Simultaneous reaction and separation of chemicals

Patent metadata

Field	Value
Publication number	US-11814285-B2
Application number	US-201816764226-A
Country	US
Kind code	B2
Filing date	Nov 16, 2018
Priority date	Nov 16, 2017
Publication date	Nov 14, 2023
Grant date	Nov 14, 2023

Abstract

The reaction rate of hydrocarbon pyrolysis can be increased to produce solid carbon and hydrogen by the use of molten materials which have catalytic functionality to increase the rate of reaction and physical properties that facilitate the formation and contamination-free separation of the solid carbon. Processes, materials, reactor configurations, and conditions are disclosed whereby methane and other hydrocarbons can be decomposed at high reaction rates into hydrogen gas and carbon products without any carbon oxides in a single reaction step. The process also makes use of specific properties of selected materials with unique solubilities and/or wettability of products into (and/or by) the molten phase to facilitate generation of purified products and increased conversion in more general reactions.

First claim

We claim:

1. A multiphase reaction system comprising:
a reactor vessel, the reactor vessel comprising:
a feed stream comprising one or more hydrocarbon gas phase reactants;
liquid phases comprising a first liquid and a second liquid, the first liquid comprising a molten metal or a metalloid, and the second liquid comprising a molten salt, wherein the molten salt is disposed as a separate phase on top of the molten metal or the metalloid;
a solid phase disposed within the liquid phases; and
one or more products, wherein the one or more products comprise solid carbon and hydrogen, wherein the solid phase and the solid carbon are different, and wherein the solid carbon is accumulated on top of the molten salt.

2. The multiphase reaction system of claim 1 , wherein the solid phase comprises a solid phase catalyst.

3. The multiphase reaction system of claim 1 , wherein the solid phase is assembled as a packed bed of solid particles or pellets with the liquid phases between the solid particles or the pellets, and wherein the solid particles or the pellets have catalytic activity to the one or more gas phase reactants.

4. The multiphase reaction system of claim 1 , wherein the solid phase comprises a metal, wherein the metal comprises nickel, iron, cobalt, copper, platinum, ruthenium, rhodium, or any combination thereof.

5. The multiphase reaction system of claim 1 , wherein the solid phase comprises a mixed metal oxide, wherein the mixed metal oxide comprises titanium oxide, zirconia, tungsten oxide, or any combination thereof.

6. The multiphase reaction system of claim 5 , wherein the solid phase is supported on alumina, silica, zirconia, or any combination thereof.

7. The multiphase reaction system of claim 1 , wherein the molten salt comprises NaCl, NaBr, KCl, KBr, LiCl, LiBr, CaCl 2 , MgCl 2 , CaBr 2 , MgBr 2 , or any combination thereof.

8. The multiphase reaction system of claim 1 , further comprising:
a gas inlet configured to introduce a gas stream into the reactor vessel above the liquid phases; entrain at least a portion of the solid carbon in the gas stream; and
remove the portion of the solid carbon from the reactor vessel in the gas stream.

9. The multiphase reaction system of claim 1 , wherein the molten metal comprises Ni, Co, Fe, Pd, Cu, Pt, Al, Sn, Pb, Au, Ag, In, Ga, Te, Bi, Sb, or any mixture thereof.

10. The system of claim 1 , wherein the molten metal or the metalloid has catalytic properties towards a reaction of the one or more hydrocarbon gas phase reactants.

11. The system of claim 1 , wherein the molten salt has a lower density than that of the molten metal or the metalloid.

12. A multiphase reaction method, the method comprising:
contacting one or more gas phase reactants with a solid phase disposed within liquid phases in a reactor, wherein the liquid phases comprises a first liquid and a second liquid, wherein the first liquid comprises a molten metal or a metalloid, wherein the second liquid comprises a molten salt, wherein the molten salt is disposed as a separate phase on top of the molten metal or the metalloid, wherein the one or more gas phase reactants comprise a hydrocarbon, and wherein the solid phase comprises a solid phase catalyst; and
producing one or more reaction products in response to contacting the one or more gas phase reactants with the solid phase, wherein the one or more reaction products comprise solid carbon and hydrogen, and wherein the solid carbon is accumulated on top of the molten salt.

13. The method of claim 12 , further comprising:
solvating or removing at least a portion of the one or more reaction products on the solid phase with the liquid phases, wherein the one or more reaction products solvated or removed with the liquid phases comprise at least a portion of the solid carbon; and
separating at least the portion of the one or more reaction products from the one or more gas phase reactants in response to the solvating or the removing.

14. The method of claim 12 , wherein the solid phase is assembled as a packed bed of solid particles or pellets with the liquid phase between the solid particles or the pellets, and wherein the solid particles or the pellets have catalytic activity to the one or more gas phase reactants.

15. The method of claim 12 , wherein the solid phase comprises a metal, wherein the metal comprises nickel, iron, cobalt, copper, platinum, ruthenium, rhodium, or any combination thereof.

16. The method of claim 15 , wherein the solid phase is supported on alumina, silica, zirconia, or any combination thereof.

17. The method of claim 12 , wherein the solid phase comprises a mixed metal oxide, wherein the mixed metal oxide comprises titanium oxide, zirconia, tungsten oxide, or any combination thereof.

18. The method of claim 12 , wherein the molten salt comprises NaCl, NaBr, KCl, KBr, LiCl, LiBr, CaCl 2 , MgCl 2 , CaBr 2 , MgBr 2 , or any combination thereof.

19. The multiphase reaction method of claim 12 , wherein the molten metal comprises Ni, Co, Fe, Pd, Cu, Pt, Al, Sn, Pb, Au, Ag, In, Ga, Te, Bi, Sb, or any mixture thereof.

20. The multiphase method of claim 12 , wherein the molten metal or the metalloid has catalytic properties towards a reaction of the one or more hydrocarbon gas phase reactants.

21. The method of claim 12 , wherein the molten salt has a lower density than that of the molten metal or the metalloid.

Assignees

• Univ California

Inventors

• Mcfarland Eric W
• Upham Ches
• Zeng Jiren
• Palmer Clarke
• Su Shizhao
• Mannini Davide
• Kang Dohyung
• Rahimi Nazanin
• Metiu Horia
• Gordon Michael

Classifications

• C01B3/26 Primary

  using catalysts · CPC title

• B01J8/0278

  Feeding reactive fluids (for solid material B01J8/0015) · CPC title

• B01J23/825

  with gallium, indium or thallium · CPC title

• B01J23/8437

  Bismuth · CPC title

• B01J27/08

  Halides · CPC title