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
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
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
Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is importan...Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is important to identify readers from cell samples so as to understand biological roles of lysine methylation.Generally,readers bind methyllysine via aromatic cages that contain tryptophan,tyrosine and phenylalanine,that offer a unique motif for selective crosslinking.We recently reported a site-selective tryptophan crosslinking strategy based on dimethylsulfonium that mimics dimethyllysine to crosslink tryptophan in aromatic cages of readers.Since tyrosine is a key residue for binding affinity to methyllysine,especially some readers that do not contain tryptophan residues in the binding pocket.Here we developed strategies of site-selective crosslinking to tyrosine.Ultraviolet(UV)source was applied to excite tyrosine at neutral pH or phenoxide at basic p H,and subsequent single-electron transfer(SET)from Tyr*to sulfonium inside the binding pocket enables selective crosslinking.In consequence,methyllysine readers with tyrosine-containing aromatic cages could be selectively crosslinked by site-specific sulfonium peptide probes.In addition,we expanded substrates from aromatic cages to tyrosine residues of proximate contact with sulfonium probes.The pair of LgBiT and SmBiT exhibited orthogonal crosslinking in complicated cell samples.As a result,we may expand sulfonium tools to target local tyrosine in future investigations.展开更多
High-temperature performance of energy storage dielectric polymers is desired for many electronics and electrical applications,but the trade-off between energy density and temperature stability remains fundamentally c...High-temperature performance of energy storage dielectric polymers is desired for many electronics and electrical applications,but the trade-off between energy density and temperature stability remains fundamentally challenging.Here,we report a general material design strategy to enhance energy storage performance at high temperatures by crosslinking a polar polymer and a high glass-transition temperature polymer as a crosslinked binary blend.Such crosslinked binary polymers display a temperature-insensitive and high energy density behavior of about6.2~8.5 J cm^(-3) up to 110℃,showing a significant enhancement in thermal resistant properties and consequently outperforming most of the other ferroelectric polymers.Further microstructural investigations reveal that the improved thermal stability stems from the confinement effect on conformational motion of the crosslinking network,which is evidenced by the increased rigid amorphous fraction and steady intermolecular distance of amorphous regions from temperature-dependent X-ray diffraction results.Our findings provide a general and straightforward strategy to attain temperature-stable,high-energy-density polymer-based dielectrics for energy storage capacitors.展开更多
Organisms are capable of self-growth through the integration of the nutrients provided by the external environment.This process slows down when they grow.In this study,we mimicked this self-regulated growth via a simp...Organisms are capable of self-growth through the integration of the nutrients provided by the external environment.This process slows down when they grow.In this study,we mimicked this self-regulated growth via a simple swelling-polymerization strategy in which the stretching polymer chains in the original networks provide entropic elasticity to restrict growth in high growth cycles.Using typical covalently crosslinked polymers,such as acrylamide-based hydrogels and HBA-based elastomers,as examples,we demonstrate that the crosslinked polymers can absorb polymerizable compounds through a swelling-polymerization process to expand their sizes,but the growth extent becomes smaller with increasing growth cycle until reaching a plateau.In addition to their size,these materials become stiffer and exhibit less swelling ability in solvents.Our work not only provides a new growing mode to tune the properties of crosslinked polymers but also discloses the underlying mechanism of crosslinked polymers in multi-cyclic swelling conditions.展开更多
Stretchability is a crucial property of flexible all-in-one supercapacitors.This work reports a novel hydrogel electrolyte,polyacrylamidedivinylbenzene-Li2SO4(PAM-DVB-Li)synthesized by using a strategy of combining hy...Stretchability is a crucial property of flexible all-in-one supercapacitors.This work reports a novel hydrogel electrolyte,polyacrylamidedivinylbenzene-Li2SO4(PAM-DVB-Li)synthesized by using a strategy of combining hydrophobic nodes and hydrophilic networks as well as a method of dispersing hydrophobic DVB crosslinker to acrylamide monomer/Li2SO4 aqueous solution by micelles and followedγ-radiation induced polymerization and crosslinking.The resultant PAM-DVB-Li hydrogel electrolyte possesses excellent mechanical properties with 5627±241%stretchability and high ionic conductivity of 53±3 mS cm^(-1).By in situ polymerization of conducting polyaniline(PANI)on the PAM-DVB-Li hydrogel electrolyte,a novel all-in-one supercapacitor,PAM-DVB-Li/PANI,with highly integrated structure is prepared further.Benefiting from the excellent properties of hydrogel electrolyte and the all-in-one structure,the device exhibits a high specific capacitance of 469 mF cm^(-2) at 0.5 mA cm^(-2),good cyclic stability,safety,and deformation damage resistance.More importantly,the device demonstrates a superior tensile resistance(working normally under no more than 300%strain,capacitance stability in 1000 cycles of 1000%stretching and 10 cycles of 3000%stretching)far beyond that of other all-in-one supercapacitors.This work proposes a novel strategy to construct tensile-resistant all-in-one flexible supercapacitors that can be used as an energy storage device for stretchable electronic devices.展开更多
With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycli...With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycling of renewable and environmentally friendly bio-based polymers as alternatives to petroleum based polymers have become hot topics in research and industrial fields.Biomass has been used as a raw material to design and synthesize closed-loop recyclable polymers,which is of great significance in addressing the waste of resources and negative impact on the environment in the traditional polymer preparation process.This review summarized recent advances in the design,synthesis,and properties of closed-loop recyclable bio-based polymers,focusing on the sustainability and recyclability of bio-based materials,followed by a brief discussion of the potential applications of closed-loop recyclable bio-based polymers in emerging applications such as 3D printing and friction electric nanogenerators.In addition,perspectives and recommendations for future research on closedloop recyclable bio-based polymers were presented.展开更多
Dielectric films are critical components in the fabrication of capacitors. However, their reliance on petroleum-derived polymers presents significant environmental challenges. To address this issue, we report on a hig...Dielectric films are critical components in the fabrication of capacitors. However, their reliance on petroleum-derived polymers presents significant environmental challenges. To address this issue, we report on a high-performance biomass-based dielectric material derived from vanillin(VA), a renewable aromatic aldehyde. Vanillin was first esterified to synthesize vanillin methacrylate(VMA), which was then copolymerized with methyl methacrylate(MMA) via free-radical polymerization to yield P(VMA-MMA). By crosslinking the aldehyde groups in VMA with the amine groups in the polyether amine D400(PEA), we fabricated a series of P(VMA-MMA)@PEA dielectric films with precisely tunable crosslinking densities. The unique molecular structure of vanillin, featuring both a benzene ring and an ester group, facilitates strong δ-π interactions and dipolar polarization, synergistically enhancing energy storage density while minimizing dielectric loss. At an optimal P(VMA-MMA) ratio of 1:10and 80% theoretical crosslinking degree, the dielectric constant reaches 3.4 at 10^(-3 )Hz, while the breakdown strength reaches 670.2 MV/m. Furthermore, the film exhibits an energy storage density of 7.1 J/cm3at 500 MV/m while maintaining a charge-discharge efficiency exceeding 90%.This study demonstrates a green and reliable strategy for designing biomass-based dielectric materials and opens new avenues for the development of eco-friendly energy-storage technologies.展开更多
This work develops a protein imprinted nanosphere with varied recognition specificity for bovine serum albumin(BSA)and lysozyme(Lyz)under different UV light through a gradient dual crosslinked imprinting strategy(i.e....This work develops a protein imprinted nanosphere with varied recognition specificity for bovine serum albumin(BSA)and lysozyme(Lyz)under different UV light through a gradient dual crosslinked imprinting strategy(i.e.,covalent crosslinking and dynamic reversible crosslinking).The imprinting cavities are initially constructed using irreversible covalent crosslinking to specifically recognize BSA,and then the coumarin residues in the imprinting cavities are crosslinked under 365 nm UV light to further imprint Lyz,because Lyz has smaller size than BSA.Since the photo-crosslinking of coumarin is a reversible reaction,the imprinting cavities of Lyz can be de-crosslinked under 254 nm UV light and restore the imprinting cavities of BSA.Moreover,the N-isopropyl acrylamide(NIPAM)and pyrrolidine residues copolymerized in the polymeric surface of the nanospheres are temperature-and p H-responsive respectively.Therefore,the protein rebinding and release behaviors of the nanospheres are controlled by external temperature and p H.As a result,the materials can selectively separate BSA from real bovine whole blood and Lyz from egg white under different UV light.This study may provide a new strategy for construction of protein imprinted materials with tunable specificity for different proteins.展开更多
Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and ...Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and stretchability that align with biological tissues.Specifically,their materials should be capable of elastic strain up to 50–80%,while the devices themselves must maintain electric stability under strains that accommodate body movements[1].展开更多
Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsP...Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsPbI_(3)perovskite solar cells(PSCs)still lags far behind that of both organic-inorganic hybrid counterparts and the theoretical PCE limit,primarily restricted by severe fill factor(FF)and opencircuit voltage(VOC)deficits.Herein,an in-situ self-crosslinking strategy is proposed to construct high-performance inverted inorganic PSCs by incorporating acrylate monomers as additives into CsPbI_(3)perovskite precursors.During the thermal annealing process of perovskite films,acrylate monomers can form network structures by breaking the C=C groups through an in-situ polymerization reaction,mainly anchored at the grain boundaries(GBs)and on the surfaces of perovskite.Meanwhile,the C=O groups of acrylate polymers can favorably coordinate with uncoordinated Pb^(2+),thereby decreasing defect density and stabilizing the perovskite phase.Particularly,with multiple crosslinking and passivation sites,the incorporation of dipentaerythritol pentaacrylate(DPHA)can effectively improve the perovskite film quality,suppress nonradiative recombination,and block moisture erosion.Consequently,the DPHAbased PSC achieves a champion PCE of 20.05%with a record-high FF of 85.05%,both of which rank among the top in the performance of inverted CsPbI_(3)PSCs.Moreover,the unencapsulated DPHA-based device exhibits negligible hysteresis,remarkably improved long-term storage,and operational stability.This work offers a facile and useful strategy to simultaneously promote the efficiency and device stability of inverted inorganic PSCs.展开更多
Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this ...Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron reagent.Facile thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory performance.The thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of thiols.Moreover,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL materials.In addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.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
The intrinsic volume changes(about 300%)of Si anode during the lithiation/delithiation leads to the serious degradation of battery performance despite of theoretical capacity of 3579 mAh g^(-1) of Si.Herein,a three-di...The intrinsic volume changes(about 300%)of Si anode during the lithiation/delithiation leads to the serious degradation of battery performance despite of theoretical capacity of 3579 mAh g^(-1) of Si.Herein,a three-dimensional(3D)conductive polymer binder with adjustable crosslinking density has been designed by employing citric acid(CA)as a crosslinker between the carboxymethyl cellulose(CMC)and the poly(3,4-ethylenedioxythiophene)poly-(styrene-4-sulfonate)(PEDOT:PSS)to stabilize Si anode.By adjusting the crosslinking density,the binder can achieve a balance between rigidity and flexibility to adapt the volume expansion upon lithiation and reversible volume recovery after delithiation of Si.Therefore,Si/CMC-CA-PEDOT:PSS(Si/CCP)electrode demonstrates an excellent performance with high capacities of 2792.3 mAh g^(-1) at 0.5 A g^(-1) and a high area capacity above 2.6 mAh cm^(-2) under Si loading of 1.38 mg cm^(-2).The full cell Si/CCP paired with Li(Ni_(0.8)Co_(0.1)Mn_(0.1))O_(2) cathode discharges a capacity of 199.0 mAh g^(-1) with 84.3%ICE at 0.1 C and the capacity retention of 95.6%after 100 cycles.This work validates the effectiveness of 3D polymer binder and provides new insights to boost the performance of Si anode.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.
基金the support from National Natural Science Foundation of China(No.22161132006)Key R&D Program of Zhejiang(No.2024SSYS0036)Westlake University Startup。
文摘Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is important to identify readers from cell samples so as to understand biological roles of lysine methylation.Generally,readers bind methyllysine via aromatic cages that contain tryptophan,tyrosine and phenylalanine,that offer a unique motif for selective crosslinking.We recently reported a site-selective tryptophan crosslinking strategy based on dimethylsulfonium that mimics dimethyllysine to crosslink tryptophan in aromatic cages of readers.Since tyrosine is a key residue for binding affinity to methyllysine,especially some readers that do not contain tryptophan residues in the binding pocket.Here we developed strategies of site-selective crosslinking to tyrosine.Ultraviolet(UV)source was applied to excite tyrosine at neutral pH or phenoxide at basic p H,and subsequent single-electron transfer(SET)from Tyr*to sulfonium inside the binding pocket enables selective crosslinking.In consequence,methyllysine readers with tyrosine-containing aromatic cages could be selectively crosslinked by site-specific sulfonium peptide probes.In addition,we expanded substrates from aromatic cages to tyrosine residues of proximate contact with sulfonium probes.The pair of LgBiT and SmBiT exhibited orthogonal crosslinking in complicated cell samples.As a result,we may expand sulfonium tools to target local tyrosine in future investigations.
基金supported by the National Natural Science Foundation of China(Grant No.52207031)the National Key R&D Program of China(Grant No.2020YFA0710500)。
文摘High-temperature performance of energy storage dielectric polymers is desired for many electronics and electrical applications,but the trade-off between energy density and temperature stability remains fundamentally challenging.Here,we report a general material design strategy to enhance energy storage performance at high temperatures by crosslinking a polar polymer and a high glass-transition temperature polymer as a crosslinked binary blend.Such crosslinked binary polymers display a temperature-insensitive and high energy density behavior of about6.2~8.5 J cm^(-3) up to 110℃,showing a significant enhancement in thermal resistant properties and consequently outperforming most of the other ferroelectric polymers.Further microstructural investigations reveal that the improved thermal stability stems from the confinement effect on conformational motion of the crosslinking network,which is evidenced by the increased rigid amorphous fraction and steady intermolecular distance of amorphous regions from temperature-dependent X-ray diffraction results.Our findings provide a general and straightforward strategy to attain temperature-stable,high-energy-density polymer-based dielectrics for energy storage capacitors.
基金financially supported by the National Natural Science Foundation of China(Nos.52203135 and 52273206)Postdoctoral Fellowship Program of CPSF(No.GZC20230372)+4 种基金Huzhou Science and Technology Program Projects(No.2023GZ18)Zhejiang Postdoctoral Research Project(No.ZJ2023133)Science and Technology Cooperation Fund Program of Chengdu-Chinese Academy of ScienceHunan Provincial Natural Science Foundation(No.2021JJ10029)Huxiang High-level Talent Gathering Project(No.2022RC4039)。
文摘Organisms are capable of self-growth through the integration of the nutrients provided by the external environment.This process slows down when they grow.In this study,we mimicked this self-regulated growth via a simple swelling-polymerization strategy in which the stretching polymer chains in the original networks provide entropic elasticity to restrict growth in high growth cycles.Using typical covalently crosslinked polymers,such as acrylamide-based hydrogels and HBA-based elastomers,as examples,we demonstrate that the crosslinked polymers can absorb polymerizable compounds through a swelling-polymerization process to expand their sizes,but the growth extent becomes smaller with increasing growth cycle until reaching a plateau.In addition to their size,these materials become stiffer and exhibit less swelling ability in solvents.Our work not only provides a new growing mode to tune the properties of crosslinked polymers but also discloses the underlying mechanism of crosslinked polymers in multi-cyclic swelling conditions.
基金financial support from National Natural Science Foundation of China(No.12375336,11875078)。
文摘Stretchability is a crucial property of flexible all-in-one supercapacitors.This work reports a novel hydrogel electrolyte,polyacrylamidedivinylbenzene-Li2SO4(PAM-DVB-Li)synthesized by using a strategy of combining hydrophobic nodes and hydrophilic networks as well as a method of dispersing hydrophobic DVB crosslinker to acrylamide monomer/Li2SO4 aqueous solution by micelles and followedγ-radiation induced polymerization and crosslinking.The resultant PAM-DVB-Li hydrogel electrolyte possesses excellent mechanical properties with 5627±241%stretchability and high ionic conductivity of 53±3 mS cm^(-1).By in situ polymerization of conducting polyaniline(PANI)on the PAM-DVB-Li hydrogel electrolyte,a novel all-in-one supercapacitor,PAM-DVB-Li/PANI,with highly integrated structure is prepared further.Benefiting from the excellent properties of hydrogel electrolyte and the all-in-one structure,the device exhibits a high specific capacitance of 469 mF cm^(-2) at 0.5 mA cm^(-2),good cyclic stability,safety,and deformation damage resistance.More importantly,the device demonstrates a superior tensile resistance(working normally under no more than 300%strain,capacitance stability in 1000 cycles of 1000%stretching and 10 cycles of 3000%stretching)far beyond that of other all-in-one supercapacitors.This work proposes a novel strategy to construct tensile-resistant all-in-one flexible supercapacitors that can be used as an energy storage device for stretchable electronic devices.
基金Natural Science Foundation of China(Grant Nos.32471815 and 32401528)Natural Science Foundation of Jiangsu Province of China(Grant Nos.BK20241745 and BK20240294).
文摘With the increasing consumption of non renewable resources such as oil,the traditional polymer manufacturing industry that relies on fossil resources is facing unprecedented challenges.The design,synthesis,and recycling of renewable and environmentally friendly bio-based polymers as alternatives to petroleum based polymers have become hot topics in research and industrial fields.Biomass has been used as a raw material to design and synthesize closed-loop recyclable polymers,which is of great significance in addressing the waste of resources and negative impact on the environment in the traditional polymer preparation process.This review summarized recent advances in the design,synthesis,and properties of closed-loop recyclable bio-based polymers,focusing on the sustainability and recyclability of bio-based materials,followed by a brief discussion of the potential applications of closed-loop recyclable bio-based polymers in emerging applications such as 3D printing and friction electric nanogenerators.In addition,perspectives and recommendations for future research on closedloop recyclable bio-based polymers were presented.
基金supported by the National Natural Science Foundation of China(No.52203011).
文摘Dielectric films are critical components in the fabrication of capacitors. However, their reliance on petroleum-derived polymers presents significant environmental challenges. To address this issue, we report on a high-performance biomass-based dielectric material derived from vanillin(VA), a renewable aromatic aldehyde. Vanillin was first esterified to synthesize vanillin methacrylate(VMA), which was then copolymerized with methyl methacrylate(MMA) via free-radical polymerization to yield P(VMA-MMA). By crosslinking the aldehyde groups in VMA with the amine groups in the polyether amine D400(PEA), we fabricated a series of P(VMA-MMA)@PEA dielectric films with precisely tunable crosslinking densities. The unique molecular structure of vanillin, featuring both a benzene ring and an ester group, facilitates strong δ-π interactions and dipolar polarization, synergistically enhancing energy storage density while minimizing dielectric loss. At an optimal P(VMA-MMA) ratio of 1:10and 80% theoretical crosslinking degree, the dielectric constant reaches 3.4 at 10^(-3 )Hz, while the breakdown strength reaches 670.2 MV/m. Furthermore, the film exhibits an energy storage density of 7.1 J/cm3at 500 MV/m while maintaining a charge-discharge efficiency exceeding 90%.This study demonstrates a green and reliable strategy for designing biomass-based dielectric materials and opens new avenues for the development of eco-friendly energy-storage technologies.
基金financial support from the National Natural Science Foundation of China(No.22275148)National Key R&D Program of China(No.2018YFB1900201)for Qiuyu Zhang+2 种基金the National Natural Science Foundation of China(No.22271232)Fundamental Research Funds for the Central Universities(No.D5000230114)for Shixin Fathe Fundamental Research Funds for the Central Universities(No.D5000220339)for Qing Liu。
文摘This work develops a protein imprinted nanosphere with varied recognition specificity for bovine serum albumin(BSA)and lysozyme(Lyz)under different UV light through a gradient dual crosslinked imprinting strategy(i.e.,covalent crosslinking and dynamic reversible crosslinking).The imprinting cavities are initially constructed using irreversible covalent crosslinking to specifically recognize BSA,and then the coumarin residues in the imprinting cavities are crosslinked under 365 nm UV light to further imprint Lyz,because Lyz has smaller size than BSA.Since the photo-crosslinking of coumarin is a reversible reaction,the imprinting cavities of Lyz can be de-crosslinked under 254 nm UV light and restore the imprinting cavities of BSA.Moreover,the N-isopropyl acrylamide(NIPAM)and pyrrolidine residues copolymerized in the polymeric surface of the nanospheres are temperature-and p H-responsive respectively.Therefore,the protein rebinding and release behaviors of the nanospheres are controlled by external temperature and p H.As a result,the materials can selectively separate BSA from real bovine whole blood and Lyz from egg white under different UV light.This study may provide a new strategy for construction of protein imprinted materials with tunable specificity for different proteins.
基金supported by generous grants from the Natural Science Foundation of Zhejiang Province(LR24E030003)Zhejiang Province Qianjiang Talent Program(ZJ-QJRC-2020-32).
文摘Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and stretchability that align with biological tissues.Specifically,their materials should be capable of elastic strain up to 50–80%,while the devices themselves must maintain electric stability under strains that accommodate body movements[1].
基金supported by the Program for Science and Technology Innovation Team in Zhejiang(Grant No.2021R01004)the Natural Science Foundation of Ningbo City(No.2023J119)+1 种基金the Ningbo Youth Science and Technology Innovation Leading Talent Project(2023QL029)K.C.Wong Magna Fund in Ningbo University,China。
文摘Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsPbI_(3)perovskite solar cells(PSCs)still lags far behind that of both organic-inorganic hybrid counterparts and the theoretical PCE limit,primarily restricted by severe fill factor(FF)and opencircuit voltage(VOC)deficits.Herein,an in-situ self-crosslinking strategy is proposed to construct high-performance inverted inorganic PSCs by incorporating acrylate monomers as additives into CsPbI_(3)perovskite precursors.During the thermal annealing process of perovskite films,acrylate monomers can form network structures by breaking the C=C groups through an in-situ polymerization reaction,mainly anchored at the grain boundaries(GBs)and on the surfaces of perovskite.Meanwhile,the C=O groups of acrylate polymers can favorably coordinate with uncoordinated Pb^(2+),thereby decreasing defect density and stabilizing the perovskite phase.Particularly,with multiple crosslinking and passivation sites,the incorporation of dipentaerythritol pentaacrylate(DPHA)can effectively improve the perovskite film quality,suppress nonradiative recombination,and block moisture erosion.Consequently,the DPHAbased PSC achieves a champion PCE of 20.05%with a record-high FF of 85.05%,both of which rank among the top in the performance of inverted CsPbI_(3)PSCs.Moreover,the unencapsulated DPHA-based device exhibits negligible hysteresis,remarkably improved long-term storage,and operational stability.This work offers a facile and useful strategy to simultaneously promote the efficiency and device stability of inverted inorganic PSCs.
基金financially supported by the National Natural Science Foundation of China(No.22171182)Sichuan Tianfu Emei Plan.
文摘Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical properties.In this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron reagent.Facile thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory performance.The thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of thiols.Moreover,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL materials.In addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.
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Financial support by the NSFC no. 52371224, 51972156, and 51872131
文摘The intrinsic volume changes(about 300%)of Si anode during the lithiation/delithiation leads to the serious degradation of battery performance despite of theoretical capacity of 3579 mAh g^(-1) of Si.Herein,a three-dimensional(3D)conductive polymer binder with adjustable crosslinking density has been designed by employing citric acid(CA)as a crosslinker between the carboxymethyl cellulose(CMC)and the poly(3,4-ethylenedioxythiophene)poly-(styrene-4-sulfonate)(PEDOT:PSS)to stabilize Si anode.By adjusting the crosslinking density,the binder can achieve a balance between rigidity and flexibility to adapt the volume expansion upon lithiation and reversible volume recovery after delithiation of Si.Therefore,Si/CMC-CA-PEDOT:PSS(Si/CCP)electrode demonstrates an excellent performance with high capacities of 2792.3 mAh g^(-1) at 0.5 A g^(-1) and a high area capacity above 2.6 mAh cm^(-2) under Si loading of 1.38 mg cm^(-2).The full cell Si/CCP paired with Li(Ni_(0.8)Co_(0.1)Mn_(0.1))O_(2) cathode discharges a capacity of 199.0 mAh g^(-1) with 84.3%ICE at 0.1 C and the capacity retention of 95.6%after 100 cycles.This work validates the effectiveness of 3D polymer binder and provides new insights to boost the performance of Si anode.
