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  1. Abstract

    Achieving a simple yet sustainable printing technique with minimal instruments and energy remains challenging. Here, a facile and sustainable 3D printing technique is developed by utilizing a reversible salting-out effect. The salting-out effect induced by aqueous salt solutions lowers the phase transition temperature of poly(N-isopropylacrylamide) (PNIPAM) solutions to below 10 °C. It enables the spontaneous and instant formation of physical crosslinks within PNIPAM chains at room temperature, thus allowing the PNIPAM solution to solidify upon contact with a salt solution. The PNIPAM solutions are extrudable through needles and can immediately solidify by salt ions, preserving printed structures, without rheological modifiers, chemical crosslinkers, and additional post-processing steps/equipment. The reversible physical crosslinking and de-crosslinking of the polymer through the salting-out effect demonstrate the recyclability of the polymeric ink. This printing approach extends to various PNIPAM-based composite solutions incorporating functional materials or other polymers, which offers great potential for developing water-soluble disposable electronic circuits, carriers for delivering small materials, and smart actuators.

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  2. Free, publicly-accessible full text available March 26, 2025
  3. Stimuli-responsive hydrogels with self-strengthening properties are promising for the use of autonomous growth and adaptation systems to the surrounding environments by mimicking biological materials. However, conventional stimuli-responsive hydrogels require structural destruction to initiate mechanochemical reactions to grow new polymeric networks and strengthen themselves. Here we report continuous self-strengthening of a nanocomposite hydrogel composed of poly( N -isopropylacrylamide) (PNIPAM) and nanoclay (NC) by using external stimuli such as heat and ionic strength. The internal structures of the NC-PNIPAM hydrogel are rearranged through the swelling–deswelling cycles or immersing in a salt solution, thus its mechanical properties are significantly improved. The effects of concentration of NC in hydrogels, number of swelling–deswelling cycles, and presence of salt in the surrounding environment on the mechanical properties of hydrogels are characterized by nanoindentation and tensile tests. The self-strengthening mechanical performance of the hydrogels is demonstrated by the loading ability. This work may offer promise for applications such as artificial muscles and soft robotics. 
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  4. The stimuli-responsive self-folding structure is ubiquitous in nature, for instance, the mimosa folds its leaves in response to external touch or heat, and the Venus flytrap snaps shut to trap the insect inside. Thus, modeling self-folding structures has been of great interest to predict the final configuration and understand the folding mechanism. Here, we apply a simple yet effective method to predict the folding angle of the temperature-responsive nanocomposite hydrogel/elastomer bilayer structure manufactured by 3D printing, which facilitates the study of the effect of the inevitable variations in manufacturing and material properties on folding angles by comparing the simulation results with the experimentally measured folding angles. The defining feature of our method is to use thermal expansion to model the temperature-responsive nanocomposite hydrogel rather than the nonlinear field theory of diffusion model that was previously applied. The resulted difference between the simulation and experimentally measured folding angle ( i.e. , error) is around 5%. We anticipate that our method could provide insight into the design, control, and prediction of 3D printing of stimuli-responsive shape morphing ( i.e. , 4D printing) that have potential applications in soft actuators, robots, and biomedical devices. 
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  5. null (Ed.)