Hydrogel Actuators Research Articles

Bioinspired Genetic and Chemical Engineering of Protein Hydrogels for Programable Multi-Responsive Actuation.

Protein hydrogels with tailored stimuli-responsive features and tunable stiffness have garnered considerable attention due to the growing demand for biomedical soft robotics. However, integrating multiple responsive features toward intelligent yet biocompatible actuators remains challenging. Here, a facile approach that synergistically combines genetic and chemical engineering for the design of protein hydrogel actuators with programmable complex spatial deformation is reported. Genetically engineered silk-elastin-like proteins (SELPs) are encoded with stimuli-responsive motifs and enzymatic crosslinking sites via simulation-guided genetic engineering strategies. Chemical modifications of the recombinant proteins are also used as secondary control points to tailor material properties, responsive features, and anisotropy in SELP hydrogels. As a proof-of-concept example, diazonium coupling chemistry is exploited to incorporate sulfanilic acid groups onto the tyrosine residues in the elastin domains of SELPs to achieve patterned SELP hydrogels. These hydrogels can be programmed to perform various actuations, including controllable bending, buckling, and complex deformation under external stimuli, such as temperature, ionic strength, or pH. With the inspiration of genetic and chemical engineering in natural organisms, this work offers a predictable, tunable, and environmentally sustainable approach for the fabrication of programmed intelligent soft actuators, with implications for a variety of biomedical materials and biorobotics needs.

Multiresponsive Bilayer Hydrogel Actuator with Switchable Shape Morphing Capability and Visible Color/Fluorescence Change.

Bilayer hydrogels, endowed with multiresponsive and switchable color-changing properties, have garnered significant attention for bioinspired artificial intelligent materials. However, the design and fabrication of such hydrogels that can fully mimic the adaptation of the live organism, i.e., simultaneous changes in shape, fluorescent, and/or visible color, still remain significant challenges. Herein, a multiresponsive (e.g., temperature, salt, and pH) and multiadaptive (shape, fluorescent color, and visible color changes) hydrogel was fabricated by employing monomers featuring pH-responsive fluorescence 4-(2-(4-(dimethylamino) phenyl)-1-isocyanovinyl) phenol (DP) and switchable color-changing 4-(2-sulfethyl) -1-(4-vinylbenzyl) pyridinium betaine (VPES). The bilayer hydrogel comprises a temperature- and pH-responsive gel layer, poly(N-isopropylacrylamide-co-2-(dimethylamino) ethyl methacrylate), along with a pH-, temperature-, and salt-responsive gel layer, poly(acrylamide-co-2-(dimethylamino)ethyl methacrylate-co-VPES)@DP. Due to the opposite swelling/shrinking behavior between the two layers, the prepared hydrogel exhibits shape changes in response to thermal, salt, and pH stimuli, along with switchable fluorescent color and visible color change that originate from DP and polyVPES, respectively. Apart from multiresponsive behavior, this hydrogel also shows an excellent antifatigue property and high sensitivity, which makes it hold significant potential in many applications. We anticipate that this strategy to realize multiresponsive capability in this work can also inspire the design of the biomimetic smart materials.

Thermo-hardening hydrogel actuators as self-locking grippers

Thermo-hardening hydrogel actuators as self-locking grippers

Light‐activated 3D printed fish‐like actuator

AbstractHydrogel‐based actuators are innovative materials that exhibit responsive and dynamic behavior in response to external stimuli, making them promising candidates for a wide range of applications in fields such as soft robotics. We employ 3D printing to create layered rectangles, using a passive ink composed of gelatin methacryloyl (GelMA) and an active ink consisting of GelMA and poly(N‐isopropylacrylamide) (PNIPAM). Our aim is to assess and compare the bending capabilities of these structures based on their layer arrangements in a buffer above the lower critical solution temperature. Therefore, an asymmetric rectangular structure is selected as the shape‐changing component in the tail of a 3D printed fish‐shaped hydrogel actuator. We show that gold nanostars integrated into the actuators serve as photothermal elements, enabling the fish tail to repeatedly bend when near infrared light is turned on and off. Our effort illustrates the potential of combining 3D printing, responsive hydrogels and photothermal elements with near infrared light towards soft robotic applications. This combination yields actuators capable of shape‐shifting without requiring localized light or transitioning between environments with varying temperatures.

Tough bilayer thermo‐responsive hydrogel actuator reinforced by Fe3+ complexation

AbstractHydrogel actuators usually suffer from the poor mechanical property, which hinders their wide applications. In this study, we propose a tough bilayer hydrogel actuator that can respond quickly to temperature. The hydrogels are composed of poly(N‐isopropylacylamide) (PNIPAM) layer and poly(acrylamide‐co‐acrylic acid) (P(AAm‐co‐AAc)) layer strengthened through Fe3+ complexation with carboxyl groups. By optimizing the PNIPAM content, the resulting bilayer hydrogel P(NIPAM0.9/AAm‐co‐AAc)‐Fe3+ exhibits fast and large‐amplitude bending and recovery in response to temperature. It also shows excellent mechanical properties with a tensile strength of 2.54 MPa, tensile modulus of 3.7 MPa, and toughness of 9.4 MJ/m3, respectively. Besides, the multiple noncovalent interactions within the hydrogels, including Fe+‐mediated coordination and hydrogen bonds, can serve as dynamic but stable associations, leading to a good self‐healing ability. The bilayer hydrogel is further made into a gripper that can effectively and sensitively respond to temperature to capture and release an object, showing its potential application in artificial intelligent devices.

Creation of Hydrogel Actuator toward Construction of On-chip Biological Models

Creation of Hydrogel Actuator toward Construction of On-chip Biological Models

Self‐strengthened hydrogel actuator based on the distribution of size‐differentiated PVA crystallites

AbstractSoft tissues, such as muscle could autonomously grow through re‐alignment and/or ‐combination of collagen nanofibrils upon the mechanical training. This adaptive capability is highly expected in artificial materials, particularly in hydrogel actuator. In order to avoid the failure for devices by suffering from the accumulated mechanical loading, in this work, a double layered thermo‐responsive hydrogel actuator capable of self‐strengthening was successfully prepared. In the bilayer, PVA nanocrystals with different particle sizes were uniformly distributed in each monolayer matrix, giving rise to the asymmetric structure and the resultant differentiated de‐swelling behaviors. Thus, the obtained hydrogel actuator with the semi‐interpenetrating network of P(NIPAM‐co‐NMA) can display diverse programmable transformations by varying the temperatures. The existence of PVA nanocrystals in both layers not only can enhance the mechanical strength, dramatically minimizing the collapse of hydrogel actuator in service due to the imbalance of the mechanical properties for bilayer structure, but also was greatly involved in the self‐reinforcing behavior. After repetitive tensile training with 80% strain, the tensile strength and fracture strain increased from 29.6 to 45.8 kPa and 95% to 104%, respectively. The experimental results indicated that the anisotropic orientation and strain‐induced‐crystallization for PVA crystalline domains readily occurred along the tensile direction, finally leading to the synchronous enhancement in mechanical strength for both layers. This work provides a new strategy for designing smart and robust biomimetic hydrogel systems that can be further used as the intelligent soft robotics in various fields.

Photothermal-Responsive Lightweight Hydrogel Actuator Loaded with Polydopamine-Modified Hollow Glass Microspheres.

Aquatic actuators based on the light-to-work conversion are of paramount significance for the development of cutting-edge fields including robots, micromachines, and intelligent systems. Herein, we report the design and synthesis of near-infrared light-driven hydrogel actuators through loading with lightweight polydopamine-modified hollow glass microspheres (PDA-HGMPs) into responsive poly(N-isopropylacrylamide) (PNIPAM) hydrogels. These PDA-HGMPs can not only function as an excellent photothermal agent but also accelerate the swelling/desewlling of hydrogels due to their reconstruction for polymer gel skeleton, which speeds up the response rate of hydrogel actuators. The resulting hydrogel actuator shows controlled movements under light illumination, including complex self-propellant and floating/sinking motions. As the proof-of-concept demonstrations, a self-sensing robot is conceptualized by integrating the PDA-HGMP-containing hydrogel actuator with an ultrathin and miniature pressure sensor. Hopefully, this work can offer some important insights into the research of smart aquatic soft actuators, paving the way to the potential applications in emerging fields including micromachines and intelligent systems.

Untethered Hydrogel Actuators Generated by an Interfacial Diffusion Reaction toward Pick-and-Place Tasks

Untethered Hydrogel Actuators Generated by an Interfacial Diffusion Reaction toward Pick-and-Place Tasks

Robust Hydrogel Actuators Functioning in Multi-Environments Enabled by Thermo-Responsive Polymer Nanoparticle Coatings on Hydrogel Surfaces.

Hydrogel actuators with anisotropic structures exhibit reversible responsiveness upon the trigger of various external stimuli, rendering them promising for applications in many fields including artificial muscles and soft robotics. However, their effective operation across multiple environments remains a persistent challenge, even for widely studied thermo-responsive polymers like poly(N-isopropyl acrylamide) (PNIPAm). Current attempts to address this issue are hindered by complex synthetic procedures or specific substrates. This study introduces a straightforward methodology to grow a thin, dense PNIPAm nanoparticle layer on diverse hydrogel surfaces, creating a highly temperature-sensitive hydrogel actuator. This actuator demonstrates adaptability across various environments, including water, oil, and open air, owing to its distinct structure facilitating self-water circulation during actuation. The thin PNIPAm layer consists of interconnected PNIPAm nanoparticles synthesized via in situ interfacial precipitation polymerization, seamlessly bonded to the hydrogel substrate through an interfacial layer containing hybrid hydrogel/PNIPAm nanoparticles. This unique anisotropic structure ensures exceptional structural stability without interfacial delamination, even enduring harsh treatments such as freezing, ultrasonic irradiation, and prolonged water immersion. Remarkably, PNIPAm films on hydrogel surfaces which enable programmable 3D actuation can also be precisely patterned. This synthetic approach opens a novel pathway for fabricating advanced hydrogel actuators with broad-ranging applications.

Localized flow control by photothermal actuation of pNIPAAm hydrogel brushes in a macroporous silicon membrane

Localized flow control by photothermal actuation of pNIPAAm hydrogel brushes in a macroporous silicon membrane

Cephalopod-Inspired Chemical-Gated Hydrogel Actuation Systems for Information 3D-Encoding Display.

Cephalopods evolve the acetylcholine-gated actuation control function of their skin muscles, which enables their dynamic/static multimode display capacities for achieving perfectly spatial control over the colors/patterns on every inch of skin. Reproduction of artificial analogs that exhibit similar multimodal display is essential to reach advanced information three-dimensional (3D) encoding with higher security than the classic 2D-encoding strategy, but remains underdeveloped. The core difficulty is how to replicate such chemical-gated actuation control function into artificial soft actuating systems. Herein, this work proposes to develop azobenzene-functionalized poly(acrylamide) (PAAm) hydrogel systems, whose upper critical solution temperature (UCST) type actuation responsiveness can be intelligently programmed or even gated by the addition of hydrophilic α-cyclodextrin (α-CD) molecules for reversible association with pendant azobenzene moieties via supramolecular host-guest interactions. By employing such α-CD-gated hydrogel actuator as an analogue of cephalopods' skin muscle, biomimetic mechanically modulated multicolor fluorescent display systems are designed, which demonstrate a conceptually new α-CD-gated "thermal stimulation-hydrogel actuation-fluorescence output" display mechanism. Consequently, high-security 3D-encoding information carriers with an unprecedented combination of single-input multiple-output, dynamic/static dual-mode and spatially controlled display capacities are achieved. This bioinspired strategy brings functional-integrated features for artificial display systems and opens previously unidentified avenues for information security.

Dampened Transient Actuation of Hydrogels Autonomously Controlled by pH-Responsive Bicontinuous Nanospheres.

The fabrication of a soft actuator with a dampened actuation response is presented. This was achieved via the incorporation into an actuating hydrogel of urease-loaded pH-responsive bicontinuous nanospheres (BCNs), whose membrane was able to regulate the permeability and thus conversion of fuel urea into ammonia. The dampened response of these nanoreactors to the enzymatically induced pH change was translated to a pH-responsive soft actuator. In hydrogels composed of a pH-responsive and nonresponsive layer, the transient pH gradient yielded an asymmetric swelling behavior, which induced a bending response. The transient actuation profile could be controlled by varying the external fuel concentrations. Furthermore, we showed that the spatial organization of the BCNs within the actuator had a great influence on the actuation response. Embedding the urease-loaded nanoreactors within the active, pH-responsive layer resulted in a reduced response due to local substrate conversion in comparison to embedding them within the passive layer of the bilayer hydrogel. Finally, we were able to induce transient actuation in a hydrogel comprising two identical active layers by the immobilization of the BCNs within one specific layer. Upon addition of urea, a local pH gradient was generated, which caused accelerated swelling in the BCN layer and transient bending of the device before the pH gradient was attenuated over time.

Microgel‐Crosslinked Thermo‐Responsive Hydrogel Actuators with High Mechanical Properties and Rapid Response

Microgel‐Crosslinked Thermo‐Responsive Hydrogel Actuators with High Mechanical Properties and Rapid Response

Light- and Solvent-Responsive Bilayer Hydrogel Actuators with Reversible Bending Behaviors.

Light-responsive hydrogel systems have gained significant attention due to their unique ability to undergo controlled and reversible swelling behavior in response to light stimuli. Combining light-responsive hydrogels with nonresponsive polymers offers a unique self-folding feature that can be used in soft robotic actuator designs. However, simple formulation of such systems with rapid response time is still a challenging task. Herein, we demonstrate a simple but versatile bilayer polymeric design combining light-responsive spiropyran-polyacrylamide (SP-PAAm) with polyacrylamide (PAAm) hydrogels. The photochromic spiropyran in our polymer design is a closed-ring, hydrophobic compound and turns into an open-ring, hydrophilic merocyanine isomer under light irradiation. The swelling degree of SP-PAAm and PAAm hydrogels was evaluated using LED lights with different wavelengths and solvent media (e.g., water, ethanol, DMF, and DMSO). We observed that SP-PAAm hydrogels reached a swelling ratio of ∼370% with the illumination of the blue LED in the DMF medium. By combining light-responsive SP-PAAm hydrogels with nonresponsive PAAm, a proof-of-concept demonstration was performed to demonstrate the applicability of our fabricated platforms. Although fabricated one-armed bilayer hydrogels possessed self-folding ability with a folding angle of ∼40° in 30 min, the four-armed bilayer platforms demonstrated more efficient and rapid folding behavior and reached a folding angle of ∼75° in ∼15 min. Given their simplicity and efficiency, we believe that such polymeric designs may offer new avenues for the fields of polymeric actuators and soft robotic systems.

Nanocellulose-mediated bilayer hydrogel actuators with thermo-responsive, shape memory and self-sensing performances

Inspired by creatures, abundant stimulus-responsive hydrogel actuators with diverse functionalities have been manufactured for applications in soft robotics. However, constructing a shape memory and self-sensing bilayer hydrogel actuator with high mechanical strength and strong interfacial bonding still remains a challenge. Herein, a novel bilayer hydrogel with a stimulus-responsive TEMPO-oxidized cellulose nanofibers/poly(N-isopropylacrylamide) (TOCN/PNIPAM) layer and a non-responsive TOCN/polyacrylamide (TOCN/PAM) layer is proposed as a thermosensitive actuator. TOCNs as a nano-reinforced phase provide a high mechanical strength and endow the hydrogel actuator with a strong interfacial bonding. Due to the incorporation of TOCNs, the TOCN/PNIPAM hydrogel exhibits a high compressive strength (~89.2 kPa), elongation at break (~170.7 %) and tensile strength (~24.0 kPa). The prepared PNIPAM/TOCN/PAM hydrogel actuator performs the roles of an encapsulation, jack, temperature-controlled fluid valve and temperature-control manipulator. The incorporation of Fe3+ further endows the bilayer hydrogel actuator with a synergistic performance of shape memory and temperature-driven, which can be used as a temperature-responsive switch to detect ambient temperature. The PNIPAM/TOCN/PAM-Fe3+ conductive hydrogel can be assembled into a flexible sensor and generate sensing signals when driven by temperature changes to achieve real-time feedback. This research may lead to new insights into the design and manufacturing of intelligent flexible soft robots.

Bilayer Hydrogel Actuators with High Mechanical Properties and Programmable Actuation via the Synergy of Double-Network and Synchronized Ultraviolet Polymerization Strategies.

Bilayer hydrogel actuators, consisting of an actuating layer and a functional layer, show broad applications in areas such as soft robotics, artificial muscles, drug delivery and tissue engineering due to their inherent flexibility and responses to stimuli. However, to achieve the compatibility of good stimulus responses and high mechanical properties of bilayer hydrogel actuators is still a challenge. Herein, based on the double-network strategy and using the synchronous ultraviolet (UV) polymerization method, an upper critical solution temperature (UCST)-type bilayer hydrogel actuator was prepared, which consisted of a poly(acrylamide-co-acrylic acid)[MC] actuating layer and an agar/poly(N-hydroxyethyl acrylamide-co-methacrylic acid)[AHA] functional layer. The results showed that the tensile stress/strain of the bilayer hydrogel actuator was 1161.21 KPa/222.07%. In addition, the UCST of bilayer hydrogels was ~35 °C, allowing the bilayer hydrogel actuator to be curled into an "◎" shape, which could be unfolded when the temperature was 65 °C, but not at a temperature of 5 °C. Furthermore, hydrogel actuators of three different shapes were designed, namely "butterfly", "cross" and "circle", all of which demonstrated good actuating performances, showing the programmable potential of bilayer hydrogels. Overall, the bilayer hydrogels prepared using double-network and synchronous UV polymerization strategies realized the combination of high mechanical properties with an efficient temperature actuation, which provides a new method for the development of bilayer hydrogel actuators.

Tetherless and Batteryless Soft Navigators and Grippers.

Remotely controllable soft actuators have promising potential applications in many fields including soft robotics, exploration, and invasion medical treatment. Shape memory polymers could store and release energy, resulting in shape deformation, and have been regarded as promising candidates to fabricate untethered soft robots. Herein, an untethered and battery-free soft navigator and gripper based on a shape memory hydrogel is presented. The shape memory hydrogel is obtained through hydrogen bonding between gelatin and tannic acid, and the hydrogel displays excellent shape memory properties on the basis of hydrogen bonding and the coil-triple helix transition of gelatin. Moreover, Fe3O4 nanoparticles are introduced to endow the hydrogel magnetic responsiveness and photothermal conversion capacity. Finally, the shape memory hydrogel in a stretched state is assembled with an inert hydrogel to achieve a bilayer hydrogel actuator, which could produce complex shape transformation due to the shape recovery of the shape memory layer induced by heat or light. Taking advantage of the magnetically control and light-responsive shape deformation, remotely controllable soft grippers that could navigate through tortuous paths and grasp objects from a hard-to-reach place have been accomplished. This approach will inspire the design and fabrication of novel shape memory hydrogels as remotely controllable soft robots.

Programmable Thermo- and Light-Responsive Hydrogel Actuator Reinforced with Bacterial Cellulose

Programmable Thermo- and Light-Responsive Hydrogel Actuator Reinforced with Bacterial Cellulose

UV Light-Mediated Hydrolytic Reaction to Develop Magnetic Hydrogel Actuators with Spatially Distributed Ferriferous Oxide Microparticles.

Magnetic hydrogel actuators are developed by incorporating magnetic fillers into the hydrogel matrix. Regulating the distribution of these fillers is key to the exhibited functionalities but is still challenging. Here a facile way to spatially synthesize ferrosoferric oxide(Fe3O4) microparticles in situ in a thermal-responsive hydrogel is reported. This method involves the photo-reduction of Fe3+ ions coordinated with carboxylate groups in polymer chains, and the hydrolytic reaction of the reduced Fe2+ ions with residual Fe3+ ions. By controlling the irradiation time and position, the concentration of Fe3O4 microparticles can be spatially controlled, and the resulting Fe3O4 pattern enables the hydrogel to exhibit complex locomotion driven by magnet, temperature, and NIR light. This method is convenient and extendable to other hydrogel systems to realize more complicated magneto-responsive functionalities.