Spider-silk inspired ultrafast alkali-induced molecular aggregation for 3D printing arbitrary tubular hydrogels

Fabricating tubular hydrogel models with arbitrary structural complexity and controllable diameters using an ultrafast, facile yet universal method is desirable for vascular prototypes yet still a great challenge. Herein, inspired by the denaturing ability of spider silks, a novel strategy to induce complexation <i>via</i> applying highly concentrated alkali into a polyvinyl alcohol/ionic liquid (PVA/IL) solution, <i>i.e.</i>, alkali-induced molecular aggregation (AMA), is proposed to achieve such purpose. This strategy enables the rapid and facile fabrication of tubular hydrogel architectures with tunable diameters, controllable thicknesses, and excellent mechanical performance with a tensile strength of up to 1.1 MPa and stretchability exceeding 600%. Importantly, this novel strategy combined with 3D printing facilitates the rapid fabrication of a variety of precise tubular hydrogel models with connected cavity structures which are difficult to achieve using current methods. This ultrafast solidification strategy could also be extended to various alkalis, cations and anions to build different hydrogels, showcasing its versatility and universality. Hence, this strategy can be pioneering to rapidly fabricate complex three-dimensional and hollow enclosed hydrogel models for simulating endovascular interventional therapy.