- Water-Driven Sol–Gel Transition in Native Cellulose/1-Ethyl-3-methylimidazolium Acetate Solutions doi link

Auteur(s): Mohamed Yunus Roshan Akdar, Koch Marcus, Dieudonne-George P., Truzzolillo D., Colby Ralph, Parisi Daniele

(Article) Publié: Acs Macro Letters, vol. 13 p.219-226 (2024)

Ref HAL: hal-04426657_v1
DOI: 10.1021/acsmacrolett.3c00710
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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.