Due to the low content of adsorption-active groups in lignin,its application in the field of adsorption is limited.Herein,we first prepared cationic kraft lignin acrylate,from which a cationic lignin(CKLA)hydrogel was...Due to the low content of adsorption-active groups in lignin,its application in the field of adsorption is limited.Herein,we first prepared cationic kraft lignin acrylate,from which a cationic lignin(CKLA)hydrogel was further prepared by cationic kraft lignin acrylate,acrylamide,and N,N’-methylenebisacrylamide.The morphology,compression properties and swelling properties of CKLA hydrogels were investigated.The prepared CKLA hydrogel was applied as an adsorbent for Congo red.The effect of CKLA hydrogel dosages,initial concentration of Congo red,and pH on adsorption efficiency was investigated.The maximum Congo red removal efficiency was obtained at the initial concentration of Congo red of 50 mg/L,pH 7,and 5 mg dosage of CKLA hydrogel with 20%cationic lignin content.After five cycles of adsorption,the adsorption efficiency of the hydrogel for Congo red still reached more than 80%.The CKLA hydrogel showed pseudo-second-order adsorption kinetics for Congo red adsorption.These results demonstrate the potential of the CKLA hydrogel as an adsorbent for water treatment.展开更多
Hydrogels are biomaterials with 3D networks of hydrophilic polymers.The generation of hydrogels is turning to the development of hydrogels with the help of enabling technologies.Plasma can tailor the hydrogels’proper...Hydrogels are biomaterials with 3D networks of hydrophilic polymers.The generation of hydrogels is turning to the development of hydrogels with the help of enabling technologies.Plasma can tailor the hydrogels’properties through simultaneous physical and chemical actions,resulting in an emerging technology of plasma-activated hydrogels(PAH).PAH can be divided into functional PAH and biological tissue model PAH.This review systematically introduces the plasma sources,plasma etching polymer surface,and plasma cross-linking involved in the fabrication of PAH.The‘diffusion-drift-reaction model’is used to study the microscopic physicochemical interaction between plasma and biological tissue PAH models.Finally,the main achievements of PAH,including wound treatment,sterilization,3D tumor model,etc,and their development trends are discussed.展开更多
Bone is a complex but orderly mineralized tissue with hydroxyapatite(HA)as the inorganic phase and collagen as the organic phase.Inspired by natural bone tissues,HA-mineralized hydrogels have been widely designed and ...Bone is a complex but orderly mineralized tissue with hydroxyapatite(HA)as the inorganic phase and collagen as the organic phase.Inspired by natural bone tissues,HA-mineralized hydrogels have been widely designed and used in bone tissue engineering.HA is majorly utilized for the treatment of bone defects because of its excellent osteoconduction and bone inductivity.Hydrogel is a three-dimensional hydrophilic network structure with similar properties to the extracellular matrix(ECM).The combination of HA and hydrogels produces a new hybrid material that could effectively promote osteointegration and accelerate the healing of bone defects.In this review,the structure and growth of bone and the common strategies used to prepare HA were briefly introduced.Importantly,we discussed the fabrication of HA mineralized hydrogels from simple blending to in situ mineralization.We hope this review can provide a reference for the development of bone repair hydrogels.展开更多
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,wh...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.展开更多
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 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.展开更多
The integrated repair of bone and cartilage boasts advantages for osteochondral restoration such as a long-term repair effect and less deterioration compared to repairing cartilage alone.Constructing multifactorial,sp...The integrated repair of bone and cartilage boasts advantages for osteochondral restoration such as a long-term repair effect and less deterioration compared to repairing cartilage alone.Constructing multifactorial,spatially oriented scaffolds to stimulate osteochondral regeneration,has immense significance.Herein,targeted drugs,namely kartogenin@polydopamine(KGN@PDA)nanoparticles for cartilage repair and miRNA@calcium phosphate(miRNA@CaP)NPs for bone regeneration,were in situ deposited on a patterned supramolecular-assembled 2-ureido-4[lH]-pyrimidinone(UPy)modified gelation hydrogel film,facilitated by the dynamic and responsive coordination and complexation of metal ions and their ligands.This hydrogel film can be rolled into a cylindrical plug,mimicking the Haversian canal structure of natural bone.The resultant hydrogel demonstrates stable mechanical properties,a self-healing ability,a high capability for reactive oxygen species capture,and controlled release of KGN and miR-26a.In vitro,KGN@PDA and miRNA@CaP promote chondrogenic and osteogenic differentiation of mesenchymal stem cells via the JNK/RUNX1 and GSK-3β/β-catenin pathways,respectively.In vivo,the osteochondral plug exhibits optimal subchondral bone and cartilage regeneration,evidenced by a significant increase in glycosaminoglycan and collagen accumulation in specific zones,along with the successful integration of neocartilage with subchondral bone.This biomaterial delivery approach represents a significant toward improved osteochondral repair.展开更多
A combination of hydrogels and microfluidics allows the construction of biomimetic three-dimensional(3D)tissue models in vitro,which are also known as organ-on-a-chipmodels.The hydrogel patterningwith awell-controlled...A combination of hydrogels and microfluidics allows the construction of biomimetic three-dimensional(3D)tissue models in vitro,which are also known as organ-on-a-chipmodels.The hydrogel patterningwith awell-controlled spatial distribution is typically achieved by embedding sophisticated microstructures to act as a boundary.However,these physical barriers inevitably expose cells/tissues to a less physiologically relevant microenvironment than in vivo conditions.Herein,we present a novel dissolvable temporary barrier(DTB)strategy that allows robust and flexible hydrogel patterning with great freedom of design and desirable flow stimuli for cellular hydrogels.The key aspect of this approach is the patterning of a water-soluble rigid barrier as a guiding path for the hydrogel using stencil printing technology,followed by a barrier-free medium perfusion after the dissolution of the DTB.Single and multiple tissue compartments with different geometries can be established using either straight or curved DTB structures.The effectiveness of this strategy is further validated by generating a 3D vascular network through vasculogenesis and angiogenesis using a vascularized microtumor model.As a new proof-of-concept in vasculature-on-a-chip,DTB enables seamless contact between the hydrogel and the culture medium in closed microdevices,which is an improved protocol for the fabrication ofmultiorgan chips.Therefore,we expect it to serve as a promising paradigm for organ-on-a-chip devices for the development of tumor vascularization and drug evaluation in the future preclinical studies.展开更多
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 composite...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.展开更多
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 ...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.展开更多
The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sens...The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sensing actuated gradient hydrogel that combines ultrafast actuation and high sensitivity for remote interaction with robotic hand. The gradient network structure, achieved through a wettability difference method involving the rapid precipitation of MoO_(2) nanosheets, introduces hydrophilic disparities between two sides within hydrogel. This distinctive approach bestows the hydrogel with ultrafast thermo-responsive actuation(21° s^(-1)) and enhanced photothermal efficiency(increase by 3.7 ℃ s^(-1) under 808 nm near-infrared). Moreover, the local cross-linking of sodium alginate with Ca^(2+) endows the hydrogel with programmable deformability and information display capabilities. Additionally, the hydrogel exhibits high sensitivity(gauge factor 3.94 within a wide strain range of 600%), fast response times(140 ms) and good cycling stability. Leveraging these exceptional properties, we incorporate the hydrogel into various soft actuators, including soft gripper, artificial iris, and bioinspired jellyfish, as well as wearable electronics capable of precise human motion and physiological signal detection. Furthermore, through the synergistic combination of remarkable actuation and sensitivity, we realize a self-sensing touch bioinspired tongue. Notably, by employing quantitative analysis of actuation-sensing, we realize remote interaction between soft-hard robot via the Internet of Things. The multifunctional self-sensing actuated gradient hydrogel presented in this study provides a new insight for advanced somatosensory materials, self-feedback intelligent soft robots and human–machine interactions.展开更多
High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use i...High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.展开更多
Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appea...Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness,high conductivity and intrinsic flexibility.However,the electrolyte/electrode interfacial contact and anti-freezing properties of current hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors.Here,we report a class of hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance.The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode.Meanwhile,the cooperative solvation of ZnCl2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures.More significantly,the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance,delivering high-energy density of 39 Wh kg^(-1)at-60°C with capacity retention of 98.7%over 10,000 cycles.With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte,the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at-60°C.This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.展开更多
The anti-freezing strategy of hydrogels and their self-healing structure are often contradictory,it is vital to break through the molecular structure to design and construct hydrogels with intrinsic anti-freezing/self...The anti-freezing strategy of hydrogels and their self-healing structure are often contradictory,it is vital to break through the molecular structure to design and construct hydrogels with intrinsic anti-freezing/self-healing for meeting the rapid development of flexible and wearable devices in diverse service conditions.Herein,we design a new hydrogel electrolyte(AF/SH-Hydrogel)with intrinsic anti-freezing/self-healing capabilities by introducing ethylene glycol molecules,dynamic chemical bonding(disulfide bond),and supramolecular interaction(multi-hydrogen bond)into the polyacrylamide molecular chain.Thanks to the exceptional freeze resistance(84%capacity retention at-20℃)and intrinsic self-healing capabilities(95%capacity retention after 5 cutting/self-healing cycles),the obtained AF/SH-Hydrogel makes the zinc||manganese dioxide cell an economically feasible battery for the state-of-the-art applications.The Zn||AF/SH-Hydrogel||MnO_(2)device offers a near-theoretical specific capacity of 285 m A h g^(-1)at 0.1 A g^(-1)(Coulombic efficiency≈100%),as well as good self-healing capability and mechanical flexibility in an ice bath.This work provides insight that can be utilized to develop multifunctional hydrogel electrolytes for application in next generation of self-healable and freeze-resistance smart aqueous energy storage devices.展开更多
Aqueous rechargeable Zn-metal batteries(ARZBs)are considered one of the most promising candidates for grid-scale energy storage.However,their widespread commercial application is largely plagued by three major challen...Aqueous rechargeable Zn-metal batteries(ARZBs)are considered one of the most promising candidates for grid-scale energy storage.However,their widespread commercial application is largely plagued by three major challenges:The uncontrollable Zn dendrites,notorious parasitic side reactions,and sluggish Zn^(2+) ion transfer.To address these issues,we design a sustainable dual crosslinked cellulose hydrogel electrolyte,which has excellent mechanical strength to inhibit dendrite formation,high Zn^(2+) ions binding capacity to suppress side reaction,and abundant porous structure to facilitate Zn^(2+) ions migration.Consequently,the Zn||Zn cell with the hydrogel electrolyte can cycle stably for more than 400 h under a high current density of 10 mA cm^(−2).Moreover,the hydrogel electrolyte also enables the Zn||polyaniline cell to achieve high-rate and long-term cycling performance(>2000 cycles at 2000 mA g^(−1)).Remarkably,the hydrogel electrolyte is easily accessible and biodegradable,making the ARZBs attractive in terms of scalability and sustainability.展开更多
Neurotrophic keratopathy is a persistent defect of the corneal epithelium,with or without stromal ulceration,due to corneal nerve deficiency caused by a variety of etiologies.The treatment options for neurotrophic ker...Neurotrophic keratopathy is a persistent defect of the corneal epithelium,with or without stromal ulceration,due to corneal nerve deficiency caused by a variety of etiologies.The treatment options for neurotrophic keratopathy are limited.In this study,an ophthalmic solution was constructed from a chitosan-based thermosensitive hydrogel with long-term release of murine nerve growth factor(CTH-mNGF).Its effectiveness was evaluated in corneal denervation(CD)mice and patients with neurotrophic keratopathy.In the preclinical setting,CTH-mNGF was assessed in a murine corneal denervation model.CTH-mNGF was transparent,thermosensitive,and ensured sustained release of mNGF for over 20 hours on the ocular surface,maintaining the local mNGF concentration around 1300 pg/mL in vivo.Corneal denervation mice treated with CTH-mNGF for 10 days showed a significant increase in corneal nerve area and total corneal nerve length compared with non-treated and CTH treated mice.A subsequent clinical trial of CTH-mNGF was conducted in patients with stage 2 or 3 neurotrophic keratopathy.Patients received topical CTH-mNGF twice daily for 8 weeks.Fluorescein sodium images,Schirmer’s test,intraocular pressure,Cochet-Bonnet corneal perception test,and best corrected visual acuity were evaluated.In total,six patients(total of seven eyes)diagnosed with neurotrophic keratopathy were enrolled.After 8 weeks of CTH-mNGF treatment,all participants showed a decreased area of corneal epithelial defect,as stained by fluorescence.Overall,six out of seven eyes had fluorescence staining scores<5.Moreover,best corrected visual acuity,intraocular pressure,Schirmer’s test and Cochet-Bonnet corneal perception test results showed no significant improvement.An increase in corneal nerve density was observed by in vivo confocal microscopy after 8 weeks of CTH-mNGF treatment in three out of seven eyes.This study demonstrates that CTH-mNGF is transparent,thermosensitive,and has sustained-release properties.Its effectiveness in healing corneal epithelial defects in all eyes with neurotrophic keratopathy suggests CTH-mNGF has promising application prospects in the treatment of neurotrophic keratopathy,being convenient and cost effective.展开更多
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 ...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.展开更多
With the exponential development in wearable electronics,a significant paradigm shift is observed from rigid electronics to flexible wearable devices.Polyaniline(PANI)is considered as a dominant material in this secto...With the exponential development in wearable electronics,a significant paradigm shift is observed from rigid electronics to flexible wearable devices.Polyaniline(PANI)is considered as a dominant material in this sector,as it is endowed with the optical properties of both metal and semiconductors.However,its widespread application got delineated because of its irregular rigid form,level of conductivity,and precise choice of solvents.Incorporating PANI in textile materials can generate promising functionality for wearable applications.This research work employed a straightforward in-situ chemical oxidative polymerization to synthesize PANI on Cotton fabric surfaces with varying dopant(HCl)concentrations.Pre-treatment using NaOH is implemented to improve the conductivity of the fabric surface by increasing the monomer absorption.This research explores the morphological and structural analysis employing SEM,FTIR and EDX.The surface resistivity was measured using a digital multimeter,and thermal stability is measured using TGA.Upon successful polymerization,a homogenous coating layer is observed.It is revealed that the simple pre-treatment technique significantly reduces the surface resistivity of Cotton fabric to 1.27 kΩ/cm with increasing acid concentration and thermal stability.The electro-thermal energy can also reach up to 38.2°C within 50 s with a deployed voltage of 15 V.The modified fabric is anticipated to be used in thermal regulation,supercapacitor,sensor,UV shielding,antimicrobial and other prospective functional applications.展开更多
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].Variou...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].展开更多
基金supported by Fundamental Research Funds of CAF(CAFYBB2020MB002).
文摘Due to the low content of adsorption-active groups in lignin,its application in the field of adsorption is limited.Herein,we first prepared cationic kraft lignin acrylate,from which a cationic lignin(CKLA)hydrogel was further prepared by cationic kraft lignin acrylate,acrylamide,and N,N’-methylenebisacrylamide.The morphology,compression properties and swelling properties of CKLA hydrogels were investigated.The prepared CKLA hydrogel was applied as an adsorbent for Congo red.The effect of CKLA hydrogel dosages,initial concentration of Congo red,and pH on adsorption efficiency was investigated.The maximum Congo red removal efficiency was obtained at the initial concentration of Congo red of 50 mg/L,pH 7,and 5 mg dosage of CKLA hydrogel with 20%cationic lignin content.After five cycles of adsorption,the adsorption efficiency of the hydrogel for Congo red still reached more than 80%.The CKLA hydrogel showed pseudo-second-order adsorption kinetics for Congo red adsorption.These results demonstrate the potential of the CKLA hydrogel as an adsorbent for water treatment.
基金supported by National Natural Science Foundation of China(No.52277149)the Interdisciplinary Program of Wuhan National High Magnetic Field Center(No.WHMFC202144)Huazhong University of Science and Technology.
文摘Hydrogels are biomaterials with 3D networks of hydrophilic polymers.The generation of hydrogels is turning to the development of hydrogels with the help of enabling technologies.Plasma can tailor the hydrogels’properties through simultaneous physical and chemical actions,resulting in an emerging technology of plasma-activated hydrogels(PAH).PAH can be divided into functional PAH and biological tissue model PAH.This review systematically introduces the plasma sources,plasma etching polymer surface,and plasma cross-linking involved in the fabrication of PAH.The‘diffusion-drift-reaction model’is used to study the microscopic physicochemical interaction between plasma and biological tissue PAH models.Finally,the main achievements of PAH,including wound treatment,sterilization,3D tumor model,etc,and their development trends are discussed.
基金supported by the National Natural Science Foundation of China(Grant no:12272253)Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(Grant no:2021SX-AT008,2021SX-AT009).
文摘Bone is a complex but orderly mineralized tissue with hydroxyapatite(HA)as the inorganic phase and collagen as the organic phase.Inspired by natural bone tissues,HA-mineralized hydrogels have been widely designed and used in bone tissue engineering.HA is majorly utilized for the treatment of bone defects because of its excellent osteoconduction and bone inductivity.Hydrogel is a three-dimensional hydrophilic network structure with similar properties to the extracellular matrix(ECM).The combination of HA and hydrogels produces a new hybrid material that could effectively promote osteointegration and accelerate the healing of bone defects.In this review,the structure and growth of bone and the common strategies used to prepare HA were briefly introduced.Importantly,we discussed the fabrication of HA mineralized hydrogels from simple blending to in situ mineralization.We hope this review can provide a reference for the development of bone repair hydrogels.
基金Funded by the National Natural Science Foundation of China(No.51873167)the National Innovation and Entrepreneurship Training Program for College Students(No.226801001)。
文摘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.
基金supported by the grants from National Research Foundation(NRF,#2021R1A5A2022318,#RS-2023-00220408,#RS-2023-00247485),Republic of Korea.
文摘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.
基金the Natural Science Foundation of China(Grant Nos.82072413,82101649)National Key Research and Development Program of China(Grant Nos.2021YFE0105400).
文摘The integrated repair of bone and cartilage boasts advantages for osteochondral restoration such as a long-term repair effect and less deterioration compared to repairing cartilage alone.Constructing multifactorial,spatially oriented scaffolds to stimulate osteochondral regeneration,has immense significance.Herein,targeted drugs,namely kartogenin@polydopamine(KGN@PDA)nanoparticles for cartilage repair and miRNA@calcium phosphate(miRNA@CaP)NPs for bone regeneration,were in situ deposited on a patterned supramolecular-assembled 2-ureido-4[lH]-pyrimidinone(UPy)modified gelation hydrogel film,facilitated by the dynamic and responsive coordination and complexation of metal ions and their ligands.This hydrogel film can be rolled into a cylindrical plug,mimicking the Haversian canal structure of natural bone.The resultant hydrogel demonstrates stable mechanical properties,a self-healing ability,a high capability for reactive oxygen species capture,and controlled release of KGN and miR-26a.In vitro,KGN@PDA and miRNA@CaP promote chondrogenic and osteogenic differentiation of mesenchymal stem cells via the JNK/RUNX1 and GSK-3β/β-catenin pathways,respectively.In vivo,the osteochondral plug exhibits optimal subchondral bone and cartilage regeneration,evidenced by a significant increase in glycosaminoglycan and collagen accumulation in specific zones,along with the successful integration of neocartilage with subchondral bone.This biomaterial delivery approach represents a significant toward improved osteochondral repair.
基金supported by the National Natural Science Foundation of China(Nos.31972929 and 62231025)the Research Program of Shanghai Science and Technology Committee(Nos.21140901300 and 20DZ2220400)+3 种基金the Natural Science Foundation of Chongqing,China(No.CSTB2022NSCQ-MSX0767)the Interdisciplinary Program of Shanghai Jiao Tong University(Nos.YG2021ZD22 and YG2023LC04)the Foundation of National Center for Translational Medicine(Shanghai)SHU Branch(No.SUITM-2023008)the Cross-disciplinary Research Fund of Shanghai Ninth People’s Hospital,Shanghai Jiao Tong University School of Medicine(No.JYJC202108).
文摘A combination of hydrogels and microfluidics allows the construction of biomimetic three-dimensional(3D)tissue models in vitro,which are also known as organ-on-a-chipmodels.The hydrogel patterningwith awell-controlled spatial distribution is typically achieved by embedding sophisticated microstructures to act as a boundary.However,these physical barriers inevitably expose cells/tissues to a less physiologically relevant microenvironment than in vivo conditions.Herein,we present a novel dissolvable temporary barrier(DTB)strategy that allows robust and flexible hydrogel patterning with great freedom of design and desirable flow stimuli for cellular hydrogels.The key aspect of this approach is the patterning of a water-soluble rigid barrier as a guiding path for the hydrogel using stencil printing technology,followed by a barrier-free medium perfusion after the dissolution of the DTB.Single and multiple tissue compartments with different geometries can be established using either straight or curved DTB structures.The effectiveness of this strategy is further validated by generating a 3D vascular network through vasculogenesis and angiogenesis using a vascularized microtumor model.As a new proof-of-concept in vasculature-on-a-chip,DTB enables seamless contact between the hydrogel and the culture medium in closed microdevices,which is an improved protocol for the fabrication ofmultiorgan chips.Therefore,we expect it to serve as a promising paradigm for organ-on-a-chip devices for the development of tumor vascularization and drug evaluation in the future preclinical studies.
基金We acknowledge the support from the National Key Research and Development Program of China(Grant No.2022YFA1405000)the Natural Science Foundation of Jiangsu Province,Major Project(Grant No.BK20212004)+1 种基金the National Natural Science Foundation of China(Grant No.62374083)the State Key Laboratory of Analytical Chemistry for Life Science(Grant No.5431ZZXM2205).
文摘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.
基金Project supported by the Key Research Project of Zhejiang Laboratory (No.K2022NB0AC03)the National Natural Science Foundation of China (No.11872334)the National Natural Science Foundation of Zhejiang Province of China (No.LZ23A020004)。
文摘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.
基金The financial support from the National Natural Science Foundation of China (32201179)Guangdong Basic and Applied Basic Research Foundation (2020A1515110126 and 2021A1515010130)+1 种基金the Fundamental Research Funds for the Central Universities (N2319005)Ningbo Science and Technology Major Project (2021Z027) is gratefully acknowledged。
文摘The development of bioinspired gradient hydrogels with self-sensing actuated capabilities for remote interaction with soft-hard robots remains a challenging endeavor. Here, we propose a novel multifunctional self-sensing actuated gradient hydrogel that combines ultrafast actuation and high sensitivity for remote interaction with robotic hand. The gradient network structure, achieved through a wettability difference method involving the rapid precipitation of MoO_(2) nanosheets, introduces hydrophilic disparities between two sides within hydrogel. This distinctive approach bestows the hydrogel with ultrafast thermo-responsive actuation(21° s^(-1)) and enhanced photothermal efficiency(increase by 3.7 ℃ s^(-1) under 808 nm near-infrared). Moreover, the local cross-linking of sodium alginate with Ca^(2+) endows the hydrogel with programmable deformability and information display capabilities. Additionally, the hydrogel exhibits high sensitivity(gauge factor 3.94 within a wide strain range of 600%), fast response times(140 ms) and good cycling stability. Leveraging these exceptional properties, we incorporate the hydrogel into various soft actuators, including soft gripper, artificial iris, and bioinspired jellyfish, as well as wearable electronics capable of precise human motion and physiological signal detection. Furthermore, through the synergistic combination of remarkable actuation and sensitivity, we realize a self-sensing touch bioinspired tongue. Notably, by employing quantitative analysis of actuation-sensing, we realize remote interaction between soft-hard robot via the Internet of Things. The multifunctional self-sensing actuated gradient hydrogel presented in this study provides a new insight for advanced somatosensory materials, self-feedback intelligent soft robots and human–machine interactions.
基金the National Natural Science Foundation of China(11875138,52077095).
文摘High-performance ion-conducting hydrogels(ICHs)are vital for developing flexible electronic devices.However,the robustness and ion-conducting behavior of ICHs deteriorate at extreme tempera-tures,hampering their use in soft electronics.To resolve these issues,a method involving freeze–thawing and ionizing radiation technology is reported herein for synthesizing a novel double-network(DN)ICH based on a poly(ionic liquid)/MXene/poly(vinyl alcohol)(PMP DN ICH)system.The well-designed ICH exhibits outstanding ionic conductivity(63.89 mS cm^(-1) at 25℃),excellent temperature resistance(-60–80℃),prolonged stability(30 d at ambient temperature),high oxidation resist-ance,remarkable antibacterial activity,decent mechanical performance,and adhesion.Additionally,the ICH performs effectively in a flexible wireless strain sensor,thermal sensor,all-solid-state supercapacitor,and single-electrode triboelectric nanogenerator,thereby highlighting its viability in constructing soft electronic devices.The highly integrated gel structure endows these flexible electronic devices with stable,reliable signal output performance.In particular,the all-solid-state supercapacitor containing the PMP DN ICH electrolyte exhibits a high areal specific capacitance of 253.38 mF cm^(-2)(current density,1 mA cm^(-2))and excellent environmental adaptability.This study paves the way for the design and fabrication of high-performance mul-tifunctional/flexible ICHs for wearable sensing,energy-storage,and energy-harvesting applications.
基金This work was supported by the Natural Science Foundation of Jiangsu Province(BK20220213)the Fundamental Research Funds of Jiangsu Key Laboratory of Biomass Energy and Material(JSBEM-S-202210 and JSBEM-S-202102).
文摘Solid-state zinc-ion capacitors are emerging as promising candidates for large-scale energy storage owing to improved safety,mechanical and thermal stability and easy-to-direct stacking.Hydrogel electrolytes are appealing solid-state electrolytes because of eco-friendliness,high conductivity and intrinsic flexibility.However,the electrolyte/electrode interfacial contact and anti-freezing properties of current hydrogel electrolytes are still challenging for practical applications of zinc-ion capacitors.Here,we report a class of hydrogel electrolytes that couple high interfacial adhesion and anti-freezing performance.The synergy of tough hydrogel matrix and chemical anchorage enables a well-adhered interface between hydrogel electrolyte and electrode.Meanwhile,the cooperative solvation of ZnCl2 and LiCl hybrid salts renders the hydrogel electrolyte high ionic conductivity and mechanical elasticity simultaneously at low temperatures.More significantly,the Zn||carbon nanotubes hybrid capacitor based on this hydrogel electrolyte exhibits low-temperature capacitive performance,delivering high-energy density of 39 Wh kg^(-1)at-60°C with capacity retention of 98.7%over 10,000 cycles.With the benefits of the well-adhered electrolyte/electrode interface and the anti-freezing hydrogel electrolyte,the Zn/Li hybrid capacitor is able to accommodate dynamic deformations and function well under 1000 tension cycles even at-60°C.This work provides a powerful strategy for enabling stable operation of low-temperature zinc-ion capacitors.
基金supported by the link project of the National Natural Science Foundation of China(52002052 and 22209020)the Key Research and Development Project of Science and Technology Department of Sichuan Province(2022YFSY0004)+2 种基金the Opening project of the State Key Laboratory of New Textile Materials and Advanced Processing Technology(FZ2021009)the Natural Science Foundation of Sichuan Province(2023NSFSC0995)the Natural Science Foundation of Hunan Province(2022JJ30227)。
文摘The anti-freezing strategy of hydrogels and their self-healing structure are often contradictory,it is vital to break through the molecular structure to design and construct hydrogels with intrinsic anti-freezing/self-healing for meeting the rapid development of flexible and wearable devices in diverse service conditions.Herein,we design a new hydrogel electrolyte(AF/SH-Hydrogel)with intrinsic anti-freezing/self-healing capabilities by introducing ethylene glycol molecules,dynamic chemical bonding(disulfide bond),and supramolecular interaction(multi-hydrogen bond)into the polyacrylamide molecular chain.Thanks to the exceptional freeze resistance(84%capacity retention at-20℃)and intrinsic self-healing capabilities(95%capacity retention after 5 cutting/self-healing cycles),the obtained AF/SH-Hydrogel makes the zinc||manganese dioxide cell an economically feasible battery for the state-of-the-art applications.The Zn||AF/SH-Hydrogel||MnO_(2)device offers a near-theoretical specific capacity of 285 m A h g^(-1)at 0.1 A g^(-1)(Coulombic efficiency≈100%),as well as good self-healing capability and mechanical flexibility in an ice bath.This work provides insight that can be utilized to develop multifunctional hydrogel electrolytes for application in next generation of self-healable and freeze-resistance smart aqueous energy storage devices.
基金This work was financially supported by the National Natural Science Foundation of China(52173106 and 22375154).
文摘Aqueous rechargeable Zn-metal batteries(ARZBs)are considered one of the most promising candidates for grid-scale energy storage.However,their widespread commercial application is largely plagued by three major challenges:The uncontrollable Zn dendrites,notorious parasitic side reactions,and sluggish Zn^(2+) ion transfer.To address these issues,we design a sustainable dual crosslinked cellulose hydrogel electrolyte,which has excellent mechanical strength to inhibit dendrite formation,high Zn^(2+) ions binding capacity to suppress side reaction,and abundant porous structure to facilitate Zn^(2+) ions migration.Consequently,the Zn||Zn cell with the hydrogel electrolyte can cycle stably for more than 400 h under a high current density of 10 mA cm^(−2).Moreover,the hydrogel electrolyte also enables the Zn||polyaniline cell to achieve high-rate and long-term cycling performance(>2000 cycles at 2000 mA g^(−1)).Remarkably,the hydrogel electrolyte is easily accessible and biodegradable,making the ARZBs attractive in terms of scalability and sustainability.
基金supported by PLA General Hospital Program,No.LB20201A010024(to LW).
文摘Neurotrophic keratopathy is a persistent defect of the corneal epithelium,with or without stromal ulceration,due to corneal nerve deficiency caused by a variety of etiologies.The treatment options for neurotrophic keratopathy are limited.In this study,an ophthalmic solution was constructed from a chitosan-based thermosensitive hydrogel with long-term release of murine nerve growth factor(CTH-mNGF).Its effectiveness was evaluated in corneal denervation(CD)mice and patients with neurotrophic keratopathy.In the preclinical setting,CTH-mNGF was assessed in a murine corneal denervation model.CTH-mNGF was transparent,thermosensitive,and ensured sustained release of mNGF for over 20 hours on the ocular surface,maintaining the local mNGF concentration around 1300 pg/mL in vivo.Corneal denervation mice treated with CTH-mNGF for 10 days showed a significant increase in corneal nerve area and total corneal nerve length compared with non-treated and CTH treated mice.A subsequent clinical trial of CTH-mNGF was conducted in patients with stage 2 or 3 neurotrophic keratopathy.Patients received topical CTH-mNGF twice daily for 8 weeks.Fluorescein sodium images,Schirmer’s test,intraocular pressure,Cochet-Bonnet corneal perception test,and best corrected visual acuity were evaluated.In total,six patients(total of seven eyes)diagnosed with neurotrophic keratopathy were enrolled.After 8 weeks of CTH-mNGF treatment,all participants showed a decreased area of corneal epithelial defect,as stained by fluorescence.Overall,six out of seven eyes had fluorescence staining scores<5.Moreover,best corrected visual acuity,intraocular pressure,Schirmer’s test and Cochet-Bonnet corneal perception test results showed no significant improvement.An increase in corneal nerve density was observed by in vivo confocal microscopy after 8 weeks of CTH-mNGF treatment in three out of seven eyes.This study demonstrates that CTH-mNGF is transparent,thermosensitive,and has sustained-release properties.Its effectiveness in healing corneal epithelial defects in all eyes with neurotrophic keratopathy suggests CTH-mNGF has promising application prospects in the treatment of neurotrophic keratopathy,being convenient and cost effective.
基金the National Natural Science Foundation of China(Grant No.52076028).
文摘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.
基金This work is supported by the International Publication Research Grant No.RDU223301 and Postgraduate Research Grant Scheme,UMP,Malaysia(PGRS210370).
文摘With the exponential development in wearable electronics,a significant paradigm shift is observed from rigid electronics to flexible wearable devices.Polyaniline(PANI)is considered as a dominant material in this sector,as it is endowed with the optical properties of both metal and semiconductors.However,its widespread application got delineated because of its irregular rigid form,level of conductivity,and precise choice of solvents.Incorporating PANI in textile materials can generate promising functionality for wearable applications.This research work employed a straightforward in-situ chemical oxidative polymerization to synthesize PANI on Cotton fabric surfaces with varying dopant(HCl)concentrations.Pre-treatment using NaOH is implemented to improve the conductivity of the fabric surface by increasing the monomer absorption.This research explores the morphological and structural analysis employing SEM,FTIR and EDX.The surface resistivity was measured using a digital multimeter,and thermal stability is measured using TGA.Upon successful polymerization,a homogenous coating layer is observed.It is revealed that the simple pre-treatment technique significantly reduces the surface resistivity of Cotton fabric to 1.27 kΩ/cm with increasing acid concentration and thermal stability.The electro-thermal energy can also reach up to 38.2°C within 50 s with a deployed voltage of 15 V.The modified fabric is anticipated to be used in thermal regulation,supercapacitor,sensor,UV shielding,antimicrobial and other prospective functional applications.
文摘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].