Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge....Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.展开更多
2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(...2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(4)H_(2)N)C_(6)H4NC(Ph)=NDipp]-,Dipp=2,6-iPr_(2)C_(6)H_(3))were investigated.The 1H NMR spectroscopy indicate that the reaction of ytrrium dialkyl complex with one equivalent of 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10) produce the mixture of ytrrium alkyl-amido complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))(CH_(2)SiMe3)](R=CH_(3),2a;R=Ph,2b)and bis(amido)complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))_(2)](R=CH_(3),3a;R=Ph,3b).The yttrium bridging imido complex[Y(L)(2-CH_(3)-1-N-o-C_(2)B_(10)H_(10))]_(2)(4a)was obtained by heating the mixture at 55℃for 12 h.Complex 3a was isolated and characterized by treating the yttrium dialkyl complex with two equivalents of 1a.The structures of complexes 3a and 4a were verified by single-crystal Xray diffraction.CCDC:2424136,3a;2424137,4a.展开更多
Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering...Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering activity,it also presents challenges such as the necessity for high reaction temperatures and difficulties in achieving uniform mixing of its raw materials.This study presents a comprehensive investigation into preparation process of AlN nanopowders using a combination of hydrothermal synthesis and CRN.In the hydrothermal reaction,a homogeneous composite precursor consisting of carbon and boehmite(γ-AlOOH)is synthesized at 200℃using aluminum nitrate as the aluminum source,sucrose as the carbon source,and urea as the precipitant.During the hydrothermal process,the precursor develops a core-shell structure,with boehmite tightly coated with carbon(γ-AlOOH@C)due to electrostatic attraction.Compared with conventional precursor,the hydrothermal hybrid offers many advantages,such as ultrafine particles,uniform particle size distribution,good dispersion,high reactivity,and environmental friendliness.The carbon shell enhances thermodynamic stability of γ-Al_(2)O_(3) compared to the corundum phase(α-Al_(2)O_(3))by preventing the loss of the surface area in alumina.This stability enables γ-Al_(2)O_(3) to maintain high reactivity during CRN process,which initiates at 1300℃,and concludes at 1400℃.The underlying mechanisms are substantiated through experiments and thermodynamic calculations.This research provides a robust theoretical and experimental foundation for the hydrothermal combined carbothermal preparation of non-oxide ceramic nanopowders.展开更多
A strategy for the green synthesis of heterocyclicβ-ketosulfides via nucleophilic substitution ofα-halogenated ketone with het-eroaryl thiols in water media is presented.Compared with the available literature report...A strategy for the green synthesis of heterocyclicβ-ketosulfides via nucleophilic substitution ofα-halogenated ketone with het-eroaryl thiols in water media is presented.Compared with the available literature reports,this new method had the advantages of base-free,additives-free,simple operation,mild condition,greenness,high efficiency,tolerance of a broad scope of substrates.Furth-more,the reaction could easily be scaled up in gram scale and the products also could easily transformed to other useful organic compounds.Mechanism investigation indicated that the tautomerism of pyrimidine-2-thiol to pyrimidine-2(1H)-thione and the hy-drogen bonds played important roles in the reaction.展开更多
The rapid integration of Internet of Things(IoT)technologies is reshaping the global energy landscape by deploying smart meters that enable high-resolution consumption monitoring,two-way communication,and advanced met...The rapid integration of Internet of Things(IoT)technologies is reshaping the global energy landscape by deploying smart meters that enable high-resolution consumption monitoring,two-way communication,and advanced metering infrastructure services.However,this digital transformation also exposes power system to evolving threats,ranging from cyber intrusions and electricity theft to device malfunctions,and the unpredictable nature of these anomalies,coupled with the scarcity of labeled fault data,makes realtime detection exceptionally challenging.To address these difficulties,a real-time decision support framework is presented for smart meter anomality detection that leverages rolling time windows and two self-supervised contrastive learning modules.The first module synthesizes diverse negative samples to overcome the lack of labeled anomalies,while the second captures intrinsic temporal patterns for enhanced contextual discrimination.The end-to-end framework continuously updates its model with rolling updated meter data to deliver timely identification of emerging abnormal behaviors in evolving grids.Extensive evaluations on eight publicly available smart meter datasets over seven diverse abnormal patterns testing demonstrate the effectiveness of the proposed full framework,achieving average recall and F1 score of more than 0.85.展开更多
Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compa...Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.展开更多
Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fl...Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.展开更多
This paper considers the short-range sensing imple-mentation in continuous-wave(CW)phased array systems.We specifically address this CW short-range sensing challenges stemming from the self-interference cancellation(S...This paper considers the short-range sensing imple-mentation in continuous-wave(CW)phased array systems.We specifically address this CW short-range sensing challenges stemming from the self-interference cancellation(SIC)operation and synthesis requirement of arbitrary beampatterns for the sensing purpose,which has rarely been researched before.In this paper,unlike the only existed work that exploits the heuris-tic method and shares no analytical solution,an SIC pattern syn-thesis design is presented with a closed-form solution.By utiliz-ing the null-space projection(NSP)method,the proposed method effectively mitigates the self-interference to enable the in-band full-duplex operation of the array system.Subsequently,the NSP design will be innovatively embedded in a singular value decomposition(SVD)based weighted alternating reserve projec-tion(WARP)approach to efficiently synthesize an arbitrary desired pattern by solving a unique rank-deficient weighted least mean square problem.Numerical results validate the effective-ness of the proposed method in terms of beampattern,SIC per-formance,and sensing performance.展开更多
In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of...In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of DAAF from synthesis to spherical coating was designed and established in this paper, which combined ultrasonic micromixing reaction with microdroplet globular template. In the rapid micromixing stage, the microfluidic mixing technology with ultrasonic was used to synergistically strengthen the uniform and rapid mass transfer mixing reaction between raw materials to ensure the uniformity of DAAF particle nucleation-growth, and to prepare high-quality DAAF crystals with uniform structure and morphology and concentrated particle size distribution. In the microdroplet globular template stage, the microfluidic droplet technology was used to form a droplet globular template with uniform size under the shear action of the continuous phase of the dispersed phase solution containing DAAF particles and binder. The size of the droplet template was controlled by adjusting the flow rate ratio between the continuous phase and the dispersed phase. In the droplet globular template, with the diffusion of the solvent in the dispersed phase droplets, the binder precipitates to coat the DAAF into a ball, forming a DAAF microsphere with high sphericity, narrow particle size distribution and good monodispersity. The problem of discontinuity and DAAF particle suspension in the process was solved, and the coating theory under this process was studied. DAAF was coated with different binder formulations of fluororubber(F2604), nitrocellulose(NC) and NC/glycidyl azide polymer(GAP), and the process verification and evaluation of the system were carried out. The balling effects of large, medium and small droplet templates under different binder formulations were studied. The scanning electron microscope(SEM) results show that the three droplet templates under the three binder formulations exhibit good balling effect and narrow particle size distribution. The DAAF microspheres were characterized by powder X-ray diffraction(XRD), differential scanning calorimetry(DSC), thermo-gravimetric(TG) and sensitivity analyzer. The results showed that the crystal structure of DAAF did not change during the process, and the prepared DAAF microspheres had lower decomposition temperature and lower mechanical sensitivity than raw DAAF. The results of detonation parameters show that the coating of DAAF by using the above three binder formulations will not greatly reduce the energy output of DAAF, and has comparable detonation performance to raw DAAF. This study proves an efficient and safe continuous system from synthesis to spherical coating modification of explosives, which provides a new way for the continuous, safe and efficient preparation of spherical explosives.展开更多
Ru nanoparticles with fcc and hcp crystal phases were obtained by chemical reduction method using different precursors and reducing agents,and their catalytic properties in ammonia synthesis were compared.The catalyti...Ru nanoparticles with fcc and hcp crystal phases were obtained by chemical reduction method using different precursors and reducing agents,and their catalytic properties in ammonia synthesis were compared.The catalytic reaction rate(666.4μmol·h^(−1)·g^(−1))of fcc Ru catalyst is higher than that of hcp Ru(378.9μmol·h^(−1)·g^(−1))at the reaction temperature(400℃)and pressure(1 MPa).The results indicate that the exposed crystal faces have a certain impact on the catalytic activity.The dissociation ability to N_(2) of fcc Ru exposed(111)and(200)is better than that of hcp Ru exposed(100).When the ruthenium catalyst was loaded on rod-like CeO_(2) support,the ammonia synthesis activity was further improved.The ammonia synthesis activity of fcc Ru/CeO_(2) is 1.4 times higher than that of hcp Ru/CeO_(2) under the test conditions.展开更多
Different solvothermal reactions of ZnC2O_(4)with oxalic acid(H_(2)ox)and 1,2,4-triazole(Htrz)successfully gave a new quaternary(NJTU-Bai83,NJTU-Bai=Nanjing Tech University Bai's group)and a new quinary(NJTU-Bai84...Different solvothermal reactions of ZnC2O_(4)with oxalic acid(H_(2)ox)and 1,2,4-triazole(Htrz)successfully gave a new quaternary(NJTU-Bai83,NJTU-Bai=Nanjing Tech University Bai's group)and a new quinary(NJTU-Bai84)anionic metal-organic frameworks(MOFs),where NJTU-Bai83=(Me_(2)NH_(2))2[Zn_(3)(trz)_(2)(ox)_(3)]·2H_(2)O and NJTU-Bai84=(Me_(2)NH_(2))[Zn_(3)(trz)_(3)(ox)_(2)]·H_(2)O,respectively.With the[Zn_(2)(ox)4(trz)_(2)]secondary building unit(SBU)in NJTU-Bai83 replaced by the[Zn_(3)(ox)_(2)(trz)_(6)]and planar[Zn(ox)_(2)(trz)_(2)]ones in NJTU-Bai84,2D supramolecular building layers(SBLs)are changed from the A-layer and B-layer to another A-layer,while pillars are transformed from the tetrahedral[Zn(ox)_(2)(trz)_(2)]SBU to the irregular tetrahedral[Zn(ox)_(2)(trz)_(2)]and planar[Zn(ox)_(2)(trz)_(2)]SBUs.Thus,cdq-topological quaternary NJTU-Bai83 is tuned to(4,4,8)-c new topological quinary NJTU-Bai84.Two MOFs were well characterized by powder X-ray diffraction,thermogravimetric analysis,elemental analysis,etc.CCDC:2351819,NJTU-Bai83;2351820,NJTU-Bai84.展开更多
High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production meth...High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production method relies on repeated impregnation-carbonization and graphitization,and is plagued by lengthy preparation cycles and high energy consumption.Phase transition-assisted self-pressurized selfsintering technology can rapidly produce high-strength graphite materials,but the fracture strain of the graphite materials produced is poor.To solve this problem,this study used a two-step sintering method to uniformly introduce micro-nano pores into natural graphite-based bulk graphite,achieving improved fracture strain of the samples without reducing their density and mechanical properties.Using natural graphite powder,micron-diamond,and nano-diamond as raw materials,and by precisely controlling the staged pressure release process,the degree of diamond phase transition expansion was effectively regulated.The strain-to-failure of the graphite samples reached 1.2%,a 35%increase compared to samples produced by fullpressure sintering.Meanwhile,their flexural strength exceeded 110 MPa,and their density was over 1.9 g/cm^(3).The process therefore produced both a high strength and a high fracture strain.The interface evolution and toughening mechanism during the two-step sintering process were investigated.It is believed that the micro-nano pores formed have two roles:as stress concentrators they induce yielding by shear and as multi-crack propagation paths they significantly lengthen the crack propagation path.The two-step sintering phase transition strategy introduces pores and provides a new approach for increasing the fracture strain of brittle materials.展开更多
In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to character...In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.展开更多
A new two-step synthetic method was successfully developed to simplify the recrystallization process of lithium difluoro(oxalate)borate(LiODFB).Meanwhile,the purity of LiODFB as-prepared was determined by NMR,ICP-AES ...A new two-step synthetic method was successfully developed to simplify the recrystallization process of lithium difluoro(oxalate)borate(LiODFB).Meanwhile,the purity of LiODFB as-prepared was determined by NMR,ICP-AES and Karl Fisher measurements,respectively.The as-prepared LiODFB presents a high purity up to 99.95%.Its metal ions and water contents are under good control as well.Besides,its structure information and thermal properties were confirmed by FTIR,Raman and DSC-TGA analyses,respectively.LiODFB exerts fine thermostability and hypo-water-sensitivity and its structure information agrees well with previous literature.Furthermore,a combination of phase diagram and Raman spectroscopy were utilized to study the thermal phase behavior and ions coordination of LiODFB-DMC binary system to optimize the synthesis and recrystallization process.Although there are three types of molecular interaction forms(CIPs,AGG-IIa,AGG-IIIb)in LiODFB-DMC binary system,LiODFB can only be isolated as large single crystal solvate as LiODFB·(DMC)3/2 by slowly cooling subjected to the nucleation kinetics.Therefore,the fundamental information of our work is helpful in accelerating the application of LiODFB in Li-ion secondary batteries.展开更多
New solid complex of the antimony trichloride and dioxane was obtained th rough a reaction of the dioxane and the absolute methanol solution of the antimony trichloride.The formula of the complex is[SbCl_(3)·{(CH...New solid complex of the antimony trichloride and dioxane was obtained th rough a reaction of the dioxane and the absolute methanol solution of the antimony trichloride.The formula of the complex is[SbCl_(3)·{(CH_(2))_(4)O_(2)}_(1.5)].The crystal structure of the comple x belongs to cubic system,space group I-43d,a=17.1417(5)?,Z=16.The trivalent antimony ion not only bonds directly to three chlorine anions,but also is co ordinated by three oxygen atoms of th e dioxane molecules.Two oxygen atoms in a dioxane molecule wi ll coordinate to different antimony ions,respectively.展开更多
为解决遥感相机在运动过程中的抖动造成的图像位置偏移问题,提出了一种实时图像校正算法。由于在FPGA中采用HDL进行算法设计难度大、开发周期长,故设计中采用了C语言进行算法设计,然后借助Calypto公司的Catapult C Synthesis工具将抽象...为解决遥感相机在运动过程中的抖动造成的图像位置偏移问题,提出了一种实时图像校正算法。由于在FPGA中采用HDL进行算法设计难度大、开发周期长,故设计中采用了C语言进行算法设计,然后借助Calypto公司的Catapult C Synthesis工具将抽象的C设计转换成硬件RTL代码。在Catapult C Synthesis中对设计的算法进行了C/C++、RLT协同仿真测试,并在Xilinx XC5VLX110T型FPGA上进行了验证。仿真测试及硬件验证结果表明,采用Catapult C Synthesis设计的算法在时序、性能方面均满足设计要求,能够对偏移的图像进行实时校正。展开更多
基金supported by National Natural Science Foundation of China(52302034,52402060,52202201,52021006)Beijing National Laboratory for Molecular Sciences(BNLMS-CXTD202001)+1 种基金Shenzhen Science and Technology Innovation Commission(KQTD20221101115627004)China Postdoctoral Science Foundation(2024T170972)。
文摘Graphdiyne(GDY)is a two-dimensional carbon allotrope with exceptional physical and chemical properties that is gaining increasing attention.However,its efficient and scalable synthesis remains a significant challenge.We present a microwave-assisted approach for its continuous,large-scale production which enables synthesis at a rate of 0.6 g/h,with a yield of up to 90%.The synthesized GDY nanosheets have an average diameter of 246 nm and a thickness of 4 nm.We used GDY as a stable coating for potassium(K)metal anodes(K@GDY),taking advantage of its unique molecular structure to provide favorable paths for K-ion transport.This modification significantly inhibited dendrite formation and improved the cycling stability of K metal batteries.Full-cells with perylene-3,4,9,10-tetracarboxylic dianhydride(PTCDA)cathodes showed the clear superiority of the K@GDY anodes over bare K anodes in terms of performance,stability,and cycle life.The K@GDY maintained a stable voltage plateau and gave an excellent capacity retention after 600 cycles with nearly 100%Coulombic efficiency.This work not only provides a scalable and efficient way for GDY synthesis but also opens new possibilities for its use in energy storage and other advanced technologies.
文摘2-substituted-1-amino-o-carboranes 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10)(R=CH_(3),1a;R=Ph,1b)were synthesized and the reactions of these compounds with the yttrium dialkyl complex[Y(L)(CH_(2)SiMe3)_(2)](L=[2-(2,5-Me_(2)C_(4)H_(2)N)C_(6)H4NC(Ph)=NDipp]-,Dipp=2,6-iPr_(2)C_(6)H_(3))were investigated.The 1H NMR spectroscopy indicate that the reaction of ytrrium dialkyl complex with one equivalent of 2-R-1-NH_(2)-o-C_(2)B_(10)H_(10) produce the mixture of ytrrium alkyl-amido complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))(CH_(2)SiMe3)](R=CH_(3),2a;R=Ph,2b)and bis(amido)complex[Y(L)(2-R-1-NH-o-C_(2)B_(10)H_(10))_(2)](R=CH_(3),3a;R=Ph,3b).The yttrium bridging imido complex[Y(L)(2-CH_(3)-1-N-o-C_(2)B_(10)H_(10))]_(2)(4a)was obtained by heating the mixture at 55℃for 12 h.Complex 3a was isolated and characterized by treating the yttrium dialkyl complex with two equivalents of 1a.The structures of complexes 3a and 4a were verified by single-crystal Xray diffraction.CCDC:2424136,3a;2424137,4a.
基金National Key Research and Development Program of China(2022YFB3708500,2023YFB3611000)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2020ZZ109)。
文摘Currently,the carbothermal reduction-nitridation(CRN)process is the predominant method for preparing aluminum nitride(AlN)powder.Although AlN powder prepared by CRN process exhibits high purity and excellent sintering activity,it also presents challenges such as the necessity for high reaction temperatures and difficulties in achieving uniform mixing of its raw materials.This study presents a comprehensive investigation into preparation process of AlN nanopowders using a combination of hydrothermal synthesis and CRN.In the hydrothermal reaction,a homogeneous composite precursor consisting of carbon and boehmite(γ-AlOOH)is synthesized at 200℃using aluminum nitrate as the aluminum source,sucrose as the carbon source,and urea as the precipitant.During the hydrothermal process,the precursor develops a core-shell structure,with boehmite tightly coated with carbon(γ-AlOOH@C)due to electrostatic attraction.Compared with conventional precursor,the hydrothermal hybrid offers many advantages,such as ultrafine particles,uniform particle size distribution,good dispersion,high reactivity,and environmental friendliness.The carbon shell enhances thermodynamic stability of γ-Al_(2)O_(3) compared to the corundum phase(α-Al_(2)O_(3))by preventing the loss of the surface area in alumina.This stability enables γ-Al_(2)O_(3) to maintain high reactivity during CRN process,which initiates at 1300℃,and concludes at 1400℃.The underlying mechanisms are substantiated through experiments and thermodynamic calculations.This research provides a robust theoretical and experimental foundation for the hydrothermal combined carbothermal preparation of non-oxide ceramic nanopowders.
文摘A strategy for the green synthesis of heterocyclicβ-ketosulfides via nucleophilic substitution ofα-halogenated ketone with het-eroaryl thiols in water media is presented.Compared with the available literature reports,this new method had the advantages of base-free,additives-free,simple operation,mild condition,greenness,high efficiency,tolerance of a broad scope of substrates.Furth-more,the reaction could easily be scaled up in gram scale and the products also could easily transformed to other useful organic compounds.Mechanism investigation indicated that the tautomerism of pyrimidine-2-thiol to pyrimidine-2(1H)-thione and the hy-drogen bonds played important roles in the reaction.
文摘The rapid integration of Internet of Things(IoT)technologies is reshaping the global energy landscape by deploying smart meters that enable high-resolution consumption monitoring,two-way communication,and advanced metering infrastructure services.However,this digital transformation also exposes power system to evolving threats,ranging from cyber intrusions and electricity theft to device malfunctions,and the unpredictable nature of these anomalies,coupled with the scarcity of labeled fault data,makes realtime detection exceptionally challenging.To address these difficulties,a real-time decision support framework is presented for smart meter anomality detection that leverages rolling time windows and two self-supervised contrastive learning modules.The first module synthesizes diverse negative samples to overcome the lack of labeled anomalies,while the second captures intrinsic temporal patterns for enhanced contextual discrimination.The end-to-end framework continuously updates its model with rolling updated meter data to deliver timely identification of emerging abnormal behaviors in evolving grids.Extensive evaluations on eight publicly available smart meter datasets over seven diverse abnormal patterns testing demonstrate the effectiveness of the proposed full framework,achieving average recall and F1 score of more than 0.85.
基金National Natural Science Foundation of China(T2188101)。
文摘Among the synthesis techniques for graphene,chemical vapor deposition(CVD)enables the direct growth of graphene films on insulating substrates.Its advantages include uniform coverage,high quality,scalability,and compatibility with industrial processes.Graphene is chemically inert and has a zero-bandgap which poses a problem for its use as a functional layer,and nitrogen doping has become an important way to overcome this.Post-plasma treatment has been explored for the synthesis of nitrogen-doped graphene,but the procedures are intricate and not suitable for large-scale production.We report the direct synthesis of nitrogen-doped graphene on a 4-inch sapphire wafer by ethanol-assisted CVD employing pyridine as the carbon feedstock,where the nitrogen comes from the pyridine and the hydroxyl group in ethanol improves the quality of the graphene produced.Additionally,the types of nitrogen dopant produced and their effects on III-nitride epitaxy were also investigated,resulting in the successful illumination of LED devices.This work presents an effective synthesis strategy for the preparation of nitrogen-doped graphene,and provides a foundation for designing graphene functional layers in optoelectronic devices.
基金financially supported by Science and Technology on Applied Physical Chemistry Laboratory,China(Grant No.61426022220303)supported by the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.52305617)。
文摘Energetic materials,characterized by their capacity to store and release substantial energy,hold pivotal significance in some fields,particularly in defense applications.Microfluidics,with its ability to manipulate fluids and facilitate droplet formation at the microscale,enables precise control of chemical reactions.Recent scholarly endeavors have increasingly harnessed microfluidic reactors in the realm of energetic materials,yielding morphologically controllable particles with enhanced uniformity and explosive efficacy.However,crucial insights into microfluidic-based methodologies are dispersed across various publications,necessitating a systematic compilation.Accordingly,this review addresses this gap by concentrating on the synthesis of energetic materials through microfluidics.Specifically,the methods based on micro-mixing and droplets in the previous papers are summarized and the strategies to control the critical parameters within chemical reactions are discussed in detail.Then,the comparison in terms of advantages and disadvantages is attempted.As demonstrated in the last section regarding perspectives,challenges such as clogging,dead zones,and suboptimal production yields are non-ignoble in the promising fields and they might be addressed by integrating sound,optics,or electrical energy to meet heightened requirements.This comprehensive overview aims to consolidate and analyze the diverse array of microfluidic approaches in energetic material synthesis,offering valuable insights for future research directions.
基金supported by the National Natural Science Foundation of China(62001227)the Academy of Finland(315858341489).
文摘This paper considers the short-range sensing imple-mentation in continuous-wave(CW)phased array systems.We specifically address this CW short-range sensing challenges stemming from the self-interference cancellation(SIC)operation and synthesis requirement of arbitrary beampatterns for the sensing purpose,which has rarely been researched before.In this paper,unlike the only existed work that exploits the heuris-tic method and shares no analytical solution,an SIC pattern syn-thesis design is presented with a closed-form solution.By utiliz-ing the null-space projection(NSP)method,the proposed method effectively mitigates the self-interference to enable the in-band full-duplex operation of the array system.Subsequently,the NSP design will be innovatively embedded in a singular value decomposition(SVD)based weighted alternating reserve projec-tion(WARP)approach to efficiently synthesize an arbitrary desired pattern by solving a unique rank-deficient weighted least mean square problem.Numerical results validate the effective-ness of the proposed method in terms of beampattern,SIC per-formance,and sensing performance.
基金National Natural Science Foundation of China(Grant No.22005275)to provide fund for conducting experiments.
文摘In order to improve the energy output consistency of 3, 3’-diamino-4, 4’-azoxyfurazan(DAAF) in the new insensitive booster and the safety and efficiency in the preparation process, a continuous preparation system of DAAF from synthesis to spherical coating was designed and established in this paper, which combined ultrasonic micromixing reaction with microdroplet globular template. In the rapid micromixing stage, the microfluidic mixing technology with ultrasonic was used to synergistically strengthen the uniform and rapid mass transfer mixing reaction between raw materials to ensure the uniformity of DAAF particle nucleation-growth, and to prepare high-quality DAAF crystals with uniform structure and morphology and concentrated particle size distribution. In the microdroplet globular template stage, the microfluidic droplet technology was used to form a droplet globular template with uniform size under the shear action of the continuous phase of the dispersed phase solution containing DAAF particles and binder. The size of the droplet template was controlled by adjusting the flow rate ratio between the continuous phase and the dispersed phase. In the droplet globular template, with the diffusion of the solvent in the dispersed phase droplets, the binder precipitates to coat the DAAF into a ball, forming a DAAF microsphere with high sphericity, narrow particle size distribution and good monodispersity. The problem of discontinuity and DAAF particle suspension in the process was solved, and the coating theory under this process was studied. DAAF was coated with different binder formulations of fluororubber(F2604), nitrocellulose(NC) and NC/glycidyl azide polymer(GAP), and the process verification and evaluation of the system were carried out. The balling effects of large, medium and small droplet templates under different binder formulations were studied. The scanning electron microscope(SEM) results show that the three droplet templates under the three binder formulations exhibit good balling effect and narrow particle size distribution. The DAAF microspheres were characterized by powder X-ray diffraction(XRD), differential scanning calorimetry(DSC), thermo-gravimetric(TG) and sensitivity analyzer. The results showed that the crystal structure of DAAF did not change during the process, and the prepared DAAF microspheres had lower decomposition temperature and lower mechanical sensitivity than raw DAAF. The results of detonation parameters show that the coating of DAAF by using the above three binder formulations will not greatly reduce the energy output of DAAF, and has comparable detonation performance to raw DAAF. This study proves an efficient and safe continuous system from synthesis to spherical coating modification of explosives, which provides a new way for the continuous, safe and efficient preparation of spherical explosives.
基金The National Natural Science Foundation of China(22102194)The Science and Technology Plan of Gansu Province(24JRRA067,23ZDFA016)The Youth Innovation Promotion Association of CAS(2022427).
文摘Ru nanoparticles with fcc and hcp crystal phases were obtained by chemical reduction method using different precursors and reducing agents,and their catalytic properties in ammonia synthesis were compared.The catalytic reaction rate(666.4μmol·h^(−1)·g^(−1))of fcc Ru catalyst is higher than that of hcp Ru(378.9μmol·h^(−1)·g^(−1))at the reaction temperature(400℃)and pressure(1 MPa).The results indicate that the exposed crystal faces have a certain impact on the catalytic activity.The dissociation ability to N_(2) of fcc Ru exposed(111)and(200)is better than that of hcp Ru exposed(100).When the ruthenium catalyst was loaded on rod-like CeO_(2) support,the ammonia synthesis activity was further improved.The ammonia synthesis activity of fcc Ru/CeO_(2) is 1.4 times higher than that of hcp Ru/CeO_(2) under the test conditions.
文摘Different solvothermal reactions of ZnC2O_(4)with oxalic acid(H_(2)ox)and 1,2,4-triazole(Htrz)successfully gave a new quaternary(NJTU-Bai83,NJTU-Bai=Nanjing Tech University Bai's group)and a new quinary(NJTU-Bai84)anionic metal-organic frameworks(MOFs),where NJTU-Bai83=(Me_(2)NH_(2))2[Zn_(3)(trz)_(2)(ox)_(3)]·2H_(2)O and NJTU-Bai84=(Me_(2)NH_(2))[Zn_(3)(trz)_(3)(ox)_(2)]·H_(2)O,respectively.With the[Zn_(2)(ox)4(trz)_(2)]secondary building unit(SBU)in NJTU-Bai83 replaced by the[Zn_(3)(ox)_(2)(trz)_(6)]and planar[Zn(ox)_(2)(trz)_(2)]ones in NJTU-Bai84,2D supramolecular building layers(SBLs)are changed from the A-layer and B-layer to another A-layer,while pillars are transformed from the tetrahedral[Zn(ox)_(2)(trz)_(2)]SBU to the irregular tetrahedral[Zn(ox)_(2)(trz)_(2)]and planar[Zn(ox)_(2)(trz)_(2)]SBUs.Thus,cdq-topological quaternary NJTU-Bai83 is tuned to(4,4,8)-c new topological quinary NJTU-Bai84.Two MOFs were well characterized by powder X-ray diffraction,thermogravimetric analysis,elemental analysis,etc.CCDC:2351819,NJTU-Bai83;2351820,NJTU-Bai84.
基金Natural Science Foundation of Shanghai(24ZR1400800)he Natural Science Foundation of China(U23A20685,52073058,91963204)+1 种基金the National Key R&D Program of China(2021YFB3701400)Shanghai Sailing Program(23YF1400200)。
文摘High-performance graphite materials have important roles in aerospace and nuclear reactor technologies because of their outstanding chemical stability and high-temperature performance.Their traditional production method relies on repeated impregnation-carbonization and graphitization,and is plagued by lengthy preparation cycles and high energy consumption.Phase transition-assisted self-pressurized selfsintering technology can rapidly produce high-strength graphite materials,but the fracture strain of the graphite materials produced is poor.To solve this problem,this study used a two-step sintering method to uniformly introduce micro-nano pores into natural graphite-based bulk graphite,achieving improved fracture strain of the samples without reducing their density and mechanical properties.Using natural graphite powder,micron-diamond,and nano-diamond as raw materials,and by precisely controlling the staged pressure release process,the degree of diamond phase transition expansion was effectively regulated.The strain-to-failure of the graphite samples reached 1.2%,a 35%increase compared to samples produced by fullpressure sintering.Meanwhile,their flexural strength exceeded 110 MPa,and their density was over 1.9 g/cm^(3).The process therefore produced both a high strength and a high fracture strain.The interface evolution and toughening mechanism during the two-step sintering process were investigated.It is believed that the micro-nano pores formed have two roles:as stress concentrators they induce yielding by shear and as multi-crack propagation paths they significantly lengthen the crack propagation path.The two-step sintering phase transition strategy introduces pores and provides a new approach for increasing the fracture strain of brittle materials.
基金Project(51378510) supported by the National Natural Science Foundation of China。
文摘In existing studies, most slope stability analyses concentrate on conditions with constant temperature, assuming the slope is intact, and employ the Mohr-Coulomb (M-C) failure criterion for saturated soil to characterize the strength of the backfill. However, the actual working temperature of slopes varies, and natural phenomena such as rainfall and groundwater infiltration commonly result in unsaturated soil conditions, with cracks typically present in cohesive slopes. This study introduces a novel approach for assessing the stability of unsaturated soil stepped slopes under varying temperatures, incorporating the effects of open and vertical cracks. Utilizing the kinematic approach and gravity increase method, we developed a three-dimensional (3D) rotational wedge failure mechanism to simulate slope collapse, enhancing the traditional two-dimensional analyses. We integrated temperature-dependent functions and nonlinear shear strength equations to evaluate the impact of temperature on four typical unsaturated soil types. A particle swarm optimization algorithm was employed to calculate the safety factor, ensuring our method’s accuracy by comparing it with existing studies. The results indicate that considering 3D effects yields a higher safety factor, while cracks reduce slope stability. Each unsaturated soil exhibits a distinctive temperature response curve, highlighting the importance of understanding soil types in the design phase.
基金Project(51371198)supported by the National Natural Science Foundation of ChinaProject(K1202039-11)supported by the Science and Technology Project of Changsha,China
文摘A new two-step synthetic method was successfully developed to simplify the recrystallization process of lithium difluoro(oxalate)borate(LiODFB).Meanwhile,the purity of LiODFB as-prepared was determined by NMR,ICP-AES and Karl Fisher measurements,respectively.The as-prepared LiODFB presents a high purity up to 99.95%.Its metal ions and water contents are under good control as well.Besides,its structure information and thermal properties were confirmed by FTIR,Raman and DSC-TGA analyses,respectively.LiODFB exerts fine thermostability and hypo-water-sensitivity and its structure information agrees well with previous literature.Furthermore,a combination of phase diagram and Raman spectroscopy were utilized to study the thermal phase behavior and ions coordination of LiODFB-DMC binary system to optimize the synthesis and recrystallization process.Although there are three types of molecular interaction forms(CIPs,AGG-IIa,AGG-IIIb)in LiODFB-DMC binary system,LiODFB can only be isolated as large single crystal solvate as LiODFB·(DMC)3/2 by slowly cooling subjected to the nucleation kinetics.Therefore,the fundamental information of our work is helpful in accelerating the application of LiODFB in Li-ion secondary batteries.
文摘New solid complex of the antimony trichloride and dioxane was obtained th rough a reaction of the dioxane and the absolute methanol solution of the antimony trichloride.The formula of the complex is[SbCl_(3)·{(CH_(2))_(4)O_(2)}_(1.5)].The crystal structure of the comple x belongs to cubic system,space group I-43d,a=17.1417(5)?,Z=16.The trivalent antimony ion not only bonds directly to three chlorine anions,but also is co ordinated by three oxygen atoms of th e dioxane molecules.Two oxygen atoms in a dioxane molecule wi ll coordinate to different antimony ions,respectively.
文摘为解决遥感相机在运动过程中的抖动造成的图像位置偏移问题,提出了一种实时图像校正算法。由于在FPGA中采用HDL进行算法设计难度大、开发周期长,故设计中采用了C语言进行算法设计,然后借助Calypto公司的Catapult C Synthesis工具将抽象的C设计转换成硬件RTL代码。在Catapult C Synthesis中对设计的算法进行了C/C++、RLT协同仿真测试,并在Xilinx XC5VLX110T型FPGA上进行了验证。仿真测试及硬件验证结果表明,采用Catapult C Synthesis设计的算法在时序、性能方面均满足设计要求,能够对偏移的图像进行实时校正。
