Methods for production of hydrogen

Patent metadata

Field	Value
Publication number	US-11724938-B2
Application number	US-201816652318-A
Country	US
Kind code	B2
Filing date	Sep 24, 2018
Priority date	Sep 29, 2017
Publication date	Aug 15, 2023
Grant date	Aug 15, 2023

Abstract

Synthesis gas containing nitrogen as the majority component is processed to increase the hydrogen to carbon dioxide ratio. Nitrogen, carbon dioxide, and other contaminants are subsequently removed by a purification unit to produce a purified hydrogen gas stream. A recycle stream within the purification unit helps achieve a hydrogen purity greater than 99.9 percent, and hydrogen recovery greater than 99 percent.

First claim

What is claimed is:

1. A method for producing a purified hydrogen gas stream, the method comprising:
flowing a fuel and an oxidizer into an internal combustion engine to produce a feed gas containing nitrogen gas (N 2 ) as the majority component, hydrogen gas (H 2 ), and carbon monoxide (CO) and having an initial H 2 to CO ratio;
flowing the feed gas into a processing unit to produce an enhanced gas containing carbon dioxide (CO 2 ) and having a second H 2 to CO ratio greater than the initial H 2 to CO ratio;
flowing the enhanced gas into a purification unit comprising a N 2 removal unit to remove N 2 and a CO 2 removal unit to remove CO 2 , wherein the purification unit produces a purified hydrogen gas stream and a tail gas containing residual H 2 ; and
recycling about 50 percent to about 100 percent of the tail gas containing residual H 2 to a point upstream of the N 2 removal unit so as to increase the H 2 recovery.

2. The method of claim 1 , wherein flowing the enhanced gas into the purification unit comprises flowing the enhanced gas into the N 2 removal unit to produce a permeate stream and a retentate stream, and flowing the permeate stream into the CO 2 removal unit to produce the purified hydrogen gas stream and the tail gas.

3. The method of claim 1 , wherein the initial H 2 to CO ratio is selected from the group consisting of: about 1 to about 3; and about 1.5 to about 2.5.

4. The method of claim 1 , wherein the processing unit comprises a water-gas shift unit configured to shift the feed gas to produce H 2 and CO 2 .

5. The method of claim 2 , wherein the N 2 removal unit comprises a membrane separation unit configured to receive the enhanced gas.

6. The method of claim 5 , wherein the membrane separation unit comprises a H 2 selective membrane.

7. The method of claim 6 , wherein the H 2 selective membrane comprises one or more of a polymer, a ceramic, a carbon compound, activated carbon, and a metallic compound.

8. The method of claim 1 , wherein a concentration of H 2 in the purified H 2 gas stream is selected from the group consisting of: greater than about 75 percent; greater than about 90 percent; greater than about 95 percent; and greater than about 99 percent.

9. A method for producing a purified hydrogen gas stream, the method comprising:
flowing a fuel and an oxidizer into an internal combustion engine to produce a feed gas containing nitrogen gas (N 2 ) as the majority component, hydrogen gas (H 2 ), and carbon monoxide (CO) and having an initial H 2 to CO ratio;
flowing the feed gas into a processing unit to produce an enhanced gas containing carbon dioxide (CO 2 ) and having a second H 2 to CO ratio greater than the initial H 2 to CO ratio;
flowing the enhanced gas into contact with a membrane in a membrane unit to produce a permeate stream and a retentate stream, wherein the membrane has a H 2 selective composition, and a concentration of H 2 in the permeate stream is greater than a concentration of H 2 in the enhanced gas, and the retentate stream comprises N 2 that has been removed from the enhanced gas;
flowing the permeate stream into contact with a sorbent material in one or more adsorption columns to produce a purified H 2 gas stream, wherein the sorbent material comprises a sorbent compound effective for removing CO 2 from the permeate stream; and
regenerating the sorbent material in at least one of the one or more adsorption columns to produce a tail gas containing residual H 2 , and recycling about 50 percent to about 100 percent of the tail gas containing residual H 2 to the enhanced gas stream at a point upstream of the membrane unit so as to increase the H 2 recovery.

10. The method of claim 9 , wherein the processing unit comprises a water-gas shift unit.

11. The method of claim 9 , wherein a mole fraction of H 2 in the purified H 2 gas stream is greater than about 99 percent.

12. The method of claim 9 , wherein an amount of H 2 present in the enhanced gas and recovered in the purified H 2 gas stream is selected from the group consisting of: greater than about 80 percent; greater than about 90 percent; greater than about 95 percent; and greater than about 99 percent.

Assignees

• Res Triangle Inst

Inventors

• Zhou Shaojun James
• Gupta Raghubir P
• Carpenter John Reeves
• Turk Brian S

Classifications

• C10K1/002 Primary

  Removal of contaminants · CPC title

• C01B2203/0405

  Purification by membrane separation · CPC title

• C01B2203/1241

  Natural gas or methane · CPC title

• C01B3/366

  Partial combustion in internal-combustion engines · CPC title

• C10G2/32

  with the use of catalysts · CPC title