Hydrogen purification unit

Abstract

A hydrogen purification device and its components are disclosed. In some embodiments, the device may include at least one foil-microscreen assembly, which is disposed between a first end frame and a second end frame and fixed to the first end frame and the second end frame. At least one foil-microscreen assembly may include at least one hydrogen selective membrane and at least one microscreen structure, the microscreen structure including a non-porous planar sheet having a plurality of orifices forming a plurality of fluid channels. The planar sheet may include substantially opposite flat surfaces configured to provide support for the permeate side. A plurality of fluid channels may extend between the opposite surfaces. At least one hydrogen selective membrane may be metallurgically bonded to at least one microscreen structure.

Description

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS

[0002] This application claims the benefit of U.S. Patent Application No. 17 / 412,581, filed on August 26, 2021, and entitled “HYDROGEN PURIFICATION APPARATUS.” This application also claims the benefit of U.S. Provisional Application No. 63 / 071,139, filed on August 27, 2020, and entitled “HYDROGEN PURIFICATION APPARATUS.” This application is also a continuation-in-part of U.S. Patent Application Serial No. 16 / 904,872, filed on June 18, 2020, and entitled “HYDROGEN PURIFICATION APPARATUS,” which is a divisional application of U.S. Patent Application Serial No. 15 / 862,474, filed on January 4, 2018, and entitled “HYDROGEN PURIFICATION APPARATUS,” and now granted U.S. Patent No. 10,717,040, which is a continuation-in-part of U.S. Patent Application Serial No. 15 / 483,265, filed on April 10, 2017, and entitled “HYDROGEN GENERATION ASSEMBLY AND HYDROGEN PURIFICATION APPARATUS,” and now granted U.S. Patent No. 10,166,506, which is a divisional application of U.S. Patent Application Serial No. 15 / 862,474, filed on January 4, 2018, and entitled “HYDROGEN PURIFICATION APPARATUS.” The application is a divisional application of U.S. patent application serial number 14 / 931,585, filed on November 3, 2015, entitled "Hydrogen Generation Assembly and Hydrogen Purification Device", and granted U.S. Patent No. 9,616,389, which is a divisional application of U.S. patent application serial number 13 / 829,766, filed on March 14, 2013, entitled "Hydrogen Generation Assembly and Hydrogen Purification Device", and now granted U.S. Patent No. 9,187,324, which is a continuation-in-part application of U.S. patent application serial number 13 / 600,096, filed on August 30, 2012, entitled "Hydrogen Generation Assembly", and now abandoned. The entire disclosure of the above application is incorporated herein by reference for all purposes. Background Art

[0003] The hydrogen generation assembly is a component that converts one or more raw materials into a product stream containing hydrogen as a main component. The raw material may include a carbonaceous raw material, and in some embodiments, may also include water. The raw material is delivered to the hydrogen generation zone of the hydrogen generation assembly from the raw material delivery system, and the raw material is usually delivered at a pressure and elevated temperature. The hydrogen generation zone is usually associated with a temperature regulating assembly, such as a heating assembly or a cooling assembly, which consumes one or more fuel streams to keep the hydrogen generation zone within a suitable temperature range for effectively producing hydrogen. The hydrogen generation assembly can generate hydrogen by any suitable (one or more) mechanism, such as steam reforming, autothermal reforming, pyrolysis and / or catalytic partial oxidation.

[0004] However, the generated or produced hydrogen gas may contain impurities. The gas may be referred to as a mixed gas stream containing hydrogen and other gases. Before using the mixed gas stream, it must be purified, such as removing at least a portion of the other gases. Therefore, the hydrogen generation component may include a hydrogen purification device for improving the hydrogen purity of the mixed gas stream. The hydrogen purification device may include at least one hydrogen selective membrane to separate the mixed gas stream into a product stream and a by-product stream. The product stream contains a higher concentration of hydrogen from the mixed gas stream and / or one or more other gases with reduced concentrations. Hydrogen purification using one or more hydrogen selective membranes is a pressure-driven separation process, wherein one or more hydrogen selective membranes are contained in a pressure vessel. The mixed gas stream contacts the mixed gas surface of the (one or more) membranes, and the product stream is formed by at least a portion of the mixed gas stream that permeates through the (one or more) membranes. The pressure vessel is typically in some embodiments, and the feedstock delivery system may be configured to deliver a feed seal to prevent gas from entering or leaving the pressure vessel unless through a defined inlet and outlet port or conduit.

[0005] The product stream can be used in a variety of applications. One such application is energy generation, such as in an electrochemical fuel cell. An electrochemical fuel cell is a device that converts a fuel and an oxidant into electricity, reaction products, and heat. For example, a fuel cell can convert hydrogen and oxygen into water and electricity. In these fuel cells, hydrogen is the fuel, oxygen is the oxidant, and water is the reaction product. A fuel cell stack includes a plurality of fuel cells and can be used with a hydrogen generation assembly to provide an energy generation assembly.

[0006] Examples of hydrogen generation assemblies, hydrogen processing assemblies, and / or components of such assemblies are described in U.S. Patent Nos. 5,861,137, 6,319,306, 6,494,937, 6,562,111, 7,063,047, 7,306,868, 7,470,293, 7,601,302, 7,632,322, 8,961,627 and U.S. Patent Application Publication Nos. 2006 / 0090397, 2006 / 0272212, 2007 / 0266631, 2007 / 0274904, 2008 / 0085434, 2008 / 0138678, 2008 / 0230039, and 2010 / 0064887. The entire disclosures of the above-identified patents and patent application publications are incorporated herein by reference for all purposes. BRIEF DESCRIPTION OF THE DRAWINGS

[0007] Figure 1 is a schematic diagram of an example of a hydrogen generation assembly.

[0008] Figure 2 yes Figure 1 Schematic diagram of an example of a hydrogen generation component.

[0009] Figure 3 yes Figure 1 Schematic diagram of a hydrogen purification device with hydrogen generation components.

[0010] Figure 4 yes Figure 3 An exploded perspective view of an example of a hydrogen purification device.

[0011] Figure 5 yes Figure 3 A top view of an example of a foil-microsieve assembly of a hydrogen purification device.

[0012] Figure 6 yes Figure 5 A top view of an example of a microsieve structure of a foil-microsieve assembly.

[0013] Figure 7 yes Figure 6 A partial view of another example of the pores of a microsieve structure.

[0014] Figure 8 yes Figure 6 Partial views of additional examples of pores of the microsieve structure.

[0015] Fig. 9 yes Figure 6 A partial view of another example of the pores of a microsieve structure.

[0016] Fig.10 yes Figure 6 A partial view of yet another example of pores of a micro-sieve structure.

[0017] Fig.11 yes Figure 3 A top view of an additional example of a foil-microsieve assembly of a hydrogen purification device.

[0018] Fig.12 yes Fig.11 A top view of an example of a microsieve structure of a foil-microsieve assembly.

[0019] Fig.13 yes Figure 3 A top view of another example of a foil-microsieve assembly of a hydrogen purification device.

[0020] Fig.14 yes Figure 3 A top view of another example of a foil-microsieve assembly of a hydrogen purification device.

[0021] Fig.15 yes Figure 3 An exploded perspective view of another example of a hydrogen purification device. DETAILED DESCRIPTION

[0022] Figure 1An example of a hydrogen generation assembly 20 is shown. Unless specifically excluded, the hydrogen generation assembly 20 may include one or more components of other hydrogen generation assemblies described in the present disclosure. The hydrogen generation assembly may include any suitable structure configured to generate a product hydrogen stream 21. For example, the hydrogen generation assembly may include a feedstock delivery system 22 and a fuel processing assembly 24. The feedstock delivery system may include any suitable structure configured to selectively deliver at least one feed stream 26 to the fuel processing assembly.

[0023] In some embodiments, the feedstock delivery system 22 may further include any suitable structure configured to selectively deliver at least one fuel stream 28 to a burner or other heating component of the fuel processing assembly 24. In some embodiments, the feed stream 26 and the fuel stream 28 may be the same stream delivered to different parts of the fuel processing assembly. The feedstock delivery system may include any suitable delivery mechanism, such as a positive displacement pump or other suitable pump or mechanism, for propelling the fluid stream. In some embodiments, the feedstock delivery system may be configured to deliver (one or more) feed streams 26 and / or (one or more) fuel streams 28 without the use of pumps and / or other electrically driven fluid delivery mechanisms. Examples of suitable feedstock delivery systems that can be used with the hydrogen generation assembly 20 include feedstock delivery systems described in U.S. Patent Nos. 7,470,293 and 7,601,302 and U.S. Patent Application Publication No. 2006 / 0090397. The complete disclosures of the above patents and patent applications are incorporated herein by reference for all purposes.

[0024] The feed stream 26 may include at least one hydrogen production fluid 30, which may include one or more fluids that can be used as reactants to produce the product hydrogen stream 21. For example, the hydrogen production fluid may include a carbon-containing feedstock, such as at least one hydrocarbon and / or alcohol. Examples of suitable hydrocarbons include methane, propane, natural gas, diesel, kerosene, gasoline, etc. Examples of suitable alcohols include methanol, ethanol, polyols (such as ethylene glycol and propylene glycol), etc. In addition, the hydrogen production fluid 30 may include water, such as when the fuel processing assembly generates the product hydrogen stream by steam reforming and / or autothermal reforming. When the fuel processing assembly 24 generates the product hydrogen stream by pyrolysis or catalytic partial oxidation, the feed stream 26 does not contain water.

[0025] In some embodiments, the feedstock delivery system 22 may be configured to deliver a hydrogen production fluid 30 comprising a mixture of water and a water-miscible carbonaceous feedstock (such as methanol and / or another water-soluble alcohol). The ratio of water to carbonaceous feedstock in such a fluid stream may vary depending on one or more factors, such as the specific carbonaceous feedstock used, user preferences, the design of the fuel processing assembly, the mechanism(s) used by the fuel processing assembly to generate the product hydrogen stream, etc. For example, the molar ratio of water to carbon may be approximately 1:1 to 3:1. In addition, a mixture of water and methanol may be delivered at or near a 1:1 molar ratio (37 wt. % water, 63 wt. % methanol), while a mixture of hydrocarbons or other alcohols may be delivered at a water-to-carbon molar ratio greater than 1:1.

[0026] When the fuel processing assembly 24 generates the product hydrogen stream 21 by reforming, the feed stream 26 may include, for example, about 25-75% by volume of methanol or ethanol (or another suitable water-miscible carbonaceous feedstock) and about 25-75% by volume of water. For feed streams that at least substantially include methanol and water, those streams may include about 50-75% by volume of methanol and about 25-50% by volume of water. Streams containing ethanol or other water-miscible alcohols may include about 25-60% by volume of alcohol and about 40-75% by volume of water. An example of a feed stream for a hydrogen generation assembly 20 that utilizes steam reforming or autothermal reforming includes 69% by volume of methanol and 31% by volume of water.

[0027] Although the feedstock delivery system 22 is shown as being configured to deliver a single feed stream 26, the feedstock delivery system may be configured to deliver two or more feed streams 26. These streams may contain the same or different feedstocks and may have different components, at least one common component, may not have a common component, or may have the same components. For example, the first feed stream may include a first component, such as a carbonaceous feedstock, and the second feed stream may include a second component, such as water. In addition, although in some embodiments, the feedstock delivery system 22 may be configured to deliver a single fuel stream 28, the feedstock delivery system may be configured to deliver two or more fuel streams. The fuel streams may have different components, at least one common component, may not have a common component, or may have the same components. In addition, the feed stream and the fuel stream may be discharged from the feedstock delivery system at different stages. For example, one of the streams may be a liquid stream and the other may be a gas stream. In some embodiments, both streams may be liquid streams, while in other embodiments, both streams may be gas streams. In addition, although the hydrogen generation assembly 20 is shown as including a single feedstock delivery system 22, the hydrogen generation assembly may include two or more feedstock delivery systems 22.

[0028] The fuel processing assembly 24 may include a hydrogen generation region 32 configured to generate an output stream 34 comprising hydrogen gas by any suitable hydrogen generation mechanism(s). The output stream may include at least hydrogen gas as a major component and may include(s) additional gaseous components. The output stream 34 may therefore be referred to as a "mixed gas stream" that includes hydrogen gas as its major component but includes other gases.

[0029] The hydrogen production zone 32 may include any suitable catalyst-containing bed or zone. When the hydrogen production mechanism is steam reforming, the hydrogen production zone may include a suitable steam reforming catalyst 36 to promote the production of (one or more) output streams 34 from (one or more) feed streams 26 comprising carbonaceous feedstock and water. In such embodiments, the fuel processing assembly 24 may be referred to as a "steam reformer", the hydrogen production zone 32 may be referred to as a "reforming zone", and the output stream 34 may be referred to as a "reformed stream". Other gases that may be present in the reformed stream may include carbon monoxide, carbon dioxide, methane, steam, and / or unreacted carbonaceous feedstock.

[0030] When the hydrogen generation mechanism is autothermal reforming, the hydrogen generation zone 32 may include a suitable autothermal reforming catalyst to facilitate the production of output stream(s) 34 from the feed stream(s) 26 comprising water and the carbonaceous feedstock in the presence of air. In addition, the fuel processing assembly 24 may include an air delivery assembly 38 configured to deliver the air stream(s) to the hydrogen generation zone.

[0031] In some embodiments, the fuel processing assembly 24 may include a purification region 40, which may include any suitable structure configured to produce at least one hydrogen-rich stream 42 from the output (or mixed gas) stream 34. The hydrogen-rich stream 42 may include a higher hydrogen concentration than the output stream 34 and / or a reduced concentration of one or more other gases (or impurities) present in the output stream. The product hydrogen stream 21 includes at least a portion of the hydrogen-rich stream 42. Thus, the product hydrogen stream 21 and the hydrogen-rich stream 42 may be the same stream and have the same composition and flow rate. Alternatively, some of the purified hydrogen in the hydrogen-rich stream 42 may be stored for later use, such as in a suitable hydrogen storage assembly and / or consumed by the fuel processing assembly. The purification region 40 may also be referred to as a "hydrogen purification device" or a "hydrogen processing assembly."

[0032] In some embodiments, the purification region 40 may produce at least one byproduct stream 44, which may contain no hydrogen or some hydrogen. The byproduct stream may be discharged, sent to a burner assembly and / or other combustion source, used as a heated fluid stream, stored for later use, and / or otherwise utilized, stored, and / or disposed of. In addition, the purification region 40 may discharge the byproduct stream as a continuous stream in response to delivery of the output stream 34, or may discharge the byproduct stream intermittently, such as in a batch process or when a byproduct portion of the output stream is at least temporarily retained in the purification region.

[0033] The fuel processing assembly 24 may include one or more purification zones configured to produce one or more byproduct streams containing sufficient hydrogen to be suitable for use as a fuel stream (or feed stream) for a heating assembly of the fuel processing assembly. In some embodiments, the byproduct stream may have a sufficient fuel value or hydrogen content to enable the heating assembly to maintain the hydrogen generation zone at a desired operating temperature or within a selected temperature range. For example, the byproduct stream may include hydrogen, such as 10-30% hydrogen by volume, 15-25% hydrogen by volume, 20-30% hydrogen by volume, at least 10 or 15% hydrogen by volume, at least 20% hydrogen by volume, etc.

[0034] The purification region 40 may include any suitable structure configured to enrich (and / or increase) the concentration of at least one component of the output stream 34. In most applications, the hydrogen-rich stream 42 will have a higher hydrogen concentration than the output stream (or mixed gas stream) 34. The hydrogen-rich stream may also have one or more non-hydrogen components present in a reduced concentration in the output stream 34, wherein the hydrogen concentration of the hydrogen-rich stream is higher, equal to, or lower than that of the output stream. For example, in a conventional fuel cell system, carbon monoxide may damage the fuel cell stack even if it is present in a few parts per million, while other non-hydrogen components that may be present in the output stream 34, such as water, may not damage the stack even if they are present in much higher concentrations. Therefore, in such an application, the purification region may not increase the overall hydrogen concentration, but may reduce the concentration of one or more non-hydrogen components that are harmful or potentially harmful to the desired application of the product hydrogen stream.

[0035] Examples of suitable devices for purification region 40 include one or more hydrogen selective membranes 46, chemical carbon monoxide removal components 48, and / or pressure swing adsorption (PSA) systems 50. Purification region 40 may include more than one type of purification device, and the devices may have the same or different structures and / or operate by the same or different mechanism(s). Fuel processing assembly 24 may include at least one throttle orifice and / or other flow restrictor such as associated with one or more product hydrogen streams, (one or more) hydrogen-rich streams, and / or (one or more) by-product streams downstream of the purification region(s).

[0036] The hydrogen selective membrane 46 is permeable to hydrogen gas but is at least substantially, if not completely, impermeable to other components of the output stream 34. The membrane 46 may be formed of any hydrogen permeable material suitable for use in the operating environment and parameters in which the purification zone 40 operates. Examples of suitable materials for the membrane 46 include palladium and palladium alloys, and particularly thin films of such metals and metal alloys. Palladium alloys have proven particularly effective, particularly palladium containing 35 to 45 weight percent copper. Palladium-copper alloys containing approximately 40 weight percent copper have proven particularly effective, although other relative concentrations and compositions may be used. Three other particularly effective alloys are: palladium with 2 to 20 weight percent gold, particularly palladium with 5 weight percent gold; palladium with 3 to 10 weight percent indium plus 0 to 10 weight percent ruthenium, particularly palladium with 6 weight percent indium plus 0.5 weight percent ruthenium; and palladium with 20 to 30 weight percent silver. When palladium and palladium alloys are used, the hydrogen selective membrane 46 may sometimes be referred to as a "foil." The typical thickness of the hydrogen permeable metal foil is less than 25 micrometers, preferably less than or equal to 15 micrometers, most preferably between 5 and 12 micrometers. The foil may be of any suitable size, such as 110 mm x 270 mm.

[0037] Chemical carbon monoxide removal assembly 48 is a device that chemically reacts carbon monoxide and / or other undesirable components of output stream 34 to form other components that are not potentially harmful. Examples of chemical carbon monoxide removal assemblies include: a water-gas shift reactor configured to produce hydrogen and carbon dioxide from water and carbon monoxide; a partial oxidation reactor configured to convert carbon monoxide and oxygen (typically from air) to carbon dioxide; and a methanation reactor configured to convert carbon monoxide and hydrogen to methane and water. Fuel processing assembly 24 may include more than one type and / or number of chemical removal devices.

[0038] Pressure swing adsorption (PSA) is a chemical process in which gaseous impurities are removed from the output stream 34 based on the principle that certain gases will adsorb more strongly to an adsorbent material than other gases under appropriate temperature and pressure conditions. Typically, non-hydrogen impurities are adsorbed and removed from the output stream 34. Adsorption of the impurity gas occurs at elevated pressure. When the pressure is reduced, the impurities are desorbed from the adsorbent material, thereby regenerating the adsorbent material. Typically, PSA is a cyclic process requiring at least two beds for continuous (as opposed to batch) operation. Examples of suitable adsorbent materials that can be used for the adsorption beds are activated carbon and zeolites. The PSA system 50 also provides an example of an apparatus for a purification zone 40 in which byproducts or removed components are not directly discharged from the zone as a gas stream while the output stream is purified. Instead, these byproduct components are removed when the adsorbent material is regenerated, or are otherwise removed from the purification zone.

[0039] exist Figure 1 , purification region 40 is shown within fuel processing assembly 24. The purification region may alternatively be located separately downstream of the fuel processing assembly, such as Figure 1 Purification region 40 may also include portions inside and outside the fuel processing assembly.

[0040] The fuel processing assembly 24 may also include a temperature regulation assembly in the form of a heating assembly 52. ​​The heating assembly may be configured to generate at least one heated exhaust stream 54 from at least one heated fuel stream 28, typically combusted in the presence of air. The heated exhaust stream 54 is heated at Figure 1 Schematically illustrated as heating the hydrogen production region 32. The heating assembly 52 may include any suitable structure configured to generate a heated exhaust stream, such as a burner or a combustion catalyst, in which a fuel is combusted with air to produce a heated exhaust stream. The heating assembly may include an igniter or ignition source 58 configured to initiate combustion of the fuel. Examples of suitable ignition sources include one or more spark plugs, glow plugs, combustion catalysts, ignition torches, piezoelectric igniters, spark igniters, hot surface igniters, etc.

[0041] In some embodiments, the heating assembly 52 may include a burner assembly 60 and may be referred to as a combustion-based or combustion-driven heating assembly. In a combustion-based heating assembly, the heating assembly 52 may be configured to receive at least one fuel stream 28 and combust the fuel stream in the presence of air to provide a hot exhaust stream 54 that may be used to heat at least the hydrogen production region of the fuel processing assembly. The air may be delivered to the heating assembly by a variety of mechanisms. For example, the air stream 62 may be delivered to the heating assembly as a separate stream, such as Figure 1 Alternatively or additionally, the air flow 62 may be delivered to the heating assembly along with at least one of a fuel flow 28 for the heating assembly 52 and / or drawn from an environment in which the heating assembly is used.

[0042] The exhaust stream 54 may additionally or alternatively be used to heat other parts of a fuel processing assembly and / or a fuel cell system used with the heating assembly. In addition, other configurations and types of heating assemblies 52 may be used. For example, the heating assembly 52 may be an electrically driven heating assembly configured to generate heat to heat at least the hydrogen production region 32 of the fuel processing assembly 24 by using at least one heating element such as a resistive heating element. In those embodiments, the heating assembly 52 may not receive and burn a combustible fuel stream to heat the hydrogen production region to a suitable hydrogen production temperature. Examples of heating assemblies are disclosed in U.S. Pat. No. 7,632,322, the entire disclosure of which is incorporated herein by reference for all purposes.

[0043] The heating assembly 52 may be housed in a common housing or in a common housing or shell with the hydrogen generation region and / or separation region (as discussed further below). The heating assembly may be positioned separately relative to the hydrogen generation region 32, but in thermal and / or fluid communication with the region to provide the desired heating of at least the hydrogen generation region. The heating assembly 52 may be partially or completely located within the common housing, and / or at least a portion (or all) of the heating assembly may be located outside the housing. When the heating assembly is located outside the housing, hot combustion gases from the burner assembly 60 may be delivered to one or more components within the housing via suitable heat transfer conduits.

[0044] The heating assembly can also be configured to heat: the feedstock delivery system 22, the feedstock supply stream, the hydrogen production zone 32, the purification (or separation) zone 40, or any suitable combination of those systems, streams and regions. The heating of the feedstock supply stream can include vaporizing a component of a liquid reactant stream or a hydrogen production fluid for producing hydrogen in the hydrogen production zone. In this embodiment, the fuel processing assembly 24 can be described as including a vaporization zone 64. The heating assembly can be further configured to heat other components of the hydrogen generation assembly. For example, the heated exhaust stream can be configured to heat a pressure vessel and / or other tank that contains heated fuel and / or forms at least a portion of the feed stream 26 and the fuel stream 28 hydrogen production fluid.

[0045] The heating assembly 52 can reach and / or maintain any suitable temperature in the hydrogen production zone 32. The steam reformer is typically operated in a temperature range of 200°C to 900°C. However, temperatures outside this range are also within the scope of the present disclosure. When the carbonaceous feedstock is methanol, the steam reforming reaction will typically be carried out in a temperature range of about 200-500°C. An example subset of this range includes 350-450°C, 375-425°C, and 375-400°C. When the carbonaceous feedstock is a hydrocarbon, ethanol, or another alcohol, a temperature range of about 400-900°C will typically be used for the steam reforming reaction. An example subset of this range includes 750-850°C, 725-825°C, 650-750°C, 700-800°C, 700-900°C, 500-800°C, 400-600°C, and 600-800°C. The hydrogen generation zone 32 may include two or more regions or portions, each of which may operate at the same or different temperatures. For example, when the hydrogen generation fluid includes hydrocarbons, the hydrogen generation zone 32 may include two different hydrogen generation portions or regions, one of which operates at a lower temperature than the other to provide a pre-reforming region. In those embodiments, the fuel processing assembly may also be referred to as including two or more hydrogen generation zones.

[0046] The fuel stream 28 may include any (one or more) flammable liquids and / or (one or more) gases suitable for being consumed by the heating component 52 to provide the desired heat output. Some fuel streams may be gases when delivered and burned by the heating component 52, while other fuel streams may be delivered to the heating component as liquid streams. Examples of heating fuels suitable for the fuel stream 28 include carbonaceous raw materials such as methanol, methane, ethane, ethanol, ethylene, propane, propylene, butane, etc. Other examples include low molecular weight condensable fuels such as liquefied petroleum gas, ammonia, light amines, dimethyl ether, and low molecular weight hydrocarbons. Still other examples include hydrogen and carbon monoxide. In an embodiment of the hydrogen generation component 20 including a temperature regulating component in the form of a cooling component rather than a heating component (such as when an exothermic hydrogen generation process, such as partial oxidation, is used to replace an endothermic process such as steam reforming), the feedstock delivery system may be configured to supply a fuel or coolant stream to the component. Any suitable fuel or cooling fluid may be used.

[0047] Fuel processing assembly 24 may further include an enclosure or housing 66 containing at least hydrogen production region 32, such as Figure 1 As shown. In some embodiments, vaporization region 64 and / or purification region 40 may additionally be contained within a housing. The housing may enable components of a steam reformer or other fuel processing mechanism to be moved as a unit. The housing may also protect components of the fuel processing assembly from damage by providing a protective enclosure and / or may reduce heating requirements for the fuel processing assembly because the components may be heated as a unit. The housing may include insulating material 68, such as solid insulating material, mat insulating material, and / or a gas-filled cavity. The insulating material may be inside the housing, outside the housing, or both. When the insulating material is outside the housing, the fuel processing assembly 24 may also include an outer cover or jacket 70 outside the insulating material, such as Figure 1 The fuel processing assembly may include a different housing that includes additional components of the fuel processing assembly, such as feedstock delivery system 22 and / or other components.

[0048] One or more components of fuel processing assembly 24 may extend beyond the enclosure or be located outside the enclosure. For example, purification region 40 may be located outside the enclosure, such as being spaced apart from the enclosure but in fluid communication with the enclosure via suitable fluid transfer conduits. As another example, a portion of hydrogen production region 32 (such as a portion of one or more reforming catalyst beds) may extend beyond the enclosure, such as Figure 1 Examples of suitable hydrogen generating assemblies and components thereof are disclosed in US Pat. Nos. 5,861,137, 5,997,594, and 6,221,117, the entire disclosures of which are incorporated herein by reference for all purposes.

[0049] Another example of a hydrogen generation assembly 20 is Figure 2 As shown, generally indicated at 72. Unless specifically excluded, the hydrogen generation assembly 72 may include one or more components of the hydrogen generation assembly 20. The hydrogen generation assembly 72 may include a feedstock delivery system 74, a vaporization region 76, a hydrogen generation region 78, and a heating assembly 80, such as Figure 2 In some embodiments, the hydrogen generation assembly 72 may further include a purification region 82 .

[0050] The feedstock delivery system may include any suitable structure, any suitable structure is configured to deliver one or more feed streams and / or fuel streams to one or more other components of the hydrogen generation assembly. For example, the feedstock delivery system may include a feedstock tank (or container) 84 and a pump 86. The feedstock tank may include any suitable hydrogen generation fluid 88, such as water and carbonaceous raw materials (such as, methanol / water mixture). Pump 86 may have any suitable structure, any suitable structure is configured to deliver hydrogen generation fluid to vaporization zone 76 and / or hydrogen generation zone 78, and the hydrogen generation fluid may be in the form of at least one liquid-containing feed stream 90 containing water and carbonaceous raw materials.

[0051] The vaporization region 76 may include any suitable structure configured to receive and vaporize at least a portion of a liquid-containing feed stream, such as liquid-containing feed stream 90. For example, the vaporization region 76 may include a vaporizer 92 configured to at least partially convert the liquid-containing feed stream 90 into one or more vapor feed streams 94. In some embodiments, the vapor feed stream may include a liquid. An example of a suitable evaporator is a coiled tube evaporator, such as a coiled stainless steel tube.

[0052] The hydrogen generation region 78 may include any suitable structure configured to receive one or more feed streams, such as (one or more) steam feed streams 94 from the vaporization region, to produce one or more output streams 96 containing hydrogen as a main component and other gases. The hydrogen generation region may generate the output stream by any suitable (one or more) mechanism. For example, the hydrogen generation region 78 may generate (one or more) output streams 96 by a steam reforming reaction. In this example, the hydrogen generation region 78 may include a steam reforming region 97 having a reforming catalyst 98 configured to facilitate and / or promote the steam reforming reaction. When the hydrogen generation region 78 generates (one or more) output streams 96 by a steam reforming reaction, the hydrogen generation assembly 72 may be referred to as a "steam reforming hydrogen generation assembly" and the output stream 96 may be referred to as a "reformed stream".

[0053] The heating assembly 80 may include any suitable structure configured to generate at least one heated exhaust stream 99 for heating one or more other components of the hydrogen generation assembly 72. For example, the heating assembly may heat the vaporization region to any suitable temperature(s), such as at least a minimum vaporization temperature or a temperature at which at least a portion of the liquid-containing feed stream is vaporized to form a vapor feed stream. Additionally, or alternatively, the heating assembly 80 may heat the hydrogen generation region to any suitable temperature(s), such as at least a minimum hydrogen generation temperature or a temperature at which at least a portion of the vapor feed stream reacts to generate hydrogen to form an output stream. The heating assembly may be in thermal communication with one or more components of the hydrogen generation assembly, such as the vaporization region and / or the hydrogen generation region.

[0054] like Figure 2 As shown, the heating assembly may include a burner assembly 100, at least one blower 102, and an igniter assembly 104. The burner assembly may include any suitable structure configured to receive at least one air stream 106 and at least one fuel stream 108 and burn at least one fuel stream in a combustion zone 110 to produce a heated exhaust stream 99. The fuel stream may be provided by the feedstock delivery system 74 and / or the purification zone 82. The combustion zone may be contained within an enclosure of the hydrogen generation assembly. The blower 102 may include any suitable structure configured to generate (one or more) air streams 106. The igniter assembly 104 may include any suitable structure configured to ignite (one or more) fuel streams 108.

[0055] The purification region 82 may include any suitable structure configured to produce at least one hydrogen-rich stream 112 that may include a higher hydrogen concentration than the output stream 96 and / or a reduced concentration of one or more other gases (or impurities) present in the output stream. The purification region may produce at least one byproduct stream or fuel stream 108 that may be sent to the combustor assembly 100 and used as a fuel stream for the assembly, such as Figure 2 Purification zone 82 may include a flow restriction orifice 111, a filter assembly 114, a membrane assembly 116, and a methanation reactor assembly 118. A filter assembly, such as one or more hot gas filters, may be configured to remove impurities from output stream 96 prior to the hydrogen purification membrane assembly.

[0056] The membrane assembly 116 may include any suitable structure configured to receive the output stream(s) 96 or the mixed gas stream(s) containing hydrogen and other gases, and configured to generate the permeate stream(s) or hydrogen-rich stream 112 containing a higher concentration of hydrogen than the mixed gas stream and / or a lower concentration of other gases than the mixed gas stream. The membrane assembly 116 may incorporate a planar or tubular hydrogen permeable (or hydrogen selective) membrane, and more than one hydrogen permeable membrane may be incorporated into the membrane assembly 116. The permeate stream(s) may be used for any suitable application, such as for one or more fuel cells. In some embodiments, the membrane assembly may generate a byproduct or fuel stream 108 including at least a substantial portion of other gases. The methanation reactor assembly 118 may include any suitable structure configured to convert carbon monoxide and hydrogen into methane and water. Although purification region 82 is shown as including restriction orifice 111, filter assembly 114, membrane assembly 116, and methanation reactor assembly 118, purification region may have fewer than all of these components and / or may alternatively or additionally include one or more other components configured to purify output stream 96. For example, purification region 82 may include only membrane assembly 116.

[0057] In some embodiments, the hydrogen generation assembly 72 may include an enclosure or housing 120 that may at least partially contain one or more other components of the assembly. For example, the enclosure may at least partially contain the vaporization region 76, the hydrogen generation region 78, the heating assembly 80, and / or the purification region 82, as shown in FIG. Figure 2 The housing may include one or more exhaust ports 122 configured to exhaust at least one combustion exhaust stream 124 generated by the heating assembly 80 .

[0058] In some embodiments, the hydrogen generation assembly 72 may include a control system 126, which may include any suitable structure configured to control the operation of the hydrogen generation assembly 72. For example, the control system 126 may include a control assembly 128, at least one valve 130, at least one pressure reducing valve 132, and one or more temperature measuring devices 134. The control assembly 128 may detect the temperature in the hydrogen generation region and / or purification region through the temperature measuring device 134, which may include one or more thermocouples and / or other suitable devices. Based on the detected temperature, the operator of the control assembly and / or the control system may adjust the delivery of the feed stream 90 to the vaporization region 76 and / or the hydrogen generation region 78 via the (one or more) valves 130 and the (one or more) pumps 86. The (one or more) valves 130 may include solenoid valves and / or any suitable (one or more) valves. The (one or more) pressure reducing valves 132 may be configured to ensure that the overpressure in the system is released.

[0059] In some embodiments, the hydrogen generation assembly 72 may include a heat exchange assembly 136, which may include one or more heat exchangers 138 configured to transfer heat from one portion of the hydrogen generation assembly to another portion. For example, the heat exchange assembly 136 may transfer heat from the hydrogen rich stream 112 to the feed stream 90 to increase the temperature of the feed stream before entering the vaporization region 76, as well as cool the hydrogen rich stream 112.

[0060] Figure 1 An example of a purification region 40 of a hydrogen generation assembly 20 is shown in Figure 3 144. Unless specifically excluded, the hydrogen purification device may include one or more components of other purification regions described in the present disclosure. The purification region 144 may include a hydrogen separation region 146 and an encapsulating shell 148. The encapsulating shell may define an interior volume 150 having an inner perimeter 152. The encapsulating shell 148 may include at least a first portion 154 and a second portion 156 that are coupled together to form a body 149 in the form of a sealed pressure vessel that may include defined input and output ports. These ports may define fluid paths through which gases and other fluids are delivered to and removed from the interior volume of the encapsulating shell.

[0061] The first part 154 and the second part 156 can be coupled together using any suitable retaining mechanism or structure 158. Examples of suitable retaining structures include welds and / or bolts. Examples of seals that can be used to provide a fluid-tight interface between the first part and the second part may include gaskets and / or welds. Additionally or optionally, the first part 154 and the second part 156 can be fixed together so that at least a predetermined amount of compression is applied to various components and / or other components that define a hydrogen separation zone within the enclosure that can be incorporated into the hydrogen generation assembly. The applied compression can ensure that the various components remain in place within the enclosure. In addition, or alternatively, the compression applied to the various components and / or other components that define the hydrogen separation zone can provide a fluid-tight interface between the various components that define the hydrogen separation zone, various other components, and / or between the various components and other components that define the hydrogen separation zone.

[0062] like Figure 3As shown, the encapsulation shell 148 may include a mixed gas zone 160 and a permeation zone 162. The mixed gas zone and the permeation zone may be separated by a hydrogen separation zone 146. At least one input port 164 may be provided, through which a fluid stream 166 is delivered to the encapsulation shell. The fluid stream 166 may be a mixed gas stream 168, which contains hydrogen 170 and other gases 172 delivered to the mixed gas zone 160. Hydrogen may be the main component of the mixed gas stream. The hydrogen separation zone 146 may extend between the mixed gas zone 160 and the permeation zone 162, so that the gas in the mixed gas zone must pass through the hydrogen separation zone to enter the permeation zone. The gas may, for example, need to pass through at least one hydrogen selective membrane, as discussed further below. The permeation gas zone and the mixed gas zone may have any suitable relative size within the encapsulation shell.

[0063] The enclosure 148 may also include at least one product output port 174 through which a permeate stream 176 may be received and removed from the permeate zone 162. The permeate stream may contain at least one of a higher concentration of hydrogen than the mixed gas stream and a lower concentration of other gases than the mixed gas stream. In some embodiments, the permeate stream 176 may at least initially include a carrier gas component or a purge gas component, such as may be delivered as a purge gas stream 178 through a purge gas port 180 in fluid communication with the permeate zone. The enclosure may also include at least one byproduct output port 182 through which a byproduct stream 184 containing at least one of a majority of the other gases 172 and a reduced concentration of hydrogen 170 (relative to the mixed gas stream) is removed from the mixed gas zone.

[0064] The hydrogen separation zone 146 may include at least one hydrogen selective membrane 186 having a first or mixed gas surface 188 and a second or permeate surface 190, the first or mixed gas surface being oriented to contact the mixed gas stream 168, and the second or permeate surface being substantially opposite to the surface 188. The mixed gas stream 168 may be delivered to the mixed gas zone of the encapsulating shell so that it contacts the mixed gas surface of one or more hydrogen selective membranes. The permeate stream 176 may be formed by at least a portion of the mixed gas stream that passes through the hydrogen separation zone to reach the permeate zone 162. The byproduct stream 184 may be formed by at least a portion of the mixed gas stream that does not pass through the hydrogen separation zone. In some embodiments, the byproduct stream 184 may include a portion of the hydrogen present in the mixed gas stream. The hydrogen separation zone may also be configured to capture or otherwise retain at least a portion of other gases, which may then be removed as a byproduct stream when the separation zone is replaced, regenerated, or otherwise refilled.

[0065] exist Figure 3166, 176, 178, and / or 184 may include more than one actual stream flowing into or out of the hydrogen purification device 144. For example, the hydrogen purification device may receive multiple mixed gas streams 168, a single mixed gas stream 168 that is split into two or more streams prior to contacting the hydrogen separation region 146, a single stream that is delivered to the interior volume 150, etc. Thus, the enclosure 148 may include more than one input port 164, product output port 174, purge gas port 180, and / or byproduct output port 182.

[0066] The hydrogen selective membrane may be formed of any hydrogen permeable material suitable for use in the operating environment and parameters in which the hydrogen purification device operates. Examples of hydrogen purification devices are disclosed in U.S. Pat. Nos. 5,997,594 and 6,537,352, the entire disclosures of which are incorporated herein by reference for all purposes and used. In some embodiments, the hydrogen selective membrane may be formed of at least one of palladium and a palladium alloy. Examples of palladium alloys include alloys of palladium with copper, silver and / or gold. Examples of various membranes, membrane configurations, and methods for preparing membranes and membrane configurations are disclosed in U.S. Pat. Nos. 6,152,995, 6,221,117; 6,319,306, and 6,537,352, the entire disclosures of which are incorporated herein by reference for all purposes.

[0067] In some embodiments, a plurality of spaced-apart hydrogen selective membranes 186 may be used in the hydrogen separation region to form at least a portion of the hydrogen separation assembly 192. When present, the plurality of membranes may collectively define one or more membrane assemblies 194. In such embodiments, the hydrogen separation assembly may generally extend from the first portion 154 to the second portion 156. Thus, the first portion and the second portion may effectively compress the hydrogen separation assembly. In some embodiments, the enclosure 148 may additionally or alternatively include end plates (or end frames) coupled to opposite sides of the body portion. In such embodiments, the end plates may effectively compress the hydrogen separation assembly (and other components that may be housed within the enclosure) between a pair of opposing end plates.

[0068] Hydrogen purification using one or more hydrogen selective membranes is typically a pressure driven separation process in which a mixed gas stream is delivered into contact with the mixed gas surface of the membrane at a higher pressure than the gas in the permeate zone of the hydrogen separation zone. In some embodiments, when the hydrogen separation zone is used to separate the mixed gas stream into a permeate stream and a byproduct stream, the hydrogen separation zone may be heated to an elevated temperature via any suitable mechanism. Examples of suitable operating temperatures for hydrogen purification using palladium and palladium alloy membranes include temperatures of at least 275°C, temperatures of at least 325°C, temperatures of at least 350°C, temperatures in the range of 275-500°C, temperatures in the range of 275-375°C, temperatures in the range of 300-450°C, temperatures in the range of 350-450°C, and the like.

[0069] An example of a hydrogen purification unit 144 is Figure 4 196. Unless specifically excluded, the hydrogen purification device 196 may include one or more components of other hydrogen purification devices and / or purification regions described in the present disclosure. The hydrogen purification device 196 may include an outer shell or enclosure 198, which may include a first end plate or end frame 200 and a second end plate or end frame 202. The first end plate and the second end plate may be configured to be fixed and / or compressed together to define a sealed pressure vessel having an internal compartment 204, in which the hydrogen separation region is supported. The first end plate and the second end plate may include input ports, output ports, purge gas ports, and byproduct ports (not shown) similar to the hydrogen purification device 144.

[0070] The hydrogen purification device 196 may also include at least one foil-microsieve assembly 205, which may be disposed between and / or secured to the first end plate and the second end plate. The foil-microsieve assembly may include at least one hydrogen selective membrane 206 and at least one microsieve structure 208, such as Figure 5 As shown. The hydrogen selective membrane may be configured to receive at least a portion of the mixed gas stream from the input port and separate the mixed gas stream into at least a portion of a permeate stream and at least a portion of a byproduct stream. The hydrogen selective membrane 206 may include a feed side 210 and a permeate side 212. At least a portion of the permeate stream is formed by a portion of the mixed gas stream that is transported from the feed side to the permeate side, wherein the remaining portion of the mixed gas stream that remains on the feed side forms at least a portion of the byproduct stream.

[0071] The one or more hydrogen selective membranes may be metallurgically bonded to the microsieve structure 208. For example, the permeate side of the hydrogen selective membrane(s) may be metallurgically bonded to the microsieve structure. In some embodiments, the one or more hydrogen selective membranes 206 (and / or the permeate sides of those membrane(s)) may be diffusion bonded to the microsieve structure to form a solid state diffusion bond between the membrane(s) and the microsieve structure. For example, the permeate side of the membrane(s) and the microsieve structure may be brought into contact with each other and exposed to elevated temperatures and / or elevated pressures to allow the surfaces of the membrane(s) and the microsieve structure to self-dissolve over time.

[0072] In some embodiments, the microsieve structure may be coated with a thin layer of metal or an intermediate bonding layer that facilitates diffusion bonding. For example, a thin coating of nickel, copper, silver, gold, or other metal that is subject to solid state diffusion bonding but does not (1) melt and enter the liquid phase at temperatures less than or equal to 700°C, and (2) form a low melting point alloy at temperatures less than or equal to 700°C after diffusion into the (one or more) hydrogen selective membranes. The thin metal layer may be applied to the microsieve structure by a suitable deposition process (e.g., electrochemical plating, vapor deposition, sputtering, etc.) of a thin coating of the intermediate bonding layer onto the surface of the microsieve structure that will contact the hydrogen selective membrane. In some embodiments, the foil-microsieve assembly 205 includes only the (one or more) hydrogen selective membranes and the (one or more) microsieve structure (with or without the above-mentioned coating) and is free of any other framework, gasket, component, and / or structure attached, bonded, and / or metallurgically bonded to one or both of the (one or more) hydrogen selective membranes and / or the (one or more) microsieve structure. In other embodiments, the hydrogen-selective membrane(s) may be secured to at least one membrane frame (not shown), which may then be secured to the first and second end frames.

[0073] The microsieve structure 208 may include any suitable structure configured to support at least one hydrogen-selective membrane. For example, the microsieve structure may include: a non-porous planar sheet 213 having generally opposing surfaces 214 and 215 configured to provide support for the permeate side 212; and a plurality of orifices 216 forming a plurality of fluid channels 217 extending between the opposing surfaces, which allow the permeate flow to flow through the microsieve structure, such as Figure 6 As shown. The orifices can be formed in the non-porous planar sheet by electrochemical etching, laser drilling and other mechanical forming processes, such as stamping or die cutting. In other words, the planar sheet is made of one or more materials that do not include any openings or orifices, and the only orifices or openings in the sheet are added by one or more of the above methods. In some embodiments, one or more orifices (or all orifices) can be formed in the non-porous planar sheet so that their longitudinal axes or the longitudinal axes of the fluid channels are perpendicular to the plane of the non-porous planar sheet, such as Figure 6 The non-porous planar sheet may have any suitable thickness, such as between 100 microns and about 200 microns.

[0074] In some embodiments, the micro-sieve structure 208 may include: one or more perforated regions (or portions) 218, the perforated regions including a plurality of pores; and one or more non-perforated regions (or portions) 219, the non-perforated regions not including (or excluding) a plurality of pores. Figure 6Only a few apertures 216 are illustrated, but the apertures 216 are distributed over the entire length and width of the (one or more) perforated portions. The (one or more) perforated areas may be discrete or spaced apart from one or more other perforated areas. The (one or more) non-perforated areas 219 may include: a perimeter area (or portion) 220 that forms a frame around one or more of the (one or more) perforated areas; and / or one or more boundary areas (or portions) 221 that separate or define two or more discrete portions of the perforated area. In other words, each perforated portion may be spaced apart from other adjacent discrete perforated portions by at least one boundary portion that does not have multiple apertures.

[0075] The aperture 216 may include any suitable pattern(s), shape(s), and / or size(s). In some embodiments, the aperture may be formed with one or more patterns that maximize the combined aperture area while maintaining a sufficiently high stiffness of the microsieve structure to prevent excessive deflection under pressure loads. The aperture 216 may be: Figure 6 The circle shown; Figures 7 to 10 The orifice 216 in the perforated area may be an elongated circular, racetrack or stadium shape as shown; an oval, elliptical, hexagonal, triangular, square, rectangular, octagonal and / or other suitable (one or more) shapes. In some embodiments, the orifice 216 in the (one or more) perforated areas may be a single consistent shape. In other embodiments, the orifice 216 in the perforated area may be any suitable combination of two or more different shapes, such as two or more of the above shapes.

[0076] The apertures 216 may have any suitable orientation(s) and / or be in any suitable pattern(s). Figure 7 The apertures 216 are shown to be oriented longitudinally (or along the length of the perforated region(s) or the length of the planar sheet) and arranged consecutively in parallel rows. In other words, each aperture 216 has a length defining a longitudinal axis 223, and Figure 7 The longitudinal axes of all the orifices in the planar sheet 213 are parallel to and / or coaxial with the longitudinal axis 225 (in Figure 6 or, Figure 9-10 The orifices are shown to be oriented laterally (or along the width of the perforated region(s) or the width of the planar sheet). In other words, Figures 9 and 10 In the example of FIG. 2 , the longitudinal axes 223 of all the orifices are perpendicular to the longitudinal axis 225 of the planar sheet 213 .

[0077] Although the orifice 216 Figure 7 and Figures 9 and 10are all shown as being in the same direction or orientation. Other embodiments of the planar sheet 213 may include orifices 216 having two or more directions and / or orientations. For example, the orifices 216 may be arranged in a staggered pattern such that the orifices in each row or column are oriented differently (e.g., 30, 45, 60, 90, 120 degrees) than the orifices in each adjacent row or column. In other words, the longitudinal axes 223 of the orifices 216 in each row or column are parallel to each other and / or non-parallel to the longitudinal axes 223 of the orifices in one or more adjacent rows or columns on the planar sheet 213. In one example, the orifices 216 are also oriented in a diagonal direction and are arranged consecutively in parallel rows such that the orifices in each row are oriented approximately ninety degrees to the orifices in the adjacent row, such as Figure 8 Alternatively or additionally, one or more apertures 216 in one or more rows and / or columns may be oriented differently than one or more other apertures in the same row and / or column.

[0078] The orifice can be of any suitable size(s). For example, when the orifice is circular, the diameter can range from about 0.003 inches to about 0.020 inches. In addition, when the orifice is oval or elliptical, the radius of the rounded end of the oval or ellipse can be in the range of 0.001 inches to about 0.010 inches and the length of the oval or ellipse can be up to ten times the radius. In addition, when the orifice is elongated circular or stadium-shaped, the width or diameter can range from 0.005 inches to 0.02 inches and the length can range from 0.05 inches to more than ten times the diameter, such as 0.8 inches. Figure 8 An example of the size of the medium orifice is 0.10 inches in diameter at the rounded end and 0.028 inches in length (ie, an aspect ratio of about 3) with 0.006 inches between orifices or 0.011 inches between the centers of adjacent orifices. Figure 8 The pattern and example dimensions shown in provide approximately 50% of the total open area in the microsieve structure.

[0079] In some examples, one or more apertures 216 are sized to span the entire or substantially the entire width or length of the perforated area. Fig. 9 In the example shown, the stadium shaped aperture is oriented transversely and is the entire width or substantially the entire width of the perforated region(s) or portion(s) such that the aspect ratio (length / width) is much greater than ten. Fig. 9 Exemplary dimensions of the medium apertures are 0.005 to 0.02 inches wide and up to 8 inches long. The apertures may be spaced about 0.006 inches apart (ie, the width of the non-perforated portion or solid area between adjacent apertures) to provide a total open area of ​​up to about 62.5%.

[0080] In some examples, the apertures 216 can have a combination of various sizes. For example, the apertures 216 can be sized such that the planar sheet 213 includes multiple rows and / or columns of apertures having (1) a smaller number of apertures having one or more longer lengths and (2) a larger number of apertures having one or more shorter lengths. In some examples, the rows and / or columns with a smaller number of apertures having longer lengths alternate with the rows and / or columns with a larger number of apertures having shorter lengths, such as in a staggered pattern. Fig.10 In the example shown, the apertures 216 are oriented transversely (or perpendicular to the longitudinal axis 225 of the planar sheet 213) and each row and / or column alternates between two apertures having a longer length and three apertures having a shorter length. The aperture lengths of each row and / or column may be the same or different. Fig.10 Examples of the dimensions of the medium orifices are 0.005 inches to 0.02 inches wide and 0.05 inches to 8 inches long. The orifices may be spaced about 0.006 inches apart from one another (i.e., the width of the non-perforated portion or solid area between adjacent orifices). Other combinations of patterns, sizes, orientations, and / or shapes of orifices 216 are possible and are included in the present disclosure.

[0081] The non-porous planar sheet may include any suitable material. For example, the non-porous planar sheet may include stainless steel. The stainless steel may include 300 series stainless steel (e.g., stainless steel 303 (aluminum modified), stainless steel 304, etc.), 400 series stainless steel, 17-7PH, 14-8PH, and / or 15-7PH. In some embodiments, the stainless steel may include aluminum in an amount of about 0.6 wt % to about 3.0 wt %. In some embodiments, the non-porous planar sheet may include carbon steel, copper or copper alloy, aluminum or aluminum alloy, nickel, nickel-copper alloy, and / or a base metal plated with silver, nickel, and / or copper. The base metal may include carbon steel or one or more of the above-mentioned stainless steels.

[0082] The hydrogen selective membrane 206 is sized to be larger than the perforated area or region of the micromesh structure such that when the hydrogen selective membrane is metallurgically bonded to the micromesh structure, the perimeter portion 222 of the hydrogen selective membrane contacts the one or more non-perforated regions 219 of the micromesh structure. In some embodiments, a single hydrogen selective membrane may be metallurgically bonded to a single micromesh structure, such as Figure 5 In other embodiments, two or more hydrogen selective membranes 206 may be metallurgically bonded to a single micromesh structure 208. For example, two, three, four, five, six, seven, eight, nine, ten, or more hydrogen selective membranes 206 may be metallurgically bonded to a single micromesh structure 208. Figure 11 to Figure 12 An example foil-microsieve assembly 205 having six hydrogen-selective membranes 206 metallurgically bonded to a single microsieve structure 208 is shown. Fig.13An example foil-microsieve assembly 205 is shown having two hydrogen selective membranes 206 metallurgically bonded to a single microsieve structure 208, while Fig.14 An example foil-microsieve assembly 205 having four hydrogen-selective membranes 206 metallurgically bonded to a single microsieve structure 208 is shown.

[0083] When two or more hydrogen-selective membranes 206 are metallurgically bonded to the microsieve structure, the microsieve structure may include two or more discrete perforated regions 218 separated by one or more non-perforated regions 219. In some embodiments, the perforated regions 218 may be sized to be the same size as the other perforated regions 218. For example, Fig.12 Six discrete perforated areas 218 of approximately the same size are shown. In other embodiments, one or more of the perforated areas 218 may be sized smaller and / or larger than other perforated areas 218. Fig.11 As shown, the hydrogen selective membrane 206 can be metallurgically bonded to each perforated region. Alternatively or additionally, the hydrogen selective membrane can be metallurgically bonded to two or more discrete perforated regions 218. The hydrogen selective membrane(s) 206 can be sized such that a perimeter portion 222 of the membrane contacts one or more non-perforated regions 219 when the membrane is metallurgically bonded to one or more perforated regions 218.

[0084] like Figure 5 As shown, the microsieve structure 208 can be sized to be contained (such as completely contained) in the open area of ​​the infiltration frame and / or supported by the membrane support structure in the open area. In other words, when the microsieve structure and the infiltration frame are fixed or compressed to the first end frame and the second end frame, the microsieve structure can be sized to not contact the perimeter frame of the infiltration frame. Alternatively, the microsieve structure can be supported and / or fixed to the non-porous perimeter wall or frame (not shown) by a non-porous perimeter wall or frame (not shown), such as being fixed to the perimeter frame of the infiltration frame. When the microsieve structure is fixed to the non-porous perimeter wall, the microsieve structure can be referred to as a "porous central area portion". Examples of other microsieve structures are disclosed in U.S. Patent Application Publication No. 2010 / 0064887, the complete disclosure of which is incorporated herein by reference for all purposes.

[0085] The hydrogen purification device 196 may also include a plurality of plates or frames 224 disposed between and secured to the first end frame and / or the second end frame. These frames may include any suitable structure and / or may be any suitable (one or more) shapes, such as square, rectangular, or circular. For example, the frame 224 may include a perimeter frame 226 and at least a first support member 228, such as Figure 4As shown. The perimeter frame can define an opening area 230 and a frame plane 232. In addition, the perimeter frame 226 may include a first opposite side 234 and a second opposite side 236, as well as a third opposite side 238 and a fourth opposite side 240, as shown. Figure 4 shown.

[0086] The first support member 228 may include any suitable structure configured to support the first portion 242 of the foil-microsieve assembly 205, such as Figure 4 For example, the first support members of the plurality of frames may be coplanar with each other (or coplanar with other first support members of other frames of the plurality of frames) within a first support plane 244 to support the first portion 242 of the hydrogen-selective membrane, as shown in FIG. Figure 4 In other words, the first support member of each frame in the plurality of frames can mirror the first support members of other frames in the plurality of frames. The first support member can have any suitable orientation relative to the frame plane 232. For example, the first support plane 244 can be perpendicular to the frame plane, such as Figure 4 Alternatively, the first membrane support plane may intersect the frame plane 232 but not be perpendicular.

[0087] In some embodiments, the frame 224 may include a second support member 246 and / or a third support member 248, which may include any suitable structure configured to support the second portion 250 and / or the third portion 252 of the foil-microsieve assembly 205, such as Figure 4 As shown. For example, second support members of the plurality of frames can be coplanar with each other (or coplanar with other second support members of the plurality of frames) within a second support plane 254 to support the second portion 250 of the foil-microsieve assembly. Additionally, third support members of the plurality of frames can be coplanar with each other (or coplanar with other third support members of the plurality of frames) within a third support plane 256 to support the third portion 252 of the foil-microsieve assembly. In other words, the second support member of each frame in the plurality of frames can mirror the second support member of the other frames in the plurality of frames, and the third support member of each frame in the plurality of frames can mirror the third support member of the other frames in the plurality of frames. The second support plane and / or the third support plane can have any suitable orientation relative to the frame plane 232. For example, the second support plane 254 and / or the third support plane 256 can be perpendicular to the frame plane, such as Figure 4 Alternatively, the second support plane and / or the third support plane may intersect the frame plane 232 but not be perpendicular.

[0088] The second support member 246 and / or the third support member 248 can have any suitable orientation relative to the first support member 228. For example, the first support member 228 can extend from the third opposite side 238 of the perimeter frame 226 into the opening area 230, the second support member 246 can extend from the fourth opposite side 240 of the perimeter frame (which is opposite the third opposite side) into the opening area, and the third support member 248 can extend from the third side into the opening area. Alternatively, the first support member, the second support member, and / or the third support member can extend from the same side into the opening area, such as from the first side, the second side, the third side, or the fourth side of the perimeter frame. In some embodiments, the first support member, the second support member, and / or the third support member can extend from the first side and / or the second side of the perimeter frame (which is opposite the first side) into the opening area.

[0089] The first support member, the second support member and / or the third support member can be, for example, in the form of one or more projections 258 attached to the perimeter frame and / or formed with the perimeter frame. The projection can extend from the perimeter frame in any suitable (one or more) direction. The projection can be the full thickness of the perimeter frame or can be less than the full thickness of the frame. The projection of each frame of the frame 224 can be squeezed on the foil-micro sieve assembly, thereby locking the assembly in place. In other words, the projection of the frame 224 can support the foil-micro sieve assembly by (one or more) extensions stacked as end frames in the first membrane support plane and / or the second membrane support plane. In some embodiments, (one or more) projections 258 may include one or more receptacles or orifices (not shown), and the receptacles or orifices are configured to receive at least one fastener (not shown) to fix the frame 224 to the first end frame and / or the second end frame.

[0090] The frame 224 may include at least one feed frame 260, at least one permeate frame 262, and a plurality of gaskets or gasket frames 264, such as Figure 4 The feed frame 260 may be disposed between one of the first end frame and the second end frame and at least one foil-microsieve assembly 205, or between two foil-microsieve assemblies 205. The feed frame may include a feed frame perimeter frame 266, a feed frame input conduit 268, a feed frame output conduit 270, a feed frame opening area 272, at least a first feed frame support member 274, and a plurality of feed frame support members 276, such as a plurality of feed frame support members 276, a plurality of feed frame support members 276, and a plurality of feed frame support members 276. Figure 4As shown. In some embodiments, the feed frame may include a second feed frame support member 276 and / or a third feed frame support member 278. In some embodiments, the end plate, the foil-microsieve assembly, and the frame 224 are fixed or compressed together, such as mechanically fixed and / or mechanically compressed by bolts and / or other fasteners, without any metallurgical bonding and / or other types of chemical bonding between two or more components of the hydrogen purification device (except for the metallurgical bonding between the above-mentioned hydrogen-selective membrane and the coated or uncoated microsieve structure within the (one or more) foil-microsieve assembly). For example, no gaskets and / or frames are metallurgically bonded or otherwise chemically bonded to the (one or more) hydrogen-selective membranes and / or the (one or more) microsieve structures of the (one or more) foil-microsieve assemblies and all other components of the hydrogen purification device.

[0091] Another example of a hydrogen purification unit 144 is Fig.15 396. Unless specifically excluded, hydrogen purification unit 396 may include one or more components of other hydrogen purification units and / or purification regions described in the present disclosure.

[0092] Hydrogen purification device 396 is similar in many respects to hydrogen purification device 196, but has a differently shaped frame, no support members, a differently sized foil-microsieve assembly, and a lesser gasket frame, as further described below. The components or parts of hydrogen purification device 396 correspond to the components or parts of hydrogen purification device 196, and Fig.15 Similar reference numerals are used in the present invention, with the general form of "3XX" instead of "1XX" and "4XX" instead of "2XX". Thus, features 398, 400, 402, 404, 405, 406, 408, 424, 426, 434, 436, 438, 440, 460, 462, 464, etc. can be the same or substantially the same as their respective counterparts in hydrogen purification unit 196, i.e., features 198, 200, 202, 204, 205, 206, 208, 224, 226, 234, 236, 238, 240, 260, 262, 264, etc.

[0093] The hydrogen purification device 396 may include an outer housing or enclosure 398, which may include a first end plate 400 and a second end plate 402. The first end plate and the second end plate may be configured to be secured and / or compressed together to define a sealed pressure vessel having an interior compartment 404 in which the hydrogen separation region is supported.

[0094] The hydrogen purification device 396 may also include at least one foil-microsieve assembly 405, which may be disposed between the first end plate and the second end plate and / or fixed to the first end plate and the second end plate. The foil-microsieve assembly may include at least one hydrogen selective membrane 406 and at least one microsieve structure 408. One or more hydrogen selective membranes may be metallurgically bonded to the microsieve structure 408. For example, one or more hydrogen selective membranes 406 may be diffusion bonded to the microsieve structure to form a solid state diffusion bond between (one or more) membranes and the microsieve structure. The foil-microsieve assembly 405 may be sized to fit the opening area of ​​the permeation frame, and therefore may be smaller in length and width than or relative to the foil-microsieve assembly 205.

[0095] The hydrogen purification device 396 may also include a plurality of plates or frames 424 disposed between and secured to the first end frame and / or the second end frame. The frame 424 may include a perimeter frame body 426. The perimeter frame body may define an open area 430. In addition, the perimeter frame body 426 may include a first opposing side 434 and a second opposing side 436, as well as a third opposing side 438 and a fourth opposing side 440. Unlike the frame 224 of the hydrogen purification device 196, the frame 424 does not include any support members.

[0096] The frame 424 may include at least one feed frame 460, at least one permeate frame 462, and a plurality of gaskets or gasket frames 464. The feed frame 460 may be disposed between one of the first end frame and the second end frame and at least the foil-microsieve assembly 405, or between two foil-microsieve assemblies 405. The feed frame may include at least substantially similar components to the feed frame 260, such as a feed frame perimeter frame, a feed frame input conduit, a feed frame output conduit, and / or a feed frame opening area.

[0097] The permeate frame 462 may be positioned such that at least one foil-microsieve assembly is disposed between one of the first end frame and the second end frame and the permeate frame or between two foil-microsieve assemblies. The permeate frame may include components at least substantially similar to the permeate frame 262, such as a permeate frame perimeter frame, a permeate frame output conduit, a permeate frame opening area, and / or a membrane support structure.

[0098] The frame 424 may also include a gasket or gasket frame 464. The gasket frame may include any suitable structure configured to provide a fluid-tight interface between other frames, such as between the first end plate 400 and the second end plate 402 and the feed frame 460, and / or between the feed frame 460 and the foil-microsieve assembly 405. Unlike the hydrogen purification device 196, the hydrogen purification device 396 does not include a gasket frame 464 between the foil-microsieve assembly and the permeate frame 462. Similar to the hydrogen purification device 196, the width of the feed frame and the gasket frame is greater than the width of the permeate frame (or the open area of ​​the feed frame and the gasket frame is less than the open area of ​​the permeate frame), so that the additional width covers the edge of the foil-microsieve assembly to eliminate or minimize leakage from the feed side to the permeate side or from the permeate side to the feed side (e.g., the additional width of the feed frame and the gasket frame covers the edge of the foil-microsieve assembly). In some embodiments, the additional width corresponds to the width of the perimeter (non-perforated) portion of the microsieve structure of the foil-microsieve assembly.

[0099] Industrial Applicability: The present disclosure, including hydrogen purification devices and components of such devices, may be applicable to the fuel processing industry and other industries that purify, produce and / or utilize hydrogen.

[0100] The above disclosure includes a plurality of different inventions with independent practicality. Although each of these inventions is disclosed in its preferred form, the specific embodiments disclosed and described here should not be considered as restrictive, because many variations are possible. The subject matter of the present invention includes all novel and non-obvious combinations and sub-combinations of various elements, features, functions and / or characteristics disclosed herein. Similarly, in the case where any claim mentions "one" or "first" element or its equivalent, such a claim should be understood to include incorporation of one or more such elements, neither requiring nor excluding two or more such elements.

[0101] Inventions embodied in various combinations and subcombinations of features, functions, elements and / or characteristics may be claimed by presenting new claims in related applications. Such new claims, whether directed to different inventions or to the same invention, and whether different, broader, narrower or the same in scope as the original claims, are also deemed to be included in the subject matter of the inventions disclosed herein.

Claims

1. A hydrogen purification device, comprising: The first end frame and the second end frame include: an input port configured to receive a mixed gas flow including hydrogen and other gases; an output port configured to receive a permeate stream comprising at least one of a higher concentration of hydrogen than the mixed gas stream and a lower concentration of other gases than the mixed gas stream; and a byproduct port configured to receive a byproduct stream comprising at least a majority of the other gas; at least one foil-microsieve assembly disposed between and secured to the first end frame and the second end frame, the at least one foil-microsieve assembly comprising: at least one hydrogen selective membrane having a feed side and a permeate side, at least a portion of the permeate stream being formed by the portion of the mixed gas stream flowing from the feed side to the permeate side, wherein the remainder of the mixed gas stream remaining on the feed side forms at least a portion of the byproduct stream, and at least one microsieve structure comprising a nonporous planar sheet having a plurality of apertures forming a plurality of fluid channels, each aperture of the plurality of apertures having a length defining a longitudinal axis, the plurality of apertures being positioned on the nonporous planar sheet in a plurality of rows such that the longitudinal axes of the apertures in the plurality of apertures in each of the plurality of rows are (1) parallel to each other and (2) non-parallel to the longitudinal axes of the apertures in the plurality of apertures in an adjacent row of the plurality of rows and (3) oriented at an angle to the longitudinal axes of the apertures in the plurality of apertures in an adjacent row of the plurality of rows, the nonporous planar sheet comprising opposing planar surfaces configured to provide support to the permeate side, the plurality of fluid channels extending between the opposing surfaces, wherein the at least one hydrogen-selective membrane is metallurgically bonded to the at least one microsieve structure; and A plurality of frames are disposed between and secured to the first and second end frames and the at least one foil-microsieve assembly, each frame of the plurality of frames including a perimeter frame body defining an open area.

2. A device according to claim 1, wherein the non-porous planar sheet comprises two or more discrete portions having the plurality of orifices, and wherein each of the two or more discrete portions is separated from an adjacent discrete portion of the two or more discrete portions by at least one boundary portion that does not have the plurality of orifices.

3. The apparatus of claim 2, wherein the at least one hydrogen-selective membrane comprises two or more hydrogen-selective membranes, and wherein a different one of the two or more hydrogen-selective membranes is metallurgically bonded to each of the two or more discrete portions.

4. The apparatus of claim 3, wherein each of the two or more hydrogen-selective membranes is sized to be larger than a corresponding discrete portion such that a perimeter portion of the hydrogen-selective membrane contacts one or more portions of the non-porous planar sheet that do not include the plurality of orifices.

5. The apparatus of claim 1, wherein the at least one hydrogen selective membrane is diffusely bonded to the at least one micromesh structure.

6. A hydrogen purification device comprising: The first end frame and the second end frame include: an input port configured to receive a mixed gas flow including hydrogen and other gases; an output port configured to receive a permeate stream comprising at least one of a higher concentration of hydrogen than the mixed gas stream and a lower concentration of other gases than the mixed gas stream; and a byproduct port configured to receive a byproduct stream comprising at least a majority of the other gas; at least one foil-microsieve assembly disposed between and secured to the first end frame and the second end frame, the at least one foil-microsieve assembly comprising: at least one hydrogen selective membrane having a feed side and a permeate side, at least a portion of the permeate stream being formed by the portion of the mixed gas stream flowing from the feed side to the permeate side, wherein the remainder of the mixed gas stream remaining on the feed side forms at least a portion of the byproduct stream, and at least one microsieve structure comprising a nonporous planar sheet having a plurality of stadium-shaped apertures forming a plurality of fluid channels, each aperture of the plurality of stadium-shaped apertures having a length greater than ten times a radius of the aperture, the planar sheet comprising opposing planar surfaces configured to provide support to the permeate side, the plurality of fluid channels extending between the opposing surfaces, wherein the at least one hydrogen-selective membrane is metallurgically bonded to the at least one microsieve structure; and a plurality of frames disposed between and secured to the first and second end frames and the at least one foil-microsieve assembly, each frame of the plurality of frames including a perimeter frame body defining an open area; wherein the non-porous planar sheet comprises a length and a width, and the plurality of stadium-shaped openings are arranged along most of the length and most of the width of the non-porous planar sheet; wherein the plurality of stadium-shaped openings are positioned on the non-porous planar sheet in the form of a plurality of columns, wherein each of the plurality of columns comprises no more than three stadium-shaped openings of the plurality of stadium-shaped openings.

7. The device of claim 6, wherein one or more of the plurality of stadium-shaped apertures has a length that is a majority of the width of the non-porous planar sheet.

8. The device according to claim 6, wherein: The plurality of stadium-shaped orifices are positioned in a plurality of columns on the non-porous planar sheet such that (1) the longitudinal axes of the stadium-shaped orifices in each of the plurality of stadium-shaped orifices in the plurality of columns are parallel to each other and to the stadium-shaped orifices in an adjacent column of the plurality of columns, and (2) the length of each stadium-shaped orifice in each of the plurality of columns is different from the length of one or more stadium-shaped orifices in an adjacent column of the plurality of columns.

9. A device according to claim 6, wherein the non-porous planar sheet includes two or more discrete portions having the plurality of stadium-shaped apertures, and wherein each of the two or more discrete portions is separated from an adjacent discrete portion of the two or more discrete portions by at least one boundary portion that does not have the plurality of stadium-shaped apertures.

10. The apparatus of claim 9, wherein the at least one hydrogen-selective membrane comprises two or more hydrogen-selective membranes, and wherein a different one of the two or more hydrogen-selective membranes is metallurgically bonded to each of the two or more discrete portions.

11. The apparatus of claim 10, wherein each of the two or more hydrogen-selective membranes is sized larger than a corresponding discrete portion such that a perimeter portion of the hydrogen-selective membrane contacts one or more portions of the non-porous planar sheet that do not include the plurality of stadium-shaped orifices.

12. The apparatus of claim 6, wherein the at least one hydrogen selective membrane is diffusely bonded to the at least one micromesh structure.

13. The device of claim 6, wherein each of the plurality of stadium-shaped apertures has a length that is at least 25% of a width of the non-porous planar sheet.

14. A foil-microsieve assembly comprising: at least one hydrogen selective membrane having a feed side and a permeate side, wherein the at least one hydrogen selective membrane is configured to receive a mixed gas stream to form a permeate stream and a byproduct stream, the permeate stream being derived from a portion of the mixed gas stream flowing from the feed side to the permeate side and the byproduct stream being derived from a remaining portion of the mixed gas stream remaining on the feed side; and At least one microsieve structure comprises a nonporous planar sheet having a plurality of apertures forming a plurality of fluid channels, each aperture of the plurality of apertures having a length defining a longitudinal axis, the plurality of apertures being positioned on the nonporous planar sheet in a plurality of rows such that the longitudinal axes of the apertures in each of the plurality of apertures in the plurality of rows are (1) parallel to each other and (2) non-parallel to the longitudinal axes of the apertures in an adjacent row of the plurality of apertures in the plurality of rows and (3) oriented at an angle to the longitudinal axes of the apertures in an adjacent row of the plurality of apertures in the plurality of rows, the nonporous planar sheet comprising opposing planar surfaces configured to provide support to the permeate side, the plurality of fluid channels extending between the opposing surfaces, wherein the permeate side of the at least one hydrogen-selective membrane is metallurgically bonded to the at least one microsieve structure.

15. A component according to claim 14, wherein the non-porous planar sheet includes two or more discrete portions having the plurality of orifices, and wherein each of the two or more discrete portions is separated from an adjacent discrete portion of the two or more discrete portions by at least one boundary portion that is free of the plurality of orifices.

16. The assembly of claim 15, wherein the at least one hydrogen-selective membrane comprises two or more hydrogen-selective membranes, and wherein a different one of the two or more hydrogen-selective membranes is metallurgically bonded to each of the two or more discrete portions.

17. The assembly of claim 16, wherein each of the two or more hydrogen-selective membranes is sized larger than a corresponding discrete portion such that a perimeter portion of the hydrogen-selective membrane contacts one or more portions of the non-porous planar sheet that do not include a plurality of stadium-shaped orifices.

18. The assembly of claim 14, wherein the at least one hydrogen selective membrane is diffusion bonded to the at least one micromesh structure.

19. A foil-microsieve assembly comprising: at least one hydrogen selective membrane having a feed side and a permeate side, wherein the at least one hydrogen selective membrane is configured to receive a mixed gas stream to form a permeate stream and a byproduct stream, the permeate stream being derived from a portion of the mixed gas stream flowing from the feed side to the permeate side and the byproduct stream being derived from a remaining portion of the mixed gas stream remaining on the feed side; and at least one microsieve structure comprising a nonporous planar sheet having a plurality of stadium-shaped apertures forming a plurality of fluid channels, each aperture of the plurality of stadium-shaped apertures having a length greater than ten times a radius of the aperture, the planar sheet comprising opposing planar surfaces configured to provide support to a permeate side, the plurality of fluid channels extending between the opposing surfaces, wherein a permeate side of the at least one hydrogen-selective membrane is metallurgically bonded to the at least one microsieve structure; wherein the non-porous planar sheet comprises a length and a width, and the plurality of stadium-shaped apertures are disposed along a majority of the length and a majority of the width of the non-porous planar sheet; wherein the plurality of stadium shaped apertures are positioned on the imperforate planar sheet in a plurality of columns, wherein each of the plurality of columns comprises no more than three stadium shaped apertures of the plurality of stadium shaped apertures.

20. The assembly of claim 19, wherein the non-porous planar sheet comprises two or more discrete portions having the plurality of stadium-shaped apertures, and wherein each of the two or more discrete portions is separated from an adjacent discrete portion of the two or more discrete portions by at least one boundary portion lacking the plurality of apertures.

21. The assembly of claim 20, wherein the at least one hydrogen-selective membrane comprises two or more hydrogen-selective membranes, and wherein a different one of the two or more hydrogen-selective membranes is metallurgically bonded to each of the two or more discrete portions.

22. The assembly of claim 21, wherein each of the two or more hydrogen-selective membranes is sized larger than a corresponding discrete portion such that a perimeter portion of the hydrogen-selective membrane contacts one or more portions of the non-porous planar sheet that do not include the plurality of apertures.

23. The assembly of claim 19, wherein the at least one hydrogen selective membrane is diffusion bonded to the at least one micromesh structure.

24. The assembly of claim 19, wherein each of the plurality of stadium-shaped apertures has a length that is at least 25% of a width of the non-porous planar sheet.

25. The assembly of claim 19, wherein one or more of the plurality of stadium shaped apertures has a length that is a majority of the width of the non-porous planar sheet.

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