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Metal-modified MFI@MFI core-shell molecular sieve catalyst and preparation thereof

A technology of metal modification and molecular sieve, applied in the direction of molecular sieve catalysts, including molecular sieve catalysts, catalysts, etc., can solve the problems of short diffusion channels, high density of strong acids, and fast deactivation

Active Publication Date: 2020-03-17
DALIAN HAIXIN CHEM IND
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, hierarchical pore structure ZSM-5 molecular sieves, such as nanocrystalline stacked ZSM-5, nano-thin layer ZSM-5, small grain ZSM-5, etc., have a high external area, short diffusion channels and excellent diffusion properties. , which is conducive to the smooth progress of the reaction of methanol to propylene, but the outer surface of the hierarchical porous molecular sieve has a high density of strong acid, and carbon deposition occurs preferentially near the outer surface, resulting in faster deactivation

Method used

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  • Metal-modified MFI@MFI core-shell molecular sieve catalyst and preparation thereof
  • Metal-modified MFI@MFI core-shell molecular sieve catalyst and preparation thereof
  • Metal-modified MFI@MFI core-shell molecular sieve catalyst and preparation thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0065] 0.2g of Mn with a particle size of 20±10nm 2 o 3 Nano-metal oxides, 2g N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, 10g hydrogen silicon aluminum than 200 small grain ZSM-5 molecular sieves are put into 20g methanol, fully stirred for 3h, and then Transfer to a high-temperature-resistant stainless steel kettle, solvent heat treatment at 270°C for 12h, and then dry at 140°C for 10h to obtain Mn 2 o 3 Modified small grain ZSM-5 molecular sieve. Add 0.12 g boric acid, 12.18 g tetrapropylammonium hydroxide (25%), 47.82 g deionized water, 2.2 g Mn 2 o 3 Modified small-grain ZSM-5 molecular sieve, 20g of tetraethyl orthosilicate, stirred for 180min at a stirring rate of 180r / min, then transferred the prepared crystallization solution into a high-pressure stainless steel kettle, and crystallized at 180°C for 72h. The obtained product is suction filtered and dried to obtain catalyst powder. The obtained catalyst XRD pattern is as follows figure 1 As shown, the SEM ima...

Embodiment 2

[0067] 0.3g of MnO with a particle size of 30±10nm 2 Nano metal oxide (SEM image as image 3 Shown), 1g N-aminoethyl-3-aminopropylmethyldimethoxysilane, 10g hydrogen-type silicon aluminum ratio 300 nanometer thin layer ZSM-5 molecular sieve are put into 40g n-hexane, fully stirred for 2h, and then transferred to put into a high-temperature-resistant stainless steel kettle, solvent heat treatment at 220 ° C for 8 h, and then dry at 100 ° C for 20 h to obtain MnO 2 Modified nano thin layer ZSM-5 molecular sieve. Add 16.24g tetrapropylammonium hydroxide (25%), 36.62g deionized water, 3.2g MnO 2 Modified nano thin layer ZSM-5 molecular sieve, 20g of silica sol (SiO 2, 40%), stirred for 300min, and the stirring rate was 120r / min, then transferred the prepared crystallization solution into a high-pressure stainless steel kettle, crystallized at 170°C for 48h, and obtained the product through suction filtration and drying to obtain catalyst powder . The obtained catalyst XRD pat...

Embodiment 3

[0069] 0.4g of CeO with a particle size of 40±20nm 2 Nano-metal oxides, 1g N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, 10g hydrogen-type silicon aluminum ratio 400 nanocrystalline stacked ZSM-5 molecular sieves are put into 30g toluene, fully stirred for 4h, and then Transfer to a high-temperature resistant stainless steel kettle, solvent heat treatment at 210°C for 24h, and then dry at 120°C for 20h to obtain CeO 2 Modified nanocrystalline stacked ZSM-5 molecular sieve. Add 6.48g tetrapropylammonium bromide, 36.62g deionized water, 3g CeO to the beaker 2 Modified nanocrystalline stacked ZSM-5 molecular sieve and 10g of coarse-pore silica gel were stirred for 240min at a stirring rate of 360r / min, then the prepared crystallization solution was transferred to a high-pressure stainless steel kettle, and crystallized at 160°C for 96h to obtain The product is suction filtered and dried to obtain catalyst powder. The obtained catalyst XRD pattern is as follows figure 1 show...

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Abstract

The invention provides a metal-modified MFI@MFI core-shell molecular sieve catalyst and preparation thereof. The preparation method includes (1) subjecting a ZSM-5 molecular sieve to metal oxide modification by adopting a nano metal oxide and through a solvothermal method to obtain a modified ZSM-5 molecular sieve, with the metal being one of or a mixture of more selected from Mn, Ce, Fe, Co, Ni,La, Ga and W; (2) subjecting the modified ZSM-5 molecular sieve obtained in the step (1) to secondary hydro-thermal synthesis in a crystallization liquid of a Silicalite-1 molecular sieve or B-ZSM-5 molecular sieve to obtain the metal-modified MFI@MFI core-shell molecular sieve catalyst. The catalyst can greatly reduce the coking rate of a methanol-to-propylene reaction, and improve the propyleneselectivity and catalytic lifetime, and the modification effect is improved more than the traditional method.

Description

technical field [0001] The invention relates to the field of chemical industry, in particular to the field of catalysts for methanol-to-propylene production, and more specifically to a metal-modified MFI@MFI core-shell molecular sieve catalyst and its preparation. Background technique [0002] Propylene is an extremely important basic raw material in the field of petrochemical industry, and has a very wide range of uses, such as the production of polypropylene, acrylonitrile, butanol, propylene oxide and other products, and its world demand is growing rapidly. The traditional propylene production route is overly dependent on petroleum resources and cannot meet the global demand for propylene. Therefore, countries around the world have begun to devote themselves to the development of non-petroleum route to propylene technology. Among them, methanol-to-propylene (MTP) technology has received more and more attention. The raw material methanol comes from a wide range of sources....

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J29/40B01J29/46B01J29/48C07C1/20C07C11/06
CPCB01J29/48B01J29/405B01J29/46C07C1/20B01J2229/186C07C2529/40C07C2529/46C07C2529/48B01J35/396C07C11/06Y02P20/52
Inventor 孙玉坤刘亚圣翟岩亮
Owner DALIAN HAIXIN CHEM IND
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