Method for manufacturing a hydrogen and nitrogen containing gas mixture

• US 7,163,648 B2
• Filed: 02/11/2002
• Issued: 01/16/2007
• Est. Priority Date: 02/16/2001
• Status: Expired due to Fees

• Current Assignee: Statoil ASA (Asa Equinor)
• Original Assignee: Norsk Hydro Asa (Norsk Hydro)
• Inventors: .ANG.sen, Knut Ingvar, Andersen, Henrik Solgaard
• Primary Examiner(s): Langel; Wayne A.
• Application Number:
  US10/467,921
• Publication Number:
  US 20040170557A1
• Time in Patent Office: 1,800 Days
• Field of Search: 252/376, 423/650, 423/651, 423/652
• US Class Current: 252/376
• CPC Class Codes: B01D 53/22 by diffusion manufacturing semi-permeable membranes B01D67/00; form, structure or properties of semi-permeable membranes B01D69/00; material for semi-permeable membranes B01D71/00
• CPC Class Codes: B01J 19/2475 Membrane reactors
• CPC Class Codes: B01J 2219/00103 in a heat exchanger separate from the reactor
• CPC Class Codes: B01J 2219/00117 with two or more reactions in heat exchange with each other, such as an endothermic reaction in heat exchange with an exothermic reaction
• CPC Class Codes: B01J 2219/00159 controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
• CPC Class Codes: B01J 2219/00191 Control algorithm
• CPC Class Codes: B01J 8/009 Membranes, e.g. feeding or removing reactants or products to or from the catalyst bed through a membrane
• CPC Class Codes: C01B 2203/0233 the reforming step being a steam reforming step
• CPC Class Codes: C01B 2203/0283 containing a CO-shift step, i.e. a water gas shift step
• CPC Class Codes: C01B 2203/041 In-situ membrane purification during hydrogen production
• CPC Class Codes: C01B 2203/047 the impurity being carbon monoxide
• CPC Class Codes: C01B 2203/0475 the impurity being carbon dioxide
• CPC Class Codes: C01B 2203/048 the impurity being an organic compound
• CPC Class Codes: C01B 2203/0495 the impurity being water
• CPC Class Codes: C01B 2203/06 Integration with other chemical processes
• CPC Class Codes: C01B 2203/068 Ammonia synthesis
• CPC Class Codes: C01B 2203/0811 by combustion of fuel
• CPC Class Codes: C01B 2203/0822 the fuel containing hydrogen
• CPC Class Codes: C01B 2203/0827 at least part of the fuel being a recycle stream
• CPC Class Codes: C01B 2203/0838 by heat exchange with exothermic reactions, other than by combustion of fuel
• CPC Class Codes: C01B 2203/0844 : the non-combustive exothermic reaction being another reforming reaction as defined in groups C01B2203/02 - C01B2203/0294
• CPC Class Codes: C01B 2203/0866 : by combination of different heating methods
• CPC Class Codes: C01B 2203/1241 : Natural gas or methane
• CPC Class Codes: C01B 2203/142 : At least two reforming, decomposition or partial oxidation steps in series
• CPC Class Codes: C01B 2203/80 : Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
• CPC Class Codes: C01B 3/025 : Preparation or purification of gas mixtures for ammonia synthesis
• CPC Class Codes: C01B 3/384 : the catalyst being continuously externally heated
• CPC Class Codes: C01B 3/48 : followed by reaction of water vapour with carbon monoxide
• CPC Class Codes: C01B 3/501 : by diffusion
• CPC Class Codes: Y02P 20/10 : Process efficiency
• CPC Class Codes: Y02P 20/129 : Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Abstract

The present invention relates to a method for manufacturing a hydrogen- and nitrogen containing gas mixture, where a mixture of steam and a carbon containing gas is fed to the retentate side of at least one hydrogen transport membrane syngas and sweep gas generator where said gas and steam are converted to synthesis gas. A part of the hydrogen in said synthesis gas is transported through the membrane to the permeate side in said generator where it reacts with oxygen in an air stream fed to said permeate side to generate heat and a nitrogen and steam containing gas. The synthesis gas is further fed to the retentate side of a downstream hydrogen transport membrane unit or a hydrogen transport membrane reactor where a major part of the hydrogen in said synthesis gas, and if a reactor is used, a major part of additional hydrogen generated at the retentate side in said reactor is transported through said downstream membrane and picked up by said nitrogen containing gas to form a hydrogen- and nitrogen containing gas mixture. Furthermore, the invention relates to a method for performing a catalytic or non-catalytic process wherein the hydrogen- and nitrogen containing gas mixture manufactured by the method according to claims 1–6 is applied as one of the reactants in said process.

Claims

1. A method for manufacturing a hydrogen- and nitrogen containing gas mixture,

wherein said method comprises:

feeding a mixture of steam and a carbon containing gas to a retentate side of at least one hydrogen transport membrane syngas and sweep gas generator where said gas and steam are converted to a synthesis gas which comprises hydrogen,

transporting a part of the hydrogen in said synthesis gas through a membrane to a permeate side in said generator where the hydrogen reacts with oxygen in an air stream fed to said permeate side to generate heat and a nitrogen- and steam containing gas, resulting in a hydrogen depleted synthesis gas,

partly using the generated heat to heat the air stream and other gases fed to the generator and partly transferring the generated heat back to the retentate side of the generator to meet a heat requirement for steam reforming the carbon containing feed gas,

further feeding the synthesis gas to the retentate side of a downstream hydrogen transport membrane unit or a hydrogen transport membrane reactor where a major part of the hydrogen in said synthesis gash and if a reactor is used, a major part of additional hydrogen generated at the retentate side in said reactor, is transported through said downstream membrane and picked up by said nitrogen containing gas to form a hydrogen- and nitrogen containing gas mixture.

2. The method according to claim 1,

wherein combustible components in the hydrogen depleted synthesis gas stream leaving the downstream hydrogen transport membrane unit or the hydrogen transport membrane reactor are oxidised to CO₂ and water directly on a membrane surface at a permeate side of a mixed conducting membrane reactor.

3. The method according to claim 1,

wherein combustible components in the hydrogen depleted synthesis gas stream leaving the downstream hydrogen transport membrane unit or the hydrogen transport membrane reactor react with oxygen that is separated from air by means of a mixed conducting membrane or by means of any other process to generate CO₂ and water.

4. The method according to claim 2,

further comprising using heat generated by combustion of hydrogen depleted synthesis gas to preheat air fed to a gas turbine combuster.

5. The method according to claim 3,

further comprising using heat generated by combustion of hydrogen depleted synthesis gas to preheat air fed to a gas turbine combuster.