IP Library Granted Patent US 11,873,219
Granted Patent B2
US 11,873,219 · App. 17/045,961 · Granted Jan 16, 2024

Process for producing hydrogen and carbon products

Inventors: Leonardo Spanu (Houston, TX); Carolus Matthias Anna Maria Mesters (Houston, TX)
Assignee: SHELL USA, INC.
C01B3/30B01J23/755C01B3/56C01B32/162H01J49/067H01J49/105H01J49/24C01B2203/0277
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Quick Facts
Patent No.
US 11,873,219
App. No.
17/045,961
Granted
Jan 16, 2024
Kind
B2
Abstract

A method of operating a mass spectrometer vacuum interface, the vacuum interface comprising an evacuated expansion chamber downstream of a plasma ion source at atmospheric or relatively high pressure, the expansion chamber having a first aperture that interfaces with the plasma ion source to form an expanding plasma downstream of the first aperture and a second aperture downstream of the first aperture from the plasma for skimming the expanding plasma to form a skimmed expanding plasma; wherein the expansion chamber is pumped by an interface vacuum pump to provide an interface pressure in the chamber; the method comprising using a controller to automatically, or according to user input, control the throughput of the interface vacuum pump to control the interface pressure dependent on one or more operating modes of the spectrometer. A pressure gauge can be located in the expansion chamber and a feedback loop provided between the pressure gauge and controller.

Claims (27)

1. A process comprising:

a. converting natural gas in a first reaction zone under first reaction conditions to produce a first gas stream and a first carbon product;

b. separating at least a portion of the first carbon product from the first gas stream; and

c. converting at least a portion of the first gas stream in a second reaction zone under second reaction conditions to produce a second gas stream and a second carbon product,

wherein the second reaction zone comprises a molten metal and/or molten salt.

2. The process of claim 1 , wherein the first reaction zone is a fluidized bed reactor.

3. The process of claim 1 , wherein the first reaction zone contains a supported catalyst.

4. The process of claim 1 , wherein the first reaction zone contains a catalyst comprising a transition metal or transition metal compound.

5. The process of claim 4 wherein the transition metal compound is iron, nickel or cobalt.

6. The process of claim 1 , wherein the first reaction conditions comprise a temperature greater than 600° C.

7. The process of claim 1 , wherein the first reaction conditions comprise a temperature in the range of from 700 to 1300° C.

8. The process of claim 1 , wherein the natural gas conversion in the first reaction zone is carried out in the absence of oxygen and water.

9. The process of claim 1 , wherein the natural gas comprises methane and the first reaction conditions are selected such that the amount of methane converted in the first reaction zone is from about 3 to about 25 wt %.

10. The process of claim 1 , wherein the first gas stream comprises hydrogen and methane.

11. The process of claim 1 , wherein the first carbon product comprises carbon nanotubes.

12. The process of claim 1 , wherein the separation is carried out in a cyclone or electrostatic precipitator.

13. The process of claim 1 , wherein the molten metal is selected from the group consisting of iron, cobalt, nickel, tin, bismuth, indium, gallium, copper, lead, molybdenum, tungsten and mixtures thereof.

14. The process of claim 1 , wherein the molten salt is selected from the group consisting of lithium chloride, sodium chloride, potassium chloride, cesium chloride, magnesium chloride, calcium chloride, strontium chloride, barium chloride and mixtures thereof.

15. The process of claim 1 , wherein the second reaction conditions comprise a temperature in the range of from 600 to 1300° C.

16. The process of claim 1 , wherein the second reaction conditions are selected such that the amount of methane converted in the second reaction zone is from about 50 to about 100 wt %.

17. The process of claim 1 , wherein the second gas stream contains at least 50 vol % hydrogen.

18. The process of claim 1 , wherein the second carbon product has a lower density than the molten metal and/or molten salt.

19. The process of claim 1 , further comprising separating the second carbon product from the molten metal and/or molten salt.

20. A process for producing hydrogen and solid carbon comprising:

a. contacting natural gas with a catalyst selected from the group consisting of iron, nickel, cobalt and mixtures thereof in a first reaction zone wherein the temperature is in a range of from 700 to 1200° C. to produce a first gas stream comprising hydrogen and unreacted natural gas and a first solid carbon product comprising carbon nanotubes;

b. separating at least a portion of the carbon nanotubes from the first gas stream in a gas/solid separation apparatus; and

passing at least a portion of the unreacted natural gas and hydrogen through a second reaction zone comprising a molten salt/metal bed wherein the molten salt/metal bed comprises metals selected from the group consisting of iron, cobalt, nickel, tin, bismuth, indium, gallium, copper, lead, molybdenum, and tungsten, or salts selected from the group consisting of alkaline halides and alkaline earth halides, or mixtures, thereof and the temperature in the second reaction zone is in a range of from 700 to 1200° C. to produce a second gas stream comprising hydrogen and unreacted natural gas and a second solid carbon product.

Assignments (2)
CHANGE OF NAME Recorded Nov 20, 2023
From: SHELL OIL COMPANY
To: SHELL USA, INC.
Reel/Frame 065629/0316 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Dec 10, 2021
From: SPANU, LEONARDO; MESTERS, CAROLUS MATTHIAS ANNA MARIA
To: SHELL OIL COMPANY
Reel/Frame 058362/0747 →
Continuity (2)
Provisional Application 62654594 · Apr 9, 2018
Related Publication 20210032101A1 · Feb 4, 2021