Ionization Engineering of Hydrogels Enables Highly Efficient Salt‑Impeded Solar Evaporation and Night‑Time Electricity Harvesting

Interfacial solar evaporation holds immense potential for brine desalination with low carbon footprints and high energy utilization.Hydrogels,as a tunable material platform from the molecular level to the macroscopic scale,have been considered the most promising candidate for solar evaporation.However,the simultaneous achievement of high evaporation efficiency and satisfactory tolerance to salt ions in brine remains a challenging scientific bottleneck,restricting the widespread application.Herein,we report ionization engineering,which endows polymer chains of hydrogels with electronegativity for impeding salt ions and activating water molecules,fundamentally overcoming the hydrogel salt-impeded challenge and dramatically expediting water evaporating in brine.The sodium dodecyl benzene sulfonate-modified carbon black is chosen as the solar absorbers.The hydrogel reaches a ground-breaking evaporation rate of 2.9 kg m−2 h−1 in 20 wt%brine with 95.6%efficiency under one sun irradiation,surpassing most of the reported literature.More notably,such a hydrogel-based evaporator enables extracting clean water from oversaturated salt solutions and maintains durability under different high-strength deformation or a 15-day continuous operation.Meantime,on the basis of the cation selectivity induced by the electronegativity,we first propose an all-day system that evaporates during the day and generates salinity-gradient electricity using waste-evaporated brine at night,anticipating pioneer a new opportunity for all-day resource-generating systems in fields of freshwater and electricity.

Nanozyme‑Engineered Hydrogels for Anti‑Inflammation and Skin Regeneration

Inflammatory skin disorders can cause chronic scarring and functional impairments,posing a significant burden on patients and the healthcare system.Conventional therapies,such as corticosteroids and nonsteroidal anti-inflammatory drugs,are limited in efficacy and associated with adverse effects.Recently,nanozyme(NZ)-based hydrogels have shown great promise in addressing these challenges.NZ-based hydrogels possess unique therapeutic abilities by combining the therapeutic benefits of redox nanomaterials with enzymatic activity and the water-retaining capacity of hydrogels.The multifaceted therapeutic effects of these hydrogels include scavenging reactive oxygen species and other inflammatory mediators modulating immune responses toward a pro-regenerative environment and enhancing regenerative potential by triggering cell migration and differentiation.This review highlights the current state of the art in NZ-engineered hydrogels(NZ@hydrogels)for anti-inflammatory and skin regeneration applications.It also discusses the underlying chemo-mechano-biological mechanisms behind their effectiveness.Additionally,the challenges and future directions in this ground,particularly their clinical translation,are addressed.The insights provided in this review can aid in the design and engineering of novel NZ-based hydrogels,offering new possibilities for targeted and personalized skin-care therapies.

Application of Optical Hydrogels in Environmental Sensing

The ever-increasing complexity of environmental pollutants urgently warrants the development of new detection technologies.Sensors based on the optical properties of hydrogels enabling fast and easy in situ detection are attracting increasing attention.In this paper,the data from 138 papers about different optical hydrogels(OHs)are extracted for statistical analysis.The detection performance and potential of various types of OHs in different environmental pollutant detection scenarios were evaluated and compared to those obtained using the standard detection method.Based on this analysis,the target recognition and sensing mechanisms of two main types of OHs are reviewed and discussed:photonic crystal hydrogels(PCHs)and fluorescent hydrogels(FHs).For PCHs,the environmental stimulus response,target receptors,inverse opal structures,and molecular imprinting techniques related to PCHs are reviewed and summarized.Furthermore,the different types of fluorophores(i.e.,compound probes,biomacromolecules,quantum dots,and luminescent microbes)of FHs are discussed.Finally,the potential academic research directions to address the challenges of applying and developing OHs in environmental sensing are proposed,including the fusion of various OHs,introduction of the latest technologies in various fields to the construction of OHs,and development of multifunctional sensor arrays.

Fluorescent Double Network Hydrogels with Ionic Responsiveness and High Mechanical Properties for Visual Detection

We developed a fluorescent double network hydrogel with ionic responsiveness and high mechanical properties for visual detection.The nanocomposite hydrogel of laponite and polyacrylamide serves as the first network,while the ionic cross-linked hydrogel of terbium ions and sodium alginate serves as the second network.The double-network structure,the introduction of nanoparticles and the reversible ionic crosslinked interactions confer high mechanical properties to the hydrogel.Terbium ions are not only used as the ionic cross-linked points,but also used as green emitters to endow hydrogels with fluorescent properties.On the basis of the “antenna effect” of terbium ions and the ion exchange interaction,the fluorescence of the hydrogels can make selective responses to various ions(such as organic acid radical ions,transition metal ions) in aqueous solutions,which enables a convenient strategy for visual detection toward ions.Consequently,the fluorescent double network hydrogel fabricated in this study is promising for use in the field of visual sensor detection.

White-light-induced synthesis of injectable alginate-based composite hydrogels for rapid hemostasis

Dear Editor,Timely and effective hemostasis is of great significance for reducing body damage and mortality of patients [1]. Alginate is generally considered to be an excellent hemostatic polymer-based biomaterial and has been approved by the Food and Drug Administration as Generally Recognized as Safe [2]. However, the violent crosslinking reaction and unstable structure at the wound site limit its clinical applications. Hence, we report a biocompatible and injectable composite hydrogel methacrylate alginate (Alg-AEMA)-based Eosin Y/N-phenylglycine (NPG)-initiated composite hydrogel (AEC) composed of photocrosslinkable alginate, viscosity modifiers and novel white light photoinitiator, namely Eosin Y/NPG system, for instant hemorrhage control.

Preparation and Swelling Behaviors of Rapid Responsive Semi-IPN NaCMC/PNIPAm Hydrogels

Semi-interpenetrating network（semi-IPN） hydrogels composed of sodium carboxylmethylcellulose（NaCMC） and poly N-isopropylacrylamide（PNIPAm） were prepared by free radical polymerization of N-isopropyl acrylamide（NIPAm） in dimethylsulfoxide（DMSO） in the presence of NaCMC. The structures of hydrogels were characterized by Fourier transform infrared spectroscopy（FTIR）, scanning electron microscopy（SEM） and differential scanning calorimetry（DSC）. SEM images show that the hydrogels present porous network structures. Most water in the hydrogels were free water and freezing water. The equilibrium swelling ratio（ESR） and swelling rate（SR） were quite different at various swelling temperature. ESR of the hydrogels ranged abruptly from 15.2 g/g to 1.56 g/g and the hydrogels changed from transparent into opaque with swelling temperature changing from 33 ℃ to 34 ℃, that is to say, the hydrogels exhibited the good temperature sensitivity at about 33 ℃ similar to low critical solution temperature（LCST） of pure PNIPAm, swelling rate were very different at below and above LCST due to hydrogel swelling with different swelling mechanism. Moreover, the semi-IPN hydrogels swelled much rapidly than pure PNIPAm hydrogels did at room temperature, the equillibrium swelling ratio（ESR） and swelling rate of the hydrogels increased with increasing of NaCMC content, i e. It is suggested that NaCMC could be potential for preparation of porous and rapid swelling hydrogels

Recent advances on thermosensitive hydrogels-mediated precision therapy

Precision therapy has become the preferred choice attributed to the optimal drug concentration in target sites,increased therapeutic efficacy,and reduced adverse effects.Over the past few years,sprayable or injectable thermosensitive hydrogels have exhibited high therapeutic potential.These can be applied as cell-growing scaffolds or drug-releasing reservoirs by simply mixing in a free-flowing sol phase at room temperature.Inspired by their unique properties,thermosensitive hydrogels have been widely applied as drug delivery and treatment platforms for precision medicine.In this review,the state-of-theart developments in thermosensitive hydrogels for precision therapy are investigated,which covers from the thermo-gelling mechanisms and main components to biomedical applications,including wound healing,anti-tumor activity,osteogenesis,and periodontal,sinonasal and ophthalmic diseases.The most promising applications and trends of thermosensitive hydrogels for precision therapy are also discussed in light of their unique features.

Advances in Biomedical Applications of Hydrogels from Seaweed-Derived Sulfated Polysaccharides:Carrageenan,Fucoidan,and Ulvan

Sulfated polysaccharides extracted from seaweeds,including Carrageenan,Fucoidan and Ulvan,are crucial bioactive compounds known for their diverse beneficial properties,such as anti-inflammatory,antitumor,immunomodulatory,antiviral,and anticoagulant effects.These polysaccharides form hydrogels hold immense promise in biomedicine,particularly in tissue engineering,drug delivery systems and wound healing.This review comprehensively explores the sources and structural characteristics of the three important sulfated polysaccharides extracted from different algae species.It elucidates the gelation mechanisms of these polysaccharides into hydrogels.Furthermore,the biomedical applications of these three sulfated polysaccharide hydrogels in wound healing,drug delivery,and tissue engineering are discussed,highlighting their potential in the biomedicine.

Development of biomedical hydrogels for rheumatoid arthritis treatment

Rheumatoid Arthritis(RA)is an autoimmune disorder that hinders the normal functioning of bones and joints and reduces the quality of human life.Every year,millions of people are diagnosed with RA worldwide,particularly among elderly individuals and women.Therefore,there is a global need to develop new biomaterials,medicines and therapeutic methods for treating RA.This will improve the Healthcare Access and Quality Index and also relieve administrative and financial burdens on healthcare service providers at a global scale.Hydrogels are soft and cross-linked polymeric materials that can store a chunk of fluids,drugs and biomolecules for hydration and therapeutic applications.Hydrogels are biocompatible and exhibit excellent mechanical properties,such as providing elastic cushions to articulating joints by mimicking the natural synovial fluid.Hence,hydrogels create a natural biological environment within the synovial cavity to reduce autoimmune reactions and friction.Hydrogels also lubricate the articulating joint surfaces to prevent degradation of synovial surfaces of bones and cartilage,thus exhibiting high potential for treating RA.This work reviews the progress in injectable and implantable hydrogels,synthesis methods,types of drugs,advantages and challenges.Additionally,it discusses the role of hydrogels in targeted drug delivery,mechanistic behaviour and tribological performance for RA treatment.

Tuning mechanical behaviors of highly entangled hydrogels with the random distribution of mobile entanglements

Highly entangled hydrogels exhibit excellent mechanical properties,including high toughness,high stretchability,and low hysteresis.By considering the evolution of randomly distributed entanglements within the polymer network upon mechanical stretches,we develop a constitutive theory to describe the large stretch behaviors of these hydrogels.In the theory,we utilize a representative volume element(RVE)in the shape of a cube,within which there exists an averaged chain segment along each edge and a mobile entanglement at each corner.By employing an explicit method,we decouple the elasticity of the hydrogels from the sliding motion of their entanglements,and derive the stress-stretch relations for these hydrogels.The present theoretical analysis is in agreement with experiment,and highlights the significant influence of the entanglement distribution within the hydrogels on their elasticity.We also implement the present developed constitutive theory into a commercial finite element software,and the subsequent simulations demonstrate that the exact distribution of entanglements strongly affects the mechanical behaviors of the structures of these hydrogels.Overall,the present theory provides valuable insights into the deformation mechanism of highly entangled hydrogels,and can aid in the design of these hydrogels with enhanced performance.

Light-based 3D printing of stimulus-responsive hydrogels forminiature devices:recent progress and perspective

Miniature devices comprising stimulus-responsive hydrogels with high environmental adaptability are now considered competitive candidates in the fields of biomedicine,precise sensors,and tunable optics.Reliable and advanced fabricationmethods are critical formaximizing the application capabilities ofminiature devices.Light-based three-dimensional(3D)printing technology offers the advantages of a wide range of applicable materials,high processing accuracy,and strong 3D fabrication capability,which is suitable for the development of miniature devices with various functions.This paper summarizes and highlights the recent advances in light-based 3D-printed miniaturized devices,with a focus on the latest breakthroughs in lightbased fabrication technologies,smart stimulus-responsive hydrogels,and tunable miniature devices for the fields of miniature cargo manipulation,targeted drug and cell delivery,active scaffolds,environmental sensing,and optical imaging.Finally,the challenges in the transition of tunable miniaturized devices from the laboratory to practical engineering applications are presented.Future opportunities that will promote the development of tunable microdevices are elaborated,contributing to their improved understanding of these miniature devices and further realizing their practical applications in various fields.

Advanced Nanocomposite Arabic Gum Polyacrylic Acid Hydrogels for Flexible Supercapacitors

In this work,the fabrication and characterization of the nanocomposite hydrogel,as a solid electrode in electro-chemical cell and gel electrolyte material using Indium titanium oxide/polyethylene terephthalate(ITO/PET)flex-ible substrate for double-layer supercapacitors have been reported.The nanocomposite hydrogel composed of Arabic gum(AG),Acrylic acid(AA),reduced graphene oxide(RGO),and silver nanoparticles(AgNPs)was fab-ricated via a physical cross-linked polymerization reaction,in which the ascorbic acid was used as a reducing agent to generate AgNPs and to convert Graphene oxide(GO)to RGO during the polymerization reaction.The morphology and structural characteristics of nanocomposite hydrogel were investigated using atomic force microscopy(AFM),scanning electron microscope(SEM),Fourier transfer infrared(FTIR),and X-rayfluores-cence(XRF).Additionally,the effect of RGO and AgNPs on hydrogel stability was assessed through Thermogra-vimetric analysis(TGA)and differential scanning calorimetry(DSC),while its mechanical properties were studied using the nanoindentation test.Electrochemical impedance spectroscopy(EIS),and cyclic voltammetry(CV)were also conducted to study the electrochemical properties of the prepared hydrogel.The effects of AgNPs,RGO,and water content were all considered in the study of supercapacitor performance.The microstructural tests showed that the nanocomposite hydrogel has a relatively high swelling rate,which has a crucial effect on the capa-citance.Furthermore,the effects of increasing AgNP concentration and water content in the hydrogel matrix showed a significant improvement in its electrochemical performance,compared with that for Arabic gum poly acrylic acid(AGPAA)hydrogel itself,were the specific capacitance exhibited a significant enhancement,convert-ing from a low value to a substantially higher capacitance value.Moreover,when the nanocomposite hydrogel was used as the working electrode in an electrochemical cell with a hydrochloric acid(HCl)electrolyte solution,it exhibited good electrode performance.Additionally,using(ITO/PET)as aflexible substrate for nanocomposite hydrogel shows an improvement in their suitability for supercapacitor applications.Therefore,it is suggested that the fabricated hydrogel supercapacitor has potential applications in thefield of renewable and clean energy harvesting.

Thermosensitive and Wound-Healing Gelatin-Alginate Biopolymer Hydrogels Modified with Humic Acids

The main goal of the article is the creation and study of thermosensitive and wound-healing gelatin-alginate bio-polymer hydrogels modified with humic acids.Their rheological properties,swelling and contraction behavior were experimentally investigated,elucidated using Fourier transform infrared spectroscopy and used to achieve the physiological melting point,which is necessary for successful drug delivery.It has been shown that in the gelatin-alginate-humic acid biopolymer hydrogels systems,it is possible to obtain a gel-sol transition temperature close to the physiological temperature of 37℃,which is important for drug delivery in the treatment of wounds.By changing the type and concentration of humic acids in the gelatin-alginate hydrogel,it turned out to be achiev-able to regulate the softening time of the gel on the human body in the range from 6 to 20 min,which provides the possibility of controlled prolonged delivery of drugs.Based on the study of the influence of calcium ions on the properties of humic acids and ion exchange,as well as the interaction of humic acids,sodium alginate and gelatin with the formation of tighter gel networks,approaches to regulate the rate of softening of hydrogels at physiological temperature and their swelling,which simulates the absorption of exudate,were proposed and implemented.In addition,low shrinkage of the hydrogel surface due to cross-linking of gelatin-alginate networks when modified with humic acids was experimentally confirmed,which is important for avoiding problems of wound contracture and contour deformations when using dressings for wound healing.Thus,the developed opti-mized innovative biopolymer hydrogels synergistically combine the outstanding properties of natural molecular polymers and humic acids and are promising for the creation of effective medicines for wound healing.

Cell Growth and Desorption on the Surface of Temperature-sensitive Semi-IPNs Hydrogels Based on Silk Sericin

Semi-interpenetrating （semi-IPNs） hydrogels containing biocompatible silk sericin （SS） and poly（N-isopropylacrylamide）（PNIPAM） were prepared as novel cellular matrices. Their maximum swelling degree and basic characteristics for biomedical applications such as mouse ？broblasts （L929） cell proliferation and desorption were investigated. The results showed that the incorporation of high hydrophilic SS into PNIPAM hydrogel increased the maximum swelling degree of the semi-IPNs hydrogels, and the adhesion and growth of the L929 on semi-IPNs hydrogels were at least comparable to, or even better than, that on conventional PNIPAM hydrogel. In addition, L929 cells were found to detach from the hydrogels surface naturally by controlling environmental temperature. These results suggest great potential of semi-IPNs hydrogels in tissue engineering.

Biomimetic fibril-like injectable hydrogels for wound management

Soft tissue repair and regeneration present a significant clinical challenge.Soft hydrogels have emerged as a promising solution for promoting stem cell differentiation and facilitating soft tissue formation[1].Various materials,including synthetic polymers like polydimethyl siloxane and natural polymers like proteins,have been be used as hydrogel matrix for hydrogel preparation[2,3].However,the limited biodegradability,inhomogeneous network structure,and inadequate mechanical properties of these hydrogels hinder their long-term application in complex environments in vivo.Inspired by the nanostructure of collagen fibrils,Li et al.developed a strategy for creating injectable nanofibrillar hydrogels by combining self-assembly and chemical crosslinking of nanoparticles[4].Moreover,injectable hydrogels offer advantages as implantable materials,including better defect filling and reduced risk of infection compared to prefabricated hydrogels[5].

A matrix metalloproteinase-responsive hydrogel system controls angiogenic peptide release for repair of cerebral ischemia/reperfusion injury

Vascular endothelial growth factor and its mimic peptide KLTWQELYQLKYKGI(QK)are widely used as the most potent angiogenic factors for the treatment of multiple ischemic diseases.However,conventional topical drug delivery often results in a burst release of the drug,leading to transient retention(inefficacy)and undesirable diffusion(toxicity)in vivo.Therefore,a drug delivery system that responds to changes in the microenvironment of tissue regeneration and controls vascular endothelial growth factor release is crucial to improve the treatment of ischemic stroke.Matrix metalloproteinase-2(MMP-2)is gradually upregulated after cerebral ischemia.Herein,vascular endothelial growth factor mimic peptide QK was self-assembled with MMP-2-cleaved peptide PLGLAG(TIMP)and customizable peptide amphiphilic(PA)molecules to construct nanofiber hydrogel PA-TIMP-QK.PA-TIMP-QK was found to control the delivery of QK by MMP-2 upregulation after cerebral ischemia/reperfusion and had a similar biological activity with vascular endothelial growth factor in vitro.The results indicated that PA-TIMP-QK promoted neuronal survival,restored local blood circulation,reduced blood-brain barrier permeability,and restored motor function.These findings suggest that the self-assembling nanofiber hydrogel PA-TIMP-QK may provide an intelligent drug delivery system that responds to the microenvironment and promotes regeneration and repair after cerebral ischemia/reperfusion injury.

Equilibrium Swelling and Solute Diffusion Characteristics of Poly (Methacrylic Acid co-Poloxamer) Hydrogels

Poly(methacrylic acid co-poloxamer) hydrogel networks were synthesized by free radical solution polymerization and their equilibrium swelling and solute permeation properties were characterized. These gels exhibited pH dependant swelling and solute diffusivity due to the formation or disruption of hydrogen bonded complexation between methacrylic acid (MAA) and etheric (EO). In neutral and basic conditions (above the swelling transition pH), the copolymer swelling was greatly higher than acid condition. In complexed hydrogels, the diffusion coefficients of vitamin B12 (VB12) were in the range of 10-10 to 10-7 cm2s-1; While in uncomplexed hydrogels, the values were about 210-6 cm2s-1. The comonomer composition and synthesis conditions have great effect on the structure, and thereby, swelling and solute diffusion characteristics of the resultant hydrogels. For the copolymers with composition of less than or more than 1:1 MAA/EO molar ratio, the plot of lnD vs 1/H-1 followed two different linear equations of 慺ree volume theory? respectively.

Synthesis and Characterization of Phosphated Konjac Glucomannan Hydrogels

Konjac glucomannan （KGM） was crosslinked with sodium tripolyphosphate （STPP） to synthesize hydrogels. The crosslinking reaction was confirmed by FT-IR. The results of degradation test show that the hydrogels retain the enzymatic degradation character of KGM and can be degraded for 74.45% in 5 days by cellulase E0240.

Tough and tunable adhesion of hydrogels:experiments and models

As polymer networks infiltrated with water, hydrogels are major constituents of animal and plant bodies and have diverse engineering applications. While natural hydrogels can robustly adhere to other biological materials, such as bonding of tendons and cartilage on bones and adhesive plaques of mussels, it is challenging to achieve such tough adhesions between synthetic hydrogels and engineering materials. Recent experiments show that chemically anchoring long-chain polymer networks of tough synthetic hydrogels on solid surfaces create adhesions tougher than their natural counterparts, but the underlying mechanism has not been well understood. It is also challenging to tune systematically the adhesion of hydrogels on solids. Here, we provide a quantitative understanding of the mechanism for tough adhesions of hydrogels on solid materials via a combination of experiments, theory, and numerical simulations. Using a coupled cohesive-zone and Mullins-effect model validated by experiments, we reveal the interplays of intrinsic work of adhesion, interfacial strength, and energy dissipation in bulk hydrogels in order to achieve tough adhesions. We further show that hydrogel adhesion can be systematically tuned by tailoring the hydrogel geometry and silanization time of solid substrates, corresponding to the control of energy dissipation zone and intrinsic work of adhesion, respectively. The current work further provides a theoretical foundation for rational design of future biocompatible and underwater adhesives.

Injectable hydrogels for cartilage and bone tissue engineering

Tissue engineering has become a promising strategy for repairing damaged cartilage and bone tissue. Among the scaffolds for tissue-engineering applications, injectable hydrogels have demonstrated great potential for use as three-dimensional cell culture scaffolds in cartilage and bone tissue engineering, owing to their high water content, similarity to the natural extracellular matrix(ECM), porous framework for cell transplantation and proliferation, minimal invasive properties, and ability to match irregular defects. In this review, we describe the selection of appropriate biomaterials and fabrication methods to prepare novel injectable hydrogels for cartilage and bone tissue engineering. In addition, the biology of cartilage and the bony ECM is also summarized. Finally, future perspectives for injectable hydrogels in cartilage and bone tissue engineering are discussed.