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Chinese Chemical Letters 2024年第4期35卷 176-180页

作者： Chao-Long Chen Rong Chen La-Sheng Long Lan-Sun Zheng xiang-jian kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China

Light-driven nitrogen fixation to produce ammonia is a green and economical technology of nitrogen reduction but is still quite challenging, especially in an air atmosphere without any sacrificial ***, we demonstrate efficient photocatalytic nitrogen fixation using water and air directly by loading lanthanide–transition metal(4f–3d) cluster NdCo_(3) on two-dimensional P-doped graphitic carbon nitrides(PCN) material surface. Benefiting from the increase in the number of nitrogen vacancies(NVs) and highly matched band gap structure and excellent hole trapping ability of clusters, the NdCo_(3)/PCN photocatalyst exhibits efficient nitrogen reduction activity with 371(in air) and 825 μmol h^(-1)g^(-1)(in pure nitrogen)without any sacrificial reagents. The introduction of potassium sulfate inhibits hydrogen production and promotes nitrogen reduction activation. This work suggests that anchoring precisely structured clusters on 2D materials may enhance photocatalytic nitrogen reduction under normal temperature and pressure.

关键词： Photocatalytic Nitrogen fixation 4f-3d Cluster Air atmosphere

Molecular solid solution of lanthanide-titanium-oxo clusters with enhanced photocatalytic hydrogen evolution

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Science China Chemistry 2024年第2期67卷 529-535页

作者： Rong Chen Chao-Long Chen Hui Zhang Zi-Han Wang Fu-Li Sun Ming-Hao Du Gui-Lin Zhuang Cheng Wang La-Sheng Long Lan-Sun Zheng xiang-jian kong Collaborative Innovation Centre of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China College of Chemical Engineering Zhejiang University of TechnologyHangzhou310032China

Molecular solid solutions of metal clusters containing different metal centers with well-defined structures can accurately regulate the HOMO-LUMO gap,but are rarely ***,a series of colorless lanthanide-titanium-oxo clusters Ln_(2)Ti_4(μ_(2)-O)_(2)(μ_(3)-O)_4(Piv)_(10)(THF)_(2)(Ln_(2)Ti_4,Ln = Eu,Gd,Tb,and Ce,HPiv = pivalic acid) were synthesized by the reaction of pivalic acid with Ln(Ac)_(3) and titanium *** light yellow crystal of cluster solid solutions Eu_(2)Ti_(4-x)Cd_(x),containing a mixture of Eu_(2)Ti_4 and Eu_(2)Ti_(3)Cd,was obtained by in situ doping Cd^(2+) and S^(2–).Eu_(2)Ti_(3.92)Cd_(0.08) displays efficient photocatalytic hydrogen evolution activity without a co-catalyst,which is up to 2.6 times that of Eu_(2)Ti_*** time-resolved transient absorption spectroscopy and spin-polarized density functional calculations showed that the enhanced photocatalytic performance of Eu_(2)Ti_(4-x)Cd_(x) can be attributed to the narrower HOMO-LUMO gap and lower LUMO position than that of Eu_(2)Ti_*** studyprovides an in situ doping method to realize the simple preparation of cluster solid solution.

关键词： molecular solid solution lanthanide-titanium-oxo clusters photocatalytic hydrogen evolution

Synthesis,structures and photoluminescence of uranyl polyoxometalate clusters based on trilacunary[TeW_(9)O_(33)]^(8-)

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钨科技(英文) 2023年第2期5卷 254-260页

作者： Hai-Ying Wang Xiu-Ying Zheng La-Sheng Long Lan-Sun Zheng xiang-jian kong State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of Chemistry College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China Henan Key Laboratory of Polyoxometalate Chemistry College of Chemistry and Chemical EngineeringHenan UniversityKaifeng 475004China Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China

Synthesis of uranyl polyoxometalate clusters attract more attention but remain great ***,two uranyl polyoxometalate inorganic clusters of{Na_(6)(NH_(4))_(19)[(TeW_(9)O_(33))_(4)[TeO_(2)(OH)](UO_(2))4(H_(2)O)_(2)]·50H_(2)O}n(1,Te-U_(4))and(NH_(4))18{Na@[(TeW_(9)O_(32)OH)(TeW_(9)O_(33))_(2)[TeO(OH)][W_(3)O_(12)(μ_(3)-OH)](UO_(2))_(6)(μ_(2)-OH)_(2)H_(2)O]}·75H_(2)O(2,Te-U6)were prepared using trilacunary[α-B-TeW_(9)O_(33)]8-as inorganic *** analysis showed that compound 1 is a one-dimensional chain structure formed by tetrameric aggregates of[(α-B-TeW_(9)O_(33))_(4)(TeO_(2)(OH))(UO_(2))_(4)(H_(2)O)2]25-as nodes and Na+ions as *** anionic tetrameric aggregates in 1 is made of two sandwich-type dimers of[(TeW_(9)O_(33))_(2)(UO_(2))_(2)H_(2)O]12-bridged by a[TeO_(2)(OH)]-*** 2 is a triangular trimeric architecture templated by Na+*** solid-state luminescence emission spectra of compounds 1 and 2 show the characteristic peaks of uranyl *** 1 with one-dimensional chain structure exhibited a higher photoluminescence quantum yields(PLQY)than that of 2,due to the more rigidity of 1 reducing the nonradiative transitions.

关键词： Uranyl Polyoxometalate Cluster Lacunary Luminescence

Lanthanide-oxo clusters for efficient catalytic reduction of carboxamides

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Science China Chemistry 2023年第2期66卷 443-448页

作者： Zhen-Zhang Weng Chao-Long Chen Long-Wu Ye La-Sheng Long Lan-Sun Zheng xiang-jian kong Collaborative Innovation Center of Chemistry for Energy Materials State Key Laboratory of Physical Chemistry of Solid Surfaces and Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

The reduction of carboxamides into high value-added amines is a very interesting but great challenging *** we demonstrate that polynuclear lanthanide-oxo clusters Ln16(Ln=Eu and Gd)can be used as efficient catalyst to reduce primary and secondary carboxamides to amines with excellent yield of 71%-98%and broad substrates *** methodology can extend to the gram-scale synthesis of phenethylamine drug with 93%*** on the isolation and characterization of catalytic intermediates,a catalytic mechanism involving multipath reaction is *** work provides efficient lanthanide cluster catalysts for the reduction of carboxamides to amines.

关键词： lanthanide clusters amide reduction metal-hydride BH3 catalytic mechanism

Synthesis,Structure and Magnetic Behavior of a Novel Series of Trinuclear Windwheel Complexes

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Chinese Journal of Chemistry 2023年第24期41卷 3662-3668页

作者： Rong Luo Chen-Ze Xie Ming-Guang Chen Hai-Yan Shi xiang-jian kong Yu-Hua Fan Feng Shao Key Laboratory of Marine Chemistry Theory and Technology Ministry of EducationCollege of Chemistry and Chemical EngineeringOcean University of ChinaQingdaoShandong266100 China Baotou Research Institute of Rare Earths BaotouInner Mongolia014040 China State Key Laboratory of Physical Chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamenFujian361005 China

A new family of trinuclear windwheel complexes with molecular formula [M^(II)_(3)(tpa)_(3)(μ-ttc)](ClO_(4))_(3)·n(sol) (ttc = 1,3,5-triazine-2,4,6-trithiol;tpa = tris(2-pyridylmethyl)amine;M = Mn,n = 2,sol = CH_(3)CN,1;M = Co,n = 1,sol = CH_(3)CN,2;M = Ni,n = 0,3) were synthesized and ***-crystal X-ray diffraction revealed that three metal centers in 1—3 are connected by ttc bridge,forming a regular triangular MII3 *** metal center is bonded by chelating S,N atoms from ttc and by N atoms from *** studies showed that 1—3 displayed antiferromagnetic behavior and further gave the easy-axis anisotropy (D = −0.77 cm^(−1) for 1 and −8.13 cm^(−1) for 2) and easy-plane anisotropy (D = 5.08 cm^(−1) for 3).Moreover,2 exhibited field-induced slow magnetic relaxation behavior and their effective energy barriers were roughly evaluated Ueff = 6.9 K.

关键词： Cluster compounds Crystal growth Magnetic properties Slow magnetic relaxation Magnetic anisotropy

Electrolyte effect on electrochemical behaviors of manganese fluoride material for aqueous asymmetric and symmetric supercapacitors

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Rare Metals 2024年第3期43卷 1048-1061页

作者： Zheng-Hua He jian-Fei Gao Ling-Bin kong State Key Laboratory of Advanced Processing and Recycling of Non-Ferrous Metals Lanzhou University of TechnologyLanzhou730050China School of Materials Science and Engineering Lanzhou University of TechnologyLanzhou730050China

Exploring wide voltage window materials is not only an available measure to enhance the energy density of hybrid supercapacitor(HSCs),but also avoids the dynamic mismatch caused by different energy storage mechanisms of two electrodes in assembled symmetrical ***,there are few reports about the wide potential window materials except Bi_(2)O_(3)and VO_(2).Therefore,the MnF_(2)synthesized by solvothermal reaction was served as the electrode for *** MnF_(2)exhibited electrochemical activity in alkaline solution in three-electrode system,especially with a wide potential window from-0.8 to+0.5 V in 2 mol·L^(-1)***,the assembled MnF_(2)//MnF_(2)symmetrical HSC had a potential window of 1.5 V,and it exhibited outstanding long-cycle ***,when MnF_(2)was taken as the negative and positive respectively,the potential windows of asymmetric devices CoMoO_(4)//MnF_(2)and MnF_(2)//Activated Carbon(AC)could reach 1.3 and 1.45 V,respectively,showing excellent cycle *** work shows that MnF_(2)material has great research value in HSC,and provides a new research direction for developing high-performance devices.

关键词： Manganese fluoride Potential window Hybrid supercapacitors Electrochemical performance

Adversarial data splitting for domain generalization

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Science China(Information Sciences) 2024年第5期67卷 28-42页

作者： xiang GU jian SUN Zongben XU School of Mathematics and Statistics Xi'an Jiaotong University

Domain generalization aims to learn a model that is generalizable to an unseen target domain,which is a fundamental and challenging task in machine learning for out-of-distribution generalization. This paper proposes a novel domain generalization approach that enforces the learned model to be able to generalize well over the train/val subset splitting of the training dataset. This idea is modeled herein as an adversarial data splitting framework, formulated as a min-max optimization problem inspired by the metalearning approach. The min-max optimization problem is solved by iteratively splitting the training dataset into the training and val subsets to maximize the domain shift measured by the objective function and updating the model parameters to enable the model to generalize well from the training subset to the val subset by minimizing the objective function. This adversarial training approach does not assume the known domain labels of the training data; instead, it automatically investigates the “hard” splitting of the train/val subsets to learn the generalizable model. Extensive experimental results using three benchmark datasets demonstrate the superiority of this approach. In addition, we derive a generalization error bound for the theoretical understanding of our proposed approach.

关键词： domain generalization adversarial learning data splitting meta-learning out of distribution

Temperature prediction model in multiphase flow considering phase transition in the drilling operations

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Petroleum Science 2024年第3期21卷 1969-1979页

作者： Yang Zhang Yong-An Li xiang-Wei kong Hao Liu Teng-Fei Sun College of Mechanical and Electrical Engineering Beijing University of Chemical TechnologyBeijing 100027China School of Petroleum Engineering Yangtze UniversityWuhan430000HubeiChina

The study considers gas compression properties,gas slippage,back pressure(BP),phase transition(PT),well depth,and differences in gas-liquid physical properties.A new temperature model for multiphase flow is proposed by considering phase transition in the drilling *** mathematical model of multiphase flow is solved using the finite difference method with annulus mesh division for grid nodes,and a module for multiphase flow calculation and analysis is *** results indicate that the temperature varies along the annulus with the variation of gas influx at the bottom of the *** the process of controlled pressure drilling,as gas slips along the annulus to the wellhead,its volume continuously expands,leading to an increase in the gas content within the annulus,and consequently,an increase in the pressure drop caused by gas *** temperature increases with the increase in BP and decreases in gas influx rate and wellbore *** gas influx,the thermal conductivity coefficient for the gas-drilling mud two phases is significantly weakened,resulting in a considerable change in temperature along the *** the context of MPD,the method of slightly changing the temperature along the annulus by controlling the back pressure is feasible.

关键词： Managed pressure drilling Phase transition Temperature Gas-drilling mud two phase

Classification of spin Hall effect in two-dimensional systems

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Frontiers of physics 2024年第3期19卷 103-114页

作者： Longjun xiang Fuming Xu Luyang Wang jian Wang College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen 518060China Quantum Science Center of Guangdong-Hongkong-Macao Greater Bay Area(Guangdong) Shenzhen 518045China Department of Physics The University of Hong KongPokfulam RoadHong KongChina

Physical properties such as the conductivity are usually classified according to the symmetry of the underlying system using Neumann’s principle, which gives an upper bound for the number of independent components of the corresponding property tensor. However, for a given Hamiltonian, this global approach usually can not give a definite answer on whether a physical effect such as spin Hall effect (SHE) exists or not. It is found that the parity and types of spin-orbit interactions (SOIs) are good indicators that can further reduce the number of independent components of the spin Hall conductivity for a specific system. In terms of the parity as well as various Rashba-like and Dresselhaus-like SOIs, we propose a local approach to classify SHE in two-dimensional (2D) two-band models, where sufficient conditions for identifying the existence or absence of SHE in all 2D magnetic point groups are presented.

关键词： spin Hall effect symmetry two-dimensional system

NbB_(2)Modified Al-Cu Alloys Fabricated by Freeze-Ablation Casting under High Cooling Rate Solidification

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Acta Metallurgica Sinica(English Letters) 2024年第5期37卷 921-938页

作者： xiang kong Yu Wang Hong Xu Haotian Fan Yuewu Zheng Beibei Xie School of Materials Science and Engineering North University of ChinaTaiyuan 030051China

At present,improving the properties of aluminum alloys is generally achieved by increasing the cooling rate of the melt and adding micro-nano *** the cooling rate of the melt to improve the refining effect of grain refiner is still a difficult problem in the aluminum alloy casting *** innovative and environmentally friendly casting process,known as freeze ablation,was introduced during the preparation of an Al–NbB_(2) intermediate *** process significantly enhanced the cooling rate of the *** results indicated that the Al–NbB_(2) intermediate alloy produced under high cooling rates had a noticeable refining effect on Al–Cu alloys,with smaller NbB2 particles demonstrating superior refining *** average grain size of the refined Al–Cu alloy decreased from 154 to 69μm,the tensile strength increased by 12%,the fluidity increased by 18.4%,and the hot tearing index decreased from 144 to *** matching degree between NbB_(2) andα-Al was calculated using high-resolution transmission electron microscopy and the edge-to-edge *** was found that the atomic interplanar spacing and the interatomic spacing mismatch between NbB_(2)’splane and Al were both less than 10%,which further proved that NbB2 could serve as an effective nucleation site forα-Al grains to achieve grain refinement.

关键词： Grain refinement Freeze ablation Particle size control Mechanical properties Process properties