二维和三维3d-4f异金属配位聚合物的合成与结构表征
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摘要
水热法合成了两例3d-4f异金属配位聚合物:{[Yb_2Cu_4(pdc)_5(bpy)_4]·5.5H_2O}_n(1)和{[HoCu_3(pdc)_3(bpy)_3]·4H_2O}_n(2);H_2pdc=吡啶-2,6-二羧酸,bpy=4,4′-联吡啶)。对两例化合物进行了红外、元素分析和X-射线单晶衍射等表征。化合物1和2均属单斜晶系,空间群都为P2/c,晶胞参数分别为a=1.838 0(4) nm,b=1.091 6(2) nm,c=2.627 9(8) nm,β=132.542(18)°;a=2.345 8(5) nm,b=1.036 4(2) nm,c=2.166 9(4) nm,β=105.16(3)°。晶体结构解析显示化合物1是二维层状结构,由Yb_2(pdc)_5二聚体和Cu(bpy)_2链两种模块构筑而成,而化合物2的三维网状结构由Ho(pdc)_3单体和Cu(bpy)_2链通过吡啶羧酸的羧基桥连形成。
In this work, we report the thermal synthesis of two 3 d-4 f heterometallic coordination polymers: {[Yb_2Cu_4(pdc)_5(bpy)_4]·5.5 H_2O}_n(1) and {[HoCu_3(pdc)_3(bpy)_3]·4 H_2O}_n(2)(H_2pdc = pyridine-2, 6-dicarboxylic acid, bpy = 4,4′-bipyridine). The two polymers were characterized by IR, elemental analysis and X-ray single crystal diffraction. Both 1 and 2 crystallize in monoclinic space group P2/c, with the crystal cell parameters for 1: a = 1.838 0(4) nm, b = 1.091 6(2) nm, c = 2.627 9(8) nm, β = 132.542(18)°; and for 2: a = 2.345 8(5) nm, b = 1.036 4(2) nm, c = 2.166 9(4) nm, β = 105.16(3)°. Crystal structure analysis results showed that compound 1 was a two-dimensional layered structure constructed by two modules, Yb_2(pdc)_5 dimer and Cu(bpy)_2 chain, whereas the three-dimensional network structure of 2 was formed by Ho(pdc)_3 monomer and Cu(bpy)_2 chain through the carboxyl bridge of pyridine-2, 6-dicarboxylate.
In this work, we report the thermal synthesis of two 3 d-4 f heterometallic coordination polymers: {[Yb_2Cu_4(pdc)_5(bpy)_4]·5.5 H_2O}_n(1) and {[HoCu_3(pdc)_3(bpy)_3]·4 H_2O}_n(2)(H_2pdc = pyridine-2, 6-dicarboxylic acid, bpy = 4,4′-bipyridine). The two polymers were characterized by IR, elemental analysis and X-ray single crystal diffraction. Both 1 and 2 crystallize in monoclinic space group P2/c, with the crystal cell parameters for 1: a = 1.838 0(4) nm, b = 1.091 6(2) nm, c = 2.627 9(8) nm, β = 132.542(18)°; and for 2: a = 2.345 8(5) nm, b = 1.036 4(2) nm, c = 2.166 9(4) nm, β = 105.16(3)°. Crystal structure analysis results showed that compound 1 was a two-dimensional layered structure constructed by two modules, Yb_2(pdc)_5 dimer and Cu(bpy)_2 chain, whereas the three-dimensional network structure of 2 was formed by Ho(pdc)_3 monomer and Cu(bpy)_2 chain through the carboxyl bridge of pyridine-2, 6-dicarboxylate.
引文
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[29] YANG H,CAO F,LI D C,et al.A family of 12-azametallacrown-4 structural motif with heterometallic Mn-III-Ln-Mn-III-Ln (Ln = Dy,Er,Yb,Tb,Y) alternate arrangement and single-molecule magnet behavior[J].Chem Eur J,2015,21:14478-14485.
[30] ZHENG X Y,ZHANG H,WANG Z X,et al.Insights into magnetic interactions in a monodisperse Gd12Fe14 metal cluster[J].Angew Chem Int Ed,2017,56(38):11475-11479.
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[34] SHEN F X,LI H Q,MIAO H,et al.Heterometallic M(II)Ln(III) (M = Co/Zn;Ln = Dy/Y) complexes with pentagonal bipyramidal 3d centers:syntheses,structures,and magnetic properties[J].Inorg Chem,2018,57(38):15526-15536.
[35] EVANGELISTI F,MORE R,HODEL F,et al.3d-4f {Co■Ln(OR)4} cubanes as bio-inspired water oxidation catalysts[J].J Am Chem Soc,2015,137(34):11076-11084.
[36] HU R X,YANG J,CHEN X,et al.Monomer,chain,layer and 3-D framework constructed by linear 4′-(4-carboxyphenyl)-2,2′:6′,2″-terpyridine[J].Inorg Chim Acta,2018,482:702-708.
[37] SHI P F,HU H C,ZHANG Z Y,et al.Heterometal-organic frameworks as highly sensitive and highly selective luminescent probes to detect I- ions in aqueous solutions[J].Chem Commun,2015,51(19):3985-3988.
[38] LIN X M,DING Y J,LIANG S M,et al.Two series of Ln(III)-Ag(I) heterometallic-organic frameworks constructed from isonicotinate and 2,2′-biphenyldicarboxylate:synthesis,structure and photoluminescence properties[J].Cryst Eng Comm,2015,17:3800-3808.
[39] JIN J,CHEN C,GAO Y,et al.Synthesis,structure,and luminescence property of a series of Ag-Ln coordination polymers with the N-heterocyclic carboxylato ligand[J].J Solid State Chem,2016,235:193-201.
[40] SHELDRICK G M.SHELXS-97,Program for crystal structure solution,University of Gottingen[CP].Germany,1997.
[41] SHELDRICK G M.SHELXL-97,Program for crystal structure refinement,University of Gottingen[CP].Germany,1997.
[42] DU M,BU X H,SHIONOYA M,et al.Metal assisted rearrangement of 2,2-pyridil with M(ClO4)2·6H2O (M=CoII,NiII and CuII):syntheses,characterization and crystal structures[J].J Mol Struct,2002,607(213):155-161.
[43] HUANG C D,QIU T R,WU Y Y,et al.Hydrothermal synthesis,crystal structure and thermal stability of two 3d-4f heterometallic coordination polymers[J].Z Anorg Allg Chem,2009,635(15):2381-2384.
[44] LIANG F P,CHEN Z L,HU R X,et al.Synthesis and crystal structure of heteronuclear LaIII-CuII complex {[LaCu2(NTA)2(4,4′-bpy)(H2O)3]NO3·5H2O}n[J].Chin J Chem,2000,18(6):828-833.
[45] BO Q B,SUN Z X,FORSLING W.A new family of 3D 3d-4f heterometallic frameworks comprising 1D inorganic lanthanide ladders and organic CuI-bipyridine chains[J].Cryst Eng Comm,2008,10(2):232-238.
[2] SAMPANI S I,AUBERT S,CATTOEN M,et al.Dinucleating Schiff base ligand in Zn/4f coordination chemistry:synthetic challenges and catalytic activity evaluation[J].Dalton Trans,2018,47(13):4486-4493.
[3] SOTNIK S A,POLUNIN R A,KISKIN M A,et al.Heterometallic coordination polymers assembled from trigonal trinuclear Fe2Ni-pivalate blocks and polypyridine spacers:topological diversity,sorption,and catalytic properties[J].Inorg Chem,2015,54(11):5169-5181.
[4] WANG L,XU C,HAN Q,et al.Ambient chemical fixation of CO2 using a highly efficient heterometallic helicate catalyst system[J].Chem Commun,2018,54(18):2212-2215.
[5] CRISTOVAO B,MIROSLAW B,KLAK J,et al.Carbonato-bridged heteronuclear Ni(2)(II)Ln(2)(III)(Ln = Tb,Dy,Ho,Er,Tm,Yb,Lu) complexes synthesized by fixation of atmospheric CO2-Structural and magnetic studies[J].Polyhedron,2015,85:697-704.
[6] WANG N,YUE S T,LIU Y L,et al.Hydrothermal syntheses,crystal structure,and magnetic characterization of two 3d-4f heterometallic coordination polymers[J].Cryst Growth Des,2009,9(1):368-371.
[7] WANG K,CHEN Z L,ZOU H H,et al.Two types of Cu-Ln heterometallic coordination polymers with 2-hydroxyisophthalate:syntheses,structures and magnetic properties[J].Cryst Growth Des,2015,15(6):2883-2890.
[8] SHIGA T,ITO N,HIDAKA A,et al.Series of trinuclear NiIILnIIINiII complexes derived from 2,6-di(acetoacetyl)pyridine:synthesis,structure,and magnetism[J].Inorg Chem,2007,46(9):3492-3501.
[9] MAHAPATRA P,KOIZUMI N,KANETOMO T,et al.A series of Cu(II)-Ln(III) complexes of an N2O3 donor asymmetric ligand and a possible Cu-II-Tb-III SMM candidate in no bias field[J].New J Chem,2019,43(2):634-643.
[10] LIANG Y,CAO R,SU W,et al.Syntheses,structures,and magnetic properties of two gadolinium(III)-copper(II) coordination polymers by a hydrothermal reaction[J].Angew Chem Int Ed,2000,39:3304-3307.
[11] ZHANG M B,ZHANG J,ZHENG S T,et al.A 3D coordination framework based on linkages of nanosized hydroxo lanthanide clusters and copper centers by isonicotinate ligands[J].Angew Chem Int Ed,2005,44(9):1385-1388.
[12] WANG M,HE L,LIN Q P.Dimension-related magnetism in heterometallic complexes based on the same [LnCu(dicarboxylpyrazole)2] building moieties[J].J Solid State Chem,2018,265:29-35.
[13] CHEN X M,AUBIN S M J,WU Y L,et al.Polynuclear Cu■M■ (M = Y,Nd,or Gd) complexes encapsulating a ClO■ anion:[Cu12M6(OH)24(H2O)18(pyb)12(ClO4)](ClO4)17·nH2O (Pyb = pyridine betaine) [J].J Am Chem Soc,1995,117:9600-9601.
[14] MEREACRE V M,AKO A M,CLéRAC R,et al.A bell-shaped Mn11Gd2 single-molecule magnet[J].J Am Chem Soc,2007,129(30):9248-9249.
[15] SHEN C J,HU S M,SHENG T L,et al.Syntheses,structures,and properties of a series of novel high-nuclear 3d-4f clusters with mixed amino acids as ligands:{Ln6Cu24}(Ln = Gd,Tb,Pr and Sm).Dalton Trans,2015,44(14):6510-6515.
[16] FELLAH F Z C,BOULEFRED S,FELLAH A C,et al.Binuclear CuLn complexes (LnIII = Gd,Tb,Dy) of alcohol-functionalized bicompartmental Schiff-base ligand.Hydrogen bonding and magnetic behaviors[J].Inorg Chim Acta,2016,439:24-29.
[17] LAMPROPOULOS C,STAMATATOS T C,ABBOUD K A,et al.Initial use of dioximate ligands in 3d/4f cluster chemistry:synthesis,structure,and magnetic studies of an unusual [Gd■MnIVO]8+ complex[J].Inorg Chem,2009,48(2):429-431.
[18] XIANG S C,HU S M,SHENG T L,et al.A fan-shaped polynuclear Gd6Cu12 amino acid cluster:a “hollow” and ferromagnetic [Gd6(μ3-OH)8] octahedral core encapsulated by six [Cu2] glycinato blade fragments[J].J Am Chem Soc,2007,129:15144-15146.
[19] SOPASIS G J,CANAJ A B,PHILIPPIDIS A,et al.Heptanuclear heterometallic [Cu6Ln] clusters:trapping lanthanides into copper cages with artificial amino acids[J].Inorg Chem,2012,51(10):5911-5918.
[20] KONG X J,REN Y P,LONG L S,et al.A keplerate magnetic cluster featuring an icosidodecahedron of Ni(II) ions encapsulating a dodecahedron of La(III) ions[J].J Am Chem Soc,2007,129(22):7016-7017.
[21] CHEN J L,FENG X,XIE S Y,et al.Synthesis,structure and characterization of a 3d-4f hetero-metallic complex based on imidazole-dicarboxylate[J].Chin J Struct Chem,2015,34(5):771-776.
[22] CHEN L,LIU Y,LOU D,et al.Solvothermal synthesis,crystal structure,and luminescent properties of three heterometallic lanthanide-transition-metal frameworks constructed from three types of CuBr motifs[J].Z Anorg Allg Chem,2017,643(15):1004-1010.
[23] ZHANG L,ZHAO L,ZHANG P,et al.Nanoscale {Ln■Zn■} triangular metalloring with magnetic refrigerant,slow magnetic relaxation,and fluorescent properties[J].Inorg Chem,2015,54(23):11535-11541.
[24] SUN Y Q,LIU Q,ZHOU L L,et al.Ln-Cd heterometal organic-inorganic hybrid materials based on diverse Ln-Cd oxo-cluster chains:syntheses,structures and visible luminescence[J].Cryst Eng Comm,2014,16(19):3986-3993.
[25] BENCINI A,BENELLI C,CANESCHI A,et al.Crystal and molecular-structure of and magnetic coupling in two complexes containing gadolinium(III) and copper(II) ions[J].J Am Chem Soc,1985,107(26):8128-8136.
[26] SCHMITZ S,KOVALCHUK A,MARTIN-RODRIGUEZ A,et al.Element-selective molecular charge transport characteristics of binuclear copper(II)-lanthanide(III) complexes[J].Inorg Chem,2018,57(15):9274-9285.
[27] WORRELL A,SUN D,MAYANS J,et al.Oximato-based ligands in 3d/4f-metal cluster chemistry:a family of {Cu3Ln} complexes with a “propeller”-like topology and single-molecule magnetic behavior[J].Inorg Chem,2018,57(31):13944-13952.
[28] WANG J,LU G,LIU Y,et al.Building block and directional bonding approaches for the synthesis of {DyMn4}n (n=2,3) metallacrown assemblies[J].Cryst Growth Des,2019,19:1896-1902.
[29] YANG H,CAO F,LI D C,et al.A family of 12-azametallacrown-4 structural motif with heterometallic Mn-III-Ln-Mn-III-Ln (Ln = Dy,Er,Yb,Tb,Y) alternate arrangement and single-molecule magnet behavior[J].Chem Eur J,2015,21:14478-14485.
[30] ZHENG X Y,ZHANG H,WANG Z X,et al.Insights into magnetic interactions in a monodisperse Gd12Fe14 metal cluster[J].Angew Chem Int Ed,2017,56(38):11475-11479.
[31] HE X X,CHENG W W,LIN Q F,et al.Syntheses,structures,luminescence,and magnetic properties of a series of novel coordination polymers constructed by nanosized [Ln8Fe4] rings[J].Cryst Growth Des,2017,17(1):347-354.
[32] CORRADINI V,GHIRRI A,CANDINI A,et al.Surface investigation on Gd4M8 (M = Zn,Ni) single molecule coolers[J].Adv Funct Mater,2014,24(30):4782-4788.
[33] DONG H M,ZHANG Z C,LI H Y,et al.High-nuclear heterometallic oxime clusters assembled from triangular subunits:solvothermal syntheses,crystal structures and magnetic properties[J].Dalton Trans,2018,47(1):169-179.
[34] SHEN F X,LI H Q,MIAO H,et al.Heterometallic M(II)Ln(III) (M = Co/Zn;Ln = Dy/Y) complexes with pentagonal bipyramidal 3d centers:syntheses,structures,and magnetic properties[J].Inorg Chem,2018,57(38):15526-15536.
[35] EVANGELISTI F,MORE R,HODEL F,et al.3d-4f {Co■Ln(OR)4} cubanes as bio-inspired water oxidation catalysts[J].J Am Chem Soc,2015,137(34):11076-11084.
[36] HU R X,YANG J,CHEN X,et al.Monomer,chain,layer and 3-D framework constructed by linear 4′-(4-carboxyphenyl)-2,2′:6′,2″-terpyridine[J].Inorg Chim Acta,2018,482:702-708.
[37] SHI P F,HU H C,ZHANG Z Y,et al.Heterometal-organic frameworks as highly sensitive and highly selective luminescent probes to detect I- ions in aqueous solutions[J].Chem Commun,2015,51(19):3985-3988.
[38] LIN X M,DING Y J,LIANG S M,et al.Two series of Ln(III)-Ag(I) heterometallic-organic frameworks constructed from isonicotinate and 2,2′-biphenyldicarboxylate:synthesis,structure and photoluminescence properties[J].Cryst Eng Comm,2015,17:3800-3808.
[39] JIN J,CHEN C,GAO Y,et al.Synthesis,structure,and luminescence property of a series of Ag-Ln coordination polymers with the N-heterocyclic carboxylato ligand[J].J Solid State Chem,2016,235:193-201.
[40] SHELDRICK G M.SHELXS-97,Program for crystal structure solution,University of Gottingen[CP].Germany,1997.
[41] SHELDRICK G M.SHELXL-97,Program for crystal structure refinement,University of Gottingen[CP].Germany,1997.
[42] DU M,BU X H,SHIONOYA M,et al.Metal assisted rearrangement of 2,2-pyridil with M(ClO4)2·6H2O (M=CoII,NiII and CuII):syntheses,characterization and crystal structures[J].J Mol Struct,2002,607(213):155-161.
[43] HUANG C D,QIU T R,WU Y Y,et al.Hydrothermal synthesis,crystal structure and thermal stability of two 3d-4f heterometallic coordination polymers[J].Z Anorg Allg Chem,2009,635(15):2381-2384.
[44] LIANG F P,CHEN Z L,HU R X,et al.Synthesis and crystal structure of heteronuclear LaIII-CuII complex {[LaCu2(NTA)2(4,4′-bpy)(H2O)3]NO3·5H2O}n[J].Chin J Chem,2000,18(6):828-833.
[45] BO Q B,SUN Z X,FORSLING W.A new family of 3D 3d-4f heterometallic frameworks comprising 1D inorganic lanthanide ladders and organic CuI-bipyridine chains[J].Cryst Eng Comm,2008,10(2):232-238.