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Catalyst for ammonia synthesis reaction

A catalyst, a technology for synthesizing ammonia, applied in physical/chemical process catalysts, organic compound/hydride/coordination complex catalysts, preparation/separation of ammonia, etc., can solve the problems of unrealizable, obvious hydrogen poisoning effect of ruthenium-based catalysts, etc.

Active Publication Date: 2019-06-04
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, the hydrogen poisoning effect of ruthenium-based catalysts is very obvious
[0004] To sum up, although the iron-based and ruthenium-based industrial ammonia synthesis catalysts have their own advantages and disadvantages, the two catalysts still cannot achieve high-efficiency synthesis of ammonia at atmospheric pressure and low temperature (~1bar, 150~300℃).

Method used

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  • Catalyst for ammonia synthesis reaction
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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0018] Li 4 RuH 6 Sample preparation process: in an argon glove box, accurately weigh lithium hydride (LiH) 0.1197g, ruthenium powder (Ru) 0.3804g (molar ratio LiH:Ru=4:1), mix the two and place them in a self-made stainless steel ball mill in the can. After sealing the ball milling tank, put it into a planetary ball mill (Fischt PM400), the ball milling condition is 150rpm, and the ball milling time is 3 hours. In an argon glove box, the resulting sample was placed into a quartz liner, which was then placed in a stainless steel reactor, which was evacuated and flushed into 10barH 2 , and then heated up to 480 ° C for 12 hours, and after it was naturally cooled to room temperature, the obtained sample was put into a glove box for use.

[0019] Li 4 RuH 6 -BM sample preparation process: accurate weighing of Li 4 RuH 6 0.1000 g was placed in a self-made ball mill jar, and after the ball mill jar was closed, it was loaded into a planetary ball mill (Fischt PM400), the bal...

Embodiment 2

[0024] Test Li 4 RuH 6 , Li 4 RuH 6 -BM, Li 4 RuH 6 The activity of -MgO-BM and Ru-Li-MgO changes with temperature (reaction conditions: catalyst 30mg, flow velocity 30ml / min, pressure 1bar, N 2 :H 2 =3:1 (molar ratio)), the activation energy was calculated according to the Arrhenius equation. like figure 2 As shown, it can be seen that four kinds of Li with different dispersion 4 RuH 6 have similar activation energies, both close to 70kJ / mol, indicating that the Li 4 RuH 6 After dispersion, its active sites did not change.

Embodiment 3

[0026] Using the same method to prepare highly dispersed Ru-K-MgO (accurately weighed Ru-MgO 0.050g, K0.0077g), Ru-Ca-MgO (accurately weighed Ru-MgO 0.050g, Ca 0.0079g) and Ru-Na -MgO (accurately weigh 0.050g of Ru-MgO, 0.0043g of Na), Ru-Ba-MgO (accurately weigh 0.050g of Ru-MgO, 0.0272g of Ca).

[0027] Accurately weigh 0.030g of Ru-Li-MgO, Ru-K-MgO, Ru-Ca-MgO-, Ru-Na-MgO, Ru-Ba-MgO and the reference catalyst Ru-MgO respectively, and place them in a fixed-bed stainless steel reaction device. Test its activity curve (reaction conditions: catalyst 30mg, flow velocity 30ml / min, pressure 1bar, N 2 :H 2 =3:1 (molar ratio)). like image 3 As shown, it can be seen that Ru-Li-MgO, Ru-MgO, Ru-Ca-MgO, Ru-Na-MgO, Ru-Ba-MgO all exhibit excellent catalytic activity. Among them, Ru-Na-MgO is active (24umol / g) at 150°C and 1bar cat / h), and the ammonia formation rate increases gradually with increasing temperature, which is higher than that of Ru-Li-MgO, Ru-K-MgO, Ru-Ca-MgO and Ru-Ba...

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Abstract

The invention relates to a transition metal hydride catalyst for ammonia synthesis. The transition metal hydride catalyst comprises a transition metal hydride and a carrier. The catalyst for ammonia synthesis has an excellent catalytic activity, especially under low temperature and low pressure conditions (1 bar and below 300 DEG C).

Description

technical field [0001] The invention relates to catalyst technology, and in particular provides a transition metal hydride catalyst for ammonia synthesis and its application in ammonia synthesis reaction, especially suitable for ammonia synthesis at low temperature and normal pressure. Background technique [0002] Ammonia is one of the most important chemical raw materials in the world. Ammonia can be used not only as a fertilizer, but also as a very important intermediate in chemical industry. But for now, industrial ammonia synthesis needs to be realized under high temperature and high pressure conditions, so that about 1% of the world's energy is used in the ammonia synthesis industry every year. Therefore, it is of great significance to develop high-efficiency ammonia synthesis catalysts under mild conditions. [0003] Iron-based and ruthenium-based catalysts are important industrial ammonia synthesis catalysts. As the first generation of ammonia synthesis catalysts, ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/12C01C1/04
CPCY02P20/52
Inventor 陈萍王倩茹郭建平王培坤高文波
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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