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Coordination environments build up and tune a superior synergistic “genome” toward novel trifunctional (TM-N_(x)O_(4−x))@g- C_(16)N_(3)-H_(3): High-throughput inspection of ultra-high activity for water splitting and oxygen reduction reactions

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Nano Research 2024年第4期17卷 2337-2351页

作者： Chunyao fang xian Wang Qiang zhang Xihang zhang Chenglong Shi Jingcheng Xu Mengyu Yang Department of Physics University of Shanghai for Science and TechnologyShanghai 200093China School of Materials and Chemistry University of Shanghai for Science and TechnologyShanghai 200093China

Emerging as a prominent area of focus in energy conversion and storage technologies,the development of highly active metal-based single-atom catalysts(SACs)holds great signiﬁcance in searching alternatives to replace precious metals toward the efficient,stable,and low-cost hydrogen evolution reaction(HER),as well as the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR).Combining the tremendous tunability of ligand and coordination environment with rich metal-based electrocatalysts can create breakthrough opportunities for achieving both high stability and ***,we propose a novel and stable holey graphene-like carbon nitride monolayer g-C_(16)N5(N_(4)@g-C_(16)N_(3))stoichiometries interestingly behaving as a natural substrate for constructing SACs((TM-N_(4))@g-C_(16)N_(3)),whose evenly distributed holes map rich and uniform nitrogen coordination positions with electron-rich lone pairs for anchoring transition metal(TM)***,we employed density functional theory(DFT)calculations to systematically investigate the electrocatalytic activity of(TM-N_(4))@g-C_(16)N_(3) toward HER/OER/ORR,meanwhile considering the synergistic modulation of H-loading and O-coordination((TM-N_(x)O_(4-x))@g-C_(16)N_(3)^(-)H_(3),x=0–4).Together a“four-step procedure”screening mechanism with the first-principles high-throughput calculations,we find that(Rh-N_(4))and(Ir-N_(2)O_(2)-II)distributed on g-C_(16)N_(3)^(-)H_(3) can modulate the adsorption strength of the adsorbates,thus achieving the best HER/OER/ORR performance among 216 candidates,and the lowest overpotential of 0.098/0.3/0.46 V and 0.06/0.48/0.45 V,***,the d-band center,crystal orbital Hamilton population(COHP),and molecular orbitals are used to reveal the OER/ORR activity ***,the Rh/Ir-d orbital is dramatically hybridized with the O-p orbital of the oxygenated adsorbates,so that the lone-electrons incipiently locate at the antibonding orbital pair up and popula

关键词： single atom catalysts loading and coordination hydrogen evolution reaction oxygen evolution reaction oxygen reduction reaction

Stabilization/solidification mechanisms of tin tailings and fuming slag-based geopolymers for different heavy metals

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Frontiers of Environmental Science & Engineering 2024年第5期18卷 43-55页

作者： xian Zhou Zhengfu zhang Hui Yang School of Materials Science and Engineering Kunming University of Science and TechnologyKunming650093China Kunming Metallurgical Research Institute Co. Ltd.Kunming650031China

Tin mine tailings(TMT)and fuming slag(FS)contain many heavy metals(As,Cr,Cu,Zn and Mn)that cause severe pollution to the ***,geopolymers were prepared using TMT,FS and flue gas desulfurization gypsum(FGDG)to immobilize heavy metals,and their compressive strength and heavy metal leaching toxicity were *** was first determined that T4F5(TMT:FS=4:5)sample exhibited the highest compressive strength(7.83 MPa).T4F5 achieved 95%immobilization efficiency for As and Cr,and nearly 100%for Cu,Zn and Mn,showing good immobilization performance.A series of characterization analyses showed that heavy metal cations can balance the charge in the geopolymer and replace Al in the geopolymer structure to form covalent *** addition,about 2%–20%of heavy metal Fe was immobilized in hydration products,heavy metal hydroxides and non-bridging Si–O and Al–O coordination with silica-aluminate ***_(3)^(3−) was oxidized into AsO_(4)^(3−),which may form Ca–As or Fe–As ***_(2)O_(7)^(2−)was converted to CrO_(4)^(2−)under alkaline environment and then combined with OH−to form Cr(OH)3 ***^(2+)may react directly with dissolved silicate to form Mn_(2)SiO_(4) and also form Mn(OH)_(2) *** unstable Mn(OH)_(2) can be further oxidized to MnO_(2).The heavy metal cations were immobilized in the silicoaluminate lattice,while the anions tended to form insoluble *** results may benefit the industry and government for better handling of TMT,FS and solid wastes containing the abovementioned five heavy metals.

关键词： Heavy metals Cementitious materials Tin tailings Stabilization/solidification Redox

Three-dimensional porous bimetallic metal–organic framework/gelatin aerogels: A readily recyclable peroxymonosulfate activator for efficient and continuous organic dye removal

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Chinese Journal of Chemical Engineering 2024年第7期71卷 193-202页

作者： Wenlong xiang xian zhang Rou Xiao Yanhui zhang College of Chemistry Chemical Engineering and EnvironmentFujian Province Key Laboratory of Morden Analytical Science and Separation TechnologyMinnan Normal UniversityZhangzhou 363000China Fujian Provincial University Key Laboratory of Pollution Monitoring and Control Minnan Normal UniversityZhangzhou 363000China

As promising catalysts for the degradation of organic pollutants,metal–organic frameworks(MOFs)often face limitations due to the particle agglomeration and challenging recovery in liquid-catalysis application,stemming from their powdery *** macroscopic structures from pulverous MOF is thus of great importance for broadening their practical *** this study,three-dimensional porous MOF aerogel catalysts were successfully fabricated for degrading organic dyes by activating peroxymonosulfate(PMS).MOF/gelatin aerogel(MOF/GA)catalysts were prepared by directly integrating bimetallic FeCo-BDC with gelatin solutions,followed by freeze-drying and low-temperature *** FeCo-BDC-0.15/GA/PMS system exhibited remarkable performance in degrading various organic dyes,eliminating 99.2%of rhodamine B within a mere 5 *** to the GA/PMS system,there was over a 300-fold increase in the reaction rate ***,high removal efficiency was maintained across varying conditions,including different solution pH,co-existing inorganic anions,and natural water *** trapping experiments and electron paramagnetic resonance analysis revealed that the degradation involved radical(SO_(4)^(-)·)and non-radical routes(^(1)O_(2)),of which ^(1)O_(2) was ***,even after a continuous 400-min reaction in a fixed-bed reactor at a liquid hourly space velocity of 27 h^(-1),the FeCo-BDC/GA composite sustained a degradation efficiency exceeding 98.7%.This work presents highly active MOF-gelatin aerogels for dye degradation and expands the potential for their large-scale,continuous treatment application in organic dye wastewater management.

关键词： Catalyst Environment Wastewater Metal–organic framework Gelatin aerogel Peroxymonosulfate

FPGA-based position reconstruction method for neutron beam flux spatial distribution measurement in BNCT

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Nuclear Science and Techniques 2024年第3期35卷 96-108页

作者： Wei Jiang Ping Cao Yi-Ming Wu xian-Ke Liu Zhu-Jun fang Zhi-Yong zhang Bin Shi Jun Chen State Key Laboratory of Particle Detection and Electronics University of Science and Technology of ChinaHefei 230026China Department of Modern Physics University of Science and Technology of ChinaHefei 230026China School of Nuclear Science and Technology University of Science and Technology of ChinaHefei 230026China National Key Laboratory for Metrology and Calibration Techniques China Institute of Atomic EnergyBeijing 102413China

A new measurement method for the spatial distribution of neutron beam flux in boron neutron capture therapy(BNCT)is being developed based on the two-dimensional Micromegas *** address the issue of long processing times in traditional offline position reconstruction methods,this paper proposes a field programmable gate array based online position reconstruction method utilizing the micro-time projection chamber *** method encapsulates key technical aspects:a self-adaptive serial link technique built upon the dynamical adjustment of the delay chain length,fast sorting,a coordinate-matching technique based on the mapping between signal timestamps and random access memory(RAM)addresses,and a precise start point-merging technique utilizing a circular combined *** performance test of the selfadaptive serial link shows that the bit error rate of the link is better than 10-12 at a confidence level of 99%,ensuring reliable data *** experiment utilizing the readout electronics and Micromegas detector shows a spatial resolution of approximately 1.4 mm,surpassing the current method’s resolution level of 5 *** beam experiment confirms that the readout electronics system can obtain the flux spatial distribution of neutron beams online,thus validating the feasibility of the position reconstruction *** online position reconstruction method avoids traditional methods,such as bubble sorting and traversal searching,simplifies the design of the logic firmware,and reduces the time complexity from O(n2)to O(n).This study contributes to the advancement in measuring neutron beam flux for BNCT.

关键词： Position reconstruction FPGA Readout electronics Neutron flux spatial distribution

Enhanced hydrogen evolution performance by 3D ordered macroporous Ru-CoP@NC electrocatalysts

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Rare Metals 2024年第3期43卷 1095-1107页

作者： Chen-Chen zhang Sheng Wei Li-xian Sun Yi-fang Ouyang Fen Xu Hai-Liang Chu Hong-GePan Li-Xin Chen Xue-zhang Xiao School of Material Science and Engineering Guilin University of Electronic TechnologyGuilin541004China School of Chemistry and Chemical Engineering Guangxi UniversityNanning530004China Shenzhen Institute of Advanced Technology Chinese Academy of SciencesShenzhen518055GuangdongChina Institute of Science and Technology for New Energy Xi'an Technological UniversityXi'an710021China School of Materials Science and Engineering Zhejiang UniversityHangzhou310058China

Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel ***,the main challenge is to develop high performance,low cost and chemically stable electrocatalysts to decline the energy barriers and enhance the sluggish kinetics of hydrogen evolution reaction(HER).Herein,a three-dimensional hierarchically ordered macroporous Ru-CoP@NC electrocatalyst(3DOM Ru-CoP@NC)derived from ordered macro-microporous metal-organic frameworks has been prepared using the precursor@template and double-solvent *** prepared 3DOM Ru-CoP@NC catalyst exhibits an overpotential of 15 mV(j=10 mA·cm^(-2))and a reaction Tafel slope of 38 mV·dec^(-1)in alkaline electrolyte,which are superior to commercial Pt@C ***,the overpotential and reaction Tafel slope of this catalyst in acidic media are 45 mV and 50 mV·dec^(-1),*** outstanding HER activities of 3DOM Ru-CoP@NC catalysts are ascribed to the 3D highly interconnectedreticular nanospaces that can increase effective reaction active *** N dope d carbon framework improves the electronic properties and ***,the strong interaction of Ru and CoP nanoparticles also boosts the HER *** results indicate that 3DOM Ru-CoP@NC catalysts with high catalytic activities have a broad application prospect in the future.

关键词： Hydrogen evolution reaction Template method 3D ordered macroporous Ru-CoP@NC

Immobilizing Triphenylamine with Photoredox Inert Sr^(2+)Forming Sr-MOF with Controlled Electron Migration for Photocatalytic Oxidation of Thiols to Disulfides

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Chinese Journal of Chemistry 2024年第10期42卷 1093-1099页

作者： Ying-Xia Wang fang Zheng Dong-Xia Song Bao-Yue Niu Lu-Qian Deng xian-Ming zhang Key Laboratory of Magnetic Molecules and Magnetic Information Materials(Ministry of Education) Schoolof Chemistry and Materials ScienceShanxi Normal UniversityTaiyuanShanxi 030006China Key Laboratory of Interface Science and Engineering in Advanced Material(Ministry of Education) College of ChemistryTaiyuan University of TechnologyTaiyuanShanxi 030024China

The photocatalytic oxidative coupling of thiols is one of the most popular methods to synthesize the *** and its derivatives(TPAs)are promising for the above reaction,but suffer from the easy polymerization and difficult *** overcome these obstacles while controlling the photogenerated electrons transfer directly to target substrates,herein,we constructed one TPA-based metal-organic framework(MOF),(Me_(2)NH_(2))[Sr(TCBPA)]·DMA·3H_(2)O(1),by direct self-assembly of tris(4′-carboxybiphenyl)amine(H_(3)TCBPA)and photoredox inert strontium ion(Sr^(2+)).DFT calculations revealed that the valence band maximum(VBM)and the conduction band minimum(CBM)are mainly located on TCBPA^(3-),successfully inhibiting the undesirable electron migration to metal *** results indicated that 1 displays superior performance than homogeneous H_(3)TCBPA,which may result from the abundant π…π and C—H…π interactions between the well-arranged TCBPA^(3-)and the build-in electric field between the anionic framework and the Me_(2)NH^(2+).This work highlights that immobilizing TPAs into MOFs is one promising approach to designing heterogeneous photocatalysts for the synthesis of disulfides by oxidative coupling of thiols.

关键词： Triphenylamine Metal-organic frameworks Strontium Photooxidation Thiols Disulfides

Limit Theorems for Critical Galton-Watson Processes with Immigration Stopped at Zero

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Acta Mathematica Sinica,English Series 2024年第2期40卷 435-450页

作者： Dou Dou LI Mei zhang xian Yu zhang College of Statistics and Data Science Faculty of ScienceBeijing University of TechnologyBeijing 100124P.R.China Laboratory of Mathematics and Complex Systems(Ministry of Education) School of Mathematical SciencesBeijing Normal UniversityBeijing 100875P.R.China

In this paper,we consider a critical Galton-Watson branching process with immigration stopped at zero *** precise estimation on the probability generating function of the n-th population are obtained,and the tail prob... 详细信息

关键词： Branching immigration critical life period limit theorems

Hybrid vibration isolation optimization of a flexible manipulator based on neural network agent model

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Chinese Journal of Aeronautics 2024年第5期37卷 482-505页

作者： Yongxin zhang Liang LI Dingguo zhang Wei-Hsin LIAO xian GUO School of Science Nanjing University of Science and TechnologyNanjing 210094China Department of Mechanical and Automation Engineering The Chinese University of Hong KongHong KongChina

Segmented Active Constrained Layer Damping(SACLD)is an intelligent vibration-damping structure,which could be applied to the sectors of aviation,aerospace,and transportation engineering to reduce the vibration of flexible ***,machine learning technology is widely used in the engineering field because of its efficient multi-objective *** dynamic simulation of a rotational segmental flexible manipulator system is presented,in which enhanced active constrained layer damping is carried out,and the neural network model of Genetic Algorithm-Back Propagation(GA-BP)algorithm is *** suppression and structural optimization of the SACLD manipulator model are studied based on vibration mode and damping *** modal responses of the SACLD manipulator model at rest and rotation are *** addition,the four model indices are optimized using the GA-BP neural network:axial incision size,axial incision position,circumferential incision size,and circumferential incision ***,the best model for vibration suppression is obtained.

关键词： Machine learning Vibration suppression Flexible manipulator Segmented active constrained layer damping Structural optimization

Improved Subsynchronous Oscillation Parameter Identification with Synchrophasor Based on Matrix Pencil Method in Power Systems

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Journal of Modern Power Systems and Clean Energy 2024年第1期12卷 22-33页

作者： Xiaoxue zhang fang zhang Wenzhong Gao Jinghan He the School of Electrical Engineering Beijing Jiaotong UniversityBeijing 100044China the Department of Electrical and Computer Engineering University of DenverDenverUSA

The subsynchronous oscillations(SSOs)related to renewable generation seriously affect the stability and safety of the power *** realize the dynamic monitoring of SSOs by utilizing the high computational efficiency and noise-resilient features of the matrix pencil method(MPM),this paper propos es an improved MPM-based parameter identification with syn *** MPM is enhanced by the angular frequency fitting equations based on the characteristic polynomial coeffi cients of the matrix pencil to ensure the accuracy of the identi fied parameters,since the existing eigenvalue solution of the MPM ignores the angular frequency conjugation constraints of the two fundamental modes and two oscillation ***,the identification and recovery of bad data are proposed by uti lizing the difference in temporal continuity of the synchropha sors before and after noise *** proposed parameter identification is verified with synthetic,simulated,and actual measured phase measurement unit(PMU)*** with the existing MPM,the improved MPM achieves better accuracy for parameter identification of each component in SSOs,better real-time performance,and significantly reduces the effect of bad data.

关键词： Subsynchronous oscillations(SSOs) synchrophasor parameter identification matrix pencil method bad data