels Based on Polyphenolic: Zwitterionic Low-Transition-Temperature Mixtures A1 Martin-Saldaña, S. A1 Sanz de León, Alberto A1 Mata Fernández, María de la A1 Politakos, N. A1 Olmedo-Martínez, J.L. A1 Müller, A.J. A1 Beloqui, A. A1 Calderón, M. A1 Picchio, M.L. A2 Ciencia de los Materiales e Ingeniería Metalúrgica y Química Inorgánica K1 betaine K1 deep eutectic solvents K1 gelatin eutectogels K1 low-transition-temperature mixtures K1 tannic acid AB Low-transition-temperature mixtures (LTTMs) are an exciting class of eutectic solvents that undergo a second-order phase transition (i.e., a glass transition) rather than a typical melting point. Herein, an innovative soft eutectogel is presented incorporating therapeutic LTTMs based on a natural polyphenol and a renewable, non-toxic, and biodegradable zwitterionic compound. This LTTM enables the formation of protein-based elastomers with multiple functional properties, including strong adhesiveness, anti-freezing and anti-drying behavior, high elasticity, water resistance, and anti-inflammatory activity. Notably, It is found that the high polyphenol content in the LTTM completely disrupts protein-protein interactions, hindering the formation of secondary structures essential for gelation in water. Instead, water-mediated protein-polyphenol interactions promote the formation of tough physically crosslinked gels, with the zwitterion playing a key role in preventing excessive binding that would otherwise lead to protein precipitation. Furthermore, the presence of the polyphenol in a dynamic liquid state provides long-lasting stickiness, which is exploited to microstructure the eutectogel surface via the breath figure technique, yielding bilayer functional materials. This study opens a new avenue for designing versatile soft materials from LTTMs, demonstrating how liquefying solid polyphenols can expand the application scope of many multifunctional building blocks. PB John Wiley and Sons Inc SN 1616-3028 YR 2025 FD 2025 LK http://hdl.handle.net/10498/38617 UL http://hdl.handle.net/10498/38617 LA eng DS Repositorio Institucional de la Universidad de Cádiz RD 10-nov-2026