Nanoparticle catalyst capable of forming aromatic hydrocarbons from CO2 and H2

Patent metadata

Field	Value
Publication number	US-9555405-B2
Application number	US-201514603628-A
Country	US
Kind code	B2
Filing date	Jan 23, 2015
Priority date	Jul 24, 2012
Publication date	Jan 31, 2017
Grant date	Jan 31, 2017

Abstract

Nanocatalysts and methods of using the same to obtain aromatic hydrocarbon compounds from a source of carbon atoms and a source of hydrogen atoms in a single reaction step is provided. The catalyst comprises an Fe/Fe 3 O 4 nanocatalyst that may be supported on a non-reactive support material such as a zeolite or alumina CO 2 and H 2 are preferred sources of carbon and hydrogen atoms for the reaction. The aromatic hydrocarbon compounds produced are suitable for direct usage as fuel without need for further refining.

First claim

We claim:

1. A method of synthesizing one or more aromatic hydrocarbon compounds comprising:
providing within a reactor a quantity of a catalytic material comprising Fe/Fe 3 O 4 core/shell nanoparticles;
introducing into said reactor and contacting said catalytic material with a quantity of reactants comprising a source of carbon atoms and a source of hydrogen atoms;
reacting said reactants within said reactor under conditions for forming said one or more aromatic hydrocarbon compounds; and
recovering said one or more aromatic hydrocarbon compounds from said reactor.

2. The method according to claim 1 , wherein said source of carbon atoms is selected from the group consisting of a biomass material, CO 2 , CO, and combinations thereof.

3. The method according to claim 2 , wherein said source of carbon atoms comprises CO 2 and/or CO.

4. The method according to claim 2 , wherein said biomass material comprises lignin.

5. The method according to claim 1 , wherein said source of hydrogen atoms is selected from the group consisting of H 2 , H 2 O, CH 4 , and combinations thereof.

6. The method according to claim 1 , wherein said reacting step within said reactor occurs at a pressure of between about 1 to about 100 atm.

7. The method according to claim 6 , wherein said reacting step within said reactor occurs at a pressure of between about 1 to about 1.1 atm.

8. The method according to claim 1 , wherein said reacting step within said reactor occurs at a temperature of between about 380° C. to about 560° C.

9. The method according to claim 1 , wherein said reactor operates as a batch reactor, said catalyst undergoing at least 10 reaction cycles prior to being regenerated.

10. The method according to claim 1 , wherein said one or more aromatic hydrocarbon compounds recovered from said reactor are selected from the group consisting of xylenes, toluene, benzene, and mixtures thereof.

11. The method according to claim 1 , wherein said one or more aromatic hydrocarbon compounds recovered from said reactor are directly usable as a fuel in an internal combustion engine upon recovery from said reactor without under going further refinement.

12. The method according to claim 1 , wherein said source of carbon atoms is not subjected to thermolysis prior to being introduced into said reactor.

13. The method according to claim 1 , wherein said nanoparticles are supported on a non-reactive support substrate.

14. The method according to claim 13 , wherein said non-reactive support substrate comprises a zeolite.

15. A method of synthesizing one or more aromatic hydrocarbon compounds comprising:
providing within a reactor a quantity of a catalytic material comprising Fe/Fe 3 O 4 core/shell nanoparticles;
introducing into said reactor and contacting said catalytic material with a quantity of reactants comprising a source of carbon atoms and a source of hydrogen atoms, said source of carbon atoms being selected from the group consisting of lignin, CO 2 , CO, and combinations thereof, said source of hydrogen atoms being selected from the group consisting of H 2 , H 2 O, CH 4 , and combinations thereof;
reacting said reactants within said reactor under conditions for forming said one or more aromatic hydrocarbon compounds, said conditions within said reactor comprise a temperature of between about 380° C. to about 560° C., and a pressure of between about 1 to about 1.1 atm; and
recovering said one or more aromatic hydrocarbon compounds from said reactor, said one or more aromatic hydrocarbon compounds being selected from the group consisting of xylenes, toluene, benzene, and mixtures thereof, said aromatic hydrocarbon compounds comprising at least 75% by weight of the total reaction products produced by said reacting step.

16. A system for synthesizing one or more aromatic hydrocarbon compounds comprising:
a reactor comprising a quantity of a catalytic material comprising Fe/Fe 3 O 4 core/shell nanoparticles;
one or more reactant feed streams coupled with said reactor and operable to deliver to said reactor a source of carbon atoms and a source of hydrogen atoms;
said reactor operating under conditions for reacting said source of carbon atoms and said source of hydrogen atoms in the presence of said catalytic material and forming said one or more aromatic hydrocarbon compounds; and
a reaction product discharge stream coupled with said reactor and operable to remove said one or more aromatic hydrocarbon compounds from said reactor.

17. The system according to claim 16 , wherein said nanoparticles are supported on a non-reactive support substrate.

18. The system according to claim 16 , wherein said reactor is a batch reactor, said catalytic material being capable of undergoing at least 10 reaction cycles prior to being replaced or regenerated.

19. The system according to claim 16 , wherein said reactor is a continuous reactor, and said source of carbon atoms comprises CO 2 , one mole of said catalytic material being capable of converting between 10,000 to 50,000 moles of CO 2 into said one or more hydrocarbon compounds before the catalyst needs to be regenerated.

20. The system according to claim 16 , wherein said reactor operates at a temperature of between about 380° C. to about 560° C., and a pressure of between about 1 to about 1.1 atm.

21. The system according to claim 16 , wherein said source of carbon atoms delivered to said reactor by said at least one reactant feed stream is selected from the group consisting of lignin, CO 2 , CO, and combinations thereof.

22. The system according to claim 16 , wherein said source of hydrogen atoms delivered to said reactor by said at least one reactant feed stream is selected from the group consisting of H 2 , H 2 O, CH 4 , and combinations thereof.

23. The system according to claim 16 , wherein said one or more aromatic hydrocarbon compounds removed from said reactor by said reaction product discharge stream are selected from the group consisting of xylenes, toluene, benzene, and mixtures thereof.

24. A catalytic material operable to catalyze a reaction resulting in the formation of one or more aromatic hydrocarbon compounds comprising: a plurality of iron/iron oxide core/shell nanoparticles having an average diameter of less than about 20 nm on a non-reactive support substrate, wherein said iron oxide consists of Fe 3 O 4 .

25. The catalytic material according to claim 24 , wherein said non-reactive support substrate comprises a zeolite.

26. The catalytic material according to claim 24 , wherein said nanoparticles comprise crystalline core and shell structures.

27. The catalytic material according to claim 24 , wherein said nanoparticles comprise an organic ligand monolayer adjacent said shell.

28. The catalytic material according to claim 24 , wherein said nanoparticles are free of silane coatings.

29. A catalytic material operable to catalyze a reaction resulting in the formation of one or more aromatic hydrocarbon compounds comprising: a plurality of Fe/Fe 3 O 4 core/shell nanoparticles having an average diameter of less than about 20 nm on a non-reactive support substrate, wherein said non-reactive support substrate comprises a zeolite.

30. A catalytic material operable to catalyze a reaction resulting in the formation of one or more aromatic hydrocarbon compounds comprising: a plurality of

Assignees

• Univ Kansas State

Inventors

• Wang Hongwang
• Bossmann Stefan H
• Wang Donghai
• Troyer Deryl L
• Shrestha Tej

Classifications

• B01J23/745 Primary

  Iron · CPC title

• B01J35/398

  Egg yolk like · CPC title

• B01J2235/30

  Scanning electron microscopy; Transmission electron microscopy · CPC title

• B01J35/45

  Nanoparticles · CPC title

• B01J2235/00

  Indexing scheme associated with group B01J35/00, related to the analysis techniques used to determine the catalysts form or properties · CPC title