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Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics:A combined experimental and theoretical study

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Chinese Chemical Letters 2024年第8期35卷 514-519页

作者： Longlong Geng Huiling liu Wenfeng Zhou Yong-Zheng Zhang Hongliang Huang Da-Shuai Zhang Hui Hu Chao Lv Xiuling Zhang suijun liu Shandong Provincial Key Laboratory of Monocrystalline Silicon Semiconductor Materials and Technology College of Chemistry and Chemical EngineeringDezhou UniversityDezhou 253023China School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255000China State Key Laboratory of Separation Membranes and Membrane Processes School of Chemical Engineering and TechnologyTiangong UniversityTianjin 300387China School of Chemistry and Chemical Engineering Jiangxi Provincial Key Laboratory of Functional Molecular Materials ChemistryJiangxi University of Science and TechnologyGanzhou 341000China

Metal-organic frameworks(MOFs)functionalized with open metal sites(OMSs)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest ***,rational tailoring of the coordination environment of metal nodes dur-ing the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with ***,we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ)sites,namely[Cu(HCOO)(pzta)]_(n)(HL-1),{[Cu(PTA)0.5(pzta)(H_(2)O)]·2H_(2)O}_(n)(HL-2)and[Cu(NA)0.5(pzta)]_(n)(HL-3)(Hpzta=3-pyrazinyl-1,2,4-triazole;PTA=terephthalic acid;NA=1,4-naphthalene dicarboxylic acid),based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ***-markably,the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions(25℃and 1 atm).In particular,the complete conversion of 4-nitrophenol(4-NP)took only 30 s on HL-2,reaching a record-high TOF value compared with previously reported metal *** combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron trans-port between the substrates,and was responsible for the outstanding *** work shined lights on the further enhancement of performance for MOFs through rational OMSs construction.

关键词： Metal-organic frameworks Open metal sites Catalysis Copper node 4-Nitrophenol

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Syntheses, structures and magnetic properties of Fe6 and Fe12 ferric wheels

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Science China Chemistry 2015年第12期58卷 1853-1857页

作者： Guojian Ren Yanqing liu Zhenxin Zhao suijun liu Songde Han Jian Xu Xianhe Bu Department of Chemistry Tianjin Key Lab of Metal- and Molecule-Based Material Chemistry and Collaborative Innovation Center of Chemical Science and Engineering (Tianjin) Nankai University

Starting from the same Fe3O(RCO2)6 complex and using a similar synthesis strategy, the Fe6 and Fe12 wheels were obtained by utilizing two designed ligands, 2-amino-2-methyl-1,3-propanediol(L1) and 1,3-propanediol(L2), respectively. A biological buffer reagent, Bis-Tris(2-[bis-(2-hydroxyethyl)amino]-2-(hydroxymethyl)propane-1,3-diol) was first introduced in the synthesis of the Fe12 wheel, playing a vital role in adjusting the acidity of reaction environment. Magnetic studies on both Fe6 and Fe12 wheels revealed strong antiferromagnetic coupling between the spins on FeIII ions.

关键词： ferric wheel syntheses Bis-Tris magnetic properties

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Syntheses, structures and magnetic properties of three Co(Ⅱ)coordination architectures based on a flexible multidentate carboxylate ligand and different N-donor ligands

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Science China Chemistry 2013年第12期56卷 1693-1700页

作者： TIAN Dan liu suijun ZHANG DaShuai CHANG Ze HU TongLiang BU XianHe Department of Chemistry and TKL of Metal- and Molecule-Based Material Chemistry Nankai University

Three new cobalt complexes, {[Co5（tci）2（bimb）3（μ3-O）2（H2O）2]·3DMF·4H2O}n（1）, {[Co3（tci）2（bib）]·2DMF·2H2O}n （2） and {[Co（Htci）（bpea）0.5]-H2O}n （3）（H3tci = tris（2-carboxyethyl）isocyanurate, bimb = 4,4＇-bis（imidazol-l-yl）biphenyl, bib = 1,4-bis（imidazol-l-yl）benzene, bpea = 1,2-bis（4-pyridyl）ethane, DMF = N,N＇-dimethylformamide）, have been successfully synthesized through the assembly of Co（If） ions, H3tci and different N-donor ligands, respectively. All complexes were structurally characterized by single crystal X-ray diffraction, elemental analyses, IR spectra, thermogravimetric （TG） analyses and X-ray powder diffraction （XRPD）. Complex 1 exhibits a 3D three-fold parallel interpenetrated 3D · 3D structure with （65.8） CdSO4 topology. Complex 2 is built from [Co3（μ/2-Ocarboxyl）2（CO2）4] clusters and linear bib ligands, displaying a two-fold par- allel interpenetrated （3,8）-connected （4^3）2（4^6.6^18·8^4） topology, while complex 3 is a 3D pillar-layered structure involving an in- finite -Co-（μ2-Ocarboxyl）（CO2）-Co-chain. The diverse structures of the three complexes indicate that the skeletons of different N-donor ligands play an important role in the assembly of such different frameworks. In addition, magnetic investigation indi- cates that besides spin-orbit coupling of Co（II） ions, there exist antiferromagnetic exchange interactions in Co5 and Co3 clus- ters of 1 and 2, respectively.

关键词： Coordination polymers cobalt clusters topology magnetic properties

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Highly selective and turn-on fluorescence probe with red shift emission for naked-eye detecting Al^(3+)and Ga^(3+)based on metal-organic framework

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Chinese Chemical Letters 2022年第1期33卷 541-546页

作者： Linhui Wu Shuli Yao Hui Xu Tengfei Zheng suijun liu Jinglin Chen Na Li Herui Wen School of Chemistry and Chemical Engineering Jiangxi University of Science and TechnologyGanzhou 341000China School of Materials Science and Engineering Tianjin Key Laboratory of Metal and Molecule-Based Material ChemistryNankai UniversityTianjin 300350China

A novel ZnII-based metal-organic framework with the formula of{[Zn_(2)(BBIP)_(2)(NDC)_(2)]·H_(2)O}n(JXUST-5)derived from 3,5-bis(benzimidazol-1-yl)pyridine(BBIP)and 1,4-naphthalenedicarboxylic acid(H_(2)NDC)has been *** adjacent Zn^(II)ions are linked through two BBIP ligands to form a[Zn_(2)(BBIP)_(2)]secondary building unit(SBU).The neighbouring SBUs are further connected by NDC^(2-)withμ2-η^(1):η^(1)andμ2-η^(1):η^(1):η^(1)bridging modes to form a two-dimensional(2D)*** analysis shows that JXUST-5 could be simplified as an uninodal fes topology with a point symbol of{4.8^(2)}.Furthermore,the 2D framework net could be extended through C-H···πinteraction to form the three-dimensional supramolecular *** experiments suggest that JXUST-5 could selectively and sensitively recognize Al^(3+)and Ga^(3+)through fluorescence enhancement effect along with a relatively large red *** detection limits for Al^(3+)and Ga^(3+)are 0.17 and 0.69 ppm,***,the sensing process for both Al^(3+)and Ga^(3+)could be directly observed with naked eyes under 365 nm UV ***,JXUST-5 could be recycled at least five times as a fluorescent sensor toward Al^(3+)and Ga^(3+),which is the second example of turn-on MOF based fluorescent sensor toward Ga^(3+).

关键词： Metal-organic frameworks Fluorescence probe Naked-eye detection Turn-on effect Red shift emission Al^(3+)and Ga^(3+)

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Two isostructural Ni(Ⅱ)/Co(Ⅱ)-based metal-organic frameworks for selective dye adsorption and catalytic cycloaddition of CO_(2) with epoxides

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Chinese Chemical Letters 2021年第1期32卷 557-560页

作者： Hui Hu Dashuai Zhang Huiling liu Yaoqiang Jin Jun Gao Yongzheng Zhang Zhongmin liu Xiuling Zhang Longlong Geng suijun liu Ranhui Zhang College of Chemistry and Chemical Engineering Dezhou UniversityDezhou 253023China School of Chemistry and Chemical Engineering Jiangxi University of Science and TechnologyGanzhou 341000China College of Chemical Engineering Qingdao University of Science and TechnologyQingdao 266000China College of Chemical and Environmental Engineering Shandong University of Science and TechnologyQingdao 266590China

Two isostructu ral Ni(Ⅱ)/Co(Ⅱ)-based metal-organic frameworks(MOFs),namely {[M_(3)(L)_(2)(bpb)_(3)(H_(2) O)_(4)]·2 DMF·2 H_(2)O}_(n) [M=Ni(HL-5,HL is short for Hui-Ling liu);M=Co(HL-6);H_(3) L=2',6'-dimethyl-[1,1'-biphenyl]-3,4',5-tricarboxylic acid;bpb=1,4-bis(pyrid-4-yl)benzene],have been hydrothermally synthesized and structu rally *** HL-5 and HL-6,which have the same three-interpenetrated3 D pillared-layer framework with sqc306 type topology,present good selective methyl orange(MO)adsorption over rhodamine B(RhB).Moreover,the catalytic CO_(2) cycloaddition properties with epoxides of the two MOFs have also been studied at ambient pressure and temperature.

关键词： Metal-organic frameworks Dye separation Heterogeneous catalysis CO_(2)cycloaddition Coordination polymers

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Two 2D uranyl coordination complexes showing effective photocatalytic degradation of Rhodamine B and mechanism study

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Chinese Chemical Letters 2021年第2期32卷 604-608页

作者： Xiaolan Tong Shan Wang Jun Zuo Yingchong Ge Qiang Gao suijun liu Jianhua Ding Fen liu Jianqiang Luo Jianbo Xiong Stare Key Laboratory of Nuclear Resources and Environment School of ChemistryBiology and Materials ScienceEast China University of TechnologyNanchang 330013China Jiangxi Province Key Laboratory of Synthetic Chemistry East China University of TechnologyNanchang 330013China School of Environmental and Chemical Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of Chemistry and Chemical Engineering Jiangxi University of Science and TechnologyCanzhou 341000China

Two new hydrostable two-dimensional(2 D) uranyl coordination complexes [(UO_(2))_(5)(μ_(3)-O)_(2)(nbca)_(2)].7 H_(2)O(1) and [(UO_(2))_(3)(nbca)_(2)(H_(2)O)_(3)]·2 H_(2)O(2)(H_(3) nbca=5-nitro-1,2,3-benzenetricarboxylic acid) were hydrothermal ***-crystal structural refinements reveal that both of the two complexes were formed by the packing of 2D uranyl coordination sheets via the hydrogen *** nbca ligand coordinating to the uranyl polyhedron centers constructed the 2D *** are UO8 hexagonal bipyramids and UO7 pentagonal bipyramids in 1 while only U07 pentagonal bipyramids in *** degradation of rhodamine B(RhB) in aqueous solution was *** 2 possesses better performance than 1 with 96.2 % of the RhB was degraded in only 60 *** studies reveal that the dissolved oxygens are essential to the RhB *** photocurrent density of 2 is more stable than that of 1,which indicating the stronger ability to separate photoexcited electrons and hole pairs of 2.

关键词： Uranyl-organic frameworks Photocatalytic degradation Coordination complexes Photocurrent Mechanism

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Construction of novel cluster-based MOF as multifunctional platform for CO_(2) catalytic transformation and dye selective adsorption

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Chinese Chemical Letters 2023年第3期34卷 473-476页

作者： Xiuling Zhang Yongzheng Zhang Wenfeng Zhou Huiling liu Dashuai Zhang Hui Hu Chao Lv suijun liu Longlong Geng College of Chemistry and Chemical Engineering Dezhou UniversityDezhou 253023China School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255000China Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry School of Chemistry and Chemical EngineeringJiangxi University of Science and TechnologyGanzhou 341000China

Synthetic conditions and ligands are the key structural defining factors of metal-organic frameworks(MOFs).Therefore,reasonable optimization of these aspects is considered to be an effective means for designing materials with novel structures and target ***,two novel Co(Ⅱ)-based MOFs,namely[Co(HL)(dibp)]_(n)(HL-8) and{[Co_(2)(L)(OH)(dibp)]·DMA}_n(HL-9)(H_(3)L=2',6'-dimethyl-[1,1'-biphenyl]-3,4',5-tricarboxylic acid;dibp=4,4'-di(1H-imidazol-1-yl)-1,1-biphenyl]),have been hydrothermally synthesized and structurally ***-8 crystallizes in the orthorhombic system (Pna2_(1)) with a grid layer structure,while HL-9 crystallizes in the monoclinic P2_(1)/n space group assembled through Co_(4)(OH)_(2)clusters with organic ***,benefiting from the finite cage-like structure,HL-9 exhibited enhanced performance in carbon dioxide(CO_(2)) adsorption/catalytic transformation and excellent size selectivity during dye molecular adsorption process.

关键词： Metal-organic frameworks Metal cluster Catalysis CO_(2)cycloaddition Dye separation

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Emissive Mononuclear Cu（Ⅰ） Triphenylphosphine Complexes with Functionalized 6-tert-Butoxycarbonyl-2,2 ＇-bipyridine

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Chemical Research in Chinese Universities 2018年第1期34卷 19-23页

作者： LUO Yansheng ZENG Xuehua WANG Wanman CHEN Jinglin HE Lihua ZHANG Mengli liu suijun WEN Herui School of Metallurgy and Chemical Engineering Jiangxi University of Science and Technology Ganzhou 341000 P. R. China

Two new emissive mononuclear copper（Ⅰ） triphenylphosphine complexes with functionalized 6-tert- butoxycarbonyl-2,2＇-bipyridiue chelating ligands were prepared and characterized. Each Cu（Ⅰ） cation has a markedly distorted P2N2 tetrahedral array with two different Cu--N bond distances, due to the addition of the bulky tert-butoxycarbonyl group at the 6-position of the 2,2＇-bipyridyl ring. A weak low-energy broad absorption band appears at 330-500 nm in their CH2Cl2 solutions, which is influenced by the methylation of the 2,2＇-bipyridyl ring. At room temperature, the photoluminescence can be clearly observed both in degassed CH2Cl2 solution and in the solid state, because of the introduction of the bulky tert-butoxycarbonyl substituent, and the emission properties are remarkably affected by both the methylation and the alkoxycarbonyl variation of the 2,2＇-bipyridyl ring. It is shown that the introduction of the bulky tert-butoxyearbonyl group is favorable for improving the emission properties of the 6-alkoxycarbonyl-2,2＇-bipyridine-based cuprous complexes.

关键词： Cuprous Methylation Alkoxyearbonyl Phosphine Lnminescence

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Blue-shifted and naked-eye recognition of H_(2)PO_(4)- and acetylacetone based on a luminescent metal-organic framework with new topology and good stability

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Chinese Chemical Letters 2023年第4期34卷 584-589页

作者： Shuli Yao Hui Xu Tengfei Zheng Yunwu Li Haiping Huang Jun Wang Jinglin Chen suijun liu Herui Wen School of Chemistry and Chemical Engineering Jiangxi Provincial Key Laboratory of Functional Molecular Materials ChemistryJiangxi University of Science and TechnologyGanzhou 341000China Fujian Key Laboratory of Functional Marine Sensing Materials Minjiang UniversityFuzhou 350108China Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical EngineeringLiaocheng UniversityLiaocheng 252000China

Fluorescence detecting both organic and inorganic analytes has aroused tremendous scientific interests, because fluorescence techniques have high sensitivity and are easy to operate. A new threedimensional(3D) MOF {[(CH_(3))_(2)NH_(2)][Zn_(3)(bbip)(BTDI)1.5(OH)]·DMF·MeOH·3H_(2)O}n(JXUST-13, bbip = 2,6-bis(benzimidazol-1-yl)pyridine and H_(4)BTDI = 5,5-(benzo[c][1,2,5]thiadiazole-4,7-diyl)diisophthalic acid)with new 4,4,8-connceted topology has been successfully synthesized and structurally characterized. Importantly, JXUST-13 could recognize H_(2)PO_(4)-and acetylacetone(Acac) by obvious fluorescence blue shift and slight enhancement with the detection limits of 2.70 μmol/L and 0.21 mmol/L, respectively. In addition, JXUST-13 exhibits relatively good thermal stability, chemical stabilities as well as reusability, and the analytes could be distinguished by naked eye and fluorescence test paper. Remarkably, JXUST-13 is the first dual-responsive MOF sensor based on fluorescence blue shift for the detection of H_(2)PO_(4)-and Acac with good selectivity in a handy, economic, and environmentally friendly manner.

关键词： Metal-organic framework Fluorescence sensing Naked-eye recognition Fluorescence blue shift H_(2)PO_(4) −and acetylacetone

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Three new Cu(Ⅱ)-Ln(Ⅲ) heterometallic coordination polymers constructed from quinolinic acid and nicotinic acid: Synthesis, structures, and magnetic properties

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Science China Chemistry 2012年第6期55卷 1064-1072页

作者： liu suijun SONG WeiChao XUE Li HAN SongDe ZENG YongFei WANG LiFu BU XianHe Department of Chemistry Tianjin Key Laboratory of Metal & Molecule-based Material Chemistry Nankai University Tianjin 300071 China

Three new Cu（Ⅱ）-Ln（Ⅲ） heterometallic coordination polymers based on two N-heterocyclic carboxylic ligands, {[LnCu（LI）2（L2）（H2O）2]· mH20},, （Ln = La（1）, Nd（2）, Gd（3）, m = 2 （for 1）, 1 （for 2, 3）, H2L1 = quinolinic acid, HE2 = nico- tinic acid）, have been synthesized and characterized. 1 has a two-dimensional （2D） layer structure with a Schlifli symbol of （44.62）, while complexes 2 and 3 are isostructural and have three-dimensional （3D） structures with a Schlafli symbol of （3.4.5）2（32.***.52.6]4.***.83.9）（32.63.7） of 3-nodal net. Magnetic investigations suggest that antiferromagnetic coupling exists be- tween NdIn and Cun in 2, while weak ferromagnetic coupling between GdⅢ and CuⅡ in 3. The difference of magnetic properties between 2 and 3 has been discussed.

关键词： Cu(Ⅱ)-Ln(Ⅲ) coordination polymers metal oxides magnetic properties

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