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Synthesis and characterization of iron clusters with an icosahedral [Fe@Fe12]16+ Core

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National Science Review 2024年第4期11卷 123-129页

作者： Gan xu Yun-Shu Cui xue-lian Jiang Cong-Qiao xu Jun Li xu-Dong Chen Jiangsu Collaborative Innovation Center of Biomedical Functional Materials and Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials Science Nanjing Normal University Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry Southern University of Science and Technology Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education Tsinghua University State Key Laboratory of Coordination Chemistry Nanjing University

Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage ***,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron *** this work,we have synthesized,crystallized,and characterized a（Tp*）4W4S12(Fe@Fe12) cluster(Tp*=tris（3,5-dimethyl-1-pyrazolyl）borate（1-）),which features a rare trideca-nuclear,icosahedral[Fe@Fe12] cluster core with direct multicenter iron-iron bonding between the interstitial iron（Fei） and peripheral irons（Fep）,as well as Fep…Fepferromagnetic *** chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the [Fe@Fe12]16+core,assisted by its bonding interactions with the peripheral tridentate [（Tp*）WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-Wσ *** ground-state electron spin is theoretically predicted to be S=32/2 for the *** existence of low oxidation-state（OS～+1.23） iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.

关键词： Fe13 cluster iron-sulfur cluster low-valence iron iron−iron bond high spin complex

Acid-rock reaction kinetics in a two-scale model based on reaction order correction

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Petroleum Science 2024年第3期21卷 2089-2101页

作者： xue-Song Li Ning Qi Ze-Hui Zhang lian Liu Xia-Qing Li xu-Hang Su School of Petroleum Engineering China University of Petroleum(East China) Key Lab of Unconventional Oil & Gas Development Ministry of Education China University of Petroleum(East China) SINOPEC Northwest Oilfield Branch Company Petroleum Engineering Technology Research Institute SINOPEC Shengli Oilfield Company

The reaction order plays a crucial role in evaluating the response rate of acid-rock. However, the conventional two-scale model typically assumes that the reaction order is constant as one, which can lead to significant deviations from reality. To address this issue, this study proposes a novel multi-order dynamic model for acid-rock reaction by combining rotating disk experimental data with theoretical *** numerical simulations, this model allows for the investigation of the impact of acidification conditions on different orders of reaction, thereby providing valuable insights for on-site *** analysis reveals that higher response orders require higher optimal acid liquid flow rates, and lower optimal H+diffusion coefficients, and demonstrate no significant correlation with acid ***, it is recommended to increase the displacement and use high-viscosity acid for reservoirs with high calcite content, while reducing the displacement and using low-viscosity acid for reservoirs with high dolomite content.

关键词： Reaction order Two-scale model Wormhole propagation Carbonate rocks Numerical simulation

Linear Quadratic Optimal Control for Systems Governed by First-Order Hyperbolic Partial Differential Equations

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Journal of Systems Science & Complexity 2024年第1期37卷 230-252页

作者： xue Xiaomin xu Juanjuan ZHANG Huanshui School of Control Science and Engineering Shandong UniversityJinan 250061China College of Electrical Engineering and Automation Shandong University of Science and TechnologyQingdao 266000China

This paper focuses on linear-quadratic(LQ)optimal control for a class of systems governed by first-order hyperbolic partial differential equations(PDEs).Different from most of the previous works,an approach of discretization-then-continuousization is proposed in this paper to cope with the infinite-dimensional nature of PDE *** contributions of this paper consist of the following aspects:(1)The differential Riccati equations and the solvability condition of the LQ optimal control problems are obtained via the discretization-then-continuousization method.(2)A numerical calculation way of the differential Riccati equations and a practical design way of the optimal controller are ***,the relationship between the optimal costate and the optimal state is established by solving a set of forward and backward partial difference equations(FBPDEs).(3)The correctness of the method used in this paper is verified by a complementary continuous method and the comparative analysis with the existing operator results is *** is shown that the proposed results not only contain the classic results of the standard LQ control problem of systems governed by ordinary differential equations as a special case,but also support the existing operator results and give a more convenient form of computation.

关键词： Discretization-then-continuousization method first-order hyperbolic partial differential equations forward and backward partial difference equations linear quadratic optimal control.

Influence of Incomplete Soil Plugs on Bearing Capacities of Bucket Foundations in Clay

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China Ocean Engineering 2024年第1期38卷 144-155页

作者： LI Hui-shan LIU Run YANG xu lian Ji-jian State Key Laboratory of Hydraulic Engineering Intelligent Construction and Operation Tianjin UniversityTianjin 300072China School of Civil Engineering Tianjin UniversityTianjin 300072China Institute of Marine Energy and Intelligent Construction Tianjin University of TechnologyTianjin 300384China

Due to the uneven seabed and heaving of soil during pumping,incomplete soil plugs may occur during the installation of bucket foundations,and the impacts on the bearing capacities of bucket foundations need to be *** this paper,the contact ratio(the ratio of the top diameter of the soil plug to the diameter of the bucket)and the soil plug ratio(the ratio of the soil heave height to the skirt height)are defined to describe the shape and size of the incomplete soil ***,finite element models are established to investigate the bearing capacities of bucket foundations with incomplete soil plugs and the influences of the contact ratios,and the soil plug ratios on the bearing capacities are *** results show that the vertical bearing capacity of bucket foundations in homogeneous soil continuously improves with the increase of the contact ***,in normally consolidated soil,the vertical bearing capacity barely changes when the contact ratio is smaller than 0.75,while the bearing capacity suddenly increases when the contact ratio increases to 1 due to the change of failure *** contact ratio hardly affects the horizontal bearing capacity of bucket ***,the moment bearing capacity improves with the increase of the contact ratio for small aspect ratios,but hardly varies with increasing contact ratio for aspect ratios larger than ***,the reduction coefficient method is proposed based on this analysis to calculate the bearing capacities of bucket foundations considering the influence of incomplete soil *** comparison results show that the proposed reduction coefficient method can be used to evaluate the influences of incomplete soil plug on the bearing capacities of bucket foundations.

关键词： bucket foundation incomplete soil plug uniaxial bearing capacity contact ratio soil plug ratio

Low-Rank Optimal Transport for Robust Domain Adaptation

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IEEE/CAA Journal of Automatica Sinica 2024年第7期11卷 1667-1680页

作者： Bingrong xu Jianhua Yin Cheng lian Yixin Su Zhigang Zeng IEEE the School of Automation Wuhan University of TechnologyWuhan 430070China Intelligent Transportation Systems Research Center Wuhan University of TechnologyWuhan 430063 Chongqing Research Institute Wuhan University of TechnologyChongqingChina the School of Artificial Intelligence and Automation Huazhong University of Science and TechnologyWuhan 430074 the Key Laboratory of Image Processing and Intelligent Control of Education Ministry of China Wuhan 430074China

When encountering the distribution shift between the source(training) and target(test) domains, domain adaptation attempts to adjust the classifiers to be capable of dealing with different domains. Previous domain adaptation research has achieved a lot of success both in theory and practice under the assumption that all the examples in the source domain are welllabeled and of high quality. However, the methods consistently lose robustness in noisy settings where data from the source domain have corrupted labels or features which is common in reality. Therefore, robust domain adaptation has been introduced to deal with such problems. In this paper, we attempt to solve two interrelated problems with robust domain adaptation:distribution shift across domains and sample noises of the source domain. To disentangle these challenges, an optimal transport approach with low-rank constraints is applied to guide the domain adaptation model training process to avoid noisy information influence. For the domain shift problem, the optimal transport mechanism can learn the joint data representations between the source and target domains using a measurement of discrepancy and preserve the discriminative information. The rank constraint on the transport matrix can help recover the corrupted subspace structures and eliminate the noise to some extent when dealing with corrupted source data. The solution to this relaxed and regularized optimal transport framework is a convex optimization problem that can be solved using the Augmented Lagrange Multiplier method, whose convergence can be mathematically proved. The effectiveness of the proposed method is evaluated through extensive experiments on both synthetic and real-world datasets.

关键词： Domain adaptation low-rank constraint noise corruption optimal transport

Persymmetric adaptive polarimetric detection of subspace range-spread targets in compound Gaussian sea clutter

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Journal of Systems Engineering and Electronics 2024年第1期35卷 31-42页

作者： xu Shuwen HAO Yifan WANG Zhuo xue Jian National Key Laboratory of Radar Signal Processing Xidian UniversityXi’an 710071China Xi’an Electronic Engineering Research Institute Xi’an 710100China Beijing Institute of Radio Measurement Beijing 100039China School of Communications and Information Engineering Xi’an University of Posts and TelecommunicationsXi’an 710121China

This paper focuses on the adaptive detection of range and Doppler dual-spread targets in non-homogeneous and nonGaussian sea *** sea clutter from two polarimetric channels is modeled as a compound-Gaussian model with different parameters,and the target is modeled as a subspace rangespread target *** persymmetric structure is used to model the clutter covariance matrix,in order to reduce the reliance on secondary data of the designed *** adaptive polarimetric persymmetric detectors are designed based on the generalized likelihood ratio test(GLRT),Rao test,and Wald *** the proposed detectors have constant falsealarm rate property with respect to the clutter texture,the speckle covariance *** results on simulated and measured data show that three adaptive detectors outperform the competitors in different clutter environments,and the proposed GLRT detector has the best detection performance under different parameters.

关键词： sea clutter adaptive polarimetric detection compound Gaussian model subspace range-spread target persymmetric structure

Vision-based docking system for an aromatic-hydrocarbon-inspired reconfigurable robot

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Science China(Technological Sciences) 2024年第6期67卷 1798-1816页

作者： XING FangYi xu Cheng LIU JinGuo xue ZhiHui State Key Laboratory of Robotics Shenyang Institute of AutomationChinese Academy of SciencesShenyang110016China School of Automation and Electrical Engineering Shenyang Ligong UniversityShenyang110158China Institutes for Robotics and Intelligent Manufacturing Chinese Academy of SciencesShenyang110169China University of Chinese Academy of Sciences Beijing100049China

Aromatic hydrocarbons generally refer to compounds containing benzene *** types of isomers can be formed by replacing hydrogen atoms on the benzene *** this paper,an aromatic-hydrocarbon-inspired modular robot(AHIMR)is *** robot can be reassembled into different configurations suitable for various task requirements.A vision-based docking system is designed for the *** system primarily consists of two stages:a remote guidance stage and a precise docking *** the remote guidance stage,an object module is identified using an illumination adaptive target recognition algorithm,and then the active module moves to the docking area through communication with *** the precise docking stage,the active module calculates the relative pose with the object module using a perspective-n-point method and dynamically adjusts its posture to *** this process,a Kalman filter is used to reduce target occlusion and jitter *** addition,the docking system feasibility is verified via several simulation *** module docking accuracy is controlled within 0.01 m,which meets the reconfiguration task requirements of the *** the AHIMR submodule docking experiment,the active module accurately moves to the expected position with a docking success rate of 95%.

关键词： modular robot reconfiguration aromatic hydrocarbon autonomous docking visual identification

Tailoring sulfur-doped and nitrogen-defective carbon nitride nanosheets for efficient photo-controlled radical polymerizations

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Science China Chemistry 2024年第7期67卷 2325-2334页

作者： xue Li Meng Kai xu Yuan Huang Tao Cai Key Laboratory of Biomedical Polymers of Ministry of Education College of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China Wuhan University Shenzhen Research Institute Shenzhen 518057China

Despite the challenges that remain,the synergistic adjustment of various microstructures and photochemical parameters of graphitic carbon nitride(g-C_(3)N_(4))in photocatalytic reactions holds promises for improving catalytic efficiency and reducing energy ***,sulfur-doped and nitrogen-defective g-C_(3)N_(4)(n-SC_(3)N_(x))nanosheets were designed and elaborately *** resultant n-SC_(3)N_(x)possessed a precisely defined 2D layer structure with extensive porosity and incremental specific surface *** photoinduced electron transfer-reversible addition-fragmentation chain transfer(PET-RAFT)polymerization of vinyl monomers with low dispersity,excellent temporal control and high chain-end fidelity was achieved under mild blue light irradiation in a nondegassed *** to their ultrathin nanostructures with nitrogen defects and sulfur dopants,n-SC_(3)N_(x)was capable of catalyzing RAFT polymerization in aqueous solutions at significantly accelerated rates,which were nearly 8 times faster compared to bulk g-C_(3)N_(4).The ease of separation and efficient reusability in subsequent polymerizations was enabled by the heterogeneous nature of n-SC_(3)N_(x).The appeal of this approach was illustrated by the fact that utilizing a reusable and metal-free photocatalyst in aqueous environments allowed for the synthesis of polymers with molecular weight up to 300 kg mol^(-1) and a dispersity of 1.32.

关键词： graphitic carbon nitride nitrogen defects sulfur dopants PET-RAFT polymerization recyclability

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Structural engineering of BaWO_(4)/CsPbX_(3)/CsPb_(2)X_(5)(X=Cl,Br,I)heterostructures towards ultrastable and tunable photoluminescence

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Nano Research 2024年第3期17卷 1636-1645页

作者： Peng Liu Yan xu Bohan Li Yuchi Zhang Hongzhou lian Jun Lin Department of Chemistry College of SciencesNortheastern UniversityShenyang 110819China State Key Laboratory of Rare Earth Resource Utilization Chang Chun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Construction of lead halide perovskite nanocrystals(LHP NCs)heterostructures is essential to obtain highly stable photoluminescence and expand their ***,a novel self-assembly strategy combining with a solvent-free thermal-assisted synthesis and a water-triggered reaction is developed to subsequently grow BaWO_(4)/CsPbX_(3)/CsPb_(2)X_(5)(X=Cl,Br,I)heterostructures at low nucleation temperature with high *** as-obtained ternary BaWO_(4)/CsPbX_(3)/CsPb_(2)X_(5)(X=Cl,Br,I)heterostructures exhibit remarkably enhanced panchromatic emission and ultrastable luminescence ascribing to the low-defect growth based on lattice *** white light-emitting diodes(WLEDs)have been constructed with a high correlated color temperature(CCT)of 7225 K and luminous efficiency of 74.4 lm·***^(3+)-doped BaWO_(4)/CsPbX_(3)/CsPb_(2)X_(5)(Ln^(3+)=Eu^(3+),Tb^(3+),Dy^(3+),Sm^(3+),Yb^(3+)/Er^(3+))nanocomposites are further designed with excitation-dependent photoluminescence and thermochromic properties,making them excellent candidates for high-level anti-counterfeiting and *** work offers a green and universal approach in assembling CsPbX_(3)(X=Cl,Br,I)on lattice-matched tungstate with adjustable panchromatic emission for versatile optical applications.

关键词： inorganic lead halide perovskites solvent-free synthesis panchromatic emission anti-counterfeiting and encryption application