Magnesia modified H-ZSM-5 as an efficient acidic catalyst for steam reforming of dimethyl ether

作者：Long, Xu; Zhang, Qijian; Liu, Zhao-Tie; Qi, Ping; Lu, Jian; Liu, Zhong-Wen^*

来源：Applied Catalysis B: Environmental , 2013, 134: 381-388.

DOI：10.1016/j.apcatb.2013.01.034

• Hydrogen production
• Steam reforming
• Dimethyl ether
• Magnesia
• ZSM-5

To develop an efficient acidic catalyst for steam reforming of dimethyl ether (DME), H-ZSM-5 was modified with a series amount of MgO (0-8.16 wt.%) via the incipient impregnation method by using Mg(NO3)(2) as a precursor. Irrespective of the MgO loadings studied, it was highly dispersed over H-ZSM-5, and very limited impact on the structure and crystallinity of the zeolite was unambiguously revealed by the techniques of XRD, FT-IR, and N-2 adsorption at low temperatures. On the contrary, significant effects of MgO on the acidity of H-ZSM-5, especially the stronger acidic sites, were clearly manifested from the temperature-programmed desorption of ammonia (NH3-TPD). The amount of the stronger acidic sites was sharply decreased after loading 0.61 wt.% MgO on H-ZSM-5, and it was continuously decreased when the MgO loading was further increased until 8.16 wt.%. In contrast, the maximum amount of weaker acidic sites was observed between 1.41 and 2.92 wt.% MgO loaded samples. The MgO-modified H-ZSM-5 physically mixed with a commercial Cu/ZnO/Al2O3 was investigated as a bifunctional catalyst for steam reforming of DME (SRD). The reaction was performed in a fixed-bed reactor under the conditions of T = 290 degrees C, P=1 atm, and GHSV = 4000 h(-1). SRD results indicate that the DME conversion, H-2 yield, and selectivity of the carbon-containing products were strongly dependent on the MgO loadings over H-ZSM-5, and the highest H-2 yield of about 93% was achieved over the bifunctional catalyst by using 1.98 wt.% MgO modified H-ZSM-5 as a solid acid. Together with the reaction and characterization results of the Mg2+-exchanged H-ZSM-5, the property of the stronger acidic sites over the MgO-modified H-ZSM-5 was revealed to be a crucial factor in determining the SRD performance of the bifunctional catalyst. The simple impregnation procedure and the high efficiency in versatile tailoring the acidity make MgO-modified H-ZSM-5 a practical, highly efficient, and promising solid acid for hydrogen production via SRD.

• 出版日期2013-5-2
• 单位陕西师范大学; 辽宁工业大学