An Information-Centric Network(ICN)provides a promising paradigm for the upcoming internet architecture,which will struggle with steady growth in data and changes in accessmodels.Various ICN architectures have been de...An Information-Centric Network(ICN)provides a promising paradigm for the upcoming internet architecture,which will struggle with steady growth in data and changes in accessmodels.Various ICN architectures have been designed,including Named Data Networking(NDN),which is designed around content delivery instead of hosts.As data is the central part of the network.Therefore,NDN was developed to get rid of the dependency on IP addresses and provide content effectively.Mobility is one of the major research dimensions for this upcoming internet architecture.Some research has been carried out to solve the mobility issues,but it still has problems like handover delay and packet loss ratio during real-time video streaming in the case of consumer and producer mobility.To solve this issue,an efficient hierarchical Cluster Base Proactive Caching for Device Mobility Management(CB-PC-DMM)in NDN Vehicular Networks(NDN-VN)is proposed,through which the consumer receives the contents proactively after handover during the mobility of the consumer.When a consumer moves to the next destination,a handover interest is sent to the connected router,then the router multicasts the consumer’s desired data packet to the next hop of neighboring routers.Thus,once the handover process is completed,consumers can easily get the content to the newly connected router.A CB-PCDMM in NDN-VN is proposed that improves the packet delivery ratio and reduces the handover delay aswell as cluster overhead.Moreover,the intra and inter-domain handover handling procedures in CB-PC-DMM for NDN-VN have been described.For the validation of our proposed scheme,MATLAB simulations are conducted.The simulation results show that our proposed scheme reduces the handover delay and increases the consumer’s interest satisfaction ratio.The proposed scheme is compared with the existing stateof-the-art schemes,and the total percentage of handover delays is decreased by up to 0.1632%,0.3267%,2.3437%,2.3255%,and 3.7313%at the mobility speeds of 5 m/s,10 m/s,15 m/s,20 m/s,and 25 m/s,and the efficiency of the packet delivery ratio is improved by up to 1.2048%,5.0632%,6.4935%,6.943%,and 8.4507%.Furthermore,the simulation results of our proposed scheme show better efficiency in terms of Packet Delivery Ratio(PDR)from 0.071 to 0.077 and a decrease in the handover delay from 0.1334 to 0.129.展开更多
The increase in the utilization of infrared heat detection technology in military applications necessitates research on composites with improved thermal transmission performance and microwave absorption capabilities.T...The increase in the utilization of infrared heat detection technology in military applications necessitates research on composites with improved thermal transmission performance and microwave absorption capabilities.This study satisfactorily fabricated a series of MoS_(2)/BN-xyz composites(which were characterized by the weight ratio of MoS_(2)to BN,denoted by xy:z)through chemical vapor depos-ition,which resulted in their improved thermal stability and thermal transmission performance.The results show that the remaining mass of MoS_(2)/BN-101 was as high as 69.25wt%at 800℃under air atmosphere,and a temperature difference of 31.7℃was maintained between the surface temperature and the heating source at a heating temperature of 200℃.Furthermore,MoS_(2)/BN-301 exhibited an im-pressive minimum reflection loss value of-32.21 dB at 4.0 mm and a wide effective attenuation bandwidth ranging from 9.32 to 18.00 GHz(8.68 GHz).Therefore,these simplified synthesized MoS_(2)/BN-xyz composites demonstrate great potential as highly efficient con-tenders for the enhancement of microwave absorption performance and thermal conductance.展开更多
With vigorous developments in nanotechnology,the elaborate regulation of microstructure shows attractive potential in the design of electromagnetic wave absorbers.Herein,a hierarchical porous structure and composite h...With vigorous developments in nanotechnology,the elaborate regulation of microstructure shows attractive potential in the design of electromagnetic wave absorbers.Herein,a hierarchical porous structure and composite heterogeneous interface are constructed successfully to optimize the electromagnetic loss capacity.The macro–micro-synergistic graphene aerogel formed by the ice template‑assisted 3D printing strategy is cut by silicon carbide nanowires(SiC_(nws))grown in situ,while boron nitride(BN)interfacial structure is introduced on graphene nanoplates.The unique composite structure forces multiple scattering of incident EMWs,ensuring the combined effects of interfacial polarization,conduction networks,and magnetic-dielectric synergy.Therefore,the as-prepared composites present a minimum reflection loss value of−37.8 dB and a wide effective absorption bandwidth(EAB)of 9.2 GHz(from 8.8 to 18.0 GHz)at 2.5 mm.Besides,relying on the intrinsic high-temperature resistance of SiC_(nws) and BN,the EAB also remains above 5.0 GHz after annealing in air environment at 600℃ for 10 h.展开更多
Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subse...Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.展开更多
The wave-absorbing materials are kinds of special electromagnetic functional materials and have been widely used in electromagnetic pollution control and military fields.In-situ integrated hierarchical structure const...The wave-absorbing materials are kinds of special electromagnetic functional materials and have been widely used in electromagnetic pollution control and military fields.In-situ integrated hierarchical structure construction is thought as a promising route to improve the microwave absorption performance of the materials.In the present work,layer-structured Co-metal-organic frameworks(Co-MOFs)precursors were grown in-situ on the surface of carbon fibers with the hydrothermal method.After annealed at 500℃ under Ar atmosphere,a novel multiscale hierarchical composite(Co@C/CF)was obtained with the support of carbon fibers,keeping the flower-like structure.Scanning electron microscope,transmission electron microscope,X-ray diffraction,Raman,and X-ray photoelectron spectroscopy were performed to analyze the microstructure and composition of the hierarchical structure,and the microwave absorption performance of the Co@C/CF composites were investigated.The results showed that the growth of the flower-like structure on the surface of carbon fiber was closely related to the metal-to-ligand ratio.The optimized Co@C/CF flower-like composites achieved the best reflection loss of−55.7 dB in the low frequency band of 6–8 GHz at the thickness of 2.8 mm,with the corresponding effective absorption bandwidth(EAB)of 2.1 GHz.The EAB of 3.24 GHz was achieved in the high frequency range of 12–16 GHz when the thickness was 1.5 mm.The excellent microwave absorption performance was ascribed to the introduction of magnetic components and the construction of the unique structure.The flower-like structure not only balanced the impedance of the fibers themselves,but also extended the propagation path of the microwave and then increased the multiple reflection losses.This work provides a convenient method for the design and development of wave-absorbing composites with in-situ integrated structure.展开更多
As modern communication and detection technologies advance at a swift pace,multifunctional electromagnetic interference(EMI)shielding materials with active/positive infrared stealth,hydrophobicity,and electric-thermal...As modern communication and detection technologies advance at a swift pace,multifunctional electromagnetic interference(EMI)shielding materials with active/positive infrared stealth,hydrophobicity,and electric-thermal conversion ability have received extensive attention.Meeting the aforesaid requirements simultaneously remains a huge challenge.In this research,the melamine foam(MF)/polypyrrole(PPy)nanowire arrays(MF@PPy)were fabricated via one-step electrochemical polymerization.The hierarchical MF@PPy foam was composed of three-dimensional PPy micro-skeleton and ordered PPy nanowire arrays.Due to the upwardly grown PPy nanowire arrays,the MF@PPy foam possessed good hydrophobicity ability with a water contact angle of 142.00°and outstanding stability under various harsh environments.Meanwhile,the MF@PPy foam showed excellent thermal insulation property on account of the low thermal conductivity and elongated ligament characteristic of PPy nanowire arrays.Furthermore,taking advantage of the high conductivity(128.2 S m^(-1)),the MF@PPy foam exhibited rapid Joule heating under 3 V,resulting in dynamic infrared stealth and thermal camouflage effects.More importantly,the MF@PPy foam exhibited remarkable EMI shielding effectiveness values of 55.77 dB and 19,928.57 dB cm^(2)g^(-1).Strong EMI shielding was put down to the hierarchically porous PPy structure,which offered outstanding impedance matching,conduction loss,and multiple attenuations.This innovative approach provides significant insights to the development of advanced multifunctional EMI shielding foams by constructing PPy nanowire arrays,showing great applications in both military and civilian fields.展开更多
Spear Phishing Attacks(SPAs)pose a significant threat to the healthcare sector,resulting in data breaches,financial losses,and compromised patient confidentiality.Traditional defenses,such as firewalls and antivirus s...Spear Phishing Attacks(SPAs)pose a significant threat to the healthcare sector,resulting in data breaches,financial losses,and compromised patient confidentiality.Traditional defenses,such as firewalls and antivirus software,often fail to counter these sophisticated attacks,which target human vulnerabilities.To strengthen defenses,healthcare organizations are increasingly adopting Machine Learning(ML)techniques.ML-based SPA defenses use advanced algorithms to analyze various features,including email content,sender behavior,and attachments,to detect potential threats.This capability enables proactive security measures that address risks in real-time.The interpretability of ML models fosters trust and allows security teams to continuously refine these algorithms as new attack methods emerge.Implementing ML techniques requires integrating diverse data sources,such as electronic health records,email logs,and incident reports,which enhance the algorithms’learning environment.Feedback from end-users further improves model performance.Among tested models,the hierarchical models,Convolutional Neural Network(CNN)achieved the highest accuracy at 99.99%,followed closely by the sequential Bidirectional Long Short-Term Memory(BiLSTM)model at 99.94%.In contrast,the traditional Multi-Layer Perceptron(MLP)model showed an accuracy of 98.46%.This difference underscores the superior performance of advanced sequential and hierarchical models in detecting SPAs compared to traditional approaches.展开更多
Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed ...Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.展开更多
Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative stru...Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.展开更多
Two-dimensional carbon-based materials have shown promising electromagnetic wave absorption capabilities in mid-and high-frequency ranges,but face challenges in low-frequency absorption due to limited control over pol...Two-dimensional carbon-based materials have shown promising electromagnetic wave absorption capabilities in mid-and high-frequency ranges,but face challenges in low-frequency absorption due to limited control over polarization response mecha-nisms and ambiguous resonance behavior.In this study,we pro-pose a novel approach to enhance absorption efficiency in aligned three-dimensional(3D)MXene/CNF(cellulose nanofibers)cavities by modifying polarization properties and manipulating resonance response in the 3D MXene architecture.This controlled polarization mechanism results in a significant shift of the main absorption region from the X-band to the S-band,leading to a remarkable reflection loss value of-47.9 dB in the low-frequency range.Furthermore,our findings revealed the importance of the oriented electromagnetic coupling in influencing electromagnetic response and microwave absorption properties.The present study inspired us to develop a generic strategy for low-frequency tuned absorption in the absence of magnetic element participation,while orientation-induced polarization and the derived magnetic resonance coupling are the key controlling factors of the method.展开更多
Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,...Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.展开更多
Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficien...Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.展开更多
In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active ...In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.展开更多
Printed micro-supercapacitors(MSCs)have shown broad prospect in flexible and wearable electronics.Most of previous studies focused on printing the electrochemically active materials paying less attention to other key ...Printed micro-supercapacitors(MSCs)have shown broad prospect in flexible and wearable electronics.Most of previous studies focused on printing the electrochemically active materials paying less attention to other key components like current collectors and electrolytes.This study presents an allprinting strategy to fabricate in-plane flexible and substrate-free MSCs with hierarchical encapsulation.This new type of“all-in-one”MSC is constructed by encapsulating the in-plane interdigital current collectors and electrodes within the polyvinyl-alcohol-based hydrogel electrolyte via sequential printing.The bottom electrolyte layer of this fully printed MSCs helps protect the device from the limitation of conventional substrate,showing excellent flexibility.The MSCs maintain a high capacitance retention of 96.84%even in a completely folded state.An optimal electrochemical performance can be achieved by providing ample and shorter transport paths for ions.The MSCs using commercial activated carbon as the active material are endowed with a high specific areal capacitance of 1892.90 mF cm^(-2)at a current density of 0.3 mA cm^(-2),and an outstanding volumetric energy density of 9.20 mWh cm^(-3)at a volumetric power density of 6.89 mW cm^(-3).For demonstration,a thermo-hygrometer is stably powered by five MSCs which are connected in series and wrapped onto a glass rod.This low-cost and versatile all-printing strategy is believed to diversify the application fields of MSCs with high capacitance and excellent flexibility.展开更多
Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume di...Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance.展开更多
Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au...Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.展开更多
Chemical resistant textiles are vital for safeguarding humans against chemical hazards in various settings.such as industrialproduction,chemicalaccidents,laboratory activities,and road transportation.However,the ideal...Chemical resistant textiles are vital for safeguarding humans against chemical hazards in various settings.such as industrialproduction,chemicalaccidents,laboratory activities,and road transportation.However,the ideal integration of chemical resistance,thermal and moisture management,and wearer condition monitoring in conventional chemically protective textiles remains challenging.Herein,the design,manufacturing,and use of stretchable hierarchical core-shell yarns(HCSYs)for integrated chemical resistance,moisture regulation,and smart sensing textiles are demonstrated.These yarns con-tain helically elastic spandex,wrapped silver-plated nylon,and surface-structuredpolytetrafluo-roethylene(PTFE)yarns and are designed and manufactured based on a scalable fabrication process.In addition to their ideal chemical resistance performance,HCSYs can function as multifunctional stretch-able electronics for real-time human motion monitoring and as the basic element of intelligent textiles.Furthermore,a desirable dynamic thermoregulation function is achieved by exploiting the fabric structure with stretching modulation.Our HCSYs may provide prospective opportunities for the future development of smart protective textiles with high durability,flexibility,and scalability.展开更多
Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reactio...Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for LSBs.The CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs crossover.In particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active materials.The unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 C.This work presents a facile strategy for exploiting high-performance LSBs.展开更多
This paper develops a novel hierarchical control strategy for improving the trajectory tracking capability of aerial robots under parameter uncertainties.The hierarchical control strategy is composed of an adaptive sl...This paper develops a novel hierarchical control strategy for improving the trajectory tracking capability of aerial robots under parameter uncertainties.The hierarchical control strategy is composed of an adaptive sliding mode controller and a model-free iterative sliding mode controller(MFISMC).A position controller is designed based on adaptive sliding mode control(SMC)to safely drive the aerial robot and ensure fast state convergence under external disturbances.Additionally,the MFISMC acts as an attitude controller to estimate the unmodeled dynamics without detailed knowledge of aerial robots.Then,the adaption laws are derived with the Lyapunov theory to guarantee the asymptotic tracking of the system state.Finally,to demonstrate the performance and robustness of the proposed control strategy,numerical simulations are carried out,which are also compared with other conventional strategies,such as proportional-integralderivative(PID),backstepping(BS),and SMC.The simulation results indicate that the proposed hierarchical control strategy can fulfill zero steady-state error and achieve faster convergence compared with conventional strategies.展开更多
基金This work was supported by the MSIT(Ministry of Science and ICT),Korea,under the ITRC(Information Technology Research Center)support program(IITP-2023-2018-0-01431)supervised by the IITP(Institute for Information&Communications Technology Planning&Evaluation).
文摘An Information-Centric Network(ICN)provides a promising paradigm for the upcoming internet architecture,which will struggle with steady growth in data and changes in accessmodels.Various ICN architectures have been designed,including Named Data Networking(NDN),which is designed around content delivery instead of hosts.As data is the central part of the network.Therefore,NDN was developed to get rid of the dependency on IP addresses and provide content effectively.Mobility is one of the major research dimensions for this upcoming internet architecture.Some research has been carried out to solve the mobility issues,but it still has problems like handover delay and packet loss ratio during real-time video streaming in the case of consumer and producer mobility.To solve this issue,an efficient hierarchical Cluster Base Proactive Caching for Device Mobility Management(CB-PC-DMM)in NDN Vehicular Networks(NDN-VN)is proposed,through which the consumer receives the contents proactively after handover during the mobility of the consumer.When a consumer moves to the next destination,a handover interest is sent to the connected router,then the router multicasts the consumer’s desired data packet to the next hop of neighboring routers.Thus,once the handover process is completed,consumers can easily get the content to the newly connected router.A CB-PCDMM in NDN-VN is proposed that improves the packet delivery ratio and reduces the handover delay aswell as cluster overhead.Moreover,the intra and inter-domain handover handling procedures in CB-PC-DMM for NDN-VN have been described.For the validation of our proposed scheme,MATLAB simulations are conducted.The simulation results show that our proposed scheme reduces the handover delay and increases the consumer’s interest satisfaction ratio.The proposed scheme is compared with the existing stateof-the-art schemes,and the total percentage of handover delays is decreased by up to 0.1632%,0.3267%,2.3437%,2.3255%,and 3.7313%at the mobility speeds of 5 m/s,10 m/s,15 m/s,20 m/s,and 25 m/s,and the efficiency of the packet delivery ratio is improved by up to 1.2048%,5.0632%,6.4935%,6.943%,and 8.4507%.Furthermore,the simulation results of our proposed scheme show better efficiency in terms of Packet Delivery Ratio(PDR)from 0.071 to 0.077 and a decrease in the handover delay from 0.1334 to 0.129.
基金supported by the Science and Technology Department of Qinghai Province,China(No.2022-ZJ-932Q).
文摘The increase in the utilization of infrared heat detection technology in military applications necessitates research on composites with improved thermal transmission performance and microwave absorption capabilities.This study satisfactorily fabricated a series of MoS_(2)/BN-xyz composites(which were characterized by the weight ratio of MoS_(2)to BN,denoted by xy:z)through chemical vapor depos-ition,which resulted in their improved thermal stability and thermal transmission performance.The results show that the remaining mass of MoS_(2)/BN-101 was as high as 69.25wt%at 800℃under air atmosphere,and a temperature difference of 31.7℃was maintained between the surface temperature and the heating source at a heating temperature of 200℃.Furthermore,MoS_(2)/BN-301 exhibited an im-pressive minimum reflection loss value of-32.21 dB at 4.0 mm and a wide effective attenuation bandwidth ranging from 9.32 to 18.00 GHz(8.68 GHz).Therefore,these simplified synthesized MoS_(2)/BN-xyz composites demonstrate great potential as highly efficient con-tenders for the enhancement of microwave absorption performance and thermal conductance.
基金sponsored by National Natural Science Foundation of China(No.52302121,No.52203386)Shanghai Sailing Program(No.23YF1454700)+1 种基金Shanghai Natural Science Foundation(No.23ZR1472700)Shanghai Post-doctoral Excellent Program(No.2022664).
文摘With vigorous developments in nanotechnology,the elaborate regulation of microstructure shows attractive potential in the design of electromagnetic wave absorbers.Herein,a hierarchical porous structure and composite heterogeneous interface are constructed successfully to optimize the electromagnetic loss capacity.The macro–micro-synergistic graphene aerogel formed by the ice template‑assisted 3D printing strategy is cut by silicon carbide nanowires(SiC_(nws))grown in situ,while boron nitride(BN)interfacial structure is introduced on graphene nanoplates.The unique composite structure forces multiple scattering of incident EMWs,ensuring the combined effects of interfacial polarization,conduction networks,and magnetic-dielectric synergy.Therefore,the as-prepared composites present a minimum reflection loss value of−37.8 dB and a wide effective absorption bandwidth(EAB)of 9.2 GHz(from 8.8 to 18.0 GHz)at 2.5 mm.Besides,relying on the intrinsic high-temperature resistance of SiC_(nws) and BN,the EAB also remains above 5.0 GHz after annealing in air environment at 600℃ for 10 h.
基金supported in part by NIH grants R01NS39600,U01MH114829RF1MH128693(to GAA)。
文摘Many fields,such as neuroscience,are experiencing the vast prolife ration of cellular data,underscoring the need fo r organizing and interpreting large datasets.A popular approach partitions data into manageable subsets via hierarchical clustering,but objective methods to determine the appropriate classification granularity are missing.We recently introduced a technique to systematically identify when to stop subdividing clusters based on the fundamental principle that cells must differ more between than within clusters.Here we present the corresponding protocol to classify cellular datasets by combining datadriven unsupervised hierarchical clustering with statistical testing.These general-purpose functions are applicable to any cellular dataset that can be organized as two-dimensional matrices of numerical values,including molecula r,physiological,and anatomical datasets.We demonstrate the protocol using cellular data from the Janelia MouseLight project to chara cterize morphological aspects of neurons.
基金financially supported by the National Natural Science of Foundation of China(No.52371097)the Shenyang Unveiling and Leading Project,China(No.22-301-1-01)。
文摘The wave-absorbing materials are kinds of special electromagnetic functional materials and have been widely used in electromagnetic pollution control and military fields.In-situ integrated hierarchical structure construction is thought as a promising route to improve the microwave absorption performance of the materials.In the present work,layer-structured Co-metal-organic frameworks(Co-MOFs)precursors were grown in-situ on the surface of carbon fibers with the hydrothermal method.After annealed at 500℃ under Ar atmosphere,a novel multiscale hierarchical composite(Co@C/CF)was obtained with the support of carbon fibers,keeping the flower-like structure.Scanning electron microscope,transmission electron microscope,X-ray diffraction,Raman,and X-ray photoelectron spectroscopy were performed to analyze the microstructure and composition of the hierarchical structure,and the microwave absorption performance of the Co@C/CF composites were investigated.The results showed that the growth of the flower-like structure on the surface of carbon fiber was closely related to the metal-to-ligand ratio.The optimized Co@C/CF flower-like composites achieved the best reflection loss of−55.7 dB in the low frequency band of 6–8 GHz at the thickness of 2.8 mm,with the corresponding effective absorption bandwidth(EAB)of 2.1 GHz.The EAB of 3.24 GHz was achieved in the high frequency range of 12–16 GHz when the thickness was 1.5 mm.The excellent microwave absorption performance was ascribed to the introduction of magnetic components and the construction of the unique structure.The flower-like structure not only balanced the impedance of the fibers themselves,but also extended the propagation path of the microwave and then increased the multiple reflection losses.This work provides a convenient method for the design and development of wave-absorbing composites with in-situ integrated structure.
基金supported by the Key Research and Development Program of Sichuan Province(Grant No.2023ZHCG0050)the Fundamental Research Funds for the Central Universities of China(Grant No.2682024QZ006 and 2682024ZTPY042)the Analytic and Testing Center of Southwest Jiaotong University.
文摘As modern communication and detection technologies advance at a swift pace,multifunctional electromagnetic interference(EMI)shielding materials with active/positive infrared stealth,hydrophobicity,and electric-thermal conversion ability have received extensive attention.Meeting the aforesaid requirements simultaneously remains a huge challenge.In this research,the melamine foam(MF)/polypyrrole(PPy)nanowire arrays(MF@PPy)were fabricated via one-step electrochemical polymerization.The hierarchical MF@PPy foam was composed of three-dimensional PPy micro-skeleton and ordered PPy nanowire arrays.Due to the upwardly grown PPy nanowire arrays,the MF@PPy foam possessed good hydrophobicity ability with a water contact angle of 142.00°and outstanding stability under various harsh environments.Meanwhile,the MF@PPy foam showed excellent thermal insulation property on account of the low thermal conductivity and elongated ligament characteristic of PPy nanowire arrays.Furthermore,taking advantage of the high conductivity(128.2 S m^(-1)),the MF@PPy foam exhibited rapid Joule heating under 3 V,resulting in dynamic infrared stealth and thermal camouflage effects.More importantly,the MF@PPy foam exhibited remarkable EMI shielding effectiveness values of 55.77 dB and 19,928.57 dB cm^(2)g^(-1).Strong EMI shielding was put down to the hierarchically porous PPy structure,which offered outstanding impedance matching,conduction loss,and multiple attenuations.This innovative approach provides significant insights to the development of advanced multifunctional EMI shielding foams by constructing PPy nanowire arrays,showing great applications in both military and civilian fields.
基金funded by the Deanship of Graduate Studies and Scientific Research at Jouf University under Grant Number(DGSSR-2023-02-02513).
文摘Spear Phishing Attacks(SPAs)pose a significant threat to the healthcare sector,resulting in data breaches,financial losses,and compromised patient confidentiality.Traditional defenses,such as firewalls and antivirus software,often fail to counter these sophisticated attacks,which target human vulnerabilities.To strengthen defenses,healthcare organizations are increasingly adopting Machine Learning(ML)techniques.ML-based SPA defenses use advanced algorithms to analyze various features,including email content,sender behavior,and attachments,to detect potential threats.This capability enables proactive security measures that address risks in real-time.The interpretability of ML models fosters trust and allows security teams to continuously refine these algorithms as new attack methods emerge.Implementing ML techniques requires integrating diverse data sources,such as electronic health records,email logs,and incident reports,which enhance the algorithms’learning environment.Feedback from end-users further improves model performance.Among tested models,the hierarchical models,Convolutional Neural Network(CNN)achieved the highest accuracy at 99.99%,followed closely by the sequential Bidirectional Long Short-Term Memory(BiLSTM)model at 99.94%.In contrast,the traditional Multi-Layer Perceptron(MLP)model showed an accuracy of 98.46%.This difference underscores the superior performance of advanced sequential and hierarchical models in detecting SPAs compared to traditional approaches.
基金the National Natural Science Foundation of China(Nos.52102036 and52301192)the Sichuan Science and Technology Program,China(No.2021JDRC0099)+3 种基金Taishan Scholars and Young Experts Program of Shandong Province,China(No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution,China(Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province,China(Structural Design of High-efficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams)“Sanqin Scholars”Innovation Teams Project of Shaanxi Province,China(Clean Energy Materials and High-Performance Devices Innovation Team of Shaanxi Dongling Smelting Co.,Ltd.)。
文摘Bioderived carbon materials have garnered considerable interest in the fields of microwave absorption and shielding due to their reproducibility and environmental friendliness.In this study,KOH was evenly distributed on biomass Tremella using the swelling induction method,leading to the preparation of a three-dimensional network-structured hierarchical porous carbon(HPC)through carbonization.The achieved microwave absorption intensity is robust at-47.34 dB with a thin thickness of 2.1 mm.Notably,the widest effective absorption bandwidth,reaching 7.0 GHz(11–18 GHz),is attained at a matching thickness of 2.2 mm.The exceptional broadband and reflection loss performance are attributed to the 3D porous networks,interface effects,carbon network defects,and dipole relaxation.HPC has outstanding absorption characteristics due to its excellent impedance matching and high attenuation constant.The uniform pore structures considerably optimize the impedance-matching performance of the material,while the abundance of interfaces and defects enhances the dielectric loss,thereby improving the attenuation constant.Furthermore,the impact of carbonization temperature and swelling rate on microwave absorption performance was systematically investigated.This research presents a strategy for preparing absorbing materials using biomass-derived HPC,showcasing considerable potential in the field of electromagnetic wave absorption.
基金funded by the National Natural Science Foundation of China(No.51873004).
文摘Materials exhibiting high-performance electromagnetic wave absorption have garnered considerable scientific and technological attention,yet encounter significant challenges.Developing new materials and innovative structural design concepts is crucial for expanding the application field of electromagnetic wave absorption.Particularly,hierarchical structure engineering has emerged as a promising approach to enhance the physical and chemical properties of materials,providing immense potential for creating versatile electromagnetic wave absorption materials.Herein,an exceptional multi-dimensional hierarchical structure was meticulously devised,unleashing the full microwave attenuation capabilities through in situ growth,selfreduction,and multi-heterogeneous interface integration.The hierarchical structure features a three-dimensional carbon framework,where magnetic nanoparticles grow in situ on the carbon skeleton,creating a necklace-like structure.Furthermore,magnetic nanosheets assemble within this framework.Enhanced impedance matching was achieved by precisely adjusting component proportions,and intelligent integration of diverse interfaces bolstered dielectric polarization.The obtain Fe_(3)O_(4)-Fe nanoparticles/carbon nanofibers/Al-Fe_(3)O_(4)-Fe nanosheets composites demonstrated outstanding performance with a minimum reflection loss(RLmin)value of−59.3 dB and an effective absorption bandwidth(RL≤−10 dB)extending up to 5.6 GHz at 2.2 mm.These notable accomplishments offer fresh insights into the precision design of high-efficient electromagnetic wave absorption materials.
基金financial support from National Key R&D Program of China(MoST,2020YFA0711500)the National Natural Science Foundation of China(NSFC,21875114),(NSFC,52303348)+1 种基金111 Project(B18030)“The Fundamental Research Funds for the Central Universities”,Nankai University.
文摘Two-dimensional carbon-based materials have shown promising electromagnetic wave absorption capabilities in mid-and high-frequency ranges,but face challenges in low-frequency absorption due to limited control over polarization response mecha-nisms and ambiguous resonance behavior.In this study,we pro-pose a novel approach to enhance absorption efficiency in aligned three-dimensional(3D)MXene/CNF(cellulose nanofibers)cavities by modifying polarization properties and manipulating resonance response in the 3D MXene architecture.This controlled polarization mechanism results in a significant shift of the main absorption region from the X-band to the S-band,leading to a remarkable reflection loss value of-47.9 dB in the low-frequency range.Furthermore,our findings revealed the importance of the oriented electromagnetic coupling in influencing electromagnetic response and microwave absorption properties.The present study inspired us to develop a generic strategy for low-frequency tuned absorption in the absence of magnetic element participation,while orientation-induced polarization and the derived magnetic resonance coupling are the key controlling factors of the method.
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金supported by The National Natural Science Foundation of China(22276137,52170087)the Fundamental Research Funds for the Central Universities(XJEDU2023Z009).
文摘Despite the promising potential of transition metal oxides(TMOs)as capacitive deionization(CDI)electrodes,the actual capacity of TMOs electrodes for sodium storage is significantly lower than the theoretical capacity,posing a major obstacle.Herein,we prepared the kinetically favorable Zn_(x)Ni_(1−x)O electrode in situ growth on carbon felt(Zn_(x)Ni_(1−x)O@CF)through constraining the rate of OH^(−)generation in the hydrothermal method.Zn_(x)Ni_(1−x)O@CF exhibited a high-density hierarchical nanosheet structure with three-dimensional open pores,benefitting the ion transport/electron transfer.And tuning the moderate amount of redox-inert Zn-doping can enhance surface electroactive sites,actual activity of redox-active Ni species,and lower adsorption energy,promoting the adsorption kinetic and thermodynamic of the Zn_(0.2)Ni_(0.8)O@CF.Benefitting from the kinetic-thermodynamic facilitation mechanism,Zn_(0.2)Ni_(0.8)O@CF achieved ultrahigh desalination capacity(128.9 mgNaCl g^(-1)),ultra-low energy consumption(0.164 kW h kgNaCl^(-1)),high salt removal rate(1.21 mgNaCl g^(-1) min^(-1)),and good cyclability.The thermodynamic facilitation and Na^(+)intercalation mechanism of Zn_(0.2)Ni_(0.8)O@CF are identified by the density functional theory calculations and electrochemical quartz crystal microbalance with dissipation monitoring,respectively.This research provides new insights into controlling electrochemically favorable morphology and demonstrates that Zn-doping,which is redox-inert,is essential for enhancing the electrochemical performance of CDI electrodes.
基金The financial supports from the National Natural Science Foundation of China (22178059, 22208054 and 22072019)Natural Science Foundation of Fujian Province, China (2020J01513)+1 种基金Sinochem Quanzhou Energy Technology Co., Ltd. (ZHQZKJ-19-F-ZS0076)Qingyuan Innovation Laboratory (00121002)
文摘Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.
基金support from the National Natural Science Foundation of China(22073033,21873032,21673087,21903032)startup fund(2006013118 and 3004013105)from Huazhong University of Science and Technology+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyRCPY116)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)
文摘In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.
基金financially supported by National Natural Science Foundation of China(Nos.U22A20193 and 51975218)Fundamental Research Funds for the Central Universities(No.2022ZYGXZR101)
文摘Printed micro-supercapacitors(MSCs)have shown broad prospect in flexible and wearable electronics.Most of previous studies focused on printing the electrochemically active materials paying less attention to other key components like current collectors and electrolytes.This study presents an allprinting strategy to fabricate in-plane flexible and substrate-free MSCs with hierarchical encapsulation.This new type of“all-in-one”MSC is constructed by encapsulating the in-plane interdigital current collectors and electrodes within the polyvinyl-alcohol-based hydrogel electrolyte via sequential printing.The bottom electrolyte layer of this fully printed MSCs helps protect the device from the limitation of conventional substrate,showing excellent flexibility.The MSCs maintain a high capacitance retention of 96.84%even in a completely folded state.An optimal electrochemical performance can be achieved by providing ample and shorter transport paths for ions.The MSCs using commercial activated carbon as the active material are endowed with a high specific areal capacitance of 1892.90 mF cm^(-2)at a current density of 0.3 mA cm^(-2),and an outstanding volumetric energy density of 9.20 mWh cm^(-3)at a volumetric power density of 6.89 mW cm^(-3).For demonstration,a thermo-hygrometer is stably powered by five MSCs which are connected in series and wrapped onto a glass rod.This low-cost and versatile all-printing strategy is believed to diversify the application fields of MSCs with high capacitance and excellent flexibility.
基金financially supported by the National Natural Science Foundation of China(52102223,51920105004)。
文摘Antimony(Sb)-ba sed anode materials are feasible candidates for sodium-ion batteries(SIBs) due to their high theoretical specific capacity and excellent electrical conductivity.However,they still suffer from volume distortion,structural collapse,and ionic conduction interruption upon cycling.Herein,a hierarchical array-like nanofiber structure was designed to address these limitations by combining architecture engineering and anion tuning strategy,in which SbPO_(4-x) with oxygen vacancy nanosheet arrays are anchored on the surface of interwoven carbon nanofibers(SbPO_(4-x)@CNFs).In particular,bulky PO_(4)^(3-) anions mitigate the large volume distortion and generate Na_(3)PO_(4) with high ionic conductivity,collectively improving cyclic stability and ionic transport efficiency.The abundant oxygen vacancies substantially boost the intrinsic electronic conductivity of SbPO_4,further accelerating the reaction dynamics.In addition,hierarchical fibrous structures provide abundant active sites,construct efficient conducting networks,and enhance the electron/ion transport capacity.Benefiting from the advanced structural design,the SbPO_(4-x)@CNFs electrodes exhibit outstanding cycling stability(1000 cycles at 1.0 A g^(-1) with capacity decay of 0.05% per cycle) and rapid sodium storage performance(293.8 mA h g^(-1) at 5.0 A g^(-1)).Importantly,systematic in-/ex-situ techniques have revealed the "multi-step conversion-alloying" reaction process and the "battery-capacitor dual-mode" sodium-storage mechanism.This work provides valuable insights into the design of anode materials for advanced SIBs with elevated stability and superior rate performance.
基金National Natural Science Foundation of China,Grant/Award Numbers:52102260,52171211,51972220,61903235,U22A20145Shandong Provincial Natural Science Foundation,Grant/Award Numbers:ZR2020QB069,ZR2022ME051+4 种基金National Key Research and Development Program of China,Grant/Award Number:2022YFB4002004Scientific and Technological Innovation Ability Improvement Project of Minor Enterprises in Shandong Province,Grant/Award Number:2022TSGC1021Announce the List and Take Charge Project in Jinan,Grant/Award Number:202214012Major innovation project for integrating science,education and industry of Qilu University of Technology (Shandong Academy of Sciences),Grant/Award Numbers:2022JBZ01-07,2022PY044China Postdoctoral Science Foundation,Grant/Award Number:2022M711545。
文摘Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.
基金the National Key Research and Development Program of China(2022YFB3805800)the National Natural Science Foundation of China(52173059 and U21A2095)+2 种基金the Postgraduate Research and Practice Innovation Program of Jiangsu Province(KYCX223203)the Major Basic Research Project of the Natural Science Foundation of the Jiangsu Higher Education Institutions(21KJA540002)the Key Research and Development Program of Hubei Province(2021BAA068).
文摘Chemical resistant textiles are vital for safeguarding humans against chemical hazards in various settings.such as industrialproduction,chemicalaccidents,laboratory activities,and road transportation.However,the ideal integration of chemical resistance,thermal and moisture management,and wearer condition monitoring in conventional chemically protective textiles remains challenging.Herein,the design,manufacturing,and use of stretchable hierarchical core-shell yarns(HCSYs)for integrated chemical resistance,moisture regulation,and smart sensing textiles are demonstrated.These yarns con-tain helically elastic spandex,wrapped silver-plated nylon,and surface-structuredpolytetrafluo-roethylene(PTFE)yarns and are designed and manufactured based on a scalable fabrication process.In addition to their ideal chemical resistance performance,HCSYs can function as multifunctional stretch-able electronics for real-time human motion monitoring and as the basic element of intelligent textiles.Furthermore,a desirable dynamic thermoregulation function is achieved by exploiting the fabric structure with stretching modulation.Our HCSYs may provide prospective opportunities for the future development of smart protective textiles with high durability,flexibility,and scalability.
基金financially supported by the Certificate of postdoctoral research grant in Henan province,the Natural Science Foundation of Henan province(Grant No.212300410281)the National Natural Science Foundation of China(Grant No.21975225).
文摘Lithium-sulfur batteries(LSBs)with high energy densities have been demonstrated the potential for energy-intensive demand applications.However,their commercial applicability is hampered by hysteretic electrode reaction kinetics and the shuttle effect of lithium polysulfides(LiPSs).In this work,an interlayer consisting of high-entropy metal oxide(Cu_(0.7)Fe_(0.6)Mn_(0.4)Ni_(0.6)Sn_(0.5))O_(4) grown on carbon nanofibers(HEO/CNFs)is designed for LSBs.The CNFs with highly porous networks provide transport pathways for Li^(+) and e^(-),as well as a physical sieve effect to limit LiPSs crossover.In particular,the grapevine-like HEO nanoparticles generate metal-sulfur bonds with LiPSs,efficiently anchoring active materials.The unique structure and function of the interlayer enable the LSBs with superior electrochemical performance,i.e.,the high specific capacity of 1381 mAh g^(-1) at 0.1 C and 561 mAh g^(-1) at 6 C.This work presents a facile strategy for exploiting high-performance LSBs.
文摘This paper develops a novel hierarchical control strategy for improving the trajectory tracking capability of aerial robots under parameter uncertainties.The hierarchical control strategy is composed of an adaptive sliding mode controller and a model-free iterative sliding mode controller(MFISMC).A position controller is designed based on adaptive sliding mode control(SMC)to safely drive the aerial robot and ensure fast state convergence under external disturbances.Additionally,the MFISMC acts as an attitude controller to estimate the unmodeled dynamics without detailed knowledge of aerial robots.Then,the adaption laws are derived with the Lyapunov theory to guarantee the asymptotic tracking of the system state.Finally,to demonstrate the performance and robustness of the proposed control strategy,numerical simulations are carried out,which are also compared with other conventional strategies,such as proportional-integralderivative(PID),backstepping(BS),and SMC.The simulation results indicate that the proposed hierarchical control strategy can fulfill zero steady-state error and achieve faster convergence compared with conventional strategies.
