Freezing Molecular Orientation under Stretch for High Mechanical Strength but Anisotropic Hydrogels

Abstract

The poor mechanical strength of hydrogels has largely limited their wide applications, and improving hydrogels' mechanical strength is a hot and important topic in the hydrogel research field. Although many successful strategies have been proposed to improve hydrogels' mechanical strength during the past decades, a hydrogel with a tensile stress surpassing dozens of mega Pascal is desirable, yet still a big challenge. To address this issue, the Fe(3+) -mediated physical crosslinking formed under stretch conditions was employed in a chemically crosslinked poly (acrylamide-co-acrylic acid) network to achieve a dual-crosslinked hydrogel. The expected molecular orientation occurs under stretch and allows the maximumu chelating interaction between pendant carboxylic anions and Fe(3+) and molecules conformation being frozen, leading to the mechanical strength improving dramatically. As a result, an unprecedentedly high mechanical strength, but anisotropic dual-crosslinked hydrogel was obtained. By optimizing the experimental parameters, the nominal tensile stress along pre-stretching direction can reach as high as ≈40 MPa with elastic modulus of ≈40 MPa at large strain (>200%). In addition, the molecular orientation also leads to big difference of mechanical performance between parallel and perpendicular direction.