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Four unprecedented V_(14)clusters as highly efficient heterogeneous catalyst for CO_(2)fixation with epoxides and oxidation of sulfides

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Science China Chemistry 2023年第1期66卷 107-116页

作者： Ji-Lei Wang Jia-Peng Cao Yin-Hua Zhu Qin Wang Ning-Fang Li Xin-Rong Fan Hua Mei Yan Xu State Key Laboratory of Materials-Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing210009China State Key Laboratory of coordination Chemistry Coordination Chemistry InstituteNanjing UniversityNanjing 210093China

Chemical fixation of carbon dioxide(CO_(2))is an energy-saving method for alleviating the greenhouse gas emissions,whereas it persists a challenge posed by the demand for efficient ***,four unprecedented examples of tetradecanuclear vanadium clusters,namely,[(C_(2)H_(8)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V_(14)-1),[(C_(3)H_(10)N_(2))_(6)(CH_(3)O)_(8)(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)](V14^(-2)),[(C_(6)H_(14)N_(2))6(CH_(3)O)8(CH_(3)OH)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(26)]·5H_(2)O(V14^(-3))and[(C_(4)H_(12)N_(2)O)_(4)(C_(4)H_(11)N_(2)O)_(2)(CH_(3)O)_(2)V_(10)^(Ⅳ)V_(4)ⅤO_(28)]·6H_(2)O(V_(14)-4),have been triumphantly designed and constructed under solvothermal *** them,compounds V_(14)-1–4 are the first cases of tetradecanuclear vanadium clusters without the introduction of inorganic acid radical *** main units[V_(10)^(Ⅳ)V_(4)ⅤO_(26)]8+and[V10ⅣV4ⅤO28]4+represent brand-new configurations of tetradecanuclear vanadium *** the fact that the presence of V^(Ⅳ)/V^(Ⅴ)can potentially facilitate electron transfer and consequently expedite catalytic reactions,we explored the catalytic activities of these ***,V_(14)-1 was further used as a heterogeneous catalyst in the CO_(2)fixation into cyclic carbonates under milder conditions(60℃,0.5 MPa)and exhibited higher catalytic ***,the experimental results indicated that V_(14)-1 could efficiently catalyze the sulfoxidation,which could fully convert most sulfides within 40 min at room ***,as a stable heterogeneous catalyst employed in CO_(2)fixation with epoxides and oxidation of sulfides,V_(14)-1 could be consecutively used multiple cycles without losing its catalytic activity.

关键词： V_(14)clusters heterogeneous catalyst CO_(2)fixation oxidation of sulfides

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Two novel interpenetrated zinc(Ⅱ) and cadmium(Ⅱ) coordination polymers based on 4-imidazole-benzoate:Syntheses,crystal structures and properties

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Science China Chemistry 2009年第4期52卷 459-464页

作者： BAI ZhengShuai,CHEN ShuiSheng,ZHANG ZhengHua,CHEN ManSheng,LIU GuangXiang & SUN WeiYin State Key Laboratory of coordination Chemistry,Institute of coordination Chemistry,School of Chemistry and Chemical Engineering,Nanjing University,Nanjing 210093,China State Key Laboratory of coordination Chemistry Institute of Coordination Chemistry School of Chemistry and Chemical Engineering Nanjing University Nanjing China

Two novel interpenetrated coordination polymers,[Zn(IBA)2]n (1) and {[Cd(IBA)2(H2O)].4H2O}n (2),have been synthesized by using 4-imidazole-benzoic acid (HIBA) as ligand under hydrothermal con-ditions. Complex 1 crystallizes in a chiral space group and has a two-fold interpenetrated 2D network structure with (4,4) topology,while complex 2 is a 3D porous dia network with four nets interpene-trating each other. The SHG activity of 1 and the photoluminescent property of 2 have been investi-gated.

关键词： coordination polymer interpenetration crystal structure photoluminescence property

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Largest 3d-4f 196-nuclear Gd_(158)Co_(38)clusters with excellent magnetic cooling

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Science China Chemistry 2022年第8期65卷 1577-1583页

作者： Ning-Fang Li Xi-Ming Luo Jia Wang Ji-Lei Wang Hua Mei You Song Yan Xu College of Chemical Engineering State Key Laboratory of Materials-Oriented Chemical EngineeringNanjing Tech UniversityNanjing 210009China coordination Chemistry Institute State Key Laboratory of Coordination ChemistryNanjing UniversityNanjing 210093China

It is a meaningful and challenging work for structural and synthetic chemists to isolate nano-sized high-nuclearity *** this work,two largest hetero-metallic nano-clusters Gd_(158)Co_(38) were obtained via the“multi-anions-template”*** from the reported giant hollow-nano-clusters,the Ln_(158) core in Gd_(158)Co_(38)(the protein-sized nano-clusters,ca.4.3 nm×3.6 nm×3.5 nm)has the highest Ln nuclear number,which is integrated by twelve halide ions(with the form of icosahedron)as key templates,while Co ions(as 3d metals)are located in its *** emergence indicates a novel structure form of non-open Ln-containing high-nuclearity clusters,and affords a consummate pattern to analyse and assemble the complex *** addition,Gd_(158)Co_(38)@Cl_(12)breaks the record magnetic entropy change of 3d-4f clusters with−∆S_(m)^(max)=46.95 J kg^(−1)K^(−1)at 7.0 T,2.0 K.

关键词： multi-anions template high-nuclearity 3d-4f cluster magnetic refrigeration

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NMR studies of the effects of axial ligand substitution by imidazole on the conformation of cytochrome c

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Science China Chemistry 1995年第6期38卷 649-657页

作者：邵伟平姚亦明唐文霞 State Key Laboratory of coordination Chemistry Nanjing University Nanjing 210093 China

A series of 1D and 2D 1H NMR studies are presented, which aim at assigning the hyperfine shifted resonances of the heme and the spin systems of more than 20 amino acid side chains, and characterizing the heme and ligand environment of the low spin imidazole complex of cytochrome c. Some details of the structure in the heme pocket of the cytochrome c-imidazole complex are shownqualitatively to have changed relatively to the native oxidized protein. The orientation of the coordinated imidazole is also determined based on the interpretation of a number of NOEs.

关键词： imidazole complex of cytochrome c NMR axial ligand conformation.

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Conversion of CO2 to ethanol by using a metal-organic framework catalyst

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Science China Chemistry 2019年第10期62卷 1263-1264页

作者： Jing-Lin Zuo State Key Laboratory of coordination Chemistry School of Chemistry and Chemical EngineeringNanjing University

With the development of CO2 capture technology, CO2 can become an attractive C1 resource for synthesizing commodity chemicals. For example, direct conversion of CO2 to ethanol is of interest, but this process is also quite challenging, because it requires both the formation of one C–C bond and the retention of one C–O bond [1]. A combination of dual active sites, one for methanol formation and one for C–C coupling has been widely investigated for such a conversion, but an unbalanced rate in the two steps frequently leads to the formation of either methanol or long-chain hydrocarbons [2].

关键词： methanol ethanol catalyst

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A Novel 6-Connected Self-interpenetrated Zn(Ⅱ) coordination Polymer Based on 1,4-Bis(2-methylimidazole-3-ium-1-yl)biphenyl and Dicarboxylate Ligand: Synthesis, Crystal Structure and Luminescent Property

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Chinese Journal of Structural Chemistry 2015年第10期34卷 1579-1584页

作者：郭锋 Key Laboratory of coordination Chemistry and Functional Materials in Universities of Shandong Dezhou University

A novel coordination polymer {[Zn2（pda）2（bmp）1.5]·2H2O}n（1, H2 pda = 1,4-phenyl enediacetic acid and bmp = 1,4-bis（2-methy limidazol-3-ium-1-yl）biphenyl） was synthesized under hydrothermal conditions and characterized by single-crystal X-ray diffraction analyses and further characterized by elemental analyses, IR spectroscopy and powder X-ray diffraction（PXRD）. Complex {[Zn2（pda）2（bmp）1.5]·2H2O}n（1） is of triclinic system, space group P1 with a = 10.132（5）, b = 11.854（5）, c = 18.784（5） A, α = 80.256（5）, β = 75.163（5）, γ = 75.620（5）°, Z = 2, V = 2099.0（15） A3, Mr = 908.54, Dc = 1.437 g/cm^3, F（000） = 938 and μ = 1.206 mm-1. The final R = 0.0541 and wR = 0.1397 for 8017 observed reflections with I 2σ（I）. Complex 1 displays a three-dimensional（3D） self-interpenetrated 6-connected topological net with point symbol（48.67）. Furthermore, the luminescent property of complex 1 was investigated in the solid state at room temperature.

关键词： crystal structure Zn(Ⅱ) coordination polymer luminescence

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Thermo-induced structural transformation with synergistic optical and magnetic changes in ytterbium and erbium complexes

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Chinese Chemical Letters 2021年第4期32卷 1519-1522页

作者： Qian Zou Jing-Cui Liu Xin-Da Huang Song-Song Bao Li-Min Zheng State Key Laboratory of coordination Chemistry Coordination Chemistry InstituteSchool of Chemistry and Chemical EngineeringCollaborative Innovation Center of Advanced MicrostructuresNanjing UniversityNanjing 210023China

Dinuclear ytterbium and erbium based bifunction complexes Ln_(2) L_(2)(depma_(2))Cl_(2)(1-Ln,Ln=Yb and Er,H_(2) L=N~1,N~3-bis(salicylideneimino)diethylenetriamine,depma_(2)=dimerized 9-diethyl-phosphonomethylanthracene)are *** undergo thermo-induced consecutive phase transitions,first the dissociation of depma_(2) ligand forming LnL(depma)Cl(2-Ln)and then the release of chloroethane forming LnL(epma)(3-Ln,epma=9-ethylphosphonomethylanthrancene).The structural transformations are accompanied with synergetic switch of the luminescence in visible and NIR regions and also magnetic dynamics.

关键词： Phase transition Lanthanide Anthracene Single molecule magnet Luminescence

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Structure and Thermal Properties of Transition Metal Imidazole Chloride

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Chinese Journal of Structural Chemistry 2004年第9期23卷 979-984页

作者：建方方仝玉萍肖海连汪庆祥焦奎 New Materials & Function coordination Chemistry Laboratory Qingdao University of Science and TechnologyQingdao 266042China

The X-ray single-crystal structure analyses have been determined for two metal imidazole chlorides: [Fe(Im)6]Cl24H2O 1 and [CuCl(Im)4]Cl 2 (Im = imidazole). The red crystal of compound 1 is of triclinic, space group Pi with Mr = 607.31 (C18H32Cl2FeN12O4), a = 8.797(2), b = 9.068(2), c = 10.581(2) ? a = 75.35(3), ?= 83.20(3), ? = 61.85(3)o, V = 720.0(2) 3, Z = 1, Dc = 1.401 g/cm3, F(000) = 316, = 0.755 mm-1, R = 0.0353 and wR = 0.1227. The blue crystal of compound 2 belongs to monoclinic, space group P21/c with Mr = 406.77 (C12H16Cl2CuN8), a = 13.909(3), b = 8.8933(18), c = 15.086(7) ? ?= 118.32(2), V = 1642.7(9) 3, Z = 4, Dc = 1.645 g/cm3, F(000) = 828, = 1.666 mm-1, R = 0.0609 and wR = 0.1726. In solid state, both 1 and 2 form three-dimensional hydrogen bond networks to stabilize the structures which were also characterized by TG and elemental analyses. The thermal gravity (TG) data indicate that the residues are Fe and Cu for 1 and 2, respectively.

关键词： imidazole ligand crystal structure chloride compound thermal property

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Understanding coupled coordination relationships between social and ecological functions of urban green spaces

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Geo-Spatial Information Science 2023年第3期26卷 431-445页

作者： Dianfeng Liu Huiying Li Mingli Qiu Yaolin Liu School of Resource and Environmental Sciences Wuhan UniversityWuhanChina Key Laboratory of Digital Cartography and Land Information Engineering Ministry of Natural ResourcesWuhan UniversityWuhanChina

Urban Green Spaces(UGSs)can provide social and ecological benefits,and the coordination of these two functions will largely advance human-nature harmony in *** such,we proposed a comprehensive framework to evaluate UGSs multifunctionality,*** coupling coordination relationship of ecological connectivity and spatial accessibility of *** City in Central China was taken as a case study,and multiple ecosystem service values of green space patches and the disordered use of UGSs multifunctionality were *** results demonstrated low-level coupling coordination of UGSs multifunctionality in *** than 70%of UGSs were imbalanced,27.91%of which featured small sizes,low connectivity and *** suggest that planners should optimize UGSs arrangement to improve species reachability,especially for species with dispersal distance less than 4 km,and to create 15-minute community life circles for residents at the same *** findings are expected to support the promotion of UGSs multifunctionality and the balance of urban development and habitat conservation.

关键词： Urban green spaces coupling coordination analysis spatial accessibility ecological connectivity Wuhan city

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Green synthesis of metal/C and metal oxide/C films by using natural membrane as support

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Frontiers of Materials Science 2014年第2期8卷 150-156页

作者： Cheng-Zhen WEI Hai-Feng MA Feng GAO Department of Materials Science and Engineering Nanjing University Nanjing 210093 China State Key Laboratory of coordination Chemistry Coordination Chemistry Institute Nanjing National Laboratory of Microstructures Nanjing University Nanjing 210093 China

A protocol aiming at making use of the huge amount of naturally existing wastes such as defoliation, pericarp and egg shell for nanostructured composite materials was proposed. In this study, a green synthetic route using naturally existing membrane as support was developed for the synthesis of nanostructured and porous metalor metal oxide-carbon composite films. Different metallic ions （Co2＋, Ni2＋, Fe3＋, Mn2＋ or Cu2＋） can be easily adsorbed onto egg membranes and the followed calcination process results in the formation of Co/C, Ni/C, Fe304/C, MnO/C or CulCu2OICuOIC composite films. The electrochemical studies demonstrate that such composite films would have potential applications in energy fields. This method would provide a general green concept for chemical synthesis and be beneficial to the global sustainable future.

关键词： green synthesis metal metal oxide composite electrochemistry

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