苄基膦酸功能配合物的设计及性能研究
摘要
本文采用1,3-二苄基膦酸(H4L1)和1,4-羧酸苄基膦酸单乙酯(H2L2')两个配体分别和金属硝酸盐进行水热反应，通过严格地调控反应体系的pH值合成了三个系列单晶相的无机-有机配合物。
配合物Ln(HL1)(H2O)2(Ln=La,1; Pr,2; Nd,3; Sm,4; Eu,5; Gd,6; Tb,7)通过{CPO3}四面体桥接{LnO7}多面体形成同种构型的二维网络，层间由配体的苄基间的C H π相互作用来堆积。荧光光谱表明配合物4、5和7分别在黄色、红色和绿色的可见光区显示强的金属中心特征发射。磁性研究表明配合物2和7呈现反铁磁性的相互作用。
配合物Ln(HL2)(H2L2)(H2O)(H3L2=HOOCC6H4CH2PO(OH)2, Ln=La,8; Ce,9; Pr,10; Nd,11; Sm,12; Eu,13; Gd,14; Tb,15)同样是通过{CPO3}四面体桥接{LnO7}多面体形成的二维框架结构，层间通过配体的羧酸基团之间的氢键作用相连。荧光光谱表明配合物13和15呈现稀土金属离子为中心的红色和绿色的特征发射。给出了配体和金属离子之间可能的能量传递过程，并估算了相关的电子激发态能级。磁性研究表明配合物14和15的稀土离子之间在临界温度以上为反铁磁性的相互作用，在临界温度以下为铁磁性相互作用。
此外，配合物M(H2L2)2(H2O)2(M=Co,16; Ni,17; Zn,18; Cd,19)为{MO6}多面体同{CPO3}四面体桥连而成的一维之字形链结构。配合物18和19的荧光发射光谱位于蓝色的可见光区，可以作为潜在的荧光材料。
Three series of novel organic–inorganic complexes based on phosphonic acidligands1,3-C6H4[CH2P(O)(OH)2]2(H4L1),1,4-HOOCC6H4CH2PO(OH)(OC2H5)(H2L2')and metal nitrates have been obtained as single phases by regulating the pH underhydrothermal conditions.
Complexes Ln(HL1)(H2O)2(Ln=La,1; Pr,2; Nd,3; Sm,4; Eu,5; Gd,6; and Tb,7) are isomorphous two-dimensional network in which {LnO7} polyhedra areinterconnected by bridging {CPO3} tetrahedra. These layers are further stacked with thebenzyl groups of ligands via C–H···π interaction. Luminescences indicate thatcomplexes4,5, and7show strong metal-centered emissions in yellow, red and greenlight region, respectively. Magnetic properties of complexes2and7indicate thatthere are antiferromagnetic interactions.
Complexes Ln(HL2)(H2L2)(H2O)(H3L2=HOOCC6H4CH2PO(OH)2, Ln=La,8;Ce,9; Pr,10; Nd,11; Sm,12; Eu,13; Gd,14; Tb,15) are also two-dimensionalframework in which the {LnO7} polyhedra are interconnected by bridging {CPO3}tetrahedra. These layers are further cross-linked by hydrogen-bonds of the COOHgroups of ligands. Luminescences show that complexes13and15display Ln-centeredstrong red and green luminescence, respectively. The possible energy transferprocesses between ligands and metal ions have been elucidated and the energy levelsof the relevant electronic states have been estimated. Magnetic properties ofcomplexes14and15indicate that there are antiferromagnetic interactions above TCand ferromagnetic interactions under TCbetween Ln3+ions.
In addition, Complexes M(H2L2)2(H2O)2(M=Co,16; Ni,17; Zn,18; Cd,19)feature a one-dimensional (1D) zigzag chain in which the {MO6} polyhedra areinterconnected by bridging {CPO3} tetrahedra. Luminescent measurements illustratethat complexes18and19are blue light emission bands and could be served aspotential luminescence materials.
配合物Ln(HL1)(H2O)2(Ln=La,1; Pr,2; Nd,3; Sm,4; Eu,5; Gd,6; Tb,7)通过{CPO3}四面体桥接{LnO7}多面体形成同种构型的二维网络，层间由配体的苄基间的C H π相互作用来堆积。荧光光谱表明配合物4、5和7分别在黄色、红色和绿色的可见光区显示强的金属中心特征发射。磁性研究表明配合物2和7呈现反铁磁性的相互作用。
配合物Ln(HL2)(H2L2)(H2O)(H3L2=HOOCC6H4CH2PO(OH)2, Ln=La,8; Ce,9; Pr,10; Nd,11; Sm,12; Eu,13; Gd,14; Tb,15)同样是通过{CPO3}四面体桥接{LnO7}多面体形成的二维框架结构，层间通过配体的羧酸基团之间的氢键作用相连。荧光光谱表明配合物13和15呈现稀土金属离子为中心的红色和绿色的特征发射。给出了配体和金属离子之间可能的能量传递过程，并估算了相关的电子激发态能级。磁性研究表明配合物14和15的稀土离子之间在临界温度以上为反铁磁性的相互作用，在临界温度以下为铁磁性相互作用。
此外，配合物M(H2L2)2(H2O)2(M=Co,16; Ni,17; Zn,18; Cd,19)为{MO6}多面体同{CPO3}四面体桥连而成的一维之字形链结构。配合物18和19的荧光发射光谱位于蓝色的可见光区，可以作为潜在的荧光材料。
Three series of novel organic–inorganic complexes based on phosphonic acidligands1,3-C6H4[CH2P(O)(OH)2]2(H4L1),1,4-HOOCC6H4CH2PO(OH)(OC2H5)(H2L2')and metal nitrates have been obtained as single phases by regulating the pH underhydrothermal conditions.
Complexes Ln(HL1)(H2O)2(Ln=La,1; Pr,2; Nd,3; Sm,4; Eu,5; Gd,6; and Tb,7) are isomorphous two-dimensional network in which {LnO7} polyhedra areinterconnected by bridging {CPO3} tetrahedra. These layers are further stacked with thebenzyl groups of ligands via C–H···π interaction. Luminescences indicate thatcomplexes4,5, and7show strong metal-centered emissions in yellow, red and greenlight region, respectively. Magnetic properties of complexes2and7indicate thatthere are antiferromagnetic interactions.
Complexes Ln(HL2)(H2L2)(H2O)(H3L2=HOOCC6H4CH2PO(OH)2, Ln=La,8;Ce,9; Pr,10; Nd,11; Sm,12; Eu,13; Gd,14; Tb,15) are also two-dimensionalframework in which the {LnO7} polyhedra are interconnected by bridging {CPO3}tetrahedra. These layers are further cross-linked by hydrogen-bonds of the COOHgroups of ligands. Luminescences show that complexes13and15display Ln-centeredstrong red and green luminescence, respectively. The possible energy transferprocesses between ligands and metal ions have been elucidated and the energy levelsof the relevant electronic states have been estimated. Magnetic properties ofcomplexes14and15indicate that there are antiferromagnetic interactions above TCand ferromagnetic interactions under TCbetween Ln3+ions.
In addition, Complexes M(H2L2)2(H2O)2(M=Co,16; Ni,17; Zn,18; Cd,19)feature a one-dimensional (1D) zigzag chain in which the {MO6} polyhedra areinterconnected by bridging {CPO3} tetrahedra. Luminescent measurements illustratethat complexes18and19are blue light emission bands and could be served aspotential luminescence materials.
引文
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