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Catalyst for methane oxyhalogenation conversion as well as preparation method and application of catalyst

A methane halide oxidation and catalyst technology, which is applied in the field of methane halide oxidation conversion catalyst and its preparation, can solve the problems of low yield of methyl halide, reduction of selectivity of methyl halide, etc.

Active Publication Date: 2018-05-25
FUSHUN RES INST OF PETROLEUM & PETROCHEMICALS SINOPEC CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0009] The methane halogen oxidation reaction in the prior art has the following technical problems. High temperature is beneficial to improve the conversion rate of methane, but it will cause deep oxidation of the generated methyl halides, especially monohalomethanes, to generate CO or CO 2 , which significantly reduces the selectivity of methyl halides, resulting in low yields of methyl halides. Therefore, it is of great significance to develop a catalyst for the methane halooxidation reaction with high methane conversion and selectivity of methyl halides.

Method used

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  • Catalyst for methane oxyhalogenation conversion as well as preparation method and application of catalyst

Examples

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Effect test

Embodiment 1

[0022] Prepare aluminum hydroxide slurry by hydrolysis of aluminum isopropoxide: mix water and aluminum isopropoxide at a molar ratio of 120:1, control the hydrolysis temperature at 80°C-85°C, hydrolyze aluminum isopropoxide for 1.5h, and then carry out aging , the aging temperature was controlled at 90°C-95°C, the aging time was 18h, and an aluminum hydroxide slurry with a solid content of 21.3wt% was obtained.

[0023] Preparation of zinc-containing silicon oxide: using equal volume impregnation method on silicon oxide (commercially available, the properties are as follows: specific surface 335m 2 / g, pore volume is 0.86ml / g) impregnated with zinc nitrate solution, dried and roasted after impregnation, the drying time is 2 hours, and the drying temperature is 130°C; the roasting time is 4 hours, the temperature is 400°C, the containing Zinc silicon oxide is spherical, and the equivalent diameter of silicon oxide containing zinc is 2mm;

[0024] Spray immersion process: mix ...

Embodiment 2

[0028] Prepare aluminum hydroxide slurry by hydrolysis of aluminum isopropoxide: mix water and aluminum isopropoxide at a molar ratio of 120:1, control the hydrolysis temperature at 80°C-85°C, hydrolyze aluminum isopropoxide for 1.5h, and then carry out aging , the aging temperature was controlled at 90°C-95°C, the aging time was 18h, and an aluminum hydroxide slurry with a solid content of 21.3wt% was obtained.

[0029] Preparation of zinc-containing silicon oxide: using equal volume impregnation method on silicon oxide (commercially available, the properties are as follows: specific surface 335m 2 / g, pore volume is 0.86ml / g) impregnated with zinc sulfate solution, dried and roasted after impregnation, the drying time is 3 hours, and the drying temperature is 120°C; the roasting time is 5 hours, the temperature is 450°C, the containing Zinc silicon oxide is spherical, and the equivalent diameter of silicon oxide containing zinc is 2mm;

[0030] Spray immersion process: mix ...

Embodiment 3

[0034] Prepare aluminum hydroxide slurry by hydrolysis of aluminum isopropoxide: mix water and aluminum isopropoxide at a molar ratio of 120:1, control the hydrolysis temperature at 80°C-85°C, hydrolyze aluminum isopropoxide for 1.5h, and then carry out aging , the aging temperature was controlled at 90°C-95°C, the aging time was 18h, and an aluminum hydroxide slurry with a solid content of 21.3wt% was obtained.

[0035] Preparation of zinc-containing silicon oxide: using equal volume impregnation method on silicon oxide (commercially available, the properties are as follows: specific surface 335m 2 / g, pore volume is 0.86ml / g) impregnated with zinc bromide solution, dried and roasted after immersion, the drying time is 4h, and the drying temperature is 100°C; the roasting time is 4h, the temperature is 500°C, the Zinc-containing silicon oxide is spherical, and the equivalent diameter of zinc-containing silicon oxide is 3mm;

[0036] Spray immersion process: mix an appropriat...

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Abstract

The invention discloses a catalyst for methane oxyhalogenation conversion as well as a preparation method and an application of the catalyst. The catalyst is of a core-shell structure, wherein the core is zinc-containing silicon oxide, and the shell is alumina containing zirconium sulfate solid acid; the weight ratio of zinc-containing silicon oxide to alumina containing zirconium sulfate solid acid is 10:1-2:1; based on the weight of alumina containing zirconium sulfate solid acid as the baseline, the weight content of zirconium sulfate solid acid is 5wt%-10wt%; based on the weight of zinc-containing silicon oxide as the baseline, content of zinc in terms of oxide is 5wt%-30wt%. The catalyst has the advantages that methane conversion rate and selectivity of halomethane as a target productare increased simultaneously, deep oxidation of halomethane is inhibited, and yield of halomethane is increased obviously.

Description

technical field [0001] The invention relates to a methane halogen oxidation conversion catalyst and its preparation method and application, in particular to a low-temperature high activity and selective methane halogen oxidation conversion catalyst and its preparation method and application. Background technique [0002] Methane does not directly react with halogen, but uses HCl, HBr or metal halide as a halogen source, and the process of reacting with the participation of oxygen to form halide is called halogen oxidation reaction. This method was first applied to the industrial production of chlorine by catalytic oxidation of HCl, known as the Deacon process. [0003] The early methane halogen oxidation reaction mainly used HCl as the halogen source, and the catalyst mainly used CuCl 2 As the active component, Bromhead et al. (Bromhead J, Font-Freide J J, Westlake D J. Process for the production of methyl or ethyl mono-chloride or bromide. EP. Patent, 0117731.1984-09-05) l...

Claims

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Application Information

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IPC IPC(8): B01J27/053C07C19/075C07C17/35
CPCC07C17/35B01J27/053B01J35/51C07C19/075
Inventor 张信伟李杰尹泽群刘全杰倪向前
Owner FUSHUN RES INST OF PETROLEUM & PETROCHEMICALS SINOPEC CORP
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