一系列基于吡啶-2,3-二羧酸的铜-稀土异金属配位聚合物（英文）
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摘要
通过LnCl_3·n H_2O,Cu(NO_3)_2·3H_2O,吡啶-2,3-二羧酸(2,3-H_2pydc)和N,N'-二(4H-1,2,4-三唑)己酰胺(dth)的水热反应合成了一系列铜-稀土异金属配位聚合物(CPs),即[Ln Cu(2,3-pydc)_2(adi)_(0.5)(H_2O)_3]·2H_2O[Ln=La(1),Pr(2),Nd(3),H_2adi=己二酸]和[Ln_2Cu_3(2,3-pydc)_6(H_2O)_(10)]·8H_2O[Ln=Sm(4),Eu(5),Gd(6),Tb(7),Dy(8),Er(9),Yb(10),Lu(11)]。通过单晶X-射线衍射,粉末X-射线衍射,元素分析,红外和热重分析对其表征。配位聚合物1-11显示两种具有不同拓扑的三维(3D)结构。adi阴离子源于dth的原位水解。研究了配合物1-11的电化学性质被研究。
A series of copper-lanthanide heterometallic coordination polymers( CPs) were synthesized by the hydrothermal reactions of LnCl_3·n H_2 O,Cu( NO_3)_2·3H_2O,pyridine-2,3-dicarboxylic acid( 2,3-H_2pydc),and N,N'-di( 4H-1,2,4-triazole) hexanamide( dth),namely,[Ln Cu( 2,3-pydc)_2( adi)_(0. 5)( H_2O)_3]·2H_2O[Ln = La( 1),Pr( 2),Nd( 3),H_2 adi = adipic acid] and [Ln_2Cu_3( 2,3-pydc)_6( H_2O)_(10)]·8H_2O [Ln =Sm( 4),Eu( 5),Gd( 6),Tb( 7),Dy( 8),Er( 9),Yb( 10),Lu( 11) ]. They were characterized by singlecrystal X-ray diffraction,powder X-ray diffraction,elemental analysis,IR,and thermogravimetric analysis. CPs1-11 show two types of three-dimensional( 3D) architectures with different topologies. The adi anion is derived from the situ hydrolysis of dth. The electrochemical properties of 1-11 were studied.
A series of copper-lanthanide heterometallic coordination polymers( CPs) were synthesized by the hydrothermal reactions of LnCl_3·n H_2 O,Cu( NO_3)_2·3H_2O,pyridine-2,3-dicarboxylic acid( 2,3-H_2pydc),and N,N'-di( 4H-1,2,4-triazole) hexanamide( dth),namely,[Ln Cu( 2,3-pydc)_2( adi)_(0. 5)( H_2O)_3]·2H_2O[Ln = La( 1),Pr( 2),Nd( 3),H_2 adi = adipic acid] and [Ln_2Cu_3( 2,3-pydc)_6( H_2O)_(10)]·8H_2O [Ln =Sm( 4),Eu( 5),Gd( 6),Tb( 7),Dy( 8),Er( 9),Yb( 10),Lu( 11) ]. They were characterized by singlecrystal X-ray diffraction,powder X-ray diffraction,elemental analysis,IR,and thermogravimetric analysis. CPs1-11 show two types of three-dimensional( 3D) architectures with different topologies. The adi anion is derived from the situ hydrolysis of dth. The electrochemical properties of 1-11 were studied.
引文
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[2]Goura J,Brambleby J,Goddard P,et al.A single-ion magnet based on a heterometallic Co III2DyIIIcomplex[J].Chem.Eur.J.,2015,21:4926-4930.
[3]Cui Y,Yue Y,Qian G,et al.Luminescent functional metal-organic frameworks[J].Chem.Rev.,2012,112:1126-1162.
[4]Sorgho L A,Cantuel M,Petoud S,et al.Optical sensitization and upconversion in discrete polynuclear chromium-lanthanide complexes[J].Coord.Chem.Rev.,2012,256:1644-1663.
[5]Amirkhanov O V,Moroz O V,Znovjyak K O,et al.Heterobinuclear Zn-Ln and Ni-Ln complexes with schiffbase and carbacylamidophosphate ligands:synthesis,crystal structures,and catalytic activity[J].Eur.J.Inorg.Chem.,2014,3720-3730.
[6]Griffiths K,Gallop C W D,Abdul-Sada A,et al.Heteronuclear 3d/DyIIIcoordination clusters as catalysts in a domino reaction[J].Chem.-Eur.J.,2015,21:6358-6361.
[7]Gurunatha K L,Mostafa G,Ghoshal D,et al.Singlecrystal-to-single-crystal structural transformation in a three-dimensional bimetallic(4f-3d)supramolecular porous framework[J].Cryst.Growth Des.,2010,10:2483-2489.
[8]Zhou Y,Hong M,Wu X.Lanthanide-transition metal coordination polymers based on multiple N and O-donor ligands[J].Chem.Commun.,2006,135-143.
[9]Zhou J M,Shi W,Xu N,et al.A New Family of 4f-3d Heterometallic metal-organic frameworks with 2,2'-bipyridine-3,3'-dicarboxylic acid:syntheses,structures and magnetic properties[J].Cryst.Growth Des.,2013,13:1218-1225.
[10]Huang Y G,Jiang F L,Hong M C.Magnetic lanthanide-transition-metal organic-inorganic hybrid materials:From discrete clusters to extended frameworks[J].Coord.Chem.Rev.,2009,253:2814-2834.
[11]Zhang S,Cheng P.Recent advances in the construction of lanthanidecopper heterometallic metal-organic frameworks[J].Cryst Eng Comm,2015,17:4250-4271.
[12]Zhang J W,Kan X M,Liu B Q,et al.Systematic investigation of reaction-time dependence of three series of copper-lanthanide/lanthanide coordination polymers:syntheses,structures,photoluminescence,and magnetism[J].Chem.-Eur.J.,2015,21:16219-16228.
[13]Zou X Y,Jiang D,Dong Y P,et al.Synthesis and crystal structure of N,N'-bis(2-hydroxy-3-methoxy benzy lidene)-1,3-propane diamine dinuclear lanthanide complex[J].Journal of Engineering of Heilongjiang Universicy,2016,7(4):31-36.
[14]Zuo D F,Zhang S,Yu Y H,et al.Syntheses and structures of two ZnIIluminescent complexes constructed from length-modulated semi-rigid pyrazol ligands[J].Journal of Natural Science of Heilongjiang University,2016,33(4):502-508.
[15]Yang T H,Silva A R,Shi F N.Two dimensional porous 3d-4f heterometallic coordination polymers constructed by pyridine-2,3-dicarboxylic acid[J].Cryst EngComm,2015,17:3852-3858.
[16]Zhang J W,Li X L,Kan X M,et al.Solvent-induced copper-lanthanide heterometallic coordination polymers based on pyridine-2,3-dicarboxylic acid:syntheses,structures,and electrochemical properties[J].Inorg.Chim.Acta,2016,447:18-21.
[17]Chen C,Wang N,Long Y,et al.Series of novel 3D microporous heterometallic 3d-4f coordination frameworks with(5,6)-connected topology:synthesis,crystal structure and magnetic properties[J].Cryst Eng Comm,2013,15:4611-4616.
[18]Zhang J W,Kan X M,Li X L,et al.A series of copper-lanthanide heterometallic coordination polymers derived from pyridine-2,3-dicarboxylic acid and in situ generated succinic acid[J].Eur.J.Inorg.Chem.,2016,1060-1067.
[19]Sarkar M,Biradha K.Amide-to-amide hydrogen bonds in the presence of a pyridine functionality:crystal structures of bis(pyridinecarboxamido)alkanes[J].Cryst.Growth Des.,2006,6:202-208.
[20]Rajput L,Singha S,Biradha K.Comparative structural studies on homologues of amides and reverse amides:unprecedented 4-fold interpenetrated quartz network,newβ-sheet,and two-dimensional layers[J].Cryst.Growth Des.,2007,7:2788-2795.
[21]Wang X L,Kang Z H,Wang E B,et al.Preparation,electrochemical property and application in chemically bulk-modified electrode of a hybrid inorganic-organic silicomolybdate nanoparticles[J].Mater.Lett.,2002,56:393-396.
[22]Sheldrick G M.A short history of SHELX[J].Acta Crystallogr.,Sect.A,2008,64:112-122.
[23]Dimos A,Tsaousis D,Michaelides A,et al.Microporous rare earth coordination polymers:effect of lanthanide contraction on crystal architecture and porosity[J].Chem.Mater.,2002,14:2616-2622.
[24]Wang X,Luan J,Lin H,et al.Effect of flexible bispyridyl-bis-amide ligands and dicarboxylates on the assembly and properties of multifunctional Cu(II)metal-organic coordination polymers[J].Dalton Trans.,2013,42:8375-8386.
[25]Wang X L,Luan J,Lu Q L,et al.Three new metaleorganic complexes derived from N,N(-bis(3-pyridinecarboxamide)-1,2-ethane and polycarboxylate ligands:synthesis,fluorescent and electrochemical properties[J].J.Organomet.Chem.,2012,719:1-7.
[26]Wang X L,Luan J,Lin H Y,et al.The various architectures and properties of a series of coordination polymers tuned by the central metals[J].Dalton Trans.,2014,43:8072-8082.
[27]Wang X L,Luan J,Lin H Y,et al.Four cobalt(II)coordination polymers based on a flexible N,N(-bis(3-pyridinecarboxamide)-1,6-hexane ligand:modulation of crystal architectures through the substituent groups of isophthalates[J].Polyhedron,2014,71:111-118.