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Stable copper boron–imidazolate cage as Cu-riched enzyme for highly efficient electrocatalytic CO2 reduction to ethylene

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Science China Chemistry 2025年

作者： Jun-Qiang Chen Qiao-Hong li qin-long Hong Ping Shao Hai-Xia Zhang Jian Zhang State Key laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences

Single-atom catalyst has garnered widespread attention to mimic mature enzymes due to its well-defined atomic structure and coordination environments. However, since the carbon–carbon（C–C） coupling reactions require synergistic catalysis of multiple sites, single-atom catalysts suffer from insufficient active sites and unclear reaction mechanisms. Controlling the reaction intermediates in a precisely targeted pocket through careful metal–organic cage design is therefore crucial. Here, we prepare a tetrahedral [Cu6l4]-type boron–imidazolate cage integrating highly active Cu sites and optimized cavity, which exhibits enzyme like specific catalytic performance in electrochemical CO2reduction reaction（CO2RR） to enhance the selectivity of *** analyses and computational calculations suggest that the single Cu site together with neighboring boron–imidazolate ligands provides suitably synergistic effects that enable the energetically favorable formation of an *COCHO intermediate, a key step determining selectivity. As a result, the [Cu6l4]-type cage of BIC-145 achieves a Faradaic efficiency of 28% for C2H4maintaining an average current density of -3.54 mA cm-2over a 5-hour electrolysis period. This work represents the first example for studying single-metal site catalysts with ultra-low coordination numbers through the rational design of metal–organic cages.

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呋虫胺和唑虫酰胺在茶叶加工过程中的残留特征及膳食风险评估

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食品科学 2025年第1期46卷 192-199页

作者：李春勇吕莹金静王霞秦曙山西农业大学山西功能农产品检验检测中心山西太原030031

为明确呋虫胺和唑虫酰胺微乳剂在茶叶种植、烘干、浸泡过程中的残留特征,在山东、浙江等10地开展规范农药登记残留田间试验,并进行加工因子校正膳食风险评估模型比较研究。样品经体积分数5%甲酸-乙腈提取、盐析分层、分散固相萃取净化后... 详细信息

为明确呋虫胺和唑虫酰胺微乳剂在茶叶种植、烘干、浸泡过程中的残留特征,在山东、浙江等10地开展规范农药登记残留田间试验,并进行加工因子校正膳食风险评估模型比较研究。样品经体积分数5%甲酸-乙腈提取、盐析分层、分散固相萃取净化后,经超高效液相色谱-串联质谱法检测,外标法定量。结果表明:在0.005~0.500μg/ml范围内,呋虫胺及其代谢物、唑虫酰胺质量浓度与其响应峰面积呈良好线性关系(R^(2)>0.99),在0.05、1.00、20.00、50.00 mg/kg(茶鲜叶、茶干叶),0.05、0.10、5.00 mg/kg(茶汤)添加水平下,呋虫胺及其代谢物1-甲基-3-[(3-四氢呋喃)甲基]脲、1-甲基-3-[(3-四氢呋喃)甲基]二氢胍盐的平均加标回收率为74%~103%,相对标准偏差为1%~9%;唑虫酰胺的平均加标回收率为75%~95%,相对标准偏差为1%~6%,方法定量限均为0.05 mg/kg;20%呋虫胺·唑虫酰胺微乳剂按推荐剂量施药后,呋虫胺(含代谢物)在茶鲜叶中的规范残留试验中值(supervised trials median residue,STMR)经烘干因子校正后与茶干叶中STMR相应的国家估算每日摄入量(national estimated daily intake,NEDI)均为4.08 mg,占每日允许摄入量(allowable daily intake,ADI)的32.4%;唑虫酰胺在茶鲜叶中的STMR经烘干因子校正后的NEDI为0.17581 mg,占ADI的46.5%,茶干叶中STMR对应的NEDI为0.18925 mg,占ADI的50.1%,呋虫胺和唑虫酰胺在不同评估模型下获得的长期膳食暴露风险均低于100%;呋虫胺(含代谢物)经加工因子校正后的国际短期膳食摄入量(international estimation of short-term dietary intake,IESTI)与校正前处于同一风险水平,低于急性参考剂量(acute reference dose,ARfD)(1 mg/kg);唑虫酰胺的IESTI为3.46×10^(-4) mg/kg(采收间隔7 d),低于ARf D(0.01 mg/kg),本研究方法在茶汤中未检测到唑虫酰胺残留,故未得到浸泡因子及相应的IESTI。综上,按推荐剂量在茶树上使用20%呋虫胺·唑虫酰胺微乳剂是安全的,最终残留量对应的长期及急性膳食摄入风险均在可接受范围,利用加工因子校正评估模型更切合实际风险水平。

关键词：呋虫胺唑虫酰胺茶叶加工因子残留特征风险评估

Stepwise assembly to construct stable copper(I) cluster-based circularly polarized luminescent MOFs

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Science China Chemistry 2025年

作者： Jing-Wen Xie Meng-Ting Wang Yan Jin Si li Jian-Hua qin Shuang-Quan Zang Tomas C.W.Mak College of Chemistry Henan Key Laboratory of Crystalline Molecular Functional Materials Zhengzhou University College of Chemistry and Chemical Engineering Luoyang Normal University Department of Chemistry The Chinese University of Hong Kong

Circularly polarized luminescence （CPl） materials have been extensively studied in recent years owing to their widespread applications in 3D display,optical storage,optical.anti-counterfeiting,and biological imaging,***（I） clusters have emerged as a promising candidate for CPl materials,driven by their cost-effectiveness,superior luminescent properties,precise structure,and low ***,the poor environmental stability of copper（I） clusters renders their synthesis and preservation challenging,thereby significantly impeding their ***,we have designed and synthesised a chiral double-coordinated ligand in order to construct copper（I） cluster nodes that can be further *** anticipated,by utilizing stepwise assembly strategy,a Cu4cluster node co-modified by chiral alkynyl ligands and triphenylphosphine was further assembled with Cd2+ions to obtain 2D layers structure,l/*** l/D-Cu4-Cd exhibits excellent stability and optical properties,including bright yellow emission,solvent-responsive luminescence,and CPl activity with a maximum glumup to 2.0×10-3,which shows potential applications in the WlED and *** interestingly,the material also exhibits deflection ability towards different wavelengths of linearly polarized light,showing certain potential in the preparation of circular polarizer.

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Performance measure for image fusion considering region information

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2007年第4期8卷 559-562页

作者： lIU Gang lü Xue-qin School of Power and Automation Engineering Shanghai University of Electric Power Shanghai 200093 China

An objective performance measure for image fusion considering region information is proposed. The measure not only reflects how much the pixel level information that fused image takes from the source image, but also considers the region information between source images and fused image. The measure is meaningful.and explicit. Several simulations were conducted to show that it accords well with the subjective evaluations.

关键词： Image fusion Information fusion Image processing

Assembly and Electrochemical Study of Transition Metal Substituted Polyoxometalates SiW_(11)NiO_(39)^(6-) and SiW_(11)MnO_(39)^(6-) on 4-Aminothio-phenol Modified Glassy Carbon Electrode

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Chemical Research in Chinese Universities 2005年第4期21卷 401-405页

作者： lüGui-qin DUJin-yan HUChang-wen InstituteforChemicalPhysics DepartmentofChemistryBeijingInstituteofTechnologyBeijing100081P.R.China InstituteforChemicalPhysics DepartmentofChemistryBeijingInstituteofTechnologyBeijing100081P.R.China／／ChemistryDepartmentAnhuiNormalUniversityWuhu241000P.R.China

Via layer-by-layer assembly, the polyoxometalates of Keggin type, SiW_ 11O_ 39Ni(H_2O) 6-(SiNiW_ 11) and {SiW_ 11O_ 39Mn(H_2O) 6-}(SiMnW_ 11) were first immobilized on a 4-aminothiophenol(4-ATP) modified glassy carbon electrode surface. The electrochemical behavior of these polyoxometalates was investigated. They exhibited some special properties in the films, which are different from those in a homogeneous aqueous solution. Their reaction mechanism in a multilayer film is proposed. The electrocatalytic behavior of these multilayer film electrodes for the reduction of BrO-_3 and NO-_2 were comparatively studied.

关键词： Polyoxometalate layer-by-layer assembly Electrochemical behavior Electrocatalytic reduction BrO_3^- NO_2^-

Chitosan-supported Borohydride Reducing Agent

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Chinese Chemical letters 2001年第12期12卷 1051-1052页

作者： qin, CQ Xiao, l Du, YM Wuhan Univ Dept Environm Sci Wuhan 430072 Peoples R China

A new chitosan-supported borohydride reducing reagent (CBER) was prepared by treatment of KBH4 with the resin of chitosan derivative, which was first synthesized from: the reaction of cross-linked chitosan microsphere... 详细信息

关键词： polymer-support borohydride reducing agent chitosan resin

Dendrite growth characteristics within liquid Fe-Sb alloy

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Science China(Physics,Mechanics & Astronomy) 2009年第5期52卷 720-728页

作者： WANG Weili lüYongJun qin HaiYan WEI BingBo Department of Applied Physics Northwestern Polytechnical UniversityXi’an 710072China

Bulk samples and small droplets of liquid Fe-10%Sb alloys are undercooled up to 429 K (0.24Tl) and 568 K (0.32Tl), respectively, with glass fluxing and free fall techniques. The high undercooling does not change the phase constitution, and only the αFe solid solution is found in the rapidly solidified alloy. The experimental results show that when the undercooling is below 296 K, the growth velocity of αFe dendrite rises exponentially with the increase of undercooling and reaches a maximum value 1.38 m/s. Subsequently, the growth velocity begins to decrease if undercooling further increases. The αFe phase grows into coarse dendrites under small undercooling conditions, whereas it becomes vermicular dendrites in highly undercooled melts. The solute trapping is closely related to the dendrite growth velocity and cooling rate rather than undercooling. Although the solute trapping can be remarkably suppressed by the rapid dendrite growth, the segregationless solidification is not observed in the present experiments due to the large solidification temperature range.

关键词： liquid physics dendrite growth solute distribution segregationless solidification

High-Order Discontinuous Galerkin Method for Hovering Rotor Simulations Based on a Rotating Reference Frame

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Transactions of Nanjing University of Aeronautics and Astronautics 2019年第1期36卷 57-70页

作者： ZHANG Tao lü Hongqiang qin Wanglong CHEN Zhengwu Department of Aerodynamics Nanjing University of Aeronautics and Astronautics China Aerodynamics Research and Development Center

An implicit higher ? order discontinuous Galerkin(DG) spatial discretization for the compressible Euler equations in a rotating frame of reference is presented and applied to a rotor in hover using hexahedral grids. Instead of auxiliary methods like grid adaptation,higher ? order simulations(fourth ? and fifth ? order accuracy) are *** numerical experiments are carefully designed,conducted and analyzed. The results show generally excellent consistence with references and vigorously demonstrate the higher?order DG method's better performance in loading distribution computations and tip vortex capturing, with much fewer degrees of freedom(DoF). Detailed investigations on the outer boundary conditions for hovering rotors are presented as well. A simple but effective speed smooth procedure is developed specially for the DG method. Further results reveal that the rarely used pressure restriction for outlet speed has a considerable advantage over the extensively adopted vertical speed restriction.

关键词： high-order method(HOM) discontinuous Glaerkin method(DGM) Euler equation hovering rotor simulation tip vortex

Solvothermal Syntheses and Crystal Structures of Two New Nonmetal Borates:C_4H_(10)N_2·B_6O_8(OH)_2 and (NH_3CH_2CH_2NH_3)B_5O_8(OH)

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Chinese Journal of Structural Chemistry 2007年第3期26卷 257-262页

作者： lü Gui-qin YANG Xin lI Min SHI Heng-Zhen School of Science Beijing Institute of Technology Beijing 100081 China Institute of Applied Catalysis Yantai University Yantai 264005 China Department of Chemistry Zhoukou Normal University Zhoukou 46600 1 China

Two new borate compounds, C4H10N2·B6O8（OH）2 and （NH3CH2CH2NH3）B5O8 （OH）2, have been solvothermally synthesized and structurally characterized by single-crystal X-ray diffraction, IR, elemental.analysis and thermal.analysis. Compound 1 crystallizes in the monoclinic system, space group P21/c, with a = 8.3318（17）, b = 6.2118（12）, c = 12.479（3） A, β = 108.96（3）°, V = 610.8（2） A^3, Mr = 313.02, Z = 2, 13,.= 1.702 g/cm^,/J = 0.150 mm^-1, F（000） = 320, R = 0.0387 and wR = 0.0924. Its layered structure is linked by infinite covalently coordinated neutral sheets with 3,20-membered window system, which are built up from alternative B6O8（OH）2 subunits donated by two piperzazine nitrogen donors. 2 crystallizes in monoclinic, space group Co, with a = 6.7207（13）, b = 11.481 （2）, c = 12.564（3）A,β = 95.25（3）°, V = 965.4（3） A^3, Mr = 261.18, Z = 4, Dc = 1.797 g/cm^3,/t = 0.164 mm^-1, F（000） = 536, R = 0.0396 and wR = 0.0752. Its oxoborate structure is generated from the sheets of 3,9-membered boron rings bonded diamine molecules through electrostatic and H-bonding interactions to form a two-dimensional layered network.

关键词： solvothermal synthesis crystal structure borate