IP Library Granted Patent US 10,377,682
Granted Patent B2
US 10,377,682 · App. 16/021,441 · Granted Aug 13, 2019

Reactors and systems for oxidative coupling of methane

Inventors: Humera A. Rafique (Dublin, CA); Srinivas Vuddagiri (Davis, CA); Guido Radaelli (South San Francisco, CA); Jarod McCormick (San Carlos, CA); Suchia Duggal (San Rafael, CA); Joel Cizeron (Redwood City, CA)
Assignee: SILURIA TECHNOLOGIES, INC.
C07C2/78B01J4/004B01J8/001B01J8/0214B01J8/0278B01J8/0285B01J8/0457B01J8/0496B01J19/0026C07C2/84C07C5/09C10G50/00C10G69/126B01J2208/00176B01J2208/02C10G2400/02
View Patent ↗
Loading inventors, assignments & file history…
Monitor This Case
Get email alerts when status or documents change.
Order Certified Copies
Most orders are placed with the USPTO same day — all within 24 business hours.
Order via The Patent Place →
Pre-filled with this patent's details
Quick Facts
Patent No.
US 10,377,682
App. No.
16/021,441
Granted
Aug 13, 2019
Kind
B2
Abstract

In an aspect, the present disclosure provides a method for the oxidative coupling of methane to generate hydrocarbon compounds containing at least two carbon atoms (C 2+ compounds). The method can include mixing a first gas stream comprising methane with a second gas stream comprising oxygen to form a third gas stream comprising methane and oxygen and performing an oxidative coupling of methane (OCM) reaction using the third gas stream to produce a product stream comprising one or more C 2+ compounds.

Claims (38)

1. A process for production of hydrocarbons, the process comprising the steps of:

converting at least a feed stream comprising methane (CH 4 ) and oxygen (O 2 ) feed into a conversion effluent by oxidative coupling of methane (OCM);

directing said conversion effluent to at least one product retrieval stage to produce one or more product streams and a remaining conversion effluent;

directing at least a portion of said remaining conversion effluent to a hydrogenation stage to produce a hydrogenation effluent, and directing said hydrogenation effluent to a methanation stage to produce a recycle stream; and

adding at least part of said recycle stream to said feed stream.

2. The method of claim 1 , wherein said hydrogenation stage and methanation stage are comprised in a recycle loop.

3. The process according to claim 2 , wherein said recycle loop further comprises a CO 2 addition stage.

4. The process according to claim 1 , wherein CO 2 is added upstream said methanation step at said CO 2 addition stage and/or directly into said methanation stage.

5. The process according to claim 1 , wherein H 2 O is at least partially removed upstream and/or downstream one or more of said product retrieval steps.

6. The process according to claim 2 , wherein said recycle loop comprises a pre-methanation step.

7. The process according to claim 6 , wherein CO, CO 2 is pre-methanated and/or higher alkanes are reformed in said pre-methanation step.

8. The process according to claim 6 , wherein said pre-methanation step is carried out at T<400° C. or >400° C.

9. The process according to claim 6 , wherein at least part of effluent from said pre-methanation is recycled to upstream said pre-methanation step.

10. The process according to claim 1 , wherein said one or more product streams obtained at said one or more product retrieval stages comprise ethylene, CO 2 , aromatics and/or raw gasoline.

11. The process according to claim 1 , wherein said recycle stream comprises 90-99% CH 4 .

12. The process according to claim 1 , wherein said recycle stream comprises H 2 and/or CO at a concentration below 5%, below 1%, below 0.5%, such as below 10 ppm when added to said feed stream.

13. The process according to claim 1 , wherein said one or more product streams is obtained by separation from said conversion effluent through pressure swing adsorption, condensation, N 2 wash and/or distillation or other separation technologies.

14. The process according to claim 6 , wherein said pre-methanation step is carried out over a nickel-based catalyst at a pressure between 0.1 and 80 bars.

15. The process according to claim 1 , wherein said methanation stage is carried out over a nickel-based catalyst at a pressure between 0.1 and 80 bars.

16. The process according to claim 1 , wherein said methanation stage is carried out at T<400° C. or T>400° C., depending on if said unsaturated hydrogenation is desired or not.

17. The process according to claim 6 , wherein said hydrogenation, pre-methanation and/or methanation is carried out in a boiling water reactor preferably in a single boiling water reactor.

18. A method for producing hydrocarbon compounds, comprising:

(a) directing a feed stream comprising methane (CH 4 ) and an oxidizing agent into an oxidative coupling of methane (OCM) unit to generate from at least a portion of said CH 4 and said oxidizing agent an OCM effluent comprising said hydrocarbon compounds;

(b) recovering a portion of said OCM effluent in one or more product streams;

(c) directing an additional portion of said OCM effluent into a recycle loop that comprises (i) a hydrogenation unit that hydrogenates at least a portion of unsaturated hydrocarbons from said additional portion of said OCM effluent, and (ii) a methanation unit that reacts hydrogen (H 2 ) with carbon monoxide (CO) or carbon dioxide (CO 2 ) from said additional portion of said OCM effluent in a methanation reaction to form CH 4 , wherein said recycle loop outputs a recycle stream comprising said CH 4 generated by said methanation unit; and

(d) directing at least a portion of said recycle stream into said OCM unit.

19. The method of claim 18 , wherein said one or more product streams comprise ethylene (C 2 H 4 ), CO 2 , and/or hydrocarbon compounds having three or more carbon atoms (C 3+ compounds).

20. The method of claim 18 , further comprising directing a CO 2 stream into said methanation unit.

21. The method of claim 18 , further comprising removing water from said OCM effluent.

22. The method of claim 18 , further comprising reducing a concentration of hydrocarbon compounds having carbon-carbon double bonds or triple bonds in said OCM effluent prior to said methanation reaction.

23. The method of claim 18 , wherein said recycle stream comprises at least about 90% CH 4 .

24. The method of claim 18 , wherein said one or more product streams are recovered using pressure swing adsorption (PSA), condensation, and/or membrane separation.

25. The method of claim 18 , further comprising removing water from said recycle stream prior to (d).

26. The method of claim 25 , wherein at least about 70% of said water is removed from said recycle stream.

27. The method of claim 18 , wherein said additional portion of said OCM effluent is a part of said portion of said OCM effluent.

28. The method of claim 18 , wherein said methanation unit comprises a catalyst comprising one or more of ruthenium, cobalt, nickel and iron.

29. The method of claim 18 , wherein said methanation unit operates at a pressure between about 2 bar (absolute) and 60 bar, and a temperature between about 150° C. and about 400° C.

30. The method of claim 18 , wherein said carbon efficiency is at least about 50%.

Assignments (4)
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Sep 3, 2020
From: SILURIA TECHNOLOGIES, INC.
To: SILURIA (ASSIGNMENT FOR THE BENEFIT OF CREDITORS), LLC
Reel/Frame 053685/0056 →
CORRECTIVE ASSIGNMENT TO CORRECT THE ASSIGNOR'S NAME PREVIOUSLY RECORDED ON REEL 050161 FRAME 0578. ASSIGNOR(S) HEREBY CONFIRMS THE ASSIGNMENT. Recorded Sep 3, 2020
From: SILURIA (ASSIGNMENT FOR THE BENEFIT OF CREDITORS), LLC
To: LUMMUS TECHNOLOGY LLC
Reel/Frame 053689/0659 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 26, 2019
From: SILURIA TECHNOLOGIES, INC.
To: LUMMUS TECHNOLOGY LLC
Reel/Frame 050161/0578 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Aug 27, 2018
From: RAFIQUE, HUMERA A.; VUDDAGIRI, SRINIVAS; RADAELLI, GUIDO; MCCORMICK, JAROD; DUGGAL, SUCHIA; CIZERON, JOEL
To: SILURIA TECHNOLOGIES, INC.
Reel/Frame 047210/0799 →
Continuity (10)
Continuation In Part 15076402 · Mar 21, 2016
Continuation 14789946 · Jul 1, 2015
Continuation 14592668 · Jan 8, 2015
Provisional Application 62086650 · Dec 2, 2014
Provisional Application 62073478 · Oct 31, 2014
Provisional Application 62050720 · Sep 15, 2014
Provisional Application 61996789 · May 14, 2014
Provisional Application 61955112 · Mar 18, 2014
Provisional Application 61925627 · Jan 9, 2014
Related Publication 20180305274A1 · Oct 25, 2018
Cited By (3)
US 12,227,466 US 12,291,681 US 12,655,075