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A metal-free hydrogenation catalyst and its application in catalyzing the hydrogenation reaction of 1,5-dinitronaphthalene

A hydrogenation catalyst and dinitronaphthalene technology are applied in physical/chemical process catalysts, preparation of organic compounds, organic chemistry, etc., and can solve the problems of low reaction temperature, loss of metal, increase in catalytic cost, etc., and achieve a simple preparation method. , Low production cost, good hydrogenation effect

Active Publication Date: 2018-07-20
XIANGTAN UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Liu Pingle et al. (CN103497113A) invented a method for hydrogenating 1,5-diaminonaphthalene using palladium carbon as a catalyst, which has high activity and relatively low reaction temperature, but the catalyst preparation cost is high, and heavy metals will cause environmental pollution
The research group (CN102172528A) also invented a hydrogenation catalyst prepared by using carbon nanotubes as the carrier to support iron, manganese and cobalt metals. The catalyst cost is significantly lower than that of noble metal catalysts, but there are still metals in the catalytic reaction process. Loss, increased catalytic costs, and caused environmental pollution
[0005] In summary, the preparation cost of noble metal catalysts is high, and metal dissolution and loss are prone to occur during the reaction, which not only leads to a continuous decline in activity, but also causes environmental pollution.
Although non-precious metals greatly reduce the cost of catalyst preparation, the catalyst process and steps are complicated, which is not conducive to engineering operations, and the amount of metal used is large. At the same time, the phenomenon of metal loss is inevitable, causing environmental pollution.

Method used

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  • A metal-free hydrogenation catalyst and its application in catalyzing the hydrogenation reaction of 1,5-dinitronaphthalene
  • A metal-free hydrogenation catalyst and its application in catalyzing the hydrogenation reaction of 1,5-dinitronaphthalene

Examples

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Effect test

Embodiment 1

[0040] A method for preparing a metal-free hydrogenation catalyst, using melamine as a nitrogen source to prepare nitrogen-doped carbon nanotubes by means of an impregnation method, specifically comprising the following steps:

[0041] (1) Oxidation treatment of carbon nanotubes: carbon nanotubes are acidified by adding a mixed acid of concentrated sulfuric acid and concentrated nitric acid with a volume ratio of 3:1 at a solid-to-liquid ratio of 1:80 for acidification for 12 hours, centrifuged and washed, and dried at 80°C for 12 hours Obtain carbon nanotubes.

[0042] (2) Take an appropriate amount of the above-mentioned oxidized carbon nanotubes, mix them with melamine at a mass ratio of 1:1, add deionized water, and add an appropriate amount of formaldehyde twice the mass of melamine, and immerse for 12 hours;

[0043] (3) Add 1mol / L NaOH dropwise to the above solution to adjust the pH to about 10;

[0044] (4) Raise the temperature to 75°C for 30 minutes;

[0045] (5) A...

Embodiment 2

[0049] A method for preparing a metal-free hydrogenation catalyst, using melamine as a nitrogen doping agent to prepare nitrogen-doped carbon nanotubes by an impregnation method, specifically comprising the following steps:

[0050] (1) Oxidation treatment of carbon nanotubes: carbon nanotubes were acidified by adding a mixed acid of concentrated sulfuric acid and concentrated nitric acid with a volume ratio of 3:1 at a solid-to-liquid ratio of 1:60 for 15 hours, centrifuged and washed, and dried at 100°C for 12 hours Obtain carbon nanotubes.

[0051] (2) Take an appropriate amount of the above-mentioned oxidized carbon nanotubes, mix them with melamine at a mass ratio of 1:1.1, add deionized water, and add an appropriate amount of formaldehyde three times the mass of melamine, and immerse for 10 hours;

[0052] (3) Add 0.5mol / L KOH dropwise to the above solution to adjust the pH to about 11;

[0053] (4) Raise the temperature to 70°C for 60 minutes;

[0054] (5) After cooli...

Embodiment 3

[0058] A method for preparing a metal-free hydrogenation catalyst, using melamine as a nitrogen doping agent to prepare nitrogen-doped carbon nanotubes by an impregnation method, specifically comprising the following steps:

[0059] (1) Oxidation treatment of carbon nanotubes: carbon nanotubes are acidified by adding a mixed acid of concentrated sulfuric acid and concentrated nitric acid with a volume ratio of 3:1 at a solid-to-liquid ratio of 1:120 for 8 hours, centrifuged and washed, and dried at 80°C for 12 hours Obtain carbon nanotubes.

[0060] (2) Take an appropriate amount of the above-mentioned oxidized carbon nanotubes, mix them with melamine at a mass ratio of 1:1.2, add deionized water, and add an appropriate amount of formaldehyde twice the mass of melamine, and immerse for 20 hours;

[0061] (3) Add 2mol / L NaCO dropwise to the above solution 3 , adjust the pH to about 12;

[0062] (4) Raise the temperature to 80°C for 30 minutes;

[0063] (5) After cooling to r...

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Abstract

The invention discloses a preparing method for a metal-free hydrogenation catalyst and application of the metal-free hydrogenation catalyst in catalyzing a 1,5-dinitronaphthalene hydrogenation reaction.The preparing method for the metal-free hydrogenation catalyst comprises the steps that an impregnation method is adopted for preparing a nitrating carbon nanotube with melamine as a nitrogen source or an in-situ method is adopted for preparing a nitrating carbon nanotube with ammonia gas as a nitrogen source.The application is that the prepared catalyst is applied to the 1,5-dinitronaphthalene hydrogenation reaction.The nitrating carbon nanotube is adopted as the 1,5-dinitronaphthalene hydrogenation catalyst without any metal active component, and the hydrogenation catalyzing target is achieved only through the nitrating modifying method.In the whole reaction process, precious metal is avoided, cost is saved, the environment can not be polluted, and the catalyst can be repeatedly used.The catalyst preparing method is simple, low in production cost and good in hydrogenation effect, the reaction is controlled easily, the catalyst is environmentally friendly, secondary pollution can not be caused on the environment, and the catalyst can be widely applied to various hydrogenation reactions.

Description

technical field [0001] The invention relates to the fields of material preparation and chemical engineering, in particular to a metal-free hydrogenation catalyst and its application in catalyzing the hydrogenation reaction of 1,5-dinitronaphthalene. Background technique [0002] At present, the catalysts used in the vast majority of catalytic hydrogenation reactions are noble metal-supported catalysts. Although the noble metal catalysts have high activity, the cost is also high, and it is easy to cause heavy metal pollution. Some transition metals such as nickel copper are also used. and other non-precious metal catalysts, but due to the low catalytic activity, the large amount of metal used and the unavoidable metal elution in the reaction, even if the cost of supporting metals is reduced, the cost of the catalyst cannot be reduced, and even increased to a certain extent. Catalyst cost. [0003] In recent years, due to the abnormal mechanical, electrical and chemical prope...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J27/24C07C209/36C07C211/58
CPCB01J27/24C07C209/36C07C211/58
Inventor 刘平乐熊伟郝芳熊绍锋罗和安
Owner XIANGTAN UNIV