IP Library Granted Patent US 9,108,187
Granted Patent B2
US 9,108,187 · App. 13/979,670 · Granted Aug 18, 2015

Fe(II)-substituted beta type zeolite, gas adsorbent containing same and method for producing same, and method for removing nitrogen monoxide and hydrocarbon

Inventors: Masaru Ogura (Tokyo, JP); Keiji Itabashi (Tokyo, JP); Tatsuya Okubo (Tokyo, JP); Shanmugam Palani Elangovan (Tokyo, JP)
Assignees: UNIZEO CO., LTD.; THE UNIVERSITY OF TOKYO
B01J20/3085B01D53/02B01J20/28061B01J20/28071C01B39/065C01B39/46B01D2253/108B01D2253/1085B01D2253/306B01D2253/311B01D2257/404B01D2257/702B01D2258/01C01P2006/12C01P2006/14F01N3/0835F01N3/0842
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Quick Facts
Patent No.
US 9,108,187
App. No.
13/979,670
Granted
Aug 18, 2015
Kind
B2
Abstract

To provide an Fe(II)-substituted beta type zeolite which has been ion-exchanged with Fe(II) ions and can effectively adsorb and remove nitrogen monoxide or hydrocarbon contained in gas to be cleaned, even if oxygen is present in the gas at a high concentration or the temperature of the gas is low. In the Fe(II)-substituted beta type zeolite, a ratio of SiO 2 /Al 2 O 3 is preferably 10 to 18, a BET specific surface area is preferably 400 m 2 /g to 700 m 2 /g, a micropore specific surface area is preferably 290 m 2 /g to 500 m 2 /g, and a micropore volume is preferably 0.15 cm 3 /g to 0.25 cm 3 /g. The amount of Fe(II) supported is preferably 0.01% by mass to 6.5% by mass based on the Fe(II)-substituted beta type zeolite.

Claims (21)

1. An Fe(II)-substituted beta type zeolite which has been ion-exchanged with Fe(II) ions,

wherein a ratio of SiO 2 /Al 2 O 3 is 10 to 18, a BET specific surface area is 400 m 2 /g to 700 m 2 /g, a micropore specific surface area is 290 m 2 /g to 500 m 2 /g, and a micropore volume is 0.15 cm 3 /g to 0.25 cm 3 /g.

2. The Fe(II)-substituted beta type zeolite according to claim 1 ,

wherein the amount of Fe(II) supported is 0.01% by mass to 6.5% by mass based on the Fe(II)-substituted beta type zeolite.

3. The Fe(II)-substituted beta type zeolite according to claim 1 that uses, as a beta type zeolite which has not yet been ion-exchanged with Fe(II) ions, a beta type zeolite in which a ratio of SiO 2 /Al 2 O 3 is 10 to 16, a BET specific surface area that is measured in a state of a sodium-type is 500 m 2 /g to 700 m 2 /g, a micropore specific surface area is 350 m 2 /g to 500 m 2 /g, and a micropore volume is 0.15 cm 3 /g to 0.25 cm 3 /g.

4. The Fe(II)-substituted beta type zeolite according to claim 3 that uses, as a beta type zeolite of which has not yet been ion-exchanged with Fe(II) ions, a beta type zeolite which is obtained by

(1) mixing a silica source, an alumina source, and an alkali source with water to obtain a reaction mixture having a composition represented by the following molar ratio,

SiO 2 /Al 2 O 3 =40 to 200

Na 2 O/SiO 2 =0.22 to 0.4

H 2 O/SiO 2 =10 to 50

(2) using, as a seed crystal, a beta type zeolite which has a ratio of SiO 2 /Al 2 O 3 of 8 to 30 and does not contain an organic compound having an average particle size of 150 nm or larger, and adding the seed crystal to the reaction mixture in a proportion of 0.1% by mass to 20% by mass based on a silica component in the reaction mixture, and

(3) heating the reaction mixture, to which the seed crystal has been added, at 100° C. to 200° C. in a sealed state.

5. A gas adsorbent containing the Fe(II)-substituted beta type zeolite according to claim 1 .

6. The gas adsorbent according to claim 5 that is used for adsorbing nitrogen monoxide.

7. The gas adsorbent according to claim 5 that is used for adsorbing hydrocarbon.

8. A method for producing an Fe(II)-substituted beta type zeolite, comprising:

a step of causing Fe(II) ions to be supported on a beta type zeolite by dispersing the beta type zeolite, in which a ratio of SiO 2 /Al 2 O 3 is 10 to 16, a BET specific surface area that is measured in a state of sodium type is 500 m 2 /g to 700 m 2 /g, a micropore specific surface area is 350 m 2 /g to 500 m 2 /g, and a micropore volume is 0.15 cm 3 /g, to 0.25 cm 3 /g, in an aqueous solution of a water-soluble divalent iron compound, and performing mixing under stirring.

9. The production method according to claim 8 ,

wherein during the mixing under stirring, ascorbic acid of a mole number that is 0.1 to 3 times greater than that of the divalent iron is added to the aqueous solution.

10. A method for removing nitrogen monoxide and/or hydrocarbon, comprising:

causing the nitrogen monoxide to be adsorbed and/or the hydrocarbon to be adsorbed onto an Fe(II)-substituted beta type zeolite by bringing the nitrogen monoxide or nitrogen monoxide-containing gas and/or the hydrocarbon or hydrocarbon-containing gas into contact with the Fe(II)-substituted beta type zeolite which has been ion-exchanged with Fe(II) ions and in which a ratio of SiO 2 /Al 2 O 3 is 10 to 18, a BET specific surface area is 400 m 2 /g to 700 m 2 /g, a micropore specific surface area is 290 m 2 /g to 500 m 2 /g, and a micropore volume is 0.15 cm 3 /g to 0.25 cm 3 /g.

Assignments (3)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jan 23, 2018
From: UNIZEO CO., LTD.
To: MITSUI MINING & SMELTING CO., LTD.; THE UNIVERSITY OF TOKYO
Reel/Frame 045127/0009 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Mar 6, 2014
From: NIPPON CHEMICAL INDUSTRIAL CO., LTD.
To: UNIZEO CO., LTD.
Reel/Frame 032369/0028 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 10, 2013
From: OGURA, MASARU; ITABASHI, KEIJI; OKUBO, TATSUYA; ELANGOVAN, SHANMUGAM PALANI
To: NIPPON CHEMICAL INDUSTRIAL CO., LTD.; THE UNIVERSITY OF TOKYO
Reel/Frame 031174/0674 →
Priority Claims (2)
JP 2011-008186 · Jan 18, 2011 · national
JP 2012-002938 · Jan 11, 2012 · national
Continuity (1)
Related Publication 20140157987A1 · Jun 12, 2014