IP Library Granted Patent US 10,322,940
Granted Patent B2
US 10,322,940 · App. 15/532,877 · Granted Jun 18, 2019

Composite, method for producing composite, ammonia synthesis catalyst, and ammonia synthesis method

Inventors: Hideo Hosono (Tokyo, JP); Michikazu Hara (Tokyo, JP); Masaaki Kitano (Tokyo, JP); Toshiharu Yokoyama (Tokyo, JP); Yasunori Inoue (Tokyo, JP)
Assignees: JAPAN SCIENCE AND TECHNOLOGY AGENCY; TOKYO INSTITUTE OF TECHNOLOGY
C01C1/0411B01J23/462B01J27/24B01J35/1014B01J37/0072B01J37/0205B01J37/0209B01J37/04B01J37/08B01J37/082B01J37/086C01B3/047C01B21/0923C01B21/0926B01J21/18B01J23/58B01J23/63B01J23/648B01J35/006B01J35/0046B01J35/0066B01J35/1019C01P2004/04Y02E60/364Y02P20/52
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Quick Facts
Patent No.
US 10,322,940
App. No.
15/532,877
Granted
Jun 18, 2019
Kind
B2
Abstract

An ammonia synthesis catalyst having high activity is obtained by having a two-dimensional electride compound having a lamellar crystal structure such as Ca 2 N support a transition metal. However, since the two-dimensional electride compound is unstable, the stability of the catalyst is low. In addition, in cases where a two-dimensional electride compound is used as a catalyst support, it is difficult to shape the catalyst depending on reactions since the two-dimensional electride compound has poor processability. A composite which includes a transition metal, a support and a metal amide compound, wherein the support is a metal oxide or a carbonaceous support; and the metal amide compound is a metal amide compound represented by general formula (1). M(NH 2 ) x   (1) (In general formula (1), M represents at least one metal atom selected from the group consisting of Li, Na, K, Be, Mg, Ca, Sr, Ba and Eu; and x represents the valence of M.).

Claims (28)

1. A composite, comprising Ru, a support, and a metal amide compound, wherein:

the support is at least one metal oxide selected from the group consisting of ZrO 2 , TiO 2 , CeO 2 , and MgO; and

the metal amide compound is Ca(NH 2 ) 2 .

2. The composite according to claim 1 , wherein the composite has a BET specific surface area of 10 m 2 /g or more.

3. A supported metal catalyst, comprising the composite according to claim 1 .

4. An ammonia synthesis catalyst, comprising the composite according to claim 1 .

5. A method of producing a composite comprising a transition metal, a support, and a metal amide compound, wherein:

the support is a metal oxide or a carbonaceous support;

the metal amide compound is a compound represented by formula (1):

M(NH 2 ) x   (1);

wherein

M represents at least one metal atom selected from the group consisting of Li, Na, K, Be, Mg, Ca, Sr, Ba and Eu; and

x represents the valence of M,

the method of producing the composite comprising:

mixing a metal atom source comprising the metal atom M, the support, and liquid ammonia;

reacting the metal atom source with the liquid ammonia to form a metal amide-supporting support comprising the metal amide compound on the support; and

supporting the transition metal on the metal amide-supporting support.

6. The method of producing a composite according to claim 5 , wherein the supporting of the transition metal on the metal amide-supporting support comprises:

supporting a transition metal raw material on the metal amide-supporting support; and

depositing the transition metal by thermally decomposing the transition metal raw material.

7. A method of synthesizing ammonia, the method comprising contacting a gas comprising nitrogen and a gas comprising hydrogen with the ammonia synthesis catalyst according to claim 4 to synthesize ammonia.

8. The method for synthesizing ammonia according to claim 7 , wherein a temperature at which the ammonia synthesis catalyst is brought into contact with the ammonia synthesis catalyst is 100° C. or more and 600° C. or less.

9. The method for synthesizing ammonia according to claim 7 , wherein the pressure when contacting the ammonia synthesis catalyst is from 10 kPa to 20 MPa.

10. A method of producing the composite according to claim 7 , comprising:

mixing a metal atom source comprising Ca, the support, and liquid ammonia;

reacting the metal atom source with the liquid ammonia to form metal amide-supporting support comprising the metal amide compound on the support; and

supporting Ru on the metal amide-supporting support.

11. The composite according to claim 1 , wherein the at least one metal oxide selected from the group consisting of ZrO 2 , TiO 2 , and CeO 2 .

Assignments (1)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 2, 2017
From: HOSONO, HIDEO; HARA, MICHIKAZU; KITANO, MASAAKI; YOKOYAMA, TOSHIHARU; INOUE, YASUNORI
To: JAPAN SCIENCE AND TECHNOLOGY AGENCY; TOKYO INSTITUTE OF TECHNOLOGY
Reel/Frame 042577/0715 →
Priority Claims (1)
JP 2014-246717 · Dec 5, 2014 · national
Continuity (1)
Related Publication 20170355607A1 · Dec 14, 2017
Cited By (15)
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