The successful synthesis of the pentazolate anion(cyclo-N-5)has been a great breakthrough in the field of energetic materials.However,the detection methods for these energetic materials based on the pentazolate anion ...The successful synthesis of the pentazolate anion(cyclo-N-5)has been a great breakthrough in the field of energetic materials.However,the detection methods for these energetic materials based on the pentazolate anion are quite rare.Herein,two fluorescent probes for cyclo-N-5anion were designed.Sensor 1(TPE2N)was synthesized with a tetraphenylethylene functionalized by two cationic groups which can generate strong electrostatic interactions with pentazolate anion and result in specific fluorescent changes.Sensor 2 was designed based on sensor 1 and supramolecular cucurbit[7]uril(CB[7]).The unique structural features of CB[7]provide sites for the interaction between the cations and N-5anion in its cavity,which would generate a platform for the detection and enhance the recognition performance.Isothermal titration calorimetry(ITC)experiment and fluorescence titration experiment indicate the binding molar ratio between sensor 1 with CB[7]is 1:2.Both sensors display typical aggregation-induced emission(AIE)features and good water-solubility.The sensors demonstrate excellent sensitivity to pentazole hydrazine salt with high enhancement constant(sensor 1:1.34×10^(6);sensor 2:3.78×10^(6))and low limit of detection(LOD:sensor 1=4.33μM;sensor 2=1.54μM).The formation of an AIE-based supramolecular sensor effectively improves the sensitivity to N-5anion.In addition,the probes also have good selectivity of N-5anion salts.The research would shed some light on the design of novel fluorescent sensors to detect pentazolate-based molecules and provides an example of supramolecular chemistry combined with fluorescent probes.展开更多
Oil-soluble bimetallic CoMoS nanoparticles were successfully synthesized by a composite-surfactants-aided-solvothermal process.The surface hydrophilicity and functionality of the products were investigated through tra...Oil-soluble bimetallic CoMoS nanoparticles were successfully synthesized by a composite-surfactants-aided-solvothermal process.The surface hydrophilicity and functionality of the products were investigated through transmission electron microscopy (TEM),Fourier transform infrared (FTIR) spectra,and Ultraviolet (UV) spectra analysis.The catalytic performance of hydrogenation on the CoMoS nanoparticles was studied with naphthalene as a model compound.It was found that CoMoS catalysts supported on active carbon (AC) was more active than conventional MoS2/γ-Al2O3.The activity of CoMoS/AC can be tailored through the change of the Co/(Co+Mo) atomic ratio.展开更多
Motile plant tissues can control their configurations and regulate their motion speed according to their specific requirements,which offer various protypes for biomimetic actuators with controlled motion speed.In this...Motile plant tissues can control their configurations and regulate their motion speed according to their specific requirements,which offer various protypes for biomimetic actuators with controlled motion speed.In this perspective,we focus on the speed control of plant tissues and the bioinspired strategies for speed regulation of artificial actuators.We begin with a summary to the strategies and mechanisms of motile plant tissues for controlling motion speed,ranging from ultrafast to ultraslow.We then exemplify the models for fabricating bioinspired artificial actuators and briefly discuss current application scenarios of actuators with varying speeds from ultrafast to ultraslow.Finally,we propose potential strategies for the speed regulation of actuators.展开更多
Passive radiative cooling is widely recognized as an environmentally sustainable method for achieving significant cooling effects.However,the mechanical properties and environmental adaptability of current radiative c...Passive radiative cooling is widely recognized as an environmentally sustainable method for achieving significant cooling effects.However,the mechanical properties and environmental adaptability of current radiative cooling materials are not sufficient to maintain high cooling performance in external environments.Here we reported an environment-adaptive phase-separation-porous fluorofilm for high-performance passive radiation cooling.Compared to the homogenous fluoro-porous network with limited scattering efficiencies,we modulated the porous structure of the fluorofilm to achieve a strong emissivity of 95.2%(8-13μm)and a high reflectivity of 97.1%(0.3-2.5μm).The fluorofilm demonstrates a temperature drop of 10.5°C and an average cooling power of 81 W·m^(−2)under a sunlight power of 770 W·m^(−2).The high mechanical performance and environmental adaptability of fluorofilms are also exhibited.Considering its significant radiative cooling capability and robust environmental adaptability,the fluorofilm is expected to have a promising future in radiative temperature regulation.展开更多
Self-pumping dressings(SPDs)have been developed as a new type of effective material for the drainage of excessive wound exudates based on the structure of asymmetric wettability.However,current SPDs are easy to lose t...Self-pumping dressings(SPDs)have been developed as a new type of effective material for the drainage of excessive wound exudates based on the structure of asymmetric wettability.However,current SPDs are easy to lose their asymmetric wettability due to the weak interfacial mechanical stability between the hydrophobic and hydrophilic layers.Herein,we report an integrated self-pumping organohydrogel dressing with aligned microchannels(SPD-AM),prepared by an ice-templating-assisted wetting-enabled-transfer(WET)polymerization strategy,that can accelerate the healing process of diabetic wounds.The WET polymerization strategy enables strong interfacial mechanical stability between the hydrophobic organogel and hydrophilic hydrogel layers.The aligned microchannels greatly improve the draining capability of SPDs.Taking a diabetic rat model as an example,the SPD-AM can significantly reduce the bacterial colonization with low inflammatory responses,enhance dermal remodeling by about 47.31%,and shorten wound closure time by about 1/5 compared with other dressings,ultimately accelerating diabetic wound healing.This study is valuable for developing next-generation SPDs with stable mechanical performance for clinical applications.展开更多
Disgusting deposits(e.g.,scale and crude oil)in daily life and industrial production are always serious problems,posing great threats to the safety and economic development.However,most of developed coatings can only ...Disgusting deposits(e.g.,scale and crude oil)in daily life and industrial production are always serious problems,posing great threats to the safety and economic development.However,most of developed coatings can only conquer one part of these deposits such as superhydrophobic coatings possess antiscaling capacity but would adhere crude oil.To integrate scale resistance with oil repellence,we herein report a robust superamphiphobic(SAB)coating simultaneously reducing pollution of scale and oil for extended period of time(two weeks with over 98%reduction).Compared with single role of superhydrophobic and amphiphilic surfaces,the SAB coating can not only inhibit interfacial nucleation of scale but also reduce the adhesion of formed scale and polluted oil.The durability of the SAB coating is evaluated via mechanical tests(sandpaper abrasion,tape stripping and sand falling)and chemical corrosion(corrosive liquid immersing),revealed by sustainable high contact angles and low contact angle hysteresis of water and oil.The universality of this strategy can be further confirmed by adding different particles like kaolin,Al_(2)O_(3),and SiO_(2),resisting multiple types of scale(i.e.,CaSO_(4),BaSO_(4)and MgCO_(3))and oil(i.e.,glycerol,glycol,and mineral oil).Therefore,this study provides an ideal avenue for resisting scale and oil,which may be used for conquering the complexity of application environments(e.g.,oil production and transportation).展开更多
Due to the various pH liquid environment in nature,the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute.However,the applied liquid environment will lead to poor m...Due to the various pH liquid environment in nature,the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute.However,the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive capability.In this work,a carbon dotsenhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dynamic PVA-borax network into a PAAm covalent polymer network.The formed hydrogel presents a partial gel-sol transition under controlled pH environments.At low pH environments(<6.0),the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel,and brings the lubricating properties on the hydrogel surface.Moreover,the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel,the blue sol layer can be observed more visually under the fluorescence microscope.The pH-response also exhibits well reversibility.The prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.展开更多
Inflammatory cytokine storms can trigger disease exacerbation and even death and have reached a consensus in the clinical treatment of acute organ failure.However,the existing strategies remain a great challenge to ef...Inflammatory cytokine storms can trigger disease exacerbation and even death and have reached a consensus in the clinical treatment of acute organ failure.However,the existing strategies remain a great challenge to efficiently suppress inflammatory cytokine storms for promoting organ repair and regeneration.Herein,fully human umbilical cord(UC)-derived adhesive materials(UCAM)that integrate decellularized extracellular matrix(ECM)nanofiber hydrogel and homologous mesenchymal stem cells(MSCs)are demonstrated to greatly suppress inflammatory cytokine storms,demonstrating high efficacy in treating acute liver failure(ALF)in rats with 90%hepatectomy.The UC-derived adhesive materials have the capacity to secrete a significant quantity of cytokines by MSCs to recruit activated immune cells to migrate into their ECM nanofiber networks,segregating them away from the infection area and thereby greatly suppressing the inflammatory cytokine storms.As expected,the UC-derived adhesive materials can significantly promote hepatocyte proliferation to achieve functional recovery and regeneration of the liver,significantly improving the survival rate in rats.Our fully human UC-derived adhesive materials provide a new avenue in suppressing inflammatory cytokine storms for promoting organ regeneration that would be really utility in clinical organ transplantation-related treatment.展开更多
Marangoni effect at the two-phase interface with different surface tension as a unique mass transfer phenomenon has been widely used in daily life and industrialmanufacture.However,their marvelous liquid-driving capab...Marangoni effect at the two-phase interface with different surface tension as a unique mass transfer phenomenon has been widely used in daily life and industrialmanufacture.However,their marvelous liquid-driving capability between miscible liquids has long been ignored,especially in water environments.Here,we first reveal a distinct underwater Marangoni effect between the solvent of glues and the water layer on solid surfaces.Driven by the Marangoni effect,organic solvents with water solubility,high dielectric constant,and low diffusivity could effectively exclude the interfacial water layer,enabling direct and effective contact between glues and solid surfaces.Our experimental results and theoretical simulation proved that a relatively large ratio of the Marangoni number in the horizontal direction and to the vertical direction ensured an effective underwater adhesion of the water-excluding glue.This surface engineering approach provides an alternative to the traditional methods of molecular engineering for realizing underwater adhesion.展开更多
Cartilage-inspired hydrogel has attracted great interest due to its tunable mechanics and low friction.However,it is incapable of self-healing under a complex dynamic shearing environment.In this work,a self-healing s...Cartilage-inspired hydrogel has attracted great interest due to its tunable mechanics and low friction.However,it is incapable of self-healing under a complex dynamic shearing environment.In this work,a self-healing semi-convertible hydrogel(SHSCH)is developed,which can recover its unique active lubricating function under shearing.Based on the cooperating strategy of noncovalent and covalent bonding,the SHSCH is composed of three interpenetrated networks including:(1)shearresponsive N-fluorenylmethoxycarbonyl-L-tryptophan(FT)supramolecular network,(2)self-healing polyhydroxyethyl acrylamide(PHEAA)network,and(3)rigid polyvinyl alcohol(PVA)covalent network.The shearresponsive lubricating function and mechanical property can be self-healed under a shearing environment through the noncovalent hydrogen-bonding assembly of PHEAA associated by theπ–πassembly of FT.The asdeveloped SCH provides a self-healing model comparable with traditional self-healing lubricating materials through encapsulating lubricant microcapsules or infusing lubricants onto surfaces.We demonstrated a proofof-concept of the self-healing lubrication of a simplified artificial worn cartilage model under a dynamic shearing condition.This study will offer a potential strategy on designing the self-healing soft devices under dynamic stimuli far beyond the lubricating materials.展开更多
The self‐assembly of block copolymers(BCPs)within emulsion droplets is a flexible strategy for the preparation of polymer particles.This strategy permits the finetuning of shapes,internal structures,and surface nanos...The self‐assembly of block copolymers(BCPs)within emulsion droplets is a flexible strategy for the preparation of polymer particles.This strategy permits the finetuning of shapes,internal structures,and surface nanostructures of the polymer particles,thus allowing many applications.Although some literature has reviewed the BCP preparation via self‐assembly within a droplet,a comprehensive summary including in‐depth understanding,controllable preparation,and application is lacked.In this review,we systematically delve into the multiple mechanisms that drive BCP self‐assembly within emulsion droplets,such as commensurability effects for minimizing total free energy,interfacial instability,organized spontaneous emulsification,phase separation of multiple components,and entropy effects between BCPs and nanoparticles.Additionally,a strategy combining selective cross‐linking and disassembly can further generate Janus particles featuring unique structures.Next,various applications across multiple disciplines are discussed,including drug delivery,display,biomedical imaging,macromolecular separation,and fuel cells.Finally,we present an overview of the current challenges and future directions for BCP emulsion self‐assembly,covering mechanism investigation,molecular design,stability control,and application exploration.We anticipate deeper understanding,more varieties,enhanced performance,and broader applications can be achieved with BCP emulsion self‐assembly after addressing the challenge.展开更多
Surface wettability is important to design biointerfaces and fimctional biomaterials in various biological applications. However, to date, it remains some confusions about how cells would response to the surfaces with...Surface wettability is important to design biointerfaces and fimctional biomaterials in various biological applications. However, to date, it remains some confusions about how cells would response to the surfaces with different wettabilities. Herein, we systematically explore the adhesive spectra of cells to the surface with wettability gradient from superhydrophilicity to superhydrophobicity, clarifying the effect of wettability on cell adhesion. We envision that this study may provide valuable information for the design of biomedical implants with controllable cell adhesion, such as neural interface devices and flexible implant.展开更多
Underwater adhesion is greatly desired in tissue transplantation, medical treatment, ocean transportation, and so on. However, common commercial polymeric adhesives are rather weakened and easily destroyed in water en...Underwater adhesion is greatly desired in tissue transplantation, medical treatment, ocean transportation, and so on. However, common commercial polymeric adhesives are rather weakened and easily destroyed in water envi- ronment. In nature, some marine organisms, such as mussels, barnacles, or tube worms, exhibiting excellent under- water adhesion up to robust bonding on the rock of sea floor, can give exciting solutions to address the problem. Among these marine organisms, mussels exhibit unique underwater adhesion via the foot proteins of byssus. It has been verified that the catechol groups from the side chain of the mussel foot proteins is the main contribution to the unique underwater adhesion. Hence, inspired by the mussels' underwater adhesion, many mussel-mimetic polymers with catechol as end chains or side chains have been developed in the past decades. Here, we review recent progress of mussel-inspired underwater adhesives polymers from their catechol-functional design to their potential applica- tions in intermediates, anti-biofouling, self-healing of hydrogels, biological adhesives, and drug delivery. The re- view may provide basis and help for the development of the commercial underwater adhesives.展开更多
Hydrogels, composed mainly of water trapped in three dimensional cross-linked polymer networks, have been widely utilized to construct underwater superoleophobic surfaces. However, the swelling nature and instability ...Hydrogels, composed mainly of water trapped in three dimensional cross-linked polymer networks, have been widely utilized to construct underwater superoleophobic surfaces. However, the swelling nature and instability of hydrogels under complex marine environment will weaken their underwater superoleophobicity. Herein, we synthesize structured poly (2-hydroxyethylmethacrylate) (PHEMA) hydrogels by using sandpaper as templates. The robust non-swelling of PHEMA hydrogel ensures that micro/nano-structures on the surface of PHEMA hydrogels can be well maintained. Moreover, when roughness Ra of about 3-4 bun, the surface has superior oil-repellency. Additionally, even after immersing in seawater for one-month, their breaking strength and toughness can be well kept. The non-swellable hydrogels with long-term stable under seawater superoleophobicity will promote the development of robust superoleophobic materials in marine antifouling coatings, biomedical devices and oil/water separation.展开更多
Multiply robust inference has attracted much attention recently in the context of missing response data. An estimation procedure is multiply robust, if it can incorporate information from multiple candidate models, an...Multiply robust inference has attracted much attention recently in the context of missing response data. An estimation procedure is multiply robust, if it can incorporate information from multiple candidate models, and meanwhile the resulting estimator is consistent as long as one of the candidate models is correctly specified. This property is appealing, since it provides the user a flexible modeling strategy with better protection against model misspecification. We explore this attractive property for the regression models with a binary covariate that is missing at random. We start from a reformulation of the celebrated augmented inverse probability weighted estimating equation, and based on this reformulation, we propose a novel combination of the least squares and empirical likelihood to separately handle each of the two types of multiple candidate models,one for the missing variable regression and the other for the missingness mechanism. Due to the separation, all the working models are fused concisely and effectively. The asymptotic normality of our estimator is established through the theory of estimating function with plugged-in nuisance parameter estimates. The finite-sample performance of our procedure is illustrated both through the simulation studies and the analysis of a dementia data collected by the national Alzheimer's coordinating center.展开更多
Studying the wetting behaviors of multicellular spheroids is crucial in the fields of embryo implantation, cancer propagation, and tissue repair. Existing strategies for controlling the wetting of multicellular sphero...Studying the wetting behaviors of multicellular spheroids is crucial in the fields of embryo implantation, cancer propagation, and tissue repair. Existing strategies for controlling the wetting of multicellular spheroids mainly focus on surface chemistry and substrate rigidity. Although topography is another important feature in the biological micro-environment, its effect on multicellular spheroid wetting has seldom been explored. In this study, the influence of topography on the surface wetting of multicellular spheroids was investigated using subcellular- patterned opal films with controllable colloidal particle diameters (from 200 to 1,500 nm). The wetting of hepatoma carcinoma cellular (Hep G2) spheroids was impaired on opal films compared with that on flat substrates, and the wetting rate decreased as colloidal particle diameter increased. The decrement reached 48.5% when the colloidal particle diameter was 1,500 nm. The subcellular-patterned topography in opal films drastically reduced the cellular mobility in precursor films, especially the frontier cells in the leading edge. The frontier cells failed to form mature focal adhesions and stress fibers on micro-patterned opal films. This was due to gaps between colloidal particles leaving adhesion vacancies, causing weak cell-substrate adhesion and consequent retarded migration of Hep G2 spheroids. Our study manifests the inhibiting effects of subcellular-patterned topography on the wetting behaviors of multicellular spheroids, providing new insight into tissue wetting-associated treatments and biomaterial design.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.22175093 and 22007047)the Natural Science Foundation of Jiangsu Province(Grant No.BK20200474)the China Postdoctoral Science Foundation(Grant No.2022M721615)。
文摘The successful synthesis of the pentazolate anion(cyclo-N-5)has been a great breakthrough in the field of energetic materials.However,the detection methods for these energetic materials based on the pentazolate anion are quite rare.Herein,two fluorescent probes for cyclo-N-5anion were designed.Sensor 1(TPE2N)was synthesized with a tetraphenylethylene functionalized by two cationic groups which can generate strong electrostatic interactions with pentazolate anion and result in specific fluorescent changes.Sensor 2 was designed based on sensor 1 and supramolecular cucurbit[7]uril(CB[7]).The unique structural features of CB[7]provide sites for the interaction between the cations and N-5anion in its cavity,which would generate a platform for the detection and enhance the recognition performance.Isothermal titration calorimetry(ITC)experiment and fluorescence titration experiment indicate the binding molar ratio between sensor 1 with CB[7]is 1:2.Both sensors display typical aggregation-induced emission(AIE)features and good water-solubility.The sensors demonstrate excellent sensitivity to pentazole hydrazine salt with high enhancement constant(sensor 1:1.34×10^(6);sensor 2:3.78×10^(6))and low limit of detection(LOD:sensor 1=4.33μM;sensor 2=1.54μM).The formation of an AIE-based supramolecular sensor effectively improves the sensitivity to N-5anion.In addition,the probes also have good selectivity of N-5anion salts.The research would shed some light on the design of novel fluorescent sensors to detect pentazolate-based molecules and provides an example of supramolecular chemistry combined with fluorescent probes.
基金supported by the Shandong Natural Science Foundation(ZR2009BQ008)China University of Petroleum(YO60419)
文摘Oil-soluble bimetallic CoMoS nanoparticles were successfully synthesized by a composite-surfactants-aided-solvothermal process.The surface hydrophilicity and functionality of the products were investigated through transmission electron microscopy (TEM),Fourier transform infrared (FTIR) spectra,and Ultraviolet (UV) spectra analysis.The catalytic performance of hydrogenation on the CoMoS nanoparticles was studied with naphthalene as a model compound.It was found that CoMoS catalysts supported on active carbon (AC) was more active than conventional MoS2/γ-Al2O3.The activity of CoMoS/AC can be tailored through the change of the Co/(Co+Mo) atomic ratio.
基金support of the National Natural Science Foundation of China(Nos.22035008,21972155,and 21988102)the International Partnership Program of Chinese Academy of Sciences(No.1A1111KYSB20200010).
文摘Motile plant tissues can control their configurations and regulate their motion speed according to their specific requirements,which offer various protypes for biomimetic actuators with controlled motion speed.In this perspective,we focus on the speed control of plant tissues and the bioinspired strategies for speed regulation of artificial actuators.We begin with a summary to the strategies and mechanisms of motile plant tissues for controlling motion speed,ranging from ultrafast to ultraslow.We then exemplify the models for fabricating bioinspired artificial actuators and briefly discuss current application scenarios of actuators with varying speeds from ultrafast to ultraslow.Finally,we propose potential strategies for the speed regulation of actuators.
基金the National Natural Science Foundation of China(Nos.22035008,22275183,21972155,and 21988102)the National Key R&D Program of China(Nos.2019YFA0709300 and 2022YFE0201200)International Partnership Program of Chinese Academy of Sciences(No.1A1111KYSB20200010).
文摘Passive radiative cooling is widely recognized as an environmentally sustainable method for achieving significant cooling effects.However,the mechanical properties and environmental adaptability of current radiative cooling materials are not sufficient to maintain high cooling performance in external environments.Here we reported an environment-adaptive phase-separation-porous fluorofilm for high-performance passive radiation cooling.Compared to the homogenous fluoro-porous network with limited scattering efficiencies,we modulated the porous structure of the fluorofilm to achieve a strong emissivity of 95.2%(8-13μm)and a high reflectivity of 97.1%(0.3-2.5μm).The fluorofilm demonstrates a temperature drop of 10.5°C and an average cooling power of 81 W·m^(−2)under a sunlight power of 770 W·m^(−2).The high mechanical performance and environmental adaptability of fluorofilms are also exhibited.Considering its significant radiative cooling capability and robust environmental adaptability,the fluorofilm is expected to have a promising future in radiative temperature regulation.
基金supported by the National Natural Science Foundation of China(22035008,21972155,22002177,and 22205244)Youth Innovation Promotion Association,Chinese Academy of Sciences(CAS)(2022027)+1 种基金CAS-Croucher Funding Scheme for Joint LaboratoriesChina Postdoctoral Science Foundation(2022M713225)。
文摘Self-pumping dressings(SPDs)have been developed as a new type of effective material for the drainage of excessive wound exudates based on the structure of asymmetric wettability.However,current SPDs are easy to lose their asymmetric wettability due to the weak interfacial mechanical stability between the hydrophobic and hydrophilic layers.Herein,we report an integrated self-pumping organohydrogel dressing with aligned microchannels(SPD-AM),prepared by an ice-templating-assisted wetting-enabled-transfer(WET)polymerization strategy,that can accelerate the healing process of diabetic wounds.The WET polymerization strategy enables strong interfacial mechanical stability between the hydrophobic organogel and hydrophilic hydrogel layers.The aligned microchannels greatly improve the draining capability of SPDs.Taking a diabetic rat model as an example,the SPD-AM can significantly reduce the bacterial colonization with low inflammatory responses,enhance dermal remodeling by about 47.31%,and shorten wound closure time by about 1/5 compared with other dressings,ultimately accelerating diabetic wound healing.This study is valuable for developing next-generation SPDs with stable mechanical performance for clinical applications.
基金financially supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB0470201)Beijing Natural Science Foundation(No.JQ23008)the National Natural Science Foundation of China(Nos.22275203 and 22035008)。
文摘Disgusting deposits(e.g.,scale and crude oil)in daily life and industrial production are always serious problems,posing great threats to the safety and economic development.However,most of developed coatings can only conquer one part of these deposits such as superhydrophobic coatings possess antiscaling capacity but would adhere crude oil.To integrate scale resistance with oil repellence,we herein report a robust superamphiphobic(SAB)coating simultaneously reducing pollution of scale and oil for extended period of time(two weeks with over 98%reduction).Compared with single role of superhydrophobic and amphiphilic surfaces,the SAB coating can not only inhibit interfacial nucleation of scale but also reduce the adhesion of formed scale and polluted oil.The durability of the SAB coating is evaluated via mechanical tests(sandpaper abrasion,tape stripping and sand falling)and chemical corrosion(corrosive liquid immersing),revealed by sustainable high contact angles and low contact angle hysteresis of water and oil.The universality of this strategy can be further confirmed by adding different particles like kaolin,Al_(2)O_(3),and SiO_(2),resisting multiple types of scale(i.e.,CaSO_(4),BaSO_(4)and MgCO_(3))and oil(i.e.,glycerol,glycol,and mineral oil).Therefore,this study provides an ideal avenue for resisting scale and oil,which may be used for conquering the complexity of application environments(e.g.,oil production and transportation).
基金supported by the National Natural Science Foundation of China(No.22175075).
文摘Due to the various pH liquid environment in nature,the pH-responsive lubricating hydrogel is widely investigated and developed for tissue interface substitute.However,the applied liquid environment will lead to poor mechanical property and weaken the pH-responsive capability.In this work,a carbon dotsenhanced pH-responsive lubricating hydrogel is developed by combining a pH-responsive section of dynamic PVA-borax network into a PAAm covalent polymer network.The formed hydrogel presents a partial gel-sol transition under controlled pH environments.At low pH environments(<6.0),the formed lubricating layer originated from dynamic disassembly of PVA-borax hydrogel,and brings the lubricating properties on the hydrogel surface.Moreover,the mechanical strength and lubrication properties are well promoted by introducing the carbon dots into the hydrogel,the blue sol layer can be observed more visually under the fluorescence microscope.The pH-response also exhibits well reversibility.The prepared hydrogel broadens the idea for designing pH-responsive soft materials for soft lubricating actuator or robot.
基金support by the National Key R&D Program of China (2022YFA1104900,2022YFA0806301)the National Natural Science Foundation of China (22075127,31972926,82371725,and 32301204)the Guangdong Key Research and Develop-ment Plan (2019B020234003).
文摘Inflammatory cytokine storms can trigger disease exacerbation and even death and have reached a consensus in the clinical treatment of acute organ failure.However,the existing strategies remain a great challenge to efficiently suppress inflammatory cytokine storms for promoting organ repair and regeneration.Herein,fully human umbilical cord(UC)-derived adhesive materials(UCAM)that integrate decellularized extracellular matrix(ECM)nanofiber hydrogel and homologous mesenchymal stem cells(MSCs)are demonstrated to greatly suppress inflammatory cytokine storms,demonstrating high efficacy in treating acute liver failure(ALF)in rats with 90%hepatectomy.The UC-derived adhesive materials have the capacity to secrete a significant quantity of cytokines by MSCs to recruit activated immune cells to migrate into their ECM nanofiber networks,segregating them away from the infection area and thereby greatly suppressing the inflammatory cytokine storms.As expected,the UC-derived adhesive materials can significantly promote hepatocyte proliferation to achieve functional recovery and regeneration of the liver,significantly improving the survival rate in rats.Our fully human UC-derived adhesive materials provide a new avenue in suppressing inflammatory cytokine storms for promoting organ regeneration that would be really utility in clinical organ transplantation-related treatment.
基金supported by the National Key R&D Program of China(project nos.2018YFA0209500 and 2019YFA0709300)the National Natural Science Foundation of China(grant nos.21621091,21972155,21975209,22005255,22035008,52025132,and 22205244)+2 种基金Projects of International Cooperation and Exchanges Natural Science Foundation of China(NSFC,grant no.1A1111KYSB20200010)National Program for Special Support of Eminent Professionals and the Fundamental Research Funds for Central Universities(grant no.20720190037)the China Postdoctoral Science Foundation(grant no.2022M713225).
文摘Marangoni effect at the two-phase interface with different surface tension as a unique mass transfer phenomenon has been widely used in daily life and industrialmanufacture.However,their marvelous liquid-driving capability between miscible liquids has long been ignored,especially in water environments.Here,we first reveal a distinct underwater Marangoni effect between the solvent of glues and the water layer on solid surfaces.Driven by the Marangoni effect,organic solvents with water solubility,high dielectric constant,and low diffusivity could effectively exclude the interfacial water layer,enabling direct and effective contact between glues and solid surfaces.Our experimental results and theoretical simulation proved that a relatively large ratio of the Marangoni number in the horizontal direction and to the vertical direction ensured an effective underwater adhesion of the water-excluding glue.This surface engineering approach provides an alternative to the traditional methods of molecular engineering for realizing underwater adhesion.
基金supported financially by the National Natural Science Foundation of China(grant nos.22175075,22035008,21972155,21774044,21425314,21434009,21421061).
文摘Cartilage-inspired hydrogel has attracted great interest due to its tunable mechanics and low friction.However,it is incapable of self-healing under a complex dynamic shearing environment.In this work,a self-healing semi-convertible hydrogel(SHSCH)is developed,which can recover its unique active lubricating function under shearing.Based on the cooperating strategy of noncovalent and covalent bonding,the SHSCH is composed of three interpenetrated networks including:(1)shearresponsive N-fluorenylmethoxycarbonyl-L-tryptophan(FT)supramolecular network,(2)self-healing polyhydroxyethyl acrylamide(PHEAA)network,and(3)rigid polyvinyl alcohol(PVA)covalent network.The shearresponsive lubricating function and mechanical property can be self-healed under a shearing environment through the noncovalent hydrogen-bonding assembly of PHEAA associated by theπ–πassembly of FT.The asdeveloped SCH provides a self-healing model comparable with traditional self-healing lubricating materials through encapsulating lubricant microcapsules or infusing lubricants onto surfaces.We demonstrated a proofof-concept of the self-healing lubrication of a simplified artificial worn cartilage model under a dynamic shearing condition.This study will offer a potential strategy on designing the self-healing soft devices under dynamic stimuli far beyond the lubricating materials.
基金National Key R&D Program of China,Grant/Award Numbers:2022YFA1206900,2019YFA0709300National Natural Science Foundation of China,Grant/Award Number:22035008+1 种基金Key Research Program of the Chinese Academy of Sciences,Grant/Award Number:XDPB24International Partnership Program of Chinese Academy of Sciences,Grant/Award Number:1A1111KYSB20200010。
文摘The self‐assembly of block copolymers(BCPs)within emulsion droplets is a flexible strategy for the preparation of polymer particles.This strategy permits the finetuning of shapes,internal structures,and surface nanostructures of the polymer particles,thus allowing many applications.Although some literature has reviewed the BCP preparation via self‐assembly within a droplet,a comprehensive summary including in‐depth understanding,controllable preparation,and application is lacked.In this review,we systematically delve into the multiple mechanisms that drive BCP self‐assembly within emulsion droplets,such as commensurability effects for minimizing total free energy,interfacial instability,organized spontaneous emulsification,phase separation of multiple components,and entropy effects between BCPs and nanoparticles.Additionally,a strategy combining selective cross‐linking and disassembly can further generate Janus particles featuring unique structures.Next,various applications across multiple disciplines are discussed,including drug delivery,display,biomedical imaging,macromolecular separation,and fuel cells.Finally,we present an overview of the current challenges and future directions for BCP emulsion self‐assembly,covering mechanism investigation,molecular design,stability control,and application exploration.We anticipate deeper understanding,more varieties,enhanced performance,and broader applications can be achieved with BCP emulsion self‐assembly after addressing the challenge.
基金supported by the National Natural Science Foundation of China(21425314,21501184,21434009,21421061,21504098)the Key Research Program of the Chinese Academy of Sciences(KJZD-EW-M01)+2 种基金Ministry of Science and Technology(2013YQ190467)the Top-Notch Young Talents Program of ChinaBeijing Municipal Science&Technology Commission(Z161100000116037)
文摘Surface wettability is important to design biointerfaces and fimctional biomaterials in various biological applications. However, to date, it remains some confusions about how cells would response to the surfaces with different wettabilities. Herein, we systematically explore the adhesive spectra of cells to the surface with wettability gradient from superhydrophilicity to superhydrophobicity, clarifying the effect of wettability on cell adhesion. We envision that this study may provide valuable information for the design of biomedical implants with controllable cell adhesion, such as neural interface devices and flexible implant.
基金This review is supported by the National Natural Science Foundation of China (Nos. 21425314, 21501184, 21434009, 21421061 and 21504098), the Key Research Program of the Chinese Academy of Sci- ences (No. KJZD-EW-M01 ), MOST (No. 2013YQI90467), the Top-Notch Young Talents Pro- gram of China, and Beijing Municipal Science & Tech- nology Commission (No. Z161100000116037).
文摘Underwater adhesion is greatly desired in tissue transplantation, medical treatment, ocean transportation, and so on. However, common commercial polymeric adhesives are rather weakened and easily destroyed in water envi- ronment. In nature, some marine organisms, such as mussels, barnacles, or tube worms, exhibiting excellent under- water adhesion up to robust bonding on the rock of sea floor, can give exciting solutions to address the problem. Among these marine organisms, mussels exhibit unique underwater adhesion via the foot proteins of byssus. It has been verified that the catechol groups from the side chain of the mussel foot proteins is the main contribution to the unique underwater adhesion. Hence, inspired by the mussels' underwater adhesion, many mussel-mimetic polymers with catechol as end chains or side chains have been developed in the past decades. Here, we review recent progress of mussel-inspired underwater adhesives polymers from their catechol-functional design to their potential applica- tions in intermediates, anti-biofouling, self-healing of hydrogels, biological adhesives, and drug delivery. The re- view may provide basis and help for the development of the commercial underwater adhesives.
基金supported by the National Natural Science Foundation (21574004, 21421061, 21434009, 21301036)the National Research Fund for Fundamental Key Projects (2012CB933800)+4 种基金the Fundamental Research Funds for the Central Universitiesthe National “Young Thousand Talents Program”Xiamen Southern Oceanographic Center (14GQT61HJ31)the Key Research Program of the Chinese Academy of Sciences (KJZD-EW-M01, KJZD-EW-M03)the Program of Introducing Talents of Discipline to Universities of China (B14009)
文摘Hydrogels, composed mainly of water trapped in three dimensional cross-linked polymer networks, have been widely utilized to construct underwater superoleophobic surfaces. However, the swelling nature and instability of hydrogels under complex marine environment will weaken their underwater superoleophobicity. Herein, we synthesize structured poly (2-hydroxyethylmethacrylate) (PHEMA) hydrogels by using sandpaper as templates. The robust non-swelling of PHEMA hydrogel ensures that micro/nano-structures on the surface of PHEMA hydrogels can be well maintained. Moreover, when roughness Ra of about 3-4 bun, the surface has superior oil-repellency. Additionally, even after immersing in seawater for one-month, their breaking strength and toughness can be well kept. The non-swellable hydrogels with long-term stable under seawater superoleophobicity will promote the development of robust superoleophobic materials in marine antifouling coatings, biomedical devices and oil/water separation.
文摘Multiply robust inference has attracted much attention recently in the context of missing response data. An estimation procedure is multiply robust, if it can incorporate information from multiple candidate models, and meanwhile the resulting estimator is consistent as long as one of the candidate models is correctly specified. This property is appealing, since it provides the user a flexible modeling strategy with better protection against model misspecification. We explore this attractive property for the regression models with a binary covariate that is missing at random. We start from a reformulation of the celebrated augmented inverse probability weighted estimating equation, and based on this reformulation, we propose a novel combination of the least squares and empirical likelihood to separately handle each of the two types of multiple candidate models,one for the missing variable regression and the other for the missingness mechanism. Due to the separation, all the working models are fused concisely and effectively. The asymptotic normality of our estimator is established through the theory of estimating function with plugged-in nuisance parameter estimates. The finite-sample performance of our procedure is illustrated both through the simulation studies and the analysis of a dementia data collected by the national Alzheimer's coordinating center.
基金This research is supported by National Natural Science Foundation of China (Nos. 21425314, 21434009, and 21421061), National Program for Special Support of Eminent Professionals, Beijing Municipal Science & Technology Commission (No. Z161100000116037), and MOST (No. 2013YQ190467).
文摘Studying the wetting behaviors of multicellular spheroids is crucial in the fields of embryo implantation, cancer propagation, and tissue repair. Existing strategies for controlling the wetting of multicellular spheroids mainly focus on surface chemistry and substrate rigidity. Although topography is another important feature in the biological micro-environment, its effect on multicellular spheroid wetting has seldom been explored. In this study, the influence of topography on the surface wetting of multicellular spheroids was investigated using subcellular- patterned opal films with controllable colloidal particle diameters (from 200 to 1,500 nm). The wetting of hepatoma carcinoma cellular (Hep G2) spheroids was impaired on opal films compared with that on flat substrates, and the wetting rate decreased as colloidal particle diameter increased. The decrement reached 48.5% when the colloidal particle diameter was 1,500 nm. The subcellular-patterned topography in opal films drastically reduced the cellular mobility in precursor films, especially the frontier cells in the leading edge. The frontier cells failed to form mature focal adhesions and stress fibers on micro-patterned opal films. This was due to gaps between colloidal particles leaving adhesion vacancies, causing weak cell-substrate adhesion and consequent retarded migration of Hep G2 spheroids. Our study manifests the inhibiting effects of subcellular-patterned topography on the wetting behaviors of multicellular spheroids, providing new insight into tissue wetting-associated treatments and biomaterial design.