Pd-Fe/α-Al₂O₃/cordierite monolithic catalysts for the synthesis of dimethyl oxalate: effects of calcination and structure

Abstract

Cordierite monoliths coated with Pd-Fe/α-Al₂O₃ catalysts were prepared at various calcination temperatures and characterized by thermogravimetry, temperature-programmed reduction, transmission electron microscopy, diffuse reflectance infrared Fourier transformation 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) (733 h^-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 α-Al₂O₃ washcoat which was accompanied with an even distribution of the active component in the coating layer along the monoliths channels.

Keywords

dimethyl oxalate / coupling / Pd / cordierite / monolith / calcination / structure

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