IP Library Granted Patent US 11,964,867
Granted Patent B2
US 11,964,867 · App. 17/949,922 · Granted Apr 23, 2024

High throughput methane pyrolysis reactor for low-cost hydrogen production

Inventors: Divyaraj Desai (Hayward, CA); Todd Karin (Fairfield, CA); Jessica Louis Baker Rivest (Palo Alto, CA)
Assignee: XEROX CORPORATION
C01B3/26B01J8/125B01J21/18B01J35/27B01J38/48C07C5/321B01J2203/06C01B2203/1005C01B2203/1041C01B2203/1241
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Quick Facts
Patent No.
US 11,964,867
App. No.
17/949,922
Granted
Apr 23, 2024
Kind
B2
Abstract

An apparatus to decompose a hydrocarbon reactant into a gaseous product and a solid product includes a reactor volume, a reservoir of liquid material, a plurality of nozzles connected to the reservoir of liquid material, the plurality of nozzles configured to distribute the liquid material into the reactor volume from the reservoir as a liquid mist, a gas inlet connected to a hydrocarbon gas source to receive hydrocarbon gas reactant, a distributor connected to the inlet to distribute the hydrocarbon gas reactant into the reactor volume, a heat source located adjacent the reactor volume configured to heat the reactor volume, a separator to separate the solid product from the liquid material, a re-circulation path connected between the reactor volume and the reservoir to re-circulate the liquid material from the reactor volume to the reservoir, a gas outlet connected to the reactor volume configured to outlet hydrogen gas from the reactor volume, and at least one filter connected to the gas outlet to remove entrained solid product from the hydrogen gas.

Claims (25)

1. An apparatus to decompose a hydrocarbon reactant into a gaseous product and a solid product comprising:

a reactor volume;

a reservoir of liquid metal material;

a plurality of nozzles connected to the reservoir of liquid metal material, the plurality of nozzles configured to distribute the liquid metal material into the reactor volume from the reservoir as a liquid mist to initially contact hydrocarbon gas reactant;

a gas inlet connected to a hydrocarbon gas source to receive the hydrocarbon gas reactant;

a distributor connected to the inlet to distribute the hydrocarbon gas reactant into the reactor volume;

a heat source located next to the reactor volume configured to heat the reactor volume;

a separator to separate the solid product from the liquid metal material;

a re-circulation path connected between the reactor volume and the reservoir to re-circulate the liquid metal material from the reactor volume to the reservoir;

a gas outlet connected to the reactor volume configured to outlet hydrogen gas from the reactor volume; and

at least one filter connected to the gas outlet to remove entrained solid product from the hydrogen gas.

2. The apparatus as claimed in claim 1 , wherein the liquid metal material has a melting point between −40° C. and 1400° C.

3. The apparatus as claimed in claim 1 , wherein the liquid metal material comprises:

a first element of a concentration of up to 90 weight percent, the first element selected from the group consisting of lithium; sodium; calcium; potassium; cadmium; aluminum; antimony; bismuth; cerium; copper; gallium; indium; lanthanum; lead; magnesium; mercury; silver; tin and zinc; and

a second element of a concentration of at least 10 weight percent, the second element selected from the group consisting of nickel; iron; cobalt; manganese; chromium scandium; titanium; vanadium; molybdenum; silicon; tantalum; technetium; tungsten; ruthenium; and palladium.

4. The apparatus as claimed in claim 1 , wherein the liquid metal material comprises one or more components, wherein at least one of the one or more components has an activation energy barrier for hydrocarbon pyrolysis of less than 300 kJ per mole.

5. The apparatus as claimed in claim 1 , wherein the liquid metal material comprises one or more components, wherein a least one of the one or more components has a carbon solubility of at least 1 atomic percent.

6. The apparatus as claimed in claim 1 , wherein the liquid metal material reservoir is positioned adjacent the heat source.

7. The apparatus as claimed in claim 1 , wherein the plurality of nozzles to distribute the liquid metal material comprises a plurality of nozzles configured to produce the mist of liquid metal material that has a surface area to volume ratio greater than 1 cm 2 per 1 cm 3 of reactor volume.

8. The apparatus as claimed in claim 1 , wherein the plurality of nozzles to distribute the liquid metal material comprises a plurality of nozzles configured to produce the mist as liquid droplets having a size of a mass-averaged diameter between 0.1 and 1,000 microns.

9. The apparatus as claimed in claim 1 , where the nozzles comprise a plurality of misting nozzles to produce a mist of liquid metal material in the reactor volume through breakup of a liquid jet.

10. The apparatus as claimed in claim 1 , wherein the nozzles comprise a plurality of misting nozzles to accelerate the breakup of a liquid jet through patterned grooves within the misting nozzles.

11. The apparatus as claimed in claim 1 , wherein the reactor volume is configured to process one of co-current, counter-current, or cross-current flows of hydrocarbon reactant and liquid metal material mist.

12. The apparatus as claimed in claim 1 , wherein the liquid metal material is introduced into the reactor volume through an outlet at the top, side, or bottom of the reactor volume.

13. The apparatus as claimed in claim 1 , wherein the hydrocarbon reactant comprises at least one selected from group consisting of: natural gas, liquefied petroleum gas, gasoline, diesel, kerosene, naphtha, kerosene-based fuel, methane, ethane, propane, butane, pentane, hexane, benzene, xylene, toluene, and any combination thereof; alkynes, alkenes, alkanes, arenes, cyclic compounds, and any combination thereof having a boiling point less than 600° C.

Assignments (8)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Nov 14, 2025
From: XEROX CORPORATION
To: GENESEE VALLEY INNOVATIONS, LLC
Reel/Frame 073562/0677 →
SECOND LIEN NOTES PATENT SECURITY AGREEMENT Recorded Jul 2, 2025
From: XEROX CORPORATION
To: U.S. BANK TRUST COMPANY, NATIONAL ASSOCIATION, AS COLLATERAL AGENT
Reel/Frame 071785/0550 →
FIRST LIEN NOTES PATENT SECURITY AGREEMENT Recorded Apr 11, 2025
From: XEROX CORPORATION
To: U.S. BANK TRUST COMPANY, NATIONAL ASSOCIATION, AS COLLATERAL AGENT
Reel/Frame 070824/0001 →
SECURITY INTEREST Recorded Feb 13, 2024
From: XEROX CORPORATION
To: CITIBANK, N.A., AS COLLATERAL AGENT
Reel/Frame 066741/0001 →
SECURITY INTEREST Recorded Nov 20, 2023
From: XEROX CORPORATION
To: JEFFERIES FINANCE LLC, AS COLLATERAL AGENT
Reel/Frame 065628/0019 →
CORRECTIVE ASSIGNMENT TO CORRECT THE REMOVAL OF US PATENTS 9356603, 10026651, 10626048 AND INCLUSION OF US PATENT 7167871 PREVIOUSLY RECORDED ON REEL 064038 FRAME 0001. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT. Recorded Jun 28, 2023
From: PALO ALTO RESEARCH CENTER INCORPORATED
To: XEROX CORPORATION
Reel/Frame 064161/0001 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Jun 20, 2023
From: PALO ALTO RESEARCH CENTER INCORPORATED
To: XEROX CORPORATION
Reel/Frame 064038/0001 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 21, 2022
From: DESAI, DIVYARAJ; KARIN, TODD; RIVEST, JESSICA LOUIS BAKER
To: PALO ALTO RESEARCH CENTER INCORPORATED
Reel/Frame 061172/0934 →
Continuity (3)
Continuation 16394041 · Apr 25, 2019
Provisional Application 62692558 · Jun 29, 2018
Related Publication 20230026987A1 · Jan 26, 2023