Mechanics-Switchable and Antiswelling Colloidal Hydrogels Inspired by the Cononsolvency Effect

Stiffness switching hydrogels have been in high demand for intelligent devices, adhesion science, soft robotics, and flexible electronics. However, it is challenging to post-tune the mechanical properties of a hydrogel once the polymer network structure is formed. Inspired by the cononsolvency effect, we prepared a mechanics-switching colloidal hydrogel through the precipitation polymerization of methacrylamide in mixed dimethyl sulfoxide and water solvents. The colloidal network enables the hydrogels to simultaneously strengthen, stiffen, and toughen. The colloidal hydrogels not only display a broad spectrum of adjustable mechanical properties (ranging from 0.08 to 57.1 MPa) via solvent response but also accomplish reversible stiffness conversion through the solvent-tuned conformational adjustment of colloidal polymer networks, with the maximum modulus conversion reaching 1427, and exhibit solvent-responsive shape memory. Based on the stable and tight colloidal network, the hydrogels exhibit antiswelling properties in various aqueous solutions and solvents. The colloidal hydrogel would provide more possibilities in various applications, such as antiimpact protection, shape memory, electronic switches, and intelligent engineering materials. It is envisioned that this work will provide key opportunities in developing mechanics-switching and on-demand tuning of soft materials for tissue engineering, flexible electronics, and biomedical science.