Facile preparation, rapid actuating, and versatile actions are great challenges in exploring new kinds of hydrogel actuators. In this paper, we presented a facile sticking method to prepare Janus bilayer and multilayer hydrogel actuators that benefited from a special tough and adhesive PAA-clay hydrogel. Combining physical and chemical cross-linking reagents, we endowed the PAA gel with both toughness and adhesion. This PAA gel was reinforced by further cross-linking with Fe. These two hydrogels with different cross-linking densities exhibited different swelling capabilities and moduli in the media manipulated by pH and ionic strength, thus acting as promising candidates for soft actuators. On the basis of these gels, we designed hydrogel actuators of rapid response in several minutes and precisely controlled actuating direction by sticking two hydrogel layers together. Elaborate soft actuators such as bidirectional bending flytrap, gel hand with grasp, open, and gesturing actions as well as word-writing actuator were prepared. This method could be generalized by using other stimuli-responsive hydrogels combined with the adhesive PAA gel, which would open a new way to programmable and versatile soft actuators.

Shape memory hydrogels containing over 76 wt % of water were synthesized in a one-pot method, and interpenetrating double network was formed by physically cross-linked gelatin network and chemically cross-linked polyacrylamide (PAM) network with graphene oxide (GO). The temporary shape was quickly fixed by cooling in ice water for 30 s after deformation at 80 °C for 10 s. Shape recovery started in 10 s under near-infrared (NIR) irradiation and almost completed within 60 s depending on the curling angle. A small amount of GO in the hydrogels (≤1.5 mg/mL) played a key role in NIR energy absorption and transformation into thermal energy. The hydrogel without GO showed no response to the NIR irradiation and cannot recover to its permanent shape by NIR irradiation. Temperature sweep was conducted in the cycle of 20 °C → 80 °C → 20 °C, and the structure change in the hydrogels with temperature was investigated according to the storage modulus G' and tangent of the loss angle tan δ as a function of the hydrogel composition. The shape-memory capability was confirmed as the contribution from the triple-helix cross-linking network of gelatin. High mechanical toughness (strength > 400 kPa and broken strain > 500%) was achieved by the double-network with the sacrificial gelatin network and GO bridging to dissipate deformation energy. The optimized composition of the hydrogel was found to be a key point to realize stable temporary shape and rapid recovery to the permanent shape controlled by NIR irradiation with reasonable strength. The facile preparation and noncontact gentle stimulus of the present hydrogel hold great potential to be used in soft actuator materials.

Rapid response and strong mechanical properties are desired for smart materials used in soft actuators. A bioinspired hybrid hydrogel actuator was designed and prepared by series combination of three trunks of tough polymer-clay hydrogels to accomplish the comprehensive actuation of "extension-grasp-retraction" like a fishing rod. The hydrogels with thermo-creep and thermo-shrinking features were successively irradiated by near-infrared (NIR) to execute extension and retraction, respectively. The GO in the hydrogels absorbed the NIR energy and transformed it into thermo-energy rapidly and effectively. The hydrogel with adhesion or magnetic force was adopted as the "hook" of the hybrid hydrogel actuator for grasping object. The hook of the hybrid hydrogel actuator was replaceable according to applications, even with functional materials other than hydrogels. This study provides an innovative concept to explore new soft actuators through combining response hydrogels and programming the same stimulus.

A multiple shape memory and self‐healing poly(acrylic acid)‐graphene oxide‐Fe3+ (PAA‐GO‐Fe3+) hydrogel with supertough strength is synthesized containing dual physically cross‐linked PAA network by GO and Fe3+. The first GO cross‐linked hydrogel can be reversibly reinforced by immersing in FeCl3/HCl and pure water and softened by immersing in HCl. The tensile strength is 2.5 MPa with the break strain of 700%. Multiple shape memory capability is found depending on this unique feature, the hydrogel can be fixed in four temporary shapes by adjusting the immersing time in FeCl3/HCl and pure water, and recovered in sequence by immersing in HCl. This hydrogel also exhibits perfect self‐healing behavior, the cut as‐prepared hydrogel is almost completely healed by immersing in FeCl3/HCl. Besides, the hydrogel shows enhanced electrical conductivity with the presence of GO and Fe3+. This supertough hydrogel provides a new way to design soft actuators.

Dopamine-containing hydrogels were synthesized by copolymerization of dopamine methacrylamide (DMA), N,N-dimethylacrylamide (DMAA), and an N,N'-methylenebisacrylamide (BIS) crosslinker in a mixed solvent of water and DMSO. The association of DMA was formed by simply immersing in water to facilely reinforce the hydrogel due to the introduction of the second physical crosslinking. The tensile strength of the hydrogels was increased greatly and regulated in a wide range from 200 kPa to over 2 MPa. The association of DMA was destroyed upon immersing in DMSO. This reversible formation and dissociation of the association structure endowed the hydrogel with shape memory and actuating capabilities. Rapid shape fixing in water and complete shape recovery in DMSO was realized within several minutes. Bioinspired functional soft actuators were designed based on the reversible association and metal ion coordination of DMA, including fast responsive hydrogel tentacles, programable multiple shape change, reversible and versatile painting and writing "hydrogel paper". The facile preparation and strength regulation provide a new way to design novel soft actuators through solvent exchange, and will inspire more complex applications upon combining the association with other properties of mussel inspired dopamine derivatives.

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