With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controllin...With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.展开更多
Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in superca...Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.展开更多
In the era of the Internet,various network platforms have evolved into new hubs for information dissemination.Currently,China has established a platform-centered content regulation framework,wherein platforms proactiv...In the era of the Internet,various network platforms have evolved into new hubs for information dissemination.Currently,China has established a platform-centered content regulation framework,wherein platforms proactively enforce content regulations in accordance with legal censorship obligations.Additionally,platform policies and user agreements augment their authority in content regulation.The platforms can achieve cost-effective and highly efficient content regulation by leveraging their strategic advantages enabled by their own technical capabilities and extensive coverage.The platform self-regulation model,however,still faces challenges.First,accurately evaluating content remains a formidable task;second,ensuring effective platform publicity through self-regulation poses difficulties;third,users may potentially face disadvantages due to the platform’s right of self-regulation;and fourth,digital copyright owners face challenges when defending digital copyright disputes under the safe harbor rule.Therefore,it is imperative to establish,review,and revise the legal framework for content regulation of network platforms in order to enhance the efficiency of their governance systems.The formulation of the legal framework for content regulation of network platforms may encompass the following aspects:rationalizing obligations pertaining to platform content regulations,enhancing supervision over platform self-regulation,and establishing a dual-track responsibility system for digital copyright content regulation.This will ensure a harmonious balance among public interests,users’personal rights and interests,and commercial benefits through regulating the content on network platforms.展开更多
Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hamper...Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.展开更多
Graph Convolutional Neural Networks(GCNs)have been widely used in various fields due to their powerful capabilities in processing graph-structured data.However,GCNs encounter significant challenges when applied to sca...Graph Convolutional Neural Networks(GCNs)have been widely used in various fields due to their powerful capabilities in processing graph-structured data.However,GCNs encounter significant challenges when applied to scale-free graphs with power-law distributions,resulting in substantial distortions.Moreover,most of the existing GCN models are shallow structures,which restricts their ability to capture dependencies among distant nodes and more refined high-order node features in scale-free graphs with hierarchical structures.To more broadly and precisely apply GCNs to real-world graphs exhibiting scale-free or hierarchical structures and utilize multi-level aggregation of GCNs for capturing high-level information in local representations,we propose the Hyperbolic Deep Graph Convolutional Neural Network(HDGCNN),an end-to-end deep graph representation learning framework that can map scale-free graphs from Euclidean space to hyperbolic space.In HDGCNN,we define the fundamental operations of deep graph convolutional neural networks in hyperbolic space.Additionally,we introduce a hyperbolic feature transformation method based on identity mapping and a dense connection scheme based on a novel non-local message passing framework.In addition,we present a neighborhood aggregation method that combines initial structural featureswith hyperbolic attention coefficients.Through the above methods,HDGCNN effectively leverages both the structural features and node features of graph data,enabling enhanced exploration of non-local structural features and more refined node features in scale-free or hierarchical graphs.Experimental results demonstrate that HDGCNN achieves remarkable performance improvements over state-ofthe-art GCNs in node classification and link prediction tasks,even when utilizing low-dimensional embedding representations.Furthermore,when compared to shallow hyperbolic graph convolutional neural network models,HDGCNN exhibits notable advantages and performance enhancements.展开更多
本文论述了图书馆期刊发布系统的计算机软件结构,介绍了在Microsof.tNET Framework2.0技术下图书馆期刊发布系统的优点与缺点,并结合本馆自身实例介绍了如何利用Microsoft公司最新的开发工具Visual Studio 2005来实现图书馆期刊发布系...本文论述了图书馆期刊发布系统的计算机软件结构,介绍了在Microsof.tNET Framework2.0技术下图书馆期刊发布系统的优点与缺点,并结合本馆自身实例介绍了如何利用Microsoft公司最新的开发工具Visual Studio 2005来实现图书馆期刊发布系统的计算机软件。展开更多
Background Pan-genomics is a recently emerging strategy that can be utilized to provide a more comprehensive characterization of genetic variation.Joint calling is routinely used to combine identified variants across ...Background Pan-genomics is a recently emerging strategy that can be utilized to provide a more comprehensive characterization of genetic variation.Joint calling is routinely used to combine identified variants across multiple related samples.However,the improvement of variants identification using the mutual support information from mul-tiple samples remains quite limited for population-scale genotyping.Results In this study,we developed a computational framework for joint calling genetic variants from 5,061 sheep by incorporating the sequencing error and optimizing mutual support information from multiple samples’data.The variants were accurately identified from multiple samples by using four steps:(1)Probabilities of variants from two widely used algorithms,GATK and Freebayes,were calculated by Poisson model incorporating base sequencing error potential;(2)The variants with high mapping quality or consistently identified from at least two samples by GATK and Freebayes were used to construct the raw high-confidence identification(rHID)variants database;(3)The high confidence variants identified in single sample were ordered by probability value and controlled by false discovery rate(FDR)using rHID database;(4)To avoid the elimination of potentially true variants from rHID database,the vari-ants that failed FDR were reexamined to rescued potential true variants and ensured high accurate identification variants.The results indicated that the percent of concordant SNPs and Indels from Freebayes and GATK after our new method were significantly improved 12%-32%compared with raw variants and advantageously found low frequency variants of individual sheep involved several traits including nipples number(GPC5),scrapie pathology(PAPSS2),sea-sonal reproduction and litter size(GRM1),coat color(RAB27A),and lentivirus susceptibility(TMEM154).Conclusion The new method used the computational strategy to reduce the number of false positives,and simulta-neously improve the identification of genetic variants.This strategy did not incur any extra cost by using any addi-tional samples or sequencing data information and advantageously identified rare variants which can be important for practical applications of animal breeding.展开更多
As the main food source for humans, the global movement of the three major grains significantly impacts human survival and development. To investigate the evolution of the world cereal trade network and its developmen...As the main food source for humans, the global movement of the three major grains significantly impacts human survival and development. To investigate the evolution of the world cereal trade network and its development trend, a weighted directed dynamic multiplexed network was established using historical data on cereal trade, cereal import dependency ratio, and arable land per capita. Inspired by the MLP framework, we redefined the weight determination method for computing layer weights and edge weights of the target layer, modified the CN, RA, AA, and PA indicators, and proposed the node similarity indicator for weighted directed networks. The AUC metric, which measures the accuracy of the algorithm, has also been improved in order to finally obtain the link prediction results for the grain trading network. The prediction results were processed, such as web-based presentation and community partition. It was found that the number of generalized trade agreements does not have a decisive impact on inter-country cereal trade. The former large grain exporters continue to play an important role in this trade network. In the future, the world trade in cereals will develop in the direction of more frequent intercontinental trade and gradually weaken the intracontinental cereal trade.展开更多
Photoelectrochemical reduction of CO_(2)to produce CO with metal-organic frameworks(MOFs)is recognized as a desirable technology to mitigate CO_(2)emission and generate sustainable energy.To achieve highly efficient e...Photoelectrochemical reduction of CO_(2)to produce CO with metal-organic frameworks(MOFs)is recognized as a desirable technology to mitigate CO_(2)emission and generate sustainable energy.To achieve highly efficient electrocatalyst,it is essential to design a new material interface and uncover new reaction mechanisms or kinetics.Herein,we developed two metal-organic Cu-MOF and Bi-MOF layers using benzene tricarboxylic acid(H_(3)BTC)ligands on CuBi_(2)O_(4) photocathodes.Both MOF layers drastically improved the photoelectrochemical stability by suppressing the photo-corrosion through conformal surface passivation.The Cu-MOF modified CuBi_(2)O_(4) showed more significant charge separation and transfer efficiencies than the Bi-MOF modified control.Based on the transient photocurrent curves under the applied potential of 0.6 V vs.RHE,the rate-law analysis showed the CO_(2)photoreduction took place through a first-order reaction.Further,the photoelectrochemical impedance spectra(PEIS)revealed this reaction order,representing an“operando”analysis.Moreover,the reaction rate constant on Cu-MOF modified sample was higher than that on Bi-MOF modified one and bare CuBi_(2)O_(4).Combined with the density functional theory calculation,the surface absorption of CO_(2)and CO molecules and the higher energy barrier for*COOH intermediates could significantly determine the first order reaction.展开更多
Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and ...Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.展开更多
Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simpl...Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simplified expression of light fields with depth information discarded. In theory, computer vision tasks may achieve better performance as long as complete light fields are acquired.展开更多
This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world sof...This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world software.The existing analysis of software security vulnerabilities often focuses on specific features or modules.This partial and arbitrary analysis of the security vulnerabilities makes it challenging to comprehend the overall security vulnerabilities of the software.The key novelty lies in overcoming the constraints of partial approaches.The proposed framework utilizes data from various sources to create a comprehensive functionality profile,facilitating the derivation of real-world security guidelines.Security guidelines are dynamically generated by associating functional security vulnerabilities with the latest Common Vulnerabilities and Exposure(CVE)and Common Vulnerability Scoring System(CVSS)scores,resulting in automated guidelines tailored to each product.These guidelines are not only practical but also applicable in real-world software,allowing for prioritized security responses.The proposed framework is applied to virtual private network(VPN)software,wherein a validated Level 2 data flow diagram is generated using the Spoofing,Tampering,Repudiation,Information Disclosure,Denial of Service,and Elevation of privilege(STRIDE)technique with references to various papers and examples from related software.The analysis resulted in the identification of a total of 121 vulnerabilities.The successful implementation and validation demonstrate the framework’s efficacy in generating customized guidelines for entire systems,subsystems,and selected modules.展开更多
Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For ins...Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.展开更多
Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore mic...Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.展开更多
Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
基金the Beijing Nova Program(20230484431)Opening Project of State Silica-Based Materials Laboratory of Anhui Province(2022KF12)is gratefully acknowledged.
文摘With the continuous advancement of communication technology,the escalating demand for electromagnetic shielding interference(EMI)materials with multifunctional and wideband EMI performance has become urgent.Controlling the electrical and magnetic components and designing the EMI material structure have attracted extensive interest,but remain a huge challenge.Herein,we reported the alternating electromagnetic structure composite films composed of hollow metal-organic frameworks/layered MXene/nanocellulose(HMN)by alternating vacuum-assisted filtration process.The HMN composite films exhibit excellent EMI shielding effectiveness performance in the GHz frequency(66.8 dB at Kaband)and THz frequency(114.6 dB at 0.1-4.0 THz).Besides,the HMN composite films also exhibit a high reflection loss of 39.7 dB at 0.7 THz with an effective absorption bandwidth up to 2.1 THz.Moreover,HMN composite films show remarkable photothermal conversion performance,which can reach 104.6℃under 2.0 Sun and 235.4℃under 0.8 W cm^(−2),respectively.The unique micro-and macrostructural design structures will absorb more incident electromagnetic waves via interfacial polarization/multiple scattering and produce more heat energy via the local surface plasmon resonance effect.These features make the HMN composite film a promising candidate for advanced EMI devices for future 6G communication and the protection of electronic equipment in cold environments.
基金We are grateful to National Natural Science Foundation of China(Grant No.22375056,52272163)the Key R&D Program of Hebei(Grant No.216Z1201G)+1 种基金Natural Science Foundation of Hebei Province(Grant No.E2022208066,B2021208014)Key R&D Program of Hebei Technological Innovation Center of Chiral Medicine(Grant No.ZXJJ20220105).
文摘Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.
基金This paper is a phased achievement of the key project of the Chongqing Municipal Education Commission entitled“Research on Establishment of Regional Legal Framework for Rural Revitalization”(Project No.23SKJD033)the university-level project of Southwest University of Political Science&Law entitled“A Comparative Study on Legislation for Agricultural and Rural Modernization”(Project No.DFLF2020Y12).
文摘In the era of the Internet,various network platforms have evolved into new hubs for information dissemination.Currently,China has established a platform-centered content regulation framework,wherein platforms proactively enforce content regulations in accordance with legal censorship obligations.Additionally,platform policies and user agreements augment their authority in content regulation.The platforms can achieve cost-effective and highly efficient content regulation by leveraging their strategic advantages enabled by their own technical capabilities and extensive coverage.The platform self-regulation model,however,still faces challenges.First,accurately evaluating content remains a formidable task;second,ensuring effective platform publicity through self-regulation poses difficulties;third,users may potentially face disadvantages due to the platform’s right of self-regulation;and fourth,digital copyright owners face challenges when defending digital copyright disputes under the safe harbor rule.Therefore,it is imperative to establish,review,and revise the legal framework for content regulation of network platforms in order to enhance the efficiency of their governance systems.The formulation of the legal framework for content regulation of network platforms may encompass the following aspects:rationalizing obligations pertaining to platform content regulations,enhancing supervision over platform self-regulation,and establishing a dual-track responsibility system for digital copyright content regulation.This will ensure a harmonious balance among public interests,users’personal rights and interests,and commercial benefits through regulating the content on network platforms.
基金supported by the National Key Research and Development Program of China(2022YFB4002100)the development project of Zhejiang Province’s“Jianbing”and“Lingyan”(2023C01226)+4 种基金the National Natural Science Foundation of China(22278364,U22A20432,22238008,22211530045,and 22178308)the Fundamental Research Funds for the Central Universities(226-2022-00044 and 226-2022-00055)the Science Foundation of Donghai Laboratory(DH-2022ZY0009)the Startup Foundation for Hundred-Talent Program of Zhejiang University,and Scientific Research Fund of Zhejiang Provincial Education DepartmentXAS data were collected at BL14W1 beamline i Beijing Synchrotron Radiation Facility(BSRF),and Taiwan Synchrotron Radiation Facility(TSRF).
文摘Metal-organic frameworks(MOFs)have been developed as an ideal platform for exploration of the relationship between intrinsic structure and catalytic activity,but the limited catalytic activity and stability has hampered their practical use in water splitting.Herein,we develop a bond length adjustment strategy for optimizing naphthalene-based MOFs that synthesized by acid etching Co-naphthalenedicarboxylic acid-based MOFs(donated as AE-CoNDA)to serve as efficient catalyst for water splitting.AE-CoNDA exhibits a low overpotential of 260 mV to reach 10 mA cm^(−2)and a small Tafel slope of 62 mV dec^(−1)with excellent stability over 100 h.After integrated AE-CoNDA onto BiVO_(4),photocurrent density of 4.3 mA cm^(−2)is achieved at 1.23 V.Experimental investigations demonstrate that the stretched Co-O bond length was found to optimize the orbitals hybridization of Co 3d and O 2p,which accounts for the fast kinetics and high activity.Theoretical calculations reveal that the stretched Co-O bond length strengthens the adsorption of oxygen-contained intermediates at the Co active sites for highly efficient water splitting.
基金supported by the National Natural Science Foundation of China-China State Railway Group Co.,Ltd.Railway Basic Research Joint Fund (Grant No.U2268217)the Scientific Funding for China Academy of Railway Sciences Corporation Limited (No.2021YJ183).
文摘Graph Convolutional Neural Networks(GCNs)have been widely used in various fields due to their powerful capabilities in processing graph-structured data.However,GCNs encounter significant challenges when applied to scale-free graphs with power-law distributions,resulting in substantial distortions.Moreover,most of the existing GCN models are shallow structures,which restricts their ability to capture dependencies among distant nodes and more refined high-order node features in scale-free graphs with hierarchical structures.To more broadly and precisely apply GCNs to real-world graphs exhibiting scale-free or hierarchical structures and utilize multi-level aggregation of GCNs for capturing high-level information in local representations,we propose the Hyperbolic Deep Graph Convolutional Neural Network(HDGCNN),an end-to-end deep graph representation learning framework that can map scale-free graphs from Euclidean space to hyperbolic space.In HDGCNN,we define the fundamental operations of deep graph convolutional neural networks in hyperbolic space.Additionally,we introduce a hyperbolic feature transformation method based on identity mapping and a dense connection scheme based on a novel non-local message passing framework.In addition,we present a neighborhood aggregation method that combines initial structural featureswith hyperbolic attention coefficients.Through the above methods,HDGCNN effectively leverages both the structural features and node features of graph data,enabling enhanced exploration of non-local structural features and more refined node features in scale-free or hierarchical graphs.Experimental results demonstrate that HDGCNN achieves remarkable performance improvements over state-ofthe-art GCNs in node classification and link prediction tasks,even when utilizing low-dimensional embedding representations.Furthermore,when compared to shallow hyperbolic graph convolutional neural network models,HDGCNN exhibits notable advantages and performance enhancements.
基金Superior Farms sheep producersIBEST for their supportfinancial support from the Idaho Global Entrepreneurial Mission
文摘Background Pan-genomics is a recently emerging strategy that can be utilized to provide a more comprehensive characterization of genetic variation.Joint calling is routinely used to combine identified variants across multiple related samples.However,the improvement of variants identification using the mutual support information from mul-tiple samples remains quite limited for population-scale genotyping.Results In this study,we developed a computational framework for joint calling genetic variants from 5,061 sheep by incorporating the sequencing error and optimizing mutual support information from multiple samples’data.The variants were accurately identified from multiple samples by using four steps:(1)Probabilities of variants from two widely used algorithms,GATK and Freebayes,were calculated by Poisson model incorporating base sequencing error potential;(2)The variants with high mapping quality or consistently identified from at least two samples by GATK and Freebayes were used to construct the raw high-confidence identification(rHID)variants database;(3)The high confidence variants identified in single sample were ordered by probability value and controlled by false discovery rate(FDR)using rHID database;(4)To avoid the elimination of potentially true variants from rHID database,the vari-ants that failed FDR were reexamined to rescued potential true variants and ensured high accurate identification variants.The results indicated that the percent of concordant SNPs and Indels from Freebayes and GATK after our new method were significantly improved 12%-32%compared with raw variants and advantageously found low frequency variants of individual sheep involved several traits including nipples number(GPC5),scrapie pathology(PAPSS2),sea-sonal reproduction and litter size(GRM1),coat color(RAB27A),and lentivirus susceptibility(TMEM154).Conclusion The new method used the computational strategy to reduce the number of false positives,and simulta-neously improve the identification of genetic variants.This strategy did not incur any extra cost by using any addi-tional samples or sequencing data information and advantageously identified rare variants which can be important for practical applications of animal breeding.
文摘As the main food source for humans, the global movement of the three major grains significantly impacts human survival and development. To investigate the evolution of the world cereal trade network and its development trend, a weighted directed dynamic multiplexed network was established using historical data on cereal trade, cereal import dependency ratio, and arable land per capita. Inspired by the MLP framework, we redefined the weight determination method for computing layer weights and edge weights of the target layer, modified the CN, RA, AA, and PA indicators, and proposed the node similarity indicator for weighted directed networks. The AUC metric, which measures the accuracy of the algorithm, has also been improved in order to finally obtain the link prediction results for the grain trading network. The prediction results were processed, such as web-based presentation and community partition. It was found that the number of generalized trade agreements does not have a decisive impact on inter-country cereal trade. The former large grain exporters continue to play an important role in this trade network. In the future, the world trade in cereals will develop in the direction of more frequent intercontinental trade and gradually weaken the intracontinental cereal trade.
基金supported by the National Natural Science Foundation of China(Project.U1604121)and Startup funding from Suzhou University of Science and Technology.
文摘Photoelectrochemical reduction of CO_(2)to produce CO with metal-organic frameworks(MOFs)is recognized as a desirable technology to mitigate CO_(2)emission and generate sustainable energy.To achieve highly efficient electrocatalyst,it is essential to design a new material interface and uncover new reaction mechanisms or kinetics.Herein,we developed two metal-organic Cu-MOF and Bi-MOF layers using benzene tricarboxylic acid(H_(3)BTC)ligands on CuBi_(2)O_(4) photocathodes.Both MOF layers drastically improved the photoelectrochemical stability by suppressing the photo-corrosion through conformal surface passivation.The Cu-MOF modified CuBi_(2)O_(4) showed more significant charge separation and transfer efficiencies than the Bi-MOF modified control.Based on the transient photocurrent curves under the applied potential of 0.6 V vs.RHE,the rate-law analysis showed the CO_(2)photoreduction took place through a first-order reaction.Further,the photoelectrochemical impedance spectra(PEIS)revealed this reaction order,representing an“operando”analysis.Moreover,the reaction rate constant on Cu-MOF modified sample was higher than that on Bi-MOF modified one and bare CuBi_(2)O_(4).Combined with the density functional theory calculation,the surface absorption of CO_(2)and CO molecules and the higher energy barrier for*COOH intermediates could significantly determine the first order reaction.
基金the support by National Research Foundation of Singapore(NRF,Project:NRF-CRP262021RS-0002),for research conducted at the National University of Singapore(NUS)。
文摘Metal-organic framework(MOF)and covalent organic framework(COF)are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features,such as large surface area,tunable pore size,and functional surfaces,which have significant values in various application areas.The emerging 3D printing technology further provides MOF and COFs(M/COFs)with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths.However,the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’microstructural features,both during and after 3D printing.It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications.In this overview,the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths.Their differences in the properties,applications,and current research states are discussed.The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF.Throughout the analysis of the current states of 3D-printed M/COFs,the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.
文摘Dear Editor,Light fields give relatively complete description of scenes from perspective of angles and positions of rays. At present time, most of the computer vision algorithms take 2D images as input which are simplified expression of light fields with depth information discarded. In theory, computer vision tasks may achieve better performance as long as complete light fields are acquired.
基金This work is the result of commissioned research project supported by the Affiliated Institute of ETRI(2022-086)received by Junho AhnThis research was supported by the National Research Foundation of Korea(NRF)Basic Science Research Program funded by the Ministry of Education(No.2020R1A6A1A03040583)this work was supported by Korea Institute for Advancement of Technology(KIAT)Grant funded by the Korea government(MOTIE)(P0008691,HRD Program for Industrial Innovation).
文摘This research aims to propose a practical framework designed for the automatic analysis of a product’s comprehensive functionality and security vulnerabilities,generating applicable guidelines based on real-world software.The existing analysis of software security vulnerabilities often focuses on specific features or modules.This partial and arbitrary analysis of the security vulnerabilities makes it challenging to comprehend the overall security vulnerabilities of the software.The key novelty lies in overcoming the constraints of partial approaches.The proposed framework utilizes data from various sources to create a comprehensive functionality profile,facilitating the derivation of real-world security guidelines.Security guidelines are dynamically generated by associating functional security vulnerabilities with the latest Common Vulnerabilities and Exposure(CVE)and Common Vulnerability Scoring System(CVSS)scores,resulting in automated guidelines tailored to each product.These guidelines are not only practical but also applicable in real-world software,allowing for prioritized security responses.The proposed framework is applied to virtual private network(VPN)software,wherein a validated Level 2 data flow diagram is generated using the Spoofing,Tampering,Repudiation,Information Disclosure,Denial of Service,and Elevation of privilege(STRIDE)technique with references to various papers and examples from related software.The analysis resulted in the identification of a total of 121 vulnerabilities.The successful implementation and validation demonstrate the framework’s efficacy in generating customized guidelines for entire systems,subsystems,and selected modules.
基金supported by the National Natural Science Foundation of China(22179006)。
文摘Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.
基金This research was supported by Natural Science Foundation of Jiangsu Province(BK20220405)National Natural Science Foundation of China(21834004,22276100,22304086)+5 种基金Key Laboratory for Organic Electronics&Information Displays,NJUPT(GZR2022010010,GZR2023010045)Nanjing Science and Technology Innovation Project for Chinese Scholars Studying Abroad(NJKCZYZZ2022-01)Research Fund for Jiangsu Distinguished Professor(RK030STP22001)Natural Science Research Start-up Foundation of Recruiting Talents of NJUPT(NY221006,NY223051)Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB150025)State Key Laboratory of Analytical Chemistry for Life Science,Nanjing University(SKLACLS2311).
文摘Covalent organic frameworks(COFs),a rapidly developing category of crystalline conjugated organic polymers,possess highly ordered structures,large specific surface areas,stable chemical properties,and tunable pore microenvironments.Since the first report of boroxine/boronate ester-linked COFs in 2005,COFs have rapidly gained popularity,showing important application prospects in various fields,such as sensing,catalysis,separation,and energy storage.Among them,COFs-based electrochemical(EC)sensors with upgraded analytical performance are arousing extensive interest.In this review,therefore,we summarize the basic properties and the general synthesis methods of COFs used in the field of electroanalytical chemistry,with special emphasis on their usages in the fabrication of chemical sensors,ions sensors,immunosensors,and aptasensors.Notably,the emerged COFs in the electrochemiluminescence(ECL)realm are thoroughly covered along with their preliminary applications.Additionally,final conclusions on state-of-the-art COFs are provided in terms of EC and ECL sensors,as well as challenges and prospects for extending and improving the research and applications of COFs in electroanalytical chemistry.
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.