Efficient Rare-Earth-Based Coordination Polymers as Green Photocatalysts for the Synthesis of Imines at Room Temperature

被引:34
作者
Aguirre-Diaz, Lina M. [1 ]
Snejko, Natalia [1 ]
Iglesias, Marta [1 ]
Sanchez, Felix [2 ]
Gutierrez-Puebla, Enrique [1 ]
Angeles Monge, M. [1 ]
机构
[1] CSIC, Dept Nuevas Arquitecturas Quim Mat, Inst Ciencia Mat Madrid, Mat Sci Factory, Sor Juana Ines de la Cruz 3, Madrid 28049, Spain
[2] Inst Quim Organ Gen, Dept Sintesis Estruct & Propiedades Compuestos Or, Juan de la Cierva 3, Madrid 28006, Spain
关键词
METAL-ORGANIC FRAMEWORKS; CATALYZED AEROBIC OXIDATION; MULTICOMPONENT REACTIONS; AMINES; RUTHENIUM; MOF; OXIDE; BENZYLAMINES; ACTIVATION; COMPLEXES;
D O I
10.1021/acs.inorgchem.8b00465
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Five new rare-earth coordination polymers (CPs) were designed in order to offer a remarkable platform that contains light-harvesting antennas and catalytic active centers to achieve solar-energy conversion as green alternatives in the synthesis of imines. These five new spirobifluorene-containing Ln-CPs, named [Er-3(Hsfdc)(3)(sfdc)(3)(H2O)]center dot xH(2)O (RPF-30-Er), [Ln(Hsfdc)(sfdc)(EtOH)]center dot S (RPF-31-Ln, where Ln = La, Nd, and Sm and S = H2O or EtOH), and [Ho(Hsfdc)(sfdc)(H2O)] (RPF-32-Ho) (RPF = rare-earth polymeric framework and H(2)sfdc = 9,9'-spirobi[9H-fluorene]-2,2'-dicarboxylic acid), have been solvothermally synthesized, and their structural features can be described as follows: (i) RPF-30-Er shows a 3D framework in which the inorganic trimers (secondary building units) are cross-linked by Hsfdc(-) and sfdc(2-) linkers displaying a pcu topology. (ii) The isostructural RPF-31-Ln series of materials, together with RPF-32-Ho, exhibit a 1D network of chains growing along the a axis with a ribbon-of-rings topology type. The photocatalytic activity of the RPF-n materials was tested in the oxidative coupling of amines using molecular oxygen and air as oxidizing agents under warm light. Among the materials investigated, RPF-31-Nd was chosen to further investigate the approach in the selectivity of different amine derivates.
引用
收藏
页码:6883 / 6892
页数:10
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