Zeolite production method

Patent metadata

Field	Value
Publication number	US-2017267536-A1
Application number	US-201715492361-A
Country	US
Kind code	A1
Filing date	Apr 20, 2017
Priority date	Jul 1, 2010
Publication date	Sep 21, 2017
Grant date	—

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.

First claim

1 - 14 . (canceled)

15 . 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 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;
wherein the reacting step occurs without the use of an organic structure-directing agent;
wherein the gel has a composition of:
SiO 2 /Al 2 O 3 =10 to 14.

16 . The method of producing a zeolite according to claim 15 ,
wherein the zeolite synthesized without the use of zeolite seed crystals has a different kind of skeletal structure as the zeolite seed crystals.

17 . The method of producing a zeolite according to claim 16 ,
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.

18 . The method of producing a zeolite according to claim 17 ,
wherein the gel has a composition of: SiO 2 /Al 2 O 3 =10 to 14, Na 2 O/SiO 2 =0.05 to 0.25, H 2 O/SiO 2 =5 to 50.

19 . The method of producing a zeolite according to claim 16 ,
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.

20 . The method of producing a zeolite according to claim 19 ,
wherein the gel has a composition of: SiO 2 /Al 2 O 3 =10 to 14, Na 2 O/SiO 2 =0.05 to 0.25, H 2 O/SiO 2 =5 to 50.

21 . The method of producing a zeolite according to claim 16 ,
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.

22 . The method of producing a zeolite according to claim 21 ,
wherein the gel has a composition of: SiO 2 /Al 2 O 3 =10 to 14, (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.

23 . The method of producing a zeolite according to claim 16 ,
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.

24 . The method of producing a zeolite according to claim 23 ,
wherein the gel has a composition of: SiO 2 /Al 2 O 3 =10 to 14, Na 2 O/SiO 2 =0.075 to 0.23, H 2 O/SiO 2 =5 to 50.

25 . The method of producing a zeolite according to claim 16 ,
wherein the zeolite produced is beta zeolite, beta 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.

26 . The method of producing a zeolite according to claim 25 ,
wherein the gel has a composition of: SiO 2 /Al 2 O 3 =10 to 14, Na 2 O/SiO 2 =0.05 to 0.25, H 2 O/SiO 2 =5 to 50,

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

28 . The method of producing a zeolite according to claim 27 ,
wherein beta zeolite is used as the zeolite.

29 . The method of producing a zeolite according to claim 16 ,
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.

30 . The method of producing a zeolite according to claim 17 ,
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.

31 . The method of producing a zeolite according to claim 18 ,
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.

32 . The method of producing a zeolite according to claim 19 ,
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.

33 . The method of producing a zeolite according to claim 20 ,
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.

34 . The method of producing a zeolite according to claim 21 ,
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.

Assignees

• Unizeo Co Ltd
• Univ Tokyo

Inventors

• Itabashi Keiji
• Okubo Tatsuya
• Kamimura Yoshihiro
• Elangovan Shanmugam Palani

Classifications

• C01B39/36

  Pentasil type, e.g. types ZSM-5, ZSM-8 or ZSM-11 · CPC title

• C01B39/365

  Type ZSM-8; Type ZSM-11; ZSM 5/11 intermediate · CPC title

• C01P2002/72

  by d-values or two theta-values, e.g. as X-ray diagram · CPC title

• C01B39/26

  Mordenite type {(C01B39/023, C01B39/026, C01B39/06 take precedence)} · CPC title

• C01B39/46 Primary

  Other types characterised by their X-ray diffraction pattern and their defined composition {(C01B39/023, C01B39/026, C01B39/06 take precedence)} · CPC title