Abstract

Integrating both green forming character and multifunctionality for physically crosslinked hydrogel fibers is challenging, but intensively desirable for emerging applications. Herein, the amorphous multi-scale structure for continuously spinning polyvinyl alcohol (PVA) hydrogel fibers is achieved with an innovatively suppressed-freezing strategy. In particular, the antifreezing salt with salting-in effect is introduced into precursor solution, in which an exceptionally homogeneous yet weak approach of polymer chains is available under weakened repelling behavior of ice crystals using liquid nitrogen as the coagulation bath. Hence, a totally amorphous network with release of free hydroxyl groups is constructed for freeze-thawed PVA hydrogel fibers, which is further stabilized by water evaporation induced densification of polymer network. Such particular multi-scale structure interestingly endows the physical hydrogel fibers with tunable mechanical properties of superior extendibility, flexibility and elasticity in a wide range, along with integrated properties of excellent transparency, antifreezing and long-term stability. Moreover, the hydrogel fibers could be knitted into fabric-like materials with arbitrary shapes, of which the extendibility and toughness are tremendously improved. Notably, benefiting from the high transparency and homogeneous structure, the physical fibers and the corresponding fabrics demonstrate light transmittance ability and deformation responsiveness, which retains even in extreme condition (−196 °C). Together with ionic-conductivity, the PVA hydrogel fibers/fabrics as strain sensors intriguingly represent conductive/optical multi-mode sensations, which are capable of dynamically monitoring subtle and sophisticated human movements. The combined advantages enable this new generation of physical hydrogel fibers to promise potential for applications in wearable electronics, biomedicine, and information transmission.

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