Europium(III), Terbium(III), and Gadolinium(III) Oxamato-Based Coordination Polymers: Visible Luminescence and Slow Magnetic Relaxation

The reaction of aqueous solutions of EuIII, TbIII, and GdIII ions with Na2Hpcpa [H3pcpa = N-(4-carboxyphenyl)oxamic acid] afforded three new isostructural oxamate-containing lanthanide(III) coordination polymers of general formula {LnIII2(Hpcpa)3(H2O)5·H2O}n [Ln = Eu (1),Tb (2), and Gd(3)]. Their structure is made up of neutral zigzag chains running parallel to the [101] direction where double syn-syn carboxylate(oxamate)-bridged dilanthanide(III) pairs (Ln1 and Ln2) are linked by three Hpcpa2- ligands, one of them with the μ-κ2O,O':κO″ coordination mode and the other two with the μ3-κ2O,O':κO″:κO'''. Additionally, two of those chains are interlinked through hydrogen bonding and π-π type in…

2D and 3D mixed MII/CuIImetal–organic frameworks (M = Ca and Sr) withN,N′-2,6-pyridinebis(oxamate) and oxalate: preparation and magneto-structural study

Three heterobimetallic complexes of formula [Ca2Cu3(mpyba)2(2-apyma)(H2O)7]·8.3H2O (1), [Sr2Cu3(mpyba)2(2-apyma)(H2O)8]·11.6H2O (2) and [Sr4.5Cu4(mpyba)4(ox)(H2O)20]·8.5H2O (3) [H4mpyba = N,N'-2,6-pyridinebis(oxamic acid), 2-apyma = 2-(6-aminopyridinyl)oxamate and ox = oxalate] have been synthesized and structurally characterized. Complexes 1 and 2 are isostructural compounds, with tricopper(ii) units having mpyba and its hydrolytic product (2-apyma) as ligands. They are interlinked through strontium(ii) (1) and calcium(ii) (2) ions to afford neutral two-dimensional networks. Two of the copper(ii) ions are five-coordinate in distorted square pyramidal (Cu3) and trigonal bipyramidal (Cu1) su…

Field-induced slow magnetic relaxation and magnetocaloric effects in an oxalato-bridged gadolinium(iii)-based 2D MOF

The coexistence of field-induced slow magnetic relaxation and moderately large magnetocaloric efficiency in the supra-Kelvin temperature region occurs in the 2D compound [GdIII2(ox)3(H2O)6]n·4nH2O (1), a feature that can be exploited in the proof-of-concept design of a new class of slow-relaxing magnetic materials for cryogenic magnetic refrigeration.

A giant hybrid organic-inorganic octahedron from a narrow rim carboxylate calixarene.

Here we discovered an unprecedented giant octahedral coordination compound bearing 16 Zn2+, 12 Na+, 8 O2-, 4 OH-, 13 H2O and 6 L4- ligands [L4- = fully deprotonated tetra(carboxymethoxy)calix[4]arene]. Its structure was elucidated by single-crystal X-ray diffraction, wavelength-dispersive X-ray spectroscopy and MALDI-TOF mass spectrometry. This compound, Zn8Na6L6⊃Zn8Na6O8(OH)4(H2O)13 (external⊃internal), has eight tetrahedral zinc ions forming the coordination vertices of an outermost cube where carboxylate groups from the sodium calixarenes are anchored. Its core consists of eight Zn2+, six Na+, eight O2-, and four OH- distributed over three layers, besides thirteen coordinated H2O molecul…

From Paramagnetic to Single‐Molecule Magnet Behaviour in Heterobimetallic Compounds Containing the Tetrakis(thiocyanato‐ κN )cobaltate(II) Anion

Synthesis, crystal structure and magnetic properties of [Co(bpcam)2]ClO4·dmso·H2O, [Co(bpcam)2]2[Co(NCS)4]·dmso·H2O and [Ni(bpcam)2]·H2O [Hbpcam = bis(2-pyrimidylcarbonyl)amide]

The preparation, spectroscopic characterization, structural study and magnetic investigation of three new complexes of formula [Co(bpcam)2]ClO4·dmso·H2O (1), [Co(bpcam)2]2[Co(NCS)4]·dmso·H2O (2) and [Ni(bpcam)2]·H2O (3) [Hbpcam = bis(2-pyrimidylcarbonyl)amide] are reported. Each bpcam group in 1–3 acts as a tridentate ligand being coordinated to the cobalt(III) (1 and 2)/nickel(II) (3) ions through three nitrogen atoms in a mer-arrangement. Six-coordinate cobalt(III) and nickel(II) occur in 1 and 3 respectively, whereas six-coordinate cobalt(III) and four-coordinate cobalt(II) coexist in 2. Cyclic voltammetry of 1 in acetonitrile shows the occurrence of one quasi reversible CoIII ↔ CoII pro…

Electroswitching of the single-molecule magnet behaviour in an octahedral spin crossover cobalt(ii) complex with a redox-active pyridinediimine ligand

Thermal-assisted spin crossover and field-induced slow magnetic relaxation coexist in the solid state for the mononuclear cobalt(II) complex with the non-innocent 2,6-bis(N-4-methoxyphenylformimidoyl)pyridine ligand. One-electron oxidation of the paramagnetic low-spin CoII ion (SCo = 1/2) to the diamagnetic low-spin CoIII ion (SCo = 0) leads to the electroswitching of the slow magnetic relaxation in acetonitrile solution.

Intermolecular interaction energies and magnetic properties of spin-isolated multinuclear CuII complexes

Dinuclear CuII complexes with 3,5-dinitrobenzoates and 2,2′-bipyridine (2) or 1,10-phenanthroline (3) were synthesized and characterized. A complete energy framework analysis using the HF/3-21G energy model was performed which found that dispersion forces and C—H...O interactions are responsible for the crystal structure features. The magnetic properties of the complexes show a weak magnetic exchange between spins, resulting in low exchange constants of −2.72 (1) cm−1 and −1.10 (1) cm−1 for complexes (2) and (3), respectively. This results from the low overlap between magnetic orbitals induced by 3,5-dinitrobenzoate bridges and the arrangement of the magnetic orbitals. Consequently, the din…

A rare isostructural series of 3d–4f cyanido-bridged heterometallic squares obtained by assembling [FeIII{HB(pz)3}(CN)3]− and LnIII ions: synthesis, X-ray structure and cryomagnetic study

A new series of cyanido-bridged {FeIIILnIII}2 neutral molecular squares of general formula [Fe{HB(pz)3}(CN)(μ-CN)2Ln(NO3)2(pyim)(Ph3PO)]2·2CH3CN [Ln = Ce (1), Pr (2), Nd (3), Gd (4), Tb (5), Dy (6) and Er (7); {HB(pz)3}− = hydrotris(pyrazolyl)borate, pyim = 2-(1H-imidazol-2-yl)pyridine and Ph3PO = triphenylphosphine oxide] were obtained by reacting the low-spin [Fe{HB(pz)3}(CN)3]− species with the preformed [LnIII(pyim)(NO3)2(pyim)(Ph3PO)]+ complex anions (generated in situ by mixing the nitrate salt of each Ln(III) ion with pyim and Ph3PO molecules). Single-crystal X-ray diffraction studies show that 1–7 are isostructural compounds that crystallize in the triclinic P space group. Their cry…

Holmium(III) Single-Ion Magnet for Cryomagnetic Refrigeration Based on an MRI Contrast Agent Derivative

The coexistence of field-induced blockage of the magnetization and significant magnetocaloric effects in the low-temperature region occurs in a mononuclear holmium(III) diethylenetriamine-N,N,N′,N″,N″-pentaacetate complex, whose gadolinium(III) analogue is a commercial MRI contrast agent. Both properties make it a suitable candidate for cryogenic magnetic refrigeration, thus enlarging the variety of applications of this simple class of multifunctional molecular nanomagnets.

CCDC 1969476: Experimental Crystal Structure Determination

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CCDC 1992815: Experimental Crystal Structure Determination

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CCDC 1484384: Experimental Crystal Structure Determination

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CCDC 1992813: Experimental Crystal Structure Determination

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CCDC 1989325: Experimental Crystal Structure Determination

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CCDC 1969477: Experimental Crystal Structure Determination

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CCDC 1449346: Experimental Crystal Structure Determination

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CCDC 1969470: Experimental Crystal Structure Determination

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CCDC 1969471: Experimental Crystal Structure Determination

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CCDC 1876681: Experimental Crystal Structure Determination

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CCDC 2000511: Experimental Crystal Structure Determination

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CCDC 1859264: Experimental Crystal Structure Determination

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CCDC 1449347: Experimental Crystal Structure Determination

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CCDC 1530054: Experimental Crystal Structure Determination

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CCDC 1484386: Experimental Crystal Structure Determination

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CCDC 1530055: Experimental Crystal Structure Determination

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CCDC 2000512: Experimental Crystal Structure Determination

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CCDC 1992814: Experimental Crystal Structure Determination

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CCDC 1530056: Experimental Crystal Structure Determination

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CCDC 1969473: Experimental Crystal Structure Determination

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CCDC 2069070: Experimental Crystal Structure Determination

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CCDC 1484383: Experimental Crystal Structure Determination

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CCDC 1969472: Experimental Crystal Structure Determination

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CCDC 2047766: Experimental Crystal Structure Determination

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CCDC 1480787: Experimental Crystal Structure Determination

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CCDC 1484385: Experimental Crystal Structure Determination

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CCDC 1969475: Experimental Crystal Structure Determination

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CCDC 1989324: Experimental Crystal Structure Determination

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