Copper oxide catalyst for preparing isobutene through isobutane dehydrogenation and preparation method and application of copper oxide catalyst

A technology for producing isobutene and copper oxide, which is applied in the direction of physical/chemical process catalysts, catalyst carriers, chemical instruments and methods, etc., can solve problems that have not been reported in the literature, achieve low price, improve isobutane dehydrogenation performance, and high Yield effect

Inactive Publication Date: 2015-03-25
CHINA PETROLEUM & CHEM CORP +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0008] So far, there has been no literature report on the use of nitrogen-doped mesoporous carbon-supported copper oxide for the oxidative dehydrogenation of isobutane with carbon dioxide

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] Dissolve 1.82 g of copper acetate (0.01 mol) and 1.05 g of citric acid (0.005 mol) in 50 mL of water, and stir at room temperature to form a blue solution. Add nitrogen content of 3% to the above solution, with a specific surface area of ​​3200 m 2 / g, 38.98 g of nitrogen-doped nanotubes with a most probable pore diameter of 2.5 nm, dried at 60 °C with constant temperature stirring, and roasted at 550 °C for 5 hours in a nitrogen atmosphere to obtain a copper oxide catalyst supported by nitrogen-doped carbon nanotubes, Determination wherein the content of copper oxide is 3%.

[0025] The prepared nitrogen-doped carbon nanotube-supported copper oxide catalyst was loaded into a fixed-bed reactor, and a mixed gas of isobutane and carbon dioxide with a material ratio of 1:3 preheated to 330 ° C was introduced, and at 0.1 MPa, the space velocity is 5 L / (g cat h) and a reaction temperature of 580°C, the conversion rate of isobutane was measured to be 29.3% and the selectivit...

Embodiment 2

[0027] Dissolve 2.42 g of copper nitrate (0.01 mol) and 2.10 g of citric acid (0.01 mol) in 18 mL of water, and stir at room temperature to form a blue solution. Add nitrogen content of 12% and specific surface area of ​​2800 m to the above solution 2 / g, 15.11 g of nitrogen-doped nanotubes with a most probable pore diameter of 3.6 nm, dried at a constant temperature of 70 °C with stirring, and roasted at 600 °C for 4 hours in a nitrogen atmosphere to obtain a nitrogen-doped mesoporous carbon-supported copper oxide catalyst, Determination wherein the copper oxide mass percentage content is 5%.

[0028] The prepared nitrogen-doped carbon nanotube-supported copper oxide catalyst was loaded into a fixed-bed reactor, and a mixed gas of isobutane and carbon dioxide with a material ratio of 1:7 preheated to 400 ° C was introduced. MPa, the space velocity is 3 L / (g cat h) and a reaction temperature of 560°C, the conversion rate of isobutane was measured to be 25.7% and the selectivi...

Embodiment 3

[0030] Dissolve 1.78 g of copper sulfate (0.01 mol) and 4.20 g of citric acid (0.02 mol) in 9 mL of water, and stir at room temperature to form a blue solution. Add nitrogen content of 18% and specific surface area of ​​2700 m to the above solution 2 / g, 7.16 g of nitrogen-doped nanotubes with a most probable pore diameter of 3.9 nm, dried at 80°C with constant temperature stirring, and roasted at 600°C for 3 hours in a nitrogen atmosphere to obtain a copper oxide catalyst supported by nitrogen-doped carbon nanotubes, Determination wherein the content of copper oxide is 10%.

[0031] The prepared nitrogen-doped carbon nanotube-supported copper oxide catalyst was loaded into a fixed-bed reactor, and a mixed gas of isobutane and carbon dioxide with a material ratio of 1:8 preheated to 400 ° C was introduced. MPa, the space velocity is 5 L / (g cath) and a reaction temperature of 600°C, the conversion rate of isobutane was measured to be 45.6% and the selectivity of isobutene was ...

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Abstract

Provided is a copper oxide catalyst for preparing isobutene by isobutane dehydrogenation, which takes nitrogen doped mesoporous carbon as a carrier and comprises 2-20% by mass of copper oxide as an active component, preferably 5-15%, being balanced with nitrogen doped mesoporous carbon. The preparation method comprises the following steps: mixing a copper-containing compound and citric acid at a mol ratio of 1:0.5-1:3; dissolving by adding water to prepare a blue solution with the copper concentration of 0.2-2.2 mol/L; adding nitrogen doped mesoporous carbon at a ratio of 319-3898 grams of nitrogen doped mesoporous per mol of copper into the aqueous solution; stirring at a constant temperature, drying, and roasting; and to obtain obtaining the copper oxide catalyst. The catalyst is used for preparing isobutene by isobutane dehydrogenation through oxidation by carbon dioxide, the conversion rate of isobutane can reach 25-70%, and the selectivity of isobutene can reach 70-96%. The catalyst free of noble metal and highly toxic chromium metallic oxide is low in cost, environment-friendly, easy to prepare, and suitable for industrial production.

Description

technical field [0001] The invention relates to a catalyst for producing isobutene by dehydrogenating isobutane, in particular to a nitrogen-doped mesoporous carbon-supported copper oxide catalyst for producing isobutene by oxidizing isobutane with carbon dioxide and a preparation method and application thereof. Background technique [0002] Isobutylene is an important C4 compound, which can be used to synthesize polyisobutylene, butyl rubber, methacrylic acid, methyl tert-butyl ether and ethyl tert-butyl ether, etc. At present, isobutene is mainly derived from by-products in the production process of ethylene in industry. With the large-scale utilization of downstream products of isobutene, the contradiction of insufficient resources will become more prominent, and the production of isobutene from isobutane dehydrogenation is the most competitive technology to solve the shortage of isobutene. [0003] my country is rich in isobutane resources. The current catalytic crackin...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J27/24B01J32/00C07C11/09C07C5/42
Inventor 李泽壮刘经伟陈韶辉杨爱武柏基业李晓强刘丽娟王英武
Owner CHINA PETROLEUM & CHEM CORP
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