Search for: All records

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. 

Abstract Shape morphing of stimuli‐responsive composite hydrogels has received considerable attention in different research fields. Although various multilayer structures with dissimilar materials are studied to achieve shape morphing, combining swellable hydrogel layers with non‐swellable layers results in issues with interface adhesion and structural integrity. In this study, single‐hydrogel‐based bilayer actuators comprising poly(N‐isopropylacrylamide) (PNIPAM) matrices and graphene oxide (GO)–PNIPAM hinges are presented. Upon temperature rising, the PNIPAM hydrogel acts as the passive layer due to the formation of dense microstructures near the surface (i.e., the skin layer effect), whereas the GO‐PNIPAM hydrogel functions as the active layer, maintaining porous due to structural modification by the presence of GO. Under light exposure, the GO‐PNIPAM hinges experience selective heating due to the photothermal effect of GO. Consequently, the resulting bilayer structures exhibit programmable dual‐responsive 3D shape morphing. Additionally, the folding kinetics of these actuators can be adjusted based on the applied stimulus (temperature changes or light), as they are driven by different mechanisms, the skin layer, or photothermal effects, respectively. Furthermore, the hinge‐based bilayer structures demonstrate walking and steering locomotion by light exposure. This approach can lead to advances in soft robotics, biomimetic systems, and autonomous soft actuators in hydrogel‐based systems. 

Programmable 3D shape morphing of stimuli-responsive hydrogels is of great interest for the fabrication of soft actuators and robots. The corporation of hydrogel matrices and functional additives is discussed in this review. 

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.