Hydrogel Layer Research Articles

Design of multiple anti-fouling and honeycomb-like NH2-AgBiS2 @g-C3N4 hydrogel layer onto PAN fiber membrane for multicomponent pollutant-oil-water emulsion treatment

Nano-structured hydrogel with unique anti-oil fouling property exhibits big advantage in oil/water separation, but its application in complex oily wastewater (contain oils, organic matter, bacteria, etc.) cleanup is hampered by the insufficient capabilities in multi-antifouling and synergistic treatment. Herein, we constructed the amino-rich NH2-AgBiS2/PANI (polyaniline)-g-C3N4 based multi-functional hydrogel functional layer onto the polyacrylonitrile (PAN) fiber membrane via polyphenol-mediated chitosan gelation and vacuum-assisted self-assembly techniques. The unique honeycomb-like structure and super-wetting feature synergistically contributed to the powerful oil resistance and flux breakthrough of composite membrane. Such membrane achieved superior permeability (up to 3558 L−1 m−2 h−1) for various SDS-stabilized oil-in-water emulsions and remarkable synergistic treatment efficiency of multicomponent pollutant-oil-water emulsion. The rational design of hydrogel layer on membrane surface intensified the photo-response ability and multiple electron transport channels, which offered the favorable photocatalytic self-cleaning performance towards degradation of organic dyes. According to the free radical quenching and EPR experiments, the photocatalytic mechanism was proposed. In addition, the inhibition rate of E. coli could reach 100 % under illumination of 24 h. Therefore, the integration of ultra-low oil adhesion, photocatalytic self-cleaning, and antibacterial features endows membrane with exceptional multiple anti-fouling performance, exhibiting unique advantages over traditional membranes in handling complex membrane fouling issues.

A simple route of providing a soft interface for PEDOT: PSS film metallic electrodes without loss of their electrical interface parameters

The work presents the development of a soft interface at PEDOT:PSS film without changing its electrical interface parameters. In the first step, PEDOT:PSS is electrodeposited on the commercial platinum electrode under the state-of-the-art conditions desirable for different electrochemical electrodes. Secondly, a pure hydrogel layer is deposited on the top of the electrodeposited PEDOT:PSS film under conditions that provide desirable mechanical properties (Young's modulus ∼10–20 kPa) and high permeability to ions from the solution. As a result, a PEDOT:PSS electrode with a soft interface desirable for different electrode applications is fabricated. The electrode exhibits electrical parameters at the same level as the state-of-the-art PEDOT:PSS film applied already for electrode applications. Moreover, the hydrogel layer additionally supports the polymeric film's electrochemical stability by inhibiting its oxidative degradation. The thickness of PEDOT film does not affect the overall electrochemical properties of the hydrogel electrode. The work shows that the specific choice of the hydrogel type and fabrication conditions allows to synthesis of the hydrogel interface on a stiff polymeric film, which does not block the ionic and electrical transfer. Moreover, the fabricated PEDOT:PSS electrode with hydrogel interface reveals interfacial impedance and potential window comparable or even better to the already published studies on PEDOT:PSS hydrogels.

A temperature-sensitive actuator based on AG/NIPAM delignification wood-based hydrogel

Hydrogels are important in smart drive materials because of their stretchability and biocompatibility. However, challenges in their mechanical properties and preparation process as actuators hinder their potential applications. In this work, a double-layer composite hydrogel actuator was proposed. The actuator consists of two layers of materials, namely delignification wood and agarose (AG)/poly(N-isopropylacrylamide) (PNIPAM) composite hydrogel, named as double-layer wood-based hydrogel (BWH). In BWH, due to the large amount of hydroxyl groups on the surface of delignification wood, abundant hydrogen bonds can be formed with the hydrogel layer to ensure the close adhesion of the two layers and achieve stable synergy. At the same time, the delignification wood can give the overall stable structure and predictable bending direction. In addition, BWH has excellent anti-swelling properties, which is due to the double network design of the hydrogel layer and the anti-swelling properties of the delignification wood skeleton itself. Based on the property of BWH sensitive to temperature deformation, its applications in the field of intelligent grasping and fluid valve were studied. This work provides a simple method for the preparation of response actuators and the idea of mechanical enhancement and adjustable deformation direction.

Microneedle System Coated with Hydrogels Containing Protoporphyrin IX for Potential Application in Pharmaceutical Technology.

The article aims to outline the potential of treating malignant skin cancer with microneedles covered with polymer layers containing a photosensitizer-protoporphyrin IX disodium salt (PPIX). The usefulness of stereolithography (SLA), which is a form of 3D-printing technology, for the preparation of a microneedle system with protoporphyrin IX was demonstrated. The SLA method allowed for pyramid-shaped microneedles to be printed that were covered with three different 0.1% PPIX hydrogels based on sodium alginate, xanthan, and poloxamer. Rheological tests and microscopic analysis of the hydrogels were performed. Microneedles coated with two layers of poloxamer-based hydrogel containing 0.1% PPIX were subjected to release tests in Franz diffusion cells. The release profile of PPIX initially increased and then remained relatively constant. The amount of substance released after a four-hour test in three Franz cells was 0.2569 ± 0.0683 mg/cm2. Moreover, the acute toxicity of this type of microneedle was assessed using the Microtox system. The obtained results show the usefulness of further development studies on microneedles as carriers of photosensitizing agents.

An Environmentally Stable, Biocompatible, and Multilayered Wound Dressing Film with Reversible and Strong Adhesion.

Reversible adhesives for wound care improve patient experiences by permitting reuse and minimizing further tissue injury. Existing reversible bandages are vulnerable to water and can undergo unwanted deformation during removal and readdressing procedures. Here, a biocompatible, multilayered, reversible wound dressing film that conforms to skin and is waterproof is designed. The inner layer is capable of instant adhesion to various substrates upon activation of the dynamic boronic ester bonds by water; intermediate hydrogel layer and outer silicone backing layer can enhance the dressing's elasticity and load distribution for adhesion, and the silicone outer layer protects the dressing from exposure to water. The adhesive layer is found to be biocompatible with mouse skin. Skin injuries on the mouse skin heal more rapidly with the film compared to no dressing controls. Evaluations of the film on skin of freshly euthanized minipigs corroborate the findings in the mouse model. The film remains attached to skins without delamination despite subjecting to various degrees of deformation. Exposure to water softens the film to allow removal from the skin without pulling any hair off. The multilayered design considers soft mechanics in each layer and will offer new insights to improve wound dressing performance and patient comfort.

Biomimetic bilayer phase change hydrogels with enhanced water adsorption and desorption for evaporative cooling

Hygroscopic hydrogels, reliable carriers for water-based evaporative materials, undergo shrinkage after evaporative cooling, and the consequent reduction in hygroscopic sites can significantly impair their recyclability in cooling period. To realize cyclic evaporative cooling for rapid regeneration and evaporation, bilayer phase change hydrogel (BPH) concept combining an upper layer of hygroscopic polymer film (CaCl2@ carboxymethyl cellulose/konjac glucomannan films, CaCl2@CMC/KGM, MAF) with a lower layer of hygroscopic hydrogel (CaCl2@poly(vinyl alcohol)/sodium tetraborate decahydrate hydrogel, CaCl2@PVA/Borax, PCH), is presented in this paper. The high liquid–vapor phase change enthalpy of BPH (1274 J/g) enables it to continuously and rapidly remove heat. Benefiting from the MAF hygroscopic porous skeleton, the saturated BPH exhibited a faster water evaporation rate (2.15 kg m−2 h−1) and comparable water vapor transmission rate (1.61 kg m−2 h−1) at 50 °C. After being heated at 50 °C for 1 h, BPH requires 9h to regain its initial mass at 25 °C, 90 % RH. Fifteen moisture adsorption–desorption cycles demonstrate the excellent cyclic regeneration capability of BPH. COMSOL Multiphysics simulation results indicate that evaporative cooling in BPH provides excellent heat dissipation (reduced by about 27 °C). BPH reduces the peak temperatures of a mobile phone by 7.8 °C while charging and 6.5 °C while gaming. This design will contribute to the future cooling of heat-related devices and global sustainability.

Hygroscopic hydrogel-based cooling system for photovoltaic panels: An experimental and numerical study

Thermal management is an essential aspect of photovoltaic (PV) system design because of the negative effects of high temperatures on the efficiency of PV panels. The use of hygroscopic hydrogels for the evaporative cooling of PV panels is an emerging technique that has attracted attention owing to the high latent heat and recyclability of these materials. However, a comprehensive understanding of the heat and mass transport mechanisms in hygroscopic hydrogels is necessary. Factors that would ensure the long-term performance of PV panel/hydrogel (PV/HG) systems under real-world conditions are still poorly understood, and the intrinsic properties of hydrogels and the effect thereof on their cooling performance have hitherto remained unexplored. Herein, we propose a mathematical model for hydrogel-cooled PV panels to study the heat and mass transfer mechanisms of PV/HG systems in practical environments. The model is used to examine the impact of the thermal conductivity, diffusion coefficient, and thickness of the hydrogel on the performance of the PV/HG system. Unlike previously reported approaches to enhance the efficiency, in this study, the external heat transfer resistance and internal mass transfer resistance were identified as the primary controlling factors. Enhancement of the thermal conductivity of the hydrogel is shown to have a limited effect on the performance, whereas improving the water diffusion within the hydrogel significantly boosts the system efficiency. Optimally, the thickness of the hydrogel must be such that it balances the heat and mass transfer distances with the available water volume. During the summer in Guangzhou, China, a 6-mm thick layer of hydrogel lowered the temperature of a PV cell by up to 7.5 °C to increase the daily power generation by 2.1%. Analysis of the nationwide situation showed that hydrogels have substantial potential for lowering the peak PV panel temperatures (by as much as 19.3 °C) to mitigate fluctuations in the output power. Our findings offer valuable insights into the design of PV/HG systems towards improving their performance.

Physicochemical characterization and potential cancer therapy applications of hydrogel beads loaded with doxorubicin and GaOOH nanoparticles

A new type of hybrid polymer particles capable of carrying the cytostatic drug doxorubicin and labeled with a gallium compound was prepared. These microparticles consist of a core and a hydrogel shell, which serves as the structural matrix. The shell can be employed to immobilize gallium oxide hydroxide (GaOOH) nanoparticles and the drug, resulting in hybrid beads with sizes of approximately 3.81 ± 0.09 μm. The microparticles exhibit the ability to incorporate a remarkably large amount of doxorubicin, approximately 0.96 mg per 1 mg of the polymeric carrier. Additionally, GaOOH nanoparticles can be deposited within the hydrogel layer at an amount of 0.64 mg per 1 mg of the carrier. These nanoparticles, resembling rice grains with an average size of 593 nm by 155 nm, are located on the surface of the polymer carrier. In vitro studies on breast and colon cancer cell lines revealed a pronounced cytotoxic effect of the hybrid polymer particles loaded with doxorubicin, indicating their potential for cancer therapies. Furthermore, investigations on doping the hybrid particles with the Ga-68 radioisotope demonstrated their potential application in positron emission tomography (PET) imaging. The proposed structures present a promising theranostic platform, where particles could be employed in anticancer therapies while monitoring their accumulation in the body using PET.

Janus Amphipathic Dressing With Liquid Self-Pumping and Blood-Clot Anti-Adhesion for Satisfactory Hemostasis.

Ideal hemostatic materials for the emergency rescue of war and traffic accident sufferers are essential to significantly control hemorrhage, reduce patient discomfort, and improve the survival ratio. However, most hemostats absorb blood quickly in contact with the wound; and then, adhere to blood clots, resulting in breaking scabs and tearing the wound when the materials are removed. Herein, an effective Janus amphipathic hemostatic dressing (Fiber@Gel/Ca2+/KL) with a fiber layer (polylactic acid/carboxymethyl chitosan) and a hydrogel layer (polyvinyl alcohol, carboxymethyl chitosan, Ca2+, and kaolin) is reported. Such a composite dressing unidirectionally drains the excessive serum from its hydrophobic side (fiber layer) to its hydrophilic side (hydrogel layer), so-called self-pumping, thereby further concentrating coagulated factors (including red blood cells and platelets). Further, Ca2+ diffused from the hydrogel layer subsequently activates platelets and coagulation cascade. Besides, the Fiber@Gel/Ca2+/KL exhibits specific blood-clot anti-adhesion property on the fiber layer, making the dressing easily and safely peel off from the wound. It is believed that this novel hemostatic dressing with good hemostatic performance, easy clots removal, and excellent biocompatibility is expected to be used as a safe and efficient hemostatic dressing in clinical applications.

Modeling cellular self-organization in strain-stiffening hydrogels

AbstractWe derive a three-dimensional hydrogel model as a two-phase system of a fibre network and liquid solvent, where the nonlinear elastic network accounts for the strain-stiffening properties typically encountered in biological gels. We use this model to formulate free boundary value problems for a hydrogel layer that allows for swelling or contraction. We derive two-dimensional plain-strain and plain-stress approximations for thick and thin layers respectively, that are subject to external loads and serve as a minimal model for scaffolds for cell attachment and growth. For the collective evolution of the cells as they mechanically interact with the hydrogel layer, we couple it to an agent-based model that also accounts for the traction force exerted by each cell on the hydrogel sheet and other cells during migration. We develop a numerical algorithm for the coupled system and present results on the influence of strain-stiffening, layer geometry, external load and solvent in/outflux on the shape of the layers and on the cell patterns. In particular, we discuss alignment of cells and chain formation under varying conditions.

Temperature-responsive self-contraction nanofiber/hydrogel composite dressing facilitates the healing of diabetic-infected wounds

Bacterial infections and long-term inflammation cause serious secondary damage to chronic diabetic wounds and hinder the wound healing processes. Currently, multifunctional hydrogels have shown promising effects in chronic wound repair. However, traditional hydrogels only keep the wound moist and protect it from bacterial infection, and cannot provide mechanical force to contract the wound edges to achieve facilitated wound closure. Here, an asymmetric composite dressing was created by combining biaxially oriented nanofibers and hydrogel, inspired by the double-layer structure of the traditional Chinese medicinal plaster patch, for managing chronic wounds. Specifically, electrospun Poly-(lactic acid-co-trimethylene carbonate) (PLATMC) nanofibers and methacrylate gelatin (GelMa) hydrogel loaded with Epinecidin-1@chitosan (Epi-1@CS) nanoparticles are assembled as the temperature-responsive self-contracting nanofiber/hydrogel (TSNH) composite dressing. The substrate layer of PLATMC nanofibers combines topological morphology with material properties to drive wound closure through temperature-triggered contraction force. The functional layer of GelMa hydrogel is loaded with Epi-1@CS nanoparticles that combine satisfactory cytocompatibility, and antioxidant, anti-inflammatory, and antibacterial properties. Strikingly, in vivo, the TSNH dressing could regulate the diabetic wound microenvironment, thereby promoting collagen deposition, facilitating angiogenesis, and reducing the inflammatory response, which promotes the rapid healing of chronic wounds. This study highlights the potential of synergizing mechanical and biochemical signals in enhancing chronic wound treatment. Overall, this TSNH composite dressing is provided as a reliable approach to solving the long-standing problem of chronically infected wound healing.

Enhanced Antifouling Capability of In Situ-Grown Hydrophilic-Hydrophobic Nanodomains on Membrane Surface in the Ultralow Pressurized Ultrafiltration Process.

Although hydrophilic modification of the membrane surface is widely adopted, polymeric membranes still suffer from irreversible fouling caused by hydrophilic components in surface water. Here, an ultrathin hydrogel layer (40 nm) with hydrophilic-hydrophobic textures was in situ grown onto the polysulfone ultrafiltration membrane surface using an organic-radical-initiated interfacial polymerization technique. The interfacial polymerization of hydrophilic and hydrophobic monomers ensured the molecular-scale distribution of hydrophilic and hydrophobic nanodomains on the membrane surface. These nanodomains, with their molecular lengths, facilitated dynamic repulsion interactions between the uniformly textured surface and foulant components with different degrees of hydrophilicity. Chemical force characterization confirmed that the adhesion force between the hydrophilic-hydrophobic textured membrane surface and foulants (dodecane, bovine serum albumin, and humic acid) was greatly reduced. Dynamic filtration experiments showed that a hydrophilic-hydrophobic textured membrane always possessed the largest water flux and the best antifouling performance. Furthermore, the foulant coverage ratio on the membrane surface was first evaluated by measuring changes in surface streaming potentials, which demonstrated a 69% reduction in the amount of foulant adhering to the hydrophilic-hydrophobic textured membrane surface. Therefore, the construction of hydrophilic-hydrophobic nanodomains on the membrane surface provides a promising strategy for alleviating membrane fouling caused by both hydrophobic and hydrophilic components during ultralow pressurized ultrafiltration processes.

Storage Optimization of Transmission Holographic Gratings in Photohydrogels.

The development and optimization of holographic materials represent a great challenge today. These materials must be synthesized according to the characteristics that are desirable in photonic devices whose application is the object of investigation. In certain holographic sensors and biosensors, it is essential that the recording material be stable in liquid media. Furthermore, the holographic gratings stored in them must have temporal and structural stability, so that they can act as transducers of the analytical signal. Therefore, it is essential to optimize its storage in terms of the chemical composition of the material and the optical parameters of recording. This work focuses on the study of the storage optimization of unslanted transmission volume phase holograms in photohydrogels based on acrylamide and N,N'-methylenebis(acrylamide). Hydrogel matrices, also composed of acrylamide and N,N'-methylenebis(acrylamide), with different degrees of cross-linking were used and analyzed by scanning electron microscopy and UV-visible spectroscopy. The best results in terms of diffraction efficiency were reached for hydrogel matrices with an acrylamide/N,N'-methylenebis(acrylamide) molar ratio between 19.9 and 26. This relationship was also optimized in the incubator solution used to incorporate the components necessary for the formation of the holograms in the hydrogel matrices. The maximum diffraction efficiency, about 35%, was achieved when using an incubation solution with an acrylamide/N,N'-methylenebis(acrylamide) molar ratio of 4.35. The influence of the physical thickness of the hydrogel layers, the intensity, and the exposure time on the diffraction efficiency was also investigated and optimized. In addition, the behavior of the hologram was analyzed after a washing stage with PBST. A simple model that considered the effects of bending and attenuation of holographic gratings was proposed and used to obtain the optical parameters of the holograms.

The Exponential Shapeshifting Response of N-Vinylcaprolactam Hydrogel Bilayers Due to Temperature Change for Potential Minimally Invasive Surgery.

Poly (N-vinylcaprolactam) (PNVCL) and poly (N-isopropylacrylamide) (PNIPAm) are two popular negatively temperature-responsive hydrogels, due to their biocompatibility, softness, hydrophilicity, superabsorbency, viscoelasticity, and near-physiological lower critical solution temperature (LCST). These characteristics make them ideal for biomedical applications. When combined with other materials, hydrogel expansion induces the morphing of the assembly due to internal stress differences. Our recent developments in NVCL hydrogel, enhanced by nanoclay incorporation, have driven us to the creation of a bilayer structure to study its shapeshifting response across various temperatures. This study focused on the bending behaviour of bilayer samples composed of an active hydrogel layer and a passive non-swellable layer. Using photopolymerisation, circular discs and rectangular bilayer samples of varying sizes were fabricated. Homogeneous circular samples demonstrated that hydrogel density increased proportionally with temperature, with the swelling ratio exhibiting two distinct rates of change below and above its LCST. In bilayer samples, the volume of the passive layer influenced bending, and its optimal volume was identified. The investigation revealed that geometry affected the overall bending effect due to changes in the passive layer stiffness. Lastly, a temperature-responsive gripper capable of picking up objects several times its own weight was demonstrated, highlighting the potential of NVCL hydrogels as bioactuators for minimally invasive surgery.

Mucus Mimic Hydrogel Coating for Lubricous, Antibiofouling, and Anti-Inflammatory Urinary Catheters.

Silicone is a common elastomer used in indwelling urinary catheters, and catheters are widely used in various medical applications due to their exceptional biocompatibility, hypoallergenic properties, and flexibility. However, silicones exhibit hydrophobic characteristics, lack inherent biolubrication, and are susceptible to nonspecific biosubstance adsorption, resulting in complications including but not limited to tissue trauma, postoperative pain, and urinary tract infections (UTIs). The development of effective surface designs for biomedical catheters to mitigate invasive damage and UITs has been a longstanding challenge. Herein, we present a novel approach to prepare a mucus mimic hydrogel coating. A thin layer of hydrogel containing xylitol is fabricated via photopolymerization. The surface modification technique and the interface-initiated hydrogel polymerization method ensure robust interfacial coherence. The resultant coating exhibits a low friction coefficient (CoF ≈ 0.1) for urinary catheter applications. Benefiting from the hydration layer and the antifouling of the xylitol unit, the xylitol hydrogel-coated surfaces (pAAAMXA) demonstrate outstanding antibiofouling properties against proteins (98.9% reduction relative to pristine polydimethylsiloxane (PDMS)). Furthermore, the pAAAMXA shows general adhesion resistance against bacteria primarily responsible for UITs (Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), Methicillin-resistant strains of Staphylococcus aureus (MRSA), and Staphylococcus epidermidis (S. epidermidis)) without compromising biotoxicity (cell viability 98%). In vivo, catheters coated with the mucus mimic hydrogel displayed excellent biocompatibility, resistance to adhesion of bio substance, and anti-inflammatory characteristics. This work describes a promising alternative to conventional silicone catheters, offering potential for clinical interventional procedures with minimized complications.

Bioinspired Self-Growing Layered Hydrogel Enabled by Catechol Chemistry-Mediated Interfacial Catalytic System.

Tissue-inspired layered structural hydrogel has attracted increasing attention in artificial muscle, wound healing, wearable electronics, and soft robots. Despite numerous efforts being devoted to developing various layered hydrogels, the rapid and efficient preparation of layered hydrogels remains challenging. Herein, inspired by the self-growth concept of living organisms, an interfacial catalytic self-growth strategy based on catechol chemistry-mediated self-catalytic system of preparing layered hydrogels is demonstrated. Typically, the tannic acid-metal ion (e.g., TA-Fe3+) complex embedded in the hydrogel substrate would catalytically trigger rapid solid-liquid interfacial polymerization to grow the hydrogel layer without bulk solution polymerization. The self-growth process can be finely controlled by changing the growth time, the molar ratio of Fe3+/TA, and so on. The strategy is applicable to prepare various layered hydrogels as well as complex layered hydrogel patterns, allowing the customization of the physicochemical properties of the hydrogel. In addition, the self-adhesive layered hydrogel was prepared and can be utilized as a wearable strain sensor to monitor physiological activities and human motions. The demonstrated interfacial catalytic self-growth strategy will provide a route to design and fabricate layered hydrogel materials.

Innovative composite fluidized hydrogel GAC particles for effective membrane fouling mitigation and membrane integrity protection

Membrane filtration is recognized as an environmentally friendly and cost-efficient technology for water treatment, but membrane fouling is still a significant challenge that increases maintenance costs and reduces membrane lifespan. Particle scouring can effectively mitigate fouling with lower energy consumption. This study investigates the use of fluidized granular activated carbon (GAC) particles encapsulated with hydrogel layers to enhance fouling mitigation in microfiltration systems treating surface water. The proposed hydrogel-modified GAC particles aim to balance scouring efficiency with membrane integrity. The results demonstrate that optimizing hydrogel preparation conditions significantly enhanced the mechanical strength and surface hydrophilicity of GAC particles. The incorporation of hydrogel layers notably improved membrane fouling mitigation, reducing transmembrane pressure (TMP) by 19.3 %, 27.1 %, and 34.3 % for layer thicknesses of 0.5 mm, 1.0 mm, and 1.5 mm, respectively. The hydrodynamic behavior of fluidized GAC particles was significantly improved, enhancing the effectiveness of fouling mitigation in water treatment processes. Additionally, the hydrogel layer effectively protected membrane integrity and inhibited carbon release, ensuring minimal damage and stable permeability. This study underscores the pivotal role of hydrogel layers in improving the performance and longevity of membrane filtration systems, when fluidized GAC particles are used for membrane fouling control.

Ionic fuel-powered hydrogel actuators for soft robotics

HypothesisHydrogel actuators powered by chemical fuels are pivotal in autonomous soft robotics. Nevertheless, chemical waste accumulation caused by chemical fuels hampers the development of programmable and reusable hydrogel actuating systems. We propose the concept of ionic fuel-powered soft robotics which are constructed by programmable salt-responsive actuators and use waste-free ionic fuels. ExperimentsHerein, soft hydrogel actuators were developed by orchestrating the Janus bilayer hydrogels’ capacity for swelling and shrinking. Decomposable and easily removable ionic fuels were applied to power the actuators. Swelling tests were used to evaluate the deformability of the hydrogels. Tensile tests were performed to investigate the modulus of the hydrogels. The bonded interface composed of the interpenetrating polymer chains from both hydrogel layers bilayer was evidenced by the optical microscopy and scanning electron microscopy. The ionic conductivities of solutions were determined by a conductivity meter. Furthermore, a range of biomimetic soft robots with various shapes and asymmetrical structures have been designed and fabricated to execute complex functions. FindingsThe programmable actuators powered by ionic fuel exhibit adjustable bending orientations, amplitudes, and durations, along with consistent cyclic actuations enabled by replenishment of the fuel without noticeable loss in performance. Many life-like programmable soft robotic systems were designed, indicating spatiotemporally controllable functions.

Interfacial Wrinkling Structures Based on a Double Cross-Linking Strategy Enable a Dual-Mode Optical Information Encryption.

Surface wrinkling structures based on a bilayer system are widely employed in storing and encrypting specific optical information. However, constructing a stable wrinkling structure with high-level security remains an extensive challenge due to the delamination issue between the skin layer and the substrate. Herein, a double cross-linking strategy is introduced between a hydrogel layer doped with fluorescent molecules and polydimethylsiloxane to establish a stable interfacial wrinkling structure with dual-mode functionality, in which the light reflection of the wrinkles and fluorescence intensity of fluorescent molecules can be simultaneously regulated by the modulus ratio between the two layers. The spontaneous wrinkling structures with a physically unclonable function can enhance the photoluminescence emission intensity of the wrinkling area under ultraviolet radiation. Meanwhile, the skin layer constructed of acrylamide and acrylic acid copolymer protects the interfacial wrinkling patterns from the loss of a detailed structure for authentication due to external damage. The stable interfacial wrinkling structures with fluorescence can find potential applications in the fields of information storage and encryption.

Bio-Inspired Double-Layered Hydrogel Robot with Fast Response via Thermo-Responsive Effect.

Bio-inspired hydrogel robots have become promising due to their advantage of the interaction safety and comfort between robots and humans, while current hydrogel robots mainly focus on underwater movement due to the hydration-dehydration process of thermo-responsive hydrogels, which greatly limits their practical applications. To expand the motion of the thermo-responsive hydrogel robot to the ground, we constructed a hydrogel robot inspired by a caterpillar, which has an anisotropic double-layered structure by the interfacial diffusion polymerization method. Adding PVA and SA to PNIPAm will cause different conformation transitions. Therefore, sticking the two layers of hydrogel together will form a double-layer anisotropic structure. The ultra-high hydrophilicity of PVA and SA significantly reduces the contact angle of the hydrogel from 53.1° to about 10° and reduces its hydration time. The responsive time for bending 30° of the hydrogel robot has been greatly reduced from 1 h to half an hour through the enhancement of photo-thermal conversion and thermal conductivity via the addition of Fe3O4 nanoparticles. As a result, the fabricated hydrogel robot can achieve a high moving speed of 54.5 mm·h-1 on the ground. Additionally, the fabricated hydrogel has excellent mechanical strength and can endure significant flexibility tests. This work may pave the road for the development of soft robots and expand their applications in industry.