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mcm‑22/zsm‑5 in-situ symbiotic methanol aromatization catalyst and preparation method thereof

A technology of MCM-22 and ZSM-5, which is applied in the field of methanol-to-aromatic catalysts, can solve the problems of low aromatization yield, achieve the effects of increasing relative content, suppressing hydrogen transfer and carbon deposition, and good technical effects

Active Publication Date: 2017-07-14
CHINA PETROLEUM & CHEM CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0010] One of the technical problems to be solved by the present invention is the technical problem of low aromatization yield in the methanol aromatization fluidized bed catalyst composition prepared by the prior art

Method used

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  • mcm‑22/zsm‑5 in-situ symbiotic methanol aromatization catalyst and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0029] Put 140 grams of kaolin (55.3% SiO 2 , 42.5% Al 2 O 3 , 2.2% other oxides), 40 grams of ZSM-5 molecular sieve (the molar ratio of silica to alumina is 400), 50 grams of silica sol (40% SiO 2 ) And 370 grams of water are mixed uniformly, spray molded to obtain 20~200μm pellets, and calcined at 900℃ for 4 hours to obtain spray microspheres ZQ1 with particle size of 10~200μm.

[0030] Take 100 grams of spray microspheres ZQ1, 0.65 grams of sodium hydroxide, 0.63 grams of aluminum nitrate, 1.7 grams of hexamethyleneimine and 500 grams of water and mix them evenly (in the composition of this mixture, the silicon oxide in the kaolin is removed, and the remaining raw materials are The ratio of silica to alumina is 200), transferred to a closed reactor and crystallized at 120°C for 120 hours. After crystallization, the product was washed, dried at 120°C for 4 hours, and calcined at 550°C for 8 hours to obtain sodium molecular sieve microspheres MZQ1. The sodium microspheres were e...

Embodiment 2

[0034] Combine 60 grams of kaolin, 120 grams of ZSM-5 molecular sieve (the molar ratio of silica to alumina is 75), and 20 grams of white carbon black (99.0% SiO 2 ) And 500 grams of water are mixed uniformly, spray molded to obtain 10~200μm pellets, calcined at 1000°C for 4 hours to obtain spray microspheres ZQ2 with particle size of 10~200μm.

[0035] Take 100 grams of spray microspheres ZQ2, 2.2 grams of sodium hydroxide, 2.96 grams of aluminum sulfate, 20 grams of hexamethyleneimine and 500 grams of water and mix them evenly (in the composition of this mixture, the silicon oxide in the kaolin is removed, and the remaining raw materials are The ratio of silica to alumina is 75), transferred to a closed reactor and crystallized at 120°C for 120 hours. After crystallization, the product was washed, dried at 120°C for 4 hours, and calcined at 550°C for 8 hours to obtain sodium molecular sieve microspheres MZQ1. The sodium microspheres were exchanged with 1 mol / L ammonium nitrate ...

Embodiment 3

[0038] Mix 40 grams of kaolin, 350 grams of silica sol, 20 grams of ZSM-5 molecular sieve (the molar ratio of silica to alumina is 20), and 300 grams of water, and spray them to obtain 10~200μm pellets, which are calcined at 950℃ Spray microspheres ZQ3 with a particle size of 10~200μm were obtained in 4 hours.

[0039] Take 100 grams of spray microspheres ZQ3, 51.6 grams of sodium hydroxide, 28.2 grams of aluminum chloride, 200 grams of hexamethyleneimine and 5000 grams of water and mix them evenly (in the composition of this mixture, remove the silicon oxide in the kaolin, and the remaining raw materials The ratio of silica to alumina is 20), transferred to a closed reactor and crystallized at 120°C for 120 hours. After crystallization, the product was washed, dried at 120°C for 4 hours, and calcined at 550°C for 8 hours to obtain sodium molecular sieve microspheres MZQ1. The sodium type microspheres were exchanged with 1 mol / L ammonium nitrate solution, washed, dried at 120°C ...

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Abstract

The invention relates to an MCM-22 / ZSM-5 in-situ intergrowth methanol aromatization catalyst and a preparation method of the MCM-22 / ZSM-5 in-situ intergrowth methanol aromatization catalyst, aiming at solving the technical problems that the existing fluidized bed catalyst has low aromatic hydrocarbon yield when used for methanol aromatization. The MCM-22 / ZSM-5 in-situ intergrowth methanol aromatization catalyst is prepared from the following components: (a) 0.5-10.0 parts of at least one of ZnO or Ga2O3; (b) 0.5-10.0 parts of oxides of at least one of P, Fe or Mn; (c) 80.0-99.0 parts of 10-200mum microspheres for in-situ synthesis of MCM-22 / ZSM-5 in-situ intergrowth molecular sieve. The MCM-22 / ZSM-5 in-situ intergrowth methyl alcohol aromatization catalyst can solve the problem and can be used for industrial production of aromatics prepared by methanol.

Description

Technical field [0001] The invention relates to a methanol-to-aromatics catalyst synthesized by in-situ technology, in particular to a MCM-22 / ZSM-5 in-situ symbiosis molecular sieve-based, methanol-to-aromatics fluidized bed catalyst. Background technique [0002] Aromatics (where benzene, toluene and xylene are called B, T and X respectively, and the three are collectively called BTX) are important basic organic chemical raw materials. Aromatics are mainly derived from catalytic reforming and steam cracking by-product pyrolysis gasoline (close to 90%)-petroleum route, only about 10% from coal route. From the perspective of energy distribution, my country is short of oil and gas but rich in coal, and its dependence on external crude oil has exceeded 50%, which has threatened national energy security. In addition, the depletion of oil resources and the long-term high and volatility of oil prices have made the energy and chemical industries based on oil routes face unprecedented c...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J29/00C07C1/20C07C15/02
CPCY02P20/52
Inventor 汪哲明周伟张铁柱
Owner CHINA PETROLEUM & CHEM CORP