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Catalyst for preparing higher olefins from methanol or/and dimethyl ether, preparation method and application

A high-carbon olefin and catalyst technology, applied in coal or/and natural gas chemical industry, can solve the problem of low selectivity of propylene

Active Publication Date: 2020-05-19
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the large pore diameter of this type of molecular sieve cannot limit the further reaction of propylene products, and propylene will further generate aromatics through polycondensation, aromatization and other reactions, resulting in low selectivity of propylene in the final product

Method used

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  • Catalyst for preparing higher olefins from methanol or/and dimethyl ether, preparation method and application
  • Catalyst for preparing higher olefins from methanol or/and dimethyl ether, preparation method and application

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0029] 12.62g tetraethylammonium hydroxide (35wt%) aqueous solution, 20.00g silica sol (30wt%), 2.00g aluminum sulfate, 1.60g sodium hydroxide and 22.80g deionized water are made into gel mixture, gel molar ratio 0.30TEAOH:1.00SiO 2 :0.03Al 2 o 3 :0.20Na 2 O:25.00H 2 O, the gel mixture was put into a stainless steel synthesis kettle, and hydrothermally crystallized at 140°C for 96 hours under rotating conditions; after crystallization, the solid product was centrifuged, washed with deionized water, and dried in an air atmosphere at 120°C to obtain SiO 2 / Al 2 o 3 Beta molecular sieve of 30.

[0030] 1.93g dimethylformamide, 6.66g silica sol, 0.006g sodium aluminate (Al 2 o 3 54.5wt%,Na 2 (041.0wt%), 0.76g sodium hydroxide and 4.33g deionized water according to molar ratio 0.80DMF:1.00SiO 2 :0.001Al 2 o 3 :0.30Na 2 O:15.00H 2 O, put the gel mixture into a stainless steel synthesis kettle, and age at 100°C for 12 hours to obtain the ZSM-23 molecular sieve precurso...

Embodiment 2

[0033] 21.00g of tetraethylammonium hydroxide, 6.0g of white carbon black, 0.26g of sodium aluminate, 0.66g of sodium hydroxide and 35.35g of deionized water were made into a gel mixture, and the gel molar ratio was 0.50TEAOH:1.00SiO 2 :0.014Al 2 o 3 :0.10Na 2 O:35H 2 O, the gel mixture was put into a stainless steel synthesis kettle, and hydrothermally crystallized at 160°C for 96 hours under rotating conditions; after crystallization, the solid product was centrifuged, washed with deionized water, and dried in an air atmosphere at 120°C to obtain SiO 2 / Al 2 o 3 60 Beta molecular sieve.

[0034] Mix 1.82g dimethylformamide, 5.00g silica sol, 0.002g sodium aluminate, 0.50g sodium hydroxide and 6.40g deionized water according to the molar ratio 1.00DMF:1.00SiO 2 :0.0005Al 2 o 3 :0.25Na 2 O:22.00H 2 O, put the gel mixture into a stainless steel synthesis kettle, and age at 80°C for 12 hours to obtain the ZSM-23 molecular sieve precursor; place 6.0g of Beta molecular s...

Embodiment 3

[0036] 10.50g of tetraethylammonium bromide, 20.83g of ethyl orthosilicate, 0.15g of pseudoboehmite, 3.20g of sodium hydroxide and 28.80g of deionized water were formulated into a gel mixture, and the gel molar ratio was 0.50TEABr :1.00SiO2 2 :0.010Al 2 o 3 :0.40Na 2 O:16.00H 2 O, the gel mixture was put into a stainless steel synthesis kettle, and hydrothermally crystallized at 140°C for 120 hours under rotating conditions; after crystallization, the solid product was centrifuged, washed with deionized water, and dried in an air atmosphere at 120°C to obtain SiO 2 / Al 2 o 3 90 Beta molecular sieve.

[0037] 0.35g of isopropylamine, 4.16g of ethyl orthosilicate, 0.0016g of aluminum sulfate, 0.896g of potassium hydroxide and 25.20g of deionized water according to the molar ratio 0.30IPA:1.00SiO 2 :0.000125Al 2 o 3 :0.40K 2 O:70.00H 2 O, put the gel mixture into a stainless steel synthesis kettle, and age at 90°C for 24 hours to obtain the ZSM-23 molecular sieve precu...

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Abstract

The invention provides a catalyst for preparing high-carbon olefins from methanol or / and dimethyl ether, a preparation method and application thereof. The catalyst is a core-shell type composite molecular sieve, which is characterized in that a Beta molecular sieve with a three-dimensional twelve-membered ring channel structure is used as a core, and a ZSM-23 molecular sieve with a one-dimensional ten-membered ring channel structure is used as a shell. The catalyst is used in the conversion of methanol or / and dimethyl ether to prepare high-carbon olefins, and the high selectivity of core phase molecular sieves for propylene and butene and the pore shape selection of shell phase molecular sieves can be used to improve the concentration of propylene and ethylene in the product. ratio, effectively inhibiting the diffusion of macromolecular aromatic products. The mass selectivity of propylene and butene in the non-aqueous product is greater than 80%, wherein the mass selectivity of propylene is greater than 50%, and the ratio of propylene to ethylene is higher than 15.

Description

technical field [0001] The invention relates to the field of coal or / and natural gas chemical industry, in particular to a catalyst for preparing high-carbon olefins from methanol or / and dimethyl ether, a preparation method and application thereof. Background technique [0002] In 1960, Weisz and Frilette first proposed the concept of shape-selective catalysis, and believed that molecular sieves with crystal structure had shape-selective catalysis. In the 1970s, Mobil Corporation of the United States developed ZSM-5 molecular sieves with two double ten-membered ring channel structures. Therefore, the shape-selective catalytic performance of molecular sieves has been rapidly developed. [0003] In 1976, Mobil Company first carried out the reaction of converting methanol into hydrocarbons on ZSM-5 molecular sieve catalyst. Since then, many research institutions and famous petrochemical companies at home and abroad have devoted themselves to the preparation of hydrocarbons fro...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/80C07C1/20C07C11/06C07C11/08
CPCB01J29/7007B01J29/7046B01J29/80C07C1/20C07C2529/70C07C2529/80C07C11/06C07C11/08Y02P20/52
Inventor 许磊袁扬扬
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI