The Internet of Things(IoT)is integral to modern infrastructure,enabling connectivity among a wide range of devices from home automation to industrial control systems.With the exponential increase in data generated by...The Internet of Things(IoT)is integral to modern infrastructure,enabling connectivity among a wide range of devices from home automation to industrial control systems.With the exponential increase in data generated by these interconnected devices,robust anomaly detection mechanisms are essential.Anomaly detection in this dynamic environment necessitates methods that can accurately distinguish between normal and anomalous behavior by learning intricate patterns.This paper presents a novel approach utilizing generative adversarial networks(GANs)for anomaly detection in IoT systems.However,optimizing GANs involves tuning hyper-parameters such as learning rate,batch size,and optimization algorithms,which can be challenging due to the non-convex nature of GAN loss functions.To address this,we propose a five-dimensional Gray wolf optimizer(5DGWO)to optimize GAN hyper-parameters.The 5DGWO introduces two new types of wolves:gamma(γ)for improved exploitation and convergence,and theta(θ)for enhanced exploration and escaping local minima.The proposed system framework comprises four key stages:1)preprocessing,2)generative model training,3)autoencoder(AE)training,and 4)predictive model training.The generative models are utilized to assist the AE training,and the final predictive models(including convolutional neural network(CNN),deep belief network(DBN),recurrent neural network(RNN),random forest(RF),and extreme gradient boosting(XGBoost))are trained using the generated data and AE-encoded features.We evaluated the system on three benchmark datasets:NSL-KDD,UNSW-NB15,and IoT-23.Experiments conducted on diverse IoT datasets show that our method outperforms existing anomaly detection strategies and significantly reduces false positives.The 5DGWO-GAN-CNNAE exhibits superior performance in various metrics,including accuracy,recall,precision,root mean square error(RMSE),and convergence trend.The proposed 5DGWO-GAN-CNNAE achieved the lowest RMSE values across the NSL-KDD,UNSW-NB15,and IoT-23 datasets,with values of 0.24,1.10,and 0.09,respectively.Additionally,it attained the highest accuracy,ranging from 94%to 100%.These results suggest a promising direction for future IoT security frameworks,offering a scalable and efficient solution to safeguard against evolving cyber threats.展开更多
Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully construct...Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.展开更多
Silicon possesses a high theoretical capacity,making it a potential contender for lithium-ion battery(LIB)anodes.Nonetheless,its practical usage is challenged by low electrical conductivity and significant volume expa...Silicon possesses a high theoretical capacity,making it a potential contender for lithium-ion battery(LIB)anodes.Nonetheless,its practical usage is challenged by low electrical conductivity and significant volume expansion during cycling.Here,we synthesized a novel silicon/carbon(Si/C)anode doped with ZnO via a template-derived method and high-temperature carbonization.The carbon structure,originated from metal-organic frameworks(MOFs)and ZnO doping,substantially enhanced the electrochemical properties of the composite material.It exhibited an initial capacity of 2100.3 mA h g^(-1)at a current density of 0.2 A g^(-1)and demonstrated excellent capacity retention over successive cycles.Moreover,the composite material displayed superior rate performance at higher current densities of 2 A g^(-1)and 3 A g^(-1).To address the low initial Coulombic efficiency(ICE)of siliconbased materials,we adopted a direct contact prelithiation approach and optimized the lithiation process by controlling the prelithiation time.After 30 min of prelithiation,the ICE reached 97.9%,thereby reducing the initial irreversible capacity loss(ICL)and realizing stable discharge-charge in subsequent cycles.This rational design provides valuable insights for achieving high-performance silicon anode.展开更多
High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carb...High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody(Ab1)and ferrocene(Fc),and used for electrochemical detection of AFP.Due to the small,homogeneous pore size of the COF,Ab1 with a big size was immobilized on the surface of the COF,while Fc with a small size was covalently modified both on the surface and in the pores of COF.The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers.Meanwhile,the enriched Fc molecules not only improved the conductivity of the COF,but also effectively transferred and amplified the electrochemical signal.This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL(S/N of 3:1)and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations.Furthermore,this immunosensor showed excellent selectivity,stability and reproducibility in the testing of real samples.This study presents an innovative prototype for construction of a precious metal-free,antibody-directly-immobilized,simple and stable electrochemical immunoprobe.展开更多
Autonomous connected vehicles(ACV)involve advanced control strategies to effectively balance safety,efficiency,energy consumption,and passenger comfort.This research introduces a deep reinforcement learning(DRL)-based...Autonomous connected vehicles(ACV)involve advanced control strategies to effectively balance safety,efficiency,energy consumption,and passenger comfort.This research introduces a deep reinforcement learning(DRL)-based car-following(CF)framework employing the Deep Deterministic Policy Gradient(DDPG)algorithm,which integrates a multi-objective reward function that balances the four goals while maintaining safe policy learning.Utilizing real-world driving data from the highD dataset,the proposed model learns adaptive speed control policies suitable for dynamic traffic scenarios.The performance of the DRL-based model is evaluated against a traditional model predictive control-adaptive cruise control(MPC-ACC)controller.Results show that theDRLmodel significantly enhances safety,achieving zero collisions and a higher average time-to-collision(TTC)of 8.45 s,compared to 5.67 s for MPC and 6.12 s for human drivers.For efficiency,the model demonstrates 89.2% headway compliance and maintains speed tracking errors below 1.2 m/s in 90% of cases.In terms of energy optimization,the proposed approach reduces fuel consumption by 5.4% relative to MPC.Additionally,it enhances passenger comfort by lowering jerk values by 65%,achieving 0.12 m/s3 vs.0.34 m/s3 for human drivers.A multi-objective reward function is integrated to ensure stable policy convergence while simultaneously balancing the four key performance metrics.Moreover,the findings underscore the potential of DRL in advancing autonomous vehicle control,offering a robust and sustainable solution for safer,more efficient,and more comfortable transportation systems.展开更多
Accelerating the development of new quality productive forces(NQPF),with innovation at its core,has become essential for firm growth in the new era.Drawing on financial data from China's A-share listed companies s...Accelerating the development of new quality productive forces(NQPF),with innovation at its core,has become essential for firm growth in the new era.Drawing on financial data from China's A-share listed companies spanning the period 2010–2023,this study empirically investigates the impact of entrepreneurial spirit on firm-level NQPF.The results indicate that entrepreneurial spirit significantly promotes firm-level NQPF.Mechanism analysis indicates that entrepreneurial effort—underpinned by technological capital accumulation,effective incentive and constraint mechanisms,and a competitive market environment—plays a mediating role in this relationship.Further heterogeneity analysis reveals that,amid China's economic transition,the positive effects of entrepreneurial spirit are more pronounced in non-state-owned enterprises,high-tech firms,and newly established firms.Accordingly,systematic efforts should be pursued across the technological,organizational,and environmental(TOE)dimensions to optimize the cultivation of entrepreneurial spirit.In particular,greater emphasis should be placed on productive entrepreneurial spirit and the constructive role of entrepreneurial effort,so as to fully leverage their contribution to the advancement of firm-level NQPF.展开更多
Gas sensors are valuable tools for human applications,and extensive research has been conducted in this field.However,practical implementation has yet to be fully realized.In response,efforts have been made to explore...Gas sensors are valuable tools for human applications,and extensive research has been conducted in this field.However,practical implementation has yet to be fully realized.In response,efforts have been made to explore metal-organic frameworks(MOFs),a novel class of porous materials,as potential solutions.MOFs exhibit exceptional porosity and highly tunable chemical compositions and structures,giving rise to a wide range of unique physical and chemical properties.Significant progress has been achieved in developing MOF-based gas sensors,improving sensing performance for various gases.This review aims to provide a comprehensive understanding of MOF-based gas sensors,even for readers unfamiliar with MOFs and gas sensors.It covers the working principles of these sensors,fundamental concepts of MOFs,strategies for tuning MOF properties,fabrication techniques for MOF films,and recent studies on MOF and MOF-derivative gas sensors.Finally,current challenges,overlooked aspects,and future directions for fully exploiting the potential of MOFs in gas sensor development are discussed.展开更多
Metal-organic frameworks(MOFs)with high porosity,specific surface area,and unique topologies are highly regarded for their applications in photocatalysis,medical treatment,and environmental pollutant degradation.Howev...Metal-organic frameworks(MOFs)with high porosity,specific surface area,and unique topologies are highly regarded for their applications in photocatalysis,medical treatment,and environmental pollutant degradation.However,due to the limitations of the tumor microenvironment(TME),traditional MOFs have limited efficacy in this environment.This paper designs multi-metal oxide-based heterostructure POMOFs nanoreactors with a nesting doll-like structure.This new structure not only exhibits therapeutic effects in TME but also utilizes ultrasound(US)to enhance the release of reactive oxygen species(ROS)for CDT&SDT co-therapy,becoming an effective sound sensitizer for destroying tumor cells.In summary,our study proposes an idea for constructing multi-metal oxide-based heterostructure MOFs nanoreactors material with a nesting doll-like structure to enhance ROS release and synergistically treat tumor diseases.展开更多
Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated cata...Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated catalysts for photocatalytic CO_(2)RR.Unfortunately,low CO_(2)adsorption ability and limited active sites of metal oxide and metal chalcogenide catalysts for CO_(2)RR make them less competitive compared to their industrial counterparts.Inspired by applications of porphyrin-based metal-organic framework(MOF)catalysts for hydrogen evolution and photodynamic therapy,the investigations of these porphyrin-based MOFs,including pristine and composite porphyrin-based MOFs in photocatalytic CO_(2)RR,have attracted significant attention in the last five years due to their excellent CO_(2)adsorption capacities,high porosity,high stability,exceptional optoelectronic properties,and multi-functionality.However,due to the difference in photocatalytic CO_(2)RR,several critical issues need to be addressed to achieve the rational design of advanced porphyrin-based MOF photocatalysts to improve activity,selectivity,and stability for CO_(2)RR.Here,we review recent developments in the field of porphyrin-based MOF CO_(2)RR photocatalysts,along with critical issues,challenges,and perspectives concerning porphyrin-based MOF catalysts for photocatalytic CO_(2)RR.展开更多
The recovery of precious metals(PMs)from secondary resources is critical for addressing global supply-chain vulnerabilities and sustainable resource utilization.This review systematically examines the transformative p...The recovery of precious metals(PMs)from secondary resources is critical for addressing global supply-chain vulnerabilities and sustainable resource utilization.This review systematically examines the transformative potential of metal-organic frameworks(MOFs)as next-generation adsorbents for PM recovery,focusing on their synthesis,functionalization,and multiscale adsorption mechanisms.We critically analyze conventional pyrometallurgical and hydrometallurgical methods and highlight their limitations in terms of selectivity,energy consumption,and secondary pollution.In contrast,MOFs offer tunable porosity,abundant active sites,and tunable surface chemistry,enabling efficient PM capture via synergistic physical and chemical adsorption.Advanced modification techniques,including direct synthesis and post-synthetic modification,are reviewed to propose strategies for enhancing the adsorption kinetics and selectivity for Au,Ag,Pt,and Pd.Key structure-property relationships are established through multiscale characterization and thermodynamic models,revealing the critical roles of hierarchical porosity,soft donor atoms,and framework stability.Industrial challenges,such as aqueous stability and scalability,are addressed via Zr-O bond strengthening,hydrophobic functionalization,and support immobilization.This study consolidates the experimental and theoretical advances in MOF-based PM recovery and provides a roadmap for translating laboratory innovations into practical applications within the circular-economy framework.展开更多
Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fund...Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fundamental trade-off between haze and transparency,coupled with impractical thicknesses(≥1 mm).Inspired by squid’s skin-peeling mechanism,this work develops a peroxyformic acid(HCOOOH)-enabled precision peeling strategy to isolate intact 10-μm-thick bamboo green(BG)frameworks—100×thinner than wood-based counterparts while achieving an unprecedented optical performance(88%haze with 80%transparency).This performance surpasses delignified biomass(transparency<40%at 1 mm)and matches engineered cellulose composites,yet requires no energy-intensive nanofibrillation.The preserved native cellulose I crystalline structure(64.76%crystallinity)and wax-coated uniaxial fibril alignment(Hermans factor:0.23)contribute to high mechanical strength(903 MPa modulus)and broadband light scattering.As a light-management layer in polycrystalline silicon solar cells,the BG framework boosts photoelectric conversion efficiency by 0.41%absolute(18.74%→19.15%),outperforming synthetic anti-reflective coatings.The work establishes a scalable,waste-to-wealth route for optical-grade cellulose materials in next-generation optoelectronics.展开更多
Three-dimensional supramolecular organic frameworks with precisely tunable pore sizes are highly demanded for a wide range of applications,e.g.,encapsulating enzymes to enhance their stability,activity,and reusability...Three-dimensional supramolecular organic frameworks with precisely tunable pore sizes are highly demanded for a wide range of applications,e.g.,encapsulating enzymes to enhance their stability,activity,and reusability.However,precise control and tune the pore size of such frameworks still remains a significant challenge to date.In this study,we constructed supramolecular polymer frameworks using rigid tetrahedral star polyisocyanides with tunable length and sufficiently narrow distribution as building block.First,a series of tetrahedral four-arm star polyisocyanides with controlled chain lengths and narrow molecular weight distributions was prepared via the Pd(Ⅱ)-catalyzed living isocyanide polymerization.Then 2-ureido-4[1H]-pyrimidinone(Upy) unit was installed onto each chain-end of polyisocyanide arms via post-polymerization functionalization.Leveraging the supramolecular hydrogen bonding interactions between the terminal Upy units,well-ordered supramolecular polymer frameworks were readily obtained.Notably,the pore size was dependent on the chain length of the polyisocyanide arms.Precisely control the chain length of polyisocyanide arms,supramolecular polymer frameworks with pore sizes ranging from 5.06 nm to 9.72 nm were achieved.These frameworks,with tunable and large pore apertures,demonstrated exceptional capabilities in encapsulating enzymes of different sizes,such as lipase(TL),horseradish peroxidase(HRP),and glucose oxidase(GOx).The encapsulated enzymes exhibited significantly enhanced catalytic activity and durability.Moreover,the frameworks' tunable and large pore apertures facilitated the co-encapsulation of multiple enzymes,enabling efficient dual-enzyme cascade reactions.展开更多
Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystall...Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystallinity and surface area of COFs,are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation,catalysis,chemical sensing,and energy storage.Therefore,it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development.In this review,we offer a comprehensive overview of recent advancements in PI-COFs,emphasizing their synthesis methods,design principles and applications.Finally,our brief outlooks on the current challenges and future developments of PI-COFs are provided.Overall,this review aims to guide the recent and future development of PI-COFs.展开更多
Ion conduction in covalent-organic framework(COF)membranes is vital for energy conversion and storage.Conventional phenomenological methods based on the Arrhenius equation offer micrometer-scale cognition of ion condu...Ion conduction in covalent-organic framework(COF)membranes is vital for energy conversion and storage.Conventional phenomenological methods based on the Arrhenius equation offer micrometer-scale cognition of ion conduction,whereas they ignore atomic details of ion-pore interactions and sophisticated conduction mechanisms,leaving gaps in high-resolution and bottom-up understanding of ion conduction in a nanoconfined space.In this study,we develop a hierarchical approach by holistically synergizing electronic structure calculations,first-principles molecular dynamics simulations,and thermodynamic integration methods to investigate the conduction of chloride(Cl^(-))and hydroxide(OH^(-))ions in a COF membrane.It is revealed that Cl^(-)ion with symmetric charge distribution undergoes weak solvation and tight ion-pore binding,which results in a tortuous conduction pathway,a high energy barrier,and slow diffusion based on the vehicular mechanism.In remarkable contrast,OH^(-)ion with heterogeneous charge distribution features strong solvation and weak ion-pore binding,and it jumps frequently via a smooth pathway and a low energy barrier.Moreover,OH^(-)ion conduction follows a mixed vehicular and Grotthuss mechanism,causing highly mutable ion identity and number,as well as superior dynamics due to proton transfer.This hierarchical approach provides sub-nanometer resolution insights into ion conduction,guiding intelligent membrane design and performance regulation to control ion conduction for emerging applications.展开更多
Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hinde...Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hindered by low ionic co nductivity and unstable Li^(+)transport at the electrode interfaces.To overcome these challenges,a previously unreported family of indium based MOFs(In-BDC-F_(x),x=0,4,6)with tunable fluorine content was synthesized and integrated into PVDF-HFP matrices to construct highperformance quasi-solid-state electrolytes.By systematically modulating linker fluorination,a bifunctional enhancement mechanism is revealed:fluorinated indium centers simultaneously suppress polymer crystallinity and establish preferential Li^(+)conduction pathways.Remarkably,In-BDC-F_(6) manifests exceptional synergistic interactions between-CF_(3) functionalities and indium coordination sites,amplifying Lewis acidity to facilitate LiTFSI dissociation and TFSI-immobilization,culminating in homogeneous LiF-enriched solid electrolyte interphases.The optimized electrolyte demonstrates compelling electrochemical performance:ionic conductivity of 9.68×10^(-4) S cm^(-1),Li^(+)transference number of 0.70,and electrochemical stability window of 4.96 V.Li‖Li symmetric cell demonstrated a critical current density of 3.5 mA cm^(-2) and stable plating/stripping for over 1000 h at 0.2 mA cm^(-2),while LiFePO_(4)‖Li cells retain96.66%capacity after 1300 cycles at 10C,underscoring the transformative potential of fluorinated MOF architectures in fast-charging solid-state batteries.展开更多
CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organ...CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.展开更多
Modern business information systems face significant challenges in managing heterogeneous data sources,integrating disparate systems,and providing real-time decision support in complex enterprise environments.Contempo...Modern business information systems face significant challenges in managing heterogeneous data sources,integrating disparate systems,and providing real-time decision support in complex enterprise environments.Contemporary enterprises typically operate 200+interconnected systems,with research indicating that 52% of organizations manage three or more enterprise content management systems,creating information silos that reduce operational efficiency by up to 35%.While attention mechanisms have demonstrated remarkable success in natural language processing and computer vision,their systematic application to business information systems remains largely unexplored.This paper presents the theoretical foundation for a Hierarchical Attention-Based Business Information System(HABIS)framework that applies multi-level attention mechanisms to enterprise environments.We provide a comprehensive mathematical formulation of the framework,analyze its computational complexity,and present a proof-of-concept implementation with simulation-based validation that demonstrates a 42% reduction in crosssystem query latency compared to legacy ERP modules and 70% improvement in prediction accuracy over baseline methods.The theoretical framework introduces four hierarchical attention levels:system-level attention for dynamic weighting of business systems,process-level attention for business process prioritization,data-level attention for critical information selection,and temporal attention for time-sensitive pattern recognition.Our complexity analysis demonstrates that the framework achieves O(n log n)computational complexity for attention computation,making it scalable to large enterprise environments including retail supply chains with 200+system-scale deployments.The proof-of-concept implementation validates the theoretical framework’s feasibility withMSE loss of 0.439 and response times of 0.000120 s per query,demonstrating its potential for addressing key challenges in business information systems.This work establishes a foundation for future empirical research and practical implementation of attention-driven enterprise systems.展开更多
The practical deployment of lithium metal batteries remains severely constrained,especially under elevated temperatures.Although metal-organic frameworks(MOFs)improve the thermal stability of liquid electrolytes by ca...The practical deployment of lithium metal batteries remains severely constrained,especially under elevated temperatures.Although metal-organic frameworks(MOFs)improve the thermal stability of liquid electrolytes by capturing them in well-ordered sub-nanopores,interparticle voids between MOF particles readily absorb liquid electrolyte,obscuring our understanding of the intrinsic role of nanopores in directing Li^(+)transport.To address this challenge,we introduce a one-dimensional(1D)MOF model architecture that eliminates interparticle effects and enables direct observation of Li^(+)solvation and de-solvation dynamics.Comparative studies of 1D HKUST-1 and ZIF-8 uncover distinct transport behaviors,supported by both experimental measurements and neural network potential-based molecular dynamics simulations.Building on these insights,we construct a hierarchical core-shell MOF architecture by integrating ZIF-8(core)and HKUST-1(shell)onto a hybrid fiber scaffold.This design harnesses the complementary strengths of both MOFs to achieve continuous ion pathways,directional Li^(+)conduction,and improved thermal and electrochemical resilience.展开更多
The recovery of gold from waste electronic and electric equipment(WEEE) has gained great attention with the increased number of WEEE,because it can largely alleviate the pressure on the environment and resources.Coval...The recovery of gold from waste electronic and electric equipment(WEEE) has gained great attention with the increased number of WEEE,because it can largely alleviate the pressure on the environment and resources.Covalent organic frameworks(COFs) are ideal adsorbents for gold recovery owing to their large surface area,good stability,easily functionalized ability,periodic structures,and definitive nanopores.Herein,a cyano-functionalized COF(COF-CN) with high crystallinity was large-scale prepared under mild conditions for the recovery of gold.The introduction of cyano groups enable COF-CN to exhibit excellent gold recovery performance,which possesses fast adsorption kinetics,high cycling stability,and adsorption capacity up to 663.67 mg/g.Excitingly,COF-CN showed extremely high selectivity for gold ions,even in the presence of various competing cations and anions.The COF-CN maintained excellent selectivity and removal efficiency in gold recovery experiments from WEEE.The facile synthesis of COF-CN and its outstanding selectivity in actual samples make it an attractive opportunity for practical gold recovery.展开更多
The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theor...The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theoretical and practical significance for guiding oil and gas exploration.The sedimentary facies and sedimentary evolution of the high-resolution sequence framework of the Carboniferous Taiyuan Formation in the Hangjinqi area have been systematically analyzed for the first time by drilling,logging and seismic data.The results show that four types of sequence interfaces can be identified in the Taiyuan Formation:regional unconformity surfaces,scour surfaces,lithologic-lithofacies transformation surfaces and flooding surfaces.According to the sedimentary response caused by the upward and downward movements of the base level at different levels,the Taiyuan Formation can be divided into 2 long-term cycles(LSC_(1)-LSC_(2)),4 mid-term cycles(MSC_(1)-MSC4)and 7 short-term cycles(SSC_(1)-SSC7).The long-and mid-term cycles correspond to members T_(1)and T_(2)and layers T_(1)-1,T_(1-2),T_(2-1),and T_(2)-2,respectively.Long-term cycles are dominated by C_(1);mid-term cycles are dominated by C_(1)and C_(2),followed by A2;and short-term cycles are dominated by C_(1),C_(2),A1 and A2.Under the high-resolution sequence stratigraphic framework,the Hangjinqi area underwent a transformation of fan delta and tidal flat depositional systems during the Taiyuan Formation sedimentary period.In the MSC_(1)-MSC_(2)stage,owing to a large-scale paleocontinent,the fan delta sedimentary body,which was limited in scale and scope,developed only in the southeastern corner and gradually transitioned basinward to tidal flat facies.In the MSC3-MSC4 stage,as the paleocontinent continuously decreased and the sedimentary range expanded,fan-delta plain sedimentation began in the study area.Several braided distributary channels with poor connectivity developed on the fan-delta plain,and between them were floodplains and peat swamps.展开更多
基金described in this paper has been developed with in the project PRESECREL(PID2021-124502OB-C43)。
文摘The Internet of Things(IoT)is integral to modern infrastructure,enabling connectivity among a wide range of devices from home automation to industrial control systems.With the exponential increase in data generated by these interconnected devices,robust anomaly detection mechanisms are essential.Anomaly detection in this dynamic environment necessitates methods that can accurately distinguish between normal and anomalous behavior by learning intricate patterns.This paper presents a novel approach utilizing generative adversarial networks(GANs)for anomaly detection in IoT systems.However,optimizing GANs involves tuning hyper-parameters such as learning rate,batch size,and optimization algorithms,which can be challenging due to the non-convex nature of GAN loss functions.To address this,we propose a five-dimensional Gray wolf optimizer(5DGWO)to optimize GAN hyper-parameters.The 5DGWO introduces two new types of wolves:gamma(γ)for improved exploitation and convergence,and theta(θ)for enhanced exploration and escaping local minima.The proposed system framework comprises four key stages:1)preprocessing,2)generative model training,3)autoencoder(AE)training,and 4)predictive model training.The generative models are utilized to assist the AE training,and the final predictive models(including convolutional neural network(CNN),deep belief network(DBN),recurrent neural network(RNN),random forest(RF),and extreme gradient boosting(XGBoost))are trained using the generated data and AE-encoded features.We evaluated the system on three benchmark datasets:NSL-KDD,UNSW-NB15,and IoT-23.Experiments conducted on diverse IoT datasets show that our method outperforms existing anomaly detection strategies and significantly reduces false positives.The 5DGWO-GAN-CNNAE exhibits superior performance in various metrics,including accuracy,recall,precision,root mean square error(RMSE),and convergence trend.The proposed 5DGWO-GAN-CNNAE achieved the lowest RMSE values across the NSL-KDD,UNSW-NB15,and IoT-23 datasets,with values of 0.24,1.10,and 0.09,respectively.Additionally,it attained the highest accuracy,ranging from 94%to 100%.These results suggest a promising direction for future IoT security frameworks,offering a scalable and efficient solution to safeguard against evolving cyber threats.
文摘Under hydrothermal and solvothermal conditions,two novel cobalt-based complexes,{[Co_(2)(CIA)(OH)(1,4-dtb)]·3.2H_(2)O}n(HU23)and{[Co_(2)(CIA)(OH)(1,4-dib)]·3.5H2O·DMF}n(HU24),were successfully constructed by coordinatively assembling the semi-rigid multidentate ligand 5-(1-carboxyethoxy)isophthalic acid(H₃CIA)with the Nheterocyclic ligands 1,4-di(4H-1,2,4-triazol-4-yl)benzene(1,4-dtb)and 1,4-di(1H-imidazol-1-yl)benzene(1,4-dib),respectively,around Co^(2+)ions.Single-crystal X-ray diffraction analysis revealed that in both complexes HU23 and HU24,the CIA^(3-)anions adopt aκ^(7)-coordination mode,bridging six Co^(2+)ions via their five carboxylate oxygen atoms and one ether oxygen atom.This linkage forms tetranuclear[Co4(μ3-OH)2]^(6+)units.These Co-oxo cluster units were interconnected by CIA^(3-)anions to assemble into 2D kgd-type structures featuring a 3,6-connected topology.The 2D layers were further connected by 1,4-dtb and 1,4-dib,resulting in 3D pillar-layered frameworks for HU23 and HU24.Notably,despite the similar configurations of 1,4-dtb and 1,4-dib,differences in their coordination spatial orientations lead to topological divergence in the 3D frameworks of HU23 and HU24.Topological analysis indicates that the frameworks of HU23 and HU24 can be simplified into a 3,10-connected net(point symbol:(4^(10).6^(3).8^(2))(4^(3))_(2))and a 3,8-connected tfz-d net(point symbol:(4^(3))_(2)((4^(6).6^(18).8^(4)))),respectively.This structural differentiation confirms the precise regulatory role of ligands on the topology of metal-organic frameworks.Moreover,the ultraviolet-visible absorption spectra confirmed that HU23 and HU24 have strong absorption capabilities for ultraviolet and visible light.According to the Kubelka-Munk method,their bandwidths were 2.15 and 2.08 eV,respectively,which are consistent with those of typical semiconductor materials.Variable-temperature magnetic susceptibility measurements(2-300 K)revealed significant antiferromagnetic coupling in both complexes,with their effective magnetic moments decreasing markedly as the temperature lowered.CCDC:2457554,HU23;2457553,HU24.
基金supported by the National Key R&D Program of China(No.2022YFA1504100)the Anhui Provincial Major Science and Technology Project(No.202203a05020017)+4 种基金the National Natural Science Foundation of China(Nos.52222210,51925207,U1910210,52161145101,51972067,51902062,and 52002083)the“Transformational Technologies for Clean Energy and Demonstration”Strategic Priority Research Program of Chinese Academy of Sciences(No.XDA21000000)the National Synchrotron Radiation Laboratory(No.KY2060000173)the Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(No.YLU-DNL Fund 2021002)the Fundamental Research Funds for the Central Universities(No.WK2060140026)。
文摘Silicon possesses a high theoretical capacity,making it a potential contender for lithium-ion battery(LIB)anodes.Nonetheless,its practical usage is challenged by low electrical conductivity and significant volume expansion during cycling.Here,we synthesized a novel silicon/carbon(Si/C)anode doped with ZnO via a template-derived method and high-temperature carbonization.The carbon structure,originated from metal-organic frameworks(MOFs)and ZnO doping,substantially enhanced the electrochemical properties of the composite material.It exhibited an initial capacity of 2100.3 mA h g^(-1)at a current density of 0.2 A g^(-1)and demonstrated excellent capacity retention over successive cycles.Moreover,the composite material displayed superior rate performance at higher current densities of 2 A g^(-1)and 3 A g^(-1).To address the low initial Coulombic efficiency(ICE)of siliconbased materials,we adopted a direct contact prelithiation approach and optimized the lithiation process by controlling the prelithiation time.After 30 min of prelithiation,the ICE reached 97.9%,thereby reducing the initial irreversible capacity loss(ICL)and realizing stable discharge-charge in subsequent cycles.This rational design provides valuable insights for achieving high-performance silicon anode.
基金the Natural Science Foundation of ZhejiangProvince(No.LZ24B020005)the National Natural Science Foundation of China(No.22071040)for financial support.
文摘High-sensitive quantitative determination of alpha-fetoprotein(AFP)is of crucial importance for early clinical diagnosis of cancers.Herein,an AuNPs-free electrochemical immunosensor(Ab1-Fc-COF)was prepared from a carboxylic group enriched COF by post-functionalization with detecting antibody(Ab1)and ferrocene(Fc),and used for electrochemical detection of AFP.Due to the small,homogeneous pore size of the COF,Ab1 with a big size was immobilized on the surface of the COF,while Fc with a small size was covalently modified both on the surface and in the pores of COF.The covalently immobilized Ab1 was quite stable and beneficial to specifically detect AFP biomarkers.Meanwhile,the enriched Fc molecules not only improved the conductivity of the COF,but also effectively transferred and amplified the electrochemical signal.This proposed immunosensor exhibited high sensitivity in detecting AFP with a detection limit of 0.39 pg/mL(S/N of 3:1)and a wide linear response range spanning from 1 pg/mL to 100 ng/mL when plotted against logarithmic concentrations.Furthermore,this immunosensor showed excellent selectivity,stability and reproducibility in the testing of real samples.This study presents an innovative prototype for construction of a precious metal-free,antibody-directly-immobilized,simple and stable electrochemical immunoprobe.
基金the Hebei Province Science and Technology Plan Project(19221909D)rincess Nourah bint Abdulrahman University Researchers Supporting Project number(PNURSP2025R308),Princess Nourah bint Abdulrahman University,Riyadh,Saudi Arabia.
文摘Autonomous connected vehicles(ACV)involve advanced control strategies to effectively balance safety,efficiency,energy consumption,and passenger comfort.This research introduces a deep reinforcement learning(DRL)-based car-following(CF)framework employing the Deep Deterministic Policy Gradient(DDPG)algorithm,which integrates a multi-objective reward function that balances the four goals while maintaining safe policy learning.Utilizing real-world driving data from the highD dataset,the proposed model learns adaptive speed control policies suitable for dynamic traffic scenarios.The performance of the DRL-based model is evaluated against a traditional model predictive control-adaptive cruise control(MPC-ACC)controller.Results show that theDRLmodel significantly enhances safety,achieving zero collisions and a higher average time-to-collision(TTC)of 8.45 s,compared to 5.67 s for MPC and 6.12 s for human drivers.For efficiency,the model demonstrates 89.2% headway compliance and maintains speed tracking errors below 1.2 m/s in 90% of cases.In terms of energy optimization,the proposed approach reduces fuel consumption by 5.4% relative to MPC.Additionally,it enhances passenger comfort by lowering jerk values by 65%,achieving 0.12 m/s3 vs.0.34 m/s3 for human drivers.A multi-objective reward function is integrated to ensure stable policy convergence while simultaneously balancing the four key performance metrics.Moreover,the findings underscore the potential of DRL in advancing autonomous vehicle control,offering a robust and sustainable solution for safer,more efficient,and more comfortable transportation systems.
基金Liaoning Provincial Social Science Fund Key Disciplines Development Project,Research on the New Supply Function of Entrepreneurs Based on Innovation Ecosystems Driven by Data(Grant No.L22ZD061)。
文摘Accelerating the development of new quality productive forces(NQPF),with innovation at its core,has become essential for firm growth in the new era.Drawing on financial data from China's A-share listed companies spanning the period 2010–2023,this study empirically investigates the impact of entrepreneurial spirit on firm-level NQPF.The results indicate that entrepreneurial spirit significantly promotes firm-level NQPF.Mechanism analysis indicates that entrepreneurial effort—underpinned by technological capital accumulation,effective incentive and constraint mechanisms,and a competitive market environment—plays a mediating role in this relationship.Further heterogeneity analysis reveals that,amid China's economic transition,the positive effects of entrepreneurial spirit are more pronounced in non-state-owned enterprises,high-tech firms,and newly established firms.Accordingly,systematic efforts should be pursued across the technological,organizational,and environmental(TOE)dimensions to optimize the cultivation of entrepreneurial spirit.In particular,greater emphasis should be placed on productive entrepreneurial spirit and the constructive role of entrepreneurial effort,so as to fully leverage their contribution to the advancement of firm-level NQPF.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(RS-2024-00333650)supported by basic science research program through the National Research Foundation of Korea funded by the Ministry of Education(NRF-2019R1A6A1A11055660)+1 种基金supported by the Technology Innovation Program(“20013621”,Center for Super Critical Material Industrial Technology)funded By the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by Strategic Networking&Development Program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(RS-2023-00268523)。
文摘Gas sensors are valuable tools for human applications,and extensive research has been conducted in this field.However,practical implementation has yet to be fully realized.In response,efforts have been made to explore metal-organic frameworks(MOFs),a novel class of porous materials,as potential solutions.MOFs exhibit exceptional porosity and highly tunable chemical compositions and structures,giving rise to a wide range of unique physical and chemical properties.Significant progress has been achieved in developing MOF-based gas sensors,improving sensing performance for various gases.This review aims to provide a comprehensive understanding of MOF-based gas sensors,even for readers unfamiliar with MOFs and gas sensors.It covers the working principles of these sensors,fundamental concepts of MOFs,strategies for tuning MOF properties,fabrication techniques for MOF films,and recent studies on MOF and MOF-derivative gas sensors.Finally,current challenges,overlooked aspects,and future directions for fully exploiting the potential of MOFs in gas sensor development are discussed.
基金funded by the National Natural Science Foundation of China(Nos.52372264,32271609and 52473109)+2 种基金The Natural Science Foundation of Heilongjiang Province of China(No.LH2023B002)The Fundamental Research Funds for the Central Universities(No.2572023CT12)Undergraduate Training Programs for Innovations by NEFU(No.202310225565)。
文摘Metal-organic frameworks(MOFs)with high porosity,specific surface area,and unique topologies are highly regarded for their applications in photocatalysis,medical treatment,and environmental pollutant degradation.However,due to the limitations of the tumor microenvironment(TME),traditional MOFs have limited efficacy in this environment.This paper designs multi-metal oxide-based heterostructure POMOFs nanoreactors with a nesting doll-like structure.This new structure not only exhibits therapeutic effects in TME but also utilizes ultrasound(US)to enhance the release of reactive oxygen species(ROS)for CDT&SDT co-therapy,becoming an effective sound sensitizer for destroying tumor cells.In summary,our study proposes an idea for constructing multi-metal oxide-based heterostructure MOFs nanoreactors material with a nesting doll-like structure to enhance ROS release and synergistically treat tumor diseases.
基金financially supported by the National Natural Science Foundation of China(No.22305009)the Science and Technology Development Fund,Macao SAR(File no.FDCT-0125/2022/A and FDCT-0006/2023/RIB1)Hong Kong Research Grant Council(RGC)General Research Fund(GRF)City U 11305419,11306920,CityU 11308721,CityU 11316522,and SIRG7020022。
文摘Photocatalytic carbon dioxide reduction reaction(CO_(2)RR)is a carbon-neutral strategy to address global energy use and its impact on climate.Metal oxide and metal chalcogenide catalysts are the most investigated catalysts for photocatalytic CO_(2)RR.Unfortunately,low CO_(2)adsorption ability and limited active sites of metal oxide and metal chalcogenide catalysts for CO_(2)RR make them less competitive compared to their industrial counterparts.Inspired by applications of porphyrin-based metal-organic framework(MOF)catalysts for hydrogen evolution and photodynamic therapy,the investigations of these porphyrin-based MOFs,including pristine and composite porphyrin-based MOFs in photocatalytic CO_(2)RR,have attracted significant attention in the last five years due to their excellent CO_(2)adsorption capacities,high porosity,high stability,exceptional optoelectronic properties,and multi-functionality.However,due to the difference in photocatalytic CO_(2)RR,several critical issues need to be addressed to achieve the rational design of advanced porphyrin-based MOF photocatalysts to improve activity,selectivity,and stability for CO_(2)RR.Here,we review recent developments in the field of porphyrin-based MOF CO_(2)RR photocatalysts,along with critical issues,challenges,and perspectives concerning porphyrin-based MOF catalysts for photocatalytic CO_(2)RR.
基金supported by the National Natural Science Foundation of China(No.52304329)the Yunnan Fundamental Research Projects(No.202201BE070001-003),Guo Lin would like to acknowledge Xing Dian talent support program of Yunnan Province.
文摘The recovery of precious metals(PMs)from secondary resources is critical for addressing global supply-chain vulnerabilities and sustainable resource utilization.This review systematically examines the transformative potential of metal-organic frameworks(MOFs)as next-generation adsorbents for PM recovery,focusing on their synthesis,functionalization,and multiscale adsorption mechanisms.We critically analyze conventional pyrometallurgical and hydrometallurgical methods and highlight their limitations in terms of selectivity,energy consumption,and secondary pollution.In contrast,MOFs offer tunable porosity,abundant active sites,and tunable surface chemistry,enabling efficient PM capture via synergistic physical and chemical adsorption.Advanced modification techniques,including direct synthesis and post-synthetic modification,are reviewed to propose strategies for enhancing the adsorption kinetics and selectivity for Au,Ag,Pt,and Pd.Key structure-property relationships are established through multiscale characterization and thermodynamic models,revealing the critical roles of hierarchical porosity,soft donor atoms,and framework stability.Industrial challenges,such as aqueous stability and scalability,are addressed via Zr-O bond strengthening,hydrophobic functionalization,and support immobilization.This study consolidates the experimental and theoretical advances in MOF-based PM recovery and provides a roadmap for translating laboratory innovations into practical applications within the circular-economy framework.
基金supported by National Natural Science Foundation of China(32494793).
文摘Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fundamental trade-off between haze and transparency,coupled with impractical thicknesses(≥1 mm).Inspired by squid’s skin-peeling mechanism,this work develops a peroxyformic acid(HCOOOH)-enabled precision peeling strategy to isolate intact 10-μm-thick bamboo green(BG)frameworks—100×thinner than wood-based counterparts while achieving an unprecedented optical performance(88%haze with 80%transparency).This performance surpasses delignified biomass(transparency<40%at 1 mm)and matches engineered cellulose composites,yet requires no energy-intensive nanofibrillation.The preserved native cellulose I crystalline structure(64.76%crystallinity)and wax-coated uniaxial fibril alignment(Hermans factor:0.23)contribute to high mechanical strength(903 MPa modulus)and broadband light scattering.As a light-management layer in polycrystalline silicon solar cells,the BG framework boosts photoelectric conversion efficiency by 0.41%absolute(18.74%→19.15%),outperforming synthetic anti-reflective coatings.The work establishes a scalable,waste-to-wealth route for optical-grade cellulose materials in next-generation optoelectronics.
基金The National Natural Science Foundation of China (NSFC,Nos.92256201,52273006,22071041,92356302,and 21971052)Natural Science Foundation of Jilin Province (No.20240101181JC) are gratefully appreciated for financial the supportssupported by the User Experiment Assist System of Shanghai Synchrotron Radiation Facility (SSRF)。
文摘Three-dimensional supramolecular organic frameworks with precisely tunable pore sizes are highly demanded for a wide range of applications,e.g.,encapsulating enzymes to enhance their stability,activity,and reusability.However,precise control and tune the pore size of such frameworks still remains a significant challenge to date.In this study,we constructed supramolecular polymer frameworks using rigid tetrahedral star polyisocyanides with tunable length and sufficiently narrow distribution as building block.First,a series of tetrahedral four-arm star polyisocyanides with controlled chain lengths and narrow molecular weight distributions was prepared via the Pd(Ⅱ)-catalyzed living isocyanide polymerization.Then 2-ureido-4[1H]-pyrimidinone(Upy) unit was installed onto each chain-end of polyisocyanide arms via post-polymerization functionalization.Leveraging the supramolecular hydrogen bonding interactions between the terminal Upy units,well-ordered supramolecular polymer frameworks were readily obtained.Notably,the pore size was dependent on the chain length of the polyisocyanide arms.Precisely control the chain length of polyisocyanide arms,supramolecular polymer frameworks with pore sizes ranging from 5.06 nm to 9.72 nm were achieved.These frameworks,with tunable and large pore apertures,demonstrated exceptional capabilities in encapsulating enzymes of different sizes,such as lipase(TL),horseradish peroxidase(HRP),and glucose oxidase(GOx).The encapsulated enzymes exhibited significantly enhanced catalytic activity and durability.Moreover,the frameworks' tunable and large pore apertures facilitated the co-encapsulation of multiple enzymes,enabling efficient dual-enzyme cascade reactions.
基金supported by the National Key R&D Program of China(No.2023YFA1507204)National Natural Science Foundation ofChina(Nos.22475074,22171139,22225109,22302055)+4 种基金Natural Science Foundation of Guangdong Province(No.2023B1515020076)Key Scientific Research Project Plan of Colleges and Universities of Henan Province(No.24B150004)The Double Thousand Talents Plan of Jiangxi Province(No.jxsq2023102003)Project supported by the Guangdong Provincial Key Laboratory of Carbon Dioxide Resource Utilization(No.2024B121201001)Project supportedby the Major Research plan of the National Natural Science Foundation of China(No.92461310).
文摘Polyimide-linkage covalent organic frameworks(PI-COFs),as a subclass of the COFs material family,featuring the unique combination of excellent thermal stability of polyimide,tunable pore sizes,as well as high crystallinity and surface area of COFs,are expected to be a novel type of promising crystalline porous material with potential applications in adsorption and separation,catalysis,chemical sensing,and energy storage.Therefore,it is increasingly important to summarize polyimide-linkage in COFs and related applications and provide in-depth insight to accelerate future development.In this review,we offer a comprehensive overview of recent advancements in PI-COFs,emphasizing their synthesis methods,design principles and applications.Finally,our brief outlooks on the current challenges and future developments of PI-COFs are provided.Overall,this review aims to guide the recent and future development of PI-COFs.
基金supported by the National Science Foundation for Distinguished Young Scholars,China(No.52025065)the Key Research and Development Program of Shaanxi,China(No.2023GXLH-016)+3 种基金A*STAR LCER-FI,Singapore projects(LCERFI010015 U2102d2004 and LCERFI01-0033 U2102d2006)the National Research Foundation Singapore(NRF-CRP26-2021RS0002)the China Scholarship Council Program,China(Project ID:202306280178)for financial supportthe support of the Computing Center in Xi’an。
文摘Ion conduction in covalent-organic framework(COF)membranes is vital for energy conversion and storage.Conventional phenomenological methods based on the Arrhenius equation offer micrometer-scale cognition of ion conduction,whereas they ignore atomic details of ion-pore interactions and sophisticated conduction mechanisms,leaving gaps in high-resolution and bottom-up understanding of ion conduction in a nanoconfined space.In this study,we develop a hierarchical approach by holistically synergizing electronic structure calculations,first-principles molecular dynamics simulations,and thermodynamic integration methods to investigate the conduction of chloride(Cl^(-))and hydroxide(OH^(-))ions in a COF membrane.It is revealed that Cl^(-)ion with symmetric charge distribution undergoes weak solvation and tight ion-pore binding,which results in a tortuous conduction pathway,a high energy barrier,and slow diffusion based on the vehicular mechanism.In remarkable contrast,OH^(-)ion with heterogeneous charge distribution features strong solvation and weak ion-pore binding,and it jumps frequently via a smooth pathway and a low energy barrier.Moreover,OH^(-)ion conduction follows a mixed vehicular and Grotthuss mechanism,causing highly mutable ion identity and number,as well as superior dynamics due to proton transfer.This hierarchical approach provides sub-nanometer resolution insights into ion conduction,guiding intelligent membrane design and performance regulation to control ion conduction for emerging applications.
基金the support of the Shenzhen Science and Technology Program(no.JCYJ20220818100405012)National Natural Science Foundation of China(NSFC,no.62374080)Shenzhen Key Laboratory of Intelligent Manufacturing for Continuous Carbon Fiber Reinforced Composites(no.ZDSYS20220527171404011)。
文摘Composite solid-state electrolytes incorporating metal-organic frameworks(MOFs)demonstrate tremendous potential for ameliorating Li^(+)conduction in lithium metal batteries.However,their practical application is hindered by low ionic co nductivity and unstable Li^(+)transport at the electrode interfaces.To overcome these challenges,a previously unreported family of indium based MOFs(In-BDC-F_(x),x=0,4,6)with tunable fluorine content was synthesized and integrated into PVDF-HFP matrices to construct highperformance quasi-solid-state electrolytes.By systematically modulating linker fluorination,a bifunctional enhancement mechanism is revealed:fluorinated indium centers simultaneously suppress polymer crystallinity and establish preferential Li^(+)conduction pathways.Remarkably,In-BDC-F_(6) manifests exceptional synergistic interactions between-CF_(3) functionalities and indium coordination sites,amplifying Lewis acidity to facilitate LiTFSI dissociation and TFSI-immobilization,culminating in homogeneous LiF-enriched solid electrolyte interphases.The optimized electrolyte demonstrates compelling electrochemical performance:ionic conductivity of 9.68×10^(-4) S cm^(-1),Li^(+)transference number of 0.70,and electrochemical stability window of 4.96 V.Li‖Li symmetric cell demonstrated a critical current density of 3.5 mA cm^(-2) and stable plating/stripping for over 1000 h at 0.2 mA cm^(-2),while LiFePO_(4)‖Li cells retain96.66%capacity after 1300 cycles at 10C,underscoring the transformative potential of fluorinated MOF architectures in fast-charging solid-state batteries.
文摘CO_(2)reduction technology can promote the resource utilization of carbon and help alleviate global warming and energy supply pressure.It is an effective way to achieve energy conversion and utilization.Covalent organic frameworks(COFs)are porous crystalline materials formed by connecting organic monomers through covalent bonds.They have the characteristics of functional diversity and rich chemical properties.Their advantages,such as high porosity,a wide range of visible light absorption,and excellent charge separation efficiency,give them good potential in CO_(2)capture,separation,and conversion.Currently,Cu is a key metal in the catalytic CO_(2)reduction reaction(CO_(2)RR)for the preparation of high-value-added chemicals.The preparation of highly stable and large-pore Cu-based COFs using COFs as an ideal sacrificial template for loading Cu can be used to develop high-performance electrocatalysts and photocatalysts.In this review,we discuss the latest advancements in this field,including the development of various Cu-based COFs and their applications as catalysts for CO_(2)RR.Here,we mainly introduce the synthesis strategies,some important characterization information,and the applications of electrocatalytic and photocatalytic CO_(2)conversion using these previously reported Cu-based COFs.
文摘Modern business information systems face significant challenges in managing heterogeneous data sources,integrating disparate systems,and providing real-time decision support in complex enterprise environments.Contemporary enterprises typically operate 200+interconnected systems,with research indicating that 52% of organizations manage three or more enterprise content management systems,creating information silos that reduce operational efficiency by up to 35%.While attention mechanisms have demonstrated remarkable success in natural language processing and computer vision,their systematic application to business information systems remains largely unexplored.This paper presents the theoretical foundation for a Hierarchical Attention-Based Business Information System(HABIS)framework that applies multi-level attention mechanisms to enterprise environments.We provide a comprehensive mathematical formulation of the framework,analyze its computational complexity,and present a proof-of-concept implementation with simulation-based validation that demonstrates a 42% reduction in crosssystem query latency compared to legacy ERP modules and 70% improvement in prediction accuracy over baseline methods.The theoretical framework introduces four hierarchical attention levels:system-level attention for dynamic weighting of business systems,process-level attention for business process prioritization,data-level attention for critical information selection,and temporal attention for time-sensitive pattern recognition.Our complexity analysis demonstrates that the framework achieves O(n log n)computational complexity for attention computation,making it scalable to large enterprise environments including retail supply chains with 200+system-scale deployments.The proof-of-concept implementation validates the theoretical framework’s feasibility withMSE loss of 0.439 and response times of 0.000120 s per query,demonstrating its potential for addressing key challenges in business information systems.This work establishes a foundation for future empirical research and practical implementation of attention-driven enterprise systems.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.RS-2023-00217581)supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2024-00406724)supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(RS-2025-25430676)。
文摘The practical deployment of lithium metal batteries remains severely constrained,especially under elevated temperatures.Although metal-organic frameworks(MOFs)improve the thermal stability of liquid electrolytes by capturing them in well-ordered sub-nanopores,interparticle voids between MOF particles readily absorb liquid electrolyte,obscuring our understanding of the intrinsic role of nanopores in directing Li^(+)transport.To address this challenge,we introduce a one-dimensional(1D)MOF model architecture that eliminates interparticle effects and enables direct observation of Li^(+)solvation and de-solvation dynamics.Comparative studies of 1D HKUST-1 and ZIF-8 uncover distinct transport behaviors,supported by both experimental measurements and neural network potential-based molecular dynamics simulations.Building on these insights,we construct a hierarchical core-shell MOF architecture by integrating ZIF-8(core)and HKUST-1(shell)onto a hybrid fiber scaffold.This design harnesses the complementary strengths of both MOFs to achieve continuous ion pathways,directional Li^(+)conduction,and improved thermal and electrochemical resilience.
基金financially supported by the National Natural Science Foundation of China (No.51972302)。
文摘The recovery of gold from waste electronic and electric equipment(WEEE) has gained great attention with the increased number of WEEE,because it can largely alleviate the pressure on the environment and resources.Covalent organic frameworks(COFs) are ideal adsorbents for gold recovery owing to their large surface area,good stability,easily functionalized ability,periodic structures,and definitive nanopores.Herein,a cyano-functionalized COF(COF-CN) with high crystallinity was large-scale prepared under mild conditions for the recovery of gold.The introduction of cyano groups enable COF-CN to exhibit excellent gold recovery performance,which possesses fast adsorption kinetics,high cycling stability,and adsorption capacity up to 663.67 mg/g.Excitingly,COF-CN showed extremely high selectivity for gold ions,even in the presence of various competing cations and anions.The COF-CN maintained excellent selectivity and removal efficiency in gold recovery experiments from WEEE.The facile synthesis of COF-CN and its outstanding selectivity in actual samples make it an attractive opportunity for practical gold recovery.
基金supported by the Fundamental Research Funds for the Liaoning Universities(Grant No.LJ202410166012).
文摘The Ordos Basin is a large superimposed hydrocarbon-bearing basin in China,and further research on the sedimentary characteristics and sedimentary evolution of the sequence framework of target layers is of great theoretical and practical significance for guiding oil and gas exploration.The sedimentary facies and sedimentary evolution of the high-resolution sequence framework of the Carboniferous Taiyuan Formation in the Hangjinqi area have been systematically analyzed for the first time by drilling,logging and seismic data.The results show that four types of sequence interfaces can be identified in the Taiyuan Formation:regional unconformity surfaces,scour surfaces,lithologic-lithofacies transformation surfaces and flooding surfaces.According to the sedimentary response caused by the upward and downward movements of the base level at different levels,the Taiyuan Formation can be divided into 2 long-term cycles(LSC_(1)-LSC_(2)),4 mid-term cycles(MSC_(1)-MSC4)and 7 short-term cycles(SSC_(1)-SSC7).The long-and mid-term cycles correspond to members T_(1)and T_(2)and layers T_(1)-1,T_(1-2),T_(2-1),and T_(2)-2,respectively.Long-term cycles are dominated by C_(1);mid-term cycles are dominated by C_(1)and C_(2),followed by A2;and short-term cycles are dominated by C_(1),C_(2),A1 and A2.Under the high-resolution sequence stratigraphic framework,the Hangjinqi area underwent a transformation of fan delta and tidal flat depositional systems during the Taiyuan Formation sedimentary period.In the MSC_(1)-MSC_(2)stage,owing to a large-scale paleocontinent,the fan delta sedimentary body,which was limited in scale and scope,developed only in the southeastern corner and gradually transitioned basinward to tidal flat facies.In the MSC3-MSC4 stage,as the paleocontinent continuously decreased and the sedimentary range expanded,fan-delta plain sedimentation began in the study area.Several braided distributary channels with poor connectivity developed on the fan-delta plain,and between them were floodplains and peat swamps.
