Ruthenium ammonia synthesis catalyst by using N-doped active carbon as carrier and preparation of ruthenium ammonia synthesis catalyst

A technology of activated carbon and nitrogen doping, which is applied in the field of ruthenium-based ammonia synthesis catalysts and its preparation, which can solve the problems of uncontrollable nitrogen content and cumbersome steps, and achieve controllable nitrogen content, controllable nitrogen doping content, and improved thermal stability sexual effect

Inactive Publication Date: 2015-07-22
FUZHOU UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

The Chinese patent application number CN200810120648.7 reports a low-temperature SCR catalyst based on nitrogen-doped activated carbon prepared by ammonia burning method; patent CN103121678 A reports a method of pre-oxidizing PET waste and then physically mixing it: and Patent CN102211033 A reports a method for platinum-nitrogen co-doped activated carbon, which uses a catalyst obtained through a series of conventional steps after sol; the above method for preparing nitrogen-doped activated carbon catalyst can achieve the purpose of nitrogen doping, but there is The amount is uncontrollable, the steps are cumbersome, etc. The invention discloses a ruthenium-based ammonia synthesis catalyst with nitrogen-doped activated carbon as a carrier that integrates a variety of technologies, which not only makes up for the gap in the application of such carriers to ammonia synthesis reactions, but also proposes A preparation method with simple operation and easy control of nitrogen content was developed, which improved its activity and stability in ammonia synthesis reaction

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0024] (1) Pretreatment of activated carbon: Weigh 4.0g of commercial activated carbon, graphitize it in an inert atmosphere, and then expand the pores to obtain pretreated activated carbon, dry and wash it for later use;

[0025] (2) Preparation of nitrogen-doped activated carbon support: 0.4mol / L CO(NH 2 ) 2 The solution was impregnated into the carrier by equal-volume impregnation method, heated and evaporated at 100°C to dry, and an activated carbon precursor with a nitrogen-doped content of 4% was obtained, which was placed in a tube furnace and calcined at 200°C for 1 h , and then roasted at 550°C for 3 hours to obtain a nitrogen-doped activated carbon carrier; after cooling to room temperature, take out the carrier, put it into a Soxhlet extractor for extraction with ethanol, until the pH of the supernatant is about 7, wash and dry to obtain nitrogen doped activated carbon material;

[0026] (3) Catalyst preparation: then impregnate 5% of the active component rutheniu...

Embodiment 2

[0030] The preparation method of the catalyst is the same as in Example 1, only CO(NH 2 ) 2 The molar concentration is 0.5mol / L, and other conditions are the same, and the ruthenium-based ammonia synthesis catalyst supported by activated carbon with a nitrogen doping amount of 5% is obtained by an equal-volume impregnation method.

[0031] Performance Testing:

[0032] in H 2 :N 2 =3:1,400℃,10000h -1 ,Under the condition of 10MPa, the outlet ammonia concentration can reach 19.8%. After 500℃, 10MPa heat resistance for 24 hours, the outlet ammonia concentration is 19.3%.

Embodiment 3

[0034] The preparation method of catalyst repeats embodiment 1, only changes CO(NH 2 ) 2 The molar concentration is 0.6mol / L, and other conditions are the same, and the ruthenium-based ammonia synthesis catalyst supported by activated carbon with a nitrogen doping amount of 6% is obtained by the equal volume impregnation method.

[0035] Performance Testing:

[0036] in H 2 :N 2 =3:1, 400℃, 10000h -1 , Under the condition of 10MPa, the outlet ammonia concentration can reach 20.1%, after 500 ℃, 10MPa heat resistance for 24 hours, the outlet ammonia concentration is 19.8%.

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Abstract

The invention belongs to the technical field of preparation of ammonia synthesis catalysts, and particularly relates to a ruthenium ammonia synthesis catalyst by using N-doped active carbon as a carrier and a preparation method of the ruthenium ammonia synthesis catalyst. The preparation method of the N-doped active carrier, disclosed by the invention, comprises the following steps: dissolving a precursor containing nitrogen in water so as to prepare a solution; loading the solution on graphitized active carbon by an equivalent-volume impregnation method; heating and evaporating the solution loaded on the graphitized active carbon at the temperature of 100 DEG C so as to be dried; then transferring the dried solution loaded on the graphitized active carbon into a tubular furnace, and roasting the transferred solution loaded on the graphitized active carbon at the temperature of 200 DEG C for some time; then performing the treatments of programmed warming and the like so as to obtain the N-doped active carbon carrier. The carrier is large in specific surface area and is high in activity, the doping content of nitrogen is controllable, and when the carrier is used for the ruthenium ammonia synthesis catalyst, the heat stability and the activity of the Ru/AC catalyst are improved.

Description

technical field [0001] The invention belongs to the technical field of preparation of ammonia synthesis catalysts, and in particular relates to a ruthenium-based ammonia synthesis catalyst with nitrogen-doped activated carbon as a carrier and a preparation method thereof. Background technique [0002] The ammonia synthesis industry is a pillar industry of my country's chemical industry. After more than 100 years of exploration, ruthenium-based ammonia synthesis catalysts have been ushered in on the basis of the first generation of iron-based catalysts. Excellent activity is known as the second generation ammonia synthesis catalyst. In the field of ammonia synthesis catalysts, activated carbon is used as the carrier of traditional ruthenium-based ammonia synthesis catalysts, and its initial activity is relatively high. Patents CN101362080A and CN101053834A have disclosed a ruthenium-based ammonia synthesis that uses activated carbon as a carrier to support alkaline earth metal...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/58B01J27/24B01J35/10
Inventor 林建新赵子琦徐家祺倪军林炳裕
Owner FUZHOU UNIV
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