Copper/Zinc-Directed Heterometallic Uranyl-Organic Polycatenating Frameworks: Synthesis, Characterization, and Anion-Dependent Structural Regulation.

By employing a multidentate ligand, 2,2'-bipyridine-5,5'-dicarboxylic acid (H2bpdc), with both O-donors and N-donors, five uranyl-Cu(II)/Zn(II) heterometallic coordination polymers, (UO2)Cu(μ4-bpdc)(μ3-bpdc) (1-Cu), (UO2)Zn(μ4-bpdc)(μ3-bpdc) (1'-Zn), (UO2)CuCl(μ3-bpdc)(μ2-Hbpdc)(H2O) (2-Cu), (UO2)2Cu2Cl2(μ3-bpdc)2(μ2-Hbpdc)2(H2O)3·2H2O (2-Cu'), and (UO2)2Zn(μ3-SO4)(μ4-bpdc)(μ3-bpdc)(H2O)3 (3-Zn), were prepared under hydrothermal conditions. Thermal stability and luminescent properties of 1-Cu, 1'-Zn, 2-Cu, and 3-Zn were also investigated. Isostructural compounds 1-Cu and 1'-Zn both have a three-dimensional (3D) framework built by polycatenating of two sets of paralleling two-dimensional (2D) grids with octahedral transition metal cations (Cu or Zn) as the cross-linking nodes. As far as we know, compounds 1-Cu and 1'-Zn are the first two cases that possess polycatenated networks in heterometallic uranyl-organic coordination polymers. Compound 2-Cu contains 3-fold interpenetrated 2D networks which are built by the connection of [(UO2)2(bpdc)2(Hbpdc)2]2- secondary building units and Cu(II). A one-dimensional tilted ladder-like structure in 2-Cu' is constructed by uranyl-bpdc chains connected by Cu(II) and Hbpdc-. Compound 3-Zn displays a layered-like 2D network contain an unusual [(UO2)2Zn(μ3-SO4)] unit. Interestingly, different anions could lead to the change of coordination sites of transition metal cations, resulting in structural diversity of heterometallic uranyl-organic frameworks.

[1]  Y. Xing,et al.  UO22+-polycarboxylate heterometallic complexes: structure, spectra, and photocatalytic properties , 2016 .

[2]  P. Burns,et al.  Cation-Dependent Hierarchical Assembly of U60 Nanoclusters into Macro-Ion Assemblies Imaged via Cryogenic Transmission Electron Microscopy. , 2016, Journal of the American Chemical Society.

[3]  L. Mei,et al.  Silver Ion-Mediated Heterometallic Three-Fold Interpenetrating Uranyl-Organic Framework. , 2015, Inorganic chemistry.

[4]  J. Harrowfield,et al.  Structural Variations in the Uranyl/4,4'-Biphenyldicarboxylate System. Rare Examples of 2D → 3D Polycatenated Uranyl-Organic Networks. , 2015, Inorganic chemistry.

[5]  J. Harrowfield,et al.  Uranyl Ion Complexes with 1,1'-Biphenyl-2,2',6,6'-tetracarboxylic Acid: Structural and Spectroscopic Studies of One- to Three-Dimensional Assemblies. , 2015, Inorganic chemistry.

[6]  Z. Chai,et al.  Umbellate distortions of the uranyl coordination environment result in a stable and porous polycatenated framework that can effectively remove cesium from aqueous solutions. , 2015, Journal of the American Chemical Society.

[7]  Yingjie Zhang,et al.  Uranium(VI) complexes with isonicotinic acid: from monomer to 2D polymer with unique U–N bonding , 2015 .

[8]  Qipeng Yang,et al.  Thermally Stable Coordination Polymer with Hybrid Functional Groups and Mn–SO4 Double Chains , 2015 .

[9]  Jijiang Wang,et al.  Cooperation of Coordinative and π···π Interaction in Directing Two-fold Interpenetrated Architecture of Two Eu/Dy(III) 2-Sulfoterephthalate Complexes with 4,4′-Bipyridine† , 2015 .

[10]  Z. Chai,et al.  Halogen Bonded Three-Dimensional Uranyl-Organic Compounds with Unprecedented Halogen-Halogen Interactions and Structure Diversity upon Variation of Halogen Substitution , 2015 .

[11]  K. Lillerud,et al.  Probing Reactive Platinum Sites in UiO-67 Zirconium Metal–Organic Frameworks , 2015 .

[12]  Junwei Zhao,et al.  Syntheses, structures and properties of three metal–organic complexes containing 2,2′-dipyridyl-5,5′-dicarboxylate ligands , 2015 .

[13]  J. Harrowfield,et al.  Uranyl Ion Complexes with trans-3-(3-Pyridyl)acrylic Acid Including a Uranyl–Copper(II) Heterometallic Framework , 2014 .

[14]  Xiangfang Peng,et al.  Synthesis, structure and luminescence property of Eu(III) metal–organic framework based on 2,2′-bipyridine-5,5′-dicarboxylic acid , 2014 .

[15]  P. Burns,et al.  Copper(I) and copper(II) uranyl heterometallic hybrid materials. , 2014, Inorganic chemistry.

[16]  C. Cahill,et al.  CuPYDC Metalloligands and Postsynthetic Rearrangement/Metalation as Routes to Bimetallic Uranyl Containing Hybrid Materials: Syntheses, Structures, and Fluorescence , 2014 .

[17]  T. Loiseau,et al.  The crystal chemistry of uranium carboxylates , 2014 .

[18]  P. Thuéry.  Increasing Complexity in the Uranyl Ion–Kemp’s Triacid System: From One- and Two-Dimensional Polymers to Uranyl–Copper(II) Dodeca- and Hexadecanuclear Species , 2014 .

[19]  Guanghua Li,et al.  Assembly of Two Flexible Metal–Organic Frameworks with Stepwise Gas Adsorption and Highly Selective CO2 Adsorption , 2014 .

[20]  C. Cahill,et al.  Postsynthetic Rearrangement/Metalation as a Route to Bimetallic Uranyl Coordination Polymers: Syntheses, Structures, and Luminescence , 2014 .

[21]  Tao Tian,et al.  Structural Variation within Heterometallic Uranyl Hybrids Based on Flexible Alkyldiphosphonate Ligands , 2014 .

[22]  Xiao-Jun Lv,et al.  High gas storage capacities and stepwise adsorption in a UiO type metal-organic framework incorporating Lewis basic bipyridyl sites. , 2014, Chemical communications.

[23]  Xiao-Jun Lv,et al.  A Series of Exceptionally Robust Luminescent Coordination Polymers Based on a Bipyridyldicarboxylate Ligand and Rare‐Earth‐Metal Ions , 2013 .

[24]  Zhonghua Zhu,et al.  Solvent or temperature induced diverse coordination polymers of silver(I) sulfate and bipyrazole systems: syntheses, crystal structures, luminescence, and sorption properties. , 2013, Inorganic chemistry.

[25]  Junwei Zhao,et al.  Syntheses, structures and properties of three new two-dimensional Cu(I)-Ln(III) heterometallic coordination polymers based on 2,2'-dipyridyl-5,5'-dicarboxylate ligands. , 2013, Spectrochimica acta. Part A, Molecular and biomolecular spectroscopy.

[26]  P. Burns,et al.  Series of uranyl-4,4'-biphenyldicarboxylates and an occurrence of a cation-cation interaction: hydrothermal synthesis and in situ Raman studies. , 2013, Inorganic chemistry.

[27]  P. Thuéry.  Uranyl–3d block metal ion heterometallic carboxylate complexes including additional chelating nitrogen donors , 2013 .

[28]  E. Rivière,et al.  Uranyl-copper(II) heterometallic oxalate complexes: coordination polymers and frameworks. , 2013, Dalton transactions.

[29]  T. Loiseau,et al.  Synthesis, Structural Characterization, and Dehydration Analysis of Uranyl Zinc Mellitate, (UO2)Zn(H2O)4(H2mel)·2H2O , 2013 .

[30]  Tao Tian,et al.  Syntheses and structures of a series of uranyl phosphonates and sulfonates: an insight into their correlations and discrepancies. , 2013, Inorganic chemistry.

[31]  P. Burns,et al.  Clusters of actinides with oxide, peroxide, or hydroxide bridges. , 2013, Chemical reviews.

[32]  T. Loiseau,et al.  Structural observations of heterometallic uranyl copper(II) carboxylates and their solid-state topotactic transformation upon dehydration. , 2013, Chemistry.

[33]  Jun Fan,et al.  Construction of luminescent three-dimensional Ln(III)–Zn(II) heterometallic coordination polymers based on 2-pyridyl imidazole dicarboxylate , 2012 .

[34]  Richard A. Taylor,et al.  Isoreticular Lanthanide Metal-Organic Frameworks: Syntheses, Structures and Photoluminescence of a Family of 3D Phenylcarboxylates , 2012 .

[35]  P. Burns,et al.  One-dimensional uranyl-2,2'-bipyridine coordination polymer with cation-cation interactions: (UO2)2(2,2'-bpy)(CH3CO2)(O)(OH). , 2012, Inorganic chemistry.

[36]  Jun Fan,et al.  Two Types of New Three-Dimensional d–f Heterometallic Coordination Polymers Based on 2-(Pyridin-3-yl)-1H-Imidazole-4,5-Dicarboxylate and Oxalate Ligands: Syntheses, Structures, Luminescence, and Magnetic Properties , 2012 .

[37]  Zhong‐Ming Sun,et al.  Tailor-Made Zinc Uranyl Diphosphonates from Layered to Framework Structures , 2012 .

[38]  Till Bousquet,et al.  Six-Fold Coordinated Uranyl Cations in Extended Coordination Polymers , 2012 .

[39]  R. Masel,et al.  Synthesis and characterization of a zinc metal–organic framework with chiral nano-pores , 2012 .

[40]  C. Cahill,et al.  Uranyl hybrid material derived from in situ ligand synthesis: formation, structure, and an unusual phase transformation. , 2012, Angewandte Chemie.

[41]  Junwei Zhao,et al.  Synthesis, structure and properties of a metal–organic complex built up from ferrous sulfate chains and 2,2'-bipyridyl-5,5'-dicarboxylic acid ligands , 2012 .

[42]  Jie Su,et al.  A Family of Flexible Lanthanide Bipyridinedicarboxylate Metal-Organic Frameworks Showing Reversible Single-Crystal to Single-Crystal Transformations , 2012 .

[43]  P. Thuéry,et al.  Uranyl–organic one- and two-dimensional assemblies with 2,2′-bipyridine-3,3′-dicarboxylic, biphenyl-3,3′,4,4′-tetracarboxylic and bicyclo[2.2.2]oct-7-ene-2,3,5,6-tetracarboxylic acids , 2012 .

[44]  Tanya K. Ronson,et al.  New coordination polymers with extended arm cyclotriguaiacyclene ligands: 1D chains, and interpenetrating or polycatenating 2D (4(2).6(2))(4.6(2))2 networks. , 2011, Dalton transactions.

[45]  T. Albrecht‐Schmitt,et al.  Heterobimetallic Copper(II) Uranyl Carboxyphenylphosphonates , 2011 .

[46]  Kaixue Wang,et al.  Extended structures and physicochemical properties of uranyl-organic compounds. , 2011, Accounts of chemical research.

[47]  J. Hupp,et al.  Cubic and rhombohedral heterobimetallic networks constructed from uranium, transition metals, and phosphonoacetate: new methods for constructing porous materials. , 2010, Chemical communications.

[48]  J. Niu,et al.  One-pot syntheses, structures and properties of two novel 1-D copper complexes: [CuII2(Hbpdc)2Cl2]2·2H2O and CuI(H2bpdc)Cl (H2bpdc = 2,2′-bipyridyl-5,5′-dicarboxylic acid) , 2010 .

[49]  Clare E. Rowland,et al.  Hydrothermal Synthesis of Disulfide-Containing Uranyl Compounds: In Situ Ligand Synthesis versus Direct Assembly , 2010 .

[50]  Youngmee Kim,et al.  Two-dimensional metal-organic frameworks with blue luminescence. , 2010, Dalton transactions.

[51]  P. Thuéry.  Two uranyl–organic frameworks with pyridinecarboxylate ligands. A novel heterometallic uranyl–copper(II) complex with a cation–cation interaction , 2009 .

[52]  Bo Xu,et al.  Anion-Assisted Structural Variation of Cadmium Coordination Polymers: From 2D → 3D Inclined Polycatenation to 2D → 3D Polythreading , 2009 .

[53]  C. Su,et al.  An unusual 3D coordination polymer assembled through parallel interpenetrating and polycatenating of (6,3) nets , 2009 .

[54]  C. Cahill,et al.  Homo- and heterometallic coordination polymers from the f elements , 2007 .

[55]  K. Lillerud,et al.  A thermally stable Pt/Y-based metal-organic framework: Exploring the accessibility of the metal centers with spectroscopic methods using H2O, CH3OH, and CH3CN as probes. , 2006, The journal of physical chemistry. B.

[56]  C. Cahill,et al.  Synthesis, structure and fluorescent studies of novel uranium coordination polymers in the pyridinedicarboxylic acid system. , 2006, Dalton transactions.

[57]  Zhong-Min Su,et al.  Entangled coordination networks with inherent features of polycatenation, polythreading, and polyknotting. , 2005, Angewandte Chemie.

[58]  K. Lii,et al.  Hydrothermal synthesis and characterization of [(UO2)2F8(H2O)2Zn2(4,4'-bpy)2].(4,4'-bpy), a mixed-metal uranyl aquofluoride with a pillared layer structure. , 2005, Inorganic chemistry.

[59]  C. Cahill,et al.  Syntheses, structures and fluorescent properties of two novel coordination polymers in the U-Cu-H3pdc system. , 2005, Dalton transactions.

[60]  S. Rizzato,et al.  New architectures from the self-assembly of MIISO4 salts with bis(4-pyridyl) ligands. The first case of polycatenation involving three distinct sets of 2D polymeric (4,4)-layers parallel to a common axis , 2003 .

[61]  D. O′Hare,et al.  Variable Dimensionality in the UO2(CH3CO2)2·2H2O/HF/Isonicotinic Acid System: Synthesis and Structures of Zero-, One-, and Two-Dimensional Uranium Isonicotinates , 2003 .

[62]  P. Nicholls,et al.  The single-crystal electronic and electron spin resonance spectra of calcium copper(II) acetate hexahydrate , 1970 .