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Ammonia synthesis catalyst and ammonia synthesis method

Foreign code F170009051
File No. J1014-13WO
Posted date Apr 26, 2017
Country United States of America
Application number 201515125462
Gazette No. 20170088433
Gazette No. 10017395
Date of filing Jan 9, 2015
Gazette Date Mar 30, 2017
Gazette Date Jul 10, 2018
International application number JP2015050545
International publication number WO2015136954
Date of international filing Jan 9, 2015
Date of international publication Sep 17, 2015
Priority data
  • P2014-050700 (Mar 13, 2014) JP
  • 2015WO-JP50545 (Jan 9, 2015) WO
Title Ammonia synthesis catalyst and ammonia synthesis method
Abstract (US10017395)
The ammonia synthesis catalyst of the present invention, comprises: a powder of a perovskite oxyhydride having hydride (H-) incorporated therein as a support; and a metal or a metal compound exhibiting a catalytic activity for ammonia synthesis, supported on the support, and the perovskite oxyhydride is represented by ATiO3-xHx (wherein A represents Ca, Sr, or Ba, and 0.1≦x≦0.6).
Scope of claims [claim1]
1. An ammonia synthesis catalyst, comprising: a powder of a perovskite oxyhydride having hydride (H-) incorporated therein as a support; and a metal or a metal compound exhibiting a catalytic activity for ammonia synthesis, supported on the support.
[claim2]
2. The ammonia synthesis catalyst according to claim 1, wherein the perovskite oxyhydride is represented by ATiO3-xHx (wherein A represents Ca, Sr, or Ba, and 0.1 <= x <= 0.6).
[claim3]
3. The ammonia synthesis catalyst according to claim 1, wherein the perovskite oxyhydride further contains nitrogen.
[claim4]
4. The ammonia synthesis catalyst according to claim 3, wherein the perovskite oxyhydride is represented by ATi(O3-zHxNy) (wherein A represents Ca, Sr, or Ba, and 0.1 <= x <= 0.6, 0<y <= 0.3, z >= x+y, and z-x-y represents the amount of oxygen defects).
[claim5]
5. The ammonia synthesis catalyst according to claim 1, wherein the metal exhibiting a catalytic activity is supported on the surface of the powder in the form of metal nanoparticles.
[claim6]
6. The ammonia synthesis catalyst according to claim 1, wherein the metal compound exhibiting a catalytic activity is mixed with the powder and supported thereon.
[claim7]
7. The ammonia synthesis catalyst according to claim 5, wherein the metal exhibiting a catalytic activity or the metal of the metal compound exhibiting a catalytic activity is Ru and the supported amount in terms of Ru metal with respect to the support is from 0.1 to 5 wt %.
[claim8]
8. A method for producing an ammonia synthesis catalyst, comprising: a first step of preparing a powder of a perovskite oxyhydride having hydride (H-) incorporated therein by keeping a powder of a perovskite titanium-containing oxide as a starting material together with a powder of an alkali metal hydride or an alkaline earth metal hydride selected from LiH, CaH2, SrH2, and BaH2 in a temperature range of 300 deg. C. or higher and lower than the melting point of the hydride in a vacuum or in an inert gas atmosphere, thereby substituting some of the oxide ions in the oxide with hydride ions;
a second step of preparing a catalyst precursor by dispersing the perovskite oxyhydride powder obtained in the first step in a solvent solution of a compound of a metal having an ammonia synthesis activity, followed by evaporating the solvent; and
a third step of preparing a catalyst having a metal compound exhibiting a catalytic activity supported on the powder by drying the catalyst precursor obtained in the second step.
[claim9]
9. The method for producing an ammonia synthesis catalyst according to claim 8, wherein the method further comprises, after the third step, a fourth step of preparing a catalyst having metal nanoparticles supported on the surface of the powder by heating and reducing the metal compound in a reducing atmosphere or thermally decomposing the metal compound in a vacuum.
[claim10]
10. The method for producing an ammonia synthesis catalyst according to claim 8, wherein the method comprises, after the first step and before the second step, a step of incorporating nitrogen in the perovskite oxyhydride by treating the powder of the perovskite oxyhydride in the presence of a nitrogen supply source substance.
[claim11]
11. The method for producing an ammonia synthesis catalyst according to claim 8, wherein the method comprises, after the third step or the fourth step, a step of incorporating nitrogen in the perovskite oxyhydride by treating the catalyst in the presence of a nitrogen supply source substance.
[claim12]
12. An ammonia synthesis method, which is a method for synthesizing ammonia by reacting hydrogen and nitrogen using a gas containing hydrogen and nitrogen as raw materials, wherein the catalyst according to claim 1 is packed in a catalytic packed bed in a synthesis reactor, and nitrogen and hydrogen as the raw materials are reacted on the catalyst under conditions of a reaction temperature of 300 deg. C. to 450 deg. C. and a reaction pressure of 10 kPa or more and less than 20 MPa.
  • Inventor, and Inventor/Applicant
  • Kageyama Hiroshi
  • Kobayashi Yoji
  • Masuda Naoya
  • Hosono Hideo
  • JAPAN SCIENCE AND TECHNOLOGY AGENCY
IPC(International Patent Classification)
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