Pd-Fe/a-AI203/cordierite monolithic catalysts for the synthesis of dimethyl oxalate： effects of calcination and structure  

作　　者：Shengping WANG Xin ZHANG Yujun ZHAO Yadong GE Jing LV Baowei WANG Xinbin MA 

机构地区：[1]Key Laboratory for Green Chemical Technology of Ministry of Education,School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China

出　　处：《Frontiers of Chemical Science and Engineering》2012年第3期259-269,共11页化学科学与工程前沿（英文版）

摘　　要：Cordierite monoliths coated with Pd-Fe/a- Al2O3 catalysts were prepared at various calcination temperatures and characterized by thermogravimetry, temperature-programmed reduction, transmission electron microscopy, diffuse reflectance infrared Fourier transfor- mation spectroscopy and X-ray diffraction. The performance of the catalytic monoliths for the synthesis of dimethyl oxalate （DMO） through a CO coupling reaction was evaluated. Monolithic catalysts with calcination temperatures ranging from 473 K to 673 K exhibited excellent dispersion of Pd, good CO adsorption properties, and excellent performance for the coupling reaction. The optimized monolithic catalyst exhibited a much higher Pd efficiency （denoted as DMO （g）.Pd （g）-1 h 1） （733h-1） than that of the granular catalyst （60.2 h-1）, which can be attributed to its honeycomb structure and the large pore sizes in the a-Al2O3 washcoat which was accompanied with an even distribution of the active component in the coating layer along the monoliths channels.Cordierite monoliths coated with Pd-Fe/a- Al2O3 catalysts were prepared at various calcination temperatures and characterized by thermogravimetry, temperature-programmed reduction, transmission electron microscopy, diffuse reflectance infrared Fourier transfor- mation spectroscopy and X-ray diffraction. The performance of the catalytic monoliths for the synthesis of dimethyl oxalate （DMO） through a CO coupling reaction was evaluated. Monolithic catalysts with calcination temperatures ranging from 473 K to 673 K exhibited excellent dispersion of Pd, good CO adsorption properties, and excellent performance for the coupling reaction. The optimized monolithic catalyst exhibited a much higher Pd efficiency （denoted as DMO （g）.Pd （g）-1 h 1） （733h-1） than that of the granular catalyst （60.2 h-1）, which can be attributed to its honeycomb structure and the large pore sizes in the a-Al2O3 washcoat which was accompanied with an even distribution of the active component in the coating layer along the monoliths channels.

关 键 词：dimethyl oxalate COUPLING PD cordierite monolith CALCINATION STRUCTURE 

分 类 号：TQ424.1[化学工程] O613.61[理学—无机化学]