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Method for preparing aromatic hydrocarbons through hydrogenation of carbon dioxide

A technology for carbon dioxide and aromatic hydrocarbons, which is applied in the production of hydrocarbons from carbon oxides, chemical instruments and methods, metal/metal oxide/metal hydroxide catalysts, etc. and high selectivity of methane, to achieve the effect of simple preparation method, good stability and simple reaction device

Active Publication Date: 2018-03-27
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI +1
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0005] The technical problem to be solved by the present invention is the low selectivity of aromatics in the prior art, the high selectivity of by-product CO and methane, and the high selectivity of CO and methane. 2 Problems such as low utilization rate, providing a new method for producing aromatics by hydrogenation of carbon dioxide

Method used

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  • Method for preparing aromatic hydrocarbons through hydrogenation of carbon dioxide
  • Method for preparing aromatic hydrocarbons through hydrogenation of carbon dioxide
  • Method for preparing aromatic hydrocarbons through hydrogenation of carbon dioxide

Examples

Experimental program
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Embodiment 1

[0039] 15.81g FeCl 3 ·6H 2 O and 6.27 g FeCl 2 4H 2 O was mixed with 80 mL of water to form an iron salt solution, and 3.5 mL of 9.0 mol / L HCl solution was added. Add about 180 mL of 1.5 mol / L NaOH solution at a constant speed at 60°C under stirring conditions. Within about 1.5 h, the pH of the solution was adjusted from acidic to about 10. After the dropwise addition, keep the temperature and continue stirring for 1 h, and finally cool to room temperature. After the reaction, the deposited product was separated by magnetic field adsorption, washed once with 400mL deionized water, and then dried at 60°C to obtain Na-Fe 3 o 4 Catalyst samples, the samples are prepared after grinding, tableting and sieving.

[0040] HMCM-22 (SiO 2 / Al 2 o 3 =30), silicon aluminum than SiO 2 / Al 2 o 3 HZSM-5 molecular sieves of 27, 50, 150, and 300, respectively, and HZSM-23 (SiO 2 / Al 2 o 3 =80) Molecular sieves were calcined at 500°C for 4 hours, and the samples were ground, pre...

Embodiment 2

[0048] Take respectively the Na-Fe prepared by the method of Example 1 according to different mass ratios 3 o 4 Catalyst and HZSM-5 (SiO 2 / Al 2 o 3 =150) Molecular sieve, composed of a granular mixed catalyst with a total mass of 1.0g, mixed uniformly and used for CO 2 hydrogenation reaction. Reduction conditions: under normal pressure, pure H 2 (25mL / min), the reduction time is 8h at 350°C. Reaction condition: H 2 / CO 2 =3.0, the temperature is 320°C, the pressure is 3.0MPa, and the space velocity is 4000mL / (h·g cat ), investigated the mass ratio of two components to Na-Fe 3 o 4 / HZSM-5 Catalyst CO 2 The impact of hydrogenation performance, the results (see Table 3) show that the composite catalyst has dual functionality, and there is a synergistic effect between the two components. As the ratio of the two components changes, when the ratio of the two components Fe / ZSM is 1:1, the composite The catalyst has the best performance and the highest selectivity for aro...

Embodiment 3

[0052] Weigh respectively the Na-Fe prepared by 0.5g embodiment 1 method 3 o 4 Catalyst and 0.5g HZSM-5 (SiO 2 / Al 2 o 3 =150) Molecular sieve particles are mixed evenly and used for CO 2 hydrogenation reaction. Reduction conditions: under normal pressure, pure H 2 (25mL / min), the reduction time is 8h at 350°C. Reaction condition: H 2 / CO 2 =3.0, the temperature is 280~380°C, the pressure is 3.0MPa, the space velocity is 2000mL / (h·g cat ), investigated the effect of reaction temperature on Na-Fe 3 o 4 / HZSM-5 Catalyst CO 2 The impact of hydrogenation performance, the results (see Table 4) show that as the reaction temperature increases, CO 2 The conversion rate increases gradually, C 5+The selectivity increased first and then decreased, and the catalyst consistently exhibited excellent CO 2 Aromatization properties.

[0053] Table 4 reaction temperature to Na-Fe 3 o 4 / HZSM-5(150) composite catalyst on CO 2 Effect of hydrogenation performance

[0054]

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Abstract

The invention provides a method for preparing aromatic hydrocarbons through hydrogenation of carbon dioxide. A gas mixture composed of carbon dioxide and hydrogen is directly converted under the catalysis of a multifunctional composite catalyst under the reaction conditions of a temperature of 250 to 450 DEG C, a pressure of 0.01 to 10.0 MPa, space velocity of 500 to 50000 mL / (h.g<cat>) and a H<2> / CO<2> mol ratio of 0.5 to 8.0 so as to produce the aromatic hydrocarbons. The composite catalyst is prepared by mixing a first component with a second component, wherein the first component is a Fe-based catalyst for preparation of low-carbon olefins through hydrogenation of carbon dioxide, and the second component is one or more than two selected from a group consisting of molecular sieves modified or unmodified by metals and mainly exerting aromatization effect on olefins. According to the method, the one-way CO2 conversion rate can reach 33% or above; the selectivity of hydrocarbon products can be controlled to be 80% or above; the content of methane in hydrocarbon products is lower than 8%; the content of C<5+> hydrocarbons is higher than 65%; and the aromatic hydrocarbons account for63% or more of the C<5+> hydrocarbons. The method opens up a novel route for production of aromatic hydrocarbons from carbon dioxide.

Description

technical field [0001] The invention relates to a method for producing aromatic hydrocarbons, in particular to a method for preparing aromatic hydrocarbons by hydrogenating carbon dioxide. Background technique [0002] As an important basic chemical raw material, aromatic hydrocarbons are mainly used in the production of chemical products such as chemical fibers, plastics and rubber. With the rapid development of the petrochemical and textile industries and the continuous development of the textile industry, the demand for aromatics is increasing worldwide. At present, the industrial production of aromatics mainly comes from petroleum and coal. The way of using petroleum as raw material includes the reforming process of refinery, the cracking of gasoline in ethylene production plant, and the disproportionation of toluene. The way of using coal as raw material mainly comes from coal coking. However, the reserves of fossil resources such as coal and petroleum are limited, so...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C07C15/04C07C15/06C07C15/073C07C15/08C07C15/02C07C1/12B01J29/46B01J29/76
CPCB01J29/46B01J29/7684B01J29/7692C07C1/12B01J2229/18B01J2229/20C07C15/04C07C15/06C07C15/073C07C15/08C07C15/02C07C2523/78C07C2529/40B01J37/03B01J37/088B01J29/40B01J29/7038B01J29/7046B01J23/745B01J29/7676B01J37/009B01J37/04C07C2523/745C07C2529/46C07C2529/48Y02P20/52C10G2/50B01J29/405B01J29/7088B01J37/06
Inventor 葛庆杰位健徐恒泳
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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