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Article Abstract
We present the synthesis of two new novel tetradentate ligands based on 1,3,4-oxadiazole, 2-(2-pyridyl)-5-[,-bis(2-pyridylmethyl)aminomethyl]-1,3,4-oxadiazole (LTetraPy-ODA) and 2-(2-phenyl)-5-[,-bis(2-pyridylmethyl)aminomethyl]-1,3,4-oxadiazole (LTetraPh-ODA). The ligands were used to prepare six mononuclear complexes [Fe(LTetraPy-ODA)(NCE)] (C1-C3) and [Fe(LTetraPh-ODA)(NCE)] (C4-C6) where E = S, Se or BH. In addition, the ligand LTetraPy-ODA was employed in the synthesis of a new di-nuclear complex [FeII2(LTetraPh)](ClO)·1 CHNO·1.5 HO (C7). Characterization of all complexes was carried out using single-crystal X-ray crystallography, elemental analysis, and infrared spectroscopy. Magnetic susceptibility measurements, performed in the temperature range of 2-300 K using a SQUID magnetometer, revealed spin crossover behaviour exclusively in the mononuclear complexes C3 and C6, in which two monodentate NCBH co-ligands coordinate. The presence of the lattice solvent was found to be crucial to the spin transition property, with complex C3 exhibiting a switching temperature () of approximately 165 K and C6 approximately 194 K. The other four mononuclear complexes C1, C2, C4, C5, as well as the dinuclear complex C7 are locked in the high spin state over the measured temperature range. Density Functional Theory (DFT) calculations were performed on complexes C1-C6 to rationalise the observed magnetic behaviour, demonstrating the significant effect of the NCS, NCSe and NCBH co-ligands ligands on the spin-crossover behaviour of the [Fe(L)(NCE)] complexes.
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