IP Library Granted Patent US 10,332,690
Granted Patent B2
US 10,332,690 · App. 15/476,116 · Granted Jun 25, 2019

Method of producing composite photocatalyst and composite photocatalyst

Inventors: Seiji Akiyama (Kanagawa, JP); Kazunari Domen (Tokyo, JP)
Assignees: MITSUBISHI CHEMICAL CORPORATION; The University of Tokyo; Japan Technological Research Association of Artificial Photosynthetic Chemical Process
H01G9/2036B01J27/24B01J35/02B01J37/34C01B3/042C25B1/04Y02E60/364Y02E60/366
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Quick Facts
Patent No.
US 10,332,690
App. No.
15/476,116
Granted
Jun 25, 2019
Kind
B2
Abstract

The present invention provides a method of producing a composite photocatalyst having a remarkable water splitting activity, which is capable of efficiently loading a co-catalyst having a small particle size in a highly dispersed manner on a surface of an optical semiconductor. According to the present invention, the method of producing a composite photocatalyst from a plurality types of optical semiconductors includes a step of heating a solid-liquid mixture containing a solvent, a co-catalyst or a co-catalyst source, and a plurality of types of optical semiconductors by irradiating the solid-liquid mixture with microwave.

Claims (32)

1. A composite photocatalyst which comprises a plurality of types of optical semiconductors on which a co-catalyst is loaded, wherein the co-catalyst is present on the surfaces of the plurality of types of the optical semiconductors, and is present in a state of being interposed between bonding surfaces of the plurality of types of the optical semiconductors, or is present in a state of covering the optical semiconductor.

2. The composite photocatalyst according to claim 1 ,

wherein at least one of the plurality of types of optical semiconductors is an oxide, a nitride, an oxynitride, a chalcogenide, or an oxychalcogenide each of which contains one or more elements selected from the group consisting of Ti, V, Ga, Zn, Bi, Nb, and Ta.

3. The composite photocatalyst according to claim 2 ,

wherein at least one of the plurality of types of optical semiconductors is BaTaO 2 N, BaNbO 2 N, TaON, Ta 3 N 5 , LaTiO 2 N, BiVO 4 , GaN:ZnO, or a partial substitution thereof.

4. The composite photocatalyst according to claim 1 , wherein the co-catalyst contains Co.

5. A method of producing a composite photocatalyst as claimed in claim 1 from a plurality of types of optical semiconductors, the method comprising:

heating a solid-liquid mixture containing a solvent, a co-catalyst or a co-catalyst source and the plurality of types of optical semiconductors by irradiating the solid-liquid mixture with microwave.

6. The method of producing a composite photocatalyst according to claim 5 , wherein before the microwave irradiation, the co-catalyst source in the solid-liquid mixture is present in a state of being dissolved in a solvent.

7. The method of producing a composite photocatalyst according to claim 5 , wherein before the microwave irradiation, the co-catalyst or a co-catalyst source and the plurality of types of optical semiconductors in the solid-liquid mixture are present as a solid in the solvent, and the cocatalyst or a co-catalyst source is in a state of being loaded on the plurality of types of optical semiconductors.

8. The method of producing a composite photocatalyst according to claim 7 , further comprising as a pre-step of the heating:

first loading a co-catalyst on a first optical semiconductor by heating with the microwave in a state where the first optical semiconductor is brought into contact with a solution in which a co-catalyst source is dissolved;

second loading a co-catalyst on a second optical semiconductor by heating with the microwave in a state where the second optical semiconductor is brought into contact with the solution in which the co-catalyst source is dissolved; and

mixing the first optical semiconductor on which the co-catalyst is loaded and the second optical semiconductor on which the co-catalyst is loaded, into the solvent so as to obtain the solid-liquid mixture.

9. The method of producing a composite photocatalyst according to claim 8 , wherein the microwave irradiation is performed in a closed system in the first loading step and the second loading step.

10. The method of producing a composite photocatalyst according to claim 8 , further comprising as pre-steps of the first loading and the second loading:

bringing a solution of one or more types of organic acids containing a polyorganic acid into contact with a surface of an oxide, an oxynitride, or a nitride containing one or more elements selected from Ti, V, Ga, Ge, Nb, La, and Ta; and

collecting the oxide, the oxynitride, or the nitride which remains as a solid content after the organic acid contact,

wherein the collected solid contents are used as the first optical semiconductor and the second optical semiconductor.

11. The method of producing a composite photocatalyst according to claim 5 , wherein at least one of the plurality of types of optical semiconductors is an oxide, a nitride, an oxynitride, a chalcogenide, or an oxychalcogenide, each of which contains one or more elements selected from the group consisting of Ti, V, Ga, Zn, Bi, Nb, and Ta.

12. The method of producing a composite photocatalyst according to claim 11 , wherein at least one of the plurality of types of optical semiconductors is BaTaO 2 N, BaNbO 2 N, TaON, Ta 3 N 5 , LaTiO 2 N, BiVO 4 , GaN:ZnO, or a partial substitution thereof.

13. The method of producing a composite photocatalyst according to claim 5 , wherein the co-catalyst or the co-catalyst source contains Co or Co-ion.

14. The method of producing a composite photocatalyst according to claim 5 , wherein the solvent is water, alcohols, or a mixed solvent thereof.

15. The method of producing a composite photocatalyst according to claim 5 , wherein the solid-liquid mixture is heated by being irradiated with the microwave in a closed system in the heating.

16. The method of producing a composite photocatalyst according to claim 15 , wherein pressure in the closed system is higher than pressure outside the system.

17. The method of producing a composite photocatalyst according to claim 5 , further comprising as a pre-step of the heating:

bringing a solution of one or more types of organic acids containing a polyorganic acid into contact with a surface of an oxide, an oxynitride, or a nitride each of which contains one or more elements selected from Ti, V, Ga, Ge, Nb, La, and Ta; and

collecting the oxide, the oxynitride, or the nitride which remains as a solid content after the organic acid contact step,

wherein the collected solid contents are used as the plurality of types of optical semiconductors.

18. The method of producing a composite photocatalyst according to claim 17 , wherein the organic acid is a polysulfonic acid.

19. The method of producing a composite photocatalyst according to claim 17 , wherein the organic acid has an aryl group.

20. The method of producing a composite photocatalyst according to claim 17 , wherein the organic acid has a weight average molecular weight in a range of 1,000 to 1,000,000.

Assignments (3)
CHANGE OF NAME Recorded Sep 5, 2017
From: MITSUBISHI RAYON CO., LTD.
To: MITSUBISHI CHEMICAL CORPORATION
Reel/Frame 043750/0834 →
MERGER Recorded Sep 4, 2017
From: MITSUBISHI CHEMICAL CORPORATION
To: MITSUBISHI RAYON CO., LTD.
Reel/Frame 043750/0207 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 31, 2017
From: AKIYAMA, SEIJI; DOMEN, KAZUNARI
To: MITSUBISHI CHEMICAL CORPORATION; THE UNIVERSITY OF TOKYO; JAPAN TECHNOLOGICAL RESEARCH ASSOCIATION OF ARTIFICIAL PHOTOSYNTHETIC CHEMICAL PROCESS
Reel/Frame 041813/0181 →
Priority Claims (3)
JP 2014-236221 · Nov 21, 2014 · national
JP 2015-013006 · Jan 27, 2015 · national
JP 2015-161131 · Aug 18, 2015 · national
Continuity (2)
Continuation PCTJP2015082804 · Nov 20, 2015
Related Publication 20170250031A1 · Aug 31, 2017