Systems and methods for preparing nano-sized crystals of BEA zeolite

Patent metadata

Field	Value
Publication number	US-11345605-B2
Application number	US-201916684360-A
Country	US
Kind code	B2
Filing date	Nov 14, 2019
Priority date	Nov 14, 2019
Publication date	May 31, 2022
Grant date	May 31, 2022

Abstract

Methods and systems for production of consistently-sized BEA zeolite nano-crystals, the method including mixing an emulsion, the emulsion comprising a surfactant and an organic solvent; heating the emulsion; mixing a zeolite solution, the zeolite solution comprising a silicon-containing compound and an aluminum-containing compound; heating the zeolite solution; adding the emulsion to the zeolite solution drop-wise over time to create an zeolite emulsion solution mixture; heating the zeolite emulsion solution mixture; and precipitating the consistently-sized BEA zeolite nano-crystals.

First claim

The invention claimed is:

1. A method for production of consistently-sized BEA zeolite nano-crystals, the method comprising the steps of:
mixing a surfactant and an organic solvent to form a mixture;
heating the mixture, where the step of heating the mixture is carried out at between about 55° C. and about 70° C.;
mixing a zeolite solution, the zeolite solution comprising a silicon-containing compound and an aluminum-containing compound;
heating the zeolite solution;
adding the mixture to the zeolite solution drop-wise over time to create a zeolite emulsion solution mixture;
heating the zeolite emulsion solution mixture; and
precipitating the consistently-sized BEA zeolite nano-crystals, in a range between about 40 nm and about 500 nm.

2. The method according to claim 1 , where the step of mixing the zeolite solution further comprises the step of controlling a ratio of the silicon-containing compound to the aluminum-containing compound, and where the step of adding the mixture to the zeolite solution comprises controlling a ratio of the mixture to the zeolite solution to precipitate the consistently-sized BEA zeolite nano-crystals.

3. The method according to claim 1 , where the surfactant comprises at least one component selected from the group consisting of: polyoxyethylene(15)oleyl ether, polyoxyethylene(20)oleyl ether, and combinations of the same.

4. The method according to claim 1 , where the organic solvent comprises at least one component selected from the group consisting of: cyclohexane, hexane, heptane, octane, dimethyl pentane, methyl hexane, methyl cyclohexane, methyl cylcopentane, and combinations of the same.

5. The method according to claim 1 , where the organic solvent is contained in an amount of between about 5 wt. % to about 40 wt. % of the mixture.

6. The method according to claim 1 , where the step of mixing a zeolite solution comprises controlling a molar ratio of silicon to aluminum to be between about 5 to about 50.

7. The method according to claim 1 , where the silicon-containing compound comprises colloidal silica and the aluminum-containing compound comprises sodium aluminate.

8. The method according to claim 1 , where the step of mixing the zeolite solution comprises heating the zeolite solution to between about 15° C. to about 35° C.

9. The method according to claim 1 , where the step of adding the mixture to the zeolite solution drop-wise comprises heating to between about 50° C. and about 75° C.

10. The method according to claim 1 , where the step of adding the mixture to the zeolite solution drop-wise over time occurs with mixture addition at between about 0.01 kg/min. to about 0.1 kg/min. and where after the step of adding the mixture to the zeolite solution drop-wise over time, the total weight of the emulsion is of between about 5 wt. % and about 40 wt. % of the weight of the zeolite solution.

11. The method according to claim 1 , where the step of adding the mixture to the zeolite solution drop-wise over time includes mixing the mixture and the zeolite solution for between about 1 hour to about 3 hours at a stirring speed between about 300 rpm to about 700 rpm and a temperature between about 50° C. to about 75° C.

12. The method according to claim 1 , where the step of heating the zeolite emulsion solution mixture is carried out at between about 145° C. and about 155° C. for a period of between about 68 hours and 76 hours.

13. The method according to claim 1 , where the step of heating the zeolite emulsion solution mixture includes the step of increasing the temperature from between about 50° C. and about 75° C. to reach about 150° C. at a heating rate of between about 1° C./min. and about 5° C./min.

14. The method according to claim 1 , further comprising the step of cooling the zeolite emulsion solution mixture to between about 15° C. to about 50° C. after the step of heating the zeolite emulsion solution mixture.

15. The method according to claim 1 , further comprising the step of washing the consistently-sized BEA zeolite nano-crystals.

16. The method according to claim 1 , further comprising the step of drying the consistently-sized BEA zeolite nano-crystals.

17. The method according to claim 16 , where the step of drying is carried out isothermally for between about 15 to about 20 hours at about 100° C.

18. The method according to claim 1 , further comprising the steps of separating aqueous solution, the surfactant, and the organic solvent via heating and recycling the surfactant for use in the step of mixing the surfactant and the organic solvent.

19. The method according to claim 1 , further comprising the step of characterizing the size range of the consistently-sized BEA zeolite nano-crystals via X-ray diffraction, scanning electron microscopy, or a combination of the same.

Assignees

• Saudi Arabian Oil Co
• Univ King Fahd Pet & Minerals

Inventors

• Al-Shafei Emad Naji
• Muraza Oki
• Ahmed Mohamed
• Choi Ki-Hyouk
• Yamani Zain Hassan

Classifications

• B01J35/45

  Nanoparticles · CPC title

• B01J35/40

  characterised by dimensions, e.g. grain size (in a colloidal state B01J35/23; crystallite size B01J35/77) · CPC title

• C01P2004/03

  obtained by SEM · CPC title

• C01P2004/64

  Nanometer sized, i.e. from 1-100 nanometer · CPC title

• B01J2229/40

  Special temperature treatment, i.e. other than just for template removal · CPC title