Immobilization of a Metal Complex in Y-Zeolite Matrix: Synthesis, X-ray Single-Crystal, and Catalytic Activities of a Copper (Schiff-Base)–Y Zeolite Based Hybrid Catalyst
作者:Pratap Kumar Saha、Surajit Banerjee、Sandip Saha、Alok Kumar Mukherjee、Subramanian Sivasanker、Subratanath Koner
DOI:10.1246/bcsj.77.709
日期:2004.4
A new zeolite-immobilized copper(II) complex catalyst has been prepared by entrapping [CuL] [LH2 = N,N′-(1,1-dimethylethylene)bis(salicylaldiimine)] on NaY zeolite matrix. The reaction of Cu–NaY and molten LH2 affords a green mass of crude catalyst that upon a treatment with CH3CN gives a gray-colored hybrid catalyst (CuL–NaY). The prepared catalyst has been characterized by IR and UV–vis spectroscopic and EPR spectrometric measurements, TG–DTA analysis, powder X-ray diffraction, and surface-area measurements. To ascertain the structure of the immobilized complex, a single-crystal X-ray diffraction analysis of [CuL] was performed. Spectroscopic measurements showed that the green crude of CuL–NaY contains a penta- or hexa-coordinated copper(II) moiety, while the CuL–NaY catalyst contains a distorted square-planar [CuL] complex moiety. A remarkable catalytic activity of the prepared hybrid catalyst has been observed in oxidation reactions of 1-naphthol and norbornene.
通过将[CuL] [LH2 = N,N′-(1,1-二甲基乙烯)双(水杨醛二亚胺)]夹杂在 NaY 沸石基体上,制备了一种新的沸石固定化铜(II)复合催化剂。Cu-NaY 与熔融 LH2 反应生成大量绿色粗催化剂,用 CH3CN 处理后生成灰色杂化催化剂(CuL-NaY)。制备的催化剂通过红外光谱、紫外-可见光谱和 EPR 光谱测量、TG-DTA 分析、粉末 X 射线衍射和表面积测量进行了表征。为了确定固定化复合物的结构,对 [CuL] 进行了单晶 X 射线衍射分析。光谱测量结果表明,CuL-NaY 的绿色粗品含有五或六配位的铜(II)分子,而 CuL-NaY 催化剂则含有扭曲的方形平面 [CuL] 复合物分子。所制备的混合催化剂在 1-萘酚和降冰片烯的氧化反应中具有显著的催化活性。