Mechanical Properties Of Hydrogels Research Articles

Effect of supramolecular peptide hydrogel scaffold charge on HepG2 viability and spheroid formation.

Supramolecular bioinspired self-assembling peptide hydrogel (SAPH) scaffolds represent a class of fully defined synthetic materials whose chemical and mechanical properties can be finely engineered. In this study, the relationship between SAPHs physicochemical properties and HepG2 cells viability, spheroid formation and function are discussed. We first report that negatively charged SAPHs promote hepatocyte proliferation and spheroids formation in vitro 3D culture while positively charged SAPHs lead to hepatocyte death irrespective of the hydrogel mechanical properties. More specifically HepG2 cultured in 3D in E(FKFE)2 negatively charged SAPH maintained a differentiated phenotype and assembled into well-defined spheroids with strong cell-cell interactions. Furthermore, HepG2 spheroids responded to acetaminophen exposure with upregulation of key CYP450 enzymes expression clearly showing their potential for drug toxicity testing. These findings demonstrate how fine-tuned functional SAPH scaffolds can be used to identify key scaffolds parameters affecting cells. In this case we demonstrated the potential of negatively charged SAPHs for the 3D culture of HepG2 with potential applications in drug screening.

Numerical modeling of heterogeneous stimuli-responsive hydrogels

In this paper, we introduce a computational technique for modeling heterogeneous thermoresponsive hydrogels. The model resolves local fluid-solid interactions in hydrogel pores during the deswelling process. The model is a Lagrangian particle-based technique, which benefits from computational grids that represent polymer beads inside hydrogel scaffolds. The results show that the mechanical properties of hydrogels during deswelling, e.g., shrinkage ratio and elastic modulus, have a direct effect on the development of the front of expelled fluid. It is also observed that in certain parameter regimes the hydrogel may generate inertial fluid jets at the early stages of deswelling. Finally, simple heterogeneous designs are developed using Menger sponge-inspired shapes to investigate the effect of design heterogeneity on promoting directional release. Published by the American Physical Society 2024

Engineering Phi29-DNAP Variants for Customized DNA Hydrogel Materials.

DNA hydrogels, which hold potential for use in medicine, biosensors, and tissue engineering, can be produced through enzymatic rolling circle amplification (RCA) using phi29 DNA polymerase (DNAP). This paper introduces new DNAP variants designed for RCA-based DNA hydrogel production, featuring enzymes with modified DNA binding, enhanced thermostability, reduced exonuclease activity, and protein tags for fluorescence detection or specific immobilization. We evaluated these enzymes by quantifying DNA output via quantitative PCR (qPCR) and assessing hydrogel mechanical properties through micromechanical indentation. The results showed that most variants generated similar DNA amounts and hydrogels with comparable mechanical properties. Additionally, all variants successfully incorporated non-natural nucleotides, such as base-modified dGTP derivatives and 2'-fluoro-dGTP, during RCA. This study's robust analytical approach offers a strong foundation for selecting new enzymes and producing DNA hydrogels with tailored material properties.

Structure-Reactivity Relationships in a Small Library of Imine-Type Dynamic Covalent Materials: Determination of Rate and Equilibrium Constants Enables Model Prediction and Validation of a Unique Mechanical Softening in Dynamic Hydrogels.

The development of next generation soft and recyclable materials prominently features dynamic (reversible) chemistries such as host-guest, supramolecular, and dynamic covalent. Dynamic systems enable injectability, reprocessability, and time-dependent mechanical properties. These properties arise from the inherent relationship between the rate and equilibrium constants (RECs) of molecular junctions (cross-links) and the resulting macroscopic behavior of dynamic networks. However, few examples explicitly measure RECs while exploring this connection between molecular and material properties, particularly for polymeric hydrogel systems. Here we use dynamic covalent imine formation to study how single-point compositional changes in NH2-terminated nucleophiles affect binding constants and resulting hydrogel mechanical properties. We explored both model small molecule studies and model polymeric macromers, and found >3-decade change in RECs. Leveraging established relationships in the literature, we then developed a simple model to describe the cross-linking equilibrium and predict changes in hydrogel mechanical properties. Interestingly, we observed that a narrow ≈2-decade range of Keq's determine the bound fraction of imines. Our model allowed us to uncover a regime where adding cross-linker before saturation can decrease the cross-link density of a hydrogel. We then demonstrated the veracity of this predicted behavior experimentally. Notably this emergent behavior is not accounted for in covalent hydrogel theory. This study expands upon structure-reactivity relationships for imine formation, highlighting how quantitative determination of RECs facilitates predicting macroscopic behavior. Furthermore, while the present study focuses on dynamic covalent imine formation, the underlying principles of this work are applicable to the general bottom-up design of soft and recyclable dynamic materials.

Microstructure and characteristics of phase-separated gels of Type-A gelatin and hydroxypropyl starch: pH responsiveness

The impact of phase separation behavior on the performance of hydrogels has always been the research focus. This study explored the relationship of “pH-microstructure-hydrogel properties” of phase-separated hydrogels composed of type-A gelatin (GE, 5 wt%) and hydroxypropyl starch (HPS, 3 wt%). The results revealed that changes in the microstructure of the hydrogel at different pHs significantly impacted the gel properties. At pH 4.00 and 11.00, phase separation occurred in the GE/HPS gel with a microstructure of HPS-in-GE. In particular, at pH 5.00, 6.00, 7.00, and 9.00, severe phase separation resulted in the separation of substantial aggregates of HPS and GE, resulting in a continuous phase structure. At pH 2.00 and 3.00, phase separation was suppressed, resulting in a homogeneous microstructure. Compared to the phase-separated gels at pH 4.00–11.00, the homogeneous systems at pH 2.00 and 3.00 displayed a synergistic effect with higher gel strength. Analysis of intermolecular forces in the GE/HPS gel indicated that hydrogen bonding was the primary interaction force. Furthermore, the addition of GE/HPS into hawthorn jelly at about pH 3.00 effectively preserved the structural appearance and exhibited higher levels of hardness, thus improving the sensory properties of hawthorn jelly. In summary, phase separation decreased the storage modulus of GE/HPS gel, but the compatibility of GE/HPS macromolecules exhibited synergistic effects at 2.00 and 3.00 and improved the hydrogel mechanical properties. This work provides some new insights for GE/HPS-based gel foods.

Antibacterial Properties of Grape Seed Extract-Enriched Cellulose Hydrogels for Potential Dental Application: In Vitro Assay, Cytocompatibility, and Biocompatibility.

Hydrogels elaborated from Dasylirion spp. and enriched with grape seed extract (GSE) were investigated for tentative use in dental treatment. Cellulose-GSE hydrogels were elaborated with varying GSE contents from 10 to 50 wt%. The mechanical and physical properties, antimicrobial effect, biocompatibility, and in vitro cytotoxicity were studied. In all the cases, the presence of GSE affects the hydrogel's mechanical properties. The elongation decreased from 12.67 mm for the hydrogel without GSE to 6.33 mm for the hydrogel with the highest GSE content. The tensile strength decrease was from 52.33 N/mm2 (for the samples without GSE) and went to 40 N/mm2 for the highest GSE content. Despite the adverse effects, hydrogels possess suitable properties for manipulation. In addition, all hydrogels exhibited excellent biocompatibility and no cytotoxicity, and the antibacterial performance was demonstrated against S. mutans, E. Faecalis, S. aureus, and P. aureginosa. Furthermore, the hydrogels with 30 wt% GSE inhibited more than 90% of the bacterial growth.

The effect of swelling/deswelling cycles on the mechanical behaviors of the polyacrylamide hydrogels

In practical applications, hydrogels experience swelling or deswelling in response to external stimuli, showcasing large deformation, tunable mechanical properties, and excellent biocompatibility. Previous studies focused on the effect of individual swelling or deswelling on the mechanical behaviors of hydrogels, neglecting the combined effects of both processes. The underlying mechanism of how the combined processes of swelling and deswelling affect the mechanical behaviors of hydrogels has not been systematically explored. To address this gap, polyacrylamide hydrogels with diverse initial compositions are prepared and subjected to controlled swelling-deswelling or deswelling-swelling cycles to achieve the same water content state. The mechanical properties of the hydrogel samples exposed to these cycles, including shear modulus, stretchability, Mullins effect, and fracture toughness, are experimentally evaluated and compared with those of as-prepared hydrogel samples without undergoing such cycles. Our findings reveal a significant reduction in stretchability, the Mullins effect, and fracture toughness of hydrogels exposed to either cycle. The extent of these reductions varies depending on the initial compositions of the hydrogels. This reduction in properties is primarily attributed to the rearrangement of hydrogel networks during these cycles, which becomes noticeable in hydrogels with network inhomogeneity. We also found that although the shear modulus of hydrogels varies after swelling-deswelling or deswelling-swelling cycles, it remains at relatively consistent levels compared to the as-prepared hydrogel. These findings suggest that the mechanical properties of hydrogels can be adjusted by optimizing the initial compositions and regulating the swelling-deswelling processing method. By studying the effects of swelling/deswelling cycles on the mechanical properties of hydrogels, we provide valuable insights for the application of hydrogels under dynamic environmental changes.

Leveraging the Physicochemical Attributes of Biomimetic Hydrogel Nanocomposites in Stem Cell Differentiation.

The field of tissue engineering has witnessed significant advancements with the advent of hydrogel nanocomposites (HNC), emerging as a highly promising platform for regenerative medicine. HNCs provide a versatile platform that significantly enhances the differentiation of stem cells into specific cell lineages, making them highly suitable for tissue engineering applications. By incorporating nanoparticles, the mechanical properties of hydrogels, such as elasticity, porosity, and stiffness, are improved, addressing common challenges such as short-term stability, cytotoxicity, and scalability. These nanocomposites also exhibit enhanced biocompatibility and bioavailability, which are crucial to their effectiveness in clinical applications. Furthermore, HNCs are responsive to various triggers, allowing for precise control over their chemical properties, which is beneficial in creating 3D microenvironments, promoting wound healing, and enabling controlled drug delivery systems. This review provides a comprehensive overview of the production methods of HNCs and the factors influencing their physicochemical and biological properties, particularly in relation to stem cell differentiation and tissue repair. Additionally, it discusses the challenges in developing HNCs and highlights their potential to transform the field of regenerative medicine through improved mechanotransduction and controlled release systems.

Quantitative Characterization of RCA-Based DNA Hydrogels - Towards Rational Materials Design.

DNA hydrogels hold significant promise for biomedical applications and can be synthesized through enzymatic Rolling Circle Amplification (RCA). Due to the exploratory nature of this emerging field, standardized RCA protocols specifying the impact of reaction parameters are currently lacking. This study varied template sequences and reagent concentrations, evaluating RCA synthesis efficiency and hydrogel mechanical properties through quantitative PCR (qPCR) and indentation measurements, respectively. Primer concentration and stabilizing additives showed minimal impact on RCA efficiency, while changes in polymerase and nucleotide concentrations had a stronger effect. Concentration of the circular template exerted the greatest influence on RCA productivity. An exponential correlation between hydrogel viscosity and DNA amplicon concentration was observed, with nucleobase sequence significantly affecting both amplification efficiency and material properties, particularly through secondary structures. This study suggests that combining high-throughput experimental methods with structural folding prediction offers a viable approach for systematically establishing structure-property relationships, aiding the rational design of DNA hydrogel material systems.

Tough and self-adhesive zwitterionic hydrogels with mechano-responsive release of bFGF for tympanic membrane repair

The tympanic membrane (TM) is constantly in a state of vibrating. However, there is currently a lack of drug-delivery scaffolds suitable for the dynamic environment of TM perforation. In this study, a mechano-responsive tough hydrogel was developed. It consists of basic fibroblast growth factor (bFGF)-loaded sodium alginate (SA) microspheres, polysulfobetaine methacrylate (polySBMA), and gelatin methacrylate (GelMA). This hydrogel was designed to serve as a TM scaffold to promote perforation healing under dynamic conditions. bFGF was encapsulated in SA microspheres, which were then incorporated into polySBMA-GelMA hydrogels through photo-initiated free radical polymerization. The mechanical properties, tissue adhesiveness, swelling properties, and degradation of the hydrogels were evaluated before and after microsphere incorporation. It was observed that incorporating bFGF-loaded SA microspheres did not significantly impact the adhesion and degradation mechanisms of the hydrogel. The compressive strength and tensile strength of the microsphere-incorporated hydrogel were up to 6.6 MPa and 64.1 kPa, respectively, suitable for a TM scaffold. The release behavior of bFGF from the hydrogel could be controlled by vibration stimulation without significantly affecting the hydrogel's mechanical properties, indicating a mechano-responsive nature of the hydrogel. The in vitro cytotoxicity assay demonstrated that the hydrogels showed no cytotoxic effects. Moreover, cell culture assays demonstrated that vibration stimulation could enhance the release of bFGF, significantly promoting cell proliferation and migration. The results demonstrate the significant potential of the mechano-responsive hydrogel as a scaffold for repairing TM perforations.

High-strength conductive hydrogels based on the Hofmeister effect for friction nanogenerators

Hydrogels have received much attention in the field of flexible electronics as materials with flexibility and multifunctionality. The mechanical strength of conventional hydrogels is usually difficult to meet the requirements of practical applications in electronic devices. How to fabricate a high-strength hydrogel should remain a challenge. Here, a strategy to enhance the mechanical properties of conductive hydrogels based on the Hofmeister effect is reported. The mechanical properties of hydrogels were enhanced by increasing the polymer chain density, enhancing the hydrophobicity and increasing the crystallinity, the high-strength and high-toughness polyvinyl alcohol/carbon nanotubes/polyethyleneimine (PVA/MWCNTs/PEI) conductive hydrogel was successfully produced. The ultimate stress of the hydrogel was as high as 3.5–6.3 MPa, the elongation at break was between 500 and 1200 %, and the toughness was up to 23.62 MJ/m3. The conductivity of high-strength, high-toughness hydrogel is 0.05–0.45 S/m. Hydrogel was manufactured into a single-electrode friction nanogenerator (TENG), and it can easily light up to 100 LEDs. Therefore, this high-strength and high-toughness conductive hydrogel has great potential for TENG applications, offering the possibility of extending the working life of TENG in harsh environments.

Tuning viscoelasticity and stiffness in bioprinted hydrogels for enhanced 3D cell culture: A multi-scale mechanical analysis

Bioprinted hydrogels are extensively studied to provide an artificial matrix for 3D cell culture. The success of bioprinting hydrogels relies on fine-tuning their rheology and composition to achieve shear-thinning behavior. However, a challenge arises from the limited viscoelastic and stiffness range accessible from a single hydrogel formulation. Nevertheless, hydrogel mechanical properties are recognized as essential cues influencing cell phenotype, migration, and differentiation. Thus, it is crucial to develop a system to easily modulate bioprinted hydrogels' mechanical behaviors.In this work, we modulated the viscoelastic properties and stiffness of bioprinted hydrogels composed of fibrinogen, alginate, and gelatin by tuning the crosslinking bath solution. Various concentrations of calcium ionically crosslinked alginate, while transglutaminase crosslinked gelatin. Subsequently, we characterized the mechanical behavior of our bioprinted hydrogels from the nanoscale to the macroscale. This approach enabled the production of diverse bioprinted constructs, either with similar elastic behavior but different elastic moduli or with similar elastic moduli but different viscoelastic behavior from the same hydrogel formulation.Culturing fibroblasts in the hydrogels for 33 days revealed a preference for cell growth and matrix secretion in the viscoelastic hydrogels. This work demonstrates the suitability of the method to decouple the effects of material mechanical from biochemical composition cues on 3D cultured cells.

Relation between the Water Content and Mechanical Properties of Hydrogels with Movable Cross-Links

Relation between the Water Content and Mechanical Properties of Hydrogels with Movable Cross-Links

Electric-field assisted cascade reactions to create alginate/carboxymethyl chitosan composite hydrogels with gradient architecture and reconfigurable mechanical properties

Rational designs of polysaccharide-based hydrogels with organ-like three-dimensional architecture provide a great possibility for addressing the shortages of allograft tissues and organs. However, spatial-temporal control over structure in bulk hydrogel and acquire satisfied mechanical properties remain an intrinsic challenge to achieve. Here, we show how electric-field assisted molecular self-assembly can be coupled to a directional reaction-diffusion (RD) process to produce macroscopic hydrogel in a controllable manner. The electrical energy input was not only to generate complex molecule gradients and initiate the molecular self-assembly, but also to guide/facilitate the RD processes for the gel rapid growth via a cascade construction interaction. The hydrogel mechanical properties can be tuned and enhanced by using an interpenetrating biopolymer network and multiple ionic crosslinkers, leading to a wide-range of mechanical modulus to match with biological organs or tissues. We demonstrate diverse 3D macroscopic hydrogels can be easily prepared via field-assisted directional reaction-diffusion and specific joint interactions. The humility-triggered dissipation of functional gradients and antibacterial performance confirm that the hydrogels can serve as an optically variable soft device for wound management. Therefore, this work provides a general approach toward the rational fabrication of soft hydrogels with controlled architectures and functionality for advanced biomedical systems.

Integrating Mechanics and Bioactivity: A Detailed Assessment of Elasticity and Viscoelasticity at Different Scales in 2D Biofunctionalized PEGDA Hydrogels for Targeted Bone Regeneration.

Methods for promoting and controlling the differentiation of human mesenchymal stem cells (hMSCs) in vitro before in vivo transplantation are crucial for the advancement of tissue engineering and regenerative medicine. In this study, we developed poly(ethylene glycol) diacrylate (PEGDA) hydrogels with tunable mechanical properties, including elasticity and viscoelasticity, coupled with bioactivity achieved through the immobilization of a mixture of RGD and a mimetic peptide of the BMP-2 protein. Despite the key relevance of hydrogel mechanical properties for cell culture, a standard for its characterization has not been proposed, and comparisons between studies are challenging due to the different techniques employed. Here, a comprehensive approach was employed to characterize the elasticity and viscoelasticity of these hydrogels, integrating compression testing, rheology, and atomic force microscopy (AFM) microindentation. Distinct mechanical behaviors were observed across different PEGDA compositions, and some consistent trends across multiple techniques were identified. Using a photoactivated cross-linker, we controlled the functionalization density independently of the mechanical properties. X-ray photoelectrin spectroscopy and fluorescence microscopy were employed to evaluate the functionalization density of the materials before the culturing of hMSCs on them. The cells cultured on all functionalized hydrogels expressed an early osteoblast marker (Runx2) after 2 weeks, even in the absence of a differentiation-inducing medium compared to our controls. Additionally, after only 1 week of culture with osteogenic differentiation medium, cells showed accelerated differentiation, with clear morphological differences observed among cells in the different conditions. Notably, cells on stiff but stress-relaxing hydrogels exhibited an overexpression of the osteocyte marker E11. This suggests that the combination of the functionalization procedure with the mechanical properties of the hydrogel provides a potent approach to promoting the osteogenic differentiation of hMSCs.

3D-bioprinted gelatin methacryloyl hydrogel culture system emulating the oviduct environment for enhanced preimplantation embryo development

Oviducts have specific biomechanical properties that support fertilization and preimplantation embryo development, both of which are essential for successful pregnancy. However, conventional plastic-based human embryo culture does not recapitulate the biomechanical environment of the oviduct. Therefore, oviduct mimic culture systems that accurately emulate biophysical conditions for reproductive cells are a significant unmet clinical need. In the present study, we designed a three-dimensional (3D)-bioprinted optimal soft hydrogel system that accurately mimics the oviduct environment and investigated signaling factors during embryo development. We developed an oviduct tube-mimic hydrogel culture dish using gelatin methacryloyl (GelMA) 3D-bioprinted hydrogel. Quantitative assessment of hydrogel mechanical properties depended on the stiffness of the GelMA 3D-bioprinted hydrogel. Embryo quality was evaluated based on cleavage speed and blastocyst ratio on the GelMA hydrogel. Whole-transcriptome next-generation sequencing (NGS) analysis of embryos was used to identify biomechanical signaling factors. Our findings revealed that 10 kPa GelMA hydrogel culture conditions performed better with respect to development speed, blastocyst ratio, and hatching ratio than the control condition. Whole transcriptome NGS revealed up-regulation of mRNA processing genes and protein transport genes by the 7 and 10 kPa hydrogels. Furthermore, the inner cell mass and the number of Oct4+ cells were significantly higher in blastocysts cultured on 10 kPa hydrogel dishes than in those cultured on conventional hard plastic dishes. These findings demonstrate that optimized oviduct-mimic hydrogel-based 3D GelMA culture dishes could improve in vitro embryo development. Hence, 3D GelMA culture dishes may be useful as human embryo culture systems for assisted reproductive techniques.

Mechanical properties of agarose hydrogels tuned by amphiphilic structures

Agarose is a biocompatible polysaccharide that is capable to form physically cross-linked hydrogels in aqueous dispersion. These materials offer a wide range of applications and are commonly used in the food industry or electrophoresis. Moreover, due to their favourable characteristics (biocompatibility, high water absorption, porosity), agarose hydrogels have recently also found applications also in drug delivery systems, wound dressing, and extracellular matrix (ECM) modelling. This paper presents a comprehensive rheological characterization of agarose hydrogels with various self-assembled amphiphilic structures (CTAB, TTAB, SDS, Tween 20) acting as simple membrane structure models. These findings demostrated that the presence of surfactants of diverse charge above their critical micellar concentration (CMC) can enhance hydrogel mechanical properties. Moreover, pronounced enhancement was observed for cationic surfactant, and even concentrations below CMC resulted in a higher stiffness of the hydrogel. Therefore, both the electrostatic effect and the amphiphilic structure effect can have a significant impact on the rheological properties on agarose hydrogels. These findings are of a significant interest in the field of polymer and surfactants interactions, since agarose is widely considered essentially uncharged. However, it is assumed, that traces of negatively charged groups on the agarose backbone can have a significant impact when interacting with oppositely charged surfactants. Moreover, these findings could be beneficial for better understanding of interaction of polysaccharides (e.g. agarose) and self-assembled amphiphilic structures and can also be considered as a crude model of ECM in which membrane structures are embedded.

Effectiveness of gellan gum scaffolds loaded with Boswellia serrata extract for in-situ modulation of pro-inflammatory pathways affecting cartilage healing

In this study, we developed a composite hydrogel based on Gellan gum containing Boswellia serrata extract (BSE). BSE was either incorporated directly or loaded into an MgAl-layered double hydroxide (LDH) clay to create a multifunctional cartilage substitute. This composite was designed to provide anti-inflammatory properties while enhancing chondrogenesis. Additionally, LDH was exploited to facilitate the loading of hydrophobic BSE components and to improve the hydrogel's mechanical properties. A calcination process was also adopted on LDH to increase BSE loading. Physicochemical and mechanical characterizations were performed by spectroscopic (XPS and FTIR), thermogravimetric, rheological, compression test, weight loss and morphological (SEM) investigations. RPLC-ESI-FTMS was employed to investigate the boswellic acids release in simulated synovial fluid. The composites were cytocompatible and capable of supporting the mesenchymal stem cells (hMSC) growth in a 3D-conformation. Loading BSE resulted in the modulation of the pro-inflammatory cascade by down-regulating COX2, PGE2 and IL1β. Chondrogenesis studies demonstrated an enhanced differentiation, leading to the up-regulation of COL 2 and ACAN. This effect was attributed to the efficacy of BSE in reducing the inflammation through PGE2 down-regulation and IL10 up-regulation. Proteomics studies confirmed gene expression findings by revealing an anti-inflammatory protein signature during chondrogenesis of the cells cultivated onto loaded specimens. Concluding, BSE-loaded composites hold promise as a tool for the in-situ modulation of the inflammatory cascade while preserving cartilage healing.

Natural Polyelectrolyte Hydrogels with Two Types of Cross-Links with Different Energy

For the first time, gels of a polymer cross-linked by two types of ionic cross-links of different energies, namely trivalent chromium (III) ions and divalent iron (II) ions, were prepared. The negatively charged polysaccharide xanthan, a polyelectrolyte of natural origin, was used as a polymer. A study of xanthan gels cross-linked with each cross-linker separately was carried out to identify the optimal concentrations of each cross-linker for the production of a double cross-linked gel. The mechanical properties of hydrogels under oscillatory shear deformations were then studied. It was demonstrated that the simultaneous use of two cross-linkers resulted in a synergistic increase in the elastic modulus (plateau storage modulus) compared to gels cross-linked with each cross-linker separately. For a gel with two types of cross-links, the elastic modulus was 16 Pa. In contrast, for gels cross-linked with either chromium (III) cations or iron (II) cations, the elastic modulus was approximately 0.6 and 0.5 Pa, respectively. The strong effect can be attributed to the different nature of cross-linking between xanthan macromolecules and chromium (III) and iron (II) cations, as well as the different strength of the cross-links formed. The optimal range of pH values was determined in which a synergistic increase in the elastic modulus of gels with two types of cross-links was observed compared to the corresponding gels cross-linked with each cross-linker separately. Consequently, the concurrent utilisation of two cross-linking agents that generate cross-links with disparate energy levels represents an efficacious strategy to improve the tensile strength of polymer hydrogels.

A light/thermal cascaded-driven equipment for machine recognition inspired by water lilies using as multifunctional soft actuator

Inspired by the natural stimulus–response of plants and animals, a range of soft equipment has been extensively developed and used in intelligent human–computer interaction, editable remote drives, and machine learning. Poly(N-isopropyl acrylamide) (PNIPAM) hydrogels have gained popularity thanks to their low phase transition temperature and excellent flexibility. However, the PNIPAM hydrogels suffer from poor mechanical properties, low electrical conductivity, and lack of self-responsiveness. Herein, a bilayer light/thermal cascaded-driven anisotropic poly acrylamide/poly(N-isopropylacrylamide-co-acrylamide)-polyvinyl alcohol-MXene (P/PP-M) actuator was prepared by a simple two-step polymerization method. The unique bionic light/thermal response mechanism enables rapid conversion of energy forms and the construction of remote editable actuators. Concretely, the mechanical properties of hydrogels (strain: 1014 %, stress: 94 KPa) have been greatly improved by copolymerizing MXene nanosheets and multiplex hydrogels through two-by-two interpenetrating molecular chains. MXene nanosheets formed dynamic networks conferring the hydrogel system with high conductivity and light/thermal conversion efficiency. The P/PP-M soft actuator features high sensitivity (Gauge factor = 3.62), fast response time (400 ms), and cycling durability (>500 cycles). Finally, the energy transfer mechanism from light to thermal energy to kinetic energy was corroborated by preparing a series of bionic equipment. Manual clips were prepared on this basis, which enables the transportation of objects and realizes the real-time reflection of the operating status of remotely driven soft manual clips through changes in electrical signals. Thus, the proposed efficient editable remote-driven machine recognition soft equipment provides new insights for developing intelligent flexible robots and wearable smart devices.