Process for the large-scale manufacture of zeolite-templated carbon

Patent metadata

Field	Value
Publication number	US-11208327-B2
Application number	US-202016741885-A
Country	US
Kind code	B2
Filing date	Jan 14, 2020
Priority date	Jan 14, 2020
Publication date	Dec 28, 2021
Grant date	Dec 28, 2021

Abstract

A method for the large-scale synthesis of a zeolite-templated carbon (ZTC). The method includes the steps of: introducing a bed material comprising a zeolite to a fluidized bed reactor and heating the bed material to a temperature between 550° C. and 800° C.; fluidizing the bed material with a fluidizing gas and maintaining the temperature of the bed material between 550° C. and 800° C.; introducing an organic carbon precursor while fluidizing the zeolite for a period of time such that carbon is deposited on the zeolite by chemical vapor deposition to produce a zeolite-carbon composite; and treating the zeolite-carbon composite with an acid solution such that the zeolite template is dissolved and the ZTC is obtained.

First claim

What is claimed is:

1. A method for large-scale synthesis of a zeolite-templated carbon (ZTC), the method comprising the steps of:
introducing a bed material comprising a zeolite to a fluidized bed reactor and heating the bed material to a first temperature between 550 degrees Celsius (° C.) and 800° C.;
fluidizing the bed material with a fluidizing gas and maintaining the temperature of the bed material between 550° C. and 800° C.;
introducing an organic carbon precursor while fluidizing the zeolite for a first period of time such that carbon is deposited on the zeolite by chemical vapor deposition to produce a zeolite-carbon composite;
treating the zeolite-carbon composite with an acid solution such that the zeolite is dissolved and the ZTC is obtained.

2. The method of claim 1 , wherein at least 100 grams of the ZTC is obtained.

3. The method of claim 1 , wherein the fluidizing gas has an average gas velocity in the fluidized bed reactor that is between 5 centimeters per second (cm/s) and 25 cm/s.

4. The method of claim 1 , wherein the step of fluidizing the bed material further comprises introducing the fluidizing gas such that the bed material is fluidized in a bubbling fluidization regime.

5. The method of claim 1 , wherein the zeolite is a bead-type zeolite having a diameter between 100 micrometers (μm) and 1,000 μm.

6. The method of claim 1 , wherein the organic carbon precursor comprises a molecule selected from the group consisting of: acetylene, ethylene, ethane, propylene, ethanol, and combinations of the same.

7. The method of claim 1 , wherein the first period of time during which the bed material is fluidized with the organic carbon precursor is between 1 hour and 6 hours.

8. The method of claim 1 , wherein the zeolite has a FAU structure and a ratio of silicon to aluminum that is between 1 and 1.4.

9. The method of claim 1 , wherein the step of treating the zeolite-carbon composite with the acid solution further comprises maintaining pH of the acid solution between 2.5 and 3.5.

10. The method of claim 1 , further comprising filtering the ZTC from the acid solution, and washing and drying the ZTC.

11. The method of claim 10 , wherein the step of drying the ZTC comprises heating the ZTC to a second temperature between 80° C. and 120° C. for a second period of time that is between 1 hour and 24 hours.

12. A method for recovering a zeolite from a dissolved zeolite acid solution byproduct, the method comprising the steps of:
synthesizing a zeolite-carbon composite by chemical vapor deposition on the zeolite, the zeolite having a FAU structure and a ratio of silicon to aluminum that is between 1 and 1.4, the zeolite-carbon composite comprising a ZTC on the zeolite;
dissolving the zeolite with a fluorine-free acid solution to obtain the ZTC and produce the dissolved zeolite acid solution;
neutralizing the dissolved zeolite acid solution with a base to precipitate an amorphous aluminosilicate;
crystallizing the amorphous aluminosilicate to obtain the zeolite.

13. The method of claim 12 , further comprising recycling the zeolite for use in synthesizing the ZTC.

14. The method of claim 12 , wherein the step of synthesizing the zeolite-carbon composite by chemical vapor deposition on the zeolite further comprises introducing an organic carbon precursor comprising a molecule selected from the group consisting of: acetylene, ethylene, ethane, propylene, ethanol, and combinations of the same.

15. The method of claim 12 , wherein the fluorine-free acid solution comprises a mineral acid selected from the group consisting of: hydrochloric acid, sulfuric acid, phosphoric acid, and combinations of the same.

16. The method of claim 12 , wherein the zeolite comprises NaX zeolite.

17. The method of claim 12 , wherein the step of dissolving the zeolite with the fluorine-free acid solution further comprises maintaining pH of the fluorine-free acid solution between 2.5 and 3.5.

18. The method of claim 12 , wherein the step of synthesizing the zeolite-carbon composite by chemical vapor deposition on the zeolite is carried out in a fluidized bed reactor.

19. The method of claim 18 , wherein the fluidized bed reactor is operated such that the zeolite is fluidized in a bubbling fluidization regime.

20. The method of claim 12 , wherein at least 100 grams of the ZTC is obtained.

Assignees

• Saudi Arabian Oil Co
• Korea Advanced Inst Sci & Tech

Inventors

• Wang Yuguo
• Othman Rashid M
• Choi Minkee
• Choi Seokin

Classifications

• B01J2208/00548

  Flow · CPC title

• C01P2006/16

  Pore diameter · CPC title

• C01B32/05 Primary

  Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30 · CPC title

• B01J2219/00006

  Large-scale industrial plants · CPC title

• C01B32/00 Primary

  Carbon; Compounds thereof (C01B21/00, C01B23/00 take precedence; percarbonates C01B15/10; carbon black C09C1/48) · CPC title