Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has ...Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has been difficult to strike a balance between the robustness and flexibility of coatings constructed by a single cross-linked network design.To overcome the conundrum,this innovative approach effectively combines two distinct cross-linked networks with unique functions,thus overcoming the challenge.Through a tightly interwoven structure comprised of added crosslinking sites,the coating achieves improved liquid repellency(WCA>100°,OSA<10°),increased durability(withstands 2,000 cycles of cotton wear),enhanced flexibility(endures 5,000 cycles of bending with a bending radius of 1 mm),and maintains high transparency(over 98%in the range of 410 nm to 760 nm).Additionally,the coating with remarkable adhesion can be applied to multiple substrates,enabling large-scale preparation and easy cycling coating,thus expanding its potential applications.The architecture of this fluoride-free dual cross-linked network not only advances liquid-repellent surfaces but also provides valuable insights for the development of eco-friendly materials in the future.展开更多
Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was pr...Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.展开更多
Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked pol...Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.展开更多
To achieve smart and personalized medicine, the development of hydrogel dressings with sensing properties and biotherapeutic properties that can act as a sensor to monitor of human health in real-time while speeding u...To achieve smart and personalized medicine, the development of hydrogel dressings with sensing properties and biotherapeutic properties that can act as a sensor to monitor of human health in real-time while speeding up wound healing face great challenge. In the present study, a biocompatible dual-network composite hydrogel(DNCGel) sensor was obtained via a simple process. The dual network hydrogel is constructed by the interpenetration of a flexible network formed of poly(vinyl alcohol)(PVA) physical cross-linked by repeated freeze-thawing and a rigid network of iron-chelated xanthan gum(XG) impregnated with Fe^(3+) interpenetration. The pure PVA/XG hydrogels were chelated with ferric ions by immersion to improve the gel strength(compressive modulus and tensile modulus can reach up to 0.62 MPa and0.079 MPa, respectively), conductivity(conductivity values ranging from 9 × 10^(-4) S/cm to 1 × 10^(-3)S/cm)and bacterial inhibition properties(up to 98.56%). Subsequently, the effects of the ratio of PVA and XG and the immersion time of Fe^(3+) on the hydrogels were investigated, and DNGel3 was given the most priority on a comprehensive consideration. It was demonstrated that the DNCGel exhibit good biocompatibility in vitro, effectively facilitate wound healing in vivo(up to 97.8% healing rate) under electrical stimulation, and monitors human movement in real time. This work provides a novel avenue to explore multifunctional intelligent hydrogels that hold great promise in biomedical fields such as smart wound dressings and flexible wearable sensors.展开更多
The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycli...The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycling performance and extending service life of LIBs.Here,we report a novel cross-linked network SHSPE(PDDP)containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and nonflammability.The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28°C without external stimulation.Furthermore,the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide(EMIMTFSI)improves the ionic conductivity(1.13×10^(−4)S cm^(−1)at 28°C)and non-flammability of PDDP.The assembled Li/PDDP/LiFePO_(4)cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g^(−1)after 300 cycles at 0.2 C.More importantly,the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.展开更多
Efficient polymeric room-temperature phosphorescence(PRTP)with excellent processability and flexibility is highly desirable but still faces formidable challenge.Herein,a general strategy is developed for efficient PRT...Efficient polymeric room-temperature phosphorescence(PRTP)with excellent processability and flexibility is highly desirable but still faces formidable challenge.Herein,a general strategy is developed for efficient PRTP through photo-polymerization of phosphor monomers and N-isopropylacrylamide(NIPAM)spontaneously without a crosslinker.Remarkably ultralong lifetime of 3.54 s with afterglow duration time of 25 s and decent phosphorescent quantum efficiency of 13%are achieved.This efficient PRTP has been demonstrated to be derived from the synergistic effect of the covalent and hydrogen bonds networks formed through photo-polymerization of NIPAM.The electron paramagnetic resonance(EPR)spectra confirmed that methyl radicals are generated under the irradiation of ultraviolet light and promote the formation of covalent cross-linking networks.This strategy has also been proved to be generalizable to several other phosphor monomers.Interestingly,the polymer films display ultrahigh temperature resistance with long afterglows even at 140℃ and unexampled ultralong lifetime of 2.45 s in aqueous solutions.This work provides a simple and feasible avenue to obtain efficient PRTP.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
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.展开更多
Medical procedures are inherently invasive and carry the risk of inducing pain to the mind and body.Recently,efforts have been made to alleviate the discomfort associated with invasive medical procedures through the u...Medical procedures are inherently invasive and carry the risk of inducing pain to the mind and body.Recently,efforts have been made to alleviate the discomfort associated with invasive medical procedures through the use of virtual reality(VR)technology.VR has been demonstrated to be an effective treatment for pain associated with medical procedures,as well as for chronic pain conditions for which no effective treatment has been established.The precise mechanism by which the diversion from reality facilitated by VR contributes to the diminution of pain and anxiety has yet to be elucidated.However,the provision of positive images through VR-based visual stimulation may enhance the functionality of brain networks.The salience network is diminished,while the default mode network is enhanced.Additionally,the medial prefrontal cortex may establish a stronger connection with the default mode network,which could result in a reduction of pain and anxiety.Further research into the potential of VR technology to alleviate pain could lead to a reduction in the number of individuals who overdose on painkillers and contribute to positive change in the medical field.展开更多
The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesiz...The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesized by polycondensation of CO_(2) with 4,7,10-trioxa-1,13-tridecanediamine and tris(2-aminoethyl)amine(TAEA).TAEA was used as cross-link reagent.The mechanical properties of PUa were significantly improved by inserted the crosslink agent of TAEA.The formed slight cross-linked PUa exhibited excellent mechanical properties with tensile strength of 26.8 MPa,elongation at break of 34%and Young’s modulus of 351 MPa.Moreover,it could be remolded for 3 times without obvious change in the mechanical properties,which are ascribed to the hydrogen bonding interaction among the main chains and the slight cross-linked structure.In addition,the synthesized CO_(2)-based PUa is of outstanding thermal performance with an initial decomposition temperature above 300℃,besides it is tolerance for a variety of organic solvents.展开更多
Physical cross-linking by hydrogen-bonds (H-bonds), providing a good combination of application properties of thermosets and processability of thermoplastics, is a potential strategy to resolve the recycling problem o...Physical cross-linking by hydrogen-bonds (H-bonds), providing a good combination of application properties of thermosets and processability of thermoplastics, is a potential strategy to resolve the recycling problem of traditional chemically cross-linked polyethylene. However, ureidopyrimidone (UPy), the most widely used H-bonding motif, is unfavorable for large-scale industrial application due to its poor thermal stability. In this work, H-bonds cross-linked polyethylene was successfully prepared by reactive melt blending maleic anhydride grafted polyethylene (PE-g-MAH) with 3-amino-1,2,4-triazole (ATA) to form amide triazole ring-carboxylic acid units. Triazole ring can easily generate multiple H-bonds with carboxylic acid and amide. More importantly, these units are more thermal stable than UPy due to the absence of unstable urea group of UPy. The introduction of H-bonds cross-linking leads to an obvious improvement in mechanical properties and creep resistance and a good maintain in thermal properties and recyclability. Furthermore, the reinforcement effect monotonically improves with increasing the density of H-bonds. The obtained good properties are mainly attributed to largely enhanced interchain interactions induced by H-bonds cross-linking and intrinsic reversibility of H-bonds. This work develops a novel way for the simple fabrication of H-bonds cross-linked PE with high performance through reactive melt blending.展开更多
Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.展开更多
Complex network models are frequently employed for simulating and studyingdiverse real-world complex systems.Among these models,scale-free networks typically exhibit greater fragility to malicious attacks.Consequently...Complex network models are frequently employed for simulating and studyingdiverse real-world complex systems.Among these models,scale-free networks typically exhibit greater fragility to malicious attacks.Consequently,enhancing the robustness of scale-free networks has become a pressing issue.To address this problem,this paper proposes a Multi-Granularity Integration Algorithm(MGIA),which aims to improve the robustness of scale-free networks while keeping the initial degree of each node unchanged,ensuring network connectivity and avoiding the generation of multiple edges.The algorithm generates a multi-granularity structure from the initial network to be optimized,then uses different optimization strategies to optimize the networks at various granular layers in this structure,and finally realizes the information exchange between different granular layers,thereby further enhancing the optimization effect.We propose new network refresh,crossover,and mutation operators to ensure that the optimized network satisfies the given constraints.Meanwhile,we propose new network similarity and network dissimilarity evaluation metrics to improve the effectiveness of the optimization operators in the algorithm.In the experiments,the MGIA enhances the robustness of the scale-free network by 67.6%.This improvement is approximately 17.2%higher than the optimization effects achieved by eight currently existing complex network robustness optimization algorithms.展开更多
Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability drama...Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.展开更多
Satellite edge computing has garnered significant attention from researchers;however,processing a large volume of tasks within multi-node satellite networks still poses considerable challenges.The sharp increase in us...Satellite edge computing has garnered significant attention from researchers;however,processing a large volume of tasks within multi-node satellite networks still poses considerable challenges.The sharp increase in user demand for latency-sensitive tasks has inevitably led to offloading bottlenecks and insufficient computational capacity on individual satellite edge servers,making it necessary to implement effective task offloading scheduling to enhance user experience.In this paper,we propose a priority-based task scheduling strategy based on a Software-Defined Network(SDN)framework for satellite-terrestrial integrated networks,which clarifies the execution order of tasks based on their priority.Subsequently,we apply a Dueling-Double Deep Q-Network(DDQN)algorithm enhanced with prioritized experience replay to derive a computation offloading strategy,improving the experience replay mechanism within the Dueling-DDQN framework.Next,we utilize the Deep Deterministic Policy Gradient(DDPG)algorithm to determine the optimal resource allocation strategy to reduce the processing latency of sub-tasks.Simulation results demonstrate that the proposed d3-DDPG algorithm outperforms other approaches,effectively reducing task processing latency and thus improving user experience and system efficiency.展开更多
Thermosensitive hydrogel can integrate vapor molecular capture,in-situ liquefaction,and thermal-induced water release for freshwater capture.This study aimed to examine the dynamic behavior of poly(N-isopropylacrylami...Thermosensitive hydrogel can integrate vapor molecular capture,in-situ liquefaction,and thermal-induced water release for freshwater capture.This study aimed to examine the dynamic behavior of poly(N-isopropylacrylamide)(PNIPAM)single chain and cross-linking thermosensitive hydrogel through molecular dynamics simulation.Specifically,the impact of lower critical solution temperature(LCST)on the conformation of polymer chain and the interaction between water and polymer chain were also investigated.The polymer chain conformation underwent a transition from coil to globule when the temperature exceeded the LCST,indicating the temperature responsiveness of PNIPAM.Additionally,thermosensitive hydrogel samples with different cross-linking degrees(DOC)were studied,and relevant parameters such as the number of free water,the diffusion coefficient of water,and the pore size distribution were counted to evaluate the temperature responsiveness and water release characteristics of thermosensitive hydrogel.展开更多
Sodium-ion batteries(SIBs)have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium-ion batteries(LIBs).Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)as a common cathode of SIBs,featur...Sodium-ion batteries(SIBs)have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium-ion batteries(LIBs).Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)as a common cathode of SIBs,features the merits of high operating voltage,small volume change and favorable specific energy density.However,it suffers from poor cycling stability and rate performance induced by its low intrinsic conductivity.Herein,we propose an ingenious strategy targeting superior SIBs through cross-linked NVPF with multi-dimensional nanocarbon frameworks composed of amorphous carbon and carbon nanotubes(NVPF@C@CNTs).This rational design ensures favorable particle size for shortened sodium ion transmission pathway as well as improved electronic transfer network,thus leading to enhanced charge transfer kinetics and superior cycling stability.Benefited from this unique structure,significantly improved electrochemical properties are obtained,including high specific capacity(126.9 mAh g^(-1)at 1 C,1 C=128 mA g^(-1))and remarkably improved long-term cycling stability with 93.9%capacity retention after 1000 cycles at 20 C.The energy density of 286.8 Wh kg^(-1)can be reached for full cells with hard carbon as anode(NVPF@C@CNTs//HC).Additionally,the electrochemical performance of the full cell at high temperature is also investigated(95.3 mAh g^(-1)after 100 cycles at 1 C at 50℃).Such nanoscale dual-carbon networks engineering and thorough discussion of ion diffusion kinetics might make contributions to accelerating the process of phosphate cathodes in SIBs for large-scale energy storages.展开更多
Two-dimensional endoscopic images are susceptible to interferences such as specular reflections and monotonous texture illumination,hindering accurate three-dimensional lesion reconstruction by surgical robots.This st...Two-dimensional endoscopic images are susceptible to interferences such as specular reflections and monotonous texture illumination,hindering accurate three-dimensional lesion reconstruction by surgical robots.This study proposes a novel end-to-end disparity estimation model to address these challenges.Our approach combines a Pseudo-Siamese neural network architecture with pyramid dilated convolutions,integrating multi-scale image information to enhance robustness against lighting interferences.This study introduces a Pseudo-Siamese structure-based disparity regression model that simplifies left-right image comparison,improving accuracy and efficiency.The model was evaluated using a dataset of stereo endoscopic videos captured by the Da Vinci surgical robot,comprising simulated silicone heart sequences and real heart video data.Experimental results demonstrate significant improvement in the network’s resistance to lighting interference without substantially increasing parameters.Moreover,the model exhibited faster convergence during training,contributing to overall performance enhancement.This study advances endoscopic image processing accuracy and has potential implications for surgical robot applications in complex environments.展开更多
基金financially supported by the National Natu-ral Science Foundation of China(Nos.22375047,22378068,and 22075046)the Natural Science Foundation of Fujian Province(No.2022J01568)+2 种基金the National Key Research and Development Program of China(Nos.2022YFB3804905 and 2022YFB3804900)China Postdoctoral Science Foundation(No.2023M743437)start-up funding from Wenzhou Institute,University of Chinese Academy of Sciences(No.WIUCASQD2019002).
文摘Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has been difficult to strike a balance between the robustness and flexibility of coatings constructed by a single cross-linked network design.To overcome the conundrum,this innovative approach effectively combines two distinct cross-linked networks with unique functions,thus overcoming the challenge.Through a tightly interwoven structure comprised of added crosslinking sites,the coating achieves improved liquid repellency(WCA>100°,OSA<10°),increased durability(withstands 2,000 cycles of cotton wear),enhanced flexibility(endures 5,000 cycles of bending with a bending radius of 1 mm),and maintains high transparency(over 98%in the range of 410 nm to 760 nm).Additionally,the coating with remarkable adhesion can be applied to multiple substrates,enabling large-scale preparation and easy cycling coating,thus expanding its potential applications.The architecture of this fluoride-free dual cross-linked network not only advances liquid-repellent surfaces but also provides valuable insights for the development of eco-friendly materials in the future.
基金supported by the National Natural Science Foundation of China(No.U22A20420)the Science and Technology Plan Project of Changzhou(No.CJ20235017)In addi-tion,the authors thank Jiangsu Development&Reform Commis-sion for their support.
文摘Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22321002,22279153)Liaoning Revitalization Talents Program(XLYC1807207,XLYC2203134)DICP I202104。
文摘Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.
基金supported by Physical Chemical Materials Analytical&Testing Center of Shandong University at Weihai,Natural Science Foundation of Shandong Province(No.ZR2022QD057)Open Project Fund for Hubei Key Laboratory of Oral and Maxillofacial Development and Regeneration(No.2021kqhm003)+1 种基金State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology)the Science Fund of Shandong Laboratory of Advanced Materials and Green Manufacturing(Yantai,No.AMGM2021F02)。
文摘To achieve smart and personalized medicine, the development of hydrogel dressings with sensing properties and biotherapeutic properties that can act as a sensor to monitor of human health in real-time while speeding up wound healing face great challenge. In the present study, a biocompatible dual-network composite hydrogel(DNCGel) sensor was obtained via a simple process. The dual network hydrogel is constructed by the interpenetration of a flexible network formed of poly(vinyl alcohol)(PVA) physical cross-linked by repeated freeze-thawing and a rigid network of iron-chelated xanthan gum(XG) impregnated with Fe^(3+) interpenetration. The pure PVA/XG hydrogels were chelated with ferric ions by immersion to improve the gel strength(compressive modulus and tensile modulus can reach up to 0.62 MPa and0.079 MPa, respectively), conductivity(conductivity values ranging from 9 × 10^(-4) S/cm to 1 × 10^(-3)S/cm)and bacterial inhibition properties(up to 98.56%). Subsequently, the effects of the ratio of PVA and XG and the immersion time of Fe^(3+) on the hydrogels were investigated, and DNGel3 was given the most priority on a comprehensive consideration. It was demonstrated that the DNCGel exhibit good biocompatibility in vitro, effectively facilitate wound healing in vivo(up to 97.8% healing rate) under electrical stimulation, and monitors human movement in real time. This work provides a novel avenue to explore multifunctional intelligent hydrogels that hold great promise in biomedical fields such as smart wound dressings and flexible wearable sensors.
基金supported by R&D Program of Power Batteries with Low Temperature and High Energy,Science and Technology Bureau of Changchun(19SS013)Key Subject Construction of Physical Chemistry of Northeast Normal University+1 种基金the Fundamental Research Funds for the Central Universities(2412020FZ007,2412020FZ008)National Natural Science Foundation of China(22102020)
文摘The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycling performance and extending service life of LIBs.Here,we report a novel cross-linked network SHSPE(PDDP)containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and nonflammability.The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28°C without external stimulation.Furthermore,the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide(EMIMTFSI)improves the ionic conductivity(1.13×10^(−4)S cm^(−1)at 28°C)and non-flammability of PDDP.The assembled Li/PDDP/LiFePO_(4)cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g^(−1)after 300 cycles at 0.2 C.More importantly,the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.
基金supported by the National Natural Science Foundation of China(22175149,21975215)the Natural Science Foundation of Hunan Province(2021JJ30661)the Scientific Research Foundation of Hunan Provincial Education Department(19A486)。
文摘Efficient polymeric room-temperature phosphorescence(PRTP)with excellent processability and flexibility is highly desirable but still faces formidable challenge.Herein,a general strategy is developed for efficient PRTP through photo-polymerization of phosphor monomers and N-isopropylacrylamide(NIPAM)spontaneously without a crosslinker.Remarkably ultralong lifetime of 3.54 s with afterglow duration time of 25 s and decent phosphorescent quantum efficiency of 13%are achieved.This efficient PRTP has been demonstrated to be derived from the synergistic effect of the covalent and hydrogen bonds networks formed through photo-polymerization of NIPAM.The electron paramagnetic resonance(EPR)spectra confirmed that methyl radicals are generated under the irradiation of ultraviolet light and promote the formation of covalent cross-linking networks.This strategy has also been proved to be generalizable to several other phosphor monomers.Interestingly,the polymer films display ultrahigh temperature resistance with long afterglows even at 140℃ and unexampled ultralong lifetime of 2.45 s in aqueous solutions.This work provides a simple and feasible avenue to obtain efficient PRTP.
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supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
文摘Medical procedures are inherently invasive and carry the risk of inducing pain to the mind and body.Recently,efforts have been made to alleviate the discomfort associated with invasive medical procedures through the use of virtual reality(VR)technology.VR has been demonstrated to be an effective treatment for pain associated with medical procedures,as well as for chronic pain conditions for which no effective treatment has been established.The precise mechanism by which the diversion from reality facilitated by VR contributes to the diminution of pain and anxiety has yet to be elucidated.However,the provision of positive images through VR-based visual stimulation may enhance the functionality of brain networks.The salience network is diminished,while the default mode network is enhanced.Additionally,the medial prefrontal cortex may establish a stronger connection with the default mode network,which could result in a reduction of pain and anxiety.Further research into the potential of VR technology to alleviate pain could lead to a reduction in the number of individuals who overdose on painkillers and contribute to positive change in the medical field.
文摘The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesized by polycondensation of CO_(2) with 4,7,10-trioxa-1,13-tridecanediamine and tris(2-aminoethyl)amine(TAEA).TAEA was used as cross-link reagent.The mechanical properties of PUa were significantly improved by inserted the crosslink agent of TAEA.The formed slight cross-linked PUa exhibited excellent mechanical properties with tensile strength of 26.8 MPa,elongation at break of 34%and Young’s modulus of 351 MPa.Moreover,it could be remolded for 3 times without obvious change in the mechanical properties,which are ascribed to the hydrogen bonding interaction among the main chains and the slight cross-linked structure.In addition,the synthesized CO_(2)-based PUa is of outstanding thermal performance with an initial decomposition temperature above 300℃,besides it is tolerance for a variety of organic solvents.
基金financially supported by the National Natural Science Foundation of China (No. 51803130)Fundamental Research Funds for Central UniversitiesChongqing University Key Laboratory of Micro/Nano Materials Engineering and Technology (No. KFJJ2005)
文摘Physical cross-linking by hydrogen-bonds (H-bonds), providing a good combination of application properties of thermosets and processability of thermoplastics, is a potential strategy to resolve the recycling problem of traditional chemically cross-linked polyethylene. However, ureidopyrimidone (UPy), the most widely used H-bonding motif, is unfavorable for large-scale industrial application due to its poor thermal stability. In this work, H-bonds cross-linked polyethylene was successfully prepared by reactive melt blending maleic anhydride grafted polyethylene (PE-g-MAH) with 3-amino-1,2,4-triazole (ATA) to form amide triazole ring-carboxylic acid units. Triazole ring can easily generate multiple H-bonds with carboxylic acid and amide. More importantly, these units are more thermal stable than UPy due to the absence of unstable urea group of UPy. The introduction of H-bonds cross-linking leads to an obvious improvement in mechanical properties and creep resistance and a good maintain in thermal properties and recyclability. Furthermore, the reinforcement effect monotonically improves with increasing the density of H-bonds. The obtained good properties are mainly attributed to largely enhanced interchain interactions induced by H-bonds cross-linking and intrinsic reversibility of H-bonds. This work develops a novel way for the simple fabrication of H-bonds cross-linked PE with high performance through reactive melt blending.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
基金National Natural Science Foundation of China(11971211,12171388).
文摘Complex network models are frequently employed for simulating and studyingdiverse real-world complex systems.Among these models,scale-free networks typically exhibit greater fragility to malicious attacks.Consequently,enhancing the robustness of scale-free networks has become a pressing issue.To address this problem,this paper proposes a Multi-Granularity Integration Algorithm(MGIA),which aims to improve the robustness of scale-free networks while keeping the initial degree of each node unchanged,ensuring network connectivity and avoiding the generation of multiple edges.The algorithm generates a multi-granularity structure from the initial network to be optimized,then uses different optimization strategies to optimize the networks at various granular layers in this structure,and finally realizes the information exchange between different granular layers,thereby further enhancing the optimization effect.We propose new network refresh,crossover,and mutation operators to ensure that the optimized network satisfies the given constraints.Meanwhile,we propose new network similarity and network dissimilarity evaluation metrics to improve the effectiveness of the optimization operators in the algorithm.In the experiments,the MGIA enhances the robustness of the scale-free network by 67.6%.This improvement is approximately 17.2%higher than the optimization effects achieved by eight currently existing complex network robustness optimization algorithms.
基金the Science and Technology Department of Henan Province of China(Grant No.222102240060 and 222300420541)the Education Department of Henan Province of China(Grant No.22B430023)supported by the Program for Innovative Research Team(in Science and Technology)in University of Henan Province(Grant No.23IRTSTHN009)。
文摘Lithium-metal anodes(LMAs)have been recognized as the ultimate anodes for next-generation batteries with high energy density,but stringent assembly-environment conditions derived from the poor moisture stability dramatically hinder the transformation of LMAs from laboratory to industry.Herein,an in situ formed cross-linked polymer layer on LMAs is designed and constructed by a facile thiol-acrylate click chemistry reaction between poly(ethylene glycol)diacrylate(PEGDA)and the crosslinker containing multi thiol groups under UV irradiation.Owing to the hydrophobic nature of the layer,the treated LMAs demonstrate remarkable humid stability for more than 3 h in ambient air(70%relative humidity).The coating humid-resistant protective layer also possesses a dual-functional characterization as solid polymer electrolytes by introducing lithium bis(trifluoromethanesulfonyl)imide in the system in advance.The intimate contact between the polymer layer and LMAs reduces interfacial resistance in the assembled Li/LiFePO_(4)or Li/LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)full cell effectively,and endows the cell with an outstanding cycle performance.
文摘Satellite edge computing has garnered significant attention from researchers;however,processing a large volume of tasks within multi-node satellite networks still poses considerable challenges.The sharp increase in user demand for latency-sensitive tasks has inevitably led to offloading bottlenecks and insufficient computational capacity on individual satellite edge servers,making it necessary to implement effective task offloading scheduling to enhance user experience.In this paper,we propose a priority-based task scheduling strategy based on a Software-Defined Network(SDN)framework for satellite-terrestrial integrated networks,which clarifies the execution order of tasks based on their priority.Subsequently,we apply a Dueling-Double Deep Q-Network(DDQN)algorithm enhanced with prioritized experience replay to derive a computation offloading strategy,improving the experience replay mechanism within the Dueling-DDQN framework.Next,we utilize the Deep Deterministic Policy Gradient(DDPG)algorithm to determine the optimal resource allocation strategy to reduce the processing latency of sub-tasks.Simulation results demonstrate that the proposed d3-DDPG algorithm outperforms other approaches,effectively reducing task processing latency and thus improving user experience and system efficiency.
基金supported by National Natural Science Foundation of China(No.52206073)Fundamental Research Funds for the Central Universities(No.3132023119)Guangdong Basic and Applied Basic Research Foundation(Nos.2024A1515011379 and 2023A1515110613).
文摘Thermosensitive hydrogel can integrate vapor molecular capture,in-situ liquefaction,and thermal-induced water release for freshwater capture.This study aimed to examine the dynamic behavior of poly(N-isopropylacrylamide)(PNIPAM)single chain and cross-linking thermosensitive hydrogel through molecular dynamics simulation.Specifically,the impact of lower critical solution temperature(LCST)on the conformation of polymer chain and the interaction between water and polymer chain were also investigated.The polymer chain conformation underwent a transition from coil to globule when the temperature exceeded the LCST,indicating the temperature responsiveness of PNIPAM.Additionally,thermosensitive hydrogel samples with different cross-linking degrees(DOC)were studied,and relevant parameters such as the number of free water,the diffusion coefficient of water,and the pore size distribution were counted to evaluate the temperature responsiveness and water release characteristics of thermosensitive hydrogel.
基金financially supported by Science and Technology Foundation of Guizhou Province(QKHZC[2020]2Y037)the Science and Technology Innovation Program of Hunan Province(2020RC4005,2019RS1004)+2 种基金Research start-up funding from Central South University(202044019)Innovation Mover Program of Central South University(2020CX007)National Natural Science Foundation of China(U21A20284)
文摘Sodium-ion batteries(SIBs)have rapidly risen to the forefront of energy storage systems as a promising supplementary for Lithium-ion batteries(LIBs).Na_(3)V_(2)(PO_(4))_(2)F_(3)(NVPF)as a common cathode of SIBs,features the merits of high operating voltage,small volume change and favorable specific energy density.However,it suffers from poor cycling stability and rate performance induced by its low intrinsic conductivity.Herein,we propose an ingenious strategy targeting superior SIBs through cross-linked NVPF with multi-dimensional nanocarbon frameworks composed of amorphous carbon and carbon nanotubes(NVPF@C@CNTs).This rational design ensures favorable particle size for shortened sodium ion transmission pathway as well as improved electronic transfer network,thus leading to enhanced charge transfer kinetics and superior cycling stability.Benefited from this unique structure,significantly improved electrochemical properties are obtained,including high specific capacity(126.9 mAh g^(-1)at 1 C,1 C=128 mA g^(-1))and remarkably improved long-term cycling stability with 93.9%capacity retention after 1000 cycles at 20 C.The energy density of 286.8 Wh kg^(-1)can be reached for full cells with hard carbon as anode(NVPF@C@CNTs//HC).Additionally,the electrochemical performance of the full cell at high temperature is also investigated(95.3 mAh g^(-1)after 100 cycles at 1 C at 50℃).Such nanoscale dual-carbon networks engineering and thorough discussion of ion diffusion kinetics might make contributions to accelerating the process of phosphate cathodes in SIBs for large-scale energy storages.
基金Supported by Sichuan Science and Technology Program(2023YFSY0026,2023YFH0004)Supported by the Institute of Information&Communications Technology Planning&Evaluation(IITP)grant funded by the Korean government(MSIT)(No.RS-2022-00155885,Artificial Intelligence Convergence Innovation Human Resources Development(Hanyang University ERICA)).
文摘Two-dimensional endoscopic images are susceptible to interferences such as specular reflections and monotonous texture illumination,hindering accurate three-dimensional lesion reconstruction by surgical robots.This study proposes a novel end-to-end disparity estimation model to address these challenges.Our approach combines a Pseudo-Siamese neural network architecture with pyramid dilated convolutions,integrating multi-scale image information to enhance robustness against lighting interferences.This study introduces a Pseudo-Siamese structure-based disparity regression model that simplifies left-right image comparison,improving accuracy and efficiency.The model was evaluated using a dataset of stereo endoscopic videos captured by the Da Vinci surgical robot,comprising simulated silicone heart sequences and real heart video data.Experimental results demonstrate significant improvement in the network’s resistance to lighting interference without substantially increasing parameters.Moreover,the model exhibited faster convergence during training,contributing to overall performance enhancement.This study advances endoscopic image processing accuracy and has potential implications for surgical robot applications in complex environments.
