Bimetallic MEL molecular sieve as well as preparation method and application thereof

A bimetallic and molecular sieve technology, applied in molecular sieve catalysts, chemical instruments and methods, catalyst activation/preparation, etc., can solve the problems of active and selective catalyst design and application, and achieve excellent catalytic performance, activity and selectivity Good, the effect of improving selectivity

Inactive Publication Date: 2019-12-13
GUANGDONG UNIV OF TECH
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  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0003] However, the activity and selectivity in the catalytic process has

Method used

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  • Bimetallic MEL molecular sieve as well as preparation method and application thereof
  • Bimetallic MEL molecular sieve as well as preparation method and application thereof
  • Bimetallic MEL molecular sieve as well as preparation method and application thereof

Examples

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Effect test

Embodiment 1

[0046] The present embodiment carries out the preparation of bimetallic MEL molecular sieve, comprises the following steps:

[0047] Weigh 16.22g of tetrabutylammonium hydroxide and place it in deionized water to obtain a 40wt% aqueous solution, slowly add 21.47g of tetrabutylammonium hydroxide under magnetic stirring, and add 38.87mL of deionized water after the solution is clarified to obtain a mixed solution; magnetic stirring After 6 hours, add 0.12 g of ferric citrate and 0.54 g of copper acetylacetonate to obtain the first product; after 8 hours of magnetic stirring, place the first product in a reaction kettle for hydrothermal crystallization at 170° C. for 72 hours; filter the crystallized product and use Repeated washing with deionized water and drying in a drying oven at 100°C for 12 hours to obtain the second product, namely all-silicon P-MEL@Cu / Fe molecular sieve; 0.015mol / L aluminum isopropoxide and 0.1mol / L tetrabutyl hydroxide were oxidized Ammonium is prepared ...

Embodiment 2

[0055] The present embodiment carries out the preparation of bimetallic MEL molecular sieve, comprises the following steps:

[0056] Weigh 16.22g of tetrabutylammonium hydroxide and place it in deionized water to obtain a 40wt% aqueous solution, slowly add 21.47g of tetrabutylammonium hydroxide under magnetic stirring, and add 38.87mL of deionized water after the solution is clarified to obtain a mixed solution; magnetic stirring After 6 hours, add 0.25 g of ferric citrate and 0.54 g of copper acetylacetonate to obtain the first product; after 8 hours of magnetic stirring, place the first product in a reaction kettle for hydrothermal crystallization at 170° C. for 72 hours; filter the crystallized product and use Repeated washing with deionized water and drying in a drying oven at 100°C for 12 hours to obtain the second product, namely all-silicon P-MEL@Cu / Fe molecular sieve; 0.015mol / L aluminum isopropoxide and 0.1mol / L tetrabutyl hydroxide were oxidized Ammonium is prepared ...

Embodiment 4

[0067] In this example, the catalytic performances of the bimetallic MEL molecular sieves of Examples 1-2, Fe metal MEL molecular sieves of Comparative Example 1 and bimetallic MEL molecular sieves of Comparative Example 2 were evaluated by Friedel-Crafts alkylation of trimethylbenzene and benzyl alcohol.

[0068] A three-neck round bottom flask equipped with a reflux condenser was tested for catalytic performance in a temperature-controlled oil bath. First, 40 mmol of mesitylene and 0.1 g of MEL molecular sieves were mixed and kept stirring at 100 ° C for 0.5 h, and then added 4mmol benzyl alcohol, with the addition time as the initial reaction time. Finally, the reaction solution was taken out to analyze the product by gas chromatography. The conversion ratio of benzyl alcohol and the selectivity of alkylation product are shown in Table 1, and Table 1 shows that the bimetallic MEL molecular sieve catalyst activity of the present invention and selectivity are better than only...

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Abstract

The invention belongs to the technical field of molecular sieve materials, and particularly relates to a bimetallic MEL molecular sieve as well as a preparation method and application thereof. The bimetallic MEL molecular sieve has mesopores and micropores, and Cu and Fe are loaded in the mesopores and the micropores; wherein the silica-alumina ratio of the bimetallic MEL molecular sieve is 48-50.The bimetallic MEL molecular sieve is an H-MEL@ Cu/Fe bimetallic molecular sieve catalyst; the bimetallic MEL molecular sieve is provided with the mesopores and micropores, and has hierarchical porestructure, Cu and Fe metals are not easy to leach in the molecular sieve skeleton; the bimetallic MEL molecular sieve can be used as a catalyst and can show excellent catalytic performance in a Friedel-Crafts alkylation reaction of trimethylbenzene and benzyl alcohol, and the Cu and Fe bimetallic synergistic effect can improve the alkylation activity and the selectivity, so that the application prospect of the molecular sieve catalyst in the field of chemical engineering is broadened.

Description

technical field [0001] The invention belongs to the technical field of molecular sieve materials, in particular to a bimetallic MEL molecular sieve and its preparation method and application. Background technique [0002] Friedel-Crafts alkylation is used in petrochemical processes to synthesize high-value diphenylmethane and diphenylmethane derivatives. Industrial applications usually use homogeneous catalysts. The inherent disadvantage of these homogeneous catalysts is their toxicity , difficult to separate and regenerate. Molecular sieves have the advantages of good hydrothermal stability, high specific surface area, adjustable acidity, easy recovery and regeneration, and no toxicity to the human body, so they have broad application prospects in Friedel-Crafts alkylation reactions. [0003] However, the activity and selectivity in the catalytic process has always been a difficult problem in the design and application of catalysts. Therefore, seeking a molecular sieve ca...

Claims

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Application Information

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IPC IPC(8): B01J29/03B01J29/88B01J37/10B01J35/10B01J37/08C07C2/86C07C15/16C01B39/06
CPCB01J37/0018B01J29/0333B01J29/0356B01J29/88B01J37/10B01J35/1057B01J35/1061B01J35/109C07C2/864C01B39/065B01J2229/18C01P2002/72C01P2004/03C01P2004/04C01P2002/85C01P2006/17C01P2006/16C07C15/16
Inventor 刘宝玉黄嘉晋廖展图
Owner GUANGDONG UNIV OF TECH
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