Method for catalytic oxidation of cyclohexane by using supported-type Au/C3N4@SBA-15 nano-catalyst

A C3N4SBA-15, nano-catalyst technology, applied in the field of chemistry and chemical industry, can solve the problems of harsh reaction conditions, low conversion rate, poor selectivity, etc., and achieve the effect of improving catalytic activity

Active Publication Date: 2016-06-08
ANHUI UNIVERSITY OF TECHNOLOGY
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The traditional cyclohexane oxidation process has problems such as low conversion rate (4%), poor selectivity (80%), harsh reaction conditions (>160°C), and serious environmental pollution. These shortcomings have always been the bottleneck restricting the development of the nylon fiber industry.
Gold catalysts show excellent performance in activating C–H bonds in the selective oxidation of alkanes with molecular oxygen as the oxidant, but the catalyst still exhibits a low conversion rate (9%). How to further improve the catalyst’s performance by proper modification Catalytic activity still key to current research

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0017] Catalyst preparation process

[0018] Weigh 0.1g of dicyandiamide and dissolve it in 70ml of distilled water, add 1g of SBA-15, sonicate for 2h, evaporate to dryness at 70°C, and dry. Nitrogen atmosphere temperature programming roasting, the rate of 2 ℃ / min increased to 550 ℃, stay 6h.

[0019] Put 0.5g of the modified SBA-15 carrier into the container, add 10.5ml2.42*10 -3 mol / L chloroauric acid solution, heated to 60°C, added a certain concentration of NaOH solution to adjust pH=6, and stirred for 2h. The catalyst is recorded as 1% Au / 0.1C 3 N 4 SBA-15, airtight storage.

[0020] oxidation reaction process

[0021] Put 30mg of the above catalyst into the reactor, add cyclohexane, raise the reactor to 130°C, and feed oxygen to 1.6MPa. After reacting for 3 hours, take out the product and analyze and measure that the conversion rate is 13.4%, and the selectivity is 91.1% %.

Embodiment 2

[0023] Catalyst preparation process

[0024] Weigh 0.8g of dicyandiamide and dissolve it in 70ml of distilled water, add 1g of SBA-15, sonicate for 2h, evaporate to dryness at 70°C, and dry. Nitrogen atmosphere temperature programming roasting, the rate of 4 ℃ / min increased to 700 ℃, stay 4h.

[0025] Put 0.5g of the modified SBA-15 carrier into the container, add 5.2ml2.42*10 -3 mol / L chloroauric acid solution, heated to 60°C, added a certain concentration of NaOH solution to adjust pH=6, and stirred for 2h. The catalyst is recorded as 0.5% Au / 0.8C 3 N 4 SBA-15, airtight storage.

[0026] oxidation reaction process

[0027] Put 30mg of the above catalyst into the reactor, add cyclohexane, raise the reactor to 150°C, and feed oxygen to 1.6MPa. After 36 minutes of reaction, the product was taken out for analysis and the conversion rate was 13.5%, and the selectivity was 90.2% %.

Embodiment 3

[0029] Catalyst preparation process

[0030] Weigh 0.6g of dicyandiamide and dissolve it in 70ml of distilled water, add 1g of SBA-15, ultrasonicate for 2h, evaporate to dryness at 70°C, and dry. Nitrogen atmosphere temperature programming roasting, the rate of 3 ℃ / min increased to 600 ℃, stay 5h.

[0031] Put 0.5g of the modified SBA-15 carrier into the container, add 1.1ml2.42*10 -3 mol / L chloroauric acid solution, heated to 60°C, added a certain concentration of NaOH solution to adjust the pH to 6, and stirred for 2 hours. The catalyst is recorded as 0.1% Au / 0.6C 3 N 4 SBA-15, airtight storage.

[0032] oxidation reaction process

[0033] Put 30mg of the above catalyst into the reactor, add cyclohexane, raise the reactor to 140°C, and feed oxygen to 1.5MPa. After reacting for 4h, take out the product and analyze and measure the conversion rate to be 14.1%, and the selectivity to be 91.4% %.

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PUM

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Abstract

The invention discloses a method for catalytic oxidation of cyclohexane by using a supported-type Au/C3N4@SBA-15 nano-catalyst, and belongs to the technical field of chemical engineering. The catalyst is prepared by the following steps: loading dicyandiamide on SBA-15 by an impregnation method, and roasting at certain temperature to prepare a C3N4@SBA-15 carrier; conducting effective loading of gold by an anion exchange method; and filtering, washing, drying and roasting. The method for catalytic oxidation of cyclohexane is as below: placing the prepared catalyst in a reactor, adding a certain amount of cyclohexane, heating the reactor to a certain temperature, introducing oxygen, rising to a certain pressure and maintaining for a period of time; and finally collecting the products and conducting gas chromatographic analysis. The cyclohexane oxidation reaction using the catalyst has selectivity on products cyclohexanol and cyclohexanone of above 90% and conversion rate of more than 13%, which are significantly better than those of an Au / SBA-15 catalyst.

Description

technical field [0001] The invention belongs to the technical field of chemistry and chemical engineering, and in particular relates to a loaded Au / C 3 N 4 SBA-15 nanocatalyst catalyzes the method of oxidizing cyclohexane. Background technique [0002] The selective oxidation of cyclohexane is an important industrial production process, and its target product is cyclohexanone. In fact, a mixture of cyclohexanone and cyclohexanol (commonly known as KA oil) is often obtained. Cyclohexanone is mainly used in the production of adipic acid and caprolactam, both of which are important organic chemical raw materials, widely used in medicine, paint, spices and other industries, and are monomers for the production of nylon 66 and nylon 6 respectively. The traditional cyclohexane oxidation process has problems such as low conversion rate (4%), poor selectivity (80%), harsh reaction conditions (>160°C), and serious environmental pollution. These shortcomings have always been the b...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C07C35/08C07C29/50C07C45/33C07C49/403B01J29/035B01J27/24
CPCB01J27/24B01J29/0354C07C29/50C07C45/33C07C35/08C07C49/403
Inventor 许立信姚芳金波李杰万超
Owner ANHUI UNIVERSITY OF TECHNOLOGY
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