화학공학소재연구정보센터
Inorganic Chemistry, Vol.51, No.17, 9282-9296, 2012
pH-Specific Hydrothermal Assembly of Binary and Ternary Pb(II)-(O,N-Carboxylic Acid) Metal Organic Framework Compounds: Correlation of Aqueous Solution Speciation with Variable Dimensionality Solid-State Lattice Architecture and Spectroscopic Signatures
Hydrothermal pH-specific reactivity in the binary/ternary systems of Pb(II) with the carboxylic acids N-hydroxyethyliminodiacetic acid (Heida), 1,3-diamino-2-hydroxypropane-N,N,N', N'-tetraacetic acid (Dpot), and 1,10-phenanthroline (Phen) afforded the new well-defined crystalline compounds [Pb(Heida)]center dot nH(2)O(1), [Pb(Phen)(Heida)]center dot 4H(2)O(2), and [Pb-3(NO3)(Dpot)](n) (3). All compounds were characterized by elemental analysis, FT-IR, solution or/and solid-state NMR, and single-crystal X-ray diffraction. The structures in 1-2 reveal the presence of a Pb(1) center coordinated to one Heida ligand, with 1 exhibiting a two-dimensional (2D) lattice extending to a three-dimensional (3D) one through H-bonding interactions. The concurrent aqueous speciation study of the binary Pb(II) Heida system projects species complementing the synthetic efforts, thereby lending credence to a global structural speciation strategy in investigating binary/ternary Pb(II)-Heida/Phen systems. The involvement of Phen in 2 projects the significance of nature and reactivity potential of N-aromatic chelators, disrupting the binary lattice in 1 and influencing the nature of the ultimately arising ternary 3D lattice. 3 is a ternary coordination polymer, where Pb(II)-Dpot coordination leads to a 2D metal organic-framework material with unique architecture. The collective physicochemical properties of 1-3 formulate the salient features of variable dimensionality metal organic-framework lattices in binary/ternary Pb(II)-(hydroxycarboxylate) structures, based on which new Pb(II) materials with distinct architecture and spectroscopic signature can be rationally, designed and pursued synthetically.