FIELD: chemistry.
SUBSTANCE: invention relates to petrochemistry and, more specifically, to a method for producing aromatic hydrocarbons by means of catalytic conversion of synthesis gas (a mixture of H2, CO and CO2), and can be used to produce aromatic hydrocarbons of the C6 to C11 fraction. Proposed according to the invention are three variants of producing HZSM-type zeolites using N1,N10-bis(2-hydroxyethyl)-N1,N1,N10,N10-tetramethyldecane-1,10-diammonium bromide producing a hybrid-type zeolite HZSM-5/HZSM-11; N1,N4-bis(2-hydroxyethyl)-N1,N1,N4,N4-tetramethylbutane-1,4-diammonium bromide producing an HZSM-12 zeolite; and N1,N6-bis(2-hydroxyethyl)-N1,N1,N6,N6-tetramethoxy-1,6-diammonium bromide producing a hybrid-type zeolite HZSM-5/HZSM-12, as templates, characterised by the Si/Al ratio of 100 to 104, the degree of crystallinity of 96 to 98%, the surface area of 274 to 298 m2/g and a pore volume of 0.21 to 0.24 cm3/g. The method for producing an HZSM-type zeolite includes the following stages: mixing aluminium, silicon and template compounds, sustaining the mixture to form a gel structure, crystallising the resulting gel, separating the crystalline product, removing the template by calcination, obtaining the NH4-form of a zeolite by conducting ion exchange, followed by isolating the resulting crystalline zeolite and converting to the H-form. Also proposed is a method for producing aromatic hydrocarbons of the C6 to C11 fraction, wherein a catalytic conversion of synthesis gas with a ratio of N2/CO equal to 1 to 2/1 mol/mol is executed at elevated pressure and temperature in the presence of a copper-zinc-aluminium catalyst K1 - MegaMax-507, separation of liquid reaction products with separation into a water condensate and liquid hydrocarbons containing aromatic hydrocarbons of the C6-C11 fraction. Additionally produced in the method is an HZSM-type zeolite , then a second zeolite catalyst K2 is obtained, containing the produced HZSM-type zeolite and aluminium oxide taken in a zeolite/Al2O3 ratio=70/30 wt./wt. The aromatic hydrocarbons are produced in one stage in a radial reactor for synthesis of aromatic hydrocarbons with a fixed layer of a composite catalyst produced by physical mixing of two components K1 and K2 in a K2/K1 ratio of 1 to 3/3 wt./wt., through which synthesis gas is passed in the flow mode at a pressure of 5 to 7 MPa.
EFFECT: simplification of the process, an increase in the selectivity of formation of aromatic hydrocarbons and the output of aromatic hydrocarbons of the C6 to C11 fraction relative to the initial carbon, as well as an opportunity to increase the productivity of the unit and to solve the problem of disposal of waste water and industrial waste by standard methods while implementing the proposed technology on an experimental industrial scale.
8 cl, 11 ex, 1 tbl, 5 dwg
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Authors
Dates
2021-08-12—Published
2020-09-17—Filed