Structure Of Hydrogels Research Articles

Pectin/PVA-Borax Hydrogel with Self-Healing Ability

Hydrogels are polymers with soft and high-water absorption characteristics similar to biological tissues, leading to several potential applications, such as artificial organs, drug delivery, tissue engineering, and strain sensor. Interestingly, hydrogels can be designed to heal themselves after being damaged. In this research, hydrogels with self-healing ability from pectin and polyvinyl alcohol were prepared by simple physical mixing. Borax was used as a crosslinking agent to obtain crosslinked hydrogel structure by the formation of dynamic boron ester bonds. Glycerol was also added to the hydrogels as an anti-freezing agent and a stabilizer. The microstructures, mechanical properties, self-healing ability and swelling properties of the pectin/PVA-borax hydrogels were characterized. The results indicate that the size of microporous structure, modulus, tensile strength, self-healing time, swelling, and equilibrium water content of the pectin/PVA hydrogels increases with the increasing borax contents.

Sponge-like characteristic of cellulose hydrogel for transport of rosmarinic acid nanoemulsion

Hydrogel has porous and sponge-like structure that can be used as a drug carrier to delivery drugs. In this study, rosmarinic acid (RA) with excellent therapeutic properties was encapsulated in a drug-carrier nanoemulsion and subsequently loaded into the sponge-like cellulose hydrogel derived from pineapple leaves fiber and Orthosiphon aristatus stem fiber. The scope of research was to determine the loading and unloading of bioactive compounds encapsulated with nanoemulsion in the sponge-like structure of cellulose hydrogel. Based on physical observation, the rosmarinic acid-encapsulated nanoemulsion (RANE) and RANE-loaded cellulose hydrogel appeared less turbid as the surfactant concentration increased. Besides, the pH of RANE decreases as surfactant concentration increases, but turns neutral after immobilized into the porous structure of cellulose hydrogel. Changes in the pH and appearance of hydrogel show that RANE has been loaded and demonstrate its usability as a drug carrier. From the RA release profile, increase of surfactant concentration increases the rate and amount of RA released, but all formulations showing prolonged release. In summary, the sponge-like of cellulose hydrogel enables the loading–unloading of therapeutic RANE into/from its porous structure could potentially be applied as drug carrier for wound dressing.

Preparation of Fe3O4@pectin nanocomposite hydrogel with high heating efficiency for hyperthermia applications

In this paper, magnetic nanoparticles (Fe3O4) were prepared by the co-precipitation method. The synthesized magnetic nanoparticles were added to the biocompatible polymer, pectin, for synthesizing Fe3O4@pectin (F@P) nanocomposite hydrogels. The structural, morphological, and magnetic characterizations were performed by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FTIR), and vibrating sample magnetometer (VSM) techniques. The XRD pattern confirmed the existence of the cubic phase of Fe3O4 nanoparticles. The FTIR spectra revealed the incorporation of pectin on the surface of Fe3O4 nanoparticles. The VSM measurement shows the proper magnetization curve of F@P nanocomposites, and good saturation magnetization value (∼33 emu/g). The results of hyperthermia temperature reveal an excellent heating efficiency of F@P nanocomposite hydrogel. The heating efficiency was quantified by a specific absorption rate (SAR) value and was obtained as 214 W/g for F@P nanocomposite hydrogels. This good hyperthermia result with biocompatible polymer (pectin) and hydrogel structure can be used for developing cancer treatment studies.

Regulate structure and properties of κ-carrageenan/konjac glucomannan composite hydrogel by filling effects of Quillaja saponin-stabilized solid lipid nanostructure

κ-Carrageenan/konjac glucomannan (κ-CA/KGM) composite hydrogels often fail to meet industrial requirements due to their low gel strength and poor mechanical properties, while solid lipid nanoparticles are potential materials to address this challenge due to their good biocompatibility. In the study, we propose using Quillaja saponin-stabilized solid lipid nanoparticle (QSLN) as nanofillers to enhance properties of κ-carrageenan/konjac glucan (κ-CA/KGM) composite hydrogels, and with emphasis on the effect of QSLN filling concentration on the structure and properties of composite hydrogels and the possible mechanisms were investigated. The best performance of QSLN-filled composite hydrogels was achieved at the QSLN concentration of 2.4 %. QSLN was uniformly distributed in the hydrogel matrix and formed electrostatic interactions and hydrogen bonding interactions with the matrix at an appropriate filling level, which enhanced the textural and rheological properties of the hydrogel greatly. In addition, the results of low-field NMR experiments showed that the filling of QSLN reduced the water mobility by enhancing the entanglement of polymer chains in the hydrogel matrix, which improved the freeze-thaw stability and regulated the swelling and deswelling behavior of the composite hydrogel. However, with the increasing of QSLN filling concentration, the above improvements were weakened by the depletion of van der Waals interactions due to the large amount of QSLN aggregation and the weakening of electrostatic interaction. In turn, the hydrogel was found to modulate the crystalline behavior of QSLN by X-ray diffraction and differential scanning calorimeter monitoring. Overall, the optimal synergistic effect between structure and properties could be achieved when the QSLN filling concentration was 2.4 %. These results provide a basis for the development of products that require excellent gel properties and structure.

Rapid fabrication of porous κ-carrageenan/cellulose nanofibrils-polydopamine composite hydrogels induced by ionic interaction for flexible electronic devices

A novel κ-carrageenan composite hydrogel via incorporation of TEMPO-oxidized cellulose nanofibrils (TCNF) and polydopamine (PDA) nanoparticles, was fabricated by ionic interaction to achieve a higher mechanical and higher conductive performance. Owing to the excellent compatibility and stability of the TCNF-PDA mixture, and the strong ionic interactions between the hydrogel precursor and metal cations in the hydrogel formation, the composite hydrogel showed improved mechanical property of 73.5 kpa and a faster gel formation process of 58 s. The gel formation mechanism was comprehensively illustrated by XPS technique, a double-network with one main noncovalent interaction was created inside the hydrogels. Moreover, the inter-connected porous hydrogel structure with smaller pores improved current carrying and diffusion of electrolyte metal cations, the conductivity reached at 2.13 S/m. It could also sensitively and stably detect the external stress applied, demonstrating such hydrogel was beneficial to be applied at flexible electronic devices.

4D-Printed Hydrogel Actuators through Diffusion-Path Architecture Design.

Recently, smart hydrogels have garnered considerable attention as biomedical devices, and several approaches have been introduced for their fabrication, including the incorporation of stimulus-responsive additives, utilization of molecular imprinting techniques, and application of multilayered hydrogels. However, the nonuniform properties resulting from these approaches limit the practical applications of hydrogels by causing inconsistent performance and behavior. In this study, we propose a novel approach to manipulating the swelling kinetics of hydrogels by engineering their diffusion-path architecture. By simply adjusting the diffusion path length within the hydrogel, we achieved a significant change in swelling kinetics. This approach enables precise control over the diffusion and transport processes within the hydrogel, resulting in enhanced swelling kinetics when reducing the diffusion path length. Furthermore, by strategically designing the diffusion-path architecture of a 3D-printed hydrogel specimen, we can fabricate smart hydrogel actuators that exhibit reversible shape transformations during swelling and deswelling through a nonequilibrium differential swelling. The proposed approach eliminates the need to modify the spatial properties of hydrogel structures such as cross-linking density, polymer, or additive compositions, thereby achieving uniform properties throughout the hydrogel and creating new possibilities for the development of advanced 4D-printed biomedical devices.

Levan-based bioactive hydrogels containing herbal liposome in treating acute wounds

Hydrogels in active wound care products are 3D polymeric scaffolds that provide the desired moisture balance in the wound area with their high water retention capacity. Thanks to their biocompatible properties, flexible and porous structures, and high hydrophilic properties, they have frequently been preferred in the repair and regeneration of cells and tissues and the controlled release of bioactive substances to the target area. In this study, hydrogel structures were developed for the first time with levan produced by Halomonas elongata 153B halophilic bacteria. Extracts from Plantago lanceolata L., commonly known as a wound herb, which has medicinal importance for cell regeneration, ensuring tissue integrity in a short time and reducing infections in the wound area, were obtained and extract-loaded liposome structures were formed for controlled release into the wound area. The wound healing efficacy of the composite material developed by loading herbal liposomes into levan-based hydrogel structures was evaluated in an in vitro wound model. Thus, a natural, biocompatible, biodegradable, and functional wound care product containing herbal liposomes suitable for both clinical applications and point-of-care use has been developed. The developed bioactive hydrogels are a promising therapeutic approach for the healing of acute wounds. Graphical abstract [Formula: see text]

Hemicelluloses hydrogel: Synthesis, characterization, and application in dye removal

Novel materials using biowaste as adsorbents in wastewater treatment have been allocated considerable interest. Herein, we present the synthesis of different hydrogels of crosslinked polyacrylamide in presence of hemicelluloses with/ without bentonite, using a soft reaction condition. The structure of new hydrogels was characterized by spectroscopic, thermal and microscopic experiments. The semi-interpenetrated network with hemicelluloses: 10 %; acrylamide 79 %; bentonite 10 %; N,N,N′,N′-tetramethylethylenediamine: 1 % allows reducing 20 % the use of non-renewable acrylamide, without changing its decomposition temperatures and keeping its water absorption capacity. This hydrogel was applied to dye removals, such as rhodamine B, methylene red and methylene blue in aqueous solutions. In the case of methylene blue, highest removal is observed with maximum adsorption of qmax = 140.66 mg/g, compared to material without hemicelluloses that only a qmax = 88.495 mg/g. The adsorption kinetics and equilibrium adsorption isotherms are in accordance with the pseudo-second-order kinetic model and Langmuir isotherm model, respectively. The developed hydrogel from hemicelluloses represents a potential alternative adsorbent for a sustainable system of sewage treatment.

Three-dimensional printing of cell-laden bioink for blood vessel tissue engineering: influence of process parameters and components on cell viability

Three-dimensional (3D) bioprinting is a potential therapeutic method for tissue engineering owing to its ability to prepare cell-laden tissue constructs. The properties of bioink are crucial to accurately control the printing structure. Meanwhile, the effect of process parameters on the precise structure is not nonsignificant. We investigated the correlation between process parameters of 3D bioprinting and the structural response of κ-carrageenan-based hydrogels to explore the controllable structure, printing resolution, and cell survival rate. Small-diameter (<6 mm) gel filaments with different structures were printed by varying the shear stress of the extrusion bioprinter to simulate the natural blood vessel structure. The cell viability of the scaffold was evaluated. The in vitro culture of human umbilical vein endothelium cells (HUVECs) on the κ-carrageenan (kc) and composite gels (carrageenan/carbon nanotube and carrageenan/sodium alginate) demonstrated that the cell attachment and proliferation on composite gels were better than those on pure kc. Our results revealed that the carrageenan-based composite bioinks offer better printability, sufficient mechanical stiffness, interconnectivity, and biocompatibility. This process can facilitate precise adjustment of the pore size, porosity, and pore distribution of the hydrogel structure by optimising the printing parameters as well as realise the precise preparation of the internal structure of the 3D hydrogel-based tissue engineering scaffold. Moreover, we obtained perfused tubular filament by 3D printing at optimal process parameters.

Photo and temperature responsive novel surface active ionic liquid-based polymeric hydrogel

Integrating more than two properties into a single polymeric hydrogel to introduce the multi-functionality has been a challenge for the scientific community in recent times. In order to impart photo and temperature responsive characteristics added with adjustable mechanical properties into the polymeric hydrogel, herein we have added newly synthesized photo-responsive ionic liquid (IL) into the polymeric (κ-carrageenan) hydrogel. The IL used is having morpholine-based ester functionalized long chain cation and azobenzene based anion that exhibited trans to cis transformation when irradiated by light of 465 nm for 50 min and show surface-active properties with CMC of 6.83 mM. IL with such photo and temperature responsive properties when mixed with the hydrogel of κ-carrageenan in KCl solution gives the photo and thermo-responsive hybrid hydrogel. The three-dimensional network structure of hydrogel made up of the ellipsoidal aggregates with major and minor axis radius of 9.3 A0 and 1.6 A0, respectively is made up of a fibrous porous structure and gets disrupted through the light irradiation and initiated the gel to sol transition, studied through the SEM images, DLS data and rheological measurements. The (IL) based hydrogel gets disrupted after light irradiation as the anion of the IL starts transforming from trans to cis isomerization. Also, the thermo-reversible transition of hydrogel within room temperature to 54 °C is also shown by rheology. Kinetics of the trans to cis transformation, controlled strain and stress measurement and thermal stability of the hydrogel are assessed here. The studied photo and temperature responsive hydrogel could start a new range of smart materials.

Dynamic Growth of Macroscopically Structured Supramolecular Hydrogels through Orchestrated Reaction-Diffusion.

Living organisms are capable of dynamically changing their structures for adaptive functions through sophisticated reaction-diffusion processes. Here we show how active supramolecular hydrogels with programmable lifetimes and macroscopic structures can be created by relying on a simple reaction-diffusion strategy. Two hydrogel precursors (poly(acrylic acid) PAA/CaCl2 and Na2 CO3 ) diffuse from different locations and generate amorphous calcium carbonate (ACC) nanoparticles at the diffusional fronts, leading to the formation of hydrogel structures driven by electrostatic interactions between PAA and ACC nanoparticles. Interestingly, the formed hydrogels are capable of autonomously disintegrating over time because of a delayed influx of electrostatic-interaction inhibitors (NaCl). The hydrogel growth process is well explained by a reaction-diffusion model which offers a theoretical means to program the dynamic growth of structured hydrogels. Furthermore, we demonstrate a conceptual access to dynamic information storage in soft materials using the developed reaction-diffusion strategy. This work may serve as a starting point for the development of life-like materials with adaptive structures and functionalities.

Dynamic Growth of Macroscopically Structured Supramolecular Hydrogels through Orchestrated Reaction‐Diffusion

AbstractLiving organisms are capable of dynamically changing their structures for adaptive functions through sophisticated reaction‐diffusion processes. Here we show how active supramolecular hydrogels with programmable lifetimes and macroscopic structures can be created by relying on a simple reaction‐diffusion strategy. Two hydrogel precursors (poly(acrylic acid) PAA/CaCl2 and Na2CO3) diffuse from different locations and generate amorphous calcium carbonate (ACC) nanoparticles at the diffusional fronts, leading to the formation of hydrogel structures driven by electrostatic interactions between PAA and ACC nanoparticles. Interestingly, the formed hydrogels are capable of autonomously disintegrating over time because of a delayed influx of electrostatic‐interaction inhibitors (NaCl). The hydrogel growth process is well explained by a reaction‐diffusion model which offers a theoretical means to program the dynamic growth of structured hydrogels. Furthermore, we demonstrate a conceptual access to dynamic information storage in soft materials using the developed reaction‐diffusion strategy. This work may serve as a starting point for the development of life‐like materials with adaptive structures and functionalities.

Design and Evaluation of Liposomal Sulforaphane-Loaded Polyvinyl Alcohol/Polyethylene Glycol (PVA/PEG) Hydrogels as a Novel Drug Delivery System for Wound Healing.

Hydrogel scaffold has been widely applied as drug delivery systems for treating skin injuries. However, the poor drug loading and rapid drug release of hydrogel restricted their application. In the current study, we present a nanoliposome containing sulforaphane (SF) as a nano-drug delivery system that is encapsulated within the scaffold hydrogel system to overcome these limitations and improve wound healing. The hydrogel substrate consisting of 10% polyvinyl alcohol (PVA)/5% polyethylene glycol 400 (PEG400) was prepared by the freeze-thaw method, and the nanoliposomal system was manufactured by the thin film hydration method at different molar ratios of cholesterol: SPC: DPPC: DSPE-PEG2000. The nanoliposome and hydrogel system was characterized by physicochemical analyses. The findings achieved from the optimization of the sulforaphane-loaded nanoliposome (SFNL) displayed an increase in the molar ratio of SPC, leading to a higher entrapment efficiency and a gradual release profile. Narrow size distribution, optimal electrical charge, and the lack of molecular interactions between SF and nanoliposome components in the FTIR analysis make SFNL a suitable drug delivery system for the wound healing process. The obtained SFNL-encapsulated freeze-thawed hydrogel system has sufficient and specific swelling ability at different pH values and increased mechanical strength and elongation. Additionally, the release pattern of SFNL at different pH values showed that the release of SF from liposomes depends on the pH value of the environment and accelerates in line with decreasing pH values. Encapsulation of nanoliposomal SF in the hydrogel structure provides a sustained release pattern of SF compared to its free form and increased as the pH environments continued to raise. The cytotoxicity and cell uptake of SFNL-loaded hydrogels against human skin fibroblasts (HFF cell line) were investigated. The in vitro analyses displayed that the toxicity properties of SF and SFNL were dose-dependent, and SFNL exhibited lower toxicity compared to free SF. Furthermore, the proper cell compatibility of the prepared hydrogel against the HFF cell line was confirmed by the MTT assay. These findings imply that the hydrogel scaffold loaded with SFNL may have wound-healing potential.

Synthesis of amine functionalized SiO2 microspheres loaded polymeric hydrogel and its application for simultaneous eviction of divalent metal ions (Pb2+, Cd2+, Cu2+ and Ni2+)

Recovery of divalent cationic elements from aquatic system is deliberated as reconciliation of rising industrial growth and access to quality drinking water. Herein we report tactically designed amino functionalized silica core-shell nanoparticle loaded polymeric hydrogel network as benchmark sorbent for divalent metal ions (Pb2+, Cd2+, Cu2+, Ni2+). The simple fabrication method for silica core-shell microspheres involves sol-gel synthesis of the polystyrene (PS) core, afterwards the formation of the silica shell by hydrolysis and condensation reaction, and finally the dissolution of the PS core. The surface of synthesized SiO2 microspheres was amine functionalized before being impregnated within a alginate matrix of polymer to generate amino functionalized SiO2 microsphere loaded polymeric hydrogel [NH2–SiO2MS-Ca-Alg] beads. Combining functionalized silica into polymeric hydrogel structure resulted extraordinary sorption capacities for divalent metal ions [191.4, 70.7, 64.9 and 35.8 mg g−1 respectively for Pb, Cd, Cu and Ni]. Density functional theory calculations were carried out to find out binding energies, preferred binding site of all four studied ions and structural changes due to their sorption. Structural evidence derived from experimental observations corroborate with the DFT analysis and speciation diagram of the divalent metal ion species. Plausible mechanistic pathway and differential uptake of four divalent metal ions were explained based on both experimental findings and theoretical studies. Developed NH2–SiO2 MS-Ca-Alg beads offered outstanding selectivity towards four divalent cations in a single prescription, excellent employability under ambient conditions without affecting essential water quality parameters which are significant breakthroughs for sustainable water remediation applications.

Regulated the Swelling Properties of Poly(acrylamide‐co‐acrylic acid) Hydrogel by Changing the Charge Density

AbstractHydrogels can swell without dissolving in water and are widely used in water treatment and biomedicine. The swelling rate of hydrogels is closely related to the network structure and charge density of hydrogels, but there are few detailed studies in this area. In this work, poly(acrylamide‐co‐acrylic acid) anionic hydrogel with acrylic acid (AA) as anionic monomer is prepared. By changing the monomer ratio, or changing the pH value of hydrogels, the internal charge density can be adjusted, and then the swelling rate can be controlled. With the increase of AA monomer content, the content of carboxylate in hydrogel increases, resulting in higher charge density. A high charge density corresponds to a high swelling rate. On the other hand, the swelling rate is closely related to the pH value, which is because the concentration of proton affects the ionization of carboxylic acid, which leads to the change of charge density. It is worth noting when pH increases to 10, the charge shielding effect of the counter‐ion (Na+) gradually increases, thus limiting the swelling of the hydrogel and reducing the swelling rate. This work has reference value for the practical application of hydrogels.

A nitric oxide-catalytically generating carboxymethyl chitosan/sodium alginate hydrogel coating mimicking endothelium function for improving the biocompatibility

Thanks to their outstanding mechanical properties and corrosion resistance in physiological environments, titanium and its alloys are broadly explored in the field of intravascular devices. However, the biocompatibility is insufficient, causing thrombus formation and even implantation failure. In this study, inspired by the functions of endothelial glycocalyx and the NO-releasing of endothelial cells (ECs), a biomimetic coating (TNTA-Se) with three-dimensional gel-like structures and NO-catalytically generating ability was constructed on the titanium surface. To this end, the titanium alloy was firstly anodized and then annealed to form nanotube structures imitating the three-dimensional villous of glycocalyx, followed by the preparation of the Cu2+-loaded polydopamine intermediate layer for the immobilization of carboxymethyl chitosan and sodium alginate to form the hydrogel structure. Finally, an organoselenium compound (selenocystamine) as an active catalyst was covalently immobilized on the surface to develop a bioactive coating mimicking endothelial function with NO-generating activity. The surface morphologies and chemical structures of the biomimetic coating were characterized by scanning electron microscopy (SEM), energy dispersion X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), and the results indicated that the NO-catalytically generating hydrogel coating was successfully constructed. The results of water contact angle and protein adsorption suggested that the TNTA-Se coating exhibited excellent hydrophilicity, the promotion of bovine serum albumin (BSA) adsorption while the inhibition of fibrinogen (FIB) adsorption. Upon the addition of NO donor S-nitroso glutathione (GSNO) and reducing agent glutathione (GSH), the surface (TNTA-NO) displayed excellent blood compatibility and cytocompatibility to ECs. Compared with other surfaces, the TNTA-NO coating can not only further promote BSA adsorption and inhibit the adhesion and activation of platelets as well as hemolysis, but also significantly enhance ECs adhesion and proliferation and up-regulate VEGF and NO expression of ECs. The current study demonstrated that the NO-catalytically generating hydrogel coating on the titanium alloy can mimic the glycocalyx structure and endothelium function to catalyze a large number of NO donors in human blood to produce NO, and thus simultaneously enhance the surface hemocompatibility and endothelialization, representing a promising strategy for long-term cardiovascular implants of titanium-based devices.

A green and sustainable approach for the preparation of Cu-containing alginate fibers

The development of biopolymer fibers is attracting considerable interest due to the need to reduce the environmental impact of the petroleum-based industry. With the aim to foster the use of biopolymer-based antimicrobial fibers, a green and sustainable preparation route for alginate fibers containing copper-based nanostructures is reported. Its strong antimicrobial properties and affinity for alginate make copper the ideal candidate for the preparation of products suitable for various applications. In this work alginate is extruded and crosslinked in a Cu2+ aqueous bath, producing a filiform hydrogel structure. Ascorbic acid was then used to reduce the metal ions and to form the aforementioned nanostructures. This in situ strategy for the reduction of coordinating Cu2+ ions is unprecedented and leads to a homogeneous distribution of the inorganic structures in the polymeric network. The entire process can be monitored through infrared spectroscopy and the performances (e.g., thermal stability, morphology, swelling, water retention, mechanical properties) of the obtained products are tunable as a function of the duration of each preparation step. The great affinity for water and the small amount of Cu2+ released as a function of time suggest promising perspectives for the use of these fibers in antimicrobial applications.

Preparation and sustained release bacteriostatic performance of pH-responsive complex hydrogel bacteriostatic microspheres for oral drug delivery

pH-responsive hydrogel antibacterial microspheres were prepared by complex coacervation method and used as drug carriers to load the antibiotic substitute potassium diformate (KDF). The results showed that the three-dimensional network structure of the composite hydrogel was formed among the polysaccharide components, and Zeolite A loaded with KDF was uniformly dispersed in it. The results of drug release behavior and kinetics in vitro showed that the drug release rate was higher and the release mechanism followed the Ritger-Peppas model, which indicated that the antibacterial microspheres had a good pH response. In vitro, the carrier showed broad-spectrum antibacterial activity, good biocompatibility, and degradability.

Wearable Liquid Metal Composite with Skin-Adhesive Chitosan-Alginate-Chitosan Hydrogel for Stable Electromyogram Signal Monitoring.

In wearable bioelectronics, various studies have focused on enhancing prosthetic control accuracy by improving the quality of physiological signals. The fabrication of conductive composites through the addition of metal fillers is one way to achieve stretchability, conductivity, and biocompatibility. However, it is difficult to measure stable biological signals using these soft electronics during physical activities because of the slipping issues of the devices, which results in the inaccurate placement of the device at the target part of the body. To address these limitations, it is necessary to reduce the stiffness of the conductive materials and enhance the adhesion between the device and the skin. In this study, we measured the electromyography (EMG) signals by applying a three-layered hydrogel structure composed of chitosan-alginate-chitosan (CAC) to a stretchable electrode fabricated using a composite of styrene-ethylene-butylene-styrene and eutectic gallium-indium. We observed stable adhesion of the CAC hydrogel to the skin, which aided in keeping the electrode attached to the skin during the subject movement. Finally, we fabricated a multichannel array of CAC-coated composite electrodes (CACCE) to demonstrate the accurate classification of the EMG signals based on hand movements and channel placement, which was followed by the movement of the robot arm.

Hybrid Vesicles Enable Mechano-Responsive Hydrogel Degradation.

Stimuli-responsive hydrogels are intriguing biomimetic materials. Previous efforts to develop mechano-responsive hydrogels have mostly relied on chemical modifications of the hydrogel structures. Here, we present a simple, generalizable strategy that confers mechano-responsive behavior on hydrogels. Our approach involves embedding hybrid vesicles, composed of phospholipids and amphiphilic block copolymers, within the hydrogel matrix to act as signal transducers. Under mechanical stress, these vesicles undergo deformation and rupture, releasing encapsulated compounds that can control the hydrogel network. To demonstrate this concept, we embedded vesicles containing ethylene glycol tetraacetic acid (EGTA), a calcium chelator, into a calcium-crosslinked alginate hydrogel. When compressed, the released EGTA sequesters calcium ions and degrades the hydrogel. This study provides a novel method for engineering mechano-responsive hydrogels that may be useful in various biomedical applications.