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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Acknowledgments

The authors greatly thank the National Key Project for the 11th Five Year Plan (Grant No. 2006BAE02B00) and the Program of Introducing Talents of Discipline to Universities (B06006) for financial support.

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