%0 Journal Article %T Water-Driven Sol–Gel Transition in Native Cellulose/1-Ethyl-3-methylimidazolium Acetate Solutions %+ University of Groningen [Groningen] %+ Leibniz Institute for New Materials (INM) %+ Laboratoire Charles Coulomb (L2C) %+ Pennsylvania State University (Penn State) %A Mohamed Yunus, Roshan Akdar %A Koch, Marcus %A Dieudonné-George, Philippe %A Truzzolillo, Domenico %A Colby, Ralph, H %A Parisi, Daniele %< avec comité de lecture %@ 2161-1653 %J ACS Macro Letters %I Washington, D.C : American Chemical Society %V 13 %P 219-226 %8 2024 %D 2024 %R 10.1021/acsmacrolett.3c00710 %Z Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft] %Z Chemical Sciences/PolymersJournal articles %X The addition of water to native cellulose/1-ethyl-3methylimidazolium acetate solutions catalyzes the formation of gels, where polymer chain-chain intermolecular associations act as cross-links. However, the relationship between water content (Wc), polymer concentration (Cp), and gel strength is still missing. This study provides the fundamentals to design water-induced gels. First, the sol-gel transition occurs exclusively in entangled solutions, while in unentangled ones, intramolecular associations hamper interchain cross-linking, preventing the gel formation. In entangled systems, the addition of water has a dual impact: at low water concentrations, the gel modulus is water-independent and controlled by entanglements. As water increases, more cross-links per chain than entanglements emerge, causing the modulus of the gel to scale as Gp ∼ C p^2 Wc^3.0±0.2. Immersing the solutions in water yields hydrogels with noncrystalline, aggregate-rich structures. Such water-ionic liquid exchange is examined via Raman, FTIR, and WAXS. Our findings provide avenues for designing biogels with desired rheological properties. %G English %2 https://hal.science/hal-04426657/document %2 https://hal.science/hal-04426657/file/ACS-MacroLetters-2024-Daniele.pdf %L hal-04426657 %U https://hal.science/hal-04426657 %~ CNRS %~ L2C %~ UNIV-MONTPELLIER %~ UM-2015-2021 %~ UM-EPE