IP Library Granted Patent US 9,670,068
Granted Patent B2
US 9,670,068 · App. 13/807,080 · Granted Jun 6, 2017

Zeolite production method

Inventors: Keiji Itabashi (Tokyo, JP); Tatsuya Okubo (Tokyo, JP); Yoshihiro Kamimura (Tokyo, JP); Shanmugam P. Elangovan (Tokyo, JP)
Assignees: UNIZEO CO., LTD.; The University of Tokyo
C01B39/46C01B39/02C01B39/026C01B39/26C01B39/36C01B39/365C01B39/38C01B39/42
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Quick Facts
Patent No.
US 9,670,068
App. No.
13/807,080
Granted
Jun 6, 2017
Kind
B2
Abstract

Disclosed is a method for readily and inexpensively producing zeolite without using an organic structure-directing agent (organic SDA). Specifically disclosed is a method whereby a gel containing a silica source, an alumina source, an alkaline source and water is reacted with zeolite seed crystals, to produce a zeolite with the same kind of skeletal structure as the zeolite. The gel used is a gel of a composition whereby, when a zeolite is synthesized from this gel only, the synthesized zeolite comprises at least one of the kinds of composite building units of the target zeolite.

Claims (74)

1. A method of producing a zeolite comprising:

reacting a gel and zeolite seed crystals to produce a zeolite having the same kind of skeletal structure as the zeolite seed crystals;

wherein:

the gel comprises a silica source, an alumina source, an alkali source and water;

the gel is capable of synthesizing a zeolite without the use of the zeolite seed crystals, wherein the zeolite synthesized without the use of the zeolite seed crystals has a different kind of skeletal structure than the zeolite seed crystals and comprises one or more building units of zeolite;

the zeolite seed crystals comprise one or more composite building units of zeolite;

the zeolite seed crystals and the zeolite synthesized without the use of zeolite seed crystals comprise at least one equivalent composite building unit of zeolite;

MFI zeolite, MEL zeolite, MSE zeolite, MTW zeolite, TUN zeolite, MFS zeolite, MOZ zeolite, EON zeolite, or LTF zeolite is used as the zeolite seed crystals;

and wherein the reacting step occurs without the use of an organic structure-directing agent.

2. The method of producing a zeolite according to claim 1 ,

wherein the zeolite produced is MFI zeolite,

MFI zeolite is used as the zeolite seed crystals, and

the gel has a composition which forms a mordenite zeolite, when the zeolite is synthesized from the gel without the use of the zeolite seed crystals.

3. The method of producing a zeolite according to claim 2 ,

wherein a gel having a composition shown in the following (a) or (b) is used as the gel,

(a)

SiO 2 /Al 2 O 3 =40 to 200,

Na 2 O/SiO 2 =0.24 to 0.4,

H 2 O/SiO 2 =10 to 50,

(b)

SiO 2 /Al 2 O 3 =10 to 40,

Na 2 O/SiO 2 =0.05 to 0.25,

H 2 O/SiO 2 =5 to 50.

4. The method of producing a zeolite according to claim 3 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

5. The method of producing a zeolite according to claim 2 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

6. The method of producing a zeolite according to claim 1 ,

wherein the zeolite produced is MEL zeolite,

MEL zeolite is used as the zeolite seed crystals, and

the gel has a composition which forms a mordenite zeolite, when the zeolite is synthesized from the gel without the use of the zeolite seed crystals.

7. The method of producing a zeolite according to claim 6 ,

wherein a gel having a composition shown in the following (a) or (b) is used as the gel,

(a)

SiO 2 /Al 2 O 3 =40 to 200,

Na 2 O/SiO 2 =0.24 to 0.4,

H 2 O/SiO 2 =10 to 50,

(b)

SiO 2 /Al 2 O 3 =10 to 40,

Na 2 O/SiO 2 =0.05 to 0.25,

H 2 O/SiO 2 =5 to 50.

8. The method of producing a zeolite according to claim 7 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

9. The method of producing a zeolite according to claim 6 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

10. The method of producing a zeolite according to claim 1 ,

wherein the zeolite produced is MSE zeolite,

MSE zeolite is used as the zeolite seed crystals, and

the gel has a composition which forms a mordenite zeolite, when the zeolite is synthesized from the gel without the use of the zeolite seed crystals.

11. The method of producing a zeolite according to claim 10 ,

wherein a gel having a composition shown in the following (a) or (b) is used as the gel,

(a)

SiO 2 /Al 2 O 3 =40 to 200,

(Na 2 O+K 2 O)/SiO 2 =0.24 to 0.4,

K 2 O/(Na 2 O+K 2 O)=0 to 0.7,

H 2 O/SiO 2 =10 to 50,

(b)

SiO 2 /Al 2 O 3 =10 to 40,

(Na 2 O+K 2 O)/Sio 2 =0.05 to 0.25,

K 2 O/(Na 2 O+K 2 O)=0 to 0.7,

H 2 O/SiO 2 =5 to 50.

12. The method of producing a zeolite according to claim 10 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

13. The method of producing a zeolite according to claim 1 ,

wherein the zeolite produced is MTW zeolite,

MTW zeolite is used as the zeolite seed crystals, and

the gel has a composition which forms an MFI zeolite, when the zeolite is synthesized from the gel without the use of the zeolite seed crystals.

14. The method of producing a zeolite according to claim 13 ,

wherein a gel having a composition shown below is used as the gel,

SiO 2 /Al 2 O 3 =10 to 150,

Na 2 O/SiO 2 =0.075 to 0.23,

H 2 O/SiO 2 =5 to 50.

15. The method of producing a zeolite according to claim 1 ,

wherein, as a post treatment, dealumination of the zeolite is carried out by mixing the zeolite and an aqueous solution of citric acid or a salt thereof, and heating a mixed aqueous solution under an autogenous pressure.

Assignments (4)
CHANGE OF NAME Recorded Mar 31, 2026
From: MITSUI MINING AND SMELTING COMPANY, LIMITED
To: MITSUI KINZOKU COMPANY, LIMITED
Reel/Frame 075357/0342 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 7, 2018
From: UNIZEO CO., LTD.
To: MITSUI MINING & SMELTING CO., LTD.
Reel/Frame 045133/0772 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 10, 2014
From: NIPPON CHEMICAL INDUSTRIAL CO., LTD.
To: UNIZEO CO., LTD.
Reel/Frame 032392/0517 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 5, 2013
From: ITABASHI, KEIJI; OKUBO, TATSUYA; KAMIMURA, YOSHIHIRO; ELANGOVAN, SHANMUGAM P.
To: NIPPON CHEMICAL INDUSTRIAL CO., LTD.; THE UNIVERSITY OF TOKYO
Reel/Frame 029922/0518 →
Priority Claims (3)
JP 2010-151489 · Jul 1, 2010 · national
JP 2010-260929 · Nov 24, 2010 · national
JP 2011-140636 · Jun 24, 2011 · national
Continuity (1)
Related Publication 20130156690A1 · Jun 20, 2013