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Preparation of flaky HZSM-5 molecular sieve catalyst and application of flaky HZSM-5 molecular sieve catalyst in preparation of aromatic hydrocarbon through carbon dioxide hydrogenation

A molecular sieve and catalyst technology, which is applied in the field of industrial catalytic material preparation and CO2 conversion and utilization, can solve the problems of thick molecular sieve thickness, etc., and achieve the effects of large total acid content, inhibition of carbon deposition rate, and good catalytic activity.

Pending Publication Date: 2022-03-11
NORTHWEST NORMAL UNIVERSITY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

In recent years, although urea has been used as an additive to prepare sheet-shaped molecular sieves, the thickness of the synthesized molecular sieves is still relatively thick, and most of them are used in the reaction of syngas to aromatics

Method used

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  • Preparation of flaky HZSM-5 molecular sieve catalyst and application of flaky HZSM-5 molecular sieve catalyst in preparation of aromatic hydrocarbon through carbon dioxide hydrogenation
  • Preparation of flaky HZSM-5 molecular sieve catalyst and application of flaky HZSM-5 molecular sieve catalyst in preparation of aromatic hydrocarbon through carbon dioxide hydrogenation
  • Preparation of flaky HZSM-5 molecular sieve catalyst and application of flaky HZSM-5 molecular sieve catalyst in preparation of aromatic hydrocarbon through carbon dioxide hydrogenation

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0018] Preparation of Flake HZSM-5 Molecular Sieve: Raw Material Molar Ratio SiO 2 : Al 2 o 3 : TPAOH: Na 2 O: H 2 O: NH 4 F=1: 1 / 60: 0.4: 1 / 60: 35: 0.8. NaOH, C 9 h 21 AlO 3 , TPAOH and TEOS were added to deionized water, stirred at room temperature for pre-crystallization, and then stirred at 90 °C for 12 h. Then NH was added to the resulting mixed sol 4 F, and supplemented with volatile water, followed by vigorous stirring at 90°C for 12 h. Then the obtained solution was transferred to a polytetrafluoroethylene-lined stainless steel autoclave, crystallized at 170 °C for 72 h, cooled to room temperature, centrifugally washed with deionized water until neutral, dried at 100 °C for 6 h, and 550 °C. Calcined at ℃ for 6 h to prepare sheet-like HZSM-5 molecular sieves.

[0019] The prepared flake HZSM-5 molecular sieve and ZnO-ZrO 2 Mix and grind at a mass ratio of 1:2 for CO 2 In the process of producing aromatics by hydrogenation (reaction pressure: 3.0 MPa, reacti...

Embodiment 2

[0021] Preparation of Flake HZSM-5 Molecular Sieve: Raw Material Molar Ratio SiO 2 : Al 2 o 3 : TPAOH: Na 2 O: H 2 O: NH 4 F=1: 1 / 60: 0.4: 1 / 60: 35: 1.5. NaOH, C 9 h 21 AlO 3 , TPAOH and TEOS were added to deionized water, stirred at room temperature for pre-crystallization, and then stirred at 90 °C for 12 h. Then NH was added to the resulting mixed sol 4 F, and supplemented with volatile water, stirred vigorously at 90°C for 12 h. Then the obtained solution was transferred to a polytetrafluoroethylene-lined stainless steel autoclave, crystallized at 170 °C for 72 h, cooled to room temperature, centrifugally washed with deionized water until neutral, dried at 100 °C for 6 h, and roasted at 550 °C 6 h, the flake HZSM-5 molecular sieve was prepared.

[0022] The prepared flake HZSM-5 molecular sieve and ZnO-ZrO 2 Mix and grind at a mass ratio of 1:2 for CO 2 In the process of producing aromatics by hydrogenation (reaction pressure: 3.0 MPa, reaction temperature: 32...

Embodiment 3

[0024] Preparation of Flake HZSM-5 Molecular Sieve: Raw Material Molar Ratio SiO 2 : Al 2 o 3 : TPAOH: Na 2 O: H 2 O: NH 4 F=1: 1 / 60: 0.4: 1 / 60: 35: 2.6. Na 2 O, C 9 h 21 AlO 3 , TPAOH and TEOS were added to deionized water, stirred at room temperature for pre-crystallization, and then stirred at 90 °C for 12 h. Then NH was added to the resulting mixed sol 4 F, and supplemented with volatile water, stirred vigorously at 90°C for 12 h. Then the obtained solution was transferred to a polytetrafluoroethylene-lined stainless steel autoclave, crystallized at 170 °C for 72 h, cooled to room temperature, centrifugally washed with deionized water until neutral, dried at 100 °C for 6 h, and roasted at 550 °C 6 h, the flake HZSM-5 molecular sieve was prepared.

[0025] The prepared flake HZSM-5 molecular sieve and ZnO-ZrO 2 Mix and grind at a mass ratio of 1:2 for CO 2 In the process of producing aromatics by hydrogenation (reaction pressure: 3.0 MPa, reaction temperature:...

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Abstract

The invention provides preparation of a flaky HZSM-5 molecular sieve catalyst and application of the flaky HZSM-5 molecular sieve catalyst in preparation of aromatic hydrocarbon through carbon dioxide hydrogenation. According to the invention, accurate control of the synthesis thickness of the HZSM-5 molecular sieve is realized by adding the mineralizer NH4F and regulating the molar addition ratio of the urea to the NH4F. The flaky HZSM-5 molecular sieve prepared by the method is large in specific surface area and large in total acid content. In addition, due to the short b-axis length, material transmission and diffusion are facilitated, guest molecules can enter active sites more easily, side reactions are inhibited, and the catalytic activity is good. The ZnO-ZrO2 metal oxide prepared by a coprecipitation method is mechanically mixed with the flaky HZSM-5 prepared by the invention, the mixture is used in a reaction for preparing aromatic hydrocarbon by CO2 hydrogenation, and the catalyst not only has relatively high reaction activity, but also has relatively high aromatic hydrocarbon selectivity, and can inhibit the generation rate of carbon deposition and prolong the service life of the catalyst at the same time.

Description

technical field [0001] The invention belongs to the preparation of industrial catalytic materials and CO 2 The technical field of conversion and utilization relates to the preparation of a flake-shaped HZSM-5 molecular sieve catalyst and its application in hydrogenation of carbon dioxide to aromatics. Background technique [0002] CO 2 As a kind of greenhouse gas, it is constantly rising under the frequent human activities and the continuous consumption of fossil resources, breaking the earth's carbon cycle, causing a series of environmental problems such as climate warming and ocean acidification, and its pollution control is particularly important. Aromatics are one of the most important basic chemicals, especially benzene, toluene and xylene (BTX) are very important basic chemical raw materials, and have broad application prospects in industries such as medicine, leather, paint, fuel and explosives. Among them, CO 2 As an abundant carbon source, it can be directly conv...

Claims

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Application Information

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IPC IPC(8): B01J29/40C07C1/12C07C15/02
CPCB01J29/40C07C1/12C07C15/02Y02P20/52
Inventor 田海锋何环环查飞郭效军唐小华
Owner NORTHWEST NORMAL UNIVERSITY
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