4.8 Article

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

期刊

APPLIED CATALYSIS B-ENVIRONMENTAL
卷 134, 期 -, 页码 381-388

出版社

ELSEVIER
DOI: 10.1016/j.apcatb.2013.01.034

关键词

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

资金

  1. Program for New Century Excellent Talents in University [NCET-08-0799]
  2. Program for Changjiang Scholars and Innovative Research Team in University [IRT1070]
  3. Fundamental Research Funds for the Central Universities [GK201002043, 2010ZYGX013]

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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. (C) 2013 Elsevier B.V. All rights reserved.

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