Multistage nano-reactor catalyst for direct preparation of aromatic compounds from synthetic gas, and preparation method and application thereof

A technology of aromatic compounds and nano-reactors, applied in the direction of carbon compound catalysts, catalyst activation/preparation, metal/metal oxide/metal hydroxide catalysts, etc., can solve intermediate product escape, non-activation reaction, and final aromatics selection high aromatics selectivity and low methane selectivity

Active Publication Date: 2017-11-17
JIANGNAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] However, the use of direct composite catalysts for the direct production of aromatics from syngas still has certain limitations. For example, for intermediate products that are easy to undergo aromatization reactions, such as C2-C5, they still need to undergo several diffusions before entering the aromatization catalyst. At the same time, these intermediate products have the opportunity to escape; at the same time, after CO passes through the CO conversion catalyst, CO often cannot continue to activate and react on the second catalyst; in addition, the physical mixing method is easy to cause two The uneven distribution of active site concentration in the reaction system will affect the aromatization reaction of intermediate products to varying degrees
Due to the existence of these problems, the selectivity and yield of final aromatics are generally not high, especially light aromatics such as benzene, toluene and xylene

Method used

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  • Multistage nano-reactor catalyst for direct preparation of aromatic compounds from synthetic gas, and preparation method and application thereof
  • Multistage nano-reactor catalyst for direct preparation of aromatic compounds from synthetic gas, and preparation method and application thereof
  • Multistage nano-reactor catalyst for direct preparation of aromatic compounds from synthetic gas, and preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0025] Dissolve a certain amount of ferric nitrate and manganese nitrate in deionized water, use ammonia water as a precipitant to precipitate at pH = 8.0, age, filter, wash and dry at 120°C for 12 hours, and finally bake at 500°C for 5 hours A precipitated FeMn catalyst with an atomic ratio of iron to manganese of 96 to 4 was obtained. The prepared catalyst is impregnated in a certain amount of tetraethyl orthosilicate solution, and stirred continuously, and then the solvent is removed by rotary evaporation and dried and roasted to obtain SiO 2 Coated samples. Then the sample was impregnated in a template containing tetrapropylammonium hydroxide, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 In the solution of O, among which tetrapropyl ammonium hydroxide, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 The ratio of O is 0.3:1.0:0.03:0.015:130, stirred for 4 hours, then put into a hydrothermal kettle, sealed, heated to 180°C, and hydrothermally crystallized for 48 hours...

Embodiment 2

[0027] Get the precipitation type FeMn catalyst that makes in the last example, place in a certain amount of aluminum isopropoxide trihydrate and keep stirring, then rotary evaporation removes solvent and dry roasting, obtain the 2 o 3Coated samples. Then place the sample in a template containing tetrapropylammonium hydroxide template, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 In the solution of O, among which tetrapropyl ammonium hydroxide, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 The ratio of O is 0.3:1.0:0.03:0.015:130, stirred for 4 hours, then put into a hydrothermal kettle, sealed, heated to 180°C, and hydrothermally crystallized for 48 hours. After the crystallization was completed and cooled, the solid product was filtered, washed until the pH of the washing solution was 8, then dried at 120°C for 12 hours, and then calcined at 500°C for 5 hours to obtain a core layer with a weight fraction of 64% and a transition layer with a weight fraction of 8%. C...

Embodiment 3

[0029] Preparation of 20wt%Fe1wt%K / SiO by Equal Volume Impregnation Method 2 Supported iron-based catalysts. Finally, the sample is placed in a certain amount of aluminum isopropoxide trihydrate and stirred continuously, and then the solvent is removed by rotary evaporation and dried and roasted to obtain a 2 o 3 Coated samples. Then place the sample in a template containing tetrapropylammonium hydroxide template, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 In the solution of O, among which tetrapropyl ammonium hydroxide, tetraethyl orthosilicate, Al 2 o 3 , NaOH, H 2 The ratio of O is 0.3:1.0:0.05:0.010:130, stirred for 4 hours, then put into a hydrothermal kettle, sealed, heated to 180°C, and hydrothermally crystallized for 48 hours. After the crystallization was completed and cooled, the solid product was filtered, washed until the pH of the washing solution was 8, then dried at 120°C for 12 hours, and then calcined at 500°C for 5 hours to obtain a core layer wit...

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Abstract

The invention discloses a multistage nano-reactor catalyst for one-step direct preparation of aromatic hydrocarbons from synthetic gas, and a preparation method and an application thereof. The catalyst comprises a core layer iron-based Fischer-Tropsch catalyst, a porous oxide or porous carbon material transition layer and a molecular sieve shell layer having an aromatization function, wherein the shell layer molecular sieve can be further modified with a metal element or a nonmetal element, and the external surface of the molecular sieve is further modified with a silicon-oxygen compound to adjust the acidic site of the external surface and the aperture of the molecular sieve in order to inhibit the formation of heavy aromatic hydrocarbons. The preparation method of the multistage nano-reactor catalyst is characterized in that the transition shell layer can be prepared from the Fischer-Tropsch catalyst through multiple steps, the shell layer contains or does not contain an assistant, and the shell layer molecular sieve undergoes or does not undergo surface modification. The catalyst can be used for the direct preparation of the aromatic compounds, especially lightweight aromatic hydrocarbons, from the synthetic gas; the selectivity of the lightweight aromatic hydrocarbons in the hydrocarbons can reach 75% or more, and the content of the aromatic hydrocarbons aromatic hydrocarbons in a liquid phase product is not less than 95%; and the catalyst has a good stability and has a very good industrial application prospect.

Description

technical field [0001] The invention belongs to the technical field of synthesis gas conversion, and relates to a catalyst for directly producing aromatic compounds from synthesis gas through a Fischer-Tropsch synthesis route, as well as its preparation and application. Background technique [0002] Aromatic compounds including benzene, toluene and xylene (BTX) are important chemical basic raw materials, which are mainly derived from petroleum-based production processes, such as naphtha steam cracking for ethylene production and catalysis for gasoline and diesel production reforming or cracking. With the lightening of olefin raw materials, the reduction of crude oil resources and the increasingly prominent environmental problems, it is challenging and unsustainable to obtain aromatic compounds from petroleum routes. Therefore, more and more attention has been paid to the production of aromatics from non-petroleum routes. Based on my country's energy structure rich in coal ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/072B01J29/076B01J23/78B01J23/889C07C1/04C07C2/42C07C9/04C07C11/02C07C15/04C07C15/06C07C15/08
CPCB01J23/78B01J23/8892B01J29/072B01J29/076B01J35/0006B01J35/0073C07C1/044C07C2/42C07C2523/78C07C2523/889C07C2529/072C07C2529/076B01J2229/20C07C9/04C07C11/02C07C15/04C07C15/06C07C15/08C07C2523/04C07C2523/34C07C2523/745C07C2529/06C07C1/0445C07C2521/04C07C2521/08B01J35/0086B01J37/0203C07C15/067B01J37/0205B01J37/0236B01J37/06B01J21/08B01J21/04B01J29/064B01J37/031B01J37/024B01J37/0018B01J37/08B01J37/30B01J2229/186Y02P20/52
Inventor 刘小浩胥月兵姜枫刘冰刘大鹏王廷
Owner JIANGNAN UNIV
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