Inorganic porous support-zeolite membrane composite, production method thereof, and separation method using the composite
View Patent ↗An object of the present invention is to provide a zeolite membrane composite satisfying both the treating amount and the separation performance at a practically sufficient level, which can be applied even in the presence of an organic material and can separate/concentrate an organic material-containing gas or liquid mixture and which is economic without requiring a high energy cost and is not limited in its application range; a production method thereof; and a separation or concentration method using the same. The present invention is an inorganic porous support-zeolite membrane composite, wherein the inorganic porous support contains a ceramic sintered body and the inorganic porous support-zeolite membrane composite has, as a zeolite membrane, a CHA-type zeolite crystal layer on the inorganic porous support surface.
1. An inorganic porous support-zeolite membrane composite, wherein the inorganic porous support contains a ceramic sintered body and the inorganic porous support-zeolite membrane composite has, as the zeolite membrane, a CHA-type zeolite crystal layer on the inorganic porous support surface, and in the X-ray diffraction pattern obtained by irradiating the zeolite membrane surface with an X-ray, the peak intensity near 2θ=17.9° is 0.5 times or more the peak intensity near 2θ=20.8°.
2. An inorganic porous support-zeolite membrane composite, wherein the inorganic porous support-zeolite membrane composite has a CHA-type zeolite crystal layer as the zeolite membrane and in the X-ray diffraction pattern obtained by irradiating the zeolite membrane surface with an X-ray, the peak intensity near 2θ=17.9° is 0.5 times or more the peak intensity near 2θ=20.8°.
3. An inorganic porous support-zeolite membrane composite, wherein the inorganic porous support-zeolite membrane composite has a CHA-type zeolite crystal layer as the zeolite membrane and in the X-ray diffraction pattern obtained by irradiating the zeolite membrane surface with an X-ray, the peak intensity near 2θ=9.6° is 4 times or more the peak intensity near 2θ=20.8°.
4. The inorganic porous support-zeolite membrane composite as claimed in claim 1 , wherein in the X-ray diffraction pattern obtained by irradiating the zeolite membrane surface with an X-ray, the peak intensity near 2θ=9.6° is 4 times or more the peak intensity near 2θ=20.8°.
5. The inorganic porous support-zeolite membrane composite as claimed in claim 1 , wherein the molar ratio SiO 2 /Al 2 O 3 of the zeolite crystal layer is 5 or more.
6. The inorganic porous support-zeolite membrane composite as claimed in claim 1 , wherein the inorganic porous support comprises at least one kind of a material selected from the group consisting of alumina, silica and mullite.
7. A method for producing the inorganic porous support-zeolite membrane composite claimed in any one of claims 1 to 3 , which comprises crystallizing a CHA-type zeolite on the inorganic porous support surface.
8. The method of producing the inorganic porous support-zeolite membrane composite as claimed in claim 7 , wherein after attaching a zeolite seed crystal to the inorganic porous support surface, the CHA-type zeolite is crystallized.
9. The method of producing the inorganic porous support-zeolite membrane composite as claimed in claim 8 , wherein the zeolite seed crystal is a CHA-type zeolite.
10. The method of producing the inorganic porous support-zeolite membrane composite as claimed in claim 7 , wherein in performing crystallization of the CHA-type zeolite, a reaction mixture containing an Si element source and an Al element source is used as a raw material such that the molar ratio (SiO 2 /Al 2 O 3 ) as the ratio between Si and Al in terms of respective oxides becomes from 5 to 10,000.
11. The method of producing the inorganic porous support-zeolite membrane composite as claimed in claim 10 , wherein an alkali metal ion is present in the reaction mixture.
12. The method of producing the inorganic porous support-zeolite membrane composite as claimed in claim 10 , wherein an organic template is further used as a raw material and the organic template is a cation derived from 1-adamantanamine.
13. A separation membrane comprising the inorganic porous support-zeolite membrane composite claimed in claim 1 .
14. A separation method comprising contacting an organic material-containing gas or liquid mixture with the inorganic porous support-zeolite membrane composite claimed in any one of claims 1 to 3 to allow for permeation of a highly permeable substance out of said mixture, thereby separating said highly permeable substance from said mixture.
15. The separation method as claimed in claim 14 , wherein the organic material-containing gas or liquid mixture is a mixture of an organic acid and water.
16. The separation method as claimed in claim 14 , wherein the organic material-containing gas or liquid mixture is a mixture of water and at least one kind of a material selected from organic compounds containing an alcohol, an ether, an aldehyde, a ketone or a nitrogen.
17. A concentration method comprising contacting an organic material-containing gas or liquid mixture with the inorganic porous support-zeolite membrane composite claimed in any one of claims 1 to 3 to allow for permeation of a highly permeable substance out of said mixture, thereby concentrating the highly permeable substance.
18. The concentration method as claimed in claim 17 , wherein the organic material-containing gas or liquid mixture is a mixture of water and at least one kind of a material selected from organic compounds containing an alcohol, an ether, an aldehyde, a ketone or a nitrogen.
19. The inorganic porous support-zeolite membrane composite as claimed in claim 2 , wherein in the X-ray diffraction pattern obtained by irradiating the zeolite membrane surface with an X-ray, the peak intensity near 2θ=9.6° is 4 times or more the peak intensity near 2θ=20.8°.
20. The inorganic porous support-zeolite membrane composite according to claim 2 , wherein the molar ratio SiO 2 /Al 2 O 3 of the zeolite crystal layer is 5 or more.
21. The inorganic porous support-zeolite membrane composite according to claim 3 , wherein the molar ratio SiO 2 /Al 2 O 3 of the zeolite crystal layer is 5 or more.
22. The inorganic porous support-zeolite membrane composite according to claim 2 , wherein the inorganic porous support comprises at least one kind of a material selected from the group consisting of alumina, silica and mullite.
23. The inorganic porous support-zeolite membrane composite according to claim 3 , wherein the inorganic porous support comprises at least one kind of a material selected from the group consisting of alumina, silica and mullite.
24. A separation membrane comprising the inorganic porous support-zeolite membrane composite according to claim 2 .
25. A separation membrane comprising the inorganic porous support-zeolite membrane composite according to claim 3 .