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Syntheses, Structures, and Magnetic Properties of a Series of Heterotri-, Tetra- and Pentanuclear LnIII⁻CoII Compounds.

ABSTRACT: Three types of Ln(III)⁻Co(II) heterometallic compounds, LnCo₂(L1)₇(bipy)₂ (Ln = Pr-1, Eu-2, Sm-3, Gd-4, Tb-5, Dy-6) (L1 = 4-chlorobenzoate, bipy = 2,2'-bipyridine), Ln₂Co₂(L₂)10(bipy)₂ (Ln = Sm-7, Gd-8, Tb-9, Dy-10, Ho-11, Er-12, Yb-13), (L2 = 2,4-dichlorobenzoate, bipy = 2,2'-bipyridine, phen = 1,10-phenanthroline), and Ln₂Co₃(L1)12(bipy)₂ (Ln = Ho-14, Er-15, Yb-16), were synthesized under hydrothermal conditions and characterized by single crystal X-ray diffraction, IR spectroscopy and magnetic measurements. Structural analyses revealed that 14⁻16 take on a unique linear pentanuclear structural motif. Interestingly, the Ho-containing compound 14 exhibits magnetic relaxation behavior.

SUBMITTER: Xu Y

PROVIDER: S-EPMC6418803 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Syntheses, Structures, and Magnetic Properties of a Series of Heterotri-, Tetra- and Pentanuclear LnIII⁻CoII Compounds.

Xu Yun Y Luo Feng F Zheng Ji-Min JM

Polymers 20190123 2

Three types of Ln(III)⁻Co(II) heterometallic compounds, LnCo₂(L1)₇(bipy)₂ (Ln = Pr-1, Eu-2, Sm-3, Gd-4, Tb-5, Dy-6) (L1 = 4-chlorobenzoate, bipy = 2,2'-bipyridine), Ln₂Co₂(L₂)10(bipy)₂ (Ln = Sm-7, Gd-8, Tb-9, Dy-10, Ho-11, Er-12, Yb-13), (L2 = 2,4-dichlorobenzoate, bipy = 2,2'-bipyridine, phen = 1,10-phenanthroline), and Ln₂Co₃(L1)12(bipy)₂ (Ln = Ho-14, Er-15, Yb-16</ ...[more]

PMID: 30960180

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Project description:The ability of tetraazalene radical bridging ligands to mediate exceptionally strong magnetic exchange coupling across a range of transition metal complexes is demonstrated. The redox-active bridging ligand N,N',N'',N'''-tetra(2-methylphenyl)-2,5-diamino-1,4-diiminobenzoquinone (NMePhLH2) was metalated to give the series of dinuclear complexes [(TPyA)2M2(NMePhL2-)]2+ (TPyA = tris(2-pyridylmethyl)amine, M = MnII, FeII, CoII). Variable-temperature dc magnetic susceptibility data for these complexes reveal the presence of weak superexchange interactions between metal centers, and fits to the data provide coupling constants of J = -1.64(1) and -2.16(2) cm-1 for M = MnII and FeII, respectively. One-electron reduction of the complexes affords the reduced analogues [(TPyA)2M2(NMePhL3-˙)]+. Following a slightly different synthetic procedure, the related complex [(TPyA)2CrIII2(NMePhL3-˙)]3+ was obtained. X-ray diffraction, cyclic voltammetry, and Mössbauer spectroscopy indicate the presence of radical NMePhL3-˙ bridging ligands in these complexes. Variable-temperature dc magnetic susceptibility data of the radical-bridged species reveal the presence of strong magnetic interactions between metal centers and ligand radicals, with simulations to data providing exchange constants of J = -626(7), -157(7), -307(9), and -396(16) cm-1 for M = CrIII, MnII, FeII, and CoII, respectively. Moreover, the strength of magnetic exchange in the radical-bridged complexes increases linearly with decreasing M-L bond distance in the oxidized analogues. Finally, ac magnetic susceptibility measurements reveal that [(TPyA)2Fe2(NMePhL3-˙)]+ behaves as a single-molecule magnet with a relaxation barrier of Ueff = 52(1) cm-1. These results highlight the ability of redox-active tetraazalene bridging ligands to enable dramatic enhancement of magnetic exchange coupling upon redox chemistry and provide a rare opportunity to examine metal-radical coupling trends across a transmetallic series of complexes.

Dataset Information

Syntheses, Structures, and Magnetic Properties of a Series of Heterotri-, Tetra- and Pentanuclear LnIII⁻CoII Compounds.

Publications

Syntheses, Structures, and Magnetic Properties of a Series of Heterotri-, Tetra- and Pentanuclear Ln<sup>III</sup>⁻Co<sup>II</sup> Compounds.

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