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Heterometallic Octanuclear Ni^II ₄Ln^III ₄ (Ln = Y, Gd, Tb, Dy, Ho, Er) Complexes Containing Ni^II ₂Ln^III ₂O₄ Distorted Cubane Motifs: Synthesis, Structure, and Magnetic Properties.

ABSTRACT: The reaction of 2-methoxy-6-[{2-(2-hydroxyethylamino)ethylimino}methyl] phenol (LH₃) with lanthanide metal salts followed by the addition of nickel acetate allowed isolation of a family of octanuclear complexes, [Ni₄Ln₄(?₂-OH)₂(?₃-OH)₄(?-OOCCH₃)₈(LH₂)₄]·(OH)₂·xH₂O. Single crystal X-ray diffraction studies of these complexes reveal that their central metallic core consists of two tetranuclear [Ni₂Ln₂O₄] cubane subunits fused together by acetate and hydroxide bridges. The magnetic study of these complexes reveals a ferromagnetic interaction between the Ln^III and the Ni^II center. The magnitude of exchange coupling between the Ni^II and Ln^III center, parametrized from the magnetic data of the Gd analogue, gives J = +0.86 cm^-1. The magneto caloric effect, studied for the Ni^II ₄Gd^III ₄ complex, shows a maximum of magnetic entropy change, -?S _m = 22.58 J kg^-1 K^-1 at 3 K for an applied external field of 5 T.

SUBMITTER: Kalita P

PROVIDER: S-EPMC6641754 | biostudies-literature | 2018 May

REPOSITORIES: biostudies-literature

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Heterometallic Octanuclear NiII 4LnIII 4 (Ln = Y, Gd, Tb, Dy, Ho, Er) Complexes Containing NiII 2LnIII 2O4 Distorted Cubane Motifs: Synthesis, Structure, and Magnetic Properties.

Kalita Pankaj P Goura Joydeb J Herrera Juan Manuel JM Colacio Enrique E Chandrasekhar Vadapalli V

ACS omega 20180514 5

The reaction of 2-methoxy-6-[{2-(2-hydroxyethylamino)ethylimino}methyl] phenol (LH3) with lanthanide metal salts followed by the addition of nickel acetate allowed isolation of a family of octanuclear complexes, [Ni4Ln4(μ2-OH)2(μ3-OH)4(μ-OOCCH3)8(LH2)4]·(OH)2·xH2O. Single crystal X-ray diffraction studies of these complexes reveal that their centra ...[more]

PMID: 31458734

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Project description:The new heterometallic compounds, [{Cu(pn)2}2Ni(NCS)6]n·2nH2O (1), [{CuII(trien)}2Ni(NCS)6CuI(NCS)]n (2) and [Cu(tren)(NCS)]4[Ni(NCS)6] (3) (pn = 1,2-diaminopropane, trien = triethylenetetramine and tren = tris(2-aminoethylo)amine), were obtained and characterized by X-ray analysis, IR spectra, XAS and magnetic measurements. Compounds 1, 2 and 3 show the structural diversity of 2D, 1D and 0D compounds, respectively. Depending on the polyamine used, different coordination polyhedron for Cu(II) was found, i.e., distorted octahedral (1), square pyramidal (2) and trigonal bipyramidal (3), whereas coordination polyhedron for nickel(II) was always octahedral. It provides an approach for tailoring magnetic properties by proper selection of auxiliary ligands determining the topology. In 1, thiocyanate ligands form bridges between the copper and nickel ions, creating 2D layers of sql topology with weak ferromagnetic interactions. Compound 2 is a mixed-valence copper coordination polymer and shows the rare ladder topology of 1D chains decorated with [CuII(tren)]2+ antennas as the side chains attached to nickel(II). The ladder rails are formed by alternately arranged Ni(II) and Cu(I) ions connected by N2 thiocyanate anions and rungs made by N3 thiocyanate. For the Cu(I) ions, the tetrahedral thiocyanate environment mixed N/S donor atoms was found, confirming significant coordination spheres rearrangement occurring at the copper precursor together with the reduction in some Cu(II) to Cu(I). Such topology enables significant simplification of the magnetic properties modeling by assuming magnetic coupling inside {NiIICuII2} trinuclear units separated by diamagnetic [Cu(NCS)(SCN)3]3- linkers. Compound 3 shows three discrete mononuclear units connected by N-H…N and N-H…S hydrogen bonds. Analysis of XAS proves that the average ligand character and the covalency of the unoccupied metal d-based orbitals for copper(II) and nickel(II) increase in the following order: 1 → 2 → 3. In 1 and 2, a weak ferromagnetic coupling between copper(II) and nickel(II) was found, but in 2, additional and stronger antiferromagnetic interaction between copper(II) ions prevailed. Compound 3, as an ionic pair, shows, as expected, a spin-only magnetic moment.

Dataset Information

Heterometallic Octanuclear Ni^II ₄Ln^III ₄ (Ln = Y, Gd, Tb, Dy, Ho, Er) Complexes Containing Ni^II ₂Ln^III ₂O₄ Distorted Cubane Motifs: Synthesis, Structure, and Magnetic Properties.

Publications

Heterometallic Octanuclear Ni<sup>II</sup> <sub>4</sub>Ln<sup>III</sup> <sub>4</sub> (Ln = Y, Gd, Tb, Dy, Ho, Er) Complexes Containing Ni<sup>II</sup> <sub>2</sub>Ln<sup>III</sup> <sub>2</sub>O<sub>4</sub> Distorted Cubane Motifs: Synthesis, Structure, and Magnetic Properties.

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