Liquid Metal-Based Self-Healable and Elastic Conductive Fiber in Complex Operating Conditions

Flexible conductive fibers are essential for wearable electronics and smart electronic textiles.However,in complex operating conditions,conductive fibers will inevitably fracture or damage.Herein,we have developed an elastic conductive self-healable fiber(C-SHF),of which the electrical and mechanical properties can efficiently heal in a wide operating range,including room temperature,underwater,and low temperature.This advantage can be owed to the combination of reversible covalent imine bond and disulfide bond,as well as the instantaneous self-healing ability of liquid metal.The C-SHF,with stretchability,conductivity stability,and universal self-healing properties,can be used as an electrical signal transmission line at high strain and under different operating conditions.Besides,C-SHF was assembled into a double-layer capacitor structure to construct a self-healable sensor,which can effectively respond to pressure as a wearable motion detector.

Self-healable gels in electrochemical energy storage devices

In the green energy and carbon-neutral technology,electrochemical energy storage devices have received continuously increasing attention recently.However,due to the unavoidable volume expansion/shrinkage of key materials or irreversible mechanical damages during application,the stability of energy storage and delivery as well as the lifetime of these devices are severely shortened,leading to serious performance degradation or even safety issues.Therefore,the utilization of self-healable gels into electrochemical energy storage devices,such as electrodes,binders,and electrolytes,is proven as an effective method to realize long-term stable operation of these devices via the self-repairing of mechanical and electrochemical characteristics.Herein,this review first summarizes the feature and fabrication of different gels,paying special attention to hydrogels,organohydrogels,and ionogels.Then,basic concepts and figure of merit of self-healable gels are analyzed with a detailed discussion at the healing mechanisms,from reversible dynamic bonds to physical molecular diffusion,and to external healing trigger.Then we introduce all the important parts of electrochemical energy storage devices,which could be replaced by healable gels to enhance the durability,including electrodes,binders,and electrolytes.Finally,the critical challenges and future perspectives regarding the future development of healable gels based high-performance electrochemical energy storage devices or electronics are provided.

An injectable,self-healable,and reusable PEDOT:PSS/PVA hydrogel patch electrode for epidermal electronics

Injectability empowers conductive hydrogels to transcend traditional limitations,unlocking a realm of possibilities for innovative medical,wearable,and therapeutic applications that can significantly enhance patient care and quality of life.Here,we report an injectable,self-healable,and reusable hydrogel obtained by mixing the concentrated poly(3,4-ethylenedioxythiophene)doped with polystyrene sulfonate(PEDOT:PSS)suspension(~2 wt.%solid content),polyvinyl alcohol(PVA),and borax.Leveraging the presence of reversible borax/hydroxyl bonds and multiple hydrogen bonds,this PEDOT:PSS/PVA hydrogel exhibits notable shear-thinning behavior and self-healing capabilities,enabling it to be injected as a gel fiber from a syringe.As-prepared injectable hydrogel also demonstrates an ultra-low modulus(~2.5 MPa),reduced on-skin impedance(~45%of commercial electrodes),and high signal-to-noise ratio(SNR)(~15-22 dB)in recording of electrocardiography(ECG),electromyography(EMG),and electroencephalogram(EEG)signals.Furthermore,the injectable hydrogels can be remolded and reinjected as the reusable electrodes,maintaining nearly identical electrophysiological recording capabilities and brain-computer interface(BCI)performance compared to commercial wet electrodes.With their straightforward fabrication,excellent material properties and electronic performance,ease of cleaning,and remarkable reusability,our injectable PEDOT:PSS/PVA hydrogels hold promise for advancements in BCI based electronics and wearable bioelectronics.

Self-healable and Robust Film Based on Electroactive Polymer Brush as Electrode for Flexible Supercapacitor

The aim of this study was to develop self-healable and robust elect roconductive film based on polyaniline copolymer for application as electrode in flexible supercapacitor.For this purpose,the electroconductive polymer brushes(EPB)was elaborated.The synthesis of EPB is based on graft polymerizations of acrylamide(AAm)on poly(vinyl alcohol)(PVA)with formation of PVA-PAAm polymer brush and subsequent graft copolymerization of aniline and p-phenylenediamine on PVA-PAAm resulting in formation of EPB with electroconducting copoly(aniline-co-pphenylenediamine)(PAPh DA).It was found that the ratio between PVA and PAAm at the first stage greatly influence the electrochemical performance of the EPBs.Electroconducting films were prepared by casting of EPB solution with subsequent drying.Investigation of electrical current distribution through the film with AFM reveal more uniform distribution of PAPhDA in EPB in comparison with reference PVA-PAPhDA and PAAm-PAPhDA samples.It was demonstrated that mechanical cha racteristics and electrical conductivity values of films restore at large extent after curring and self-healing under optimal relative humidity level(58%).The flexile supercapacitor cell with EPB film electrodes demon strate specific capacitance 602 mF·cm^(-2)at the current density of 1 mA·cm^(-2)and retention 94%of initial capacitance after 5000 charge/discharge cycles.

Neutral color and self-healable electrochromic system based on CuI/Cu and I_(3)^(-)/I^(-)conversions

The electrochromic(EC)mechanisms of inorganic materials are usually based on reversible cation insertion/extraction or metal deposition/dissolution,which are plagued by ion trapping and dendrite growth,respectively.In this paper,a novel conversion-type electrochromic mechanism is proposed,by making good use of the CuI/Cu redox couple.This CuI-based electrochromic system shows a neutral color switching from transparent and dim grey.By simply increasing the bleaching voltage,I_(3)^(-)/I^(-)redox couple can be further activated.The generated I_(3)^(-)will readily react with Cu,effectively improving the conversion reversibility and thereby rejuvenating the degraded electrochromic performance.Thanks to the well-designed electrode and the self-healing ability,this conversion electrochromic system achieves rapid response times(tcoloring:23 s,tbleaching:6 s),decant optical modulation amplitude(26.4%),high coloration efficiency(86.15 cm^(2)·C^(-1)),admirable cyclic durability(without performance degradation after 480 cycles)and excellent optical memory ability(transmittance variation<1%after 10 h open-circuit storage).The establishment of this conversion-type electrochromism may inspire the exploration of novel electrochromic materials and devices.

Crosslinked Natural Rubber and Styrene Butadiene Rubber Blends/Carbon Black Composites for Self-healable and Energy-saved Applications

Crosslinking natural rubber (NR) and styrene butadiene rubber (SBR) composites with carbon black (CB) have been utilized in the tire tread industry.A sulfur-based lightly crosslinker can potentially enhance the self-healing capabilities of rubber.Moreover,the rubber composites were studied for non-covalent interactions between the benzene rings of SBR and CB.In this research,rubber samples were prepared,and their structure was investigated using Fourier transform infrared (FTIR),and Raman spectroscopy.The red shift in Raman spectroscopy confirmed noncovalent interaction or hydrophobic interaction between SBR and CB in NR/SBR composites exposed to CB due to environmental change.The differential scanning calorimetry (DSC) thermograms showed that NR and SBR were incompatible.Additionally,the mechanical properties of these rubber blends were enhanced as the proportion of NR increased.The maximum self-healing performance reached 40%for the formulation containing 25 phr NR and 75 phr SBR,which also saved energy with low chain end movements.Therefore,these composites could be utilized as a semi-empirical model for studying crosslinked rubber blends,specifically in the rubber tire industry.

Emerging trends in self-healable nanomaterials for triboelectric nanogenerators:A comprehensive review and roadmap

A thorough analysis of triboelectric nanogenerators (TENGs) that make use of self-healable nanomaterials is presented in this review. These TENGs have shown promise as independent energy sources that do not require an external power source to function. TENGs are developing into a viable choice for powering numerous applications as low-power electronics technology advances. Despite having less power than conventional energy sources, TENGs do not directly compete with these. TENGs, on the other hand, provide unique opportunities for future self-powered systems and might encourage advancements in energy and sensor technologies. Examining the many approaches used to improve nanogenerators by employing materials with shape memory and self-healable characteristics is the main goal of this review. The findings of this comprehensive review provide valuable information on the advancements and possibilities of TENGs, which opens the way for further research and advancement in this field. The discussion of life cycle evaluations of TENGs provides details on how well they perform in terms of the environment and identifies potential improvement areas. Additionally, the cost-effectiveness, social acceptability, and regulatory implications of self-healing TENGs are examined, as well as their economic and societal ramifications.

Solvent-Free Synthesis of Self-Healable and Recyclable Crosslinked Polyurethane Based on Dynamic Oxime-Urethane Bonds

Polyurethane is widely used for its versatility in design and range of performance.Self-healing and recyclable dynamic polyurethane networks have attracted extensive attention due to their potential to extend service life and ensure safety in use,as well as to promote sustainable use of resources.Developing green and environment-friendly methods to obtain this material is an interesting and challenging task,as the majority of current dynamic polyurethane networks utilize the solution polymerization method.The use of solvents makes the processes complicated,harmful to environment,and increase the cost.Poly(oxime-urethanes)(POUs)are emerging dynamic polyurethanes and show great potential in diverse fields,such as biomaterials,hot melt adhesives,and flexible electronics.In this study,we utilized the solubility properties of dimethylglyoxime in raw material poly(ethylene glycol)to prepare POUs through bulk polymerization for the first time.This method is simple,convenient and cost-efficient.Simultaneously,copper ion coordination improves POUs strength and dynamic properties,with mechanical strength up from 0.54 MPa to 1.03 MPa and self-healing recovery rate up from 85.5%to 91.8%,and activation energy down from 119.6 k J/mol to 95.4 k J/mol.To demonstrate the application of this technology,self-healing and stretchable circuits are constructed from this dynamic polyurethane network.

Self-healable, recyclable, ultrastretchable, and high-performanceNO_(2) sensors based on an organohydrogel for room and sub-zero temperature and wireless operation

To date,development of high-performance,stretchable gas sensors operating at and below room temperature(RT)remains a challenge in terms of traditional sensing materials.Herein,we report on a high-performance NO_(2) gas sensor based on a self-healable,recyclable,ultrastretchable,and stable polyvinyl alcohol–cellulose nanofibril double-network organohydrogel,which features ultrahigh sensitivity(372%/ppm),low limit of detection(2.23 ppb),relatively fast response and recovery time(41/144 s for 250 ppb NO_(2)),good selectivity against interfering gases(NH3,CO_(2),ethanol,and acetone),excellent reversibility,repeatability,and long-term stability at RT or even at−20°C.In particular,this sensor shows outstanding stability against large deformations and mechanical damages so that it works normally after rapid self-healing or remolding after undergoing mechanical damage without significant performance degradation,which has major advantages compared to state-of-the-art gas sensors.The high NO_(2) sensitivity and selectivity are attributed to the selective redox reactions at the threephase interface of gas,gel,and electrode,which is even boosted by applying tensile strain.With a specific electrical circuit design,a wireless NO_(2) alarm system based on this sensor is created to enable continuous,real-time,and wireless NO_(2) detection to avoid the risk of exposure to NO_(2) higher than threshold concentrations.

Mechanical reliable,NIR light-induced rapid self-healing hydrogel electrolyte towards flexible zinc-ion hybrid supercapacitors with low-temperature adaptability and long service life

Hydrogel electrolytes hold great potential in flexible zinc ion supercapacitors(ZICs)due to their high conductivity,good safety,and flexibility.However,freezing of electrolytes at low temperature(subzero)leads to drastic reduction in ionic conductivity and mechanical properties that deteriorates the performance of flexible ZICs.Besides,the mechanical fracture during arbitrary deformations significantly prunes out the lifespan of the flexible device.Herein,a Zn^(2+)and Li^(+)co-doped,polypyrrole-dopamine decorated Sb_(2)S_(3)incorporated,and polyvinyl alcohol/poly(N-(2-hydroxyethyl)acrylamide)double-network hydrogel electrolyte is constructed with favorable mechanical reliability,anti-freezing,and self-healing ability.In addition,it delivers ultra-high ionic conductivity of 8.6 and 3.7 S m^(-1)at 20 and−30°C,respectively,and displays excellent mechanical properties to withstand tensile stress of 1.85 MPa with tensile elongation of 760%,together with fracture energy of 5.14 MJ m^(-3).Notably,the fractured hydrogel electrolyte can recover itself after only 90 s of infrared illumination,while regaining 83%of its tensile strain and almost 100%of its ionic conductivity during−30–60°C.Moreover,ZICs coupled with this hydrogel electrolyte not only show a wide voltage window(up to 2 V),but also provide high energy density of 230 Wh kg^(-1)at power density of 500 W kg^(-1)with a capacity retention of 86.7%after 20,000 cycles under 20°C.Furthermore,the ZICs are able to retain excellent capacity even under various mechanical deformation at−30°C.This contribution will open up new insights into design of advanced wearable flexible electronics with environmental adaptability and long-life span.

Visible Light-driven Self-healable Mechanochromic Polyurethanes

Polyurethanes incorporating spiropyran(SP)and diselenide(DiSe)in the main chain,which are confined in different hard segments are developed.Visible light-driven diselenide metathesis and mechanically induced ring opening of SP offer self-healing and mechanochromic properties of the polymers,respectively.Delicate selection of the polymer backbone is found essential to promote the dual functions.In particular for polyurethane with SP coupled into 4,4'-methylenebis(cyclohexyl isocyanate)and DiSe linked with isophorone diisocyanate,excellent mechanical,mechanochromic and self-healing properties are estimated.Moreover,combining self-healing and self-reporting moieties in one chain allows the discrimination of different healing mechanisms,including bond formation and chain entanglement,in a visualized way.

A Biomimetic Tooth Replicate That Is Hard,Damage-Tolerant,and Self-Healable

Hard materials typically lack the mechanism of energy dissipation and cannot self-heal.Nature addresses this challenge by creating multiscale interfaces between high-contrast materials,namely minerals and biopolymers.Inspired by the enamel-dentin junction in nature,an enamel-like crown consisting ofβFeOOH nanocolumns is interdigitated with a flexible self-healing layer.The iron oxide top layer has exceptionally high modulus and hardness,which is more resistant to cyclic deformation than the bottom layer.The latter however provides an additional pathway for viscous and plastic energy dissipation and enables self-healing by allowing upward polymer diffusion to seal the damage.Picture-frame crack patterns were observed under large loading conditions using microindentation,which localizes the damage at the indentation site.The bending properties can be optimized by varying the thickness of the bottom layer,and the crack induced by bending can be effectively captured at the interface without any delamination.The biomimetic tooth replicate is highly adhesive to a ceramic surface and shows an obvious inhibition effect against Streptococcus mutans,a significant contributor to tooth decay.Combined with ultralow thermal diffusivity,this has great potential as dental material.Learning from nature,our work thus provides a powerful pathway to broadening the scope of synthetic materials for dental replicates.

A Self-Healing Optoacoustic Patch with High Damage Threshold and Conversion Efficiency for Biomedical Applications

Compared with traditional piezoelectric ultrasonic devices,optoacoustic devices have unique advantages such as a simple preparation process,anti-electromagnetic interference,and wireless long-distance power supply.However,current optoacoustic devices remain limited due to a low damage threshold and energy conversion efficiency,which seriously hinder their widespread applications.In this study,using a self-healing polydimethylsiloxane(PDMS,Fe-Hpdca-PDMS)and carbon nanotube composite,a flexible optoacoustic patch is developed,which possesses the self-healing capability at room temperature,and can even recover from damage induced by cutting or laser irradiation.Moreover,this patch can generate high-intensity ultrasound(>25 MPa)without the focusing structure.The laser damage threshold is greater than 183.44 mJ cm^(-2),and the optoacoustic energy conversion efficiency reaches a major achievement at 10.66×10^(-3),compared with other carbon-based nanomaterials and PDMS composites.This patch is also been successfully examined in the application of acoustic flow,thrombolysis,and wireless energy harvesting.All findings in this study provides new insight into designing and fabricating of novel ultrasound devices for biomedical applications.

Multifunctional phase change film with high recyclability, adjustable thermal responsiveness, and intrinsic self-healing ability for thermal energy storage

Phase change materials(PCMs) present promising potential for guaranteeing safety in thermal management systems.However,most reported PCMs have a single application in energy storage for thermal management systems,which does not meet the growing demand for multi-functional materials.In this paper,the flexible material and hydrogen-bonding function are innovatively combined to design and prepare a novel multi-functional flexible phase change film(PPL).The 0.2PPL-2 film exhibits solid-solid phase change behavior with energy storage density of 131.8 J/g at the transition temperature of42.1℃,thermal cycling stability(500 cycles),wide-temperature range flexibility(0-60℃) and selfhealing property.Notably,the PPL film can be recycled up to 98.5% by intrinsic remodeling.Moreover,the PPL film can be tailored to the desired colors and configurations and can be cleverly assembled on several thermal management systems at ambient temperature through its flexibility combined with shape-memory properties.More interestingly,the transmittance of PPL will be altered when the ambient temperature changes(60℃),conveying a clear thermal signal.Finally,the thermal energy storage performance of the PPL film is successfully tested by human thermotherapy and electronic device temperature control experiments.The proposed functional integration strategy provides innovative ideas to design PCMs for multifunctionality,and makes significant contributions in green chemistry,highefficiency thermal management,and energy sustainability.

Flexible,thermal processable,self-healing,and fully bio-based starch plastics by constructing dynamic imine network

The serious environmental threat caused by petroleum-based plastics has spurred more researches in developing substitutes from renewable sources.Starch is desirable for fabricating bioplastic due to its abundance and renewable nature.However,limitations such as brittleness,hydrophilicity,and thermal properties restrict its widespread application.To overcome these issues,covalent adaptable network was constructed to fabricate a fully bio-based starch plastic with multiple advantages via Schiff base reactions.This strategy endowed starch plastic with excellent thermal processability,as evidenced by a low glass transition temperature(T_(g)=20.15℃).Through introducing Priamine with long carbon chains,the starch plastic demonstrated superior flexibility(elongation at break=45.2%)and waterproof capability(water contact angle=109.2°).Besides,it possessed a good thermal stability and self-adaptability,as well as solvent resistance and chemical degradability.This work provides a promising method to fabricate fully bio-based plastics as alternative to petroleum-based plastics.

An intrinsically self-healing and anti-freezing molecular chains induced polyacrylamide-based hydrogel electrolytes for zinc manganese dioxide batteries

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.

Effect of drying cracks on swelling and self-healing of bentonite-sand blocks used as engineered barriers for radioactive waste disposal

Experiments were conducted to evaluate the healing of drying cracks in air-dried bentonite-sand blocks after hydration and swelling in groundwater,providing justifications to simplify the protection of blocks prior to installation in a high-level radioactive waste repository.Synthetic groundwater was prepared to represent the geochemistry of Beishan groundwater,and was used to hydrate the blocks during the swelling pressure and swelling strain measurements,as Beishan is the most promising site for China's repository.Healing of the surface cracks was recorded by photography,and healing of the internal cracks was visualized by CT images and hydraulic conductivity of air-dried blocks.The results indicate that the maximum swelling pressure and swelling strain are primarily affected by the geochemistry of Beishan groundwater,but not affected by the drying cracks.The maximum swelling pressure and swelling strain of air-dried blocks are comparable to or even higher than the pressure and strain of fresh blocks.The maximum swelling pressure measured in strong(i.e.high ion strength)Beishan groundwater was 44%of the pressure measured in deionized(DI)water,and the maximum swelling strain was reduced to 23%of the strain measured in DI water.Nevertheless,the remained swelling of the blocks hydrated in strong Beishan groundwater was sufficient to heal the surface and internal drying cracks,as demonstrated by the pictures of surface cracks and CT images.The hydraulic conductivity of the air-dried block permeated with strong groundwater was comparable(3.7×higher)to the hydraulic conductivity of the fresh block,indicating the self-healing of drying cracks after hydration and swelling in groundwater.A simplified method of protecting the block with plastic wraps before installation is recommended,since the remained swelling of the block hydrated in Beishan groundwater is sufficient to heal the drying cracks.

High performance photodegradation resistant PVA@TiO_(2)/carboxyl-PES self-healing reactive ultrafiltration membrane

The occurrence of ultrafiltration(UF)membrane fouling frequently hampers the sustainable advancement of UF technology.Reactive self-cleaning UF membranes can effectively alleviate the problem of membrane fouling.Nevertheless,the self-cleaning process may accelerate membrane aging.Addressing these concerns,we present an innovative design concept for composite self-healing materials based on self-cleaning UF membranes.To begin,TiO_(2)nanoparticles were incorporated into the polymer molecular structure via molecular design,resulting in the synthesis of TiO_(2)/carboxyl-polyether sulfone(PES)hybrid materials.Subsequently,the nonsolvent-induced phase inversion technique was employed to prepare a novel of UF membrane.Lastly,a polyvinyl alcohol(PVA)hydrogel coating was applied to the hybrid UF membrane surface to create PVA@TiO_(2)/carboxyl-PES self-healing reactive UF membranes.By establishing a covalent bond,the TiO_(2)nanoparticles were effectively and uniformly dispersed within the UF membrane,leading to exceptional self-cleaning properties.Furthermore,the water-absorbing and swelling properties of PVA hydrogel,along with its capacity to form hydrogen bonds with water molecules,resulted in UF membranes with improved hydrophilicity and active self-healing abilities.The results demonstrated that the water contact angle of PVA@5%TiO_(2)/carboxyl-PES UF membrane was 43.1°.Following a 1-h exposure to simulated solar exposure,the water flux recovery ratio increased from 48.16%to 81.03%.Moreover,even after undergoing five cycles of 12-h simulated sunlight exposure,the UF membranes exhibited a consistent retention rate of over 97%,thus fully demonstrating their exceptional self-cleaning,antifouling,and selfhealing capabilities.We anticipate that the self-healing reactive UF membrane system will serve as a pioneering and comprehensive solution for the self-cleaning antifouling challenges encountered in UF membranes while also effectively mitigating the aging effects of reactive UF membranes.

Self-healable wire-shaped supercapacitors with two twisted NiCo_2O_4 coated polyvinyl alcohol hydrogel fibers

Wire-shaped supercapacitors（SCs） possessing light-weight, good flexibility and weavability have caught much attention, but it is still a challenge to extend the lifespan of the devices with gradual aging due to the rough usage or external factors. Herein, we report a new stretchable and selfhealable wire-shaped SC. In the typical process, two polyvinyl alcohol/potassium hydroxide（PVA/KOH） hydrogel wrapped with urchin-like NiCo2O4 nanomaterials were twisted together to form a complete SC devices. It is noted that the as-prepared PVA hydrogel can be easily stretched up to 300% with small tensile stress of 12.51 kPa, superior to nearly 350 kPa at 300%strain of the polyurethane. Moreover, the wire-like SCs exhibit excellent electrochemical performance with areal capacitance of 3.88 mF cm^-2 at the current density of 0.053 mA cm^-2, good cycling stability maintaining 88.23% after 1000 charge/discharge cycles, and 82.19% capacitance retention even after four damaging/healing cycles. These results indicate that wireshaped SCs with two twisted NiCo2O4 coated polyvinyl alcohol hydrogel fibers is a promising structure for achieving the goal of high stability and long-life time. This work may provide a new solution for new generation of self-healable and wearable electronic devices.

Robust and Self-healable Antibiofilm Multilayer Coatings

The infection induced by implantation of biomedical materials may result from the biofilm formation after bacteria attachment.Hence,the antibiofilm surface coating represents a novel technique to improve the antibacterial activity of biomedical materials.The traditional antibiofilm surface coatings exhibited some disadvantages and provided a limited service life.In this work,we used polyethyleneimine grafted 3-maleimidopropionic acid(PEIM)and poly(acrylic acid)grafted 2-furfurylamine(PAAF)to achieve robust and self-healable crosslinked multilayer coatings,employing Layer-by-Layer(LbL)self-assembly technique and Diels-Alder reaction.Then,thiol-terminated poly((3-acrylamidopropyl)trimethylammonium chloride)(PAMPTMA-SH)was grafted onto the crosslinked multilayer coating by thiol-ene click reaction to form a novel multilayer coating(PEIM/PAAF)_(10)-PAMPTMA.We found that this coating showed robust and self-healable activity,and significantly inhibited the bacterial growth and biofilm formation after infection with Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus)by in vitro and in vivo assays for 120 h.In addition,the multilayer coating did not induce significant hemolysis or affect the cell viability of red blood cells.In vivo studies also showed that(PEIM/PAAF)_(10)-PAMPTMA coating efficiently blocked the infiltration of inflammatory cells and gene expression in the mouse skin challenged with E coli or S.aureus.Taken together,these results showed that the prepared multilayer coating exhibited strong antibiofilm activity and provided a new strategy for the application of highly efficient antibiofilm surface coating of biomedical materials.