Ostwald ripening for designing time-dependent crystal hydrogels

Angew Chem Int Ed Engl. 2024 Apr 22;63(17):e202320095. doi: 10.1002/anie.202320095. Epub 2024 Mar 15.

Abstract

Ostwald ripening (OR), a classic solution theory describing molecular transfer from metastable crystal to stable one, is applied to design time-dependent crystal hydrogels that can automatically change their mechanical properties. Using a system made from crosslinked polyacrylamide (PAM) and sodium acetate (NaAc), we demonstrate that metastable fibrous crystal networks of NaAc preferably form in PAM hydrogels via a polymer-involving mismatch nucleation. These fibrous crystals would undergo OR and evolve into isolated bulk crystals, leading to a significant reduction in material rigidity (179 folds) and interfacial adhesion (20 folds). This transformation can be applied to program time-dependent self-recovery in shape and self-delamination. Since OR is a ubiquitous, robust feature of various crystals, the approach reported here represents a new direction for designing advanced transient soft materials.

Keywords: Ostwald ripening; crystal hydrogel; mechanical properties; mismatch nucleation; time-dependency.