Methane Transformation using Light Gasoline as Co-Reactant over Zn/H-ZSM11
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Catalysis Letters Vol. 107, Nos. 1–2, February 2006 (Ó 2006) DOI: 10.1007/s10562-005-9738-6
Methane transformation using light gasoline as co-reactant over Zn/H-ZSM11 Oscar A. Anunziata* and Griselda Gonza´lez Mercado Grupo Fisicoquı´mica de Nuevos Materiales, Centro de Investigacio´n y Tecnologı´a Quı´mica (CITeQ), Universidad Tecnolo´gica Nacional, Facultad Regional Co´rdoba, Maestro Lo´pez esq. Cruz Roja, s/n, 5016, Co´rdoba, Argentina
Received 6 July 2005; accepted 17 November 2005
The catalytic conversion of methane (C1) to aromatic hydrocarbons (AH) such as benzene, toluene and xylenes (BTX) over a Zn/H-ZSM-11 catalyst using Light Gasoline (C5+C6) as co-reactant was studied. AH yields were as high as 30 %mol at 500 °C, w/f = 40 g h mol)1 at C1 molar fraction = 0.20. The contact time and time-on-stream effects on the product distribution, were analyzed in detail in order to obtain information about the evolution of different species. The C1 conversion reached 36 mol% C using Zn/HZSM-11 with content of 2.13 mol of Zn2+ per cell unit. KEY WORDS: Zn/HZSM-11; methane activation; light gasoline; co-reactant.
1. Introduction The dependence on oil last century is expected to be gradually offset in this century by increasing dependence on natural gas. Thus, it has been of considerable interest to convert natural gas into more commercially useful chemicals and liquid fuels. On the other hand, natural gas is currently being used for home and industrial heating as well as for the generation of electrical power. Moreover, the reserves are increasing more rapidly than those of liquid petroleum, and it is anticipated that this trend will extend into the 21st century. Methane (C1) is the principal component of most natural gas world reserves [1], consequently, its direct conversion is under extensive study but despite the enormous experimental efforts done, many aspects of that remain as challenging scientific and catalytic topics of ongoing discussion. The use of metal-exchanged zeolites, particularly exchanged Ga and Zn/H-zeolites, ZSM-5 and ZSM-11 [2–5] to catalyze dehydro-cyclo-dimerization reactions improves the selective conversion of light alkanes (C1– C4) to aromatics via non-oxidative routes. In 1993, Wang et al. [6] reported on the dehydro-aromatization of C1 under non-oxidizing conditions on H-ZSM5 catalyst modified with Mo and Zn, and denoted that benzene yield increases with the increasing of the C1 partial pressure. Previously, they [7] informed that adding an alkene in the feed as co-reactant, it plays a role of initiating species. Solymosi and Szo¨ke [8] reported high ethane (C2) conversion and benzene selectivity using * To whom correspondence should be addressed. E-mail: [email protected]
MoC/ZSM-5 at 700 °C. Considering this conclusions and taking account of the chemical similarity between ethane and methane Pierella et al. [9] studied C1 transformation over Mo-HZSM11 at lower temperature (500–600 °C). They used a mixture of C1 and C2+ as feed, obtaining a C1 conversion of 27% and a BTX (benzen
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