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Boreskov Institute of Catalysis of the Siberian Branch of Russian ...

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PP-IV-24ONE-STAGE CATALYTIC CONVERSION OF NATURAL GASTO LIQUID PRODUCTSA.V. Vosmerikov 1 , L.N. Vosmerikova 1 , G.V. Echevskii 2 , L.L. Korobitsyna 11 <strong>Institute</strong> <strong>of</strong> Petroleum Chemistry, <strong>Siberian</strong> <strong>Branch</strong> <strong>of</strong> <strong>the</strong> <strong>Russian</strong> Academy <strong>of</strong> Sciences3, Akademichesky Avenue, 634021, Tomsk, Russia2 <strong>Boreskov</strong> <strong>Institute</strong> <strong>of</strong> <strong>Catalysis</strong>, <strong>Siberian</strong> <strong>Branch</strong> <strong>of</strong> <strong>the</strong> <strong>Russian</strong> Academy <strong>of</strong> Sciences5, Ak. Lavrentieva Avenue, 630090, Novosibirsk, Russiafax: (3822)491-457; e-mail: pika@ipc.tsc.ruNatural and associated gas, along with coal, oil and plant debris, has become <strong>the</strong> majorsource for <strong>the</strong> production <strong>of</strong> organic compounds [1]. Currently, most natural gas is used asfuel; its share in energy consumption is 24% [2]. The potentional value <strong>of</strong> natural gas is farhigher than a mere energy source. Natural gas can substitute for oil in <strong>the</strong> production <strong>of</strong> mostorganic compounds. Here, we report our studies <strong>of</strong> <strong>the</strong> catalytic properties <strong>of</strong> galliumcontainingzeolites, intercalated with gallium directly hydro<strong>the</strong>rmal syn<strong>the</strong>sis, in <strong>the</strong>conversion <strong>of</strong> natural gas to aromatic hydrocarbons.Galloaluminosilicates (Ga-AS) with silica ratios (M) from 30 to 80 were prepared by <strong>the</strong>isomorphic substitution <strong>of</strong> gallium (III) for silicon (IV) in <strong>the</strong> zeolite during hydro<strong>the</strong>rmalsyn<strong>the</strong>sis, via partially substituting gallium for aluminum ions in <strong>the</strong> precursor aluminosilicagel. The gallium oxide concentration in <strong>the</strong> sample was 1.2 or 2.2 wt %. The zeolitessyn<strong>the</strong>sized were converted to <strong>the</strong> H-form by double decationization with a 25% NH 4 Clsolution at 90 °C for 2 h; <strong>the</strong>y were dried at 110 °C for 8 h and calcined in air at 550 °C for 6 h.Natural gas had <strong>the</strong> following composition, wt %: methane, 81.60; ethane, 6.46; propane,7.40; butane, 4.04; and pentanes, 0.47. Conversion was carried out on a flow-through setupequipped with a silica glass reactor (14 mm in inner diameter) under <strong>the</strong> atmospheric pressureat <strong>the</strong> reaction temperature equal to 500-650 °C and <strong>the</strong> flow rate (W) equal to 1000 h –1 .Fig. 1 illustration <strong>the</strong> temperature effect on <strong>the</strong> product composition <strong>of</strong> natural gasconversion over <strong>the</strong> 2.2% Ga-AS (M = 60) catalyst at a gas flow rate <strong>of</strong> 1000 h –1 . The degree<strong>of</strong> natural gas conversion and aromatic hydrocarbon yield increased with rising temperature to600 °C; <strong>the</strong> benzene, naphthalene, and alkylnaphthalene concentrations in <strong>the</strong> productincreased, while <strong>the</strong> toluene concentration decreased. The highest selectivity <strong>of</strong> aromatichydrocarbons formation (71.9%) was achieved on <strong>the</strong> 2.2% Ga-AS (M = 60) sample at600 °C. The degree <strong>of</strong> natural gas conversion was 2.1% higher than for 1.2% Ga-AS (M = 30)sample under <strong>the</strong> same conditions.438

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