A Generic Strategy to Create Mechanically Interlocked Nanocomposite/Hydrogel Hybrid Electrodes for Epidermal Electronics

Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body.As the primary compliant conductors used in these devices,metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin.Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces.However,chemical modifications are typically needed for reliable bonding,which can alter their original properties.To overcome this limitation,this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes.In this physical process,soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface,which forms an interpenetrating network with the hydrogel.The microfoam-enabled bonding strategy is generally compatible with various polymers.The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids.These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels.They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing mus-cle contractions.Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.

Improving physical properties of poly(vinyl alcohol)/montmorillonite nanocomposite hydrogels via the Hofmeister effect

Hydrogel is a kind of three-dimensional crosslinked polymer material with high moisture content.However,due to the network defects of polymer gels,traditional hydrogels are usually brittle and fragile,which limits their practical applications.Herein,we present a Hofmeister effect-aided facile strategy to prepare high-performance poly(vinyl alcohol)/montmorillonite nanocomposite hydrogels.Layered montmorillonite nanosheets can not only serve as crosslinking agents to enhance the mechanical properties of the hydrogel but also promote the ion conduction.More importantly,based on the Hofmeister effect,the presence of(NH_(4))_(2)SO_(4)can endow nanocomposite hydrogels with excellent mechanical properties by affecting PVA chains'aggregation state and crystallinity.As a result,the as-prepared nanocomposite hydrogels possess unique physical properties,including robust mechanical and electrical properties.The as-prepared hydrogels can be further assembled into a high-performance flexible sensor,which can sensitively detect large-scale and small-scale human activities.The simple design concept of this work is believed to provide a new prospect for developing robust nanocomposite hydrogels and flexible devices in the future.

Layered Potassium Titanium Niobate/Reduced Graphene Oxide Nanocomposite as a Potassium‑Ion Battery Anode

With graphite currently leading as the most viable anode for potassium-ion batteries(KIBs),other materials have been left relatively underexamined.Transition metal oxides are among these,with many positive attributes such as synthetic maturity,longterm cycling stability and fast redox kinetics.Therefore,to address this research deficiency we report herein a layered potassium titanium niobate KTiNbO5(KTNO)and its rGO nanocomposite(KTNO/rGO)synthesised via solvothermal methods as a high-performance anode for KIBs.Through effective distribution across the electrically conductive rGO,the electrochemical performance of the KTNO nanoparticles was enhanced.The potassium storage performance of the KTNO/rGO was demonstrated by its first charge capacity of 128.1 mAh g^(−1) and reversible capacity of 97.5 mAh g^(−1) after 500 cycles at 20 mA g^(−1),retaining 76.1%of the initial capacity,with an exceptional rate performance of 54.2 mAh g^(−1)at 1 A g^(−1).Furthermore,to investigate the attributes of KTNO in-situ XRD was performed,indicating a low-strain material.Ex-situ X-ray photoelectron spectra further investigated the mechanism of charge storage,with the titanium showing greater redox reversibility than the niobium.This work suggests this lowstrain nature is a highly advantageous property and well worth regarding KTNO as a promising anode for future high-performance KIBs.

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.

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.

Bio-inspired Hydroxyapatite/Gelatin Transparent Nanocomposites

Hydroxyapatite(HA)nanoparticles impart outstanding mechanical properties to organicinorganic nanocomposites in bone.Inspired by the composite structure of HA nanoparticles and collagen in bone,a high performance HA/gelatin nanocomposite was first developed.The nanocomposites have much better mechanical properties(elongation at break 29.9%,tensile strength 90.7 MPa,Young’s modulus 5.24 GPa)than pure gelatin films(elongation at break 9.3%,tensile strength 90.8 MPa,Young’s modulus 2.5 GPa).In addition,the composite films keep a high transmittance in visible wavelength range from 0%to 60%of the HA solid content.These differences in properties are attributed to the homogeneous distribution of HA nanoparticles in the gelatin polymer matrix and the strong interaction between the particle surfaces and the gelatin molecules.This protocol should be promising for HA-based nanocomposites with enhanced mechanical properties for biomedical applications.

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.

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.

Predicting the Mechanical Behavior of a Bioinspired Nanocomposite through Machine Learning

The bioinspired nacre or bone structure represents a remarkable example of tough,strong,lightweight,and multifunctional structures in biological materials that can be an inspiration to design bioinspired high-performance materials.The bioinspired structure consists of hard grains and soft material interfaces.While the material interface has a very low volume percentage,its property has the ability to determine the bulk material response.Machine learning technology nowadays is widely used in material science.A machine learning model was utilized to predict the material response based on the material interface properties in a bioinspired nanocomposite.This model was trained on a comprehensive dataset of material response and interface properties,allowing it to make accurate predictions.The results of this study demonstrate the efficiency and high accuracy of the machine learning model.The successful application of machine learning into the material property prediction process has the potential to greatly enhance both the efficiency and accuracy of the material design process.

Assembly of functional carboxymethyl cellulose/polyethylene oxide/anatase TiO_(2) nanocomposites and tuning the dielectric relaxation, optical, and photoluminescence performances

Nanocomposite films consisting of carboxymethyl cellulose,polyethylene oxide(CMC/PEO),and anatase titanium diox-ide(TO)were produced by the use of sol-gel and solution casting techniques.TiO2 nanocrystals were effectively incorporated into CMC/PEO polymers,as shown by X-ray diffraction(XRD)and attenuated total reflectance fourier transform infrared(ATR-FTIR)analysis.The roughness growth is at high levels of TO nanocrystals(TO NCs),which means increasing active sites and defects in CMC/PEO.In differential scanning calorimetry(DSC)thermograms,the change in glass transition temperature(Tg)val-ues verifies that the polymer blend interacts with TO NCs.The increment proportions of TO NCs have a notable impact on the dielectric performances of the nanocomposites,as observed.The electrical properties of the CMC/PEO/TO nanocomposite undergo significant changes.The nanocomposite films exhibit a red alteration in the absorption edge as the concentration of TO NCs increases in the polymer blend.The decline in the energy gap is readily apparent as the weight percentage of TO NCs increases.The photoluminescence(PL)emission spectra indicate that the sites of the luminescence peak maximums show slight variation;peaks get wider,while their intensities decrease dramatically as the concentration of TO increases.These nanocomposite materials show potential for multifunctional applications including optoelectronics,antireflection coatings,pho-tocatalysis,light emitting diodes,and solid polymer electrolytes.

Phase field model for electric-thermal coupled discharge breakdown of polyimide nanocomposites under high frequency electrical stress

In contrast to conventional transformers, power electronic transformers, as an integral component of new energy power system, are often subjected to high-frequency and transient electrical stresses, leading to heightened concerns regarding insulation failures. Meanwhile, the underlying mechanism behind discharge breakdown failure and nanofiller enhancement under high-frequency electrical stress remains unclear. An electric-thermal coupled discharge breakdown phase field model was constructed to study the evolution of the breakdown path in polyimide nanocomposite insulation subjected to high-frequency stress. The investigation focused on analyzing the effect of various factors, including frequency, temperature, and nanofiller shape, on the breakdown path of Polyimide(PI) composites. Additionally, it elucidated the enhancement mechanism of nano-modified composite insulation at the mesoscopic scale. The results indicated that with increasing frequency and temperature, the discharge breakdown path demonstrates accelerated development, accompanied by a gradual dominance of Joule heat energy. This enhancement is attributed to the dispersed electric field distribution and the hindering effect of the nanosheets. The research findings offer a theoretical foundation and methodological framework to inform the optimal design and performance management of new insulating materials utilized in high-frequency power equipment.

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].

Nanocomposite Polymer Hydrogels Reinforced by Carbon Dots and Hectorite Clay

Herein, two nanoparticles with different dimensions, spherical carbon dots (C-dots) and sheetlike hectorite clay, were used as physical crosslinkers to fabricate C-dots-clay-poly(N-isopropylacrylamide)nanocompositehydrogels (coded as C-dots-clay-PNIPAm hydrogels). The mechanical properties, fluorescence features and thermal-responsive properties of the C-dots-clay-PNIPAm hydrogels were evaluated. The experimental results indicate that synergistic effects of C-dots and hectorite clay nanoparticles are able to significantly enhance mechanical properties of the hydrogels. The hydrogels can be stretched up to 1730%with strength as high as 250 kPa when the C-dots concentration is 0.1wt%and the clay concentration is 6wt%. The hydrogels exhibit complete self-healing through autonomic reconstruction of crosslinked network a damaged interface. The hydrogels show favorable thermal-responsive properties with the volume phase transition around 34℃. In addition, the hydrogels are endowed with fluorescence features that are associated with C-dots in the hydrogels. It can be expected that the as-fabricated C-dots-clay-PNIPAm hydrogels are promising for applications in sensors, biomedical carriers and tissue engineering.

On mechanical properties of nanocomposite hydrogels:Searching for superior properties

Nanocomposite hydrogels are the combination of known components that are a hydrogel and nanometre-sized fillers,typically leading to improved mechanical properties or new functionalities.With simplicity of design and ease of synthesis,recent advances have highlighted that this family of hydrogels holds the significant promise of application in diverse biomedical and engineering fields.The elaborate design and investigation as well as suitable application of nanocomposite hydrogels require the synergy of mechanics,materials science,engineering,and biology.Despite similarities in design and fabrication,the data of mechanical properties for nanocomposite hydrogels scatter in a large space.It is worthwhile comparing various nanocomposite hydrogels for similarities and differences in mechanical properties to aid in designing novel hydrogels with extreme properties,and guide practical applications.This review aims to fill,in the literature,the missing gap of addressing mechanical measurement methods and comparison of mechanical properties in this ever-evolving broad area of research.Finally,the challenges and future research opportunities are highlighted.

Thermal-responsive Photonic Crystals based on Physically Cross-linked Inverse Opal Nanocomposite Hydrogels

A thermal-responsive photonic crystal material was fabricated by forming an inverse opal nanocomposite hydrogel of poly(N-isopropylacrylamide)(IONHPNIPAm)within the interstitial space of a polystyrene photonic crystal template.In IONHPNIPAm,PNIPAm were physically cross-linked with two kinds of nanoparticles(carbon dots and laponite clays).The integration of carbon dots and laponite clays for physical crosslinking endowed IONHPNIPAm sufficient strength and self-healing property.IONHPNIPAm films can be completely peeled from the substrates to be utilized as an independent photonic crystal material.The structural color and optical diffraction of the IONHPNIPAm exhibits a rapid reversible change in response to external thermal stimuli due to its physical cross-linking feature.Moreover,the IONHPNIPAm shows clear fluorescence due to the introduction of carbon dots,which enables a convenient way for chemical detection(such as the detection of silver ions).This stimuli-responsive photonic crystal materials based on physically cross-linked inverse opal nanocomposite hydrogels with fast response and good mechanical stability are promising for applications in the fields of smart optical detectors,thermal-responsive sensors and chemical detectors.

Fabrication and Characterization of Chitosan Based Injectable Thermosensitive Hydrogels Containing Silica/Calcium Phosphate Nanocomposite Particles

In this study, the effect of silica/calcium phosphate (SiCaP) nanocomposite particles on the properties of a novel chitosan-based thermosensitive hydrogel system was examined. SiCaP nanocomposite powder was fabricated using a sol-gel method and then used to fabricate nanocomposite hydrogels (Ch- β/7.5SiCaP and Ch-β/15SiCaP) including chitosan and β-glycerophosphate (Ch-β) as a matrix. Results revealed that compared to the Ch-β hydrogel without SiCaP, the presence of SiCaP particles in nanocomposite hydrogels maintained pH stability during the sol-gel transition, accelerated the gelation and improved the stiffness of nanocomposite hydrogels. Gelation time at 37℃ was reduced approximately 75% and stiffness was increased approximately 115%. Both of these changes are attributed to chemical and physical interactions of the SiCaP bioactive particles with chitosan. Furthermore, compared to the Ch-β hydrogel, the presence of SiCaP in the Ch-β/7.5SiCaP nanocomposite hydrogel did not affect biocompatibility negatively, but improved osteoblastic cell differentiation. Our studies suggest that these nanocomposite hydrogels may offer an innovative approach to bone regeneration strategies.

Preparation and Characterization of Eco-friendly Carboxymethyl Cellulose Antimicrobial Nanocomposite Hydrogels

Carboxymethyl cellulose hydrogels were developed through crosslinking process using eco-friendly crosslinkers such as maleic,succinic,and citric acids.Carboxymethyl cellulose was prepared from the cellulosic fraction of olive industry residues.A series of hydrogels with varying crosslinker acid concentrations,reaction times,and reaction temperatures was produced to study the swelling capacities and gel fraction of the obtained hydrogels.Additional study pertains to the preparation of antimicrobial nanocomposite hydrogels through in-situ incorporation of the silver nanoparticles during the crosslinking reaction.Silver nanoparticles were prepared by reduction of AgNO3 with leaves of Ricinus communis.The particle size of prepared silver nanoparticles was detected by transmission electron microscopy(TEM).Chemical structure and morphological characterizations of the prepared hydrogels were performed using Fourier transform infrared spectroscopy(FTIR),scanning electron microscopy(SEM),and energy-dispersive X-ray spectroscopy(EDX).Finally,the antimicrobial activity of the loaded silver hydrogels against Gram negative(G-ve),Gram positive(G+ve),and Candida albicans yeast was demonstrated.

Formation and Collapse of Cellulose Nanocrystals and Hydrophobic Association-induced Dual Cross-linked Nanocomposite Hydrogels: A Rheological Study

The rheological characteristics of a physical gelation system,in which cellulose nanocrystals(CNC_(s))induced the entanglement of poly(acrylic acid)(PAA)chains and partial hydrophobic association of octylphenol polyoxyethylene acrylate(OP-10-AC)branches in a micellar solution of sodium dodecyl sulfate(SDS),were investigated.The gelation time of the physical gels decreased as the CNC content and number of hydrophobic branch units increased.At the gel point,the storage modulus(G')and loss modulus(G")followed the same frequency dependence(G'≈G"≈ωn),where the hydrophobic moieties attached to the side chains had a significant impact on the values of viscoelastic exponent(n).Beyond the gel point,the initial polymer solution was transformed to a solid-like gel,and the strength of the gel network was governed by associations between both the CNCs and hydrophobic groups.The evolution of the viscoelasticity during the gel-sol transition was monitored,demonstrating that due to a reversible arrangement of the hydrophobic units,a large proportion of physical cross-links dissociated under a thermal trigger and were reversibly reformed when the solution was cooled,while no such partial recovery was observed in the case of the single CNC-induced network systems(with no hydrophobic branches).