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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Tuning of spin crossover behaviour in iron(iii) complexes involving pentadentate Schiff bases and pseudohalides
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Tuning of spin crossover behaviour in iron(iii) complexes involving pentadentate Schiff bases and pseudohalides

机译：调节含五齿席夫碱和拟卤化物的铁（iii）配合物的自旋交叉行为

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摘要

Investigations on a series of eight novel mononuclear iron(iii) Schiff base complexes with the general formula [Fe(L~5)(L~1)]·S (where H_2L~5 = pentadentate Schiff-base ligand, L ~1 = a pseudohalido ligand, and S is a solvent molecule) are reported. Several different aromatic 2-hydroxyaldehyde derivatives were used in combination with a non-symmetrical triamine 1,6-diamino-4-azahexane to synthesize the H_2L~5 Schiff base ligands. The consecutive reaction with iron(iii) chloride resulted in the preparation of the [Fe(L ~5)Cl] precursor complexes which were left to react with a wide range of the L~1 pseudohalido ligands. The low-spin compounds were prepared using the cyanido ligand: [Fe(3m-salpet)(CN)]·CH_3OH (1a), [Fe(3e-salpet)(CN)]·H_2O (1b), while the high-spin compounds were obtained by the reaction of the pseudohalido (other than cyanido) ligands with the [Fe(L~5)Cl] complex arising from salicylaldehyde derivatives: [Fe(3Bu5Me-salpet)(NCS)] (2a), [Fe(3m-salpet)(NCO)]·CH_3OH (2b) and [Fe(3m-salpet)(N_3)] (2c). The compounds exhibiting spin-crossover phenomena were prepared only when L~5 arose from 2-hydroxy-1-naphthaldehyde (H_2L~5 = H_2napet): [Fe(napet)(NCS)]·CH_3CN (3a, T_(1/2) = 151 K), [Fe(napet)(NCSe)]·CH_3CN (3b, T_(1/2) = 170 K), [Fe(napet)(NCO)] (3c, T_(1/2) = 155 K) and [Fe(napet)(N_3)], which, moreover, exhibits thermal hysteresis (3d, T_(1/2)↑ = 122 K, T_(1/2)↓ = 117 K). These compounds are the first examples of octahedral iron(iii) spin-crossover compounds with the coordinated pseudohalides. We report the structure and magnetic properties of these complexes. The magnetic data of all the compounds were analysed using the spin Hamiltonian formalism including the ZFS term and in the case of spin-crossover, the Ising-like model was also applied.
机译：研究了八种具有通式[Fe（L〜5）（L〜1）]·S的新型单核铁（iii）Schiff碱配合物（其中H_2L〜5 =五齿席夫碱配体，L〜1 =假卤代配体，S为溶剂分子）。几种不同的芳族2-羟基醛衍生物与不对称三胺1,6-二氨基-4-氮杂己烷结合使用，合成了H_2L〜5席夫碱配体。与氯化铁（iii）的连续反应导致制备了[Fe（L〜5）Cl]前体复合物，该前体复合物可与各种L〜1假卤代配体反应。使用氰基配体制备低自旋化合物：[Fe（3m-salpet）（CN）]·CH_3OH（1a），[Fe（3e-salpet）（CN）]·H_2O（1b），而高通过假卤代（氰基除外）配体与由水杨醛衍生物[Fe（3Bu5Me-salpet）（NCS）]（2a），[Fe （3m-salpet）（NCO）]·CH_3OH（2b）和[Fe（3m-salpet）（N_3）]（2c）。仅当由2-羟基-1-萘醛（H_2L〜5 = H_2napet）产生L〜5时，才能制备出具有自旋交叉现象的化合物：[Fe（napet）（NCS）]·CH_3CN（3a，T_（1/2 ）= 151 K），[Fe（napet）（NCSe）]·CH_3CN（3b，T_（1/2）= 170 K），[Fe（napet）（NCO）]（3c，T_（1/2）= 155 K）和[Fe（napet）（N_3）]，它们还表现出热滞后性（3d，T_（1/2）↑= 122 K，T_（1/2）↓= 117 K）。这些化合物是具有配位假卤化物的八面体铁（iii）自旋交联化合物的首个实例。我们报告了这些配合物的结构和磁性。使用包括ZFS项在内的自旋哈密顿形式对所有化合物的磁数据进行了分析，并且在自旋交叉的情况下，还使用了类似于Ising的模型。

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