Composite double-layer catalyst and method for preparing ethylbenzene and/or propylbenzene through carbon dioxide/carbon monoxide hydrogenation coupling benzene alkylation

A composite double-layer, catalyst technology, applied in the direction of catalyst activation/preparation, chemical instruments and methods, molecular sieve catalysts, etc.

Active Publication Date: 2021-11-05
XIAMEN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0004] The above two kinds of raw materials ethylene and benzene are directly or indirectly derived from the exploitation and refining of petroleum resources, which will inevitably be limited by the adverse effects of the non-renewable nature of petroleum resources

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  • Composite double-layer catalyst and method for preparing ethylbenzene and/or propylbenzene through carbon dioxide/carbon monoxide hydrogenation coupling benzene alkylation
  • Composite double-layer catalyst and method for preparing ethylbenzene and/or propylbenzene through carbon dioxide/carbon monoxide hydrogenation coupling benzene alkylation

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preparation example Construction

[0039] In the present invention, the preparation method of the CHA molecular sieve preferably comprises the following steps:

[0040] Mixing silicon source, aluminum source, phosphorus source, template agent and polar solvent (hereinafter referred to as the second mixing) for hydrothermal reaction to obtain CHA molecular sieve precursor;

[0041] The CHA molecular sieve precursor is calcined (hereinafter referred to as the second calcination) to obtain the CHA molecular sieve.

[0042] In the invention, silicon source, aluminum source, phosphorus source, template agent and polar solvent are mixed for hydrothermal reaction to obtain CHA molecular sieve precursor. In the present invention, the silicon source is preferably one or more of silica sol, silicon dioxide, white carbon black, tetraethyl orthosilicate, tetrapropyl orthosilicate and water glass, more preferably silicon Sol or silicon dioxide, the silicon dioxide is preferably nano silicon dioxide, and the particle size o...

Embodiment 1

[0088] Ammonium carbonate aqueous solution is added dropwise in the mixed solution of zinc nitrate and zirconium nitrate (the molar concentration of zinc ion is 0.01mol / L, and the molar concentration of zirconium ion is 0.1mol / L), carries out co-precipitation reaction, after reaction finishes, After centrifuging and washing the solid product with deionized water until the washing liquid is neutral, put the solid product in an oven for drying at a drying temperature of 100°C. After drying to constant weight, the solid product is calcined at a temperature of 500 ℃, the holding time for calcination is 3h, and the heating rate from room temperature to the temperature of calcination is 5℃ / min to obtain ZnZrO x .

[0089] Silica sol, pseudoboehmite, phosphoric acid, tetraethylammonium hydroxide and deionized water are mixed for hydrothermal reaction, wherein tetraethylammonium hydroxide, silica sol (calculated as silicon dioxide), pseudoboehmite The molar ratio of bauxite (calculat...

Embodiment 2

[0094] Ammonium carbonate aqueous solution is added dropwise in the mixed solution of zinc nitrate and zirconium nitrate (the molar concentration of zinc ion is 0.01mol / L, and the molar concentration of zirconium ion is 0.1mol / L), carries out co-precipitation reaction, after reaction finishes, After centrifuging and washing the solid product with deionized water until the washing liquid is neutral, put the solid product in an oven for drying at a drying temperature of 100°C. After drying to constant weight, the solid product is calcined at a temperature of 500 ℃, the holding time for calcination is 3h, and the heating rate from room temperature to the temperature of calcination is 5℃ / min to obtain ZnZrO x .

[0095] Silica sol, pseudoboehmite, phosphoric acid, tetraethylammonium hydroxide and deionized water are mixed for hydrothermal reaction, wherein tetraethylammonium hydroxide, silica sol (calculated as silicon dioxide), pseudoboehmite The molar ratio of bauxite (calculat...

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Abstract

The invention belongs to the technical field of catalyst preparation, and particularly relates to a composite double-layer catalyst and a method for preparing ethylbenzene and / or propylbenzene through carbon dioxide / carbon monoxide hydrogenation coupling benzene alkylation. The invention provides a composite double-layer catalyst for preparing ethylbenzene and / or propylbenzene through CO2 / CO hydrogenation coupling benzene alkylation, the composite double-layer catalyst comprises a first-layer catalyst and a second-layer catalyst, the first-layer catalyst comprises a metal oxide catalyst and a CHA molecular sieve, the second-layer catalyst comprises an acidic molecular sieve, the acidic molecular sieve comprises an MFI molecular sieve or a phosphorus-modified MFI molecular sieve. The composite double-layer catalyst provided by the invention not only can be used for coupling low-carbon olefin prepared by CO2 / CO hydrogenation and ethylbenzene and / or propylbenzene prepared by alkylation of benzene and low-carbon olefin, but also has high content of the target product ethylbenzene and / or propylbenzene in aromatic hydrocarbon products.

Description

technical field [0001] The invention belongs to the technical field of catalyst preparation, and in particular relates to a method for preparing ethylbenzene and / or propylbenzene by composite double-layer catalyst, carbon dioxide / carbon monoxide hydrogenation coupling benzene alkylation. Background technique [0002] Ethylbenzene and propylbenzene are important petrochemical products, and 90% of their output is used to prepare styrene, which is then used to synthesize widely used polymer materials such as ABS plastics, polystyrene and styrene-butadiene rubber. [0003] At present, the industrial production routes of ethylbenzene and propylbenzene mainly include the following two types, taking the preparation of ethylbenzene as an example: first, ethylbenzene is produced by ethylating benzene and ethylene in MFI molecular sieves. However, the deep ethylation reaction of ethylbenzene is prone to produce diethylbenzene, and the catalyst is prone to deactivation due to carbon de...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/40B01J29/70B01J29/78B01J37/02C07C1/12C07C2/66C07C11/02C07C15/02C07C15/073C07C15/06
CPCB01J29/7065B01J29/783B01J37/0244B01J29/40C07C1/12C07C2/66B01J2229/37B01J2229/18C07C15/02C07C15/073C07C15/06C07C11/02Y02P20/52
Inventor 袁友珠左佳昌韩孝琴温丹璐谢亚飞叶林敏
Owner XIAMEN UNIV
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