Inorganic/Organic Double-Network Ion Gels with Partially Developed Silica-Particle Network

Tough inorganic/organic composite network gels consisting of a partially developed silica-particle network and a large amount of an ionic liquid, named micro-double-network (μ-DN) ion gel, are fabricated via two methods. One is a one-pot/one-step process conducted using a simultaneous network formation via sol–gel reaction of tetraethyl orthosilicate and free radical polymerization of N,N-dimethylacrylamide in an ionic liquid. When the network formation rates of the inorganic and organic networks are almost the same, the μ-DN structure is formed. The second method is simpler and involved the use of silica nanoparticles as the starting material. By controlling the dispersion state of the silica nanoparticles in an ionic liquid, the μ-DN structure is formed. In both μ-DN ion gels, silica nanoparticles partially aggregate and form network-like clusters. When a large deformation is induced in the μ-DN ion gels, the silica-particle clusters rupture and dissipate the loaded energy. The fracture stress and Young’s modulus of the μ-DN ion gel increase as the size of the silica nanoparticles decreases. The increment in the mechanical strength would have been caused by the increase in the total van der Waals attraction forces and the total number of hydrogen bonding in the silica-particle networks.