Conversion of the Propane-Butane Fraction into Arenes on MFI Zeolites Modified by Zinc Oxide and Activated by Low-Temperature Plasma.

Abstract

The effect of modification of MFI zeolite 1–5 wt.% ZnO activated by plasma on acid and catalytic properties in the conversion of the propane–butane fraction into arenes was investigated. The high-silica zeolites with silicate module 45 were synthesized from alkaline alumina–silica gels in the presence of an ‘X-oil’ organic structure-forming additive. The modification of the zeolite with zinc was carried out by impregnating the zeolite granules in the H-form with an aqueous solution of Zn(NO3)2. The obtained zeolites were characterized by X-ray phase analysis and IR spectroscopy. It is shown that the synthesized zeolites belong to the high-silica MFI zeolites. The study of microporous zeolite-containing catalysts during the conversion of C3-C4 alkanes to aromatic hydrocarbons made it possible to establish that the highest yield of aromatic hydrocarbons is observed on zeolite catalysts modified with 1 and 3% ZnO and amount to 63.7 and 64.4% at 600 °C, respectively, which is 7.7–8.4% more than on the original zeolite. The preliminary activation of microporous zeolites modified with 1–5% ZnO and plasma leads to an increase in the yield of aromatic hydrocarbons from the propane–butane fraction; the maximum yield of arenes is observed in zeolite catalysts modified with 1 and 3% ZnO and activated by plasma, amounting to 64.9 and 65.5% at 600 °C, respectively, which is 8.9–9.5% more than on the initial zeolite. The activity of the zeolite catalysts modified by ZnO and activated by plasma show good agreement with their acid properties. Activation of the zeolites modified by 1 and 3% ZnO and plasma leads to an increase in the concentration of the weak acid sites of the catalyst to 707 and 764 mmol/g in comparison with plasma-inactivated 1 and 3% ZnO/ZKE-XM catalysts at 626 and 572 mmol/g, respectively.