Oxynitride-hydride, metal-supported material containing oxynitride-hydride, and ammonia synthesis catalyst

Patent metadata

Field	Value
Publication number	US-12350654-B2
Application number	US-202117801816-A
Country	US
Kind code	B2
Filing date	Feb 16, 2021
Priority date	Feb 26, 2020
Publication date	Jul 8, 2025
Grant date	Jul 8, 2025

Abstract

The present invention is related to an oxynitride-hydride which is capable of achieving both stabilization and improvement of catalyst performance when used as a support, and the oxynitride-hydride can be easily synthesized. The oxynitride-hydride is represented by the following general formula (1),

A n B m O l-x N y H z   (1)
wherein in the general formula (1), x represents a number represented by 0.1≤x≤3.5; y represents a number represented by 0.1≤y≤2.0; and z represents a number represented by 0.1≤z≤2.0.

First claim

The invention claimed is:

1. An oxynitride-hydride, which is represented by the following general formula (1),
A n B m O l-x N y H z   (1)

wherein, in the general formula (1), A is at least one selected from the group consisting of Ba and Sr; B is at least one selected from the group consisting of Al, Ga, In, Si, and Ge; n is an integer of 1 to 3; m is 1 or 2; l is 4 or 5; x represents a number represented by 0.1≤x≤3.5; y represents a number represented by 0.1≤y≤2.0; and z represents a number represented by 0.1≤z≤2.0.

2. The oxynitride-hydride according to claim 1 , wherein, in the general formula (1), B is at least one selected from the group consisting of Al, Ga, and In; n=1; m=2; and l=4.

3. The oxynitride-hydride according to claim 1 , wherein, in the general formula (1), B is at least one selected from the group consisting of Si, and Ge; n=3; m=1; and l=5.

4. A method of producing an oxynitride-hydride represented by the following general formula (1), comprising:
a step of heating a compound represented by the following general formula (2) and a compound represented by the following general formula (3) under an ammonia atmosphere,
A n B m O l-x N y H z   (1)

A(NH 2 ) 2   (2)

B k O j   (3)

wherein, in the general formulae (1) to (3), A is at least one selected from the group consisting of Ba and Sr; B is at least one selected from the group consisting of Al, Ga, In, Si, and Ge; n is an integer of 1 to 3; m is 1 or 2; l is 4 or 5; k is 1 or 2; j is 1 to 3; x represents a number represented by 0.1≤x≤3.5; y represents a number represented by 0.1≤y≤2.0; and z represents a number represented by 0.1≤z≤2.0.

5. The method of producing the oxynitride-hydride according to claim 4 , wherein, in the general formula (1), B is at least one selected from the group consisting of Al, Ga, and In; n=1; m=2; and l=4.

6. The method of producing the oxynitride-hydride according to claim 4 , wherein, in the general formula (1), B is at least one selected from the group consisting of Si, and Ge; n=3; m=1; and l=5.

7. A metal-supported material in which a transition metal (M) is supported on a support,
wherein the support is a composition comprising an oxynitride-hydride which is represented by the following general formula (1),
A n B m O l-x N y H z   (1)

wherein, in the general formula (1), A is at least one selected from the group consisting of Ba and Sr; B is at least one selected from the group consisting of Al, Ga, In, Si, and Ge; n is an integer of 1 to 3; m is 1 or 2; l is 4 or 5; x represents a number represented by 0.1≤x≤3.5; y represents a number represented by 0.1≤y≤2.0; and z represents a number represented by 0.1≤z≤2.0.

8. The metal-supported material according to claim 7 , wherein a loading amount of the transition metal (M) is 0.01 parts by mass to 50 parts by mass with respect to 100 parts by mass of the support.

9. The metal-supported material according to claim 7 , wherein the transition metal (M) is at least one selected from the group consisting of Ru, Co, and Fe.

10. A supported-metal catalyst comprising the metal-supported material according to claim 7 .

11. An ammonia synthesis catalyst comprising the metal-supported material according to claim 7 .

12. An ammonia synthesis catalyst, which is a composition comprising an oxynitride-hydride which is represented by the following general formula (1),
A n B m O l-x N y H z   (1)

wherein, in the general formula (1), A is at least one selected from the group consisting of Ba and Sr; B is at least one selected from the group consisting of Al, Ga, In, Si, and Ge; n is an integer of 1 to 3; m is 1 or 2; l is 4 or 5; x represents a number represented by 0.1≤x≤3.5; y represents a number represented by 0.1≤y≤2.0; and z represents a number represented by 0.1≤z≤2.0.

13. The metal-supported material according to claim 7 , wherein, in the general formula (1), B is at least one selected from the group consisting of Al, Ga, and In; n=1; m=2; and l=4.

14. The metal-supported material according to claim 7 , wherein, in the general formula (1), B is at least one selected from the group consisting of Si, and Ge; n=3; m=1; and l=5.

15. A method of producing the metal-supported material according to claim 7 , comprising:
a step of producing the oxynitride-hydride represented by the general formula (1) by heating a compound represented by the following general formula (2) and a compound represented by the following general formula (3) under an ammonia atmosphere,
A(NH 2 ) 2   (2)

B k O j   (3)

wherein, in the general formulae (2) to (3), A is at least one selected from the group consisting of Ba and Sr; B is at least one selected from the group consisting of Al, Ga, In, Si, and Ge; k is 1 or 2; j is 1 to 3; and

a step of loading the transition metal (M) on the oxynitride-hydride.

16. The method of producing the metal-supported material according to claim 15 , wherein, in the general formula (1), B is at least one selected from the group consisting of Al, Ga, and In; n=1; m=2; and l=4.

17. The method of producing the metal-supported material according to claim 15 , wherein, in the general formula (1), B is at least one selected from the group consisting of Si, and Ge; n=3; m=1; and l=5.

Assignees

• Japan Science & Tech Agency

Inventors

• Kitano Masaaki
• Hosono Hideo
• Yokoyama Toshiharu
• KUJIRAI Jun
• OGASAWARA Kiya

Classifications

• B01J2235/15

  X-ray diffraction · CPC title

• B01J35/70

  characterised by their crystalline properties, e.g. semi-crystalline (catalysts comprising carbon B01J21/18; molecular sieves B01J29/00) · CPC title

• B01J35/394

  Metal dispersion value, e.g. percentage or fraction · CPC title

• C01C1/0411 Primary

  characterised by the catalyst · CPC title

• B01J37/08

  Heat treatment {(B01J37/0009, B01J37/0018 take precedence)} · CPC title