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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Spin crossover Fe(II) complexes of a cross-bridged cyclam derivative
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Spin crossover Fe(II) complexes of a cross-bridged cyclam derivative

机译：旋转交叉FE（II）跨桥循环衍生物的复合物

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摘要

A cross-bridged cyclam derivative containing two 2-pyridylmethyl pendant arms (L = 4,11-bis((pyridin-2-yl)methyl)-1,4,8,11-tetraaza-bicyclo[6.6.2]hexadecane) was synthesized by dialkylation of the cross-bridged cyclam with 2-chloromethylpyridine. A series of Fe(ii) complexes with L and different counter anions of the formulas [Fe(L)][FeCl4 center dot H2O (1-H2O), [Fe(L)Cl-2.4H(2)O (2.4H(2)O), [Fe(L)](BF4)(2)center dot 0.5CH(3)CN (3.0.5CH(3)CN) and [Fe(L)](BPh4)(2)center dot CH3OH (4 center dot CH3OH) was prepared and thoroughly characterized. In all the cases, the [Fe(L)]2 cation adopts a cis-V configuration with a distorted octahedral geometry, and with the FeN6 donor set. The magnetic measurements within the temperature interval of 5-400 K revealed the spin crossover (SCO) behaviour of all the complexes with the transition temperature T-1/2 increasing with the counter anion in the order BF4- (3) [FeCl4](2-) (1) BPh4- (4). However, the SCO process was complete in the case of compound 3 only, with T1/2 = 177 K, which proceeded after removal of co-crystallized CH3CN molecules accompanied by a change of the crystallographic phase. The SCO behaviour of 3 was also confirmed by a single crystal X-ray analysis providing the average (Fe N)distances of 2.086 angstrom at 120 K and 2.197 angstrom at 293 K typical of low-spin, and high-spin Fe-II complexes, respectively. The obtained results clearly showed that the nature of the counter anion and the presence/absence of co-crystallized solvent molecule(s) significantly affected the temperature as well as the abruptness of the spin transition. This is the first report of SCO behaviour observed for iron complexes containing a cross-bridged cyclam derivative.
机译：含有两个2-吡啶基甲基侧臂（L = 4,11-双（（吡啶-2-基）甲基）-1,4,8,11-Tetraaza-biCyClo [6.6.2]十六烷的交叉桥桥衍生物通过用2-氯甲基吡啶的交叉桥环的二烷基化合成。一系列Fe（II）配合物，具有L和不同的配方的抗体[Fe（L）] [FeCl4中心点H2O（1-H 2 O），[Fe（1）Cl-2.4h（2）O（2.4h （2）O），[Fe（1）]（BF4）（2）中心点0.5CH（3）CN（3.0.5CH（3）CN）和[Fe（L）]（BPH4）（2）中心点制备CH 3 OH（4中心点CH 3 OH）并彻底表征。在所有情况下，[Fe（L）] 2阳离子采用具有扭曲八面体几何形状的CIS-V配置，以及FEN6供体组。在5-400k的温度间隔内的磁性测量揭示了所有复合物的旋转交叉（SCO）行为，转变温度T-1/2随着BF4-（3）＆lt中的顺序的反阴离子而增加。 [FECL4]（2-）（1）＆ BPH4-（4）。然而，在化合物3的情况下，SCO过程仅完成，T1 / 2 = 177 k，其在除去伴随结晶相的变化的共结晶的CH3CN分子之后进行。通过单晶X射线分析还确认了3的SCO行为，在典型的低旋转的293K和高旋转Fe-II复合物中，单晶X射线分析提供平均（Fe N）距离为120 k和2.197埃距。 ， 分别。所得结果清楚地表明，抗衡阴离子的性质和共结晶的溶剂分子的存在/不存在显着影响了温度以及旋转过渡的突然性。这是对于含有交叉桥族衍生物的铁络合物观察到的SCO行为的第一份报告。

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