The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving c...The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.展开更多
Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst...Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.展开更多
Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturin...Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturing was employed to fabricate pure Zn with a heterogeneous microstructure and exceptional strength-ductility synergy.An optimized processing window of LPBF was established for printing Zn samples with relative densities greater than 99%using a laser power range of 80∼90 W and a scanning speed of 900 mm s−1.The Zn sample printed with a power of 80 W at a speed of 900 mm s−1 exhibited a hierarchical heterogeneous microstructure consisting of millimeter-scale molten pool boundaries,micrometer-scale bimodal grains,and nanometer-scale pre-existing dislocations,due to rapid cooling rates and significant thermal gradients formed in the molten pools.The printed sample exhibited the highest ductility of∼12.1%among all reported LPBF-printed pure Zn to date with appreciable ultimate tensile strength(∼128.7 MPa).Such superior strength-ductility synergy can be attributed to the presence of multiple deformation mechanisms that are primarily governed by heterogeneous deformation-induced hardening resulting from the alternative arrangement of bimodal Zn grains with pre-existing dislocations.Additionally,continuous strain hardening was facilitated through the interactions between deformation twins,grains and dislocations as strain accumulated,further contributing to the superior strength-ductility synergy.These findings provide valuable insights into the deformation behavior and mechanisms underlying exceptional mechanical properties of LPBF-printed Zn and its alloys for implant applications.展开更多
Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT...Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.展开更多
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec...Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.展开更多
The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which ...The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which not only provides the optical gain which is absent from native Si substrates and enables complete photonic functionalities on chip,but also improves the system performance through advanced heterogeneous integrated packaging.This paper reviews recent progress of silicon-based optoelectronic heterogeneous integration in high performance optical interconnection.The research status,development trend and application of ultra-low loss optical waveguides,high-speed detectors,high-speed modulators,lasers and 2D,2.5D,3D and monolithic integration are focused on.展开更多
Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete hetero...Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete heterogeneous neuron networks are rarely reported.In this study,a new four-stable discrete locally active memristor is proposed and its nonvolatile and locally active properties are verified by its power-off plot and DC V–I diagram.Based on two-dimensional(2D)discrete Izhikevich neuron and 2D discrete Chialvo neuron,a heterogeneous discrete neuron network is constructed by using the proposed discrete memristor as a coupling synapse connecting the two heterogeneous neurons.Considering the coupling strength as the control parameter,chaotic firing,periodic firing,and hyperchaotic firing patterns are revealed.In particular,multiple coexisting firing patterns are observed,which are induced by different initial values of the memristor.Phase synchronization between the two heterogeneous neurons is discussed and it is found that they can achieve perfect synchronous at large coupling strength.Furthermore,the effect of Gaussian white noise on synchronization behaviors is also explored.We demonstrate that the presence of noise not only leads to the transition of firing patterns,but also achieves the phase synchronization between two heterogeneous neurons under low coupling strength.展开更多
Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveragi...Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.展开更多
Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,...Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,and supply chain management.Blockchain interactions in the heterogeneous network have fascinated more attention due to the authentication of their digital application exchanges.However,the exponential development of storage space capabilities across the blockchain-based heterogeneous network has become an important issue in preventing blockchain distribution and the extension of blockchain nodes.There is the biggest challenge of data integrity and scalability,including significant computing complexity and inapplicable latency on regional network diversity,operating system diversity,bandwidth diversity,node diversity,etc.,for decision-making of data transactions across blockchain-based heterogeneous networks.Data security and privacy have also become the main concerns across the heterogeneous network to build smart IoT ecosystems.To address these issues,today’s researchers have explored the potential solutions of the capability of heterogeneous network devices to perform data transactions where the system stimulates their integration reliably and securely with blockchain.The key goal of this paper is to conduct a state-of-the-art and comprehensive survey on cybersecurity enhancement using blockchain in the heterogeneous network.This paper proposes a full-fledged taxonomy to identify the main obstacles,research gaps,future research directions,effective solutions,andmost relevant blockchain-enabled cybersecurity systems.In addition,Blockchain based heterogeneous network framework with cybersecurity is proposed in this paper tomeet the goal of maintaining optimal performance data transactions among organizations.Overall,this paper provides an in-depth description based on the critical analysis to overcome the existing work gaps for future research where it presents a potential cybersecurity design with key requirements of blockchain across a heterogeneous network.展开更多
Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,h...Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.展开更多
A significant obstacle in intelligent transportation systems(ITS)is the capacity to predict traffic flow.Recent advancements in deep neural networks have enabled the development of models to represent traffic flow acc...A significant obstacle in intelligent transportation systems(ITS)is the capacity to predict traffic flow.Recent advancements in deep neural networks have enabled the development of models to represent traffic flow accurately.However,accurately predicting traffic flow at the individual road level is extremely difficult due to the complex interplay of spatial and temporal factors.This paper proposes a technique for predicting short-term traffic flow data using an architecture that utilizes convolutional bidirectional long short-term memory(Conv-BiLSTM)with attention mechanisms.Prior studies neglected to include data pertaining to factors such as holidays,weather conditions,and vehicle types,which are interconnected and significantly impact the accuracy of forecast outcomes.In addition,this research incorporates recurring monthly periodic pattern data that significantly enhances the accuracy of forecast outcomes.The experimental findings demonstrate a performance improvement of 21.68%when incorporating the vehicle type feature.展开更多
With the development of intelligent and interconnected traffic system,a convergence of traffic stream is anticipated in the foreseeable future,where both connected automated vehicle(CAV)and human driven vehicle(HDV)wi...With the development of intelligent and interconnected traffic system,a convergence of traffic stream is anticipated in the foreseeable future,where both connected automated vehicle(CAV)and human driven vehicle(HDV)will coexist.In order to examine the effect of CAV on the overall stability and energy consumption of such a heterogeneous traffic system,we first take into account the interrelated perception of distance and speed by CAV to establish a macroscopic dynamic model through utilizing the full velocity difference(FVD)model.Subsequently,adopting the linear stability theory,we propose the linear stability condition for the model through using the small perturbation method,and the validity of the heterogeneous model is verified by comparing with the FVD model.Through nonlinear theoretical analysis,we further derive the KdV-Burgers equation,which captures the propagation characteristics of traffic density waves.Finally,by numerical simulation experiments through utilizing a macroscopic model of heterogeneous traffic flow,the effect of CAV permeability on the stability of density wave in heterogeneous traffic flow and the energy consumption of the traffic system is investigated.Subsequent analysis reveals emergent traffic phenomena.The experimental findings demonstrate that as CAV permeability increases,the ability to dampen the propagation of fluctuations in heterogeneous traffic flow gradually intensifies when giving system perturbation,leading to enhanced stability of the traffic system.Furthermore,higher initial traffic density renders the traffic system more susceptible to congestion,resulting in local clustering effect and stop-and-go traffic phenomenon.Remarkably,the total energy consumption of the heterogeneous traffic system exhibits a gradual decline with CAV permeability increasing.Further evidence has demonstrated the positive influence of CAV on heterogeneous traffic flow.This research contributes to providing theoretical guidance for future CAV applications,aiming to enhance urban road traffic efficiency and alleviate congestion.展开更多
Heterogeneous catalysis remains at the core of various bulk chemical manufacturing and energy conversion processes,and its revolution necessitates the hunt for new materials with ideal catalytic activities and economi...Heterogeneous catalysis remains at the core of various bulk chemical manufacturing and energy conversion processes,and its revolution necessitates the hunt for new materials with ideal catalytic activities and economic feasibility.Computational high-throughput screening presents a viable solution to this challenge,as machine learning(ML)has demonstrated its great potential in accelerating such processes by providing satisfactory estimations of surface reactivity with relatively low-cost information.This review focuses on recent progress in applying ML in adsorption energy prediction,which predominantly quantifies the catalytic potential of a solid catalyst.ML models that leverage inputs from different categories and exhibit various levels of complexity are classified and discussed.At the end of the review,an outlook on the current challenges and future opportunities of ML-assisted catalyst screening is supplied.We believe that this review summarizes major achievements in accelerating catalyst discovery through ML and can inspire researchers to further devise novel strategies to accelerate materials design and,ultimately,reshape the chemical industry and energy landscape.展开更多
The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(...The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(28)Al_(4)Ti_(3)Co_(3) immiscible high-entropy alloy(HEA)was developed.After vacuum arc melting and copper mold suction casting,this HEA exhibits a unique phase separation microstructure,which consists of striped Cu-rich regions and Fe-rich region.Further magnification of the striped Cu-rich region reveals that it is composed of a Cu-rich dot-like phase and a Fe-rich region.The aging alloy is further strengthened by a L1_(2)-Ni_(3)(AlTi)nanoprecipitates,achieving excellent yield strength(1185 MPa)and uniform ductility(~8.8%).The differential distribution of the L1_(2) nanoprecipitate in the striped Cu-rich region and the external Fe-rich region increased the strength difference between these two regions,which increased the strain gradient and thus improved hetero-deformation induced(HDI)hardening.This work provides a new route to improve the HDI hardening of Fe-Cu alloys.展开更多
This paper studies the evolutionary process of cooperative behavior in a public goods game model with heterogeneous investment strategies in square lattices.In the proposed model,players are divided into defectors,coo...This paper studies the evolutionary process of cooperative behavior in a public goods game model with heterogeneous investment strategies in square lattices.In the proposed model,players are divided into defectors,cooperators and discreet investors.Among these,defectors do not participate in investing,discreet investors make heterogeneous investments based on the investment behavior and cooperation value of their neighbors,and cooperators invest equally in each neighbor.In real life,heterogeneous investment is often accompanied by time or economic costs.The discreet investors in this paper pay a certain price to obtain their neighbors'investment behavior and cooperation value,which quantifies the time and economic costs of the heterogeneous investment process.The results of Monte Carlo simulation experiments in this study show that discreet investors can effectively resist the invasion of the defectors,form a stable cooperative group and expand the cooperative advantage in evolution.However,when discreet investors pay too high a price,they lose their strategic advantage.The results in this paper help us understand the role of heterogeneous investment in promoting and maintaining human social cooperation.展开更多
Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electro...Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electrocatalysts,such as platinum(Pt),has been hindered by their high cost.In this study,we developed an easy-to-implement method to create ultrathin Pt nanomembranes,which catalyze HER at a cost significantly lower than commercial Pt/C and comparable to non-noble metal electrocatalysts.These Pt nanomembranes consist of highly distorted Pt nanocrystals and exhibit a heterogeneous elastic strain field,a characteristic rarely seen in conventional crystals.This unique feature results in significantly higher electrocatalytic efficiency than various forms of Pt electrocatalysts,including Pt/C,Pt foils,and numerous Pt singleatom or single-cluster catalysts.Our research offers a promising approach to develop highly efficient and cost-effective low-dimensional electrocatalysts for sustainable hydrogen production,potentially addressing the challenges posed by the climate crisis.展开更多
Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental friendliness.However,their widespread applications are imp...Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental friendliness.However,their widespread applications are impeded by basic components aggregation and low stability.In this work,we fabricate single calcium atoms on graphene(denoted as Ca1/G)by use of a redox strategy for the first time,producing solid strong base catalyst with high activity and stability.The precursor Ca(NO_(3))_(2)is first reduced to CaO at 400℃ by the support graphene,forming CaO/G with conventional basic sites,and the subsequent reduction at 850℃results in the generation of Ca1/G with atomically dispersed Ca.Various characterizations reveal that Ca single atoms are anchored on graphene in tetra-coordination(Ca-C_(2)-N_(2))where N is in situ doped from Ca(NO_(3))_(2).The atomically dispersed Ca,along with their anchoring on the support,endow Ca1/G with high activity and stability toward the transesterification reaction of ethylene carbonate with methanol.The turnover frequency value reaches 128.0 h^(-1)on Ca1/G,which is much higher than the traditional counterpart CaO/G and various reported solid strong bases(2.9-46.2 h^(-1)).Moreover,the activity of Ca1/G is well maintained during 5 cycles,while 60%of activity is lost for the conventional analogue CaO/G due to the leaching of Ca.展开更多
Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electro...Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.展开更多
The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we ...The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we propose an intelligent DHR architecture,which is more feasible by intelligently combining the random distribution based dynamic scheduling algorithm(RD-DS)and information weight and heterogeneity based arbitrament(IWHA)algorithm.In the proposed architecture,the random distribution function and information weight are employed to achieve the optimal selection of executors in the process of RD-DS,which avoids the case that some executors fail to be selected due to their stability difference in the conventional DHR architecture.Then,through introducing the heterogeneity to restrict the information weights in the procedure of the IWHA,the proposed architecture solves the common mode escape issue caused by the existence of multiple identical error output results of similar vulnerabilities.The experimental results characterize that the proposed architecture outperforms in heterogeneity,scheduling times,security,and stability over the conventional DHR architecture under the same conditions.展开更多
Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since ...Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since the low diffusivity ions such as Ti^(4+)will be concentrated on grain boundaries,which hinders the grain growth.In order to synthesize large single-crystal layered oxide cathodes,considering the different diffusivities of different dopant ions,we propose a simple two-step multi-element co-doping strategy to fabricate core–shell structured LiCoO_(2)(CS-LCO).In the current work,the high-diffusivity Al^(3+)/Mg^(2+)ions occupy the core of single-crystal grain while the low diffusivity Ti^(4+)ions enrich the shell layer.The Ti^(4+)-enriched shell layer(~12 nm)with Co/Ti substitution and stronger Ti–O bond gives rise to less oxygen ligand holes.In-situ XRD demonstrates the constrained contraction of c-axis lattice parameter and mitigated structural distortion.Under a high upper cut-off voltage of 4.6 V,the single-crystal CS-LCO maintains a reversible capacity of 159.8 mAh g^(−1)with a good retention of~89%after 300 cycles,and reaches a high specific capacity of 163.8 mAh g^(−1)at 5C.The proposed strategy can be extended to other pairs of low-(Zr^(4+),Ta^(5+),and W6+,etc.)and high-diffusivity cations(Zn^(2+),Ni^(2+),and Fe^(3+),etc.)for rational design of advanced layered oxide core–shell structured cathodes for lithium-ion batteries.展开更多
基金financial support from the King Abdullah University of Science and Technology(KAUST).
文摘The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.
基金the National Natural Science Foundation of China(22368014)the Guizhou Provincial S&T Project(ZK[2022]011,GCC[2023]011)+2 种基金the Natural Science Foundation of Guangxi Zhuang Autonomous Region(2023JJA120098)the Guangxi Key Laboratory of Green Chemical Materials and Safety Technology,the Beibu Gulf University(2022SYSZZ02,2022ZZKT04)the Guizhou Provincial Higher Education Institution Program(Qianjiaoji[2023]082)。
文摘Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.
基金National Natural Science Foundation of China (52305358)the Fundamental Research Funds for the Central Universities (2023ZYGXZR061)+3 种基金Guangdong Basic and Applied Basic Research Foundation (2022A1515010304)Science and Technology Program of Guangzhou (202201010362)Young Elite Scientists Sponsorship Program by CAST . (2023QNRC001)Young Talent Support Project of Guangzhou (QT-2023-001)
文摘Zinc(Zn)is considered a promising biodegradable metal for implant applications due to its appropriate degradability and favorable osteogenesis properties.In this work,laser powder bed fusion(LPBF)additive manufacturing was employed to fabricate pure Zn with a heterogeneous microstructure and exceptional strength-ductility synergy.An optimized processing window of LPBF was established for printing Zn samples with relative densities greater than 99%using a laser power range of 80∼90 W and a scanning speed of 900 mm s−1.The Zn sample printed with a power of 80 W at a speed of 900 mm s−1 exhibited a hierarchical heterogeneous microstructure consisting of millimeter-scale molten pool boundaries,micrometer-scale bimodal grains,and nanometer-scale pre-existing dislocations,due to rapid cooling rates and significant thermal gradients formed in the molten pools.The printed sample exhibited the highest ductility of∼12.1%among all reported LPBF-printed pure Zn to date with appreciable ultimate tensile strength(∼128.7 MPa).Such superior strength-ductility synergy can be attributed to the presence of multiple deformation mechanisms that are primarily governed by heterogeneous deformation-induced hardening resulting from the alternative arrangement of bimodal Zn grains with pre-existing dislocations.Additionally,continuous strain hardening was facilitated through the interactions between deformation twins,grains and dislocations as strain accumulated,further contributing to the superior strength-ductility synergy.These findings provide valuable insights into the deformation behavior and mechanisms underlying exceptional mechanical properties of LPBF-printed Zn and its alloys for implant applications.
基金the National Natural Science Foundation(No.52073187)NSAF Foundation(No.U2230202)for their financial support of this project+3 种基金National Natural Science Foundation(No.51721091)Programme of Introducing Talents of Discipline to Universities(No.B13040)State Key Laboratory of Polymer Materials Engineering(No.sklpme2022-2-03)support of China Scholarship Council
文摘Pre-polymerized vinyl trimethoxy silane(PVTMS)@MWCNT nano-aerogel system was constructed via radical polymerization,sol-gel transition and supercritical CO_(2)drying.The fabricated organic-inorganic hybrid PVTMS@MWCNT aerogel structure shows nano-pore size(30-40 nm),high specific surface area(559 m^(2)g^(−1)),high void fraction(91.7%)and enhanced mechanical property:(1)the nano-pore size is beneficial for efficiently blocking thermal conduction and thermal convection via Knudsen effect(beneficial for infrared(IR)stealth);(2)the heterogeneous interface was beneficial for IR reflection(beneficial for IR stealth)and MWCNT polarization loss(beneficial for electromagnetic wave(EMW)attenuation);(3)the high void fraction was beneficial for enhancing thermal insulation(beneficial for IR stealth)and EMW impedance match(beneficial for EMW attenuation).Guided by the above theoretical design strategy,PVTMS@MWCNT nano-aerogel shows superior EMW absorption property(cover all Ku-band)and thermal IR stealth property(ΔT reached 60.7℃).Followed by a facial combination of the above nano-aerogel with graphene film of high electrical conductivity,an extremely high electromagnetic interference shielding material(66.5 dB,2.06 mm thickness)with superior absorption performance of an average absorption-to-reflection(A/R)coefficient ratio of 25.4 and a low reflection bandwidth of 4.1 GHz(A/R ratio more than 10)was experimentally obtained in this work.
基金supported by the National Natural Science Foundation of China(52272194)Liaoning Revitalization Talents Program(XLYC2007155)。
文摘Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.
基金Project supported in part by the National Key Research and Development Program of China(Grant No.2021YFB2206504)the National Natural Science Foundation of China(Grant No.62235017)the China Postdoctoral Science Foundation(Grant No.2021M703125).
文摘The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which not only provides the optical gain which is absent from native Si substrates and enables complete photonic functionalities on chip,but also improves the system performance through advanced heterogeneous integrated packaging.This paper reviews recent progress of silicon-based optoelectronic heterogeneous integration in high performance optical interconnection.The research status,development trend and application of ultra-low loss optical waveguides,high-speed detectors,high-speed modulators,lasers and 2D,2.5D,3D and monolithic integration are focused on.
基金Project supported by the National Natural Science Foundations of China(Grant Nos.62171401 and 62071411).
文摘Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete heterogeneous neuron networks are rarely reported.In this study,a new four-stable discrete locally active memristor is proposed and its nonvolatile and locally active properties are verified by its power-off plot and DC V–I diagram.Based on two-dimensional(2D)discrete Izhikevich neuron and 2D discrete Chialvo neuron,a heterogeneous discrete neuron network is constructed by using the proposed discrete memristor as a coupling synapse connecting the two heterogeneous neurons.Considering the coupling strength as the control parameter,chaotic firing,periodic firing,and hyperchaotic firing patterns are revealed.In particular,multiple coexisting firing patterns are observed,which are induced by different initial values of the memristor.Phase synchronization between the two heterogeneous neurons is discussed and it is found that they can achieve perfect synchronous at large coupling strength.Furthermore,the effect of Gaussian white noise on synchronization behaviors is also explored.We demonstrate that the presence of noise not only leads to the transition of firing patterns,but also achieves the phase synchronization between two heterogeneous neurons under low coupling strength.
基金financial support from the Swiss National Science Foundation via the Southeast Asia–Europe Joint Funding Scheme 2020(Grant No.IZJFZ2_202476)funding from the National Natural Science Foundation of China(Grant Nos.22209118 and 00301054A1073)the Fundamental Research Funds for the Central Universities(Grant Nos.1082204112A26,20826044D3083,and 20822041G4080)。
文摘Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.
基金The authors would like to acknowledge the Institute for Big Data Analytics and Artificial Intelligence(IBDAAI),Universiti TeknologiMARA and the Ministry of Higher Education,Malaysia for the financial support through Fundamental Research Grant Scheme(FRGS)Grant No.FRGS/1/2021/ICT11/UITM/01/1.
文摘Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,and supply chain management.Blockchain interactions in the heterogeneous network have fascinated more attention due to the authentication of their digital application exchanges.However,the exponential development of storage space capabilities across the blockchain-based heterogeneous network has become an important issue in preventing blockchain distribution and the extension of blockchain nodes.There is the biggest challenge of data integrity and scalability,including significant computing complexity and inapplicable latency on regional network diversity,operating system diversity,bandwidth diversity,node diversity,etc.,for decision-making of data transactions across blockchain-based heterogeneous networks.Data security and privacy have also become the main concerns across the heterogeneous network to build smart IoT ecosystems.To address these issues,today’s researchers have explored the potential solutions of the capability of heterogeneous network devices to perform data transactions where the system stimulates their integration reliably and securely with blockchain.The key goal of this paper is to conduct a state-of-the-art and comprehensive survey on cybersecurity enhancement using blockchain in the heterogeneous network.This paper proposes a full-fledged taxonomy to identify the main obstacles,research gaps,future research directions,effective solutions,andmost relevant blockchain-enabled cybersecurity systems.In addition,Blockchain based heterogeneous network framework with cybersecurity is proposed in this paper tomeet the goal of maintaining optimal performance data transactions among organizations.Overall,this paper provides an in-depth description based on the critical analysis to overcome the existing work gaps for future research where it presents a potential cybersecurity design with key requirements of blockchain across a heterogeneous network.
基金financial support from the Chang Jiang Scholars Program (51073047)the National Natural Science Foundation of China (51773049)+5 种基金the China Aerospace Science and Technology Corporation-Harbin Institute of Technology Joint Center for Technology Innovation Fund (HIT15-1A01)the Harbin City Science and Technology Projects (2013DB4BP031 and RC2014QN017035)the Natural Science Foundation of Shandong Province of China (ZR2023QE071)the College Students’ Innovation and Entrepreneurship Training Program Projects of Shandong Province (S202211065048)the Scientific Research Foundation of Qingdao University (DC1900009425)the China Postdoctoral Science Foundation (2022TQ0282)
文摘Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.
文摘A significant obstacle in intelligent transportation systems(ITS)is the capacity to predict traffic flow.Recent advancements in deep neural networks have enabled the development of models to represent traffic flow accurately.However,accurately predicting traffic flow at the individual road level is extremely difficult due to the complex interplay of spatial and temporal factors.This paper proposes a technique for predicting short-term traffic flow data using an architecture that utilizes convolutional bidirectional long short-term memory(Conv-BiLSTM)with attention mechanisms.Prior studies neglected to include data pertaining to factors such as holidays,weather conditions,and vehicle types,which are interconnected and significantly impact the accuracy of forecast outcomes.In addition,this research incorporates recurring monthly periodic pattern data that significantly enhances the accuracy of forecast outcomes.The experimental findings demonstrate a performance improvement of 21.68%when incorporating the vehicle type feature.
基金Project supported by the Fundamental Research Funds for Central Universities,China(Grant No.2022YJS065)the National Natural Science Foundation of China(Grant Nos.72288101 and 72371019).
文摘With the development of intelligent and interconnected traffic system,a convergence of traffic stream is anticipated in the foreseeable future,where both connected automated vehicle(CAV)and human driven vehicle(HDV)will coexist.In order to examine the effect of CAV on the overall stability and energy consumption of such a heterogeneous traffic system,we first take into account the interrelated perception of distance and speed by CAV to establish a macroscopic dynamic model through utilizing the full velocity difference(FVD)model.Subsequently,adopting the linear stability theory,we propose the linear stability condition for the model through using the small perturbation method,and the validity of the heterogeneous model is verified by comparing with the FVD model.Through nonlinear theoretical analysis,we further derive the KdV-Burgers equation,which captures the propagation characteristics of traffic density waves.Finally,by numerical simulation experiments through utilizing a macroscopic model of heterogeneous traffic flow,the effect of CAV permeability on the stability of density wave in heterogeneous traffic flow and the energy consumption of the traffic system is investigated.Subsequent analysis reveals emergent traffic phenomena.The experimental findings demonstrate that as CAV permeability increases,the ability to dampen the propagation of fluctuations in heterogeneous traffic flow gradually intensifies when giving system perturbation,leading to enhanced stability of the traffic system.Furthermore,higher initial traffic density renders the traffic system more susceptible to congestion,resulting in local clustering effect and stop-and-go traffic phenomenon.Remarkably,the total energy consumption of the heterogeneous traffic system exhibits a gradual decline with CAV permeability increasing.Further evidence has demonstrated the positive influence of CAV on heterogeneous traffic flow.This research contributes to providing theoretical guidance for future CAV applications,aiming to enhance urban road traffic efficiency and alleviate congestion.
基金supported by the National Natural Science Foundation of China(22109020 and 22109082).
文摘Heterogeneous catalysis remains at the core of various bulk chemical manufacturing and energy conversion processes,and its revolution necessitates the hunt for new materials with ideal catalytic activities and economic feasibility.Computational high-throughput screening presents a viable solution to this challenge,as machine learning(ML)has demonstrated its great potential in accelerating such processes by providing satisfactory estimations of surface reactivity with relatively low-cost information.This review focuses on recent progress in applying ML in adsorption energy prediction,which predominantly quantifies the catalytic potential of a solid catalyst.ML models that leverage inputs from different categories and exhibit various levels of complexity are classified and discussed.At the end of the review,an outlook on the current challenges and future opportunities of ML-assisted catalyst screening is supplied.We believe that this review summarizes major achievements in accelerating catalyst discovery through ML and can inspire researchers to further devise novel strategies to accelerate materials design and,ultimately,reshape the chemical industry and energy landscape.
基金Projects(52001083,52171111,U2141207)supported by the National Natural Science Foundation of ChinaProject(LH2020E060)supported by the Natural Science Foundation of Heilongjiang,China。
文摘The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(28)Al_(4)Ti_(3)Co_(3) immiscible high-entropy alloy(HEA)was developed.After vacuum arc melting and copper mold suction casting,this HEA exhibits a unique phase separation microstructure,which consists of striped Cu-rich regions and Fe-rich region.Further magnification of the striped Cu-rich region reveals that it is composed of a Cu-rich dot-like phase and a Fe-rich region.The aging alloy is further strengthened by a L1_(2)-Ni_(3)(AlTi)nanoprecipitates,achieving excellent yield strength(1185 MPa)and uniform ductility(~8.8%).The differential distribution of the L1_(2) nanoprecipitate in the striped Cu-rich region and the external Fe-rich region increased the strength difference between these two regions,which increased the strain gradient and thus improved hetero-deformation induced(HDI)hardening.This work provides a new route to improve the HDI hardening of Fe-Cu alloys.
基金Project supported by the Open Foundation of Key Laboratory of Software Engineering of Yunnan Province(Grant Nos.2020SE308 and 2020SE309).
文摘This paper studies the evolutionary process of cooperative behavior in a public goods game model with heterogeneous investment strategies in square lattices.In the proposed model,players are divided into defectors,cooperators and discreet investors.Among these,defectors do not participate in investing,discreet investors make heterogeneous investments based on the investment behavior and cooperation value of their neighbors,and cooperators invest equally in each neighbor.In real life,heterogeneous investment is often accompanied by time or economic costs.The discreet investors in this paper pay a certain price to obtain their neighbors'investment behavior and cooperation value,which quantifies the time and economic costs of the heterogeneous investment process.The results of Monte Carlo simulation experiments in this study show that discreet investors can effectively resist the invasion of the defectors,form a stable cooperative group and expand the cooperative advantage in evolution.However,when discreet investors pay too high a price,they lose their strategic advantage.The results in this paper help us understand the role of heterogeneous investment in promoting and maintaining human social cooperation.
基金The research of YY is supported by the Research Grant Council(RGC)through the General Research Fund(GRF)with the grant number N_CityU 109/21,CityU11213118 and CityU11209317.
文摘Hydrogen production through hydrogen evolution reaction(HER)offers a promising solution to combat climate change by replacing fossil fuels with clean energy sources.However,the widespread adoption of efficient electrocatalysts,such as platinum(Pt),has been hindered by their high cost.In this study,we developed an easy-to-implement method to create ultrathin Pt nanomembranes,which catalyze HER at a cost significantly lower than commercial Pt/C and comparable to non-noble metal electrocatalysts.These Pt nanomembranes consist of highly distorted Pt nanocrystals and exhibit a heterogeneous elastic strain field,a characteristic rarely seen in conventional crystals.This unique feature results in significantly higher electrocatalytic efficiency than various forms of Pt electrocatalysts,including Pt/C,Pt foils,and numerous Pt singleatom or single-cluster catalysts.Our research offers a promising approach to develop highly efficient and cost-effective low-dimensional electrocatalysts for sustainable hydrogen production,potentially addressing the challenges posed by the climate crisis.
基金supported by the National Science Fund for Distinguished Young Scholars(22125804)the National Natural Science Foundation of China(22078155 and 22178163)the National Students'platform for innovation and entrepreneurship training program(20210291013Z).
文摘Solid strong base catalysts are highly attractive for diverse reactions owing to their advantages of neglectable corrosion,facile separation,and environmental friendliness.However,their widespread applications are impeded by basic components aggregation and low stability.In this work,we fabricate single calcium atoms on graphene(denoted as Ca1/G)by use of a redox strategy for the first time,producing solid strong base catalyst with high activity and stability.The precursor Ca(NO_(3))_(2)is first reduced to CaO at 400℃ by the support graphene,forming CaO/G with conventional basic sites,and the subsequent reduction at 850℃results in the generation of Ca1/G with atomically dispersed Ca.Various characterizations reveal that Ca single atoms are anchored on graphene in tetra-coordination(Ca-C_(2)-N_(2))where N is in situ doped from Ca(NO_(3))_(2).The atomically dispersed Ca,along with their anchoring on the support,endow Ca1/G with high activity and stability toward the transesterification reaction of ethylene carbonate with methanol.The turnover frequency value reaches 128.0 h^(-1)on Ca1/G,which is much higher than the traditional counterpart CaO/G and various reported solid strong bases(2.9-46.2 h^(-1)).Moreover,the activity of Ca1/G is well maintained during 5 cycles,while 60%of activity is lost for the conventional analogue CaO/G due to the leaching of Ca.
基金financially supported by the National Nature Science Foundation of Jiangsu Province(BK20221259)。
文摘Transition metal sulfides have high theoretical capacities and are considered as potential anode materials for sodium-ion batteries.However,due to low inherent conductivity and significant volume expansion,the electrochemical performance is greatly limited.In this study,a nickel/manganese sulfide material(Ni_(0.96)S_(x)/MnS_(y)-NC)with adjustable sulfur vacancies and heterogeneous hollow spheres was prepared using a simple method.The introduction of a concentration-adjustable sulfur vacancy enables the generation of a heterogeneous interface between bimetallic sulfide and sulfur vacancies.This interface collectively creates an internal electric field,improving the mobility of electrons and ions,increasing the number of electrochemically active sites,and further optimizing the performance of Na~+storage.The direction of electron flow is confirmed by Density functional theory(DFT)calculations.The hollow nano-spherical material provides a buffer for expansion,facilitating rapid transfer kinetics.Our innovative discovery involves the interaction between the ether-based electrolyte and copper foil,leading to the formation of Cu_9S_5,which grafts the active material and copper current collector,reinforcing mechanical supporting.This results in a new heterostructure of Cu_9S_5 with Ni_(0.96)S_(x)/MnS_(y),contributing to the stabilization of structural integrity for long-cycle performance.Therefore,Ni_(0.96)S_(x)/MnS_(y)-NC exhibits excellent electrochemical properties following our modification route.Regarding stability performance,Ni0_(.96)S_(x)/MnS_(y)-NC demonstrates an average decay rate of 0.00944%after 10,000 cycles at an extremely high current density of 10000 mA g^(-1),A full cell with a high capacity of 304.2 mA h g^(-1)was also successfully assembled by using Na_(3)V_(2)(PO_(4))_(3)/C as the cathode.This study explores a novel strategy for interface/vacancy co-modification in the fabrication of high-performance sodium-ion batteries electrode.
基金supported by the National Key Research and Development Program of China(2020YFE0200600)the National Natural Science Foundation of China(U22B2026)。
文摘The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we propose an intelligent DHR architecture,which is more feasible by intelligently combining the random distribution based dynamic scheduling algorithm(RD-DS)and information weight and heterogeneity based arbitrament(IWHA)algorithm.In the proposed architecture,the random distribution function and information weight are employed to achieve the optimal selection of executors in the process of RD-DS,which avoids the case that some executors fail to be selected due to their stability difference in the conventional DHR architecture.Then,through introducing the heterogeneity to restrict the information weights in the procedure of the IWHA,the proposed architecture solves the common mode escape issue caused by the existence of multiple identical error output results of similar vulnerabilities.The experimental results characterize that the proposed architecture outperforms in heterogeneity,scheduling times,security,and stability over the conventional DHR architecture under the same conditions.
基金the Hong Kong Polytechnic University(Q-CDBG),the Science and Technology Program of Guangdong Province of China(2020A0505090001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.PolyU152178/20E)+2 种基金the National Natural Science Foundation of China(22379052)the Natural Science Foundation of Guangdong(No.2022A1515011667)China Postdoctoral Science Foundation(2021T140268).
文摘Inactive elemental doping is commonly used to improve the structural stability of high-voltage layered transition-metal oxide cathodes.However,the one-step co-doping strategy usually results in small grain size since the low diffusivity ions such as Ti^(4+)will be concentrated on grain boundaries,which hinders the grain growth.In order to synthesize large single-crystal layered oxide cathodes,considering the different diffusivities of different dopant ions,we propose a simple two-step multi-element co-doping strategy to fabricate core–shell structured LiCoO_(2)(CS-LCO).In the current work,the high-diffusivity Al^(3+)/Mg^(2+)ions occupy the core of single-crystal grain while the low diffusivity Ti^(4+)ions enrich the shell layer.The Ti^(4+)-enriched shell layer(~12 nm)with Co/Ti substitution and stronger Ti–O bond gives rise to less oxygen ligand holes.In-situ XRD demonstrates the constrained contraction of c-axis lattice parameter and mitigated structural distortion.Under a high upper cut-off voltage of 4.6 V,the single-crystal CS-LCO maintains a reversible capacity of 159.8 mAh g^(−1)with a good retention of~89%after 300 cycles,and reaches a high specific capacity of 163.8 mAh g^(−1)at 5C.The proposed strategy can be extended to other pairs of low-(Zr^(4+),Ta^(5+),and W6+,etc.)and high-diffusivity cations(Zn^(2+),Ni^(2+),and Fe^(3+),etc.)for rational design of advanced layered oxide core–shell structured cathodes for lithium-ion batteries.
