Facile Preparation of a Photo-Cross-Linked Silk Fibroin-Poly Ionic Liquid Hydrogel with Antifreezing and Ion Conductive Properties

The silk fibroin (SF)/ionic liquid (IL) based hydrogel is a kind of remarkable substrate for flexible devices because of its subzero-temperature elasticity, electrical conductivity, and water retention, although the procedure of the gelation is considered complex and time-consuming. In this work, we introduced an approximate method for the development of novel photo-cross-linked SF/IL hydrogel, that is, SF-IMA/PIL hydrogel via the modification of silk fibroin chain with 2-isocyanatoethyl methacrylate (SF-IMA) in a certain ionic liquid with an unsaturated double bond. The chemical cross-linking between methacrylated SF and IL was triggered by UV light, while the physical cross-linking of the hydrogel was attributed to the β-sheet formation of SF in SF-IMA/IL mixed solution. In addition to being a UV-induced three-dimensional (3D) printable one, the SF-IMA/PIL hydrogel performed significant ionic conductivity between room temperature and −50 °C and water retention within a wide range of relative humidity, which were the featured advantages as the ionic liquid involved. Moreover, the static and dynamic mechanical tests demonstrated that the hydrogel reserved its great elasticity at −50 °C and displayed its stiffness transition temperatures between −100 and −70 °C.