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Composite molecular sieve-based catalyst for methanol to gasoline and preparation method and application thereof

A compound molecular sieve and methanol-to-gasoline technology, which is applied in the direction of molecular sieve catalysts, physical/chemical process catalysts, chemical instruments and methods, etc., can solve the problems of limited technology popularization and application, no breakthrough progress, frequent regeneration, etc.

Inactive Publication Date: 2013-01-09
QINGDAO INST OF BIOENERGY & BIOPROCESS TECH CHINESE ACADEMY OF SCI
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  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although HZSM-5 exhibits high catalytic activity in the MTG reaction, its strong acidity leads to a high content of aromatics in the oil phase product, and it is easy to coke and requires frequent regeneration, which limits the popularization and application of the technology
In the past few decades, researchers have carried out a lot of researches on the modification of ZSM-5 molecular sieve, MTG technology, deactivation and regeneration of catalyst (CN 101186313A, CN87102695A, ZL 200610048299.3, CN 101016475A, CN 101104813A) and so on. research, but no breakthroughs have been made so far

Method used

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  • Composite molecular sieve-based catalyst for methanol to gasoline and preparation method and application thereof
  • Composite molecular sieve-based catalyst for methanol to gasoline and preparation method and application thereof

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Experimental program
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preparation example Construction

[0056] (1) Preparation of catalyst

[0057] The preparation method of the ZSM-5 / MCM-48 composite molecular sieve-based catalyst provided by the invention to prepare gasoline from methanol comprises the following steps in turn:

[0058] ① Dissolve tetrapropylammonium hydroxide and aluminum isopropoxide in deionized water, stir until clarified, then add tetraethyl orthosilicate and sodium hydroxide aqueous solution dropwise, put it into a hydrothermal reaction kettle, under autogenous pressure and crystallization Crystallization under hydrothermal conditions at a temperature of 60-140°C for 2-6 hours to prepare the ZSM-5 microporous molecular sieve precursor;

[0059] ②Mix the ZSM-5 microporous molecular sieve precursor with cetyltrimethylammonium bromide sodium hydroxide aqueous solution (pH = 12), stir, and move it into a hydrothermal reaction kettle. Crystallize under hydrothermal conditions at -200°C for 4-12 hours, filter, wash, dry at 90-120°C for 6-24 hours, and roast at...

Embodiment 1

[0066] The molar ratio of each raw material prepared by ZSM-5 / MCM-48 composite molecular sieve is: TPAOH: TEOS: CTAB: NaOH: Al: H 2 O=0.137:1:0.12:0.55:0.0127:118.

[0067] Mix 11.328g of template agent tetrapropylammonium hydroxide (TPAOH) aqueous solution with a mass concentration of 25% and 59.212g of deionized water, add 0.26g of aluminum isopropoxide to the above solution, stir at a constant temperature of 35°C until clear, dropwise Add 21.24g tetraethyl orthosilicate (TEOS), add 0.2g sodium hydroxide to the above solution, continue to stir for 4h, transfer to the reaction kettle, and crystallize at 100°C for 4h. After the crystallization is completed, the reactor is taken out and cooled to room temperature to obtain a ZSM-5 precursor solution.

[0068] 4.459g of template agent cetyltrimethylammonium bromide (CTAB) was dissolved in 149.08g of sodium hydroxide in an aqueous solution with a mass concentration of 0.96%, stirred at 28°C until clear, and added dropwise to the...

Embodiment 2

[0072] The molar ratio of each raw material prepared by ZSM-5 / MCM-48 composite molecular sieve is: n-butylamine: TEOS: CTAB: NaOH: Al: H 2 O=0.186:1:0.1:0.5:0.015:105.

[0073] 4.07g template agent n-butylamine (or ethylenediamine and ethylamine mixed in any molar ratio) aqueous solution with a mass concentration of 25% was mixed with 57.973g deionized water, 0.3064g aluminum isopropoxide was added to the above solution, 35 Stir at constant temperature at ℃ until clarification, add 21.24g tetraethyl orthosilicate (TEOS) dropwise, add 0.22g sodium hydroxide to the above solution, continue stirring for 2h, transfer to a reaction kettle for crystallization at 100°C for 6h. After the crystallization is completed, the reactor is taken out and cooled to room temperature to obtain a ZSM-5 precursor solution.

[0074] 3.72g of cetyltrimethylammonium bromide (CTAB) was dissolved in 133.54g of sodium hydroxide in an aqueous solution with a mass concentration of 1.34%, stirred at 32°C u...

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Abstract

A composite molecular sieve-based catalyst for methanol to gasoline is prepared by the following method: (a) template and aluminium source are dissolved in deionized water and stirred until the deionized water is clear, silicon source and alkali source are then dripped in, and after crystallization under the hydrothermal conditions of self-generated pressure and crystallization temperature, ZSM-5 molecular sieve precursor is prepared; (b) the ZSM-5 molecular sieve precursor and the alkali solution of cetyl trimethyl ammonium bromide as template are mixed, and after crystallization under the hydrothermal conditions of self-generated pressure and crystallization temperature and roasting, ZSM-5 / MCM-48 composite molecular sieve is prepared; (c) the ZSM-5 / MCM-48 composite molecular sieve and acid solution are subjected to ion exchange and are roasted, so that acidic HZSM-5 / MCM-48 composite molecular sieve is prepared; (d) the HZSM-5 / MCM-48 composite molecular sieve and binder are uniformly mixed, kneaded with nitric acid solution with volume concentration less than 10 percent to shape and roasted, so that the catalyst is prepared. The invention also discloses the preparation method for the catalyst.

Description

technical field [0001] The invention relates to a catalyst for methanol to gasoline. [0002] The present invention also relates to a method for preparing the above-mentioned catalyst. [0003] The invention also relates to the application of the above-mentioned catalyst in the methanol-to-gasoline reaction. Background technique [0004] my country's energy structure is characterized by rich coal, little oil, lack of gas, and relatively rich biomass resources. In recent years, the rising and uncertain international oil prices have had an important impact on my country's economy, and have also brought considerable pressure on my country's energy security. Liquid transportation fuels such as gasoline and diesel are imperative. Among the developed coal and biomass to liquid fuels (CTL&BTL) routes, methanol conversion to gasoline (MTG) technology is considered to be one of the most promising solutions to solve the current shortage of transportation fuels in my country. Especi...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/80C10G3/00
CPCY02P20/52Y02P30/20
Inventor 杨成焦雪静狄佐星宋建军李建青吴晋沪
Owner QINGDAO INST OF BIOENERGY & BIOPROCESS TECH CHINESE ACADEMY OF SCI
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