A kind of multistage nano-reactor catalyst for directly preparing aromatic compounds from syngas and its preparation and application

An aromatic compound, nano-reactor technology, applied in the direction of carbon compound catalyst, catalyst activation/preparation, metal/metal oxide/metal hydroxide catalyst, etc., can solve the escape of intermediate products, uneven distribution, and final aromatics selection. To solve the problems of low methane selectivity and low yield, it can achieve the effect of low methane selectivity and high aromatics selectivity.

Active Publication Date: 2020-10-09
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 be activated and reacted 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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  • A kind of multistage nano-reactor catalyst for directly preparing aromatic compounds from syngas and its preparation and application
  • A kind of multistage nano-reactor catalyst for directly preparing aromatic compounds from syngas and its preparation and application
  • A kind of multistage nano-reactor catalyst for directly preparing aromatic compounds from syngas and its preparation and application

Examples

Experimental program
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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 impregnate the sample 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. Afte...

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 3 Coated samples. Then place the sample in a template containing tetrapropylammonium hydroxide template, tetraethyl orthosilicate, Al2 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%. Ca...

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 multi-level nano-reactor catalyst capable of directly converting synthesis gas into aromatics in one step, as well as its preparation and application. The catalyst consists of a core layer iron-based Fischer-Tropsch catalyst, a transition layer of porous oxide or porous carbon material and a molecular sieve shell layer with aromatization function. Among them, the shell molecular sieve can be further modified with metal elements or non-metal elements, and the outer surface of the molecular sieve can be further modified with silicon oxide compounds to adjust the acidic sites on the outer surface and the pore size of the molecular sieve, thereby inhibiting the formation of heavy aromatics. The preparation method of the multi-stage nanoreactor catalyst of the present invention can be obtained by the iron-based Fischer-Tropsch catalyst through multi-steps, and the molecular sieve containing the transition layer, the shell layer containing additives or no additives, and the shell layer containing surface modification or not containing . The catalyst can be used to directly prepare aromatic compounds, especially light aromatic compounds, from synthesis gas; the selectivity of light aromatics in hydrocarbons can reach more than 75%, and the content in liquid phase products is not less than 95%; the catalyst has good stability, It has 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 Patents(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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