Pd-Fe/α-Al<sub>2</sub>O<sub>3</sub>/cordierite monolithic catalysts for the synthesis of dimethyl oxalate: effects of calcination and structure

doi:10.1007/s11705-012-1212-6

Front Chem Sci Eng

2012, Vol. 6

Issue (3) : 259-269 https://doi.org/10.1007/s11705-012-1212-6

RESEARCH ARTICLE

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

Shengping WANG, Xin ZHANG, Yujun ZHAO, Yadong GE, Jing LV, Baowei WANG, Xinbin MA(

)

Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China

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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

Corresponding Author(s): MA Xinbin,Email:xbma@tju.edu.cn

Issue Date: 05 September 2012

Cite this article:

Yujun ZHAO,Yadong GE,Jing LV, et al. Pd-Fe/α-Al₂O₃/cordierite monolithic catalysts for the synthesis of dimethyl oxalate: effects of calcination and structure[J]. Front Chem Sci Eng, 2012, 6(3): 259-269.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-012-1212-6
https://academic.hep.com.cn/fcse/EN/Y2012/V6/I3/259

Fig.1 Thermal decompositions of (a) PdCl, (b) PdCl-FeCl/α-AlO, (c) FeCl?6HO

Fig.2 TPR tests of Pd/α-AlO, Fe/α-AlO and Pd-Fe/α-AlO calcined at 473 K

Fig.3 TPR tests of Pd-Fe/α-AlO catalysts calcined at (a) 393 K, (b) 473 K, (c) 573 K, (d) 673 K, (e) 773 K, and (f) 873 K

Fig.4 TEM images of Pd-Fe/α-AlO/cordierite monolithic catalyst calcined at (a) 393 K, (b) 473 K, (c) 573 K, (d) 673 K, (e) 773 K, and (f) 873 K

Fig.5 Particle size distribution of Pd-Fe/α-AlO/cordierite monolithic catalyst calcined at (a) 393 K, (b) 473 K, (c) 573 K, (d) 673 K, (e) 773 K, and (f) 873 K

Tab.1 Performance of the catalysts calcined at different temperatures for CO coupling to dimethyl oxalate

Fig.6 DRIFT spectra of CO adsorbed on Pd-Fe/α-AlO/cordierite monolithic catalysts calcined at (a) 393 K, (b) 473 K, (c) 573 K, (d) 673 K, (e) 773 K, and (f) 873 K

Tab.2 Pore-structure properties of different α-AlO support samples

Fig.7 SEM images and element profiles in cross-section of the monolithic catalyst (a, b) and the granule catalyst (c, d)

Fig.8 TEM images of the monolithic and granule Pd-Fe/α-AlO catalysts obtained after calcination at 473 K

Fig.9 XRD patterns of the monolithic and granule Pd-Fe/α-AlO catalysts

Tab.3 Comparison of the catalytic performance of the monolithic and granule catalysts

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