It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible d...It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display technologies.Herein,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino groups.Subsequently,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the tetrafluorostyrene.The transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 nm.The thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.展开更多
Polyimide(PI)is widely used in high-tech fields such as microelectronics,aerospace,and national defense because of its excellent optical properties,high-and low-temperature resistance,and good dimensional stability.To...Polyimide(PI)is widely used in high-tech fields such as microelectronics,aerospace,and national defense because of its excellent optical properties,high-and low-temperature resistance,and good dimensional stability.To achieve the desired properties of PI,the monomers 2,6-diaminopyrimidin-4-ol(DAPD)and 6-(2,3,5,6-tetrafluoro-4-vinylphenoxy)pyrimidin-2,4-diamine(DAFPD),which contains crosslinkable functional groups,were designed and synthesized successfully and copolymerized with 4,4'-oxydianiline(ODA)and 4,4-hexafluoroisopropylphthalic anhydride(6FDA).The prepared PI film(PI-3),with rigid backbones and loose packing had excellent heat resistance(Td5%=489℃)and optical properties(T450=82%).Furthermore,a crosslinked PI film(c-PI-3)with more heat-resistant(Td5%=524℃)and better mechanical properties(σ=125.46MPa),can be obtained through thermal crosslinking of tetrafluorostyrene.In addition,the changes in the properties caused by the proportion of DAFPD added during copolymerization are discussed comprehensively.This study provides a promising candidate for heat-resistant PI materials.展开更多
Two crosslinkable poly（p-phenyleneethynylene）s（PPEs）： poly[2,5-di（2＇-ethyl-hexyloxy）-1,4-phenylenecthynylene] with end-capped vinyl（PPE1） and poly[2,5-di（allyloxy）-1,4-phenyleneethynylene-2,5-di（2＇-ethyl...Two crosslinkable poly（p-phenyleneethynylene）s（PPEs）： poly[2,5-di（2＇-ethyl-hexyloxy）-1,4-phenylenecthynylene] with end-capped vinyl（PPE1） and poly[2,5-di（allyloxy）-1,4-phenyleneethynylene-2,5-di（2＇-ethyl-hexyloxy）-1,4-phenyleneethynylene]（PPE2） were synthesized. Via the thermal addition reactions of vinyl end groups of PPE1 and allyloxy side groups of PPE2, crosslinked polymers C-PPE1 and C-PPE2 were obtained, respectively. The two polymers were characterized by wide-angle X-ray diffraction（WXRD）, ultraviolet-visible（UV-Vis） absorption, and photoluminescence（PL）. The results indicate that in the solid state, the polymer chains of PPE1 were packed with a low degree of crystallinity because of the sterically hindered（2＇-ethyl-hexyl）oxy branched side chains, but, because of the introduction of allyloxy side chains, the polymer chains of PPE2 were packed in an order fashion with a high degree of crystallinity. Because of the high crosslinking density in C-PPE2, the formation of aggregates and excimer was hampered by the formed crosslinking network more effectively in C-PPE2 film than in C-PPE1 film.展开更多
Three new functional group containing borazine derivatives, 2,4,6-tri（allylamino）borazine, 2,4,6-tri（3-ethynylanilino）borazine, and 2,4,6-tri（4-propargyl oxyanilino）borazine were synthesized by aminolysis reacti...Three new functional group containing borazine derivatives, 2,4,6-tri（allylamino）borazine, 2,4,6-tri（3-ethynylanilino）borazine, and 2,4,6-tri（4-propargyl oxyanilino）borazine were synthesized by aminolysis reaction of 2,4,6-trichloroborazine ClaB3N3H3（TCB）. The new compounds were characterized by infrared （IR） spectra, nuclear magnetic resonance （NMR）, and mass spectrometry （MS）.展开更多
Two commercial crosslinkable polyethylene insulation cable granules, designed for 110 and 35 kV voltage insulation, with similar crosslinking temperature but different melting temperature, were chosen as experimental ...Two commercial crosslinkable polyethylene insulation cable granules, designed for 110 and 35 kV voltage insulation, with similar crosslinking temperature but different melting temperature, were chosen as experimental samples for examining their linear dynamic responses during cross-linking. It has been found that the gel contents of cable compounds for 110 and 35 kV insulation are almost the same after they have been cross-linked at the same temperature, pressure and time. And the sample melts show the similar dependence of the dynamic storage modulus, G; on strain. On the other hand, the dynamic temperature ramp test and the dynamic time sweep test indicate that the samples exhibit different dynamic viscoelastic responses during their crosslinking. An expression for describing their erosslinking process was proposed via probing rheokinetics of crosslinking for the two samples.展开更多
To date,more biodegradable polymers have been developed due to the growing recognition of the advantages of biodegradable and biocompatible polymers for biomedical applications.In this study,we introduce the synthesis...To date,more biodegradable polymers have been developed due to the growing recognition of the advantages of biodegradable and biocompatible polymers for biomedical applications.In this study,we introduce the synthesis and characterization of innovative polymers that incorporate biodegradable backbones composed of trimethylol-propane and adipic acid moieties and biocleavable side chains containing pyridyl disulfide groups.Notably,their synthesis is straightforward and catalyst-free under ambient conditions,minimizing potential toxicity and immune responses caused by catalyst residues in polymer materials.The new polymers have desired molecular weight(Mn:18.8 kDa)with a narrow dispersion(PDI:1.32)and offer complete biodegradability,biocompatibility,crosslinking capabilities,and opportunities for covalent chemical modifications.These features make them particularly suitable for use in biomedical materials and devices.Additionally,due to their unique properties,these polymers have been successfully formulated into polymeric gels and nanogels,which are biodegradable as well.Using a near-infrared fluorescent probe as a model cargo,we demonstrated the creation of a biosafe and sustainable nanogel system for agent delivery,with an average size of approximately 70 nm.In these nanogels,agent molecules are covalently attached to the scaffold,thereby avoiding uncontrolled premature release and burst release in the bloodstream and mitigating associated systemic toxicity and side effects.The nanogels can also be easily functionalized with targeting ligands for disease-specific delivery.These polymers induced minimal toxicity toward human cells and displayed excellent in vivo biocompatibility,highlighting the significant potential of their polymeric gels and nanogels for a broad spectrum of biomedical applications.展开更多
The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water ev...The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.展开更多
The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild r...The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.展开更多
With the growth of global protein demand and the development of plant-based foods,pea protein,as a low-allergenic,nutritionally balanced and environmentally friendly plant protein,has shown great potential in replacin...With the growth of global protein demand and the development of plant-based foods,pea protein,as a low-allergenic,nutritionally balanced and environmentally friendly plant protein,has shown great potential in replacing animal protein.Pea protein is mainly composed of globulin and albumin,with a protein content of 20%to 30%,and has a balanced amino acid composition,as well as being rich in minerals and dietary fiber.It also possesses good foaming,gelling,emulsifying and antioxidant functional properties.However,pea protein also has inherent defects that limit its application in the food industry.This article systematically reviews the extraction techniques,functional properties,modification methods and application fields of pea protein,and focuses on evaluating the effects of different extraction and modification strategies on protein yield and functional properties.Research shows that ultrasonic-assisted alkaline extraction can reduce solvent usage by 55%,shorten extraction time by 50%,and increase extraction rate by 12.51%;under optimized conditions,ultrafiltration membrane technology can achieve a protein purity of 91%.In terms of modification,ultrasonic treatment increases foaming capacity by 37.4%,and phenolic cross-linking increases gel strength from 3.0 kPa to 48 kPa.This article provides data support and theoretical reference for the efficient extraction and functional optimization of pea protein,and has promoting significance for its wide application in plant-based foods.展开更多
RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progre...RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progression of numerous diseases,making RBPs potential therapeutic targets.However,the limited tissue penetration of 254 nm UV irradiation makes it difficult to efficiently crosslink weak and dynamic RNA-protein interactions in mammal tissues.Additionally,RNA degradation in metal catalyzed click reaction further hinders the enrichment of RNA-protein complexes(RPCs).Due to these inherent limitations,globally profiling the RNA binding proteome in mammal organs has long been a challenge.Herein,we proposed a novel method,which utilized a dual crosslinking with formaldehyde and 254 nm UV irradiation,metabolic labeling and metal-free thiol-yne click reaction to enable large-scale enrichment and identification of RBPs in mouse liver,called FTYc_UV.In this method,formaldehyde is first used to crosslink the crude RNA-protein complexes(cRPCs) in situ to address the problem of poor tissue penetration of 254 nm UV irradiation.Furthermore,this method integrates metabolic labeling with a metal-free thiol-yne click reaction to achieve non-destructive RNA tagging.After specifically RNA-RBPs crosslinking by 254 nm UV irradiation in tissue lysates,formaldehyde decrosslinking is employed to remove non-specific proteins,leading to effective enrichment of RPCs from mouse liver and thereby overcoming the poor specificity of formaldehyde crosslinking.Application of FTYc_UV in mouse liver successfully identified over 1600 RBPs covering approximately 75 % of previously reported RBPs.Furthermore,420 candidate RBPs,including 151metabolic enzymes,were also obtained,demonstrating the sensitivity of FTYc_UV and the potential of this method for in-depth exploration of RNA-protein interactions in biological and clinical research.展开更多
Porous hydrogel sensors have attracted significant attention in fields such as smart wearables and medical monitoring due to their high sensitivity.However,existing fabrication methods typically degrade the surface sm...Porous hydrogel sensors have attracted significant attention in fields such as smart wearables and medical monitoring due to their high sensitivity.However,existing fabrication methods typically degrade the surface smoothness of hydrogels when introducing porous structures and face significant challenges in removing fillers completely.To address these challenges,we herein introduce a novel one-step,thermosensitive spray-coating technique for the preparation of aircell hydrogel(ACH).This method leverages the rapid cooling of a thermoresponsive gelatin methacryloyl solution through atomization,enabling rapid cross-linking within seconds and air bubbles encapsulated in situ.Additionally,the transient flow of the pre-gel facilitates the repair of voids formed by ruptured surface bubbles,leading to the creation of the ACH with uniformly distributed inner air bubbles and a smooth outer surface.The mold-free fabrication method is independent of substrate surface properties,enabling the creation of a porous hydrogel film with a thickness as thin as 163 µm.Furthermore,the dual-crosslinked network endows the ACH with excellent anti-swelling properties,and the physical crosslinking between gelatin molecules allows the ACH to self-heal.The ACH exhibits excellent sensitivity in deformation sensing and can even successfully track minor external forces,which enables it to effectively complete various tasks such as facial expression recognition,pitch differentiation,and motion detection.By integrating the ACH into a sensing glove,we also demonstrate the significant potential of the ACH for applications in human-machine interaction and tactile sensing.Ultimately,the ACH sensors are also applied to motion mapping and machine tactile feedback,indicating their promising potential in human-machine interaction.展开更多
Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need fo...Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water.Here,we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions.These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants,characterized by high apparent adsorption rate constants(kobs)and maximum adsorption capacities(qmax,e).Notably,Compound NCCP-1 demonstrated a remarkable qmax,e of 459 mg/g for bisphenol A(BPA),ranking among the highest values reported for organic polymer adsorbents.In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them,primarily mediated by the hydrophobic effect.Furthermore,NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles,highlighting its potential for practical applications in water treatment.展开更多
With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics fo...With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics for continuous foot gait monitoring.Nevertheless,existing biomass-based TENG often faces challenges of insufficient mechanical robustness and durability in practical applications,where they are prone to surface abrasion and structural fracture under continuous compression and friction,severely limiting their long-term performances.In order to address these challenges,this work proposed a multiscale crosslinking strategy,which strengthened the noncovalent interactions within the polymer by constructing multiple reinforcement networks,successfully fabricating a dual-network C-lignin-based triboelectric material(CLTM)with excellent durability and crack resistance.Among them,the optimal CLTM(PSGCL-0.2)exhibited high mechanical strength(strain 445%,tensile strength 41.56 MPa,Young's modulus 41.25 MPa,toughness 159.67 MJ/m^(3))and excellent cyclic stability(300 cycles)with versatile functionalities,including antibacterial,antioxidant,and UV-shielding properties,water stabilization(255.51 g/m^(2)/d),efficient photothermal conversion,and full recyclability.Furthermore,biomass-based TENG device assembled from PSGCL-0.2 achieved stable triboelectric output properties(102.5 V,2.9μA,and 61.3 nC),and sustainable for 2000 cycles,fast response time(68 ms),and excellent power density(325.9 mW/m^(2)),effectively converting mechanical energy into electrical energy.Especially,PSGCL 0.2 was also integrated into the wireless self-powered smart insole,successfully enabling real-time visual monitoring of plantar pressure distribution and dynamic gait.Meanwhile,combined with the machine learning algorithm,the self-powered smart insole achieved precise recognition and classification of eight different motion states with an accuracy of 98%.This study provides the feasible strategy for developing extremely stable and durable biomass-based TENG,aimed at advancing sustainable intelligent healthcare systems.展开更多
Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the...Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the blood is crucial for the treatment of liver diseases.Hemoperfusion,which relies on adsorbents to efficiently adsorb toxins,is a widely applied procedure for the removal of blood toxins.To broaden and improve the range and performance of hemoperfusion adsorbents,we synthesized cationic hyper crosslinked polymers(HCPs)with strong affinity for bilirubin.This material exhibited outstanding adsorption performance,with a maximum adsorption capacity of 934 mg/g and a removal efficiency of 96%.Further investigation confirmed their excellent selectivity,reusability,and biocompatibility.These findings expand the potential applications of HCPs and provide insight into strategies for constructing promising hemoperfusion adsorbent materials.展开更多
Conventional polyethylene(PE)fibers face limitations in large-scale industrial applications due to their poor thermal stability and inherent hydrophobicity,which restrict processing temperatures and dyeability,especia...Conventional polyethylene(PE)fibers face limitations in large-scale industrial applications due to their poor thermal stability and inherent hydrophobicity,which restrict processing temperatures and dyeability,especially in blended fabric production.In this research,a one-step ultraviolet(UV)irradiation technology was employed to modify medium molecular weight PE fibers through simultaneous crosslinking and grafting modifications,aiming to enhance their thermal stability and hydrophilicity.The modification employed a cost-effective,UV-initiated crosslinking system consisting of benzophenone(BP)as the photoinitiator and triallyl isocyanurate(TAIC)as the cocrosslinker.Acrylic acid(AA)was selected as the grafting monomer.These modifiers were thoroughly mixed with the PE matrix in a liquid-phase environment,and the mixture was melt-spun into fibers.The resulting fibers were then subjected to UV irradiation,which triggered the crosslinking and grafting reactions.The effects of the mass fraction of each component and irradiation parameters on modification efficacy were systematically investigated,followed by a comprehensive characterization of the modified PE fibers.The modified PE fibers achieved optimal thermal stability under the following conditions:2.0%mass fractions for both BP and TAIC,a UV irradiation intensity of 2000 mW/cm^(2),and an equivalent irradiation time of 60 s.This synergistic modification approach enables the fibers to maintain superior morphological integrity and mechanical performance when exposed to elevated temperatures ranging from 130 to 150℃.Meanwhile,an AA grafting mass fraction of 2.0%maximizes hydrophilicity with minimal impact on other properties,as evidenced by a dramatic reduction in the water contact angle(WCA)from 105.0°(hydrophobic)to 48.4°(hydrophilic).These improvements confirm the effectiveness of the modification strategy in synergistically enhancing both thermal stability and hydrophilicity of PE fibers.展开更多
In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still face...In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.展开更多
Rapid and accurate visible-light photopolymerization is essential for advancing bioprinted engineered tissues.In this study,we developed a novel three-component photoinitiator system for visible light-induced crosslin...Rapid and accurate visible-light photopolymerization is essential for advancing bioprinted engineered tissues.In this study,we developed a novel three-component photoinitiator system for visible light-induced crosslinking of gelatin methacryloyl(GelMA)hydrogels,designed to improve polymerization kinetics,mechanical strength,and structural integrity.Incorporation of 2-bromoacetophenone(BAP)considerably accelerated photopolymerization,with reaction rates increasing alongside BAP concentration,enabling the rapid fabrication of stable hydrogel scaffolds.Printing experiments confirmed that BAP promoted fast crosslinking of GelMA bioinks under visible light,reducing printing time while preserving high-resolution structural features.Additionally,the incorporation of BAP induced microscale structural transformations in the hydrogels during hydration,as evidenced by scanning electron microscopy imaging and swelling analyses.This unique property enabled the fabrication of multilayer constructs exhibiting time-dependent deformation,demonstrating four-dimensional(4 D)printing ca pabilities.Moreover,biocompatibility evaluations revealed that cells maintained high viability in BAP-containing hydrogels.Overall,the BAP-based photoinitiator system offers a promising strategy for high-speed,high-resolution bioprinting,combining enhanced mechanical performance,reduced fabrication time,and dynamic structural adaptability-features that make it highly suitable for advanced biofabrication and tissue engineering applications.展开更多
As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(H...As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.展开更多
Polyethylene glycol(PEG)with different chains was used to modify epoxy asphalt.Molecular models of PEG⁃modified epoxy asphalt were developed using molecu⁃lar simulations(MS).The thermodynamic and mechanical properties...Polyethylene glycol(PEG)with different chains was used to modify epoxy asphalt.Molecular models of PEG⁃modified epoxy asphalt were developed using molecu⁃lar simulations(MS).The thermodynamic and mechanical properties of PEG⁃modified epoxy asphalt were analyzed,and its toughening mechanisms were explored.A method based on the Dijkstra algorithm was proposed to evaluate ep⁃oxy asphalt crosslinked networks.The results show that the introduction of PEG chains into epoxy asphalt can lower the glass transition temperature and enhance its toughness be⁃cause of the extended length of the PEG chains,which can in⁃crease the free volume and improve the mobility of the epoxy resin in the epoxy asphalt.The crosslinked network quantita⁃tive evaluation method based on the Dijkstra algorithm can ef⁃fectively evaluate the distribution of epoxy asphalt crosslink⁃ing bonds,providing further explanation of the toughening mechanism of PEG⁃modified epoxy asphalt.The feasibility of designing and screening epoxy asphalt materials by MS is verified,and a guide for toughening mechanism research of epoxy asphalt at the molecular level is provided.展开更多
Heavy metal pollution poses serious risks to the human health and the natural environment,and there is an urgent need to develop efficient heavy metal removal technologies.The adsorption strategy is one of the most fa...Heavy metal pollution poses serious risks to the human health and the natural environment,and there is an urgent need to develop efficient heavy metal removal technologies.The adsorption strategy is one of the most famous strategies for the capture of heavy metal ions.In recent years,hyper crosslinked polymers(HCPs),a kind of hyper crosslinked porous material prepared by Friedel-Crafts alkylation reaction,have attracted more and more attention because of their advantages of ultra-light framework,wide range of building monomers,easy modification and functionalization.This review focuses on the advances of HCPs in the efficient applications to the removal of heavy metal ions.The fundamentals are presented including physicochemical properties,adsorption mechanism,and preparation strategies.Subsequently,the application and influencing factors of HCPs toward heavy metal ion adsorption are discussed in detail.Furthermore,the opportunities and challenges of HCPs in this promising research field are summarized and anticipated.We are convinced that the advanced HCP-based materials will make further contributions to heavy metal removal in wastewater treatment,further paving the way of advancing researches in this field.展开更多
基金financially supported by the Natural Science Foundation of Shandong Province(Nos.ZR2021ME055,ZR2022QB170 and ZR2022MB034)the Foundation(No.GZKF202128)of State Key Laboratory of Biobased Material and Green Papermaking,Qilu University of Technology,Shandong Academy of Sciencesthe Development Program Project of Young Innovation Team of Institutions of Higher Learning in Shandong Province.
文摘It is urgent to develop high-performance polyimide(PI)films that simultaneously exhibit high transparency,exceptional thermal stability,mechanical robustness,and low dielectric to fulfil the requirements of flexible display technologies.Herein,a series of fluorinated polyimide films(FPIs)were fabricated by the condensation of 5,5′-(perfluoropropane-2,2-diyl)bis(isobenzofuran-1,3-dione)(6FDA)and the fluorinated triphenylmethane diamine monomer(EDA,MEDA and DMEDA)with heat-crosslinkable tetrafluorostyrene side groups,which was incorporated by different numbers of methyl groups pendant in the ortho position of amino groups.Subsequently,the FPI films underwent heating to produce crosslinking FPIs(C-FPIs)through the self-crosslinking of double bonds in the tetrafluorostyrene.The transparency,solvent resistance,thermal stability,mechanical robustness and dielectric properties of FPI and C-FPI films can be tuned by the number of methyl groups and crosslinking,which were deeply investigated by virtue of molecular dynamics(MD)simulations and density functional theory(DFT).As a result,all the films exhibited exceptional optically colorless and transparent,with transmittance in the visible region of 450-700 nm exceeding 79.9%,and the cut-off wavelengths(λ_(off))were nearly 350 nm.The thermal decomposition temperatures at 5% weight loss(T_(d5%))for all samples exceeded 504℃.These films exhibited a wide range of tunable tensile strength(46.5-75.1 MPa).Significantly,they showed exceptional dielectric properties with the dielectric constant of 2.3-2.5 at full frequency(10^(7)-20 Hz).This study not only highlights the relationship between the polymer molecular structure and properties,but offer insights for balancing optical transparency,heat resistance and low dielectric constant in PI films.
基金supported by the National Key Research and Development Program of China(No.2022YFB3603101)。
文摘Polyimide(PI)is widely used in high-tech fields such as microelectronics,aerospace,and national defense because of its excellent optical properties,high-and low-temperature resistance,and good dimensional stability.To achieve the desired properties of PI,the monomers 2,6-diaminopyrimidin-4-ol(DAPD)and 6-(2,3,5,6-tetrafluoro-4-vinylphenoxy)pyrimidin-2,4-diamine(DAFPD),which contains crosslinkable functional groups,were designed and synthesized successfully and copolymerized with 4,4'-oxydianiline(ODA)and 4,4-hexafluoroisopropylphthalic anhydride(6FDA).The prepared PI film(PI-3),with rigid backbones and loose packing had excellent heat resistance(Td5%=489℃)and optical properties(T450=82%).Furthermore,a crosslinked PI film(c-PI-3)with more heat-resistant(Td5%=524℃)and better mechanical properties(σ=125.46MPa),can be obtained through thermal crosslinking of tetrafluorostyrene.In addition,the changes in the properties caused by the proportion of DAFPD added during copolymerization are discussed comprehensively.This study provides a promising candidate for heat-resistant PI materials.
基金Supported by the National Natural Science Foundation of China(Nos.20771030 and 20671025)
文摘Two crosslinkable poly（p-phenyleneethynylene）s（PPEs）： poly[2,5-di（2＇-ethyl-hexyloxy）-1,4-phenylenecthynylene] with end-capped vinyl（PPE1） and poly[2,5-di（allyloxy）-1,4-phenyleneethynylene-2,5-di（2＇-ethyl-hexyloxy）-1,4-phenyleneethynylene]（PPE2） were synthesized. Via the thermal addition reactions of vinyl end groups of PPE1 and allyloxy side groups of PPE2, crosslinked polymers C-PPE1 and C-PPE2 were obtained, respectively. The two polymers were characterized by wide-angle X-ray diffraction（WXRD）, ultraviolet-visible（UV-Vis） absorption, and photoluminescence（PL）. The results indicate that in the solid state, the polymer chains of PPE1 were packed with a low degree of crystallinity because of the sterically hindered（2＇-ethyl-hexyl）oxy branched side chains, but, because of the introduction of allyloxy side chains, the polymer chains of PPE2 were packed in an order fashion with a high degree of crystallinity. Because of the high crosslinking density in C-PPE2, the formation of aggregates and excimer was hampered by the formed crosslinking network more effectively in C-PPE2 film than in C-PPE1 film.
文摘Three new functional group containing borazine derivatives, 2,4,6-tri（allylamino）borazine, 2,4,6-tri（3-ethynylanilino）borazine, and 2,4,6-tri（4-propargyl oxyanilino）borazine were synthesized by aminolysis reaction of 2,4,6-trichloroborazine ClaB3N3H3（TCB）. The new compounds were characterized by infrared （IR） spectra, nuclear magnetic resonance （NMR）, and mass spectrometry （MS）.
基金Supported by the National Key Technologies Research and Development Program of China During the 11th Five-Year Plan Period(No.2007BAE19B01)the Industrial Research Projects of the Science and Technology Plan of Ningbo City,China (No.2007B10033)
文摘Two commercial crosslinkable polyethylene insulation cable granules, designed for 110 and 35 kV voltage insulation, with similar crosslinking temperature but different melting temperature, were chosen as experimental samples for examining their linear dynamic responses during cross-linking. It has been found that the gel contents of cable compounds for 110 and 35 kV insulation are almost the same after they have been cross-linked at the same temperature, pressure and time. And the sample melts show the similar dependence of the dynamic storage modulus, G; on strain. On the other hand, the dynamic temperature ramp test and the dynamic time sweep test indicate that the samples exhibit different dynamic viscoelastic responses during their crosslinking. An expression for describing their erosslinking process was proposed via probing rheokinetics of crosslinking for the two samples.
基金support from the National Science Foundation(CHE-2213445 and 2117699)the University of North Dakota(Early Career Scholars Award).
文摘To date,more biodegradable polymers have been developed due to the growing recognition of the advantages of biodegradable and biocompatible polymers for biomedical applications.In this study,we introduce the synthesis and characterization of innovative polymers that incorporate biodegradable backbones composed of trimethylol-propane and adipic acid moieties and biocleavable side chains containing pyridyl disulfide groups.Notably,their synthesis is straightforward and catalyst-free under ambient conditions,minimizing potential toxicity and immune responses caused by catalyst residues in polymer materials.The new polymers have desired molecular weight(Mn:18.8 kDa)with a narrow dispersion(PDI:1.32)and offer complete biodegradability,biocompatibility,crosslinking capabilities,and opportunities for covalent chemical modifications.These features make them particularly suitable for use in biomedical materials and devices.Additionally,due to their unique properties,these polymers have been successfully formulated into polymeric gels and nanogels,which are biodegradable as well.Using a near-infrared fluorescent probe as a model cargo,we demonstrated the creation of a biosafe and sustainable nanogel system for agent delivery,with an average size of approximately 70 nm.In these nanogels,agent molecules are covalently attached to the scaffold,thereby avoiding uncontrolled premature release and burst release in the bloodstream and mitigating associated systemic toxicity and side effects.The nanogels can also be easily functionalized with targeting ligands for disease-specific delivery.These polymers induced minimal toxicity toward human cells and displayed excellent in vivo biocompatibility,highlighting the significant potential of their polymeric gels and nanogels for a broad spectrum of biomedical applications.
基金financially supported by the Natural Science Foundation of Jiangxi Province(No.20232ACB204002)the Jiangxi Provincial Key Laboratory of Flexible Electronics(No.20242BCC32010).
文摘The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.
基金financially supported by the National Natural Science Foundation of China(Grant 22205173)the Innovation Capability Support Program of Shaanxi(Grant 2024CX‐GXPT‐12)。
文摘The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.
文摘With the growth of global protein demand and the development of plant-based foods,pea protein,as a low-allergenic,nutritionally balanced and environmentally friendly plant protein,has shown great potential in replacing animal protein.Pea protein is mainly composed of globulin and albumin,with a protein content of 20%to 30%,and has a balanced amino acid composition,as well as being rich in minerals and dietary fiber.It also possesses good foaming,gelling,emulsifying and antioxidant functional properties.However,pea protein also has inherent defects that limit its application in the food industry.This article systematically reviews the extraction techniques,functional properties,modification methods and application fields of pea protein,and focuses on evaluating the effects of different extraction and modification strategies on protein yield and functional properties.Research shows that ultrasonic-assisted alkaline extraction can reduce solvent usage by 55%,shorten extraction time by 50%,and increase extraction rate by 12.51%;under optimized conditions,ultrafiltration membrane technology can achieve a protein purity of 91%.In terms of modification,ultrasonic treatment increases foaming capacity by 37.4%,and phenolic cross-linking increases gel strength from 3.0 kPa to 48 kPa.This article provides data support and theoretical reference for the efficient extraction and functional optimization of pea protein,and has promoting significance for its wide application in plant-based foods.
基金financial support from the National Key R&D Program of China (No.2021YFA1302604)Scientific and technological innovation project of China Academy of Chinese Medical Sciences (No.CI2021B017)China Postdoctoral Science Foundation (No.2023T160727)。
文摘RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progression of numerous diseases,making RBPs potential therapeutic targets.However,the limited tissue penetration of 254 nm UV irradiation makes it difficult to efficiently crosslink weak and dynamic RNA-protein interactions in mammal tissues.Additionally,RNA degradation in metal catalyzed click reaction further hinders the enrichment of RNA-protein complexes(RPCs).Due to these inherent limitations,globally profiling the RNA binding proteome in mammal organs has long been a challenge.Herein,we proposed a novel method,which utilized a dual crosslinking with formaldehyde and 254 nm UV irradiation,metabolic labeling and metal-free thiol-yne click reaction to enable large-scale enrichment and identification of RBPs in mouse liver,called FTYc_UV.In this method,formaldehyde is first used to crosslink the crude RNA-protein complexes(cRPCs) in situ to address the problem of poor tissue penetration of 254 nm UV irradiation.Furthermore,this method integrates metabolic labeling with a metal-free thiol-yne click reaction to achieve non-destructive RNA tagging.After specifically RNA-RBPs crosslinking by 254 nm UV irradiation in tissue lysates,formaldehyde decrosslinking is employed to remove non-specific proteins,leading to effective enrichment of RPCs from mouse liver and thereby overcoming the poor specificity of formaldehyde crosslinking.Application of FTYc_UV in mouse liver successfully identified over 1600 RBPs covering approximately 75 % of previously reported RBPs.Furthermore,420 candidate RBPs,including 151metabolic enzymes,were also obtained,demonstrating the sensitivity of FTYc_UV and the potential of this method for in-depth exploration of RNA-protein interactions in biological and clinical research.
基金financially supported by the National Key R&D Program of China(Grant No.2023YFE0108900)EU HORIZON 2021 L4DNANO(No.101086227)。
文摘Porous hydrogel sensors have attracted significant attention in fields such as smart wearables and medical monitoring due to their high sensitivity.However,existing fabrication methods typically degrade the surface smoothness of hydrogels when introducing porous structures and face significant challenges in removing fillers completely.To address these challenges,we herein introduce a novel one-step,thermosensitive spray-coating technique for the preparation of aircell hydrogel(ACH).This method leverages the rapid cooling of a thermoresponsive gelatin methacryloyl solution through atomization,enabling rapid cross-linking within seconds and air bubbles encapsulated in situ.Additionally,the transient flow of the pre-gel facilitates the repair of voids formed by ruptured surface bubbles,leading to the creation of the ACH with uniformly distributed inner air bubbles and a smooth outer surface.The mold-free fabrication method is independent of substrate surface properties,enabling the creation of a porous hydrogel film with a thickness as thin as 163 µm.Furthermore,the dual-crosslinked network endows the ACH with excellent anti-swelling properties,and the physical crosslinking between gelatin molecules allows the ACH to self-heal.The ACH exhibits excellent sensitivity in deformation sensing and can even successfully track minor external forces,which enables it to effectively complete various tasks such as facial expression recognition,pitch differentiation,and motion detection.By integrating the ACH into a sensing glove,we also demonstrate the significant potential of the ACH for applications in human-machine interaction and tactile sensing.Ultimately,the ACH sensors are also applied to motion mapping and machine tactile feedback,indicating their promising potential in human-machine interaction.
基金supported by the National Natural Science Foundation of China(Nos.22322107,22101169 and 22071144)by Shanghai Scientific and Technological Committee(No.22010500300).
文摘Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water.Here,we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions.These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants,characterized by high apparent adsorption rate constants(kobs)and maximum adsorption capacities(qmax,e).Notably,Compound NCCP-1 demonstrated a remarkable qmax,e of 459 mg/g for bisphenol A(BPA),ranking among the highest values reported for organic polymer adsorbents.In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them,primarily mediated by the hydrophobic effect.Furthermore,NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles,highlighting its potential for practical applications in water treatment.
基金supported by the grants from National Natural Science Foundation of China(Nos.22278091,22278046)Young Elite Sci-entists Sponsorship Program by CAST(No.2024QNRC0387)+2 种基金the Guangxi Natural Science Foundation of China(Nos.2025GXNSFBA069146,2023GXNSFGA026001,GKAD25069076)the Foundation(No.202403)of Tianjin Key Laboratory of Pulp&Paper(Tianjin University of Science&Technology)P.R.China,and the Foundation of Guangxi Key Laboratory of Clean Pulp&Papermaking and Pollution Control,College of Light Industry and Food Engineering,Guangxi University(No.2021KF01).
文摘With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics for continuous foot gait monitoring.Nevertheless,existing biomass-based TENG often faces challenges of insufficient mechanical robustness and durability in practical applications,where they are prone to surface abrasion and structural fracture under continuous compression and friction,severely limiting their long-term performances.In order to address these challenges,this work proposed a multiscale crosslinking strategy,which strengthened the noncovalent interactions within the polymer by constructing multiple reinforcement networks,successfully fabricating a dual-network C-lignin-based triboelectric material(CLTM)with excellent durability and crack resistance.Among them,the optimal CLTM(PSGCL-0.2)exhibited high mechanical strength(strain 445%,tensile strength 41.56 MPa,Young's modulus 41.25 MPa,toughness 159.67 MJ/m^(3))and excellent cyclic stability(300 cycles)with versatile functionalities,including antibacterial,antioxidant,and UV-shielding properties,water stabilization(255.51 g/m^(2)/d),efficient photothermal conversion,and full recyclability.Furthermore,biomass-based TENG device assembled from PSGCL-0.2 achieved stable triboelectric output properties(102.5 V,2.9μA,and 61.3 nC),and sustainable for 2000 cycles,fast response time(68 ms),and excellent power density(325.9 mW/m^(2)),effectively converting mechanical energy into electrical energy.Especially,PSGCL 0.2 was also integrated into the wireless self-powered smart insole,successfully enabling real-time visual monitoring of plantar pressure distribution and dynamic gait.Meanwhile,combined with the machine learning algorithm,the self-powered smart insole achieved precise recognition and classification of eight different motion states with an accuracy of 98%.This study provides the feasible strategy for developing extremely stable and durable biomass-based TENG,aimed at advancing sustainable intelligent healthcare systems.
基金financially supported by the International Cooperation Program of the Ministry of Science and Technology of Hubei Province(No.2023EHA069)Shenzhen Science and Technology Program(No.JCYJ20230807143702005)the National Foreign Experts Program(No.G2022027015L)。
文摘Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the blood is crucial for the treatment of liver diseases.Hemoperfusion,which relies on adsorbents to efficiently adsorb toxins,is a widely applied procedure for the removal of blood toxins.To broaden and improve the range and performance of hemoperfusion adsorbents,we synthesized cationic hyper crosslinked polymers(HCPs)with strong affinity for bilirubin.This material exhibited outstanding adsorption performance,with a maximum adsorption capacity of 934 mg/g and a removal efficiency of 96%.Further investigation confirmed their excellent selectivity,reusability,and biocompatibility.These findings expand the potential applications of HCPs and provide insight into strategies for constructing promising hemoperfusion adsorbent materials.
文摘Conventional polyethylene(PE)fibers face limitations in large-scale industrial applications due to their poor thermal stability and inherent hydrophobicity,which restrict processing temperatures and dyeability,especially in blended fabric production.In this research,a one-step ultraviolet(UV)irradiation technology was employed to modify medium molecular weight PE fibers through simultaneous crosslinking and grafting modifications,aiming to enhance their thermal stability and hydrophilicity.The modification employed a cost-effective,UV-initiated crosslinking system consisting of benzophenone(BP)as the photoinitiator and triallyl isocyanurate(TAIC)as the cocrosslinker.Acrylic acid(AA)was selected as the grafting monomer.These modifiers were thoroughly mixed with the PE matrix in a liquid-phase environment,and the mixture was melt-spun into fibers.The resulting fibers were then subjected to UV irradiation,which triggered the crosslinking and grafting reactions.The effects of the mass fraction of each component and irradiation parameters on modification efficacy were systematically investigated,followed by a comprehensive characterization of the modified PE fibers.The modified PE fibers achieved optimal thermal stability under the following conditions:2.0%mass fractions for both BP and TAIC,a UV irradiation intensity of 2000 mW/cm^(2),and an equivalent irradiation time of 60 s.This synergistic modification approach enables the fibers to maintain superior morphological integrity and mechanical performance when exposed to elevated temperatures ranging from 130 to 150℃.Meanwhile,an AA grafting mass fraction of 2.0%maximizes hydrophilicity with minimal impact on other properties,as evidenced by a dramatic reduction in the water contact angle(WCA)from 105.0°(hydrophobic)to 48.4°(hydrophilic).These improvements confirm the effectiveness of the modification strategy in synergistically enhancing both thermal stability and hydrophilicity of PE fibers.
基金the financial support from the National Natural Science Foundation of China (No. 52072390)the National High-Level Talents Special Support Program (Leading Talent of Technological Innovation)+2 种基金the China Postdoctoral Science Foundation (No. 2023M743648)the Young Scientists Fund of the National Natural Science Foundation of China (No. 52302330)the support from the Shanghai Emperor of Cleaning Hi-Tech Co.,LTD
文摘In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.
基金supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)Discovery Grant(No.RGPIN-2020-04559)the Canada Foundation for Innovation John R.Evans Leaders Fund(JELF).
文摘Rapid and accurate visible-light photopolymerization is essential for advancing bioprinted engineered tissues.In this study,we developed a novel three-component photoinitiator system for visible light-induced crosslinking of gelatin methacryloyl(GelMA)hydrogels,designed to improve polymerization kinetics,mechanical strength,and structural integrity.Incorporation of 2-bromoacetophenone(BAP)considerably accelerated photopolymerization,with reaction rates increasing alongside BAP concentration,enabling the rapid fabrication of stable hydrogel scaffolds.Printing experiments confirmed that BAP promoted fast crosslinking of GelMA bioinks under visible light,reducing printing time while preserving high-resolution structural features.Additionally,the incorporation of BAP induced microscale structural transformations in the hydrogels during hydration,as evidenced by scanning electron microscopy imaging and swelling analyses.This unique property enabled the fabrication of multilayer constructs exhibiting time-dependent deformation,demonstrating four-dimensional(4 D)printing ca pabilities.Moreover,biocompatibility evaluations revealed that cells maintained high viability in BAP-containing hydrogels.Overall,the BAP-based photoinitiator system offers a promising strategy for high-speed,high-resolution bioprinting,combining enhanced mechanical performance,reduced fabrication time,and dynamic structural adaptability-features that make it highly suitable for advanced biofabrication and tissue engineering applications.
基金supported by the National Research Foundation(NRF)of Korea,funded by the Korean Government(MSIT)(Grant No.RS-2023-00240043).
文摘As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.
基金The Major Science and Technology Project of Nan⁃jing(No.202209012)the Postgraduate Research and Practice Innova⁃tion Program of Jiangsu Province(No.KYCX22⁃0277).
文摘Polyethylene glycol(PEG)with different chains was used to modify epoxy asphalt.Molecular models of PEG⁃modified epoxy asphalt were developed using molecu⁃lar simulations(MS).The thermodynamic and mechanical properties of PEG⁃modified epoxy asphalt were analyzed,and its toughening mechanisms were explored.A method based on the Dijkstra algorithm was proposed to evaluate ep⁃oxy asphalt crosslinked networks.The results show that the introduction of PEG chains into epoxy asphalt can lower the glass transition temperature and enhance its toughness be⁃cause of the extended length of the PEG chains,which can in⁃crease the free volume and improve the mobility of the epoxy resin in the epoxy asphalt.The crosslinked network quantita⁃tive evaluation method based on the Dijkstra algorithm can ef⁃fectively evaluate the distribution of epoxy asphalt crosslink⁃ing bonds,providing further explanation of the toughening mechanism of PEG⁃modified epoxy asphalt.The feasibility of designing and screening epoxy asphalt materials by MS is verified,and a guide for toughening mechanism research of epoxy asphalt at the molecular level is provided.
基金supported by Innovation Platform(Base)and Talent Special Project,Jilin Provincial Science&Technology Department,China(No.20230508033RC)。
文摘Heavy metal pollution poses serious risks to the human health and the natural environment,and there is an urgent need to develop efficient heavy metal removal technologies.The adsorption strategy is one of the most famous strategies for the capture of heavy metal ions.In recent years,hyper crosslinked polymers(HCPs),a kind of hyper crosslinked porous material prepared by Friedel-Crafts alkylation reaction,have attracted more and more attention because of their advantages of ultra-light framework,wide range of building monomers,easy modification and functionalization.This review focuses on the advances of HCPs in the efficient applications to the removal of heavy metal ions.The fundamentals are presented including physicochemical properties,adsorption mechanism,and preparation strategies.Subsequently,the application and influencing factors of HCPs toward heavy metal ion adsorption are discussed in detail.Furthermore,the opportunities and challenges of HCPs in this promising research field are summarized and anticipated.We are convinced that the advanced HCP-based materials will make further contributions to heavy metal removal in wastewater treatment,further paving the way of advancing researches in this field.
