Structures and Magnetic Properties of an Antiferromagnetically Coupled Polymeric Copper(II) Complex and Ferromagnetically Coupled Hexanuclear Nickel(II) Clusters

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Reactions between 2,6-diformyl-4-methylphenol (DFMF) and tris(hydroxymethyl) aminomethane (THMAM = H3L2) in the presence of copper(II) salts, CuX2 (X = CH3CO2–, BF4–, ClO4–, Cl–, NO3–) and Ni(CH3CO2)2 or Ni(ClO4)2/NaC6H5CO2, sodium azide (NaN3), and triethylamine (TEA), in one pot self-assemble giving a coordination polymer consisting of repeating pentanuclear copper(II) clusters {[Cu2(H5L2–)(μ-N3)]2[Cu(N3)4]·2CH3OH}n (1) and hexanuclear Ni(II) complexes [Ni6(H3L1–)2(HL22–)2(μ-N3)4(CH3CO2)2]·6C3H7NO·C2H5OH (2) and [Ni6(H3L1–)2(HL22–)2(μ-N3)4(C6H5CO2)2]·3C3H7NO·3H2O·CH3OH (3). In 1, H5L2– and in 2 and 3 H3L1– and HL22– represent doubly deprotonated, singly deprotonated, and doubly deprotonated Schiff-base ligands H7L and H4L1 and a tripodal ligand H3L2, respectively. 1 has a novel double-stranded ladder-like structure in which [Cu(N3)4]2– anions link single chains comprised of dinuclear cationic subunits [Cu2(H5L2–)(μ-N3)]+, forming a 3D structure of interconnected ladders through H bonding. Nickel(II) clusters 2 and 3 have very similar neutral hexanuclear cores in which six nickel(II) ions are bonded to two H4L1, two H3L2, four μ-azido, and two μ-CH3CO2–/μ-C6H5CO2– ligands. In each structure two terminal dinickel (Ni2) units are connected to the central dinickel unit through four doubly bridging end-on (EO) μ-azido and four triply bridging μ3-methoxy bridges organizing into hexanuclear units. In each terminal dinuclear unit two nickel centers are bridged through one μ-phenolate oxygen from H3L1–, one μ3-methoxy oxygen from HL22–, and one μ-CH3CO2– (2)/μ-C6H5CO2– (3) ion. Bulk magnetization measurements on 1 show moderately strong antiferromagnetic coupling within the [Cu2] building block (J1 = −113.5 cm–1). Bulk magnetization measurements on 2 and 3 demonstrate that the magnetic interactions are completely dominated by ferromagnetic coupling occurring between Ni(II) ions for all bridges with coupling constants (J1, J2, and J3) ranging from 2.10 to 14.56 cm–1 (in the Ĥ = –J1(Ŝ1Ŝ2) – J1(Ŝ2Ŝ3) – J2(Ŝ3Ŝ4) – J1(Ŝ4Ŝ5) – J1(Ŝ5Ŝ6) – J2(Ŝ1Ŝ6) – J3(Ŝ2Ŝ6) – J3(Ŝ2Ŝ5) – J3(Ŝ3Ŝ5) convention).

创建时间：

2016-02-22