Spin-coating-assisted fabrication of ultrathin physical hydrogel films with high toughness and fast response

Hydrogel films have promising applications in medical dressings, flexible electronics, etc. However, it is challenging to fabricate ultrathin hydrogel films with high toughness and controllable thickness. Here, we report a facile approach to prepare tough physical hydrogel films by spin-coating of a poly(acrylic acid-co-acrylamide) (P(AAc-co-AAm)) solution and subsequent gelation in FeCl3 solution to form carboxyl-Fe3+ coordination complexes. The thickness of the obtained gel films, ranging from several to hundreds of micrometers, was easily tunable by adjusting the spin conditions and polymer concentration. The thus obtained hydrogel films showed excellent mechanical properties, with tensile breaking strengths of 0.6-14.5 MPa, breaking strains of 140-840%, Young's moduli of 0.1-61.7 MPa, and tearing fracture energies of 300-1300 J m-2. Based on this approach, responsive tough hydrogel films can also be prepared by spin-coating of a poly(acrylic acid-co-N-isopropylacrylamide) (P(AAc-co-NIPAm)) solution. The obtained gel films showed a fast response (<60 s) and a large output force (∼0.2 MPa) triggered by a concentrated saline solution, making them an ideal material in the design of chemomechanical devices. Furthermore, a bilayer hydrogel film was fabricated by two-step spin-coating of P(AAc-co-NIPAm) and P(AAc-co-AAm) solutions, which showed reversible bending deformation under external stimuli. This simple yet effective approach should be applicable to other systems to prepare versatile hydrogel films with tunable thickness and promising applications in diverse areas.