Mechanical nonreciprocity in a uniform composite material.

Mechanical nonreciprocity, or the asymmetric transmission of mechanical quantities between two points in space, is crucial for developing systems that can guide, damp, and control mechanical energy. We report a uniform composite hydrogel that displays substantial mechanical nonreciprocity, owing to direction-dependent buckling of embedded nanofillers. This material exhibits an elastic modulus more than 60 times higher when sheared in one direction compared with the opposite direction. Consequently, it can transform symmetric vibrations into asymmetric ones that are applicable for mass transport and energy harvest. Furthermore, it exhibits an asymmetric deformation when subjected to local interactions, which can induce directional motion of various objects, including macroscopic objects and even small living creatures. This material could promote the development of nonreciprocal systems for practical applications such as energy conversion and biological manipulation.

Self-Wrinkling in Polyacrylamide Hydrogel Bilayers.

Swelling of a gel film attached to a soft substrate can induce surface instability, which results in the formation of highly ordered patterns such as wrinkles and folds. This phenomenon has been exploited to fabricate functional devices and rationalize morphogenesis. However, obtaining centimeter-scale patterns without immersing the film in a solvent remains challenging. Here, we show that wrinkles with wavelengths of up to a few centimeters can be spontaneously created during the open-air fabrication of film-substrate bilayers of polyacrylamide (PAAm) hydrogels. When the film of an aqueous pregel solution of acrylamide prepared on the PAAm hydrogel substrate undergoes open-air gelation, hexagonally packed dimples initially emerge on the surface, which later evolve into randomly oriented wrinkles. The formation of such self-organized patterns can be attributed to the surface instability resulting from autonomous water transport in the bilayer system during open-air fabrication. The temporal evolution of the patterns can be ascribed to an increase in overstress in the hydrogel film due to continued water uptake. The wrinkle wavelength can be controlled in the centimeter-scale range by adjusting the film thickness of the aqueous pregel solution. Our self-wrinkling method provides a simple mechanism for the generation of swelling-induced centimeter-scale wrinkles without requiring an external solvent, which is unachievable with conventional approaches.

Implicit rule on the elastic function of a swollen polyacrylamide hydrogel.

A full understanding of the elastic properties of hydrogels under swelling is required for their practical application in the chemical and biomedical engineering fields. This is because hydrogels are expected to retain water during mechanical use in moist atmospheres. In the present study, we investigated the relationship between the elastic modulus and the swelling ratio in a specific type of hydrogel (a polyacrylamide gel). The elasticity and swelling data revealed that these two parameters are proportionally related in hydrogels comprising adequate amounts of monomers and crosslinkers. We also demonstrated that this proportional relationship inherently conforms to the linear elastic behaviour predicted by the Flory-Rehner free energy function (the F-R model). The implicit rule is established by the extended F-R model with two scaling exponents. The extended model is capable of representing the irregular elasticity of swollen gels formed from low- or high-molecular-weight polymers.

Evaluation of the effects of cross-linking and swelling on the mechanical behaviors of hydrogels using the digital image correlation method.

Experimental evaluation and modeling are important steps in the investigation of the mechanical behaviors of hydrogels in the small- to large-strain range. In this study, the effects of cross-linking and swelling on the true stress-strain response of a specific type of hydrogel (polyacrylamide) were evaluated using a uniaxial tensile test. The development of true strain on the surface of the hydrogel was measured using the digital image correlation method. The specimens with higher cross-link density exhibited a higher initial elastic modulus and earlier orientation hardening. The initial elastic modulus was reduced by the swelling, whereas the orientation hardening occurred in an earlier strain range in the swollen hydrogel. The mechanical responses of the as-prepared and swollen hydrogels with different cross-linker contents were fitted using a non-Gaussian statistical model. The conventional model underestimated the decrease in the elasticity owing to the swelling effect and overestimated the increase in the stress in the large-strain range. The mechanical model was suitably modified to yield an accurate reproduction of the mechanical responses. The proposed model, which was characterized by five material parameters, was found to reproduce the characteristics of the mechanical responses of the as-prepared and swollen hydrogels with different cross-linker contents.