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

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

参考文献

[1] Zhao T J, Chen D, Dai Y C, Yuan W K, Holmen A. Synthesis of dimethyl oxalate from CO and CH₃ONO on carbon nanofiber supported palladium catalysts. Industrial & Engineering Chemistry Research, 2004, 43(16): 4595–4601

[2] Zhao X G, Lv X L, Zhao H G, Zhu Y Q, Xiao W D. Study on Pd/α-Al₂O₃ catalyst for vapor-phase coupling reaction of CO with CH₃ONO to (CH₃OOC)₂. Chinese Journal of Catalysis, 2004, 25(2): 125–128

[3] Jiang X Z, Su Y H, Lee B J, Chien S H. A study on the synthesis of diethyl oxalate over Pd/α-Al₂O₃ catalysts. Applied Catalysis A: General, 2001, 211(1): 47–51

[4] Lin Q, Ji Y, Jiang Z D, Xiao W D. Effects of precursors on preparation of Pd/α-alumina catalyst for synthesis of dimethyl oxalate. Industrial & Engineering Chemistry Research, 2007, 46(24): 7950–7954

[5] Zhao X G, Lin Q, Xiao W D.Characterization of Pd-CeO₂/α-alumina catalyst for synthesis of dimethyl oxalate. Applied Catalysis A: General, 2005, 284(1-2): 253–257

[6] Ji Y, Liu G, Li W, Xiao W. The mechanism of CO coupling reaction to form dimethyl oxalate over Pd/α-Al₂O₃. Journal of Molecular Catalysis A: Chemical, 2009, 314(1-2): 63–70

[7] Uchiumi S I, Ataka K, Matsuzaki T. Oxidative reactions by a palladium-alkyl nitrite system. Journal of Organometallic Chemistry, 1999, 576(1-2): 279–289

[8] Gao Z H, Liu Z C, He F, Xu G H. Combined XPS and in situ DRIRS study of mechanism of Pd-Fe/α-Al₂O₃ catalyzed CO coupling reaction to diethyl oxalate. Journal of Molecular Catalysis A: Chemical, 2005, 235(1): 143–149

[9] Ma X B, Xu G H, Chen J W, Chen H F. Kinetics of carbon monoxide catalytic coupling to diethyl oxalate in gaseous phase. Journal of Chemical Industry and Engineering (China), 1995, 46(1): 50–56 (In Chinese)

[10] Meng F D, Xu G H, Guo Q R. Kinetics of the catalytic coupling reaction of carbon monoxide to diethyl oxalate over Pd-Fe/α-Al₂O₃ catalyst. Journal of Molecular Catalysis A: Chemical, 2003, 201(1-2): 283–288

[11] Meng F D, Xu G H, Guo R Q, Yan H F, Chen M Q. Kinetic study of carbon monoxide coupling reaction over supported palladium catalyst. Chemical Engineering and Processing, 2004, 43(6): 785–790

[12] Xu G H, Ma X B, He F, Chen H F. Characteristics of catalyst for carbon monoxide coupling reaction. Industrial & Engineering Chemistry Research, 1995, 34(7): 2379–2382

[13] Wu D F, Jiang W, Zhou J C. Effect of drying and calcination on the toluene combustion activity of a monolithic CuMnAg/γ-Al₂O₃/cordierite catalyst. Journal of Chemical Technology and Biotechnology (Oxford, Oxfordshire), 2010, 85(4): 569–576

[14] Tsubota S, Nakamura T, Tanaka K, Haruta M. Effect of calcination temperature on the catalytic activity of Au colloids mechanically mixed with TiO₂ powder for CO oxidation. Catalysis Letters, 1998, 56(2): 131–135

[15] Agostini G, Pellegrini R, Leofanti G, Bertinetti L, Bertarione S, Groppo E, Zecchina A, Lamberti C. Determination of the particle size, available surface area, and nature of exposed sites for silica-alumina-supported Pd nanoparticles: a multitechnical approach. Journal of Physical Chemistry C, 2009, 113(24): 10485–10492

[16] Nijhuis T A, Kreutzer M T, Romijn A C J, Kapteijn F, Moulijn J A. Monolithic catalysts as efficient three-phase reactors. Chemical Engineering Science, 2001, 56(3): 823–829

[17] Nijhuis T A, Beers A E W, Vergunst T, Hoek I, Kapteijn F, Moulijn J A. Preparation of monolithic catalysts. Catalysis Reviews, 2001, 43(4): 345–380

[18] Heck R M, Gulati S, Farrauto R J. The application of monoliths for gas phase catalytic reactions. Chemical Engineering Journal, 2001, 82(1-3): 149–156

[19] Casanovas A, De Leitenburg C, Trovarelli A, Llorca J. Catalytic monoliths for ethanol steam reforming. Catalysis Today, 2008, 138(3-4): 187–192

[20] Zhao Y J, Zhou J, Zhang J G, Wang S D. Monolithic Ru-based catalyst for selective hydrogenation of benzene to cyclohexene. Catalysis Communications, 2008, 9(3): 459–464

[21] Zhao Y J, Zhou J, Zhang J G, Li D, Wang S D. Selective hydrogenation of benzene to cyclohexene on a Ru/Al₂O₃/cordierite monolithic catalyst: effect of mass transfer on the catalytic performance. Industrial & Engineering Chemistry Research, 2008, 47(14): 4641–4647

[22] Zhang J G, Li D F, Zhao Y J, Kong Q D, Wang S D A. Pd/Al₂O₃/cordierite monolithic catalyst for hydrogenation of 2-ethylanthraquinone. Catalysis Communications, 2008, 9(15): 2565–2569

[23] Neri G, Rizzo G, Corigliano F, Arrigo I, Caprì M, De Luca L, Modafferi V, Donato A. A novel Pt/zeolite-based honeycomb catalyst for selective CO oxidation in a H₂-rich mixture. Catalysis Today, 2009, 147S: S210–S214

[24] Yue H R, Zhao Y J, Zhao L, Lv J, Wang S P, Gong J L, Ma X B.Hydrogenation of dimethyl oxalate to ethylene glycol on a Cu/SiO₂/cordierite monolithic catalyst: enhanced internal mass transfer and stability. AIChE Journal, 2011,

[25] Gao X C, Zhao Y J, Wang S P, Yin Y L, Wang B W, Ma X B A. Pd-Fe/α-Al₂O₃/cordierite monolithic catalyst for CO coupling to oxalate. Chemical Engineering Science, 2011, 66(15): 3513–3522

[26] Leofanti G, Padovan M, Garilli M, Carmello D, Marra G L, Zecchina A, Spoto G, Bordiga S, Lamberti C. Alumina-supported copper chloride. 2 . Effect of aging and thermal treatments. Journal of Catalysis, 2000, 189(1): 105–116

[27] Leofanti G, Marsella A, Cremaschi B, Garilli M, Zecchina A, Spoto G, Bordiga S, Fisicaro P, Berlier G, Prestipino C, Casali G, Lamberti C. Alumina-supported copper chloride. 3. Effect of exposure to ethylene. Journal of Catalysis, 2001, 202(2): 279–295

[28] Leofanti G, Marsella A, Cremaschi B, Garilli M, Zecchina A, Spoto G, Bordiga S, Fisicaro P, Prestipino C, Villain F, Lamberti C. Alumina-supported copper chloride. 4.Effect of exposure to O₂ and HCl. Journal of Catalysis, 2002, 205(2): 375–381

[29] Prestipino C, Bordiga S, Lamberti C, Vidotto S, Garilli M, Cremaschi B, Marsella A, Leofanti G, Fisicaro P, Spoto G, Zecchina A. Structural determination of copper species on the alumina-supported copper chloride catalyst: a detailed EXAFS study. Journal of Physical Chemistry B, 2003, 107(21): 5022–5030

[30] Bartholomew C H. Mechanisms of catalyst deactivation. Applied Catalysis A: General, 2001, 212(1-2): 17–60

[31] Seshu Babu N, Lingaiah N, Vinod Kumar J, Sai Prasad P S. Studies on alumina supported Pd-Fe bimetallic catalysts prepared by deposition-precipitation method for hydrodechlorination of chlorobenzene. Applied Catalysis A: General, 2009, 367(1-2): 70–76

[32] Yue B H, Zhou R X, Wang Y J, Zheng X M. Study of the methane combustion and TPR/TPO properties of Pd/Ce-Zr-M/Al₂O₃ catalysts with M= Mg, Ca, Sr, Ba. Journal of Molecular Catalysis A: Chemical, 2005, 238(1-2): 241–249

[33] Wang C B, Lin H K, Ho C M. Effects of the addition of titania on the thermal characterization of alumina-supported palladium. Journal of Molecular Catalysis A: Chemical, 2002, 180(1-2): 285–291

[34] Bertarione S, Scarano D, Zecchina A, Johánek V, Hoffmann J, Schauermann S, Frank M M, Libuda J, Rupprechter G, Freund H J. Surface reactivity of Pd nanoparticles supported on polycrystalline substrates as compared to thin film model catalysts: infrared study of CO adsorption. Journal of Physical Chemistry B, 2004, 108(11): 3603–3613

[35] van der Eerden A M J, Visser T, Nijhuis T A, Ikeda Y, Lepage M, Koningsberger D C, Weckhuysen B M. Atomic XAFS as a tool to probe the electronic properties of supported noble metal nanoclusters. Journal of the American Chemical Society, 2005, 127(10): 3272–3273

[36] Groppo E, Bertarione S, Rotunno F, Agostini G, Scarano D, Pellegrini R, Leofanti G, Zecchina A, Lamberti C. Role of the support in determining the vibrational properties of carbonyls formed on Pd supported on SiO₂-Al₂O₃, Al₂O₃, and MgO. Journal of Physical Chemistry C, 2007, 111(19): 7021–7028

[37] Tüshaus M, Berndt W, Conrad H, Bradshaw A, Persson B. Understanding the structure of high coverage CO adlayers. Applied Physics A: Materials Science & Processing, 1990, 51(2): 91–98

[38] Szanyi J, Kuhn W K, Goodman D W. CO adsorption on Pd (111) and Pd (100): low and high pressure correlations. Journal of Vacuum Science & Technology. A, Vacuum, Surfaces, and Films, 1993, 11(4): 1969–1974

[39] Fukui K, Miyauchi H, Iwasawa Y. CO adsorption and oxidation on Pd (110)-c (2 × 4)-O by reflection-absorption infrared spectroscopy. Journal of Physical Chemistry, 1996, 100(48): 18795–18801

[40] Cook J C, Clowes S K, Mccash E M. Reflection absorption IR studies of vibrational energytransfer processes and adsorptionenergetics. Journal of the Chemical Society, Faraday Transactions, 1997, 93(13): 2315–2322

[41] Bourguignon B, Carrez S, Dragnea B, Dubost H. Vibrational spectroscopy of imperfect CO/Pd (111) surfaces obtained by adsorption between 150 and 230 K. Surface Science, 1998, 418(1): 171–180

[42] Giorgi J B, Schroeder T, Bäumer M, Freund H J. Study of CO adsorption on crystalline-silica-supported palladium particles. Surface Science, 2002, 498(1): L71–L77

[43] Sanchez-Escribano V, Arrighi L, Riani P, Marazza R, Busca G. Characterization of Pd-Cu alloy nanoparticles on γ-Al₂O₃-supported catalysts. Langmuir, 2006, 22(22): 9214–9219

[44] Sheu L L, Karpinski Z, Sachtler W M H. Effects of palladium particle size and palladium silicide formation on Fourier transform infrared spectra and carbon monoxide adsorbed on palladium/silicon dioxide catalysts. Journal of Physical Chemistry, 1989, 93(12): 4890–4894

[45] Zhao X G, Lin Q, Xiao W D. Characterization of Pd-CeO₂/α-alumina catalyst for synthesis of dimethyl oxalate. Applied Catalysis A: General, 2005, 284(1-2): 253–257

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.

版权

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