Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors c...Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors consume less power,but lack the capability to resolve static stimuli.Here,we address this issue by utilizing the unique polarization chemistry of conjugated polymers for the first time and propose a new type of bioinspired,passive,and bio-friendly tactile sensors for resolving both static and dynamic stimuli.Specifically,to emulate the polarization process of natural sensory cells,conjugated polymers(including poly(3,4-ethylenedioxythiophen e):poly(styrenesulfonate),polyaniline,or polypyrrole)are controllably polarized into two opposite states to create artificial potential differences.The controllable and reversible polarization process of the conjugated polymers is fully in situ characterized.Then,a micro-structured ionic electrolyte is employed to imitate the natural ion channels and to encode external touch stimulations into the variation in potential difference outputs.Compared with the currently existing tactile sensing devices,the developed tactile sensors feature distinct characteristics including fully organic composition,high sensitivity(up to 773 mV N^(−1)),ultralow power consumption(nW),as well as superior bio-friendliness.As demonstrations,both single point tactile perception(surface texture perception and material property perception)and two-dimensional tactile recognitions(shape or profile perception)with high accuracy are successfully realized using self-defined machine learning algorithms.This tactile sensing concept innovation based on the polarization chemistry of conjugated polymers opens up a new path to create robotic tactile sensors and prosthetic electronic skins.展开更多
Machine learning(ML)has emerged as a powerful tool for predicting polymer properties,including glass transition temperature(Tg),which is a critical factor influencing polymer applications.In this study,a dataset of po...Machine learning(ML)has emerged as a powerful tool for predicting polymer properties,including glass transition temperature(Tg),which is a critical factor influencing polymer applications.In this study,a dataset of polymer structures and their Tg values were created and represented as adjacency matrices based on molecular graph theory.Four key structural descriptors,flexibility,side chain occupancy length,polarity,and hydrogen bonding capacity,were extracted and used as inputs for ML models:Extra Trees(ET),Random Forest(RF),Gaussian Process Regression(GPR),and Gradient Boosting(GB).Among these,ET and GPR achieved the highest predictive performance,with R2 values of 0.97,and mean absolute errors(MAE)of approximately 7–7.5 K.The use of these extracted features significantly improved the prediction accuracy compared to previous studies.Feature importance analysis revealed that flexibility had the strongest influence on Tg,followed by side-chain occupancy length,hydrogen bonding,and polarity.This work demonstrates the potential of data-driven approaches in polymer science,providing a fast and reliable method for Tg prediction that does not require experimental inputs.展开更多
Tumor blockade therapy inhibits tumor progression by cutting off essential supplies of nutrients,oxygen,and biomolecules from the surrounding microenvironments.Inspired by natural processes,tumor biomineralization has...Tumor blockade therapy inhibits tumor progression by cutting off essential supplies of nutrients,oxygen,and biomolecules from the surrounding microenvironments.Inspired by natural processes,tumor biomineralization has evolved due to its biocompatibility,self-reinforcing capability,and penetrationindependent mechanism.However,the selective induction of tumor biomineralization using synthetic tools presents a significant challenge.Herein,a metabolic glycoengineering-assistant tumor biomineralization strategy was developed.Specifically,the azido group(N_(3))was introduced onto the cytomembrane by incubating tumor cells with glycose analog Ac4ManNAz.In addition,a bisphosphonate-containing polymer,dibenzocyclooctyne-poly(ethylene glycol)-alendronate(DBCO-PEG-ALN,DBPA)was synthesized,which attached to the tumor cell surface via"click chemistry"reaction between DBCO and N_(3).Subsequently,the bisphosphonate group on the cell surface chelated with positively charged ions in the microenvironments,triggering a consecutive process of biomineralization.This physical barrier significantly reduced tumor cell viability and mobility in a calcium ion concentration-dependent manner,suggesting its potential as an effective anti-tumor strategy for in vivo applications.展开更多
Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundame...Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.展开更多
The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous de...The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous development of such recyclable polymers.Herein,PPDOPLLA-PU copolymers were synthesized from poly(p-dioxanone)-diol(PPDO-diol)and poly(L-lactide)-diol(PLLA-diol)by chain extension reaction.The chemical structures and microphase structures of PPDO-PLLA-PU were characterized,and their crystalline properties,mechanical properties,and degradation behaviors were further investigated.Significantly,the distribution of PLLA phase in the copolymer matrix showed a rod-like microstructure with a slight orientation,despite the thermodynamic incompatibility of PPDO and PLLA segments.Moreover,on the basis of this microphase separation,PPDO spherulites can crystallize using the interface of the two phases as nucleation sites.Accordingly,the combined effect of above two contributes to the enhanced mechanical properties.In addition,PPDO-PLLA-PU copolymers have good processability and recyclability,making them valuable for a wide range of applications.展开更多
Integrating multiple modalities of cancer therapies for synergistic and enhanced therapeutic efficacy remains challenging.Herein,flash nanoprecipitation(FNP),a kinetically driven process,was employed to expedite the c...Integrating multiple modalities of cancer therapies for synergistic and enhanced therapeutic efficacy remains challenging.Herein,flash nanoprecipitation(FNP),a kinetically driven process,was employed to expedite the coordination reaction time required for nano-encapsulate components with completely opposite physiochemical properties including sorafenib(SRF),hemoglobin(Hb),chlorin e6(Ce6),and indocyanine green(ICG)into a multi-component HSCI nanomedicine.Hydrophilic components Hb and ICG interact to form hydrophobic ICG-Hb complexes under electrostatic and hydrophobic interactions.This process facilitates the characteristic time of nucleation(τ_(nucleation))to match the characteristic mixing time(τ_(mix))of the FNP process,resulting in the formulation of kinetically stable nanomedicine,overcoming the long equilibrium times and instability issues associated with thermodynamic assembly.Importantly,pH-responsive structure is also easily but effectively integrated in nanomedicine during this kinetically driven formulation to manipulate its structures.In the acidic tumor microenvironment(TME),the pH-stimulated morphology transformation of HSCI nanomedicine boosts its reactive oxygen species(ROS)generation efficiency and photothermal efficacy,endowing it with better antitumor suppression.In vitro and in vivo experiments reveal that the HSCI nanomedicine offers a synergistic therapeutic effect and stronger tumor suppression compared with single therapies.These results open a new window for developing strategies for multimodal combinatory cancer therapies.展开更多
Low dielectric constant(low-k)materials are critical for advanced packaging in high-density microelectronic devices and high-frequency communication technologies.Ladder polysiloxanes,which are characterized by their u...Low dielectric constant(low-k)materials are critical for advanced packaging in high-density microelectronic devices and high-frequency communication technologies.Ladder polysiloxanes,which are characterized by their unique double-chain structure and intrinsic microporosity,offer remarkable advantages in terms of thermal stability,oxidation resistance,and dielectric performance.However,structural defects in ladder polysiloxanes,such as cage-like and irregular oligomers,and their effects on dielectric properties remain underexplored.In this study,a series of ladder-like polysiloxanes(X-TMS)with diverse side groups weresynthesized via a one-step base-catalyzed method.The influence of the benzocyclobutene(BCB)side groups on the formation of regular ladder structures was systematically investigated.Notably,BCB incorporation disrupted the structural regularity,favoring the formation of cage-like and irregular topologies,which were extensively characterized using 29silicon nuclear magnetic resonance spectroscopy(^(29)Si-NMR),Fourier transform infrared spectroscopy(FTIR),gel permeation chromatography(GPC),and X-ray diffraction(XRD).These structural defects were beneficial for improving the hydrophobicity and thermal stability.Copolymerization of X-TMS with commercial DVS-BCB resins further enhanced the mechanical properties,with the elastic modulus increasing from 3.6 GPa to 4.4 GPa and water absorption reduced from 0.33 wt%to 0.06 wt%.This study establishes a clear correlation between topological structures and material properties.These findings not only advance the understanding of the structure-property relationships in ladder polysiloxanes but also provide a novel approach for designing high-performance interlayer dielectric materials for next-generation microelectronics.展开更多
Intrinsic stretchability is a promising attribute of polymer organic solar cells(OSCs).However,rigid molecular blocks typically exhibit poor tensile properties,rendering polymers vulnerable to mechanical stress.In thi...Intrinsic stretchability is a promising attribute of polymer organic solar cells(OSCs).However,rigid molecular blocks typically exhibit poor tensile properties,rendering polymers vulnerable to mechanical stress.In this study,we introduce a different approach utilizing all-small-molecule donors and acceptors to fabricate stretchable OSCs.An elastomer,styrene-b-ethylene-butylene-styrene(SEBS),was embedded to modulate film crystallization and stretchability.SEBS effectively confines the growth process of donors and acceptors,leading to enhancement of the crystallization quality,thus contributing to enhanced device efficiencies.Meanwhile,SEBS can absorb and release mechanical stress during stretching,thereby preventing mechanical degradation of donors and acceptors.The mechanical properties of the OSCs were significantly improved by the incorporation of SEBS.Notably,the crack-onset strain increased from 1.03% to 5.99% with SEBS embedding.These findings present a straightforward strategy for achieving stretchable OSCs using all small molecules,offering a different perspective for realizing stretchable devices.展开更多
Effective thermal transport across solid-solid interfaces which is essential in thermal interface materials(TIMs),necessitates both optimal thixotropy and high thermal conductivity.The role of filler surface modificat...Effective thermal transport across solid-solid interfaces which is essential in thermal interface materials(TIMs),necessitates both optimal thixotropy and high thermal conductivity.The role of filler surface modification,a fundamental aspect of TIM fabrication,in the influence of these properties is not fully understood.This study employs the use of a silane coupling agent(SCA)to modify alumina,integrating experimental approaches with molecular dynamics simulations,to elucidate the interface effects on thixotropy and thermal conductivity in polydimethylsiloxane(PDMS)-based TIMs.Our findings reveal that the variations of SCAs modify both interface binding energy and transition layer thickness.The interface binding energy restricts macromolecular segmental relaxation near the interface,hindering desirable thixotropy and bond line thickness.On the contrary,the thickness of the transition layer at the interface positively influences thermal conductivity,facilitating the transport of phonons between the polymer and filler.Consequently,selecting an optimal SCA allows a balance between traditionally conflicting goals of high thermal conductivity and minimal bond line thickness,achieving an impressively low interface thermal resistance of just 2.45-4.29 K·mm^(2)·W^(-1)at275.8 kPa.展开更多
Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using ...Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer(PS-PEO-PS),resulting in a porous structure with good interconnections,which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes(GPEs).It has been demonstrated that post-cross-linking of the precursor membranes increa ses the rigidity of the nanofibers,which allows the polymer film to be dimensionally sta ble up to 260℃while maintaining superior electrochemical properties.The obtained cross-linked GPEs(CGPEs)showed high ionic conductivity up to 4.53×10^(-3)S·cm^(-1).With the CGPE-25,the assembled Li/LiFeP04 half cells exhibited good rate capability and maintained a capacity of 99.4%and a coulombic efficiency of99.3%at 0.1 C.These results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance,particularly useful for Lithium-ion battery applications that require high-temperature usage.展开更多
The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly co...The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.展开更多
The quest for scalable integration of monolayer graphene into functional composites confronts the bottleneck of high-fidelity transfer onto substrates,crucial for unlocking graphene’s full potential in advanced appli...The quest for scalable integration of monolayer graphene into functional composites confronts the bottleneck of high-fidelity transfer onto substrates,crucial for unlocking graphene’s full potential in advanced applications.Addressing this,our research introduces the camphor-assisted transfer(CAT)method,a novel approach that surmounts common issues of residue and structural deformation endemic to existing techniques.Grounded in the sublimation dynamics of camphor,the CAT method achieves a clean,contiguous transfer of centimeter-scale monolayer graphene onto an array of polymer films,including ultra-thin polyethylene films.The resultant ultrathin graphene-polyethylene(gPE)films,characterized by their exceptional transparency and conductivity,reveal the CAT method’s unique ability to preserve the pristine quality of graphene,underscoring its practicality for preparing flexible transparent electrodes by monolayer graphene.In-depth mechanism investigation into the camphor sublimation during CAT has led to a pivotal realization:the porosity of the target polymer substrate is a determinant in achieving high-quality graphene transfer.Ensuring that camphor sublimates initially from the polymer side is crucial to prevent the formation of wrinkles or delamination of graphene.By extensive examination of CAT on a spectrum of commonly used polymer films,including PE,PP,PTFE,PI and PET,we have confirmed this important conclusion.This discovery offers crucial guidance for fabricating monolayer graphene-polymer composite films using methods akin to CAT,underscoring the significance of substrate selection in the transfer process.展开更多
The preparation of high-performance thermal conductive composites containing liquid metals(LM)has attracted significant attention.However,the stable dispersion of LM within polymer solution and effective property cont...The preparation of high-performance thermal conductive composites containing liquid metals(LM)has attracted significant attention.However,the stable dispersion of LM within polymer solution and effective property contribution of liquid metals remains significant challenges that need to be overcome.Inspired by the properties of the dendritic structure of the tree root system in grasping the soil,“shear-induced precipitation-interfacial reset-reprotonation”processing strategy is proposed to prepare nanocomposites based on aramid micron fibers(AMFs)with hierarchical dendritic structure.Thanks to the combination of van der Waals force provided by hierarchical dendritic structure,electrostatic interaction between AMFs and LM,coordinative bonding of―NH to LM,together with interfacial re-setting and multi-step protonation,several features can be achieved through such strategy:conducive to the local filler network construction,improvement of interfacial interaction,improvement of the stability of filler dispersion in the solvent,and enhancement of mechanical and thermal properties of the films.The resulting AMFsp H=4/LM films demonstrate a thermal conductivity of 10.98 W·m^(-1)·K^(-1)at 70%filler content,improvement of 126.8%compared to ANFs/LM film;while maintaining a strength of~85.88 MPa,improvement of 77%compared to AMFs/LM film.They also possess insulation properties,enable heat dissipation for high power electronics.This work provides an effective strategy for the preparation of high performance polymer composites containing liquid metal.展开更多
Organic photovoltaics(OPVs)need to overcome limitations such as insufficient thermal stability to be commercialized.The reported approaches to improve stability either rely on the development of new materials or on ta...Organic photovoltaics(OPVs)need to overcome limitations such as insufficient thermal stability to be commercialized.The reported approaches to improve stability either rely on the development of new materials or on tailoring the donor/acceptor morphology,however,exhibiting limited applicability.Therefore,it is timely to develop an easy method to enhance thermal stability without having to develop new donor/acceptor materials or donor–acceptor compatibilizers,or by introducing another third component.Herein,a unique approach is presented,based on constructing a polymer fiber rigid network with a high glass transition temperature(T_(g))to impede the movement of acceptor and donor molecules,to immobilize the active layer morphology,and thereby to improve thermal stability.A high-T_(g) one-dimensional aramid nanofiber(ANF)is utilized for network construction.Inverted OPVs with ANF network yield superior thermal stability compared to the ANF-free counterpart.The ANF network-incorporated active layer demonstrates significantly more stable morphology than the ANF-free counterpart,thereby leaving fundamental processes such as charge separation,transport,and collection,determining the device efficiency,largely unaltered.This strategy is also successfully applied to other photovoltaic systems.The strategy of incorporating a polymer fiber rigid network with high T_(g) offers a distinct perspective addressing the challenge of thermal instability with simplicity and universality.展开更多
Electromagnetic interference(EMI)shielding materials with superior shielding efficiency and low-reflection properties hold promising potential for utilization across electronic components,precision instruments,and fif...Electromagnetic interference(EMI)shielding materials with superior shielding efficiency and low-reflection properties hold promising potential for utilization across electronic components,precision instruments,and fifth-generation communication equipment.In this study,multistage microcellular waterborne polyurethane(WPU)composites were constructed via gradient induction,layer-by-layer casting,and supercritical carbon dioxide foaming.The gradient-structured WPU/ironcobalt loaded reduced graphene oxide(FeCo@rGO)foam serves as an impedance-matched absorption layer,while the highly conductive WPU/silver loaded glass microspheres(Ag@GM)layer is employed as a reflection layer.Thanks to the incorporation of an asymmetric structure,as well as the introduction of gradient and porous configurations,the composite foam demonstrates excellent conductivity,outstanding EMI SE(74.9 dB),and minimal reflection characteristics(35.28%)in 8.2-12.4 GHz,implying that more than 99.99999%of electromagnetic(EM)waves were blocked and only 35.28%were reflected to the external environment.Interestingly,the reflectivity of the composite foam is reduced to 0.41%at 10.88 GHz due to the resonance for incident and reflected EM waves.Beyond that,the composite foam is characterized by low density(0.47 g/cm^(3))and great stability of EMI shielding properties.This work offers a viable approach for craft-ing lightweight,highly shielding,and minimally reflective EMI shielding composites.展开更多
In the present work,by virtue of the synergistic and independent effects of Janus structure,an asymmetric nickel-chain/multiwall carbon nanotube/polyimide(Ni/MWCNTs/PI)composite foam with absorption-dominated electrom...In the present work,by virtue of the synergistic and independent effects of Janus structure,an asymmetric nickel-chain/multiwall carbon nanotube/polyimide(Ni/MWCNTs/PI)composite foam with absorption-dominated electromagnetic interference(EMI)shielding and thermal insulation performances was successfully fabricated through an ordered casting and directional freeze-drying strategy.Water-soluble polyamic acid(PAA)was chosen to match the oriented freeze-drying method to acquire oriented pores,and the thermal imidization process from PAA to PI exactly eliminated the interface of the multilayered structure.By controlling the electro-magnetic gradient and propagation path of the incident microwaves in the MWCNT/PI and Ni/PI layers,the PI composite foam exhibited an efficient EMI SE of 55.8 dB in the X-band with extremely low reflection characteristics(R=0.22).The asymmetric conductive net-work also greatly preserved the thermal insulation properties of PI.The thermal conductivity(TC)of the Ni/MWCNT/PI composite foam was as low as 0.032 W/(m K).In addition,owing to the elimination of MWCNT/PI and Ni/PI interfaces during the thermal imidization process,the composite foam showed satisfactory compressive strength.The fabricated PI composite foam could provide reliable electromagnetic protection in complex applications and withstand high temperatures,which has great potential in cuttingedge applications such as advanced aircraft.展开更多
Bioactive molecules have shown great promise for effectively regulating various bone formation processes,rendering them attractive therapeutics for bone regeneration.However,the widespread application of bioactive mol...Bioactive molecules have shown great promise for effectively regulating various bone formation processes,rendering them attractive therapeutics for bone regeneration.However,the widespread application of bioactive molecules is limited by their low accumulation and short half-lives in vivo.Hydrogels have emerged as ideal carriers to address these challenges,offering the potential to prolong retention times at lesion sites,extend half-lives in vivo and mitigate side effects,avoid burst release,and promote adsorption under physiological conditions.This review systematically summarizes the recent advances in the development of bioactive molecule-loaded hydrogels for bone regeneration,encompassing applications in cranial defect repair,femoral defect repair,periodontal bone regeneration,and bone regeneration with underlying diseases.Additionally,this review discusses the current strategies aimed at improving the release profiles of bioactive molecules through stimuli-responsive delivery,carrier-assisted delivery,and sequential delivery.Finally,this review elucidates the existing challenges and future directions of hydrogel encapsulated bioactive molecules in the field of bone regeneration.展开更多
To address the increasing demand for massive data storage and processing,brain-inspired neuromorphic comput-ing systems based on artificial synaptic devices have been actively developed in recent years.Among the vario...To address the increasing demand for massive data storage and processing,brain-inspired neuromorphic comput-ing systems based on artificial synaptic devices have been actively developed in recent years.Among the various materials inves-tigated for the fabrication of synaptic devices,silicon carbide(SiC)has emerged as a preferred choices due to its high electron mobility,superior thermal conductivity,and excellent thermal stability,which exhibits promising potential for neuromorphic applications in harsh environments.In this review,the recent progress in SiC-based synaptic devices is summarized.Firstly,an in-depth discussion is conducted regarding the categories,working mechanisms,and structural designs of these devices.Subse-quently,several application scenarios for SiC-based synaptic devices are presented.Finally,a few perspectives and directions for their future development are outlined.展开更多
All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional l...All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.展开更多
Poly(phthalazinone ether sulfone ketone)(PPESK)is a new-generation high-performance thermoplastic resin that exhibits excellent thermal stability and mechanical properties.However,its damage and failure mechanisms und...Poly(phthalazinone ether sulfone ketone)(PPESK)is a new-generation high-performance thermoplastic resin that exhibits excellent thermal stability and mechanical properties.However,its damage and failure mechanisms under high-temperature and high-strain-rate coupling conditions remain unclear,significantly limiting the engineering applications of PPESK-based composites in extreme environments such as aerospace.To address this issue,in this study,a temperature-controlled split Hopkinson pressure bar experimental platform was developed for dynamic tensile/compressive loading scenarios.Combined with scanning electron microscopy and molecular dynamics simulations,the thermomechanical behavior and failure mechanisms of PPESK were systematically investigated over the temperature range of 293-473 K.The study revealed a novel"dynamic hysteresis brittle behavior"and its underlying"segmental activation±response lag antagonistic mechanism".The results showed that the strain-rate-induced response lag of polymer chain segments significantly weakened the viscous dissipation capacity activated by thermal energy at elevated temperatures.Although high-strain-rate conditions led to notable enhancement in the dynamic strength of the material(with an increase of 8%-233%,reaching 130%-330%at elevated temperatures),the fracture surface morphology tended to become smoother,and brittle fracture characteristics became more pronounced.Based on these findings,a temperature±strain rate hysteresis antagonistic function was constructed,which effectively captured the competitive relationship between temperature-driven relaxation behavior and strain-rateinduced hysteresis in thermoplastic resins.A multiscale damage evolution constitutive model with temperature±rate coupling was subsequently established and numerically implemented via the VUMAT user subroutine.This study not only unveils the nonlinear damage mechanisms of PPESK under combined service temperatures and dynamic/static loading conditions,but also provides a strong theoretical foundation and engineering guidance for the constitutive modeling and parametric design of thermoplastic resin-based materials.展开更多
基金financially supported by the Sichuan Science and Technology Program(2022YFS0025 and 2024YFFK0133)supported by the“Fundamental Research Funds for the Central Universities of China.”。
文摘Tactile perception plays a vital role for the human body and is also highly desired for smart prosthesis and advanced robots.Compared to active sensing devices,passive piezoelectric and triboelectric tactile sensors consume less power,but lack the capability to resolve static stimuli.Here,we address this issue by utilizing the unique polarization chemistry of conjugated polymers for the first time and propose a new type of bioinspired,passive,and bio-friendly tactile sensors for resolving both static and dynamic stimuli.Specifically,to emulate the polarization process of natural sensory cells,conjugated polymers(including poly(3,4-ethylenedioxythiophen e):poly(styrenesulfonate),polyaniline,or polypyrrole)are controllably polarized into two opposite states to create artificial potential differences.The controllable and reversible polarization process of the conjugated polymers is fully in situ characterized.Then,a micro-structured ionic electrolyte is employed to imitate the natural ion channels and to encode external touch stimulations into the variation in potential difference outputs.Compared with the currently existing tactile sensing devices,the developed tactile sensors feature distinct characteristics including fully organic composition,high sensitivity(up to 773 mV N^(−1)),ultralow power consumption(nW),as well as superior bio-friendliness.As demonstrations,both single point tactile perception(surface texture perception and material property perception)and two-dimensional tactile recognitions(shape or profile perception)with high accuracy are successfully realized using self-defined machine learning algorithms.This tactile sensing concept innovation based on the polarization chemistry of conjugated polymers opens up a new path to create robotic tactile sensors and prosthetic electronic skins.
文摘Machine learning(ML)has emerged as a powerful tool for predicting polymer properties,including glass transition temperature(Tg),which is a critical factor influencing polymer applications.In this study,a dataset of polymer structures and their Tg values were created and represented as adjacency matrices based on molecular graph theory.Four key structural descriptors,flexibility,side chain occupancy length,polarity,and hydrogen bonding capacity,were extracted and used as inputs for ML models:Extra Trees(ET),Random Forest(RF),Gaussian Process Regression(GPR),and Gradient Boosting(GB).Among these,ET and GPR achieved the highest predictive performance,with R2 values of 0.97,and mean absolute errors(MAE)of approximately 7–7.5 K.The use of these extracted features significantly improved the prediction accuracy compared to previous studies.Feature importance analysis revealed that flexibility had the strongest influence on Tg,followed by side-chain occupancy length,hydrogen bonding,and polarity.This work demonstrates the potential of data-driven approaches in polymer science,providing a fast and reliable method for Tg prediction that does not require experimental inputs.
基金supported by the National Natural Science Foundation of China(Nos.U23A20591 and 52273158)the Science and Technology Development Program of Jilin Province(Nos.20240101002JJ and 20210504001GH).
文摘Tumor blockade therapy inhibits tumor progression by cutting off essential supplies of nutrients,oxygen,and biomolecules from the surrounding microenvironments.Inspired by natural processes,tumor biomineralization has evolved due to its biocompatibility,self-reinforcing capability,and penetrationindependent mechanism.However,the selective induction of tumor biomineralization using synthetic tools presents a significant challenge.Herein,a metabolic glycoengineering-assistant tumor biomineralization strategy was developed.Specifically,the azido group(N_(3))was introduced onto the cytomembrane by incubating tumor cells with glycose analog Ac4ManNAz.In addition,a bisphosphonate-containing polymer,dibenzocyclooctyne-poly(ethylene glycol)-alendronate(DBCO-PEG-ALN,DBPA)was synthesized,which attached to the tumor cell surface via"click chemistry"reaction between DBCO and N_(3).Subsequently,the bisphosphonate group on the cell surface chelated with positively charged ions in the microenvironments,triggering a consecutive process of biomineralization.This physical barrier significantly reduced tumor cell viability and mobility in a calcium ion concentration-dependent manner,suggesting its potential as an effective anti-tumor strategy for in vivo applications.
基金financial support from the National Natural Science Foundation of China(52203123)the Sichuan Science and Technology Program(2023NSFSC0991)+2 种基金the State Key Laboratory of Polymer Materials Engineering(sklpme 2023-1-05 and sklpme 2024-2-04)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘Solvation structures fundamentally control the ion-transport dynamics and mechanical properties of polymer electrolytes.However,there is a lack of strategies to rationally regulate the solvation structures and fundamental understanding on how they control the electrochemical performances.Herein,by harnessing the electrostatic adsorption of one-dimensional nanofiller(i.e.,surface-charged halloysite nanotubes,d-HNTs),we successfully fabricate a high-performance polymer nanocomposite electrolyte enabled by strong surface adsorption,referred as adsorption-state polymer electrolyte(ASPE).This ASPE shows fast ion transport(0.71±0.05 mS cm^(-1)at room temperature),high mechanical strength and toughness(10.3±0.05 MPa;15.73 MJ m^(-3)),improved lithium-ion transference number,and long cycle life with lithium metal anode,in comparison with the sample without the d-HNT adsorption effect.To fundamentally understand these high performances,an anion-rich asymmetric solvent structure model is further proposed and evidenced by both experiments and simulation studies.Results show that the electrostatic adsorption among the d-HNT,ionic liquid electrolyte,and polymer chain generates a nano filler-supported fast ion-conduction pathway with asymmetric Li+-coordination microenvironment.Meanwhile,the anion-rich asymmetric solvent structure model of ASPE also generates a fast de-solvation and anion-derived stable solid-electrolyte interphase for lithium metal anode.The high performance and understanding of the mechanism for ASPE provide a promising path to develop advanced polymer electrolytes.
基金financially supported by the National Key R&D Program of China(No.2021YFB3801901)the National Natural Science Foundation of China(Nos.52403138 and U19A2095)+1 种基金Institutional Research Fund from Sichuan University(No.2020SCUNL205)Fundamental Research Funds for the Central Universities,and 111 Project(No.B20001)。
文摘The development of degradable and chemically recyclable polymers is a promising strategy to address pressing environmental and resource-related challenges.Despite significant progress,there is a need for continuous development of such recyclable polymers.Herein,PPDOPLLA-PU copolymers were synthesized from poly(p-dioxanone)-diol(PPDO-diol)and poly(L-lactide)-diol(PLLA-diol)by chain extension reaction.The chemical structures and microphase structures of PPDO-PLLA-PU were characterized,and their crystalline properties,mechanical properties,and degradation behaviors were further investigated.Significantly,the distribution of PLLA phase in the copolymer matrix showed a rod-like microstructure with a slight orientation,despite the thermodynamic incompatibility of PPDO and PLLA segments.Moreover,on the basis of this microphase separation,PPDO spherulites can crystallize using the interface of the two phases as nucleation sites.Accordingly,the combined effect of above two contributes to the enhanced mechanical properties.In addition,PPDO-PLLA-PU copolymers have good processability and recyclability,making them valuable for a wide range of applications.
基金supported by the National Natural Science Foundation of China(22378126)National Key Research and Development Program of the International scientific and technological innovation cooperation project among governments(2021YFE0100400)Shanghai Science and Technology Innovation Action Plan(22501100500).
文摘Integrating multiple modalities of cancer therapies for synergistic and enhanced therapeutic efficacy remains challenging.Herein,flash nanoprecipitation(FNP),a kinetically driven process,was employed to expedite the coordination reaction time required for nano-encapsulate components with completely opposite physiochemical properties including sorafenib(SRF),hemoglobin(Hb),chlorin e6(Ce6),and indocyanine green(ICG)into a multi-component HSCI nanomedicine.Hydrophilic components Hb and ICG interact to form hydrophobic ICG-Hb complexes under electrostatic and hydrophobic interactions.This process facilitates the characteristic time of nucleation(τ_(nucleation))to match the characteristic mixing time(τ_(mix))of the FNP process,resulting in the formulation of kinetically stable nanomedicine,overcoming the long equilibrium times and instability issues associated with thermodynamic assembly.Importantly,pH-responsive structure is also easily but effectively integrated in nanomedicine during this kinetically driven formulation to manipulate its structures.In the acidic tumor microenvironment(TME),the pH-stimulated morphology transformation of HSCI nanomedicine boosts its reactive oxygen species(ROS)generation efficiency and photothermal efficacy,endowing it with better antitumor suppression.In vitro and in vivo experiments reveal that the HSCI nanomedicine offers a synergistic therapeutic effect and stronger tumor suppression compared with single therapies.These results open a new window for developing strategies for multimodal combinatory cancer therapies.
基金financially supported by the National Natural Science Foundation of China(Nos.52373316,22075298,and52373020)the Beijing Municipal Natural Science Foundation(No.2212053)。
文摘Low dielectric constant(low-k)materials are critical for advanced packaging in high-density microelectronic devices and high-frequency communication technologies.Ladder polysiloxanes,which are characterized by their unique double-chain structure and intrinsic microporosity,offer remarkable advantages in terms of thermal stability,oxidation resistance,and dielectric performance.However,structural defects in ladder polysiloxanes,such as cage-like and irregular oligomers,and their effects on dielectric properties remain underexplored.In this study,a series of ladder-like polysiloxanes(X-TMS)with diverse side groups weresynthesized via a one-step base-catalyzed method.The influence of the benzocyclobutene(BCB)side groups on the formation of regular ladder structures was systematically investigated.Notably,BCB incorporation disrupted the structural regularity,favoring the formation of cage-like and irregular topologies,which were extensively characterized using 29silicon nuclear magnetic resonance spectroscopy(^(29)Si-NMR),Fourier transform infrared spectroscopy(FTIR),gel permeation chromatography(GPC),and X-ray diffraction(XRD).These structural defects were beneficial for improving the hydrophobicity and thermal stability.Copolymerization of X-TMS with commercial DVS-BCB resins further enhanced the mechanical properties,with the elastic modulus increasing from 3.6 GPa to 4.4 GPa and water absorption reduced from 0.33 wt%to 0.06 wt%.This study establishes a clear correlation between topological structures and material properties.These findings not only advance the understanding of the structure-property relationships in ladder polysiloxanes but also provide a novel approach for designing high-performance interlayer dielectric materials for next-generation microelectronics.
基金financially supported by the National Natural Science Foundation of China(Nos.52303239 and 51933001)Natural Science Foundation of Shandong Province(Nos.ZR2022QB141 and 2023HWYQ-087).
文摘Intrinsic stretchability is a promising attribute of polymer organic solar cells(OSCs).However,rigid molecular blocks typically exhibit poor tensile properties,rendering polymers vulnerable to mechanical stress.In this study,we introduce a different approach utilizing all-small-molecule donors and acceptors to fabricate stretchable OSCs.An elastomer,styrene-b-ethylene-butylene-styrene(SEBS),was embedded to modulate film crystallization and stretchability.SEBS effectively confines the growth process of donors and acceptors,leading to enhancement of the crystallization quality,thus contributing to enhanced device efficiencies.Meanwhile,SEBS can absorb and release mechanical stress during stretching,thereby preventing mechanical degradation of donors and acceptors.The mechanical properties of the OSCs were significantly improved by the incorporation of SEBS.Notably,the crack-onset strain increased from 1.03% to 5.99% with SEBS embedding.These findings present a straightforward strategy for achieving stretchable OSCs using all small molecules,offering a different perspective for realizing stretchable devices.
基金financially supported by the National Natural Science Foundation of China(Nos.52373042 and 52103091)the National Key Research and Development Project of China(No.2022YFB3806900)the International Visiting Program for Excellent Young Scholars of SCU。
文摘Effective thermal transport across solid-solid interfaces which is essential in thermal interface materials(TIMs),necessitates both optimal thixotropy and high thermal conductivity.The role of filler surface modification,a fundamental aspect of TIM fabrication,in the influence of these properties is not fully understood.This study employs the use of a silane coupling agent(SCA)to modify alumina,integrating experimental approaches with molecular dynamics simulations,to elucidate the interface effects on thixotropy and thermal conductivity in polydimethylsiloxane(PDMS)-based TIMs.Our findings reveal that the variations of SCAs modify both interface binding energy and transition layer thickness.The interface binding energy restricts macromolecular segmental relaxation near the interface,hindering desirable thixotropy and bond line thickness.On the contrary,the thickness of the transition layer at the interface positively influences thermal conductivity,facilitating the transport of phonons between the polymer and filler.Consequently,selecting an optimal SCA allows a balance between traditionally conflicting goals of high thermal conductivity and minimal bond line thickness,achieving an impressively low interface thermal resistance of just 2.45-4.29 K·mm^(2)·W^(-1)at275.8 kPa.
基金financially supported by the National Natural Science Foundation of China(Nos.21574087 and 51973128)Science and Technology Department of Sichuan Province(Nos.2019YJ0128 and 2019YFG0277)supports from the Fundamental Research Funds for the Central Universities。
文摘Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer(PS-PEO-PS),resulting in a porous structure with good interconnections,which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes(GPEs).It has been demonstrated that post-cross-linking of the precursor membranes increa ses the rigidity of the nanofibers,which allows the polymer film to be dimensionally sta ble up to 260℃while maintaining superior electrochemical properties.The obtained cross-linked GPEs(CGPEs)showed high ionic conductivity up to 4.53×10^(-3)S·cm^(-1).With the CGPE-25,the assembled Li/LiFeP04 half cells exhibited good rate capability and maintained a capacity of 99.4%and a coulombic efficiency of99.3%at 0.1 C.These results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance,particularly useful for Lithium-ion battery applications that require high-temperature usage.
基金financially supported by the National Natural Science Foundation of China(No.51933007,No.52373047,No.52302106)the Sichuan Youth Science and Technology Innovation Research Team Project(No.2022JDTD0012)+2 种基金the Program for Featured Directions of Engineering Multidisciplines of Sichuan University(No.2020SCUNG203)the Natural Science Foundation of Sichuan Province(No.2023NSFSC0418)the Program for State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-10)。
文摘The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered architectures.Polypyrrole(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world applicability.Here,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass loading.The preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer electrode.In agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based supercapacitors.This work highlights a promising route to preparing high energy density energy storage modules for real-world applications.
基金This work was financially supported by the National Natural Science Foundation of China(NSFC)(Nos.52233002 and 52103042)the Natural Science Foundation of Sichuan Province(No.24NSFSC6554)the State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-3-09).
文摘The quest for scalable integration of monolayer graphene into functional composites confronts the bottleneck of high-fidelity transfer onto substrates,crucial for unlocking graphene’s full potential in advanced applications.Addressing this,our research introduces the camphor-assisted transfer(CAT)method,a novel approach that surmounts common issues of residue and structural deformation endemic to existing techniques.Grounded in the sublimation dynamics of camphor,the CAT method achieves a clean,contiguous transfer of centimeter-scale monolayer graphene onto an array of polymer films,including ultra-thin polyethylene films.The resultant ultrathin graphene-polyethylene(gPE)films,characterized by their exceptional transparency and conductivity,reveal the CAT method’s unique ability to preserve the pristine quality of graphene,underscoring its practicality for preparing flexible transparent electrodes by monolayer graphene.In-depth mechanism investigation into the camphor sublimation during CAT has led to a pivotal realization:the porosity of the target polymer substrate is a determinant in achieving high-quality graphene transfer.Ensuring that camphor sublimates initially from the polymer side is crucial to prevent the formation of wrinkles or delamination of graphene.By extensive examination of CAT on a spectrum of commonly used polymer films,including PE,PP,PTFE,PI and PET,we have confirmed this important conclusion.This discovery offers crucial guidance for fabricating monolayer graphene-polymer composite films using methods akin to CAT,underscoring the significance of substrate selection in the transfer process.
基金financially supported by the National Key Research&Development Plan(No.2022YFA1205200)。
文摘The preparation of high-performance thermal conductive composites containing liquid metals(LM)has attracted significant attention.However,the stable dispersion of LM within polymer solution and effective property contribution of liquid metals remains significant challenges that need to be overcome.Inspired by the properties of the dendritic structure of the tree root system in grasping the soil,“shear-induced precipitation-interfacial reset-reprotonation”processing strategy is proposed to prepare nanocomposites based on aramid micron fibers(AMFs)with hierarchical dendritic structure.Thanks to the combination of van der Waals force provided by hierarchical dendritic structure,electrostatic interaction between AMFs and LM,coordinative bonding of―NH to LM,together with interfacial re-setting and multi-step protonation,several features can be achieved through such strategy:conducive to the local filler network construction,improvement of interfacial interaction,improvement of the stability of filler dispersion in the solvent,and enhancement of mechanical and thermal properties of the films.The resulting AMFsp H=4/LM films demonstrate a thermal conductivity of 10.98 W·m^(-1)·K^(-1)at 70%filler content,improvement of 126.8%compared to ANFs/LM film;while maintaining a strength of~85.88 MPa,improvement of 77%compared to AMFs/LM film.They also possess insulation properties,enable heat dissipation for high power electronics.This work provides an effective strategy for the preparation of high performance polymer composites containing liquid metal.
基金financially supported by the Sichuan Science and Technology Program(Grant Nos.2023YFH0087,2023YFH0085,2023YFH0086,and 2023NSFSC0990)State Key Laboratory of Polymer Materials Engineering(Grant Nos.sklpme2022-3-02 and sklpme2023-2-11)+1 种基金Tibet Foreign Experts Program(Grant No.2022wz002)supported by the King Abdullah University of Science and Technology(KAUST)Office of Research Administration(ORA)under Award Nos.OSR-CARF/CCF-3079 and OSR-2021-CRG10-4701.
文摘Organic photovoltaics(OPVs)need to overcome limitations such as insufficient thermal stability to be commercialized.The reported approaches to improve stability either rely on the development of new materials or on tailoring the donor/acceptor morphology,however,exhibiting limited applicability.Therefore,it is timely to develop an easy method to enhance thermal stability without having to develop new donor/acceptor materials or donor–acceptor compatibilizers,or by introducing another third component.Herein,a unique approach is presented,based on constructing a polymer fiber rigid network with a high glass transition temperature(T_(g))to impede the movement of acceptor and donor molecules,to immobilize the active layer morphology,and thereby to improve thermal stability.A high-T_(g) one-dimensional aramid nanofiber(ANF)is utilized for network construction.Inverted OPVs with ANF network yield superior thermal stability compared to the ANF-free counterpart.The ANF network-incorporated active layer demonstrates significantly more stable morphology than the ANF-free counterpart,thereby leaving fundamental processes such as charge separation,transport,and collection,determining the device efficiency,largely unaltered.This strategy is also successfully applied to other photovoltaic systems.The strategy of incorporating a polymer fiber rigid network with high T_(g) offers a distinct perspective addressing the challenge of thermal instability with simplicity and universality.
基金supported by the Natural Science Foundation of Anhui Province(No.2308085QE146 and 2208085ME116)the National Natural Science Foundation of China(No.52173039)+1 种基金the Natural Science Foundation of Jiangsu Province(No.BK20210894)the Anhui Provincial Universities Outstanding Youth Research Project(No.2023AH020018).
文摘Electromagnetic interference(EMI)shielding materials with superior shielding efficiency and low-reflection properties hold promising potential for utilization across electronic components,precision instruments,and fifth-generation communication equipment.In this study,multistage microcellular waterborne polyurethane(WPU)composites were constructed via gradient induction,layer-by-layer casting,and supercritical carbon dioxide foaming.The gradient-structured WPU/ironcobalt loaded reduced graphene oxide(FeCo@rGO)foam serves as an impedance-matched absorption layer,while the highly conductive WPU/silver loaded glass microspheres(Ag@GM)layer is employed as a reflection layer.Thanks to the incorporation of an asymmetric structure,as well as the introduction of gradient and porous configurations,the composite foam demonstrates excellent conductivity,outstanding EMI SE(74.9 dB),and minimal reflection characteristics(35.28%)in 8.2-12.4 GHz,implying that more than 99.99999%of electromagnetic(EM)waves were blocked and only 35.28%were reflected to the external environment.Interestingly,the reflectivity of the composite foam is reduced to 0.41%at 10.88 GHz due to the resonance for incident and reflected EM waves.Beyond that,the composite foam is characterized by low density(0.47 g/cm^(3))and great stability of EMI shielding properties.This work offers a viable approach for craft-ing lightweight,highly shielding,and minimally reflective EMI shielding composites.
基金supported by the Natural Science Foundation of Shanxi Province(Nos.20210302123015 and 20210302123035)the Opening Project of State Key Laboratory of Polymer Materials Engineering(Sichuan University)(No.sklpme2022-4-06)the Open Foundation of China-Belarus Belt and Road Joint Laboratory on Electromagnetic Environment Effect(No.ZBKF2022030301).
文摘In the present work,by virtue of the synergistic and independent effects of Janus structure,an asymmetric nickel-chain/multiwall carbon nanotube/polyimide(Ni/MWCNTs/PI)composite foam with absorption-dominated electromagnetic interference(EMI)shielding and thermal insulation performances was successfully fabricated through an ordered casting and directional freeze-drying strategy.Water-soluble polyamic acid(PAA)was chosen to match the oriented freeze-drying method to acquire oriented pores,and the thermal imidization process from PAA to PI exactly eliminated the interface of the multilayered structure.By controlling the electro-magnetic gradient and propagation path of the incident microwaves in the MWCNT/PI and Ni/PI layers,the PI composite foam exhibited an efficient EMI SE of 55.8 dB in the X-band with extremely low reflection characteristics(R=0.22).The asymmetric conductive net-work also greatly preserved the thermal insulation properties of PI.The thermal conductivity(TC)of the Ni/MWCNT/PI composite foam was as low as 0.032 W/(m K).In addition,owing to the elimination of MWCNT/PI and Ni/PI interfaces during the thermal imidization process,the composite foam showed satisfactory compressive strength.The fabricated PI composite foam could provide reliable electromagnetic protection in complex applications and withstand high temperatures,which has great potential in cuttingedge applications such as advanced aircraft.
基金supported by the National Natural Science Foundation of China(51925304)Natural Science Foundation of Sichuan Province(2024NSFSC1023)Medical Research Program of Sichuan Province(Q23015).
文摘Bioactive molecules have shown great promise for effectively regulating various bone formation processes,rendering them attractive therapeutics for bone regeneration.However,the widespread application of bioactive molecules is limited by their low accumulation and short half-lives in vivo.Hydrogels have emerged as ideal carriers to address these challenges,offering the potential to prolong retention times at lesion sites,extend half-lives in vivo and mitigate side effects,avoid burst release,and promote adsorption under physiological conditions.This review systematically summarizes the recent advances in the development of bioactive molecule-loaded hydrogels for bone regeneration,encompassing applications in cranial defect repair,femoral defect repair,periodontal bone regeneration,and bone regeneration with underlying diseases.Additionally,this review discusses the current strategies aimed at improving the release profiles of bioactive molecules through stimuli-responsive delivery,carrier-assisted delivery,and sequential delivery.Finally,this review elucidates the existing challenges and future directions of hydrogel encapsulated bioactive molecules in the field of bone regeneration.
基金supported by the Natural Science Foundation of Zhejiang Province(Grant No.LQ24F040007)the National Natural Science Foundation of China(Grant No.U22A2075)the Opening Project of State Key Laboratory of Polymer Materials Engineering(Sichuan University)(Grant No.sklpme2024-1-21).
文摘To address the increasing demand for massive data storage and processing,brain-inspired neuromorphic comput-ing systems based on artificial synaptic devices have been actively developed in recent years.Among the various materials inves-tigated for the fabrication of synaptic devices,silicon carbide(SiC)has emerged as a preferred choices due to its high electron mobility,superior thermal conductivity,and excellent thermal stability,which exhibits promising potential for neuromorphic applications in harsh environments.In this review,the recent progress in SiC-based synaptic devices is summarized.Firstly,an in-depth discussion is conducted regarding the categories,working mechanisms,and structural designs of these devices.Subse-quently,several application scenarios for SiC-based synaptic devices are presented.Finally,a few perspectives and directions for their future development are outlined.
基金National Natural Science Foundation of China (52203123)Sichuan Science and Technology Program (2023NSFSC0991)+2 种基金State Key Laboratory of Polymer Materials Engineering (sklpme-2023-1-05 and sklpme-2024-2-04)Fundamental Research Funds for the Central UniversitiesThis research was also partially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
基金supported by National Key Research and Development Program"Advanced Structures and Composite Materials"Special Project[Grant No.2024YFB3712800]the Fundamental Research Funds for the Central Universities[Grant No.DUT22-LAB605]Liaoning Province's"Unveiling the List and Leading the Way"Science and Technology Research and Development Special Project[Grant No.2022JH1/10400043]。
文摘Poly(phthalazinone ether sulfone ketone)(PPESK)is a new-generation high-performance thermoplastic resin that exhibits excellent thermal stability and mechanical properties.However,its damage and failure mechanisms under high-temperature and high-strain-rate coupling conditions remain unclear,significantly limiting the engineering applications of PPESK-based composites in extreme environments such as aerospace.To address this issue,in this study,a temperature-controlled split Hopkinson pressure bar experimental platform was developed for dynamic tensile/compressive loading scenarios.Combined with scanning electron microscopy and molecular dynamics simulations,the thermomechanical behavior and failure mechanisms of PPESK were systematically investigated over the temperature range of 293-473 K.The study revealed a novel"dynamic hysteresis brittle behavior"and its underlying"segmental activation±response lag antagonistic mechanism".The results showed that the strain-rate-induced response lag of polymer chain segments significantly weakened the viscous dissipation capacity activated by thermal energy at elevated temperatures.Although high-strain-rate conditions led to notable enhancement in the dynamic strength of the material(with an increase of 8%-233%,reaching 130%-330%at elevated temperatures),the fracture surface morphology tended to become smoother,and brittle fracture characteristics became more pronounced.Based on these findings,a temperature±strain rate hysteresis antagonistic function was constructed,which effectively captured the competitive relationship between temperature-driven relaxation behavior and strain-rateinduced hysteresis in thermoplastic resins.A multiscale damage evolution constitutive model with temperature±rate coupling was subsequently established and numerically implemented via the VUMAT user subroutine.This study not only unveils the nonlinear damage mechanisms of PPESK under combined service temperatures and dynamic/static loading conditions,but also provides a strong theoretical foundation and engineering guidance for the constitutive modeling and parametric design of thermoplastic resin-based materials.
