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Applied Catalysis A: General 345 (2008) 43–50 Contents lists available at ScienceDirect Applied Catalysis A: General journal homepage: www.elsevier.com/locate/apcata Methanol to gasoline over zeolite H-ZSM-5: Improved catalyst performance by treatment with NaOH Morten Bjørgen a, Finn Joensen b, Martin Spangsberg Holm b, Unni Olsbye c, Karl-Petter Lillerud c, Stian Svelle c,* a Norwegian University of Science and Technology, Department of Chemistry, Høgskoleringen 5, N-7491 Trondheim, Norway b Haldor Topsøe, Nymøllevej 55, DK-2800 Lyngby, Denmark c Centre for Materials Science and Nanotechnology, Department of Chemistry, University of Oslo, P.O. Box 1033, Blindern, N-0315 Oslo, Norway ARTICLE INFO Article history: Received 4 December 2007 Received in revised form 16 April 2008 Accepted 16 April 2008 Available online 24 April 2008 Keywords: Zeolite Methanol ZSM-5 Desilication Post-synthesis Methanol to gasoline (MTG) Methanol to hydrocarbons (MTH) 1. Introduction The world depends heavily on fossil fuels for energy. About 80% of the worldwide energy consumption is derived from coal, oil, and natural gas. Of these three, oil is by far the largest contributor (35% from oil, 23% from coal, and 21% from gas). More than 95% of all transportation fuels are derived from petroleum, thereby con- suming more than 60% of all oil produced. Oil is also crucial for the production of a large variety of petrochemicals. Most estimates suggest that the overall reserves of fossil fuels will last from 200 to 300 years. However, the increasing energy demand can only be based so heavily on liquid petroleum for a few more decades (proven reserves of oil will last 40 years at present rate of consumption). Natural gas is more abundant, and the reserves will outlast those of oil (70 years at current consumption). The reserves of coal are even larger, representing about 170 years of supply at * Corresponding author. E-mail address: stian.svelle@kjemi.uio.no (S. Svelle). 0926-860X/$ – see front matter ß 2008 Elsevier B.V. All rights reserved. doi:10.1016/j.apcata.2008.04.020 ABSTRACT This work outlines how treatment of zeolite H-ZSM-5 (Si/Al = 46) with NaOH may improve the catalytic performance in the conversion of methanol to gasoline. The zeolite was treated with 0.05 or 0.20 M NaOH solution for 2 4 h at 75 8C. XRD confirmed the retention of crystallinity. The Si/Al ratio of the catalyst decreased as a consequence of the treatment, in particular for the more severely treated sample, but the total acidity determined by NH3-TPD was not altered, showing that the treated samples contain significant amounts of Al not giving rise to acidity. The BET surface area increased from 313 to 419 m2/g as a consequence of the desilication, and the N2 adsorption measurements indicated mesopore generation. Diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) indicated presence of Lewis acidity in the treated samples. Methanol conversion was carried out in a fixed bed reactor at 370 8C and WHSV = 8 g g1 h1. The catalyst lifetime, quantified as the total conversion capacity, increased by a factor of 3.3 as a consequence of the most severe treatment. The procedure led to a moderate increase in the initial activities. Further, the product selectivities were altered dramatically. The selectivity towards the gasoline fraction (C5+) was at best increased by a factor of 1.7. Hydrogen transfer reactions became faster and led to more aromatic and paraffinic compounds in the products. Increases in the propene/ ethene ratios were observed at moderate conversion. The results are well rationalized by alterations of acidic properties, mesopore formation, and improved diffusivity. ß 2008 Elsevier B.V. All rights reserved. the current rate of consumption. In addition, there are large reserves of unconventional oil sources, such as tar sands and oil shale [1]. Based on these perspectives, technologies for the upgrading of coal or gas into liquid fuels or petrochemical building blocks become highly attractive. Most such routes rely on transformation of the carbon source into synthesis gas (CO + H2). Synthesis gas may be converted into diesel fuels and waxes in what is known as the Fischer–Tropsch process. Alternatively, methanol may be produced from the synthesis gas. Methanol, in turn, may then be reacted into light alkenes for petrochemistry or high octane gasoline using acidic zeolite/zeotype catalysts. Hence, the con- version of methanol to gasoline (MTG) is complementary rather than a competitor to Fischer–Tropsch synthesis for the upgrading of coal or natural gas into liquid fuels. This report will focus on improved production of an aromatics rich C5+ hydrocarbon mixture suitable for blending into the gasoline pool from methanol over acidic zeolite catalysts. Mobil Oil was the first to discover and develop this zeolite- based methanol to hydrocarbons (MTH) technology, resulting inPDF Image | Methanol to gasoline over zeolite H-ZSM-5
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