Y沸石和多级孔Y沸石封装CuPhen配合物催化性能的比较

摘要

1,10-phenanthroline Cu(Ⅱ) complexes (CuPhen) were successfully encapsulated in the cavities of conventional zeolite-Y and hierarchical zeolite-Y hosts obtained via post-treatment by the flexible ligand method.The physicochemical properties of the prepared hybrids were characterized by X-ray diffraction,TEM,Fourier transform infrared spectroscopy,Ultraviolet-visible spectroscopy and N2 adsorption-desorption.A comparative study on the catalytic performances of the Cu complexes encapsulated in the different zeolite-Y hosts was carried out with different substrates.The results show that the hierarchical zeolite-Y exhibites superior host performance to the conventional zeolite-Y,and Cu complexes encapsulated in hierarchical zeolite-Y has higher catalytic activities in various cycloalkane oxidation reactions than those in the conventional zeolite-Y using H2O2 as the oxidant.In addition,Cu complexes encapsulated in the hierarchical zeolite-Y exhibites the same stability and reusability as those in the conventional zeolite-Y.%选用常规Y沸石和经后处理法制备的多级孔Y沸石为主体,采用自由配体法将铜菲咯啉(CuPhen)配合物封装在不同Y沸石中,制备了CuPhen/Y复合催化材料.采用X射线衍射、TEM、紫外-可见光谱、N2吸附-脱附、ICP和TG等手段对所制备复合催化材料的物化性质进行了较为详细的表征,并对封装在不同Y沸石主体中的铜配合物在不同尺寸大小反应底物中的催化氧化性能进行了比较研究.结果表明,在以双氧水为氧化剂的反应体系中,封装于多级孔Y沸石中的铜配合物在不同环烷烃氧化反应中的催化活性均高于封装在常规Y沸石中的催化活性,体现出多级孔Y沸石更为优越的主体性能.此外,同封装于常规Y沸石中的铜配合物一样,封装在多级孔Y沸石主体中的金属配合物催化剂也具有良好的稳定性.