以含氮杂芳香环为配体的新型配位化合物的合成及其性质研究
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摘要
本论文以2-(3,5-二甲基吡唑)-1,10-邻菲啰啉化合物(L)为配体,共设计合成了五个新型单核配合物,即,单核Mn(II)配合物[Mn(L)(NCS)_2] (1);单核Cu(II)配合物[Cu(L)(L_1)Br](ClO_4)(H_2O) (2) (L_1=3,5-二甲基吡唑);三个单核Cd(II)配合物[Cd(L)(NCS)_2] (3),[Cd(L)Cl_2] (4)和[Cd(L)(O_2N)Cl] (5)。对所合成的配合物进行了红外光谱表征及X-射线单晶衍射结构表征。对配合物(1)和(2)中所存在的π-π重叠结构特点进行了研究;对配合物(3)、(4)和(5)进行了配体结构特性与其配合物特征间的结构关联因素研究;对配合物(1)在温度区间为2-300K内进行了变温磁化率测定。对变温磁化率数据使用双核Mn(II)拟合公式进行了拟合,所得拟合参数表明,由于π-π重叠而导致相邻Mn(II)离子间存在弱的反铁磁相互作用,其2J=-0.36 cm~(-1)。本论文的研究成果对于探索了解π-π重叠与其相关联的顺磁金属离子间的磁耦合机理及合成理想的分子基铁磁材料方面具有重要的理论与实验指导意义。
In this dissertation five novel coordination complexes have been designed and synthesized dealing with the 2-(3,5-dimethyl-1H-pyrazol-1-yl)-1,10-phe- nanthroline (L) as ligands and the five complexes include the mononuclear manganese(II) complex [Mn(L)(NCS)_2] (1);the mononuclear copper(II) complex [Cu(L)(L_1)Br](ClO_4)(H_2O) (2) (L_1=3,5-dimethyl-1H-pyrazol-1-yl) and the three mononuclear cadmium(II) complexes, namely, [Cd(L)(NCS)_2] (3), [Cd(L)Cl_2] (4) and [Cd(L)(O_2N)Cl] (5).The five complexes were characterized by infrared spectra and their crystal structures determined by X-ray crystallographic analysis. The study on the correlation between the structures of ligands and the coordination characters has been made and some correlation factors has been obtained. The varied-temperature magnetic susceptibilities were measured on complex (1) in the 2-300 K temperature range and the fitting with formula of a binuclear Manganese(II) has been processed based on the data of the susceptibilities and some correlation factors between theπ-πstacking and the magnetic coupling have been obtained, which indicates that theπ-πstacking resulted in a weak anti-ferromagnetic interaction between the neighbor mangase(II) ions. The obtained results will benefit the understanding of magnetic coupling mechanism forπ-πstacking and the preparation for ideal molecular magnets. The obtained results also will play an important role in understanding of coordination characters and structure specialties for complexes with the derivatives of 1,10-phenanthroline as ligands.
In this dissertation five novel coordination complexes have been designed and synthesized dealing with the 2-(3,5-dimethyl-1H-pyrazol-1-yl)-1,10-phe- nanthroline (L) as ligands and the five complexes include the mononuclear manganese(II) complex [Mn(L)(NCS)_2] (1);the mononuclear copper(II) complex [Cu(L)(L_1)Br](ClO_4)(H_2O) (2) (L_1=3,5-dimethyl-1H-pyrazol-1-yl) and the three mononuclear cadmium(II) complexes, namely, [Cd(L)(NCS)_2] (3), [Cd(L)Cl_2] (4) and [Cd(L)(O_2N)Cl] (5).The five complexes were characterized by infrared spectra and their crystal structures determined by X-ray crystallographic analysis. The study on the correlation between the structures of ligands and the coordination characters has been made and some correlation factors has been obtained. The varied-temperature magnetic susceptibilities were measured on complex (1) in the 2-300 K temperature range and the fitting with formula of a binuclear Manganese(II) has been processed based on the data of the susceptibilities and some correlation factors between theπ-πstacking and the magnetic coupling have been obtained, which indicates that theπ-πstacking resulted in a weak anti-ferromagnetic interaction between the neighbor mangase(II) ions. The obtained results will benefit the understanding of magnetic coupling mechanism forπ-πstacking and the preparation for ideal molecular magnets. The obtained results also will play an important role in understanding of coordination characters and structure specialties for complexes with the derivatives of 1,10-phenanthroline as ligands.
引文
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