One Pot Synthesis of Ultra-High Copper Contented Cu/SBA-15 Material as Excellent Catalyst in the Hydrogenation of Dimeth
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One Pot Synthesis of Ultra-High Copper Contented Cu/SBA-15 Material as Excellent Catalyst in the Hydrogenation of Dimethyl Oxalate to Ethylene Glycol Xiuying Guo Æ Anyuan Yin Æ Wei-Lin Dai Æ Kangnian Fan
Received: 15 April 2009 / Accepted: 27 May 2009 / Published online: 10 June 2009 Ó Springer Science+Business Media, LLC 2009
Abstract High copper contented mesoporous Cu/SBA-15 catalysts with high copper dispersion were successfully synthesized via the simple ammonia-driving depositionprecipitation method. The physicochemical properties of these Cu/SBA-15 catalysts have been studied through various characterization methods such as BET, XRD, SEM, TEM and TPR. The catalytic activities of these catalysts were determined on the hydrogenation of dimethyl oxalate (DMO) to ethylene glycol (EG) under gasphase fixed-bed conditions at high space-time yield. The results revealed that the high copper contented Cu/SBA-15 catalyst still has high specific area, proper pore volume and mesoporous structure, and the catalysts showed much high activities compared to the one prepared by impregnation method. This finding opens a new avenue for the selection of better catalyst for the hydrogenation of DMO to EG. Keywords Cu/SBA-15 Mesoporous material Ammonia-driving deposition-precipitation Hydrogenation Dimethyl oxalate Ethylene glycol
1 Introduction It is well known that mesoporous materials which possess high surface area, large pore volume, regular structure, uniform pore size distribution, and relative high thermal stability have drawn much attention in the field of separation, adsorption, and drug delivery [1–4]. Immobilization
X. Guo A. Yin W.-L. Dai (&) K. Fan Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, 200433 Shanghai, People’s Republic of China e-mail: [email protected]
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of nanoscopic materials in such high-surface area supports with improved catalytic activity and product selectivity is a task of great economic and environmental importance in the chemical and pharmaceutical industries. SBA-15, first synthesized by Zhao et. al. [5], is regarded as one of the most promising mesoporous materials because of its particular pore size (both mesoporous and microporous) and highly ordered two-dimensional hexagonal structure. Ethylene glycol (EG), an important chemical widely used in antifreeze and polyester manufacture, is universally produced from petroleum-derived ethylene via its epoxidation in the present industrial approach [6]. However, this process is greatly restricted by the dwindling petroleum resource. In this respect, the indirect synthesis of EG from syngas via the coupling of CO with nitrite esters to obtain oxalates and then hydrogenation of oxalates to EG has huge potential both in the economic and environmental persistent development [7, 8]. The indirect method provides an alternative route to sustainable production of EG. It is well-established that copper-containing catalysts have been of great interest due to their go
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