Hydrogen purification device

Abstract

Hydrogen purification devices and components thereof are disclosed. In some embodiments, a device includes a permeation frame that can include a perimeter portion and a membrane support portion surrounded by the perimeter portion. The membrane support portion can include opposing first and second surfaces, each of the first and second surfaces having a plurality of grooves. The membrane support portion can contact and support at least one hydrogen-selective membrane. The membrane support portion can be integrally formed with the perimeter portion. The permeation frame can also include one or more output apertures in at least one of the perimeter portion and the membrane support portion. The permeation frame can also include at least one input aperture in the perimeter portion. The at least one input aperture can be distinct and spaced apart from the one or more output apertures.

Description

Background Technology

[0001] A hydrogen generation assembly is an assembly that converts one or more feedstocks into a product stream containing hydrogen as the primary component. Feedstocks may include carbonaceous feedstocks, and in some embodiments, may also include water. The feedstock is delivered from a feedstock delivery system to the hydrogen generation zone of the hydrogen generation assembly, typically under pressure and at elevated temperatures. The hydrogen generation zone is typically associated with temperature control components, such as heating or cooling components, which consume one or more fuel streams to maintain the hydrogen generation zone within a suitable temperature range for efficient hydrogen production. The hydrogen generation assembly can generate hydrogen via any suitable mechanism(s), such as steam reforming, autothermal reforming, pyrolysis, and / or catalytic partial oxidation.

[0002] However, the generated or produced hydrogen may contain impurities. This 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 by removing at least a portion of the other gases. Therefore, the hydrogen generation assembly 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 byproduct stream. The product stream contains a higher concentration of hydrogen from the mixed gas stream and / or a reduced concentration of one or more other gases. Hydrogen purification using one or more hydrogen-selective membranes is a pressure-driven separation process in which one or more hydrogen-selective membranes are contained within a pressure vessel. The mixed gas stream contacts the mixed gas surface of the membrane(s), while the product stream is formed by at least a portion of the mixed gas stream permeating through the membrane(s). The pressure vessel is typically sealed to prevent gas from entering or leaving the pressure vessel except through defined inlet and outlet ports, or inlet and outlet conduits.

[0003] The product stream can be used in a variety of applications. One such application is energy generation, such as in electrochemical fuel cells. An electrochemical fuel cell is a device that converts fuel and 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 comprises multiple fuel cells and can be used in conjunction with a hydrogen generation component to provide an energy generation component.

[0004] Examples of hydrogen generation components, hydrogen processing components, and / or parts thereof 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 Publications Nos. 2006 / 0090397, 2006 / 0272212, 2007 / 0266631, 2007 / 0274904, 2008 / 0085434, 2008 / 0138678, 2008 / 0230039, and 2010 / 0064887. The full contents of the aforementioned patent and patent application publication texts are incorporated herein by reference for all purposes. Attached Figure Description

[0005] Figure 1 This is a schematic diagram of an example of a hydrogen generation component.

[0006] Figure 2 yes Figure 1 A schematic diagram of an example of a hydrogen generation component.

[0007] Figure 3 yes Figure 1 or Figure 2 A schematic diagram of a hydrogen purification device for a hydrogen generation component.

[0008] Figure 4 yes Figure 3 An isometric view of an example hydrogen purification apparatus.

[0009] Figure 5 yes Figure 4 An exploded isometric view of a hydrogen purification apparatus, not showing the end frame and fasteners, but showing one of the two foil-microscreen assemblies exploded.

[0010] Figure 6 yes Figure 4 A partial view of an example of the microsieve support structure of a hydrogen purification device.

[0011] Figure 7 yes Figure 4 A partial view of the hydrogen purification apparatus, showing examples of the feed frame and gasket frame.

[0012] Figure 8 yes Figure 4 A partial view of the hydrogen purification apparatus, showing examples of the permeation frame, foil-microscreen assembly, and gasket frame.

[0013] Figure 9 yes Figure 8A partial view of the permeation frame, showing an example of trenches in the membrane support portion of the permeation frame.

[0014] Figure 10 yes Figure 8 A partial view of the permeation frame shows another example of trenches in the membrane support portion of the permeation frame.

[0015] Figure 11 yes Figure 8 A partial view of the permeation frame shows yet another example of trenches in the membrane support portion of the permeation frame.

[0016] Figure 12 yes Figure 8 A partial view of the permeation frame shows yet another example of trenches in the membrane support portion of the permeation frame.

[0017] Figure 13 yes Figure 8 Top view of the permeation frame, foil-microscreen assembly, and gasket frame.

[0018] Figure 14 yes Figure 13 Partial view of the permeation frame, foil-microscreen assembly, and gasket frame.

[0019] Figure 15 yes Figure 4 A top view of another example of the permeation frame of a hydrogen purification device.

[0020] Figure 16 yes Figure 14 The penetration framework and Figure 8 Top view of the foil-microscreen assembly and gasket frame.

[0021] Figure 17 yes Figure 16 Partial view of the permeation frame, foil-microscreen assembly, and gasket frame.

[0022] Figure 18 yes Figure 4 A top view of another example of the permeation frame of a hydrogen purification device.

[0023] Figure 19 yes Figure 18 The penetration framework and Figure 8 Top view of the foil-microscreen assembly and gasket frame.

[0024] Figure 20 yes Figure 19 Partial view of the permeation frame, foil-microscreen assembly, and gasket frame.

[0025] Figure 21 It shows the manufacturing process. Figure 8 , Figure 14or Figure 18 A flowchart illustrating an example of the penetration testing framework's methods. Detailed Implementation

[0026] Figure 1 An 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 this 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.

[0027] In some embodiments, the feed delivery system 22 may additionally 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 portions of the fuel processing assembly. The feed 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 feed delivery system may be configured to deliver one or more feed streams 26 and / or one or more fuel streams 28 without requiring the use of a pump and / or other electrically driven fluid delivery mechanism. Examples of suitable feed delivery systems that may be used with the hydrogen generation assembly 20 include those described in U.S. Patent Nos. 7,470,293 and 7,601,302 and U.S. Patent Application Publication No. 2006 / 0090397. The entire disclosure of the foregoing patents and patent applications is incorporated herein by reference for all purposes.

[0028] Feed stream 26 may include at least one hydrogen-generating fluid 30, which may include one or more fluids that can be used as reactants to produce product hydrogen stream 21. For example, the hydrogen-generating fluid may include a carbonaceous 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, hydrogen-generating fluid 30 may include water, as is the case when the fuel processing assembly generates product hydrogen stream via steam reforming and / or autothermal reforming. When the fuel processing assembly 24 generates product hydrogen stream via pyrolysis or catalytic partial oxidation, feed stream 26 does not contain water.

[0029] In some embodiments, feedstock delivery system 22 may be configured to deliver a hydrogen-generating fluid 30 comprising a mixture of water and a water-miscible carbonaceous feedstock (such as methanol and / or another water-soluble alcohol). The water-to-carbonaceous feedstock ratio in this 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, and one or more mechanisms of the hydrogen generation stream used by the fuel processing assembly. For example, the water-to-carbon molar ratio may be approximately 1:1 to 3:1. Furthermore, mixtures of water and methanol may be delivered at or near a 1:1 molar ratio (37% water by weight, 63% methanol by weight), while mixtures of hydrocarbons or other alcohols may be delivered at a water-to-carbon molar ratio greater than 1:1.

[0030] When the fuel processing assembly 24 generates product hydrogen via reforming product hydrogen stream 21, the feed stream 26 may include, for example, about 25-75 vol% methanol or ethanol (or another suitable water-miscible carbonaceous feedstock) and about 25-75 vol% water. For feed streams that consist at least substantially of methanol and water, those streams may include about 50-75 vol% methanol and about 25-50 vol% water. Streams containing ethanol or other water-miscible alcohols may contain about 25-60 vol% alcohol and about 40-75 vol% water. An example of a feed stream for a hydrogen generation assembly 20 utilizing steam reforming or autothermal reforming contains 69 vol% methanol and 31 vol% water.

[0031] Although the illustrated feed delivery system 22 is configured to deliver a single feed stream 26, the feed delivery system may be configured to deliver two or more feed streams 26. These streams may contain the same or different feeds and may have different compositions, at least one common component, no common component, or the same composition. For example, a first feed stream may include a first component, such as a carbon-containing feedstock, and a second feed stream may include a second component, such as water. Furthermore, although in some embodiments the feed delivery system 22 may be configured to deliver a single fuel stream 28, the feed delivery system may also be configured to deliver two or more fuel streams. The fuel streams may have different compositions, at least one common component, no common component, or the same composition. Furthermore, the feed streams and fuel streams may exit the feed delivery system at different stages. For example, one of the streams may be a liquid stream and the other a gaseous stream. In some embodiments, both streams may be liquid streams, while in other embodiments, both streams may be gaseous streams. Additionally, although the hydrogen generation assembly 20 is shown as including a single feed delivery system 22, the hydrogen generation assembly may include two or more feed delivery systems 22.

[0032] The fuel processing assembly 24 may include a hydrogen production zone 32, which is configured to produce an output stream 34 containing hydrogen via any suitable hydrogen production mechanism(s). The output stream may include hydrogen as at least the majority component, and may include one or more additional gaseous components(s). The output stream 34 may therefore be referred to as a “mixed gas stream” containing hydrogen as the majority component, but also including other gases.

[0033] The hydrogen production zone 32 may include any suitable catalyst bed or region. When the hydrogen production mechanism is steam reforming, the hydrogen production zone may include a suitable steam reforming catalyst 36 to facilitate the production of one or more output streams 34 from one or more feed streams 26 containing 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 as a “reformation zone,” and the output stream 34 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.

[0034] When the hydrogen production mechanism is autothermal reforming, the hydrogen production zone 32 may include a suitable autothermal reforming catalyst to facilitate the generation of one or more output streams 34 from one or more feed streams 26 containing water and carbonaceous feedstock in the presence of air. Furthermore, the fuel processing assembly 24 may include an air delivery assembly 38 configured to deliver one or more air streams to the hydrogen production zone.

[0035] In some embodiments, the fuel processing assembly 24 may include a purification (or separation) zone 40, which may include any suitable structure configured to generate 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 one or more other gases (or impurities) present in the output stream at reduced concentrations. 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 zone 40 may also be referred to as a "hydrogen purification device" or a "hydrogen processing assembly".

[0036] In some embodiments, purification zone 40 may generate at least one byproduct stream 44, which may contain no hydrogen or contain 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. Additionally, purification zone 40 may discharge the byproduct stream as a continuous stream in response to the delivery of output stream 34, or it may discharge the byproduct stream intermittently, such as during batch processing or when a portion of the byproduct stream is at least temporarily retained in purification zone.

[0037] The fuel processing assembly 24 may include one or more purification zones configured to generate one or more byproduct streams, the byproduct streams containing sufficient hydrogen to be suitable as a fuel stream (or feed stream) for use as a heating element of the fuel processing assembly. In some embodiments, the byproduct streams may have sufficient fuel value or hydrogen content to enable the heating element to maintain the hydrogen generation zone at a desired operating temperature or a selected temperature range. For example, the byproduct streams may include hydrogen, such as 10-30 vol% hydrogen, 15-25 vol% hydrogen, 20-30 vol% hydrogen, at least 10 or 15 vol% hydrogen, at least 20 vol% hydrogen, etc.

[0038] Purification zone 40 may include any suitable structure configured to enrich (and / or increase) the concentration of at least one component of output stream 21. In most applications, hydrogen-rich stream 42 will have a higher hydrogen concentration than output stream (or mixed gas stream) 34. Hydrogen-rich stream may also contain one or more non-hydrogen components present in reduced concentrations in output stream 34, wherein the hydrogen concentration of hydrogen-rich stream is higher than, equal to, or lower than that of output stream. For example, in conventional fuel cell systems, carbon monoxide, even present in parts per million, can damage the fuel cell stack, while other non-hydrogen components that may be present in output stream 34, such as water, will not damage the stack, even in much higher concentrations. Therefore, in such applications, purification zone may not increase the overall hydrogen concentration but will reduce the concentration of one or more non-hydrogen components that are detrimental or potentially harmful to the desired application of the product hydrogen stream.

[0039] Examples of suitable devices for purification zone 40 include one or more hydrogen-selective membranes 46, chemical carbon monoxide removal components 48, and / or pressure swing adsorption (PSA) systems 50. Purification zone 40 may include more than one type of purification device, and these devices may have the same or different structures and / or operate through the same or different mechanisms(s). Downstream of purification zone(s), fuel processing component 24 may include at least one throttling orifice and / or other flow restrictor, such as one or more product hydrogen streams, one or more hydrogen-rich streams, and / or one or more byproduct streams.

[0040] The hydrogen-selective membrane 46 is permeable to hydrogen, but at least substantially (if not completely) impermeable to other components of the output stream 34. Membrane 46 can be formed from any hydrogen-permeable material suitable for use under the operating conditions and parameters to which the purification zone 40 is operated. Examples of suitable materials for membrane 46 include palladium and palladium alloys, particularly thin films of such metals and metal alloys. Palladium alloys have proven particularly effective, especially alloys of palladium with 35% to 45% copper. Although other relative concentrations and compositions can be used, palladium-copper alloys containing approximately 40% copper have proven particularly effective. Three other particularly effective alloys are: palladium alloys with 2% to 20% gold, especially palladium alloys with 5% gold; palladium alloys with 3% to 10% indium and 0% to 10% ruthenium, especially palladium alloys with 6% indium and 0.5% ruthenium; and palladium alloys with 20% to 30% silver. When using palladium and palladium alloys, 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, and most preferably between 5 and 12 micrometers. The foil can be any suitable size, such as 110 mm × 270 mm.

[0041] The chemical carbon monoxide removal assembly 48 is a device that chemically reacts carbon monoxide and / or other undesirable components in the output stream 34 to form other components that are not potentially hazardous. 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) into carbon dioxide; and a methanation reactor configured to convert carbon monoxide and hydrogen into methane and water. The fuel treatment assembly 24 may include more than one type and / or number of chemical carbon monoxide removal assemblies 48.

[0042] Pressure swing adsorption (PSA) is a chemical process that removes gaseous impurities from the output stream 34 based on the principle that certain gases, under appropriate temperature and pressure conditions, adsorb more strongly onto the adsorbent material than others. Typically, non-hydrogen impurities are adsorbed and removed from the output stream 34. Adsorption of the impurity gas occurs under increased pressure. When the pressure decreases, the impurities desorb from the adsorbent material, thereby regenerating the adsorbent material. PSA is typically a cyclic process requiring at least two beds for continuous (as opposed to batch) operation. Examples of suitable adsorbent materials for adsorption beds are activated carbon and zeolite. 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 as a gas stream from the purification output stream. Instead, these byproduct components are removed during adsorbent material regeneration or otherwise removed from the purification zone.

[0043] exist Figure 1 In the diagram, purification zone 40 is shown within fuel processing assembly 24. Alternatively, the purification zone may be located separately downstream of the fuel processing assembly, such as... Figure 1 The dotted lines in the diagram illustrate this. The purification zone 40 may also include portions within and outside the fuel processing assembly.

[0044] The fuel treatment assembly 24 may also include a temperature regulating assembly in the form of a heating assembly 52. ​​The heating assembly may be configured to generate at least one heated exhaust stream (or combustion stream) 54 from at least one heated fuel stream 28, typically for combustion in the presence of air. The heated exhaust stream 54... Figure 1 The heating assembly 52 is schematically illustrated as heating the hydrogen production zone 32. The heating assembly 52 may include any suitable structure configured to generate a heated exhaust stream, such as a burner or combustion catalyst that burns fuel with air to produce a heated exhaust stream. The heating assembly may include an igniter or ignition source 58 configured to initiate fuel combustion. Examples of suitable ignition sources include one or more spark plugs, glow plugs, combustion catalysts, ignition lamps, piezoelectric igniters, spark igniters, hot surface igniters, etc.

[0045] 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, in the presence of air, combust the fuel stream to provide a hot combustion stream 54. The hot combustion stream 54 may be used to at least heat the hydrogen production zone of the fuel processing assembly. Air may be delivered to the heating assembly via various mechanisms. For example, an air stream 62 may be delivered to the heating assembly as a separate stream, such as... Figure 1As shown. Alternatively or additionally, the airflow 62 may be delivered to the heating assembly along with at least one of the fuel flows 28 for the heating assembly 52, and / or drawn from the environment in which the heating assembly is used.

[0046] The combustion stream 54 may additionally or alternatively be used to heat the fuel processing assembly and / or other parts of the fuel cell system used in conjunction with the heating assembly. Alternatively, 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 using at least one heating element, such as a resistance heating element, to at least heat the hydrogen production zone 32 of the fuel processing assembly 24. In those embodiments, the heating assembly 52 may not receive and burn the combustible fuel stream to heat the hydrogen production zone to a suitable hydrogen production temperature. Examples of heating assemblies are disclosed in U.S. Patent No. 7,632,322, the entire disclosure of which is incorporated herein by reference for all purposes.

[0047] The heating assembly 52 may be housed together with the hydrogen generation zone and / or separation zone within a common housing or enclosure (as discussed further below). The heating assembly may be positioned separately relative to the hydrogen generation zone 32, but in thermal and / or fluid communication with that zone to provide at least the desired heating of that hydrogen generation zone. The heating assembly 52 may be partially or entirely 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.

[0048] The heating assembly can also be configured to heat: feed delivery system 22, feed supply stream, hydrogen generation zone 32, purification (or separation) zone 40, or any suitable combination of these systems, streams, and zones. Heating the feed supply stream may include vaporizing components of a liquid reactant stream or a hydrogen-generating fluid used to generate hydrogen in the hydrogen generation zone. In this embodiment, fuel handling assembly 24 may be described as including vaporization zone 64. The heating assembly can be additionally configured to heat other components of the hydrogen generation assembly. For example, a heated discharge stream may be configured to heat a pressure vessel and / or other tank containing heated fuel and / or hydrogen-generating fluid forming at least a portion of the feed stream 26 and fuel stream 28.

[0049] Heating assembly 52 can reach and / or maintain any suitable temperature in hydrogen production zone 32. Steam reformers typically operate in a temperature range of 200°C to 900°C. However, temperatures outside this range are also within the scope of this disclosure. When the carbonaceous feedstock is methanol, steam reforming reactions are typically carried out in a temperature range of approximately 200-500°C. Example subsets of this range include 350-450°C, 375-425°C, and 375-400°C. When the carbonaceous feedstock is hydrocarbons, ethanol, or another alcohol, a temperature range of approximately 400-900°C is typically used for steam reforming reactions. Example subsets of this range include 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 production zone 32 may include two or more regions or sections, each of which may operate at the same or different temperatures. For example, when the hydrogen-producing fluid includes hydrocarbons, the hydrogen production zone 32 may include two distinct hydrogen-producing sections or regions, one of which operates at a lower temperature than the other to provide a pre-reforming zone. In those embodiments, the fuel processing assembly may also be referred to as including two or more hydrogen production zones.

[0050] Fuel stream 28 may include any one or more combustible liquids and / or one or more gases suitable for consumption by the heating assembly 52 to provide the desired heat output. Some fuel streams may be gases when delivered and combusted by the heating assembly 52, while others may be delivered to the heating assembly as liquid streams. Examples of heating fuels for fuel stream 28 include carbonaceous feedstocks 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 light hydrocarbons. Other examples also include hydrogen and carbon monoxide. In embodiments of hydrogen generation assembly 20 that include a temperature-regulating assembly in the form of a cooling assembly rather than a heating assembly (such as when using an exothermic hydrogen production process, for example, partial oxidation, instead of an endothermic process, such as steam reforming), the feedstock delivery system may be configured to supply a fuel or coolant stream to the assembly. Any suitable fuel or coolant may be used.

[0051] Fuel processing assembly 24 may additionally include a housing or enclosure 66, which contains at least a hydrogen production zone 32, such as Figure 1As shown. In some embodiments, the vaporization zone 64 and / or purification zone 40 may be additionally included within the housing. The housing 66 allows components of the steam reformer or other fuel treatment assembly to be moved as a unit. The housing may also protect components of the fuel treatment assembly from damage by providing a protective enclosure and / or reduce the heating requirements of the fuel treatment assembly because the components can be heated as a unit. The housing 66 may include an insulating material 68, such as a solid insulating material, a blanket insulating material, and / or an air-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 treatment assembly 24 may also include an outer cover or sheath 70 outside the insulating material, such as... Figure 1 As illustrated schematically. The fuel processing assembly may include different housings that contain additional components of the fuel processing assembly, such as the feed delivery system 22 and / or other components.

[0052] One or more components of the fuel processing assembly 24 may extend beyond the housing or be located outside the housing. For example, the purification zone 40 may be located outside the housing 66, such as being spaced apart from the housing but fluidly connected via suitable fluid transfer conduits. As another example, a portion of the hydrogen production zone 32 (such as portions of one or more reforming catalyst beds) may extend beyond the housing, such as... Figure 1 The dashed lines in the diagram indicate alternative housing configurations. Examples of suitable hydrogen generation components and their parts are disclosed in U.S. Patent Nos. 5,861,137, 5,997,594, and 6,221,117, the full disclosure of which is incorporated herein by reference for all purposes.

[0053] Another example of hydrogen generation component 20, generally indicated by 72, is as follows: Figure 2 As shown. Unless otherwise specified, hydrogen generation assembly 72 may include one or more components of hydrogen generation assembly 20. Hydrogen generation assembly 72 may include feed delivery system 74, vaporization zone 76, hydrogen production zone 78, and heating assembly 80, as shown. Figure 2 As shown. In some embodiments, the hydrogen generation component 20 may further include a purification zone 82.

[0054] The feed delivery system may include any suitable structure 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 feed delivery system may include a feed tank (or container) 84 and a pump 86. The feed tank may contain any suitable hydrogen-generating fluid 88, such as water and carbonaceous feedstock (such as a methanol / water mixture). The pump 86 may have any suitable structure configured to deliver a hydrogen-generating fluid to a vaporization zone 76 and / or a hydrogen generation zone 78, which may be in the form of at least one liquid-containing feed stream 90 containing water and carbonaceous feedstock.

[0055] The vaporization zone 76 may include any suitable structure configured to receive and vaporize at least a portion of a liquid-containing feed stream, such as a liquid-containing feed stream 90. For example, the vaporization zone 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. Examples of suitable vaporizers are coiled tube vaporizers, such as coiled stainless steel tubes.

[0056] The hydrogen generation zone 78 may include any suitable structure configured to receive one or more feed streams, such as steam feed streams 94 from one or more vaporization zones, to produce one or more output streams 96 comprising hydrogen and other gases as primary components. The hydrogen generation zone may generate the output streams via any suitable mechanism. For example, the hydrogen generation zone 78 may generate one or more output streams 96 via a steam reforming reaction. In this example, the hydrogen generation zone 78 may include a steam reforming zone 97 having a reforming catalyst 98 configured to facilitate and / or promote the steam reforming reaction. When the hydrogen generation zone 78 generates one or more output streams 96 via 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."

[0057] 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 zone 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 vaporizes to form a vapor feed stream. Additionally or alternatively, the heating assembly 80 may heat the hydrogen generation zone 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 produce hydrogen, thereby forming 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 zone and / or the hydrogen generation zone.

[0058] like Figure 2As shown, the heating assembly may include a burner assembly 100, at least one blower 102, and an igniter assembly 107. 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 within a combustion zone 110 to produce a heated exhaust stream 99. The fuel stream may be provided by a feed delivery system 74 and / or a purification zone 82. The combustion zone may be contained within an enclosure of a hydrogen generation assembly. The blower 102 may include any suitable structure configured to generate one or more air streams 106. The igniter assembly 107 may include any suitable structure configured to ignite one or more fuel streams 108, such as a spark plug, catalytic igniter, hot surface igniter, and ignition flame.

[0059] Purification zone 82 may include any suitable structure configured to generate at least one hydrogen-rich stream 112, which may include a hydrogen concentration higher than that of output stream 96 and / or may include a concentration of one or more other gases (or impurities) lower than that present in the output stream. The purification zone may generate at least one byproduct stream or fuel stream 108, which may be fed to combustor assembly 100 and used as a fuel stream for that assembly, such as... Figure 2 As shown. Purification zone 82 may include flow restrictor 111, filter assembly 114, membrane assembly 116, and methanation reactor assembly 118. The filter assembly (such as one or more hot gas filters) may be configured to remove impurities from the output stream 96 prior to the hydrogen purification membrane assembly.

[0060] Membrane module 116 may include any suitable structure configured to receive one or more output streams or mixed gas streams 96 comprising hydrogen and other gases, and configured to generate one or more permeate streams or hydrogen-rich streams 112 comprising hydrogen at a higher concentration than the mixed gas stream and / or other gases at a lower concentration than the mixed gas stream. Membrane module 116 may incorporate planar or tubular hydrogen-permeable (or hydrogen-selective) membranes, and more than one hydrogen-permeable membrane may be incorporated into membrane module 116. The one or more permeate streams may be used for any suitable application, such as for one or more fuel cells. In some embodiments, the membrane module may generate a byproduct or fuel stream 108 comprising at least a substantial portion of other gases. Methanation reactor assembly 118 may include any suitable structure configured to convert carbon monoxide and hydrogen into methane and water. Although purification zone 82 is shown as including flow restrictor 111, filter assembly 114, membrane assembly 116, and methanation reactor assembly 118, the purification zone may have fewer components than all of these, and / or may alternatively or additionally include one or more other components configured to purify output stream 96. For example, purification zone 82 may include only membrane assembly 116.

[0061] In some embodiments, the hydrogen generation assembly 72 may include a housing or casing 120, which may at least partially contain one or more other components of the hydrogen generation assembly 72. For example, the housing 120 may at least partially contain a vaporization zone 76, a hydrogen generation zone 78, a heating assembly 80, and / or a purification zone 82, such as... Figure 2 As shown. The housing 120 may include one or more discharge ports 122 configured to discharge at least one combustion exhaust stream 124 generated by the heating assembly 80.

[0062] 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 assembly 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 zone and / or purification zone via 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 control system may adjust the delivery of the feed flow 90 to the vaporization zone 76 and / or hydrogen generation zone 78 via one or more valves 130 and one or more pumps 86, or adjust the airflow 106 from the blower 102. One or more valves 130 may include solenoid valves and / or any suitable valves. One or more pressure reducing valves 132 may be configured to ensure that overpressure in the system is released.

[0063] 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 part of the hydrogen generation assembly to another. For example, the heat exchange assembly 136 may transfer heat from the hydrogen-rich stream 112 to the feed stream 90 to raise the temperature of the feed stream before it enters the vaporization zone 76, and to cool the hydrogen-rich stream 112.

[0064] Figure 1 An example of the purification zone 40 (or hydrogen purification device) of the hydrogen generation component 20 is shown in Figure 3The designation is generally 144. Unless specifically excluded, the hydrogen purification apparatus may include one or more components of other purification zones described in this disclosure. The hydrogen purification apparatus 40 may include a hydrogen separation zone 146 and a housing 148. The housing may define an internal volume 150 having an inner perimeter 152. The housing 148 may include at least a first portion 154 and a second portion 156, which are coupled together to form a body 149 in the form of a sealed pressure vessel, which may include defined inlet and outlet ports. These ports may define fluid paths through which gases and other fluids are delivered into and removed from the internal volume of the housing.

[0065] 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 leak-proof interface between the first and second parts may include gaskets and / or welds. Additionally or alternatively, the first part 154 and the second part 156 may be secured together such that at least a predetermined amount of compression is applied to the various components defining the hydrogen separation zone within the housing and / or other components that may be incorporated into the hydrogen generation assembly. The applied compression can ensure that the various components remain in proper position within the housing. Furthermore, or alternatively, the compression applied to the various components defining the hydrogen separation zone and / or other components can provide a leak-proof interface between the various components defining the hydrogen separation zone, between the various other components, and / or between the various components defining the hydrogen separation zone and other components.

[0066] like Figure 3 As shown, the package 148 may include a mixing gas region 160 and a permeation region 162. The mixing gas region and the permeation region may be separated by a hydrogen separation region 146. At least one inlet port 164 may be provided through which a fluid flow 166 is delivered to the package. The fluid flow 166 may be a mixing gas flow 168 containing hydrogen 170 and other gases 172 delivered to the mixing gas region 160. Hydrogen may be the dominant component of the mixing gas flow. The hydrogen separation region 146 may extend between the mixing gas region 160 and the permeation region 162 such that gases in the mixing gas region must pass through the hydrogen separation region to enter the permeation region. The gases may, for example, need to pass through at least one hydrogen-selective membrane, as discussed further below. The permeation gas region and the mixing gas region may have any suitable relative size within the package.

[0067] The encapsulation housing 148 may further include at least one product outlet port 174 through which a permeate stream 176 can be received from and removed from the permeation zone 162. The permeate stream may contain at least one of a hydrogen concentration higher than that of the mixed gas stream and a concentration of other gases lower than that of the mixed gas stream. In some embodiments, the permeate stream 176 may initially include at least a carrier gas component or a purge gas component, such as being delivered as a purge stream 178 via a purge gas port 180 in fluid communication with the permeation zone. The encapsulation housing may also include at least one byproduct outlet port 182 through which a byproduct stream 184 containing at least one 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.

[0068] The hydrogen separation zone 146 may include at least one hydrogen-selective membrane 186 having a first surface or mixed gas surface 188 and a second surface or permeation surface 190, the first surface or mixed gas surface 188 being oriented to contact a mixed gas stream 168, and the second surface or permeation surface 190 generally opposite surface 188. The mixed gas stream 168 may be delivered to the mixed gas zone of the package housing to contact the mixed gas surfaces of one or more hydrogen-selective membranes. A permeation stream 176 may be formed by at least a portion of the mixed gas stream reaching the permeation zone 162 through the hydrogen separation zone. A 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 contain a portion of hydrogen present in the mixed gas stream. The hydrogen separation zone may also be configured to trap 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.

[0069] exist Figure 3 In this configuration, streams 166, 176, 178, and / or 184 may include more than one actual stream flowing into or out of the hydrogen purification unit 144. For example, the hydrogen purification unit may receive multiple mixed gas streams 168, a single mixed gas stream 168 split into two or more streams before contacting the hydrogen separation zone 146, a single stream delivered into the internal volume 150, and so on. Therefore, the enclosure 148 may include more than one input port 164, a product output port 174, a purge gas port 180, and / or a byproduct output port 182.

[0070] Hydrogen-selective membranes can be formed from any hydrogen-permeable material suitable for use in the operating environment and parameters of a hydrogen purification apparatus. Examples of hydrogen purification apparatuses are disclosed in U.S. Patent Nos. 5,997,594 and 6,537,352, the entire disclosures of which are incorporated herein by reference for all purposes. In some embodiments, the hydrogen-selective membrane may be formed from at least one of palladium and palladium alloys. Examples of palladium alloys include alloys of palladium with copper, silver, and / or gold. Examples of various membranes, membrane structures, and methods for preparing membranes and membrane structures are disclosed in U.S. Patent 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.

[0071] 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 typically extend from a first portion 154 to a second portion 156. Thus, the first and second portions can effectively compress the hydrogen separation assembly. In some embodiments, the encapsulation housing 148 may additionally or optionally include end plates (or end frames) coupled to opposite sides of the body portion. In such embodiments, the end plates can effectively compress the hydrogen separation assembly (and other components that may be housed within the encapsulation housing) between the pair of opposite end plates.

[0072] Hydrogen purification using one or more hydrogen-selective membranes is typically a pressure-driven separation process in which a mixed gas stream is delivered to contact the mixed gas surface of the membrane at a pressure higher than that of 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, at least 325°C, at least 350°C, in the range of 275–500°C, in the range of 275–375°C, in the range of 300–450°C, and in the range of 350–450°C.

[0073] An example of hydrogen purification device 144 is shown in Figures 4-5The hydrogen purification apparatus 196 is generally indicated by 196. Unless specifically excluded, the hydrogen purification apparatus 196 may include one or more components of other hydrogen purification apparatuses and / or purification zones described in this disclosure. The hydrogen purification apparatus 196 may include a housing or encapsulation shell 198, which may include a first end plate or first end frame 200 and a second end plate or second end frame 202. The first and second end plates may be configured to be fixed and / or compressed together to define a sealed pressure vessel having an internal compartment 207 in which the hydrogen separation zone is supported. The first and / or second end plates may include various input ports, output ports, purge gas ports, control ports, and byproduct ports 211 similar to those of the hydrogen purification apparatus 144.

[0074] In some embodiments, the enclosure 198 may additionally include a first side plate 203 and a second side plate 205. In those embodiments, the first side plate 203 and the second side plate 205 may be attached to the first end frame 200 and the second end frame 202 and / or attached to each other. In some examples, the first side plate and the second side plate may be seal-welded to each other and / or seal-welded to the first frame and the second frame. Each side plate may include an elongated base member 209 (one or both having a leak or mixed gas port 213) and a side member 215 attached to or formed at the opposing longitudinal ends of the elongated base member. The leak port may be configured to receive gas leaking from one or more various regions, zones, and / or conduits of the hydrogen purification device, such as at interfaces between and / or between adjacent frames(s). In other words, gas leaking from the frames of the hydrogen purification device may accumulate in the internal space 217 between the first and second side plates and the frames and can be removed from this internal space through the leak port 213. Figure 4-5 In the example shown, the side members are vertically attached to or formed on the elongated base member. However, other examples of the hydrogen purification device 196 may include side plates 203, 205. Side plates 203, 205 have side members attached to or formed on the elongated base member in a non-vertical orientation, such as conforming to the shape of a frame.

[0075] like Figure 5As shown, the hydrogen purification apparatus 196 may further include at least one foil-microsieve assembly 208, which may be disposed between 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 210 and at least one microsieve structure 212. 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 the permeate stream and at least a portion of the byproduct stream. The hydrogen-selective membrane 210 may include a feed side 214 and a permeate side 216. At least a portion of the permeate stream is formed by the portion of the mixed gas stream conveyed from the feed side to the permeate side, wherein the remaining portion of the mixed gas stream retained on the feed side forms at least a portion of the byproduct stream.

[0076] One or more hydrogen-selective membranes may be metallurgically bonded to the microsieve structure 212. For example, the permeate side of one or more hydrogen-selective membranes may be metallurgically bonded to the microsieve structure. In some embodiments, one or more hydrogen-selective membranes 210 (and / or the permeate sides of those membranes) may be diffusely bonded to the microsieve structure to form a solid-state diffusion bond between the membranes and the microsieve structure. For example, the permeate sides of the membranes 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 membranes and the microsieve structure to self-diffuse over time.

[0077] The microsieve structure 212 may include any suitable structure configured to support one or more hydrogen-selective membranes. For example, the microsieve structure may include: a non-porous planar sheet 218 having generally opposing surfaces 220 and 222 configured to provide support for the permeate side 216; and a plurality of orifices 224 forming a plurality of fluid channels extending between the opposing surfaces, the plurality of fluid channels allowing permeate flow through the microsieve structure, such as… Figure 6 As shown. Orifices can be formed on a non-porous planar sheet by electrochemical etching, chemical etching, laser drilling, and other mechanical forming processes such as stamping or die cutting. In other words, the planar sheet may be made of one or more materials that are not porous and / or do not contain any openings or orifices, and the only orifices or openings on the sheet are added by one or more of the methods described above. In some embodiments, one or more orifices (or all orifices) may be formed on the non-porous planar sheet such that their longitudinal axis or the longitudinal axis of the fluid channel is perpendicular to the plane of the non-porous planar sheet. The non-porous planar sheet may have any suitable thickness, such as between 50 micrometers and about 200 micrometers.

[0078] In some embodiments, the microsieve structure 212 may include: one or more perforated regions (or portions) 226, the perforated regions including a plurality of orifices; and one or more non-perforated regions (or portions) 228, the non-perforated regions 228 not including (or excluding) the plurality of orifices, such as... Figure 6 As shown. Orifices 224 are distributed over the entire length and width of the perforated portion(s). The perforated regions(s) may be discrete or spaced apart from one or more other perforated regions. Orifices 224 may include any suitable pattern(s), shape(s), and / or size(s). In some embodiments, orifices may be formed in one or more patterns that maximize the combined orifice area while maintaining sufficient rigidity of the microsieve structure to prevent excessive deflection under pressure loads. Orifices 224 may be circular (round), elongated circular (such as...) Figure 6 (As shown), runway-shaped or stadium-shaped, oval, elliptical, hexagonal, triangular, square, rectangular, octagonal, and / or other suitable shapes (one or more). In some embodiments, the openings 224 in the perforated areas (one or more) may be a single, uniform shape, such as Figure 6 As shown. In other embodiments, the openings 224 in the perforated regions (one or more) can be any suitable combination of two or more different shapes, such as two or more of the shapes described above.

[0079] The apertures 224 may have any suitable orientation(s) and / or be in any suitable pattern(s). For example, the apertures 224 may be oriented longitudinally (or along the length of the perforated area(s) or the length of the flat sheet) and arranged continuously in parallel rows. Alternatively, the apertures 224 may be oriented laterally (or along the width of the perforated area(s) or the width of the flat sheet). Furthermore, other embodiments of the flat sheet 218 may include apertures 224 having two or more orientations and / or directions. For example, the apertures 224 may be arranged in an alternating pattern such that the apertures in each row or column are oriented differently from the apertures in each adjacent row or column (e.g., 30, 45, 60, 90, 120 degrees). In one example, the apertures 224 are also oriented diagonally and arranged continuously in parallel rows such that the apertures in each row are oriented at approximately ninety degrees to the apertures in the adjacent rows. Alternatively or additionally, one or more orifices 224 in one or more rows and / or columns may be oriented differently from one or more other orifices in the same row and / or column.

[0080] The orifice can be any suitable size(s). For example, when the orifice is circular, the diameter can range from approximately 0.003 inches to approximately 0.020 inches. Furthermore, when the orifice is oval or elliptical, the radius of the rounded corners of the oval or elliptical shape can range from approximately 0.001 inches to approximately 0.010 inches, and the length of the oval or elliptical shape can be up to ten times the radius. Additionally, 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.

[0081] In some examples, the size of one or more openings 224 is set to span the entire or substantially the entire width or length of the perforated area. Stadium-shaped openings may be laterally oriented and / or may be the entire or substantially the entire width of (one or more) perforated areas or (one or more) perforated portions, such that the aspect ratio (length / width) is much greater than 10. Examples of such opening dimensions are 0.005 inches to 0.02 inches wide and up to 8 inches long. Openings may be spaced approximately 0.006 inches apart (i.e., the width of the non-perforated portion or solid area between adjacent openings) to provide a maximum of approximately 62.5% of the total opening area.

[0082] In some examples, the aperture 224 can have a variety of combinations of sizes. For example, the size of the aperture 224 can be such that the planar sheet 218 includes multiple rows and / or columns of apertures having (1) a smaller number of apertures with one or more longer lengths and (2) a larger number of apertures with one or more shorter lengths. In some examples, rows and / or columns with a smaller number of apertures with longer lengths alternate with rows and / or columns with a larger number of apertures with shorter lengths, such as in an interlaced pattern. For example, the aperture 224 can be oriented such that each row and / or column alternates between two apertures with longer lengths and three apertures with shorter lengths. The lengths of the apertures in each row and / or column can be the same or different. Examples of such aperture dimensions are widths of 0.005 inches to 0.02 inches and lengths of 0.05 inches to 8 inches. The apertures can be spaced about 0.006 inches apart (i.e., the width of the non-perforated portion or solid area between adjacent apertures). Other combinations of the style, size, orientation and / or shape of the aperture 224 are possible and are included in this disclosure.

[0083] The non-porous flat sheet can comprise any suitable material. For example, the non-porous flat sheet can comprise stainless steel. Stainless steel can comprise 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 can comprise about 0.6 wt% to about 3.0 wt% aluminum. In some embodiments, the non-porous flat sheet can comprise carbon steel, copper or copper alloy, aluminum or aluminum alloy, nickel, nickel-copper alloy (e.g., Monel® 400, Monel® K-500, Monel® R-405, etc.), and / or a base metal plated with silver, nickel, and / or copper. The base metal can comprise carbon steel or one or more of the above-described stainless steels.

[0084] The hydrogen-selective membrane 210 is configured to be larger than the perforated regions or segments of the microsieve structure, such that when the hydrogen-selective membrane is metallurgically bonded to the microsieve structure, the peripheral portion of the hydrogen-selective membrane contacts one or more non-perforated regions 228 of the microsieve structure. In some embodiments, a single hydrogen-selective membrane may be metallurgically bonded to a single microsieve structure, such as... Figure 5 As shown. In other embodiments, two or more hydrogen-selective membranes 210 may be metallurgically bonded to a single microsieve structure 212. For example, two, three, four, five, six, seven, eight, nine, ten or more hydrogen-selective membranes 210 may be metallurgically bonded to a single microsieve structure 212. When two or more hydrogen-selective membranes 210 are metallurgically bonded to a microsieve structure, the microsieve structure may include two or more discrete perforated regions separated by one or more non-perforated regions 228.

[0085] like Figure 5 As shown, the microsieve structure 212 can be sized to be contained (e.g., completely contained) within an open region of the permeation frame and / or supported by a membrane support structure within that open region. In other words, the microsieve structure can be sized such that, when the microsieve structure and the permeation frame are fixed or compressed to the first end frame and the second end frame, the microsieve structure does not contact the perimeter frame of the permeation frame. Alternatively, the microsieve structure can be supported by and / or fixed to a non-porous perimeter wall or frame (not shown), such as fixed to the perimeter frame of the permeation frame. When the microsieve structure is fixed to a non-porous perimeter wall, the microsieve structure may be referred to as a "porous central region portion". Examples of other microsieve structures are disclosed in U.S. Patent Application Publication No. 2010 / 0064887, the entire disclosure of which is incorporated herein by reference for all purposes.

[0086] In some embodiments, the microsieve structure may be coated with a thin metal layer or intermediate bonding layer that facilitates diffusion bonding. For example, a thin coating of nickel, copper, silver, gold, palladium, or other metals that is subjected to solid-state diffusion bonding but does not (1) melt and enter the liquid phase at less than or equal to 700°C, and (2) form a low-melting-point alloy at less than or equal to 700°C after diffusion into 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.) by coating the thin intermediate bonding layer onto the surface of the microsieve structure, the surface of which will be in contact with the hydrogen-selective membrane. In some embodiments, the foil-microsieve assembly 208 comprises only one or more hydrogen-selective membranes and one or more microsieve structures (with or without the above-described coating) and no other frames, gaskets, components, and / or structures attached, bonded, and / or metallurgically bonded to one or both of the one or more hydrogen-selective membranes and / or one or more microsieve structures. In other embodiments, one or more hydrogen-selective membranes may be anchored to at least one membrane frame (not shown), which in turn may be anchored to a first end frame and a second end frame. Although it is stated that the hydrogen-selective membrane 210 and the microsieve structure 212 are metallurgically bonded to each other, other examples of the foil-microsieve assembly 208 may include the hydrogen-selective membrane 210 and the microsieve structure 212 that are not metallurgically bonded to each other. Further examples of the foil-microsieve assembly 208 are shown in U.S. Patent Application Publication No. 2021 / 0402349, the entire disclosure of which is incorporated herein by reference for all purposes.

[0087] The hydrogen purification device 196 may further include a plurality of plates or frames 230 disposed between and fixed to the first end frame and / or the second end frame. Each frame 230 defines a longitudinal axis 231 and a lateral axis 233 perpendicular to the longitudinal axis. These frames may include any suitable structure and / or may be any suitable shape(s), such as square, rectangular, or circular. For example, the frame 230 may include a perimeter base or perimeter frame 232, such as... Figure 5 As shown. The perimeter frame can be planar and / or may define an open area or zone 234. Furthermore, the perimeter frame 232 may include opposing first sides 238 and second sides 240, as well as opposing third sides 242 and fourth sides 244, as shown. Figure 5As shown. Furthermore, the perimeter frame 226 may include at least one inlet port 246 and / or at least one outlet port 248. The inlet ports of the frame 230 may collectively form at least one inlet conduit 250 configured to receive at least a portion of the mixed gas flow. Similarly, the outlet ports of the frame 230 may collectively form at least one outlet conduit 252 configured to receive at least a portion of the permeate flow. Although the outlet port 248 is shown extending longitudinally along the perimeter frame and the inlet port 246 is shown extending laterally along the perimeter frame, the outlet port may alternatively extend laterally and the inlet port may alternatively extend longitudinally along the perimeter frame.

[0088] Frame 230 may include at least one feed frame 260, multiple gasket or gasket frames 262, and at least one permeation frame 264, such as Figures 5-20 As shown. The feed frame 260 may be disposed between one of the first end frame and the second end frame and at least one foil-micro sieve assembly 208, or disposed between two foil-micro sieve assemblies 208. The feed frame may include a feed frame perimeter frame 266, a feed frame open area 268 surrounded by the feed frame perimeter frame, at least one feed frame output orifice 270 in the feed frame perimeter frame, a first feed frame support member 272, and a second feed frame support member 274, as shown. Figure 7 As shown. Although the feed frame 260 is shown to include a first feed frame support member and a second feed frame support member, other examples of the feed frame 260 may exclude both support members or include only one of the support members, or include more than two support members.

[0089] The feed frame perimeter 266 defines a longitudinal axis 277 and a lateral axis 279 perpendicular to the longitudinal axis. An open area 268 may be fluidly connected to and / or in fluid communication with the input conduit 250. The open area may be different from and / or spaced apart from the feed frame output orifice 270. The open area may be configured to receive at least a portion of the mixed gas flow. The feed frame output orifice 270 may form part of the output conduit 252 with corresponding output orifices of other frames of the frame 230. The feed frame output orifice may be spaced apart from and different from the open area 268.

[0090] The first feed frame support member 272 and the second feed frame support member 274 may include any suitable structure configured to induce mixing (turbulence) in the mixed gas flow and / or support the feed frame perimeter frame 266 to prevent outward deviation from the feed frame open area 268. The first and second feed frame support members may be spaced apart from each other and different, and / or may be coplanar. Although the first and second feed frame support members are shown as completely spanning the open area connecting the longitudinal sides of the feed frame, other examples of the feed frame 260 may include a first and / or second feed frame support member that does not completely span the open area and / or extends from the same side or from different sides. The first and second feed frame support members may be the full thickness of the perimeter frame or may be less than the full thickness of the frame.

[0091] exist Figure 7 In the example shown, the feed frame 260 also includes a first feed frame membrane support assembly 278 and a second feed frame membrane support assembly 280, which are received in recesses 281 of the feed frame perimeter frame 266. These recesses are in fluid communication with the open area 268. In other embodiments, the feed frame may exclude the aforementioned recesses, and the feed frame membrane support assemblies may be attached to the feed frame. Furthermore, the first feed frame membrane support assembly 278 and the second feed frame membrane support assembly 280 provide a flow path for the mixed gas flow. A first feed frame support member 272 and a second feed frame support member 274 may be disposed between the first membrane support assembly 278 and the second membrane support assembly 280. However, other examples of the feed frame 260 may include other configurations, such as distributing the first and second membrane support assemblies between the first and second feed frame support members. Furthermore, other examples of the feed frame 260 may include more or fewer membrane support assemblies. In one example, the feed frame may include three, four, or more membrane support assemblies, with or without feed frame support members. In another example, the feed frame may exclude the membrane support assembly and include only one or more feed frame support members.

[0092] Each of the first feed frame membrane support assembly and the second feed frame membrane support assembly may include a first feed frame membrane support plate 282 and a second feed frame membrane support plate 284, such as Figure 7As shown. The first feed frame membrane support plate may include opposing first surfaces 286 and second surfaces 290. Similarly, the second feed frame membrane support plate 284 may include opposing first surfaces 292 and second surfaces 294. The first surfaces of the first and / or second feed frame membrane support plates may include microgrooves 296. Furthermore, the first surfaces of the first and second feed frame membrane support plates may face each other. In other words, the first and second membrane support plates may be stacked in the feed frame membrane support assembly such that the first surface of the first feed frame membrane support plate faces and / or contacts the first surface of the second feed frame membrane support plate, and / or vice versa.

[0093] Microgrooves 296 provide and / or facilitate the flow path of the mixed gas stream received in the open area of ​​the feed frame. Figure 7 In the example shown, the microgroove 296 is diagonal or inclined relative to the sides of the first and second feed frame membrane support plates. The first and second feed frame membrane support plates can be positioned such that the microgroove of the first feed frame membrane support plate is substantially parallel or parallel to the microgroove of the second feed frame membrane support plate, as shown. Figure 7 As shown. Alternatively, the first feed frame membrane support plate and the second feed frame membrane support plate may be positioned such that the microgroove of the first feed frame membrane support plate is substantially perpendicular to, substantially inclined to, or extends across the microgroove of the second feed frame membrane support plate.

[0094] In some embodiments, the feed frame 260 may further include at least one feed frame leak hole, slot, or orifice 276 in the feed frame perimeter frame. The feed frame leak hole 276 may be configured to receive a portion of a leaked mixed gas flow from an open area and / or from an input conduit, such as across and / or between interfaces of adjacent frames. The feed frame leak hole may be different from and spaced apart from the open area 268 and(one or more) feed frame output orifices 270, and / or may be located between the open area 268 and(one or more) feed frame output orifices 270. When the feed frame 260 includes feed frame output orifices 270 on opposite sides of the feed frame, each of these sides may include at least one feed frame leak hole 276 located between the open area and the feed frame output orifice on that side.

[0095] One or more feed frame leakage orifices may at least substantially surround one or more feed frame output orifices 270 to ensure that any mixed gas flow leaking from, for example, an open area and / or an inlet conduit will be received by the feed frame leakage orifices, and not by the one or more feed frame output orifices and output conduits. Figure 7In the example shown, one or more feed frame leakage orifices 276 surround or extend at least 180 degrees around or along three of the four sides of the feed frame output orifice (i.e., two of the two lateral sides and one of the two longitudinal sides), with the remaining unenclosed sides closest to or adjacent to the edge of the feed frame. In other examples, the feed frame leakage orifices may surround the feed frame output orifice (one or more) by more than 180 degrees, such as 200, 220, 250, or 270 degrees. In yet another example, the feed frame leakage orifices may simply extend beyond the length of the feed frame output orifices without surrounding them. In other words, the feed frame leakage orifices may span and extend only beyond one side of the feed frame output orifice.

[0096] The feed frame leakage orifice 276 can be of any suitable shape(s) and / or size(s) and / or can terminate at any suitable location on the feed frame. Figure 7 In the example shown, the feed frame leakage orifice 276 is elongated and terminates at a position spaced apart from the longitudinal edge 297 of the perimeter frame of the feed frame 260. In other words, the feed frame leakage orifice 276 does not terminate at the longitudinal edge of the perimeter frame of the feed frame to maintain the mechanical integrity of the feed frame.

[0097] The feed frame 260 may include any suitable number of feed frame leak orifices 276. For example, the feed frame 260 may include two or more leak orifices 276, increasing the mechanical integrity of the feed frame relative to a single leak orifice 276 having a total length of two or more leak orifices. When the feed frame 260 includes two or more feed frame leak orifices 276 on the same side of the feed frame, those orifices may be different from each other and spaced apart, and portions of the feed frame leak orifices may overlap each other and / or be configured to ensure that leaking mixed gas flow does not flow or escape between the feed frame leak orifices and enter into one or more feed frame output orifices. Figure 7 In the example shown, the feed frame leakage orifice 276 includes a first feed frame leakage orifice 298 and a second feed frame leakage orifice 300 spaced apart from and different from the first feed frame leakage orifice. A substantial portion 302 of the first feed frame leakage orifice 298 may be collinear with a substantial portion 304 of the second feed frame leakage orifice 300.

[0098] The first feed frame leakage orifice 298 may include opposing longitudinal end portions 306 and 308, while the second feed frame leakage orifice 300 may include opposing longitudinal end portions 310 and 312. End portions 306 and 312 may surround the feed frame output orifice 270 and may be fluidly connected to or in fluid communication with a notch in the gasket frame (as discussed further below). Furthermore, end portion 310 may surround end portion 308 and / or may overlap end portion 308 to minimize leaking gas mixtures flowing between the first and second feed frame leakage orifices, such as leaking gas mixtures flowing parallel to lateral axes of the perimeter frame. In other words, end portion 310 may be coaxial with end portion 308 along a plurality of lateral axes perpendicular to the longitudinal axes of the feed frame perimeter frame. End portion 310 may be spaced apart from end portion 308 to increase the mechanical integrity of the feed frame.

[0099] The feed frame leakage orifice 276 can be formed by any suitable method(s). For example, metal etching can be used to form these orifices. In metal etching, a mask is applied to a suitable metal sheet to protect certain areas from the chemical erosion of the etching fluid. Typically, the etching fluid is applied to both surfaces of the metal sheet simultaneously, causing etching to occur from both opposite sides at nearly the same rate. As a result, the etching only slightly exceeds half the material thickness, meaning that the metal thickness is completely etched through. Etching typically produces features at least 1.5 times the etch depth. Other suitable methods for forming feed frame leakage orifices include laser cutting and milling. Feed frame leakage orifices are sometimes referred to as “feed frame venting channels.”

[0100] The gasket frame 262 may include any suitable structure configured to provide a mechanical seal between two or more adjacent frames and / or components. For example, each gasket frame may include a perimeter base or frame 314, an open area or zone 316 surrounded by the perimeter base, at least one gasket inlet port 318 in the perimeter base, and at least one gasket outlet port 320 in the perimeter base, such as... Figure 7As shown. Open region 316 may be fluidly connected to and / or in fluid communication with open region 268 of the feed frame. Open region may be different from and spaced apart from one or more gasket inlet orifices 318 and one or more gasket outlet orifices 320. One or more gasket inlet orifices 318 may be spaced apart from and different from open region 316 and one or more outlet orifices 310. One or more gasket inlet orifices form part of inlet conduit 250 with corresponding inlet orifices of other frames of frame 230. One or more gasket outlet orifices 320 may be spaced apart from and different from open region 316 and one or more inlet orifices 318. One or more gasket outlet orifices may form part of outlet conduit 252 with corresponding outlet orifices of other frames of frame 320. Each or more gasket outlet orifice 320 defines gasket outlet orifice axis 321.

[0101] In some embodiments where the feed frame(s) include one or more venting channels(s), each gasket frame 262 may include at least one notch 322 in the perimeter base. The notches 322(s) may be in or along the opposing longitudinal edges 324, 326 of the perimeter base 314. In other words, unlike feed frame leak orifices, the notches 322(s) may terminate at opposing longitudinal edges of the perimeter base. The notches 322(s) may be fluidly connected to the end portion 306 of the first feed frame leak orifice and the end portion 312 of the second leak feed frame orifice, or may be in fluid communication with the end portions 306 of the first feed frame leak orifice and the end portions 312 of the second leak feed frame orifice. The location of the notches on the feed frame edges allows leaked gas mixtures to escape from the frame 230 and accumulate in the internal space between the frame and the first and second side plates to flow through the leak ports of those side plates. The hydrogen purification device 196 includes any suitable number of gasket frames 262, and those frames can be positioned between the foil-microscreen assembly, one or more feed frames, and / or permeation frames. Figure 5 and Figure 7 In the example shown, each feed frame 260 is positioned between the first gasket frame 328 and the second gasket frame 330. Other examples of the hydrogen purification apparatus 196 may include more or fewer gasket frames 262.

[0102] During operation, the mixed gas flow typically flows across the open area of ​​the feed frame. Any deviation from this general flow, such as leakage between the feed frame and the adjacent gasket frame, should flow at least substantially toward the feed frame leakage orifice (rather than into the feed frame outlet orifice and outlet conduit) and out of the frame through the notch 322 of the gasket frame. Any leaked gas will accumulate in the internal space between the frame and the first and second side plates until those gases are removed through the leakage port 214 of one or both of the first and second side plates.

[0103] The permeation frame 264 can be disposed between the foil-microscreen assembly 208, such as Figure 5 and Figure 8 As shown. Unless explicitly excluded, the permeation frame 264 may additionally or alternatively include one or more other components and / or structures of one or more other permeation frames described in this disclosure. The permeation frame may be an integral frame made of a single material or a combination of materials. Suitable materials for permeation frames include 300 series stainless steels, such as 304 and 316. The permeation frame 264 may include a permeation frame perimeter portion 336, a membrane support portion 338 partially or completely surrounded and / or enclosed by the permeation frame perimeter portion, and at least one permeation frame inlet orifice 342 in the permeation frame perimeter portion. Figure 8 In the example shown, the membrane support portion is integrally formed with the perimeter portion of the permeation frame. In other words, the perimeter portion of the permeation frame and the membrane support portion are made of the same integral frame. The membrane support portion may be configured to contact and / or support the foil-microscreen assembly 208. The membrane support portion 338 includes opposing first surfaces 339 and second surfaces 340, which may be planar or generally planar surfaces.

[0104] One or both of surfaces 339 and 340 may include a plurality of channels or grooves 341. The grooves on the first and second surfaces can be of any suitable configuration. For example, the grooves on the first surface 339 may be parallel to each other, and the grooves on the second surface 340 may be parallel to each other. Furthermore, the grooves 341 on the first surface 339 relative to the grooves 341 on the second surface 340 can be of any suitable configuration. For example, the grooves 341 on the first surface 339 may be parallel to the grooves 341 on the second surface 340, such as... Figure 9 As shown. In other words, the groove 341 on the first surface 339 forms a zero-degree angle with respect to the groove 341 on the second surface 340.

[0105] Alternatively, the groove 341 on the first surface 339 can form any suitable non-zero angle relative to the groove 341 on the second surface 340. For example, the groove on the first surface 339 can form an angle of approximately 20 degrees relative to the groove on the second surface 340, such as... Figure 10 As shown. In other words, if the grooves on the first surface and the second surface are placed on the same surface with the same orientation, the groove from the first surface will form an angle of approximately 20 degrees with the groove from the second surface. Alternatively, the groove on the first surface 339 can form an angle of approximately 45 degrees with respect to the groove on the second surface 340, such as... Figure 11 As shown. In other words, if the grooves on the first surface and the second surface are placed on the same surface with the same orientation, the groove from the first surface will form an angle of approximately 45 degrees with the groove from the second surface. In another configuration, the groove on the first surface 339 may be at a 90-degree angle or perpendicular to the groove on the second surface 340, as shown. Figure 12 As shown. In other words, if the grooves on the first surface and the second surface are placed on the same surface with the same orientation, the groove from the first surface will form an angle of approximately 90 degrees with the groove from the second surface.

[0106] The grooves on the first and / or second surfaces can be any suitable shape(s), such as square, U-shaped, and / or V-shaped. Figures 9-12 In the example shown, each trench 341 is U-shaped, with opposing vertical walls and a curved bottom. The trench can span from one edge of the membrane support portion to the opposite edge, from one edge to a portion spaced apart from the opposite edge, or it can span between these edges.

[0107] Furthermore, the trenches on the first and / or second surfaces can be of any suitable size(s), such as any suitable depth(s). For example, one or more (or all) trenches on each of the first and / or second surfaces can be less than half the thickness of the membrane support portion. In this example, the trenches on the first surface do not intersect with the trenches on the second surface. In other words, the trenches on the first surface are not in fluid communication with the trenches on the second surface. Figures 10-12 In the example shown, one or more (or all) grooves on each of the first and / or second surfaces are at least half or more the thickness of the membrane support portion, such that the grooves on the first surface and the grooves on the second surface form a plurality of intersections 343 defining an output orifice 348. In other words, the grooves on the first surface are in fluid communication with the grooves on the second surface at the intersections. One or more (or all) output orifices 348 may additionally or alternatively be located in the perimeter portion 336 of the permeation frame. One or more (or all) output orifices 348 may form part of one or more output conduits 252 with corresponding output orifices of one or more other frames 230. Each of the one or more output orifices 348 defines a permeation frame output orifice axis 349.

[0108] One or more permeation frame inlet ports 342 may be spaced apart from and different from one or more permeation frame outlet ports 348. One or more permeation frame inlet ports may form part of one or more inlet conduits 250 with corresponding inlet ports of other frames of frame 230.

[0109] In some embodiments, the permeation frame 264 may include at least one permeation frame leak hole, slot, or orifice 344 in the perimeter frame of the permeation frame. One or more permeation frame leak holes 344 may be configured to receive a portion of a leaked mixed gas flow from the permeation frame membrane support portion and / or from an inlet conduit, such as across and / or between interfaces of adjacent frames. One or more permeation frame leak holes may be different from and spaced apart from one or more permeation frame inlet orifices 342 and one or more permeation frame outlet orifices 348, and / or may be located between the permeation frame membrane support portion 338 and one or more permeation frame inlet orifices 342. One or more permeation frame leak holes may at least substantially surround or completely surround or enclose one or more permeation frame inlet orifices 342 to ensure that any mixed gas flow leaking from, for example, an inlet conduit will be received by the permeation frame leak hole, and not by one or more permeation frame outlet orifices. Figure 8 In the example shown, one or more permeable frame leak orifices 344 surround one side of one or more permeable frame inlet orifices 342. In other examples, permeable frame leak orifices may surround permeable frame inlet orifices at 180 degrees or more, such as 200, 220, 250 or 270 degrees.

[0110] The permeation frame leakage orifice 344 can be of any suitable shape(s) and / or size(s) and / or may terminate at any suitable location(s) within the perimeter frame of the permeation frame. Figure 8 In the example shown, the permeate frame leakage orifice 344 is elongated and terminates at a position spaced apart from the longitudinal edge 350 of the perimeter frame of the permeate frame 264. In other words, the permeate frame leakage orifice 344 does not terminate at the longitudinal edge of the perimeter frame of the permeate frame to maintain the mechanical integrity of the permeate frame. The permeate frame leakage orifice may sometimes be referred to as a "permeate frame venting channel".

[0111] The permeation frame 264 may include any suitable number of permeation frame leak orifices 344. Figure 8In the example shown, for each permeable frame inlet orifice 342, the permeable frame 264 includes a single permeable frame leak orifice 344. However, other examples of the permeable frame 264 may include two or more permeable frame leak orifices 344 on each side or for each permeable frame inlet orifice 342. When the permeable frame 264 includes two or more permeable frame leak orifices 344 for each permeable frame inlet orifice 342, portions of the permeable frame leak orifices may overlap each other and / or may be configured to ensure that a leaking mixed gas flow does not flow or escape between the leak orifices and into one or more permeable frame outlet orifices. The permeable frame leak orifices 344 may include opposing longitudinal end portions 356 and 358, which may be fluidly connected to or in fluid communication with the notch 322 of the gasket frame, such as Figure 13 As shown. The permeation frame leakage orifice 344 can be formed by any suitable method, such as etching, laser cutting, and milling, as discussed above for the feed frame leakage orifice.

[0112] refer to Figures 13-14 One of the gasket frames 262 is shown above and / or adjacent to the permeate frame 264. The same or similar view would be seen if viewed along an imaginary plane parallel to frame 230 and passing between the feed frame 260 and the adjacent gasket frame 262 through the hydrogen purification apparatus 196, and looking toward this gasket frame. As previously described, the gasket frame 262 includes gasket outlet orifices 320. Each gasket outlet orifice 320 includes a length 360 measured parallel to the longitudinal axis 231 of the gasket frame, and a width 362 measured perpendicular to the longitudinal axis 231 or parallel to the lateral axis 233. The membrane support portion 338 of the permeate frame 264 includes opposing end portions 364 and a central portion 366 disposed between the end portions; both types of portions have outlet orifices 348 at the intersection 343 of grooves 341 on the first surface 339 and the second surface 340 as previously described. The output ports 348 are arranged and / or positioned in multiple rows, such as the first row 370, the second row 372, and the third row 374. Figures 13-14 In the example shown, the permeation frame 264 does not include any output orifice 348 in the perimeter portion 336.

[0113] Opposite end portions 364 of the membrane support portion 338 of the permeate frame may be horizontally aligned, sized, and / or positioned relative to the gasket outlet orifices 320 such that one or more (or all) of these end portions 360 have outlet orifices 348 in direct fluid communication with the gasket outlet orifices 320. In other words, each outlet orifice 348 in the end portions 364 defines a permeate frame outlet orifice axis 349, and each of these axes is parallel to the gasket outlet orifice axis 321 and passes through one of the gasket outlet orifices 320. Conversely, the permeate frame outlet orifice axis defined by the outlet orifices 348 located in the central portion 366 of the membrane support portion 338, rather than in the end portions 364, is parallel to the gasket outlet orifice axis 321 but does not pass through any of the gasket outlet orifices, and therefore is in fluid communication with the gasket outlet orifices but not in direct fluid communication with those gasket outlet orifices.

[0114] exist Figures 13-14 In the example shown, when viewed along an imaginary plane parallel to frame 230 and passing through the hydrogen purification device 196 between feed frame 260 and adjacent gasket frame 262, and looking toward the gasket frame, the end portion 360 spans all or substantially all of the width 362 and / or all or substantially all of the length 360 of the gasket outlet orifice 320. Figure 14 Ideally, two or more rows of outlet ports 348 are in direct fluid communication with the gasket outlet ports 320. Specifically, a portion of the first row 370, the second row 372, and the third row 374 of the outlet ports 348 are in direct fluid communication with the gasket outlet ports.

[0115] refer to Figure 15 Another example of a permeation frame 264, generally indicated by 376, is shown. Unless explicitly excluded, the permeation frame 376 may additionally or alternatively include one or more other components and / or structures of one or more other permeation frames described in this disclosure. The permeation frame 376 may include a permeation frame perimeter portion 378, a membrane support portion 380 partially or completely surrounded and / or enclosed by the permeation frame perimeter portion, and at least one permeation frame inlet orifice 382 in the permeation frame perimeter portion. Figure 15In the example shown, the membrane support portion 380 is integrally formed with the perimeter portion 378 of the permeate frame. Unlike the permeate frame 264, the permeate frame 376 includes one or more outlet orifices 384 in the perimeter portion 378, in addition to one or more outlet orifices in the membrane support portion 380 (such as intersections formed by trenches with a depth of 50% or more of the thickness of the membrane support portion). The outlet orifices in the perimeter portion 378 are spaced apart from the longitudinal edge 386 of the membrane support portion 380. In other words, one or more solid portions 388 of the perimeter portion 378 are disposed between the longitudinal edge 386 of the membrane support portion 380 and the outlet orifices 384 of the perimeter portion.

[0116] refer to Figures 16-17 One of the gasket frames 262 is shown above and / or adjacent to the permeate frame 264. The same or similar view would be seen if viewed along an imaginary plane parallel to frame 230 and passing between feed frame 260 and adjacent gasket frames 262 through the hydrogen purification apparatus 196, and looking toward this gasket frame. The membrane support portion 380 of the permeate frame 376 includes opposing end portions 390 and a central portion 392 disposed between the end portions; both types of portions have an outlet orifice 384 at the intersection 394 of grooves 396 on opposing first surfaces 398 and second surfaces 400. Unlike the permeate frame 264, the end portions 390 of the permeate frame 376 are much narrower than the end portions of the permeate frame 264 (smaller width, measured perpendicular to the longitudinal axis of the frame). The outlet orifices 384 in the membrane support portion 380 are arranged and / or positioned in multiple rows, such as a first row 404, etc.

[0117] Opposite end portions 390 of the membrane support portion 380 of the permeate frame may be horizontally aligned, sized, and / or positioned relative to the gasket outlet orifices 320 such that one or more (or all) of these end portions 390 have outlet orifices 384 in direct fluid communication with the gasket outlet orifices 320. In other words, each outlet orifice 384 in the end portions 390 defines a permeate frame outlet orifice axis 406, and each of these axes is parallel to the gasket outlet orifice axis 321 and passes through one of the gasket outlet orifices 320. Conversely, the permeate frame outlet orifice axes defined by outlet orifices 384 not located in the end portions 390 of the membrane support portion 380 are parallel to the gasket outlet orifice axis 321 but do not pass through any of the gasket outlet orifices, and are therefore in fluid communication with the gasket outlet orifices but not in direct fluid communication with them.

[0118] exist Figures 16-17In the example shown, when viewed along an imaginary plane parallel to frame 230 and passing through the hydrogen purification device 196 between feed frame 260 and adjacent gasket frame 262, and looking toward the gasket frame, the end portion 390 spans only a small portion (e.g., less than about 20%, 15%, or 10% of the width) and / or all or substantially all of the length 360 of the gasket outlet orifice 320. Figure 17 As shown, only a single row of output orifices 384 are in direct fluid communication with the gasket output orifice 320. Specifically, only the output orifices along the first row 404 are in direct fluid communication with the gasket output orifice. The output orifices 384 in the perimeter portion 378 are also in direct fluid communication with the gasket output orifice 320. The solid portion 388 of the perimeter portion 378 (e.g., the portion without any orifices, such as input and output orifices) spans the width and length of the output orifice portion of the gasket frame.

[0119] refer to Figure 18 Another example of a permeation frame 264, generally indicated by 406, is shown. Unless explicitly excluded, the permeation frame 406 may additionally or alternatively include one or more other components and / or structures of one or more other permeation frames described in this disclosure. The permeation frame 406 may include a permeation frame perimeter portion 408, a membrane support portion 410 partially or completely surrounded and / or enclosed by the permeation frame perimeter portion, and at least one permeation frame inlet orifice 412 in the permeation frame perimeter portion. Figure 18 In the example shown, the membrane support portion 410 is integrally formed with the perimeter portion 408 of the permeation frame. The permeation frame 406 is similar to the permeation frame 376, except that one or more outlet orifices 414 in the perimeter portion 408 are adjacent to the longitudinal edge 416 of the membrane support portion 410. In other words, there is no solid portion of the perimeter portion 408 between the longitudinal edge 416 of the membrane support portion 410 and the outlet orifices 414 in the perimeter portion. Furthermore, the outlet orifices 414 in the perimeter portion are wider than the outlet orifices of the permeation frame 376 (measured perpendicular to the longitudinal axis defined by the frame).

[0120] refer to Figures 19-20One of the gasket frames 262 is shown above and / or adjacent to the permeate frame 264. The same or similar view would be seen if viewed along an imaginary plane parallel to the frame 230 and passing through the hydrogen purification apparatus 196 between the feed frame 260 and the adjacent gasket frame 262, and looking toward this gasket frame. The membrane support portion 410 of the permeate frame 406 includes opposing end portions 418 and a central portion 420 disposed between the end portions; both types of portions have an outlet orifice 422 at the intersection 424 of grooves 426 on opposing first surfaces 428 and second surfaces 430. Similar to the permeate frame 376, the end portions 418 of the membrane support portion 410 of the permeate frame 406 are much narrower than the end portions of the membrane support portion of the permeate frame 264 (smaller width, measured perpendicular to the longitudinal axis of the frame). The outlet orifices 422 in the membrane support portion 410 are arranged and / or positioned in multiple rows, such as the first row 434, etc.

[0121] Opposite end portions 418 of the membrane support portion 410 of the permeate frame may be horizontally aligned with gasket outlet orifices 320 such that one or more (or all) outlet orifices 422 of these end portions 418 are in direct fluid communication with gasket outlet orifices 320. In other words, each outlet orifice 422 in the end portions 418 defines a permeate frame outlet orifice axis 436, and each of these axes is parallel to the gasket outlet orifice axis 321 and passes through one of the gasket outlet orifices 320. Conversely, the permeate frame outlet orifice axes defined by outlet orifices 422 not located in the end portions 418 of the membrane support portion 410 are parallel to the gasket outlet orifice axis 321 but do not pass through any of the gasket outlet orifices, and are therefore in fluid communication with the gasket outlet orifices but not in direct fluid communication with those gasket outlet orifices.

[0122] exist Figures 19-20 In the example shown, when viewed along an imaginary plane parallel to frame 230 and passing through the hydrogen purification device 196 between feed frame 260 and adjacent gasket frame 262, and looking toward the gasket frame, the end portion 418 spans only a small portion (e.g., less than about 20%, 15%, or 10% of the width) and / or all or substantially all of the length 360 of the gasket outlet orifice 320. Figure 20 As shown in the optimal configuration, only a single row of outlet orifices 422 is in direct fluid communication with the gasket outlet orifice 320. Specifically, only the outlet orifices along the first row 434 are in direct fluid communication with the gasket outlet orifice. The outlet orifices 414 in the perimeter portion 408 are also in direct fluid communication with the gasket outlet orifice 320. Unlike previous permeation frames, the solid portion of the perimeter portion spanning the width and / or length of the gasket outlet orifice is substantially less.

[0123] Although each of the above-described permeation frames is shown and described as an integral frame having a perimeter portion and a membrane support portion integrally formed with the perimeter portion, other examples of permeation frames may include perimeter members defining an open area that receives separate and distinct membrane support plates having grooves on opposing surfaces.

[0124] During operation, the permeate flow typically flows laterally across the membrane support section toward the output orifice of the permeate frame, which is in direct fluid communication with the corresponding output orifice and output conduit of the other frames. If there is any leakage of the mixed gas flow from the inlet orifice(s) of the permeate frame(s), such as leakage between the permeate frame and one or more adjacent components, those leaks will flow at least substantially toward the permeate frame leak orifice(if present) (rather than into the permeate frame output orifice), and out of the frame through the notch of the gasket frame, into the internal space between the frame and the first and second side plates, for removal through the leak port of one or both of the first and second side plates.

[0125] In some embodiments, the end plate, foil-microsieve assembly, and frame 224 may be fixed or compressed together, such as by bolts and / or other fasteners, without creating any metallurgical bonding and / or other types of chemical bonding between the two or more components of the hydrogen purification apparatus (except for the metallurgical bonding between the hydrogen selective membrane and the coated or uncoated microsieve structures within the foil-microsieve assembly as described above). For example, there are no gaskets and / or frames metallurgically bonded or otherwise chemically bonded to the hydrogen selective membrane and / or the microsieve structures of the foil-microsieve assembly, as well as to all other components of the hydrogen purification apparatus.

[0126] refer to Figure 21 This illustrates a method for fabricating the penetration framework of this disclosure and provides an example generally indicated by 500. Although in Figure 21 Specific steps are shown, but other examples of method 500 may omit, modify, repeat, and / or add one or more steps. Furthermore, these steps can be performed in any suitable order. At 502, one or more input orifices are created or formed in the peripheral portion of the overall frame. At 504, one or more output orifices are created or formed in the peripheral portion and / or membrane support portion or central portion of the overall frame (the central portion being partially or completely surrounded and / or enclosed by the peripheral portion).

[0127] At 506, one or more grooves are created or formed on opposite surfaces of the central portion of the overall frame. The grooves can be in any suitable configuration. For example, the grooves can be parallel to each other on one or two opposite surfaces. Furthermore, a groove on one surface may or may not be parallel to a groove on another surface. In some examples, the grooves are less than 50% of the thickness or depth of the central portion, such that even if the grooves on one surface are parallel to each other and parallel to the grooves on another surface, the grooves on one surface do not intersect with the grooves on the other surface. In other examples, one or more (or all) output orifices can be created or formed by creating grooves with a depth of 50% or more of the thickness or depth of the central portion and not parallel to the grooves on the other surface, such that the output orifices are formed at the intersections of these grooves. Input orifices, output orifices, and / or grooves can be created or formed by any suitable method or combination of suitable methods, such as chemical etching, laser etching, milling, die cutting, etc.

[0128] Although examples of manufacturing methods have been described above for the permeation frames (one or more) of various hydrogen purification devices, these methods can be applied to other frames of these devices.

[0129] Industrial applicability This disclosure includes hydrogen purification apparatus and components thereof, applicable to the fuel processing industry and other industries that purify, produce and / or utilize hydrogen.

[0130] The foregoing disclosure includes a number of different inventions with independent practical applicability. While each of these inventions is disclosed in its preferred form, the specific embodiments disclosed and described herein should not be considered limiting, as many variations are possible. The subject matter of this invention includes all novel and non-obvious combinations and sub-combinations of the various elements, features, functions, and / or characteristics disclosed herein. Similarly, where any claim refers to an element “a” or “first” or its equivalent, such a claim should be understood to include one or more such elements, neither requiring nor excluding two or more such elements.

[0131] Inventions embodied in various combinations and sub-combinations of features, functions, elements, and / or characteristics may be claimed by filing new claims in related applications. Such new claims, whether for different or the same invention, and whether they differ in scope, are broader, narrower, or the same as the original claims, are also considered to be included within the subject matter of this disclosure.

Claims

1. A hydrogen purification apparatus, comprising: The first end frame and the second end frame include: The input port is capable of receiving a mixed gas stream containing hydrogen and other gases; The output port is capable of receiving a permeate stream, the permeate stream comprising at least one of a hydrogen concentration higher than that of the mixed gas stream and a concentration of other gases lower than that of the mixed gas stream; and The byproduct port is capable of receiving a byproduct stream containing at least most of the other gases. At least one hydrogen-selective membrane is disposed between and fixed to the first end frame and the second end frame, the at least one hydrogen-selective membrane having a feed side and a permeate side, at least a portion of the permeate flow being formed by a portion of the mixed gas flow flowing from the feed side to the permeate side, wherein the remaining portion of the mixed gas flow retained on the feed side forms at least a portion of the byproduct flow; and Multiple frames are disposed between and fixed to the first end frame and the second end frame and the at least one hydrogen-selective membrane, the multiple frames including a permeation frame disposed between the at least one hydrogen-selective membrane and the first end frame, the permeation frame comprising: Perimeter section, A membrane support portion, surrounded by the peripheral portion, has opposing first and second surfaces, each of which has a plurality of grooves. The membrane support portion contacts and supports the at least one hydrogen-selective membrane, and is integrally formed with the peripheral portion. One or more output orifices are located in at least one of the perimeter portion and the membrane support portion, at least one of the one or more output orifices forming part of at least one output conduit with a corresponding output orifice of the other frames of the plurality of frames, and the at least one output conduit is capable of receiving at least a portion of the permeate flow. At least one input port is located in the perimeter portion, the at least one input port being different from and spaced apart from the one or more output ports, the at least one input port forming part of at least one input conduit with corresponding input ports of other frames of the plurality of frames, and the at least one input conduit being capable of receiving at least a portion of the mixed gas flow.

2. The apparatus of claim 1, wherein the sizes of the plurality of grooves on the first surface and the second surface are set such that the plurality of grooves on the first surface do not intersect with the plurality of grooves on the second surface.

3. The apparatus of claim 1, wherein the sizes of the plurality of grooves on the first surface and the second surface are configured such that one or more grooves on the first surface intersect one or more grooves on the second surface at one or more intersection points, and at least some of the at least one output orifice are located at the one or more intersection points.

4. The apparatus of claim 3, wherein all of the at least one output orifice are located at the one or more intersections.

5. The apparatus of claim 3, wherein the at least one output port comprises at least a first output port at the one or more intersections and at least a second output port in the perimeter portion.

6. The apparatus of claim 1, wherein the at least one output orifice is located only in the perimeter portion.

7. The apparatus of claim 6, wherein the plurality of grooves on the first surface are parallel to each other, and wherein the plurality of grooves on the second surface are parallel to each other and parallel to the plurality of grooves on the first surface.

8. The apparatus of claim 7, wherein the solid portion of the perimeter portion is disposed between the at least one output orifice and the membrane support portion.

9. The apparatus of claim 1, wherein the plurality of frames includes at least one gasket frame, the at least one hydrogen-selective membrane is disposed between the permeation frame and the at least one gasket frame, the at least one gasket frame comprising: The perimeter base of the plane, The open area surrounded by the perimeter base, At least one inlet port in the perimeter base, the at least one inlet port being different from and spaced apart from the open area, and the at least one inlet port in the perimeter base forming part of the at least one inlet conduit with the at least one inlet port of the permeation frame, and At least one output port in the perimeter base, the at least one output port being different from and spaced apart from the open area and the at least one input port, and the at least one output port in the perimeter base forming part of the at least one output conduit with the at least one output port of the permeation frame.

10. The apparatus of claim 9, wherein the at least one outlet orifice of the permeation frame is in direct fluid communication with the at least one outlet orifice of the at least one gasket frame.

11. The apparatus of claim 10, wherein the at least one output orifice of the at least one gasket frame defines a gasket orifice axis, and wherein the at least one output orifice of the permeation frame defines a permeation orifice axis, the permeation orifice axis being parallel to the gasket orifice axis and passing through the at least one output orifice of the at least one gasket frame.

12. The apparatus of claim 11, wherein the permeation frame is positioned in multiple rows of the one or more output orifices in the membrane support portion, and wherein the at least one output orifice of the permeation frame comprises two or more rows of the one or more output orifices of the permeation frame.

13. The apparatus of claim 11, wherein the permeation frame is positioned in multiple rows of the one or more output orifices in the membrane support portion, and wherein the at least one output orifice of the permeation frame comprises only a single end row of the one or more output orifices of the permeation frame.

14. The apparatus of claim 9, wherein the plurality of frames define a longitudinal axis, wherein the at least one output orifice in the peripheral base has a length measured parallel to the longitudinal axis and a width measured perpendicular to the longitudinal axis, wherein the plurality of frames includes at least one feed frame, and the at least one gasket frame is disposed between the at least one feed frame and the at least one hydrogen selective membrane.

15. The apparatus according to claim 14, wherein, When viewed along a plane parallel to the plurality of frames and passing through the device between the at least one feed frame and the at least one gasket frame, and looking toward the at least one gasket frame, the end portion of the membrane support portion visible through the at least one output orifice of the at least one gasket frame spans the entire width of the at least one output orifice of the at least one gasket frame.

16. The apparatus according to claim 14, wherein, When viewed along a plane parallel to the plurality of frames and passing through the device between the at least one feed frame and the at least one gasket frame, and looking toward the at least one gasket frame, the end portion of the membrane support portion visible through the at least one output orifice of the at least one gasket frame spans only a portion of the width of the at least one output orifice of the at least one gasket frame.

17. The apparatus according to claim 14, wherein, When viewed along a plane parallel to the plurality of frames and passing through the device between the at least one feed frame and the at least one gasket frame, and looking toward the at least one gasket frame, the end portion of the membrane support portion and the solid portion of the perimeter portion, visible through the at least one output orifice of the at least one gasket frame, span only a portion of the width of the at least one output orifice of the at least one gasket frame.

18. The apparatus of claim 1, further comprising at least one microscreen structure having a plurality of microscreen openings, wherein the at least one hydrogen-selective membrane metallurgy is incorporated into the at least one microscreen structure.

19. A method for manufacturing a permeation frame for a hydrogen purification apparatus, comprising: Create one or more input openings in the perimeter portion of the overall frame; One or more output openings are created in at least one of the peripheral portion and the central portion of the overall frame, the peripheral portion surrounding the central portion; as well as Multiple grooves are created on the opposing first and second surfaces of the central portion of the overall frame.

20. The method of claim 19, wherein creating a plurality of trenches includes creating a plurality of trenches whose size is set such that a plurality of trenches on the first surface do not intersect with a plurality of trenches on the second surface.

21. The method of claim 19, wherein creating one or more output orifices includes creating a plurality of grooves on the first surface and the second surface, the size of the plurality of grooves being set such that at least some of the one or more output orifices are located at positions where the plurality of grooves formed on the first surface intersect with the plurality of grooves on the second surface.

22. The method of claim 21, wherein creating one or more output apertures includes, in addition to the at least some of the one or more output apertures formed at locations where the plurality of grooves on the first surface intersect with the plurality of grooves on the second surface, also creating one or more output apertures in the perimeter portion.

23. The method of claim 21, wherein creating one or more output orifices includes creating a plurality of grooves on the first surface and the second surface, the size of the plurality of grooves being set such that all of the plurality of grooves formed on the first surface in the one or more output orifices intersect with the plurality of grooves on the second surface.

24. The method of claim 19, wherein creating the plurality of trenches comprises creating the plurality of trenches on the first surface and the second surface such that the plurality of trenches on the first surface are parallel to each other, and the plurality of trenches on the second surface are parallel to each other and parallel to the plurality of trenches on the first surface.

25. The method of claim 19, wherein creating one or more input apertures includes etching the one or more input apertures.

26. The method of claim 25, wherein creating one or more output apertures includes etching the one or more output apertures.

27. The method of claim 26, wherein creating the plurality of trenches includes etching the plurality of trenches.

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