Membrane base hydrogen purifier

Abstract

A membrane-based hydrogen purifier has a graphite frame component. The purifier includes a hydrogen separation membrane module having at least one membrane unit comprising: at least one hydrogen-selective membrane including a permeate surface and an opposing mixed-gas surface, and a fluid-permeable support structure substantially contacting and supporting at least a central region of the permeate surface. The membrane unit further includes a permeate-side frame component and a mixed-gas-side frame component. The permeate-side frame component is inserted between the hydrogen-selective membrane and the fluid-permeable support structure to substantially contact a peripheral region of the permeate surface and a peripheral region of the fluid-permeable support structure. The mixed-gas-side frame component substantially contacts a peripheral region of the mixed-gas surface. At least one of the permeate-side frame component and the mixed-gas-side frame component is a graphite frame component.

Description

[0001] This application claims priority to U.S. Application No. 17 / 107,523, filed November 30, 2020, the full disclosure of which is hereby incorporated by reference. Technical Field

[0002] This invention relates to membrane-based hydrogen purifiers, and more specifically, to membrane-based hydrogen purifiers having graphite frame components. Background Technology

[0003] A membrane-based hydrogen purifier is a device that uses one or more hydrogen-selective membranes to separate a mixture of hydrogen and gases. The hydrogen-selective membrane is permeable to hydrogen but impermeable to other gases, allowing hydrogen to selectively diffuse through the membrane, thus separating the hydrogen from the gas mixture. The hydrogen separated by the hydrogen purifier can be stored or used as fuel for various energy-generating devices such as fuel cell stacks.

[0004] Membrane-based hydrogen purifiers typically include a membrane support assembly that supports a hydrogen-selective membrane and can form various seals within the purifier to separate hydrogen separated by the hydrogen-selective membrane from other gases. More specifically, the membrane support assembly may include one or more membrane contact frame members, such as gaskets, that substantially contact at least a peripheral region of the hydrogen-selective membrane and can be compressed against the membrane to form a seal therewith. With this in mind, the composition of the frame members can affect the efficiency and rate at which the hydrogen purifier separates hydrogen from gas mixtures, as well as the lifespan of the hydrogen-selective membrane. More specifically, conventional frame members typically include impurities that impair or otherwise hinder the operation of the hydrogen-selective membrane supported by the frame members, thus adversely affecting the performance of the hydrogen purifier.

[0005] For example, conventional frame components may include particulate matter that can form perforations in the hydrogen-selective membrane when the conventional frame component contacts and supports the hydrogen-selective membrane within the hydrogen purifier. Such perforations can reduce the efficiency of the hydrogen-selective membrane and / or necessitate its replacement. As another example, conventional frame components may include chemical impurities that can interact with the hydrogen-selective membrane and reduce its hydrogen permeability. This reduction in hydrogen permeability can decrease the rate at which the hydrogen purifier can purify hydrogen. Therefore, there is a need for hydrogen purifiers with improved membrane contact frame components that may include reduced particulate matter and / or reduced chemical impurities, thereby improving the efficiency and / or rate at which the hydrogen purifier can purify hydrogen and / or increasing the lifespan of the hydrogen-selective membrane. Summary of the Invention

[0006] This invention relates to a membrane-based hydrogen purifier with a graphite frame component. The membrane-based hydrogen purifier includes a hydrogen separation membrane module comprising at least one membrane unit. The membrane unit includes a hydrogen-selective membrane defining a permeate surface and an opposing mixed-gas surface. The membrane unit further includes a mixed-gas-side frame component and a fluid-permeable support structure, the fluid-permeable support structure substantially contacting and supporting at least a central region of the permeate surface of the hydrogen-selective membrane. The membrane unit further includes a permeate-side frame component and a mixed-gas-side frame component. The permeate-side frame component is inserted between the hydrogen-selective membrane and the fluid-permeable support structure such that the permeate-side frame component substantially contacts a peripheral region of the permeate surface and a peripheral region of the fluid-permeable support structure. The mixed-gas-side frame component substantially contacts a peripheral region of the mixed-gas surface. At least one of the permeate-side frame component and the mixed-gas-side frame component is a graphite frame component. The graphite framework component may include at least a minimum limiting weight percentage of carbon, a limiting composition of insufficient particulate matter, particulate matter that is fine particulate matter, and / or a maximum limiting composition of at most one or more impurities. The membrane unit may include a pair of hydrogen-selective membranes and a corresponding pair of fluid-permeable support structures, a permeate-side framework component, and a mixed-gas-side framework component. The membrane module may include multiple membrane units, and the membrane-based hydrogen purifier may be included in and / or used with: a fuel processor; a fuel treatment system that generates a hydrogen-containing mixed-gas stream purified by the membrane module; and / or an assembly that generates and consumes hydrogen. Attached Figure Description

[0007] Figure 1 For illustrative purposes, an example of a hydrogen purifier according to the present invention is provided, which includes a hydrogen purifier that may be incorporated into a fuel processor and / or a fuel treatment system.

[0008] Figure 2 An example of a membrane unit for a hydrogen purifier is illustrated by an isometric exploded view according to the present invention.

[0009] Figure 3 The isometric exploded view according to the invention illustrates an example of a membrane unit comprising a pair of hydrogen-selective membranes.

[0010] Figure 4 This is a partial schematic representation of an example of a membrane unit located within a hydrogen purifier according to the present invention.

[0011] Figure 5 This is a partial cross-sectional view through a schematic membrane unit comprising a pair of hydrogen-selective membranes according to the present invention.

[0012] Figure 6 The isometric exploded view according to the invention illustrates a less schematic example of the membrane unit and feed plate assembly.

[0013] Figure 7 An exploded view of the membrane module according to the present invention, the membrane module comprising a plurality of membrane units and forming at least a portion of a hydrogen purifier.

[0014] Figure 8 This is a schematic representation of a hydrogen purifier included in a hydrogen-producing fuel processing system according to the present invention, which is, as appropriate, part of an assembly that generates and consumes hydrogen. Detailed Implementation

[0015] Figures 1 to 8 According to the present invention, examples of the following are provided: a membrane-based hydrogen purifier 38; a membrane module 44 of the membrane-based hydrogen purifier 38; a fuel processor 12 that includes and / or utilizes the membrane-based hydrogen purifier 38; a hydrogen-generating and consuming assembly 10 that includes and / or utilizes the membrane-based hydrogen purifier 38; and / or an energy-generating and consuming assembly 13 that includes and / or utilizes the membrane-based hydrogen purifier. Figures 1 to 8 In each of these, elements serving similar or at least substantially similar purposes are marked with the same number, and such elements may be disregarded. Figures 1 to 8 Each of these is discussed in detail in this article. Similarly, in Figures 1 to 8 In each of these documents, not all elements may be labeled, but for consistency, reference numbers associated with the stated elements may be used herein. References in this document... Figures 1 to 8 The elements, components and / or features discussed in one or more of the above may include: Figures 1 to 8 Any of the above and / or used in conjunction with the above without departing from the scope of the invention. Generally, elements that may be included in a particular embodiment are drawn with solid lines, while elements that are selected as appropriate and / or are environmentally friendly for a particular embodiment are drawn with dashed lines. However, elements shown with solid lines may not be necessary for all embodiments, and in some embodiments may be omitted without departing from the scope of the invention.

[0016] Figure 1An example of a membrane-based hydrogen purifier 38 according to the invention is illustrated schematically. As shown, the membrane-based hydrogen purifier 38 is configured to receive a mixed gas stream 36 comprising hydrogen 62 and one or more other gases 63. The membrane-based hydrogen purifier 38 is further configured to separate the mixed gas stream 36 into a purified hydrogen stream 42 and a byproduct stream 40. In other words, the membrane-based hydrogen purifier 38 can be described as being configured to produce purified hydrogen 62 from a mixture of gases including hydrogen and other gases. The membrane-based hydrogen purifier 38 may be referred to herein as hydrogen purifier 38 and / or purifier 38. The membrane-based hydrogen purifier 38 may be configured to produce pure or at least substantially pure hydrogen. As used herein, substantially pure hydrogen may be greater than 90%, greater than 95%, greater than 99%, greater than 99.5%, greater than 99.9%, and / or up to 100% pure. Unless otherwise indicated, percentages used herein are weight percentages.

[0017] The gas stream 36 may be rich in hydrogen, including a considerable concentration of hydrogen, and / or may include hydrogen as a major component. As used herein, a major component means a component present in a higher percentage or amount than other components, and a minor component means a component present in a lower percentage or amount than at least the major component. Examples of other gases that may be present in the gas stream 36 include carbon dioxide, carbon monoxide, and methane. The purified hydrogen stream 42 may include hydrogen at an increased concentration relative to the gas stream 36 and other gases at a decreased concentration relative to the gas stream 36. Therefore, the byproduct stream 40 may include hydrogen at a decreased concentration relative to the gas stream 36 and other gases at an increased concentration relative to the gas stream 36. The purified hydrogen stream 42 may contain at least a majority or most of the hydrogen in the gas stream 36, and the byproduct stream 40 may contain at least a majority or most of other gases. That is, the byproduct stream 40 may include a non-zero amount or concentration of hydrogen, and the purified hydrogen stream 42 may include a non-zero amount of other gases. In view of the above, the purified hydrogen stream 42 can also be described as a hydrogen-rich stream 42 and / or a product hydrogen stream 42.

[0018] like Figure 1 As shown, the hydrogen purifier 38 includes a hydrogen separation membrane module 44, which includes at least one hydrogen selective membrane 46 configured to separate the mixed gas stream 36 into a purified hydrogen stream 42 and a byproduct stream 40. The hydrogen separation membrane module 44 may also be referred to herein as membrane module 44.

[0019] A hydrogen-selective membrane 46 divides, partitions, or separates membrane module 44 into a gas mixing zone 86 and a permeate zone 88. The hydrogen-selective membrane 46 is hydrogen-permeable, meaning that hydrogen can permeate through the membrane during the operational use of the hydrogen purifier 38. The hydrogen-selective membrane 46 is constructed to allow hydrogen to diffuse from the gas mixing zone 86 to the permeate zone 88, while restricting other gases contained in the gas mixing stream 36 to the gas mixing zone 86. In other words, during operation of the hydrogen purifier 38, other gases can be at least substantially or completely fluidly isolated from the permeate zone 88, while the hydrogen-selective membrane 46 allows hydrogen to diffuse from the gas mixing zone 86 to the permeate zone 88. In other words, membrane module 44 can be described as being constructed to separate the gas mixing stream 36 into a purified hydrogen stream 42 and a byproduct stream 40 by selectively allowing hydrogen contained in the gas mixing stream 36 to diffuse from the gas mixing zone 86 through the hydrogen-selective membrane 46 to the permeate zone 88. Therefore, the byproduct stream 40 can be described as the portion of the mixed gas stream 36 that does not permeate through the hydrogen-selective membrane 46, and the purified hydrogen stream 42 can be described as the portion of the mixed gas stream 36 that permeates through the hydrogen-selective membrane 46. With this in mind, the hydrogen-selective membrane 46 may also be referred to herein as a hydrogen-permeable membrane 46, a hydrogen-permeable metal membrane 46, and / or a hydrogen separation membrane 46.

[0020] like Figure 1 The diagram schematically indicates that membrane module 44 may include a plurality of hydrogen-selective membranes 46. As discussed in more detail herein, hydrogen-selective membranes 46 may be configured in membrane module 44 as pairs 202 of hydrogen-selective membranes 46. Each hydrogen-selective membrane 46 is included in membrane unit 200, and membrane module 44 may include at least one and / or a plurality of membrane units 200. Each membrane unit 200 includes at least one hydrogen-selective membrane 46 and, where appropriate, pairs 202 of hydrogen-selective membranes 46. Each membrane unit 200 further includes a membrane support assembly 220 that supports the hydrogen-selective membrane 46 and, where appropriate, pairs 202 of hydrogen-selective membranes 46. Membrane module 44 may also include at least one feed assembly 210 configured to supply or deliver hydrogen-selective membranes via mixed gas stream 36 to membrane unit 200. A portion of the membrane support assembly 220 may form a fluid seal with at least one peripheral region of the hydrogen selective membrane 46, such that the membrane support assembly 220 and the hydrogen selective membrane 46 form a hydrogen-permeable fluid seal between the gas mixing region 86 and the permeate region 88.

[0021] The hydrogen-selective membrane 46 is formed of any suitable material that allows hydrogen to diffuse through the membrane while restricting the diffusion of other materials and / or gases contained in the mixed gas stream 36. Examples of the hydrogen-selective membrane 46 according to the invention include membranes having at least one of a metal, a noble metal, a metal alloy, a binary alloy, a ternary alloy, palladium, a palladium alloy, a palladium-copper (Pd-Cu) alloy, a palladium-yttrium alloy, and a palladium-ruthenium alloy, as well as other metal membranes made of substantially pure or alloyed metals. Examples of suitable hydrogen-selective membrane compositions containing Pd-Cu alloys include Pd-Cu alloys having a copper composition that is at least one of at least 15 wt%, at least 20 wt%, at least 25 wt%, at least 30 wt%, at least 35 wt%, at least 40 wt%, at least 45 wt%, at least 50 wt%, and / or at most 60 wt%, at most 55 wt%, at most 53 wt%, at most 50 wt%, at most 45 wt%, at most 40 wt%, at most 35 wt%, at most 30 wt%, and at most 25 wt%. As further examples, the Pd-Cu alloy may comprise at least one of 15 wt% to 45 wt% copper, which includes alloys having 15 wt% to 25 wt% copper, 35 wt% to 45 wt% copper, 20 wt% (or approximately 20 wt%) copper, or 40 wt% (or approximately 40 wt%) copper. Examples of suitable hydrogen-selective membranes and membrane compositions are disclosed in U.S. Patent Nos. 6,537,352 and 10,476,093 and U.S. Patent Application Publication No. 2008 / 0210088, the full disclosures of which are hereby incorporated herein by reference.

[0022] Generally, membrane module 44 separates the transmixed gas stream 36 in a pressure-driven process, wherein the transmixed gas stream 36 is supplied at high pressure to transmixed gas region 86 to facilitate hydrogen diffusion through hydrogen-selective membrane 46. For example, membrane module 44 may be configured to operate using transmixed gas stream 36 supplied at pressures of at least 50 psi (pounds per square inch), at least 100 psi, at least 125 psi, at least 150 psi, at least 175 psi, at least 200 psi, up to 150 psi, up to 175 psi, up to 250 psi, up to 300 psi, up to 500 psi, and / or up to 1000 psi. Membrane module 44 may also be configured to operate at ambient temperature or at high temperatures. As an example, membrane module 44 can be configured to operate at temperatures of at least 100°C, including temperatures greater than 175°C, 200°C, 250°C, 275°C, 300°C, 350°C, 400°C, and 450°C, and temperatures in the range of 100°C to 500°C (including temperatures in the ranges of 100°C to 450°C, 150°C to 425°C, 200°C to 400°C, 225°C to 350°C, 275°C to 450°C, 100°C to 275°C, 140°C to 240°C, 350°C to 450°C, and 300°C to 500°C), but temperatures outside these ranges are also within the scope of the invention. As one embodiment, for a hydrogen-selective membrane 46 containing an alloy of palladium and approximately 35% to 45% copper, a suitable hydrogen separation temperature may include a temperature in the range of 300°C to 450°C.

[0023] The membrane module 44 may include: a mixed gas inlet 82, which is in fluid communication with the mixed gas zone 86 and configured to receive the mixed gas stream 36; a byproduct outlet 84, which is in fluid communication with the mixed gas zone 86 and configured to remove the byproduct stream 40 from the mixed gas zone 86; and a purified hydrogen outlet 85, which is in fluid communication with the permeate zone 88 and configured to remove the purified hydrogen stream 42 from the permeate zone 88.

[0024] The hydrogen purifier 38 can be configured to receive the mixed gas stream 36 from any suitable source, and the purified hydrogen stream 42 generated by the hydrogen purifier 38 can be used for any suitable purpose. For example... Figure 1As shown, a hydrogen purifier 38 may be included in and / or used with a fuel processor 12, which is configured to generate hydrogen from a feed stream 16 comprising at least one feedstock 18. Specifically, the fuel processor 12 includes a hydrogen production zone 32 configured to receive the feed stream 16 and generate a mixed gas stream 36 comprising hydrogen from the feed stream 16. The hydrogen production zone 32 may generate hydrogen from the feed stream 16 by any number of suitable hydrogen production mechanisms. Examples of suitable hydrogen production mechanisms include steam reforming and autothermal reforming, wherein a reforming catalyst is used in the hydrogen production zone 32 to generate hydrogen from the feed stream 16 comprising a carbonaceous feedstock and water 20. In this configuration, feedstock 18 may be referred to herein as or may be carbonaceous feedstock 18. Examples of suitable carbonaceous feedstocks include at least one hydrocarbon or alcohol. Examples of suitable hydrocarbons include methane, propane, natural gas, diesel, kerosene, gasoline, and the like. Examples of suitable alcohols include methanol, ethanol, and polyols such as ethylene glycol and / or propylene glycol. Other suitable mechanisms for generating hydrogen include the pyrolysis and catalytic partial oxidation of the carbonaceous feedstock 18, in which case the feed stream 16 does not contain water but may contain oxygen. When the mixed gas stream received by the hydrogen purifier 38 is generated by the hydrogen production zone 32, the mixed gas stream 36 may also contain unreacted carbonaceous feedstock, which can be separated into a byproduct stream 40 by the hydrogen purifier 38.

[0025] When hydrogen production zone 32 produces hydrogen via a reforming process, it may be referred to as reforming zone 32 and may include a reforming catalyst 34. Specifically, when hydrogen production zone 32 produces hydrogen via a steam reforming process and includes a steam reforming catalyst, fuel processor 12 may be referred to as a steam reformer 30. Alternatively, when hydrogen production zone 32 produces hydrogen via a self-heating reforming process and includes a self-heating reforming catalyst, fuel processor 12 may be referred to as a self-heating reformer. In both instances, reforming zone 32 produces a mixed gas stream 36 comprising hydrogen and one or more other gases from a feed stream 16 comprising water and carbonaceous feedstock 18. When the mixed gas stream 36 is produced by reforming zone 32 and / or via a reforming process, the mixed gas stream 36 may be referred to as a reformed gas stream 36. In other words, hydrogen purifier 38 may be described as being constructed to separate the reformed gas stream 36 into a purified hydrogen stream 42 and a byproduct stream 40 when included in or used with a fuel processing system. When included in or used with the fuel processor 12, the hydrogen purifier 38 may be referred to as the purification zone 38, the separation zone 38, and / or the separation assembly 38.

[0026] like Figure 1As shown, byproduct stream 40 can be supplied to a heating assembly 91, which may include a burner assembly 92 comprising one or more burners, and the burner assembly 92 can combust or otherwise utilize byproduct stream 40 to generate heat. Heating assembly 91 may be configured to heat at least a portion of fuel processor 12, such as hydrogen production zone 32, hydrogen purifier 38, and / or membrane module 44. For example, heating assembly 91 may be configured to heat portions of the fuel processing system to a suitable operating temperature or operating temperature range for hydrogen production, hydrogen purification, etc. Heating assembly 91 may also be configured to heat various streams within fuel processor 12. As an example, heating assembly 91 may include a vaporization zone or vaporizer configured to vaporize any liquid portion of feed stream 16, such that feed stream 16 may be vaporized upon, after, or before entering hydrogen production zone 32.

[0027] The fuel processor 12 may also include a heated containment structure 94 defining an internal compartment, which may contain at least a portion of the hydrogen purifier 38, membrane module 44, hydrogen production zone 32, and / or feed flow delivery system 17, as well as any suitable valves, conduits, and / or piping associated with the above components. Any components contained within the heated containment structure 94 may be maintained at substantially the same temperature or at different temperatures. Also within the scope of the invention, the heated containment structure 94 may include an insulating material that reduces the rate of heat transfer between the internal compartment of the heated containment structure 94 and the environment and / or controls heat flow among the components contained within the internal compartment.

[0028] The hydrogen purifier 38 is not limited to use in the fuel processor 12 and can be used to purify hydrogen outside the fuel processor 12 without departing from the scope of the invention. As an example, the hydrogen purifier can be constructed to purify a mixed gas stream from a stored gas containing hydrogen from industrial or commercial processes and a mixed gas or impure hydrogen stream.

[0029] The hydrogen purifier 38 may also include various additional components besides the membrane module 44, such as components for supplying the mixed gas stream 36 to the membrane module 44 and / or removing the purified hydrogen stream 42 from the membrane module 44. For example, and as... Figure 1As shown, the hydrogen purifier 38 may include, or be in fluid communication with, a polishing zone 45 that receives purified hydrogen stream 42 from membrane module 44 and is configured to further purify the purified hydrogen stream 42 by removing selected impurities that may be present in the purified hydrogen stream 42, reducing the concentration of selected impurities, and / or chemically reacting with selected impurities. Examples of components that may be used in the polishing zone 45 include water shift reactors, methanation catalysts that convert carbon monoxide and hydrogen to methane and water, and / or other components, structures, and / or compositions that convert carbon monoxide to carbon dioxide or otherwise absorb or remove carbon monoxide from the purified hydrogen stream. For example, when the purified hydrogen stream 42 is intended for use in a fuel cell stack 22 that includes a proton exchange membrane (PEM) or would be damaged if the purified hydrogen stream 42 includes a determined concentration of carbon monoxide or carbon dioxide, the polishing zone 45 may include at least one methanation catalyst bed.

[0030] Now refer to Figure 2 The exploded view according to the invention illustrates an example of a membrane unit 200 forming part of a membrane module 44. The membrane unit 200 may also be referred to herein as a membrane encapsulation 200 and / or a membrane housing 200. As shown, the membrane unit 200 includes a hydrogen-selective membrane 46 defining a permeate surface 52 and a mixed-gas surface 50. The mixed-gas surface 50 is positioned within or facing the mixed-gas region 86 of the membrane module 44. The permeate surface 52 is positioned within or facing the permeate region 88 of the membrane module 44. The mixed-gas surface 50 may also be referred herein as facing the mixed-gas region 50, the recombinant surface 50, and / or facing the recombinant region 50, and the permeate surface 52 may also be referred herein as facing the permeate region 52, facing the product hydrogen region 52, and / or facing the purified hydrogen region 52. The hydrogen-selective membrane 46 may be constructed to have any suitable thickness, which can be measured between the mixed-gas surface 50 and the permeate surface 52. In detail, the diffusivity of hydrogen through the hydrogen-selective membrane and / or the hydrogen permeability of the hydrogen-selective membrane 46 can be proportional to the thickness of the hydrogen-selective membrane or the distance that hydrogen must diffuse through the hydrogen-selective membrane. Thus, when used under the same operating conditions, a thinner hydrogen-selective membrane 46 can have greater hydrogen permeability than a thicker hydrogen-selective membrane that is otherwise identical. Therefore, the hydrogen purifier 38 according to the invention can utilize a hydrogen-selective membrane 46 that is extremely thin, such as having a thickness of 15 to 25 micrometers. As an example, each hydrogen-selective membrane 46 of the membrane unit 200, membrane module 44, and / or hydrogen purifier 38 according to the invention can have a membrane thickness of up to 25 micrometers, up to 20 micrometers, up to 15 micrometers, up to 10 micrometers, up to 5 micrometers, at least 1 micrometer, at least 2 micrometers, at least 4 micrometers, at least 6 micrometers, at least 8 micrometers, at least 10 micrometers, and at least 12 micrometers.

[0031] As discussed herein, membrane module 44 receives the mixed gas stream 36 within the mixed gas zone 86, and the hydrogen-selective membrane 46 allows at least a portion of the hydrogen 62 contained within the mixed gas stream 36 to diffuse into the permeate zone 88, while confining other gases 63 present in the mixed gas stream 36 to the mixed gas zone 86. The hydrogen 62 diffused through the hydrogen-selective membrane 46 is removed from membrane module 44 as a purified hydrogen stream 42.

[0032] like Figure 2 As shown, membrane unit 200 also includes a fluid-permeable support structure 233 that physically contacts and supports at least a central region 230 of the permeate surface 52. More specifically, during operation of membrane module 44, the mixed gas flow 36 can be supplied to the mixed gas region 86 at a pressure higher than the pressure of the purified hydrogen flow 42 within the permeate region 88, and the fluid-permeable support structure 233 can counteract the pressure difference between the mixed gas region 86 and the permeate region 88 to support at least the central region 230 of the hydrogen-selective membrane 46. The fluid-permeable support structure 233 may comprise any suitable fluid-permeable or porous material or a combination of one or more porous materials, constructed to support the hydrogen-selective membrane 46 and allow fluid to flow from the permeate surface 52 of the hydrogen-selective membrane 46. As an example, the fluid-permeable support structure 233 may include one or more of the following: a sieve structure, one or more mesh sieves, one or more fine-mesh sieves, one or more coarse-mesh sieves, one or more expanded metal sieves, one or more porous ceramic components, filter cloth, and / or combinations thereof. Figure 2 As shown, the fluid-permeable support structure 233 may be located within or define a portion of the permeable region 88. The fluid-permeable support structure 233 may also be referred to herein as support structure 233.

[0033] Membrane unit 200 also includes a permeate-side frame member 226, which is inserted between the hydrogen-selective membrane 46 and the fluid-permeable support structure 233 and substantially contacts the peripheral region 228 of both the hydrogen-selective membrane 46 and the fluid-permeable support structure 233. The permeate-side frame member 226 supports the peripheral region 228 of the hydrogen-selective membrane 46 and can also be configured to form a fluid seal with the peripheral region 228 of the permeate surface 52. The permeate-side frame member 226 includes a central region 239, which may be an open central region and / or a fluid-permeable central region, allowing hydrogen 62 to flow from the permeate surface 52 of the hydrogen-selective membrane 46 to the permeate region 88. In other words, the permeate-side frame member 226 can be described as having substantial contact with the peripheral region 228 of the fluid-permeable support structure 233 and the hydrogen-selective membrane 46, and / or can be described as a gasket and / or has a gasket shape.

[0034] Membrane unit 200 further includes a gas-mixing side frame member 224 that substantially contacts a peripheral region 228 of the gas-mixing surface 50 of the hydrogen-selective membrane 46. The gas-mixing side frame member 224 is configured to form a fluid seal with the peripheral region 228 of the gas-mixing surface 50 and the peripheral region of the feed assembly 210 supplying the gas-mixing flow 36 to the gas-mixing surface 50. The gas-mixing side frame member 225 may also be configured to support the peripheral region 228 of the gas-mixing surface 50 of the hydrogen-selective membrane 50. The gas-mixing side frame member 224 also includes a central region 239 that may be open and / or fluid-permeable, such that the gas-mixing side frame member 224 allows the gas-mixing flow 36 to contact at least the central region 230 of the hydrogen-selective membrane 46. In other words, the gas-mixing side frame member 224 may be described as having a peripheral region 228 that substantially contacts and supports the hydrogen-selective membrane 46 and / or may be described as a gasket and / or have a gasket shape. Figure 2 As shown, the mixed gas side frame component 224, the permeate side frame component 226, and the fluid permeable support structure 233 can be described as defining the membrane support assembly 220 and / or included in the membrane support assembly.

[0035] Continue to refer to Figure 2 At least one of the permeate-side frame component 226 and the gas-mixing-side frame component 224 is a graphite frame component 250. More specifically, the gas-mixing-side frame component 224 may be a graphite frame component 250, the permeate-side frame component 226 may be a graphite frame component, or both the gas-mixing-side frame component 224 and the permeate-side frame component 226 may be graphite frame components 250. The gas-mixing-side frame component 224, the permeate-side frame component 226, and the graphite frame component 250 may be referred to as frame components. The graphite frame component 250 comprises graphite and / or is formed from graphite. Specifically, the graphite frame component 250 may comprise high-purity graphite and / or may be formed from high-purity graphite. As an example, the graphite frame component 250 may comprise at least 99 wt% carbon. As further examples, the graphite frame component 250 may include at least one of at least 99.1 wt% carbon, 99.2 wt% carbon, 99.3 wt% carbon, 99.4 wt% carbon, 99.5 wt% carbon, at least 99.6 wt% carbon, at least 99.7 wt% carbon, at least 99.8 wt% carbon, and at least 99.9 wt% carbon. Alternatively or additionally, the graphite frame component 250 may include up to 99.999 wt% carbon.

[0036] In other words, the graphite frame component 250 may include impurities and / or components other than graphite in low and / or reduced amounts, concentrations, and / or present amounts. More specifically, the graphite frame component 250 may include impurities in low, reduced, and / or harmless amounts, concentrations, and / or present amounts that may impede, damage, hinder, and / or impede the operation of the hydrogen selective membrane 46 and / or membrane module 44 during the operational use of the hydrogen purifier 38. As mentioned, the permeate-side frame component 226 and / or the gas-mixing-side frame component 224 may form a fluid seal with the peripheral region 228 of the hydrogen selective membrane 46 to fluidly isolate the permeate region 88 from other gases 63 in the gas-mixing flow 36. With this in mind, the graphite frame component 250 may include any components or impurities in low, reduced, and / or harmless amounts or concentrations that may damage, hinder, and / or compromise the fluid seal formed with the hydrogen selective membrane 46.

[0037] As a more specific example, the gas-mixed side frame component 224, the permeate-side frame component 226, and / or the graphite frame component 250 may include a non-zero amount of particulate matter 290, such as at least 0.001 wt% particulate matter. Particulate matter 290 may include particles or particles of material that can create surface roughness in the respective frame components, compromise the fluid seal formed between the frame components and the hydrogen-selective membrane 46, and / or form perforations in the hydrogen-selective membrane 46. As an example, particulate matter 290 may include particles of ash, MgO, Al2O3, CaO, Fe2O3, and / or a material that may have greater hardness than the hydrogen-selective membrane 46 and / or be hard enough to allow the particles to penetrate or perforate the hydrogen-selective membrane 46. With this in mind, the graphite frame component 250 may be formed, constructed, and / or constructed to include low, reduced, or harmless amounts, concentrations, or quantities of particulate matter 290. In other words, the graphite frame component 250 may include less than a maximum number of particulate particles 290 that are not detrimental or harmful to the operation of the hydrogen-selective membrane 46 and / or membrane module 44, and / or do not cause harmful surface roughening in the graphite frame component 250 and / or do not compromise the fluid seal formed with the hydrogen-selective membrane 46. As an example, the graphite frame component 250 may include up to 1 wt% particulate particles, up to 0.9 wt% particulate particles, up to 0.8 wt% particulate particles, up to 0.7 wt% particulate particles, up to 0.6 wt% particulate particles, up to 0.5 wt% particulate particles, up to 0.4 wt% particulate particles, up to 0.3 wt% particulate particles, up to 0.2 wt% particulate particles, up to 0.1 wt% particulate particles, or up to 0.01 wt% particulate particles.

[0038] Alternatively, the graphite frame component 250 may be formed as, constructed and / or constructed to include particulate particles 290 of a type, form and / or size that are non-damaging, non-harmful and / or non-hazardous to the operation of the hydrogen-selective membrane 46, the membrane module 44 and / or the fluid seal formed with the hydrogen-selective membrane 46. For example, particulate particles 290 including larger or coarse particles may create surface roughness in individual frame components, may impair the fluid seal formed with the hydrogen-selective membrane 46, and / or may form perforations in the hydrogen-selective membrane 46. In contrast, particulate particles 290 composed of fine particles 292, composed of small or fine particulate particles and / or excluding coarse or larger particles may not create surface roughness in individual frame components, may not impair the fluid seal formed with the hydrogen-selective membrane 46, and / or may not form perforations in the hydrogen-selective membrane 46. With this in mind, the graphite frame component 250 may comprise only fine granular particles 292 and / or may at least substantially contain no coarse or larger granular particles. Specifically, the fine granular particles 292 may consist of granular particles having a maximum size of up to 400 micrometers, while the coarse granular particles may consist of granular particles having a maximum size of at least 400 micrometers. As further examples, the fine granular particles 292 may consist of granular particles having a maximum size of at least one of the following: up to 400 micrometers, up to 300 micrometers, up to 200 micrometers, up to 150 micrometers, up to 100 micrometers, up to 80 micrometers, up to 60 micrometers, up to 40 micrometers, up to 20 micrometers, up to 10 micrometers, up to 5 micrometers, up to 1 micrometer, up to 0.5 micrometers, up to 0.2 micrometers, and / or at least 0.1 micrometers.

[0039] like Figure 2 As shown, the graphite frame component 250 includes at least one membrane contact surface 234 that substantially contacts and supports the hydrogen-selective membrane 46. The membrane contact surface 234 of the graphite frame component 250 may be a smooth surface and / or may be configured to form a seal with the hydrogen-selective membrane 46. Alternatively or additionally, this seal may be referred to herein as a fluid seal, a non-perforated seal, and / or a non-perforated fluid seal.

[0040] Continue to refer to Figure 2The gas-mixing side frame component 224, the permeate-side frame component 226, and / or the graphite frame component 250 may also include one or more chemical impurities 294. When present in a sufficiently large amount, quantity, or concentration within the frame components, the chemical impurities 294 can, for example, hinder, damage, impede, and / or impede the operation of the hydrogen selective membrane 46 and / or membrane module 44 during the operational use of the hydrogen purifier 38. Therefore, the hydrogen purifier 38 according to the invention may include the gas-mixing side frame component 224, the permeate-side frame component 226, and / or the graphite frame component 250, which are formed, constructed, and / or constructed to have such chemical impurities 294 in amounts below this critical limit.

[0041] As a more specific example, chemical impurities 294 may include sulfur, sulfur compounds, and / or sulfide ions, which may be dispersed, embedded, and / or adsorbed onto or within the mixed gas-side frame component 224, the permeate-side frame component 226, and the graphite frame component 250. As used herein, the term "adsorption" means by any process that includes at least adsorption, absorption, chemical bonding, or a combination thereof, and / or retention of a composition, contaminant, or other species. When sulfur is present in a sufficiently large amount, quantity, or concentration within the frame component, sulfur may be transported from the frame component, such as during operation of the membrane module 44 at high temperatures, and adsorbed onto the hydrogen-selective membrane 46. Adsorption of sulfur onto the hydrogen-selective membrane 46 can be detrimental and / or reduce the hydrogen permeability of the hydrogen-selective membrane 46. With this in mind, the graphite frame component 250 may include low, reduced, or harmless amounts, concentrations, or quantities of sulfur. In other words, the graphite frame component 250 may include sulfur at concentrations or amounts below the threshold, which are harmless or non-impeding to the hydrogen-selective membrane 46 under any of the pressures and / or temperatures discussed herein during operation of the membrane module 44. As examples, the graphite frame component 250 may include at least one of the following: up to 450 parts per million (ppm) of sulfur, up to 400 ppm of sulfur, up to 350 ppm of sulfur, up to 300 ppm of sulfur, up to 250 ppm of sulfur, up to 200 ppm of sulfur, up to 100 ppm of sulfur, up to 50 ppm of sulfur, and up to 20 ppm of sulfur. The graphite frame component 250 may include small, harmless, or non-interacting concentrations of sulfur, such as at least 0.5 ppm of sulfur or at least 1 ppm of sulfur.

[0042] Another example of chemical impurities 294 that may be present in the gas-mixed side frame component 224, the permeate-side frame component 226, and the graphite frame component 250 is a halide. More specific examples of halides include bromides, chlorides, and / or compounds thereof. When present in the frame components in sufficiently high quantities, amounts, or concentrations, halides can be transported from the frame components, such as during operation of the membrane module 44 at high temperatures, and adsorbed onto the hydrogen-selective membrane 46. Adsorption of halides onto the hydrogen-selective membrane 46 can be detrimental and / or reduce the hydrogen permeability of the hydrogen-selective membrane 46. With this in mind, the graphite frame component 250 may include one or more halides and / or total concentrations of halides in low, reduced, or harmless amounts, concentrations, or quantities. In other words, the graphite frame component 250 may include one or more halides in concentrations or quantities below a threshold that are harmless or non-adverse to the hydrogen-selective membrane 46, such as during operation of the membrane module 44 at any of the pressures and / or temperatures discussed herein. As an example, the graphite frame component 250 may include at least one of up to 100 ppm halide, up to 80 ppm halide, up to 60 ppm halide, up to 40 ppm halide, up to 20 ppm halide, up to 10 ppm halide, and up to 1 ppm halide. The graphite frame component 250 may include small, harmless, or non-interacting concentrations of halide, such as at least 0.05 ppm halide or at least 0.2 ppm halide.

[0043] The graphite frame component 250 according to the invention can be configured to support and / or form a seal, such as a perforation-free seal, with the hydrogen-selective membrane 46 and / or the feed assembly 210 under any suitable applied pressure. More specifically, compressive forces can be applied to the peripheral region 228 of the feed assembly 210 and / or the peripheral region 228 of the membrane support assembly 220 to form a plurality of fluid seals for the inner membrane shell 222. Specifically, the hydrogen selective membrane 46 can be compressed against the pressure of at least one of the following: the mixed gas side frame component 224, the permeate side frame component 226, and / or the graphite frame component 250: at least 2000 psi (13.8 MPa), at least 2900 psi (20 MPa), at least 3000 psi (20.7 MPa), at least 3200 psi (22.1 MPa), at least 3400 psi (23.4 MPa), at least 3600 psi (24.8 MPa), and / or at most 3100 psi (21.4 MPa), at most 3200 psi (22.1 MPa), at most 3600 psi (24.8 MPa), at most 3700 psi (25.5 MPa), at most 3800 psi (26.2 MPa), and at most 4000 psi (27.6 MPa). As discussed herein, either of the two faces of the graphite frame component 250 may be a smooth surface, which allows the graphite frame component 250 to be supported under either of these applied pressures and / or to form a fluid seal such as a non-perforated fluid seal with the hydrogen selective membrane 46 and / or the feed assembly 210.

[0044] The graphite frame component 250, the gas-mixed side frame component 224, and the permeate-side frame component 226 may each have any suitable density. As an example, the graphite frame component 250 may have a graphite frame component density that is at least one of the following: at least 0.7 g / cm³ (g / cc), at least 0.8 g / cc, at least 0.9 g / cc, at least 1 g / cc, at least 1.1 g / cc, at least 1.2 g / cc, at least 1.3 g / cc, at least 1.4 g / cc, at least 1.5 g / cc, up to 1.8 g / cc, up to 1.7 g / cc, up to 1.6 g / cc, up to 1.5 g / cc, up to 1.4 g / cc, up to 1.3 g / cc, up to 1.2 g / cc, up to 1.1 g / cc, and up to 1 g / cc. The gas-mixed side frame component 224 and the permeate-side frame component 226 may have the same or different densities. In some instances, the gas-mixing side frame component 224 and the permeate side frame component 226 may have different densities. More specifically, in some hydrogen purifiers 38, the density of the gas-mixing side frame component 224 may be less than the density of the permeate side frame component 226, because this facilitates the assembly of the membrane unit 200 and / or allows the membrane unit 200 to be compressed in a manner that does not impair the hydrogen-selective membrane 46.

[0045] With this in mind, the permeate-side frame component 226 may have a permeate-side frame component density greater than that of the mixed-gas-side frame component 224. As an example, the permeate-side frame component 226 of the hydrogen purifier 38 according to the invention may include a permeate-side frame component density of at least one of the following: at least 0.7 g / cc, at least 0.8 g / cc, at least 0.9 g / cc, at least 1.0 g / cc, at least 1.1 g / cc, at least 1.2 g / cc, at least 1.3 g / cc, at least 1.4 g / cc, at least 1.5 g / cc, at most 1.8 g / cc, at most 1.7 g / cc, at most 1.6 g / cc, at most 1.5 g / cc, and at most 1.4 g / cc. As further examples, the gas-mixed side frame component 224 may include a gas-mixed side frame component density of at least one of the following: at least 0.7 g / cc, at least 0.8 g / cc, at least 0.9 g / cc, at least 1 g / cc, at least 1.1 g / cc, at least 1.2 g / cc, up to 1.4 g / cc, up to 1.3 g / cc, up to 1.2 g / cc, up to 1.1 g / cc, and up to 1 g / cc. As a more specific example, the gas-mixed side frame component density may be a critical fraction of the permeate side frame component density, wherein examples of critical fractions include 95%, 90%, 85%, 80%, 78%, 75%, 70%, or 65%. Therefore, when the gas-mixed side frame component 224 and the permeate side frame component 226 are graphite frame components 250, each graphite frame component 250 may be constructed to have a different density.

[0046] The mixed gas side frame component 224 and the permeate side frame component 226 of the hydrogen purifier 38 according to the present invention may have any suitable thickness, which is also within the scope of the present invention. Examples of the thickness of the permeate side frame component 226 include at least 0.05 mm, at least 0.075 mm, at least 0.1 mm, at least 0.125 mm, up to 0.25 mm, up to 0.20 mm, up to 0.175 mm, up to 0.15 mm, and / or up to 0.125 mm. Examples of the thickness of the mixed gas side frame component 224 include at least 0.15 mm, at least 0.2 mm, at least 0.25 mm, at least 0.3 mm, up to 0.6 mm, up to 0.5 mm, up to 0.45 mm, up to 0.4 mm, and / or up to 0.35 mm. The permeate side frame component 226 and the mixed gas side frame component 224 may have the same or different thicknesses. In some instances, the thickness of the permeate-side frame member 226 may differ from the thickness of the corresponding mixed-gas-side frame member 224. More specifically, the thickness of the permeate-side frame member 226 may be less than the thickness of the corresponding mixed-gas-side frame member 224. This thickness difference can reduce stress and / or deformation on the hydrogen-selective membrane 46.

[0047] The thickness of the permeate-side frame component 226 may differ from the thickness of the gas-mixing-side frame component 224 by any suitable amount. As an example, the thickness of the permeate-side frame component may be less than 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 52%, 50%, and / or 45% of the thickness of the gas-mixing-side frame component.

[0048] In view of the above, the graphite frame component 250 may be constructed to have any suitable thickness, such as any of the thicknesses discussed herein with reference to the gas-mixing side frame component 224 and / or the permeate side frame component 226. As a more specific example, when both the gas-mixing side frame component 224 and the permeate side frame component 226 are graphite frame components 250, the graphite frame component 250 may include the same or different thicknesses.

[0049] Although Figure 2 The illustration shows an example in which membrane unit 200 includes a single hydrogen-selective membrane 46, but it is within the scope of the invention that membrane unit 200 may include two hydrogen-selective membranes 46 that can be configured as a pair 202 of hydrogen-selective membranes. Figure 3The diagram is an exploded view illustrating an example of membrane unit 200 comprising a pair 202 of hydrogen selective membrane 46. As shown, the pair 202 of hydrogen selective membrane 46 includes a first hydrogen selective membrane 270, a second hydrogen selective membrane 272, and a membrane support assembly 220 supporting the first hydrogen selective membrane 270 and the second hydrogen selective membrane 272. The first hydrogen selective membrane 270 defines a first trans-mixed gas surface 300 facing the trans-mixed gas region 86 and a first permeate surface 304 facing the permeate region 88. The second hydrogen selective membrane 272 defines a second trans-mixed gas surface 306 facing the trans-mixed gas region 86 and a second permeate surface 302 facing the permeate region 88.

[0050] The membrane support assembly 220 includes a fluid-permeable support structure 233 positioned between at least a central region 230 of a first hydrogen-selective membrane 270 and at least a central region 230 of a second hydrogen-selective membrane 272, such that the fluid-permeable support structure 233 substantially contacts and supports at least a central region 230 of a first permeate surface 304 and at least a central region 230 of a second permeate surface 302. In this manner, the first permeate surface 304 of the first hydrogen-selective membrane 270 and the second permeate surface 302 of the second hydrogen-selective membrane 272 are generally supported by the fluid-permeable support structure 233, which supports the central region 230 of the first hydrogen-selective membrane 270, which is spaced apart from or in a spaced-apart relationship with the central region 230 of the second hydrogen-selective membrane 272.

[0051] The membrane support assembly 220 further includes a first mixed-gas side frame member 274 and a first permeate side frame member 278 supporting a first hydrogen-selective membrane 270, as discussed herein, and a second mixed-gas side frame member 276 and a second permeate side frame member 280 supporting a second hydrogen-selective membrane 272, as discussed herein. Figure 3 As shown herein, one or more of the first gas-mixing side frame component 274 and the first permeate side frame component 278, and each of them as appropriate, is a graphite frame component 250, and one or more of the second gas-mixing side frame component 276 and the second permeate side frame component 280, and each of them as appropriate, is a graphite frame component 250. As discussed herein, the first gas-mixing side frame component 274 and the first permeate side frame component 278 may be referred to herein as corresponding frame components. Similarly, the second gas-mixing side frame component 276 and the second permeate side frame component 280 may be referred to herein as corresponding frame components.

[0052] Figure 4 This is a schematic representation of an example of a portion of a membrane module 44 comprising at least one graphite frame member 250 according to the present invention. More specifically, Figure 4This is a partial cross-sectional schematic diagram of membrane module 44, showing a single membrane unit 200 and one or more corresponding feed assemblies 210. As shown, membrane module 44 includes membrane unit 200 having at least one hydrogen-selective membrane 46, and, where appropriate, pairings 202 of hydrogen-selective membranes 46. Also as shown, membrane module 44 includes membrane support assembly 220 having a mixed gas-side frame component 224, a permeate-side frame component 226, and a fluid-permeable support structure 233 that contacts, supports, and / or seals with, such as the hydrogen-selective membrane 46 discussed herein.

[0053] like Figure 4 As shown in the examples, the membrane module 44 according to the invention may also include at least one feed assembly 210 associated with the membrane unit 200, which may be configured to supply the mixed gas stream 36 to the mixed gas zone 86 and / or receive the byproduct stream 40 and / or the mixed gas stream 36 from the mixed gas zone 86. Figure 4 An example of the feed assembly 210 is illustrated schematically. As shown, the feed assembly 210 may include a feed plate 212, which may include and / or define a supply region 215 for supplying the mixed gas stream 36 to the mixed gas region 86 and / or a discharge region 216 for receiving the mixed gas stream 36 and / or the byproduct stream 40 from the mixed gas region 86. The feed assembly 210 may also include a feed frame 214 positioned between the feed plate 212 and the membrane unit 200. More specifically, the feed frame 214 may be positioned between the feed plate 212 and the mixed gas side frame member 224 such that the feed frame 214 operatively contacts the peripheral area of ​​the mixed gas side frame member 224 and the feed plate 212, and supports the feed plate 212 spaced apart from the mixed gas side frame member 224. As shown, the feed frame 214, together with the gas-mixing side frame component 224, can form an open volume 119 between the hydrogen selective membrane 46 and the feed plate 212 to allow the gas-mixing flow 36 to flow across the gas-mixing surface 50 and / or allow fluid flow between the supply area 215 and the discharge area 216.

[0054] Continue to refer to Figure 4Membrane unit 200 is shown as comprising a pair 202 of hydrogen-selective membranes 46 supported by a common fluid-permeable support structure 233. Specifically, the fluid-permeable support structure 233 supports at least a central region 230 of the spaced-apart pairs 202 of hydrogen-selective membranes 46, wherein permeate regions 88 are defined between the hydrogen-selective membranes. When membrane unit 200 includes pairs 202 of hydrogen-selective membranes 46, membrane module 44 may include a pair of feed assemblies 210 associated with membrane unit 200, wherein the pair of feed assemblies 210 includes a first feed assembly 320 configured to supply a mixed gas flow 36 to a mixed gas surface 50 of a first hydrogen-selective membrane 270, and a second feed assembly 322 configured to supply a mixed gas flow 36 to a mixed gas surface 50 of a second hydrogen-selective membrane 272.

[0055] like Figure 4 As shown, membrane module 44 may include an inner membrane shell 222 configured to fluidly isolate the permeate region 88 from the gas-mixing region 86. The inner membrane shell 222 may be formed by at least a peripheral region 228 of the gas-mixing side frame member 224, the permeate side frame member 226, the hydrogen-selective membrane 46, and the feed assembly 210. More specifically, at least a portion of the permeate region 88 may be confined by the permeate surface 52 of the hydrogen-selective membrane 46, while the peripheral region 228 of the fluid-permeable support structure 233 may allow the purified hydrogen flow 42 to pass from within the inner membrane shell 222 to the outside of the inner membrane shell 222, such that at least a portion of the permeate region 88 is defined outside the inner membrane shell 222. Membrane module 44 may also include an outer membrane shell 240 surrounding the inner membrane shell 222 and the permeate region 88. In detail, the inner surface of the outer membrane shell 240 may surround the inner membrane shell 222 and the permeate region 88. The outer membrane shell 240 and the inner membrane shell 222 may be spaced apart from each other, such that the inner surface of the outer membrane shell 240 and the outer surface of the inner membrane shell 222 may define a conduit for collecting the purified hydrogen gas flow 42.

[0056] The inner membrane shell 222 may include multiple fluid seals that fluidly isolate the gas-mixing region 86 from the permeate region 88, such as fluid seals formed between the gas-mixing side frame member 224 and the feed assembly 210 and / or fluid seals formed between the gas-mixing side frame member 224 and the hydrogen-selective membrane 46. With this in mind, the gas-mixing side frame member 224 may be a graphite frame member 250, such that a non-perforated fluid seal is formed between the gas-mixing side frame member 224 and the peripheral region 228 of the hydrogen-selective membrane 46 and / or between the gas-mixing side frame member 224 and the feed assembly 210. In this application, the feed assembly contact surface 238 of the graphite frame member 250 may also be a smooth surface for membrane contact surfaces, as discussed herein, such that the graphite frame member 250 can form a non-perforated fluid seal with the feed assembly 210.

[0057] Figure 5 This is a partial cross-sectional view of a schematic example of a membrane unit 200 penetrating the membrane module 44 according to the present invention. Figure 5 In one example, membrane unit 200 includes a first hydrogen-selective membrane 270 and a second hydrogen-selective membrane 272 forming a pair 202 of hydrogen-selective membrane 46. A fluid-permeable support structure 233 is positioned between and in contact with the first hydrogen-selective membrane 270 and the second hydrogen-selective membrane 272. The first hydrogen-selective membrane 270 is contacted by a first gas-mixing side frame member 274 and a first permeate-side frame member 278, as discussed herein. Similarly, the second hydrogen-selective membrane 272 is contacted by a second gas-mixing side frame member 276 and a second permeate-side frame member 280, as discussed herein. As further shown, at least one of the first gas-mixing side frame member 274 and the second gas-mixing side frame member 276 is a graphite frame member 250, and at least one of the first permeate-side frame member 278 and the second permeate-side frame member 280 is a graphite frame member 250. Figure 5 In this example, the thickness T1 of the first permeate-side frame component 278 is less than the thickness T2 of the first mixed-gas-side frame component 274. Similarly, the thickness of the second permeate-side frame component 280 is less than the thickness of the second mixed-gas-side frame component 276.

[0058] The graphite frame component 250 according to the invention can be a flexible graphite frame component 252, which, in addition to including any of the features, functions, compositions, properties, and / or configurations discussed for the graphite frame component 250, can also be flexible. The flexible graphite frame component 252 can be configured to bend, deform, and / or elastically deform to smooth surface changes and / or can be configured to resist the hydrogen-selective membrane 46 under compression in a manner that prevents damage to the hydrogen-selective membrane 46 and / or prevents permeation in the inner membrane shell 222. For example, in Figure 5 As illustrated schematically, the hydrogen-selective membrane 46 may not be flat when supported by the fluid-permeable support structure 233. More specifically, the fluid-permeable support structure 233 may include a sieve structure, and the central region 230 of each hydrogen-selective membrane 46 may have undulations A because it conforms to the shape of the sieve structure. The peripheral region 228 of each hydrogen-selective membrane 46 may have smaller undulations or reduced undulations relative to the central region 230. In detail, the flexible graphite frame component 252 may smooth or buffer the surface variations in the peripheral region 228 of the fluid-permeable support structure 233 to provide a smooth or buffered support surface to the hydrogen-selective membrane 46. With this in mind, the permeate-side frame component 226 (see...) Figure 2 ,and Figure 5The frame components 278 and 280 in the feed assembly 210 can be flexible graphite frame components 252. That is, the mixed gas side frame component 224 can be flexible graphite frame component 252, such that the flexible graphite frame component 252 can be smoothed out from any surface variations that may exist in the feed assembly 210.

[0059] Figures 6 to 7 The present invention provides a more detailed and / or less illustrative description of examples of a membrane module 44, components of the membrane module 44 and / or a membrane-based hydrogen purifier 38, and / or a fuel processor 12 and / or a hydrogen-generating and consuming assembly 10, wherein the hydrogen-generating and consuming assembly includes and / or utilizes the hydrogen purifier 38. The hydrogen purifier 38, the membrane module 44, the fuel processor 12 and / or the hydrogen-generating and consuming assembly 10 may include those referenced herein. Figures 6 to 7 The features, functions, structures, components, attributes, etc., discussed herein may include any one of them, but need not include all such features, functions, structures, components, attributes, etc. Similarly, references in this article... Figures 1 to 5 All features, functions, structures, components, properties, etc., of the disclosed hydrogen purifier 38, membrane module 44, fuel processor 12, and / or hydrogen-generating and consuming assembly 10 may be included in Figures 6 to 7 In instances and / or used with it, without needing to include all such features, functions, structures, components, properties, etc.

[0060] Initial Reference Figure 6 An exploded view is illustrated therein, showing an example of membrane unit 200 and the corresponding feed assembly 210. As discussed herein, membrane unit 200 may include a pair 202 of hydrogen-selective membranes 46 configured around a common fluid permeable support structure 233, such that the pair 202 of hydrogen-selective membranes 46 can be described as defining a common permeate channel therebetween through which a purified hydrogen stream can be collected. Membrane unit 200 further includes a mixed gas-side frame member 224 and a permeate-side frame member 226, configured to support the hydrogen-selective membranes 46 and configured to seal, support, and / or interconnect membrane units 200 when membrane module 44 includes multiple membrane units. Figure 6 The diagram further illustrates that at least one permeate-side frame component 226 and / or at least one gas-mixed side frame component 224 is a graphite frame component 250.

[0061] The fluid-permeable support structure 233 includes a sieve structure 312 that fits within and / or extends at least partially over the surface of the permeate frame 314 to form a permeate plate assembly 310. Permeate-side frame members 226 extend and / or are positioned on each planar side of the permeate plate assembly 310 and can be used to seal the permeate plate assembly 310 to another structure of the membrane unit 200, such as via a mixed-gas-side frame member 224 and / or a hydrogen-selective membrane 46.

[0062] The feed assembly 210 is positioned adjacent to the membrane unit 200 to deliver the mixed gas stream to the membrane unit 200 and remove the resulting dehydrogenated mixed gas stream and / or byproduct stream from the membrane unit 200. When the membrane module 44 includes multiple membrane units 200, the feed assembly 210 may be positioned between adjacent membrane units 200. As shown, the feed assembly 210 includes a feed plate 212 that can separate the membrane unit 200 from another membrane unit and / or separate the membrane unit 200 from the end plate assembly. The feed plate 212 has a central region 213 and a supply region 215 and a discharge region 216 defined on the periphery of the feed plate 212. The central region 213 of the feed plate 212 may be fluid-impermeable, or at least substantially fluid-impermeable. The supply region 215 connects the supply manifold 110 to the mixed gas region 86 via one or more supply channels 114. Similarly, discharge zone 216 connects discharge manifold 112 to mixed gas zone 86 via one or more discharge channels 116. Supply channel 114 and discharge channel 116 are formed through the thickness or full thickness of feed plate 212.

[0063] The feed assembly 210 further includes a feed frame 214 positioned on either side or face of the feed plate 212. When the feed assembly 210 is inserted between the membrane unit 200 and an adjacent membrane unit, the feed frame 214, positioned opposite the membrane unit 200, can interface with and / or contact the adjacent membrane unit. When assembled, the feed frame 214 overlaps with the periphery of each side of the feed plate 212 and can create an open volume 119 between the central region 213 and the adjacent hydrogen-selective membrane 46, wherein the open volume 119 is formed by the thickness of the feed frame 214 and the thickness of the mixed gas side frame member 224. The feed frame 214 may overlap with the central portions of the supply channel 114 and the discharge channel 116 but may not overlap with either end of the supply channel 114 and the discharge channel 116. Thus, the mixed gas flow provided by the supply manifold 110 can flow through the supply channel 114 and flow below the feed frame 214, and then flow into the open volume 119. Similarly, dehydrogenated gas or byproduct streams can flow from open volume 119 through discharge channel 116 to discharge manifold 112. Therefore, the width of feed frame 214 in the region overlapping the central portions of supply channel 114 and discharge channel 116 must be smaller than the span or length of channels 114 and 116, such that supply manifold 110 and discharge manifold 112 are fluidly connected to open volume 119.

[0064] like Figure 6As shown, each feed frame 214 may include two or more separate parts. For example, the feed frame 214 may include an outer feed frame component 316 and a feed plate gasket 318 inserted between the outer feed frame component 316 and the feed plate 212. In this way, the feed plate gasket 318 may be configured to contact the feed plate 212, while the outer feed frame component 316 may be configured to contact another structure of the membrane module 44, such as the gas-mixing side frame component 224.

[0065] When assembled, the gas-mixing side frame component 224, the permeate side frame component 226, the hydrogen-selective membrane 46, the permeate frame 314, and the feed assembly 210 can be compressed against each other to form part of the inner membrane shell 222, which isolates the permeate zone 88 from the supply manifold 110, the discharge manifold 112, and / or the gas-mixing zone 86. The sieve structure 312 forms peripheral regions along both sides of the permeate plate assembly 310 to allow hydrogen diffused through the hydrogen-selective membrane 46 to flow from the inner membrane shell 222 and be collected as a purified hydrogen stream. The permeate frame 314 forms peripheral regions on the other two sides of the permeate plate assembly 310 to form a fluid seal with the permeate side frame component 226 and to isolate the permeate zone 88 from the gas-mixing zone 86, the supply manifold 110, and / or the discharge manifold 112.

[0066] Turn Figure 7 The diagram illustrates an isometric exploded view illustrating an example of a membrane module 44, which can be configured for use in or as a hydrogen purifier according to the invention. The membrane module 44 includes a plurality of membrane units 200 and a plurality of feed assemblies 210 positioned between the membrane units 200. The membrane units 200 and feed assemblies 210 may be collectively referred to as forming a membrane stack 65, which can be described as forming an inner membrane shell 222 configured to prevent gases other than hydrogen contained in the mixed gas zone 86, the exhaust manifold 112, and / or the supply manifold 110 from entering the permeate zone 88. As further shown, each membrane unit 200 includes at least one graphite frame member 250 supporting a hydrogen-selective membrane 46 and may form part of an inner membrane shell 222 as discussed herein.

[0067] When assembled, membrane unit 200 and feed assembly 210 are stacked between two end plates 140 and enclosed in a cylindrical housing 142. The end plates 140 and cylindrical housing 142 may form at least a portion of the encloseable permeate region 88 of the outer membrane shell 240. In this example, feed assembly 210 includes a feed plate 212 positioned between the outer feed frame component 316 and the feed plate gasket 318. Feed assembly 210 is positioned at the end of membrane stack 65 closest to the mixed gas inlet 82, such that feed assembly 210 is inserted between membrane unit 200 and mixed gas inlet 82.

[0068] exist Figure 7 In this example, the membrane module 44 further includes at least one flexible pad 96 positioned between the membrane stack 65 and the end plate 140. The flexible pad 96 can compensate for dimensional tolerance variations in the metal components of the membrane unit 200 and / or the feed assembly 210 and / or compensate for dimensional variations caused by assembling the membrane unit 200, for example, by welding or other assembly methods (e.g., bolting). The flexible pad 96 allows for a wide range of displacements during the assembly process while keeping the load applied to the membrane encapsulation within acceptable limits. For example, several thinner flexible pads or one thicker pad can be used. In other words, the desired total thickness of the flexible pads can be achieved by either one thick pad or several thinner pads.

[0069] Depending on the situation, the end plates 140 can be mechanically fastened to each other via rods 146 that extend through holes 148 disposed around the peripheral areas of the membrane stack 65 and the flexible gasket 96. Rods 146 can be used to align the component portions of the membrane stack 65 with each other.

[0070] like Figure 7 As shown, membrane module 44 also includes a mixed gas inlet 82 through which a mixed gas flow 36 is supplied to a supply manifold 110. From the supply manifold 110, the mixed gas flow 36 can be divided among the membrane units 200 and flows across the membrane units 200 toward the discharge manifold 112. A byproduct outlet 84 is provided in membrane module 44 to receive and discharge byproduct flow 40 from the discharge manifold 112, and is provided via a purified hydrogen outlet 85 to remove the purified hydrogen flow 42 from the permeate zone 88.

[0071] Figure 8 The following example is illustrated schematically: a hydrogen purifier 38 is included in and / or used with a hydrogen production fuel processing system 11, a hydrogen production and consumption assembly 10, and / or an energy production and consumption assembly 13. As shown, the hydrogen production fuel processing system 11 includes: a fuel processor 12, such as those referenced herein. Figure 1 Any of the fuel processors 12 discussed; and a feed stream delivery system 17 configured to deliver one or more feed streams 16 to the fuel processor 12. The feed stream delivery system 17 delivers feed streams 16 containing carbonaceous feedstock 18 and, where appropriate, water 20. The feed stream delivery system 17 can deliver feed streams 16 to the fuel processor 12 via one or more streams. When the carbonaceous feedstock 18 is miscible with water, the carbonaceous feedstock 18 can be mixed with, for example... Figure 8 Water 20 is delivered together with the feed stream 16, as shown by the solid line in the center. When the carbon-containing feedstock 18 is immiscible or only slightly miscible with water, these components typically act as... Figure 8The dashed lines indicate individual or different feed streams 16, or feed streams delivered to the fuel processor 12. Individual feed streams may be combined within the fuel processor when in use. In another example, carbonaceous feedstock 18 and / or water 20 may be vaporized and delivered as a single feed stream. The feed stream delivery system 17 may include one or more pumps 26 that can deliver components of the feed stream 16 from one or more individual supplies 19. The feed stream delivery system 17 may additionally or alternatively include a valve assembly 29 configured to regulate the flow of components of the feed stream 16 from at least one pressurized supply 19. The supply 19 may be located outside the hydrogen-producing fuel processing system 11 and / or may be housed within or adjacent to the hydrogen-producing fuel processing system 11.

[0072] The hydrogen purifier 38 may also be included in and / or used with the hydrogen-generating and consuming assembly 10. For example... Figure 8 As shown, the hydrogen-generating and consuming assembly 10 includes: a hydrogen production fuel processing system 11; and a hydrogen consumption assembly 43 configured to receive a purified hydrogen stream 42 from the hydrogen production fuel processing system 11 and consume or otherwise use at least a portion of the purified hydrogen stream 42. As an example, the hydrogen consumption assembly 43 may be or include a fuel cell stack 22 configured to generate an electrical output 27 from the purified hydrogen stream 42. The fuel cell stack 22 contains at least one, and typically multiple, fuel cells 24 configured to generate an electric current from a portion of the purified hydrogen stream 42 delivered thereto and an oxidant 15 such as oxygen. Examples of suitable fuel cells include proton exchange membrane (PEM) fuel cells and alkaline fuel cells. The fuel cell stack 22 may receive some or all of the purified hydrogen stream 42. Alternatively or additionally, at least a portion of the purified hydrogen stream 42 may be delivered for use in another hydrogen consumption process, such as combustion for heating and / or storage for later use. The electrical output 27 generated by the fuel cell stack 22 can be used to meet the energy demand of the energy consumption device 25 or the applied load. As examples, the energy consumption device 25 may include motor vehicles, SUVs, boats, tools, lamps or lighting assemblies, appliances (such as household, commercial, or industrial appliances), residences, buildings, communication equipment, etc. Alternatively or additionally, the electrical output 27 may be stored for later use in an energy storage device 28, which may include any suitable means for storing electrical energy, such as one or more batteries. When the electrical output 27 generated by the fuel cell stack 22 is supplied to the energy consumption device 25 and / or the energy storage device 28, the hydrogen purifier 38 may be described as being included in and / or used with the energy-generating and energy-consuming assembly 13, such as… Figure 8 As shown in the image.

[0073] As used herein, the term "and / or" placed between the first entity and the second entity means one of the following: (1) the first entity, (2) the second entity, and (3) the first entity and the second entity. Multiple entities listed using "and / or" should be interpreted in the same way, i.e., "one or more" of the entities thus combined. Other entities may exist besides those specifically identified by the "and / or" clause, whether related to or unrelated to those specifically identified entities. Therefore, as a non-limiting example, the reference to "A and / or B," when used in conjunction with open-ended language such as "includes," may: in one embodiment, mean only A (including entities other than B, as appropriate); in another embodiment, mean only B (including entities other than A, as appropriate); and in yet another embodiment, mean both A and B (including other entities, as appropriate). Such entities may refer to elements, actions, structures, steps, operations, values, and the like.

[0074] As used herein, the phrase "at least one" referring to a list of one or more entities should be understood to mean at least one entity selected from any one or more entities in the list of entities, but does not necessarily include at least one of every entity specifically listed in the list of entities, and does not exclude any combination of entities in the list of entities. This definition also allows for the presence of entities other than those specifically identified in the list of entities referred to by the phrase "at least one," whether related to or not related to those specifically identified entities. Thus, as a non-limiting example, "at least one of A and B" (or equivalently "at least one of A or B" or, equivalently "at least one of A and / or B") may in one embodiment refer to at least one (whether including more than one) A without B (and, whether including entities other than B); in another embodiment, refer to at least one (whether including more than one) B without A (and, whether including entities other than A); and in yet another embodiment, refer to at least one (whether including more than one) A and at least one (whether including more than one) B (and, whether including other entities). In other words, the phrases "at least one," "one or more," and "and / or" are open-ended expressions that can function as both conjunctions and antonymous conjunctions in practice. For example, each of the expressions "at least one of A, B, and C," "at least one of A, B, or C," "one or more of A, B, and C," "one or more of A, B, or C," and "A, B, and / or C" can mean only A, only B, only C, A and B together, A and C together, B and C together, A, B, and C together, and, as appropriate, any of the above combined with at least one other entity.

[0075] Where any patent, patent application or other reference is incorporated herein by reference and (1) defines a term in a manner that is inconsistent with and / or (2) otherwise inconsistent with the non-incorporated portion of the invention or any other incorporated reference, the non-incorporated portion of the invention shall be controlled and the terms therein or incorporated disclosures shall be controlled only with respect to the references that define the terms and / or the originally presented incorporated disclosures.

[0076] As used herein, the terms "adapted" and "constructed" mean that an element, component, or other subject is designed and / or intended to perform a given function. Therefore, the use of the terms "adapted" and "constructed" should not be construed as meaning that a given element, component, or other subject is simply "capable" of performing a given function, but rather that the element, component, and / or other subject is specifically selected, generated, implemented, used, programmed, and / or designed to perform the function. Elements, components, and / or other described subjects described as adapted to perform a particular function may also be alternatively or alternatively described as constructed to perform that function, and vice versa, which is also within the scope of this invention.

[0077] As used herein, the phrases "for example," "as an example," and / or the abbreviated term "example," when used with reference to one or more components, features, details, structures, embodiments, and / or methods according to the invention, are intended to convey that the described components, features, details, structures, embodiments, and / or methods are illustrative, non-exclusive examples of the components, features, details, structures, embodiments, and / or methods according to the invention. Therefore, the described components, features, details, structures, embodiments, and / or methods are not intended to be limiting, essential, or exclusive / exhaustive; and other components, features, details, structures, embodiments, and / or methods (including structurally and / or functionally similar and / or equivalent components, features, details, structures, embodiments, and / or methods) are also within the scope of the invention.

[0078] Examples of membrane-based hydrogen purifiers, fuel processors, fuel processing systems, and assemblies that generate and consume hydrogen according to the present invention are presented in the following paragraphs.

[0079] A1. A hydrogen purifier comprising a hydrogen separation membrane module, the membrane module comprising:

[0080] At least one membrane unit comprising:

[0081] (i) A hydrogen-selective membrane that defines a permeate surface and an opposing mixed gas surface;

[0082] (ii) A fluid-permeable support structure that substantially contacts and supports at least a central region of the permeable surface;

[0083] (iii) A permeate-side frame component inserted between the hydrogen-selective membrane and the fluid-permeable support structure, such that the permeate-side frame component substantially contacts a peripheral region of the permeate surface and a peripheral region of the fluid-permeable support.

[0084] (iv) A gas-mixing side frame component that substantially contacts a peripheral area of ​​the gas-mixing surface; and

[0085] At least one of the permeate-side frame component and the mixed gas-side frame component is a graphite frame component.

[0086] A2. The membrane module as described in paragraph A1, wherein the graphite frame component contains at least 99% by weight (wt%) carbon.

[0087] A2.1. A membrane module as described in any of paragraphs A1 to A2, wherein the mixed gas side frame component is the graphite frame component.

[0088] A2.2. A membrane module as described in any of paragraphs A1 to A2.1, wherein the permeate-side frame component is the graphite frame component.

[0089] A2.3. A membrane module as described in any of paragraphs A1 to A2.2, wherein the gas-mixing side frame component and the permeate side frame component are graphite frame components.

[0090] A2.4. A membrane module as described in any of paragraphs A2 to A2.3, wherein the graphite frame component comprises at least one of at least 99.1 wt% carbon, 99.2 wt% carbon, 99.3 wt% carbon, 99.4 wt% carbon, 99.5 wt% carbon, at least 99.6 wt% carbon, at least 99.7 wt% carbon, at least 99.8 wt% carbon, and at least 99.9 wt% carbon.

[0091] A2.5 The membrane module as described in paragraph A2.4, wherein the graphite frame component contains up to 99.999 wt% carbon.

[0092] A2.6. A membrane module as described in any of paragraphs A2 to A2.5, wherein the graphite frame component is a flexible graphite frame component.

[0093] A3. A membrane module as described in any of paragraphs A1 to A2.6, wherein each of the gas-mixed side frame component, the permeate side frame component, and the graphite frame component comprises particulate particles.

[0094] A3.1. The membrane module as described in paragraph A3, wherein the graphite framework component comprises up to 1 wt% granular particles, up to 0.9 wt% granular particles, up to 0.8 wt% granular particles, up to 0.7 wt% granular particles, up to 0.6 wt% granular particles, up to 0.5 wt% granular particles, up to 0.4 wt% granular particles, up to 0.3 wt% granular particles, up to 0.2 wt% granular particles, up to 0.1 wt% granular particles, or up to 0.01 wt% granular particles.

[0095] A3.2. A membrane module as described in paragraph A3.1, wherein the graphite framework component contains at least 0.001 wt% particulate particles.

[0096] A4. A membrane module as described in any of paragraphs A3 to A3.2, wherein the granular particles of the graphite framework component are fine granular particles, which consist of granular particles having a maximum size of up to 400 micrometers.

[0097] A4.1. The membrane module of paragraph A4, wherein the fine particulate particles are composed of particulate particles having a maximum size, the maximum size being at least one of up to 300 micrometers, up to 200 micrometers, up to 150 micrometers, up to 100 micrometers, up to 80 micrometers, up to 60 micrometers, up to 40 micrometers, up to 20 micrometers, up to 10 micrometers, up to 5 micrometers, up to 1 micrometer, up to 0.5 micrometers, and up to 0.2 micrometers.

[0098] A4.2 The membrane module as described in paragraph A4.1, wherein the maximum size of the fine particulate particles is at least 0.1 micrometers.

[0099] A5. A membrane module as described in any of paragraphs A3 to A4.2, wherein the particulate matter comprises one or more of ash, MgO, Al2O3, SiO2, CaO, and Fe2O3.

[0100] A6. A membrane module as described in any of paragraphs A1 to A5, wherein each of the gas-mixing side frame component, the permeate side frame component, and the graphite frame component contains sulfur.

[0101] A6.1. The membrane module as described in paragraph A6, wherein the graphite frame component contains at least one of up to 450 ppm sulfur, up to 400 ppm sulfur, up to 350 ppm sulfur, up to 300 ppm sulfur, up to 250 ppm sulfur, up to 200 ppm sulfur, up to 100 ppm sulfur, up to 50 ppm sulfur, and up to 20 ppm sulfur.

[0102] A6.2. A membrane module as described in paragraph A6.1, wherein the graphite frame component contains at least 1 ppm sulfur.

[0103] A7. A membrane module as described in any of paragraphs A1 to A6.2, wherein the permeate-side frame component, the mixed gas-side frame component, and the graphite frame component comprise a halide.

[0104] A7.1. The membrane module as described in paragraph A7, wherein the graphite frame component comprises at least one of up to 100 ppm halide, up to 80 ppm halide, up to 60 ppm halide, up to 40 ppm halide, up to 20 ppm halide, up to 10 ppm halide, and up to 1 ppm halide.

[0105] A7.2. A membrane module as described in paragraph A7.1, wherein the graphite frame component contains at least 0.2 ppm of halide.

[0106] A7.3. A membrane module as described in any of paragraphs A7 to A7.2, wherein the halide comprises one or more of a chloride and a bromide.

[0107] A8. A membrane module as described in any of paragraphs A1 to A7.3, wherein the gas-mixing side frame component is configured to form a fluid seal with the peripheral region of the gas-mixing surface of the hydrogen-selective membrane and a peripheral region of a feed assembly.

[0108] A8.1. A membrane module as described in any of paragraphs A1 to A8, wherein the permeate-side frame component is configured to form a fluid seal with the peripheral region of the permeate surface of the hydrogen-selective membrane.

[0109] A9. A membrane module as described in any of paragraphs A1 to A8.1, wherein the permeate-side frame component is configured to support the peripheral region of the permeate surface of the hydrogen-selective membrane.

[0110] A9.1 A membrane module as described in any of paragraphs A1 to A9, wherein the gas-mixing side frame component is configured to support the peripheral region of the gas-mixing surface of the hydrogen-selective membrane and one / one / the peripheral region of the feed assembly.

[0111] A10. A membrane module as described in any of paragraphs A1 to A9.1, wherein one / the membrane contact surface of the graphite frame component is a smooth surface, and wherein the smooth surface is configured to form a non-perforated fluid seal with the hydrogen-selective membrane.

[0112] A11. A membrane module as described in any of paragraphs A1 through A10, wherein the hydrogen-selective membrane is compressed against the mixed gas-side frame component and the permeate-side frame component by a pressure of at least one of the following: at least 2000 psi (13.8 MPa), at least 2900 psi (20 MPa), at least 3000 psi (20.7 MPa), at least 3200 psi (22.1 MPa), at least 3400 psi (23.4 MPa), at least 3600 psi (24.8 MPa) and / or at most 3100 psi (21.4 MPa), at most 3200 psi (22.1 MPa), at most 3600 psi (24.8 MPa), at most 3700 psi (25.5 MPa), at most 3800 psi (26.2 MPa) and at most 4000 psi (27.6 MPa).

[0113] A12. A membrane module as described in any of paragraphs A1 to A11, wherein the hydrogen-selective membrane has a membrane thickness, and wherein the membrane thickness is at least one of at most 25 micrometers, at most 20 micrometers, at most 15 micrometers, at most 10 micrometers, at most 5 micrometers, at least 1 micrometer, at least 2 micrometers, at least 4 micrometers, at least 6 micrometers, at least 8 micrometers, at least 10 micrometers, and at least 12 micrometers.

[0114] A12.1. A membrane module as described in any of paragraphs A1 to A12, wherein the hydrogen-selective membrane is formed from at least one of the following: a metal, a noble metal, a metal alloy, a binary alloy, a ternary alloy, palladium, a palladium alloy, a palladium-copper (Pd-Cu) alloy, a palladium-yttrium alloy, and a palladium-ruthenium alloy.

[0115] A12.2. The membrane module as described in paragraph A12.1, wherein the hydrogen-selective membrane comprises the Pd-Cu alloy, and wherein the Pd-Cu alloy has a copper composition having at least one of the following: at least 15 wt%, at least 20 wt%, at least 25 wt%, at least 30 wt%, at least 35 wt%, at least 40 wt%, at least 45 wt%, at least 50 wt%, and / or at most 60 wt%, at most 55 wt%, at most 53 wt%, at most 50 wt%, at most 45 wt%, at most 40 wt%, at most 35 wt%, at most 30 wt%, and at most 25 wt%.

[0116] A12.3 A membrane module as described in any of paragraphs A1 to A12.1, wherein the fluid-permeable support structure comprises one or more of a sieve structure, one or more mesh sieves, one or more fine mesh sieves, and one or more coarse mesh sieves.

[0117] A13. A membrane module as described in any of paragraphs A1 to A12.3, wherein a thickness of the permeate-side frame component is less than a thickness of the mixed gas-side frame component.

[0118] A13.1. The membrane module as described in paragraph A13, wherein the thickness of the permeate-side frame component is less than 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 52%, 50%, or 45% of the thickness of the mixed gas-side frame component.

[0119] A14. A membrane module as described in any of paragraphs A1 to A13, wherein the permeate-side frame component has a permeate-side frame component density, and further wherein the mixed-gas-side frame component has a mixed-gas-side frame component density less than a threshold fraction of the permeate-side frame component density, wherein the threshold fraction is 95%, 90%, 85%, 80%, 78%, 75%, 70%, or 65%.

[0120] A15. A membrane module as described in any of paragraphs A1 to A11, wherein a density of the graphite framework component is at least one of the following:

[0121] (i) at least 0.7 g / cc, at least 0.8 g / cc, at least 0.9 g / cc, at least 1 g / cc, at least 1.1 g / cc, at least 1.2 g / cc, at least 1.3 g / cc, at least 1.4 g / cc, and at least 1.5 g / cc; and

[0122] (ii) up to 1.8 g / cc, up to 1.7 g / cc, up to 1.6 g / cc, up to 1.5 g / cc, up to 1.4 g / cc, up to 1.3 g / cc, up to 1.2 g / cc, up to 1.1 g / cc and up to 1 g / cc.

[0123] A16. A membrane module as described in any of paragraphs A1 to A15, wherein the at least one membrane unit comprises a pair of hydrogen-selective membranes, wherein the hydrogen-selective membrane is a first hydrogen-selective membrane of the pair, wherein the permeate surface is a first permeate surface and the gas-mixed surface is a first gas-mixed surface, the gas-mixed side frame member is a first gas-mixed side frame member, and the permeate side frame member is a first permeate side frame member, wherein the at least one membrane unit further comprises:

[0124] (i) A second hydrogen-selective membrane in the pair of hydrogen-selective membranes, wherein the second hydrogen-selective membrane defines a second permeate surface and an opposing second mixed gas surface, wherein the fluid-permeable support structure is positioned between the first hydrogen-selective membrane and the second hydrogen-selective membrane such that the fluid-permeable support structure substantially contacts at least the central region of the first permeate surface and at least the central region of the second permeate surface, and also such that the central region of the first permeate surface is spaced apart from the central region of the second permeate surface;

[0125] (ii) a second permeate-side frame member inserted between the second hydrogen-selective membrane and the fluid-permeable support structure, such that the second permeate-side frame member substantially contacts a peripheral region of the second permeate surface and the peripheral region of the fluid-permeable support structure; and

[0126] (iii) A second gas-mixing side frame component that substantially contacts a peripheral area of ​​the second gas-mixing surface.

[0127] A16.1. The membrane module as described in paragraph A16, wherein the second permeate-side frame member supports the peripheral region of the second permeate surface and the peripheral region of the fluid-permeable support structure.

[0128] A16.2. A membrane module as described in any of paragraphs A16 to A16.1, wherein the second permeate-side frame component forms a fluid seal with the peripheral region of the second permeate surface and the peripheral region of the fluid-permeable support structure.

[0129] A16.3 A membrane module as described in any of paragraphs A16 to A16.2, wherein the second gas-mixing side frame component forms a fluid seal with the peripheral region of the second gas-mixing surface.

[0130] A16.4. A membrane module as described in any of paragraphs A16 to A16.3, wherein a second gas-mixing side frame member supports a peripheral region of the second gas-mixing surface.

[0131] A17. A membrane module as described in any of paragraphs A16 to A16.4, wherein at least one of the second permeate-side frame component and the second mixed gas-side frame component is the graphite frame component.

[0132] A18. A membrane module as described in any of paragraphs A1 to A17, wherein the membrane module comprises multiple membrane units.

[0133] A18.1. A membrane module as described in paragraph A18, wherein the plurality of membrane units include a stack of membrane units, and wherein the membrane module includes a corresponding feed plate assembly positioned between each adjacent pair of membrane units in the stack of membrane units.

[0134] A19. A hydrogen purifier comprising a membrane module as described in any of paragraphs A1 to A18.1, wherein the hydrogen purifier is configured to receive a mixed gas stream comprising hydrogen and one or more other gases and to separate the mixed gas stream into a purified hydrogen stream and a byproduct stream.

[0135] A19.1. The membrane module of paragraph A19, wherein the hydrogen selective membrane separates the hydrogen separation membrane module into a mixed gas region and a permeate region, wherein the membrane module is configured to receive the mixed gas stream in the mixed gas region, and wherein the hydrogen selective membrane is configured to allow hydrogen contained in the mixed gas stream to diffuse through the hydrogen selective membrane to the permeate region to separate the mixed gas stream into the purified hydrogen stream and the byproduct stream, and wherein the purified hydrogen stream is the portion of the mixed gas stream diffused through the hydrogen selective membrane.

[0136] A20. A fuel processor comprising:

[0137] A hydrogen production zone, configured to receive a feed stream and generate a / from the feed stream a mixed gas stream; and

[0138] A hydrogen purifier comprising a membrane module as described in any of paragraphs A1 to A19.1, wherein the membrane module is configured to receive the mixed gas stream and separate the mixed gas stream into one / the purified hydrogen stream and one / the byproduct stream.

[0139] A21. A fuel processor as described in paragraph A20, wherein the hydrogen-producing region includes a recombining region containing a recombining catalyst.

[0140] A22. A fuel processing system comprising a fuel processor as described in any of paragraphs A20 to A21, wherein the fuel processing system further comprises a feed stream delivery system configured to supply the feed stream to the hydrogen-producing region.

[0141] A23. An assembly that produces and consumes hydrogen, comprising a fuel processing system as described in paragraph A22; and

[0142] A fuel cell stack, wherein the fuel cell stack is configured to receive the purified hydrogen flow from the fuel processor and generate an electric current from the purified hydrogen flow.

[0143] A24. The hydrogen-generating and hydrogen-consuming assembly as described in paragraph A23 further includes an energy-consuming device configured to receive the current from the fuel cell stack.

[0144] Industrial applicability

[0145] The hydrogen purifiers, fuel processors, fuel processing systems, and assemblies that generate and consume hydrogen disclosed in this article are applicable to hydrogen production and energy production industries, including the fuel cell industry.

[0146] Where any patent, patent application or other reference is incorporated herein by reference and (1) defines a term in a manner that is inconsistent with and / or (2) otherwise inconsistent with the non-incorporated portion of the invention or any other incorporated reference, the non-incorporated portion of the invention shall be controlled and the terms therein or incorporated disclosures shall be controlled only with respect to the references that define the terms and / or the originally presented incorporated disclosures.

[0147] It is believed that the above disclosures cover multiple distinct inventions with independent utility. While each of these inventions has been disclosed in a preferred form, the specific embodiments disclosed and described herein are not intended to be limiting, as numerous 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 attributes disclosed herein. Similarly, where the claims refer to "a" or "a first" element or its equivalents, these claims should be understood to include one or more such elements, neither requiring nor excluding two or more such elements.

[0148] As used herein, when modifying degree or relation, "at least substantially" includes not only the stated "substantial" degree or relation, but also the entire range of the stated degree or relation. A substantial number of stated degrees or relations may include at least 75% of the stated degree or relation. For example, an object formed at least substantially of a material includes an object in which at least 75% of the object is formed of that material, and also includes an object formed entirely of that material. As another example, a first direction at least substantially parallel to a second direction includes a first direction forming an angle of at most 22.5 degrees with respect to the second direction, and also includes a first direction completely parallel to the second direction. As another example, a first length substantially equal to a second length includes a first length that is at least 75% of the second length, a first length equal to the second length, and a first length exceeding the second length such that the second length is at least 75% of the first length.

[0149] It is believed that, as specifically indicated in the following claims, certain combinations and sub-combinations are novel and non-obvious to one of the disclosed inventions. Inventions embodied in other combinations and sub-combinations of features, functions, elements, and / or attributes may be claimed by amending the current claims or presenting new claims in this or related applications. Such amended or new claims, whether for different or the same invention, and regardless of whether their scope differs from, is broader than, narrower than, or equal to the scope of the original claims, are also considered to be included within the subject matter of the invention.

Claims

1. A hydrogen purifier comprising a hydrogen separation membrane module, the membrane module comprising: At least one membrane unit comprising: (i) A hydrogen-selective membrane that defines a permeate surface and an opposing mixed gas surface; (ii) A fluid-permeable support structure that substantially contacts and supports at least a central region of the permeable surface; (iii) A permeate-side frame component inserted between the hydrogen-selective membrane and the fluid-permeable support structure, such that the permeate-side frame component substantially contacts a peripheral area of ​​the permeate surface and a peripheral area of ​​the fluid-permeable support structure. (iv) A gas-mixing side frame component that substantially contacts a peripheral region of the gas-mixing surface of the hydrogen-selective membrane; and At least one of the permeate-side frame component and the mixed-gas-side frame component is a graphite frame component; and The graphite framework component comprises granular particles having a non-graphite component, wherein the granular particles consist of granular particles having a maximum size of up to 400 micrometers and at least 0.01 micrometers.

2. The hydrogen purifier of claim 1, wherein the graphite frame component contains at least 99 wt% carbon.

3. The hydrogen purifier as claimed in claim 1, wherein the mixed gas side frame component is the graphite frame component.

4. The hydrogen purifier as claimed in claim 1, wherein the permeate-side frame component is the graphite frame component.

5. The hydrogen purifier as claimed in claim 1, wherein the mixed gas side frame component and the permeate side frame component are graphite frame components.

6. The hydrogen purifier of claim 1, wherein the graphite frame component comprises at least 99.8 wt% carbon and at most 99.999 wt% carbon.

7. The hydrogen purifier of claim 1, wherein the graphite frame component is a flexible graphite frame component.

8. The hydrogen purifier of claim 1, wherein the graphite frame component comprises at least 0.001 wt% particulate matter, and wherein the graphite frame component comprises at most 1 wt% particulate matter.

9. The hydrogen purifier of claim 8, wherein the particulate matter comprises one or more of ash, MgO, Al2O3, SiO2, CaO and Fe2O3.

10. The hydrogen purifier of claim 1, wherein the graphite frame component contains at least 1 ppm sulfur, and wherein the graphite frame component contains at most 450 ppm sulfur.

11. The hydrogen purifier of claim 1, wherein the graphite frame component comprises a halide, wherein the graphite frame component comprises at least 0.2 ppm of halide, and wherein the graphite frame component comprises at most 100 ppm of halide.

12. The hydrogen purifier of claim 1, wherein the graphite frame component includes a membrane contact surface that substantially contacts and supports the peripheral region of the hydrogen selective membrane, wherein the membrane contact surface of the graphite frame component includes a surface roughness having a maximum amplitude of at least 0.01 micrometers and at most 400 micrometers.

13. The hydrogen purifier of claim 1, wherein the hydrogen selective membrane has a membrane thickness, and wherein the membrane thickness is at most 25 micrometers and at least 1 micrometer.

14. The hydrogen purifier of claim 1, wherein the density of the graphite frame component is at least 0.7 g / cc; and at most 1.8 g / cc.

15. The hydrogen purifier of claim 1, wherein the permeate-side frame member supports the peripheral region of the hydrogen selective membrane, and further wherein the gas-mixing-side frame member forms a fluid seal with the peripheral region of the gas-mixing surface of the hydrogen selective membrane.

16. The hydrogen purifier of claim 1, wherein the at least one membrane unit comprises a pair of hydrogen-selective membranes, wherein the hydrogen-selective membrane is a first hydrogen-selective membrane of the pair, wherein the permeate surface is a first permeate surface and the gas-mixed surface is a first gas-mixed surface, the gas-mixed side frame member is a first gas-mixed side frame member, and the permeate side frame member is a first permeate side frame member, wherein the at least one membrane unit further comprises: (i) A second hydrogen-selective membrane in the pair of hydrogen-selective membranes, wherein the second hydrogen-selective membrane defines a second permeate surface and an opposing second mixed gas surface, wherein the fluid-permeable support structure is positioned between the first hydrogen-selective membrane and the second hydrogen-selective membrane such that the fluid-permeable support structure substantially contacts at least the central region of the first permeate surface and at least the central region of the second permeate surface, and also such that the central region of the first permeate surface is spaced apart from the central region of the second permeate surface; (ii) A second permeate-side frame member inserted between the second hydrogen-selective membrane and the fluid-permeable support structure, such that the second permeate-side frame member substantially contacts a peripheral region of the second permeate surface and the peripheral region of the fluid-permeable support structure. (iii) A second gas-mixing side frame component, which substantially contacts a peripheral area of ​​the second gas-mixing surface; and At least one of the second permeate-side frame component and the second mixed gas-side frame component is the graphite frame component.

17. The hydrogen purifier of claim 16, wherein the second permeate-side frame member supports the peripheral region of the second permeate surface and the peripheral region of the fluid-permeable support structure, and further wherein the second mixed-gas-side frame member and the peripheral region of the second mixed-gas surface form a fluid seal.

18. The hydrogen purifier of claim 1, wherein the membrane module comprises a plurality of membrane units.

19. The hydrogen purifier of claim 1, wherein the hydrogen purifier is configured to receive a mixed gas stream comprising hydrogen and one or more other gases and to separate the mixed gas stream into a purified hydrogen stream and a byproduct stream, wherein the hydrogen selective membrane separates the hydrogen separation membrane module into a mixed gas region and a permeate region, wherein the membrane module is configured to receive the mixed gas stream in the mixed gas region, and wherein the hydrogen selective membrane is configured to allow hydrogen contained in the mixed gas stream to diffuse through the hydrogen selective membrane to the permeate region to separate the mixed gas stream into the purified hydrogen stream and the byproduct stream, and wherein the purified hydrogen stream is the portion of the mixed gas stream diffused through the hydrogen selective membrane.

20. A fuel processor comprising: A hydrogen production zone, configured to receive a feed stream and generate a mixed gas stream from the feed stream; and The hydrogen purifier of claim 19, wherein the membrane module is configured to receive the mixed gas stream and separate the mixed gas stream into the purified hydrogen stream and the byproduct stream.

21. The hydrogen purifier of claim 1, wherein the particulate particles have a hardness greater than a remainder of the hardness of the graphite frame component.

22. The hydrogen purifier of claim 1, wherein the granular particles of the graphite frame component are fine granular particles, wherein the fine granular particles produce a lower surface roughness in the graphite frame component compared to a coarse granular particle.

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