KR102566860B1 - Hydrogen purification devices - Google Patents

Abstract

A hydrogen purification device and components thereof are disclosed. In some embodiments, the device may include at least one foil-to-microscreen assembly disposed between and secured to the first end frame and the second end frame. At least one foil-microscreen assembly can include at least one microscreen structure comprising at least one hydrogen-selective membrane and a non-porous planar sheet having a plurality of apertures defining a plurality of fluid passageways. A planar sheet may include generally opposed planar surfaces configured to provide support to the permeate side. A plurality of fluid passages may extend between the opposing surfaces. At least one hydrogen-selective membrane may be metallurgically bonded to the at least one microscreen structure. In some embodiments, the device may include a transmission frame having at least one membrane support structure spanning at least a substantial portion of the open area and configured to support at least one foil-microscreen assembly.

Description

Hydrogen purification device {HYDROGEN PURIFICATION DEVICES}

CROSS REFERENCES TO RELATED APPLICATIONS

This application is a continuation-in-part of U.S. Patent Application Serial No. 13/600,096, filed on August 30, 2012, entitled "Hydrogen Generation Assemblies," filed on March 14, 2013, and entitled "Hydrogen Generation Assemblies and Hydrogen U.S. Patent Application Serial No. 13/829,766, "Purification Devices", a continuation-part of a U.S. patent application currently granted as U.S. Patent No. 9,187,324, U.S. Patent Application filed January 4, 2018, entitled "Hydrogen Purification Devices" Priority is claimed to No. 15/862,474. The entire disclosure of the foregoing application is hereby incorporated by reference for all purposes.

A hydrogen generating assembly is an assembly that converts one or more feedstocks into a product stream comprising hydrogen gas as a major component. The feedstock may include a carbon-containing feedstock and, in some embodiments, may also include water. The feedstock is delivered from the feedstock delivery system to the hydrogen-producing region of the hydrogen-producing assembly, typically the feedstock is delivered under pressure and at an elevated temperature. The hydrogen-producing region is often associated with a temperature control assembly, such as a heating assembly or a cooling assembly, which temperature control assembly is one to maintain the hydrogen-producing region within a suitable temperature range for efficiently producing hydrogen gas. consumes more than one fuel stream. The hydrogen generating assembly may produce hydrogen gas through any suitable mechanism(s), such as steam reforming, autothermal reforming, pyrolysis, and/or catalytic partial oxidation.

However, the produced or produced hydrogen gas may have impurities. Such a gas may be referred to as a mixed gas stream comprising hydrogen gas and other gases. Prior to use of the mixed gas stream, the mixed gas stream must be purified, eg to remove at least some of the other gases. Accordingly, the hydrogen generating assembly may include a hydrogen purification device for increasing the hydrogen purity of the mixed gas stream. The hydrogen refinery can include at least one hydrogen-selective membrane for separating the mixed gas stream into a product stream and a byproduct stream. The product stream includes a higher concentration of hydrogen gas and/or one or more other gases from the lower concentration of the mixed gas stream. Hydrogen purification using one or more hydrogen-selective membranes is a pressure-driven separation process in which one or more hydrogen-selective membranes are housed within a pressure vessel. The mixed gas stream is contacted with the mixed gas surface of the membrane(s), and a product stream is formed from at least a portion of the mixed gas stream that has permeated the membrane(s). Pressure vessels are typically sealed to prevent gases from entering or leaving the pressure vessel, except through prescribed inlet and outlet ports or conduits.

The product stream can be used in a variety of applications. One such use is energy production, such as in electrochemical fuel cells. An electrochemical fuel cell is a device that converts fuel and oxidant into electricity, reaction products, and heat. For example, fuel cells can convert hydrogen and oxygen into water and electricity. In such a fuel cell, hydrogen is the fuel, oxygen is the oxidizing agent, and water is the reaction product. A fuel cell stack includes a plurality of fuel cells and can be used in conjunction with a hydrogen generating assembly to provide an energy producing assembly.

Hydrogen generating assemblies, hydrogen processing assemblies, and/or components of such assemblies are described in U.S. Patent Nos. 5,861,137; 6,319,306; 6,494,937; 6,562,111; 7,063,047; 7,306,868; 7,470,293; 7,601,302; 7,632,322; No. 8,961,627; and US Patent Application Publication Nos. 2006/0090397; 2006/0272212; 2007/0266631; 2007/0274904; 2008/0085434; 2008/0138678; 2008/0230039; and 2010/0064887. The entire disclosures of the foregoing patents and patent application publications are incorporated herein by reference for all purposes.

Some embodiments may provide a hydrogen purification device. In some embodiments, a hydrogen refinery device may include first and second end frames including inlet ports configured to receive a mixed gas stream comprising hydrogen gas and another gas. the first and second end frames comprising an exhaust port configured to receive a permeate stream comprising at least one of a higher concentration of hydrogen gas and a lower concentration of other gases than the mixed gas stream, and at least a substantial portion of the other gases; It may additionally include a byproduct port configured to receive a byproduct stream. The hydrogen purification device additionally includes at least one foil-microscreen assembly disposed between and secured between the first end frame and the second end frame. At least one foil-microscreen assembly includes at least one hydrogen-selective membrane having a feed side and a permeate side. At least a portion of the permeate stream is formed from a portion of the mixed gas stream passing from the feed side to the permeate side, and the remaining portion of the mixed gas stream remaining on the feed side forms at least a portion of the byproduct stream.

The at least one foil-microscreen assembly additionally includes at least one microscreen structure comprising a non-porous planar sheet having a plurality of apertures defining a plurality of fluid passageways. A planar sheet includes generally opposed planar surfaces configured to provide support to the permeate side. A plurality of fluid passages extend between the opposing surfaces. At least one hydrogen-selective membrane is metallurgically bonded to the at least one microscreen structure. The hydrogen purification apparatus further includes a plurality of frames disposed between the first end frame and the second end frame and the at least one foil-microscreen assembly and secured to the first and second end frames. Each frame of the plurality of frames includes a perimeter shell defining an open area.

In some embodiments, a hydrogen refinery device may include first and second end frames including inlet ports configured to receive a mixed gas stream comprising hydrogen gas and another gas. the first and second end frames comprising an exhaust port configured to receive a permeate stream comprising at least one of a higher concentration of hydrogen gas and a lower concentration of other gases than the mixed gas stream, and at least a substantial portion of the other gases; It may additionally include a byproduct port configured to receive a byproduct stream. The hydrogen purification device additionally includes at least one foil-microscreen assembly disposed between and secured to the first end frame and the second end frame. The at least one foil-microscreen assembly includes at least one hydrogen-selective membrane having a feed side and a permeate side. At least a portion of the permeate stream is formed from a portion of the mixed gas stream passing from the feed side to the permeate side, and the remaining portion of the mixed gas stream remaining on the feed side forms at least a portion of the byproduct stream. The at least one foil-microscreen assembly additionally includes at least one microscreen structure, the microscreen structure having generally opposing planar surfaces configured to provide support to the permeate side, and opposing surfaces. and a plurality of fluid passages extending therebetween. At least one hydrogen-selective membrane is metallurgically bonded to the at least one microscreen structure.

The hydrogen purification apparatus further includes a plurality of frames disposed between the first end frame and the second end frame and the at least one foil-microscreen assembly and secured to the first and second end frames. The plurality of frames includes at least one transmission frame disposed between at least one foil-microscreen assembly and the second end frame. The at least one permeate frame includes a perimeter shell and an exhaust conduit, the exhaust conduit formed on the perimeter shell and configured to receive at least a portion of the permeate stream from the at least one hydrogen-selective membrane. The at least one permeable frame additionally includes an open area surrounded by a perimeter shell, and at least one membrane support structure spanning at least a substantial portion of the open area and configured to support the at least one foil-microscreen assembly. . At least one membrane support structure is not perforated.

Some embodiments may provide a foil-microscreen assembly. The foil-microscreen assembly can include at least one hydrogen-selective membrane having a feed side and a permeate side. The at least one hydrogen-selective membrane is configured to receive a mixed gas stream, to form a permeate stream from a portion of the mixed gas stream passing from the feed side to the permeate side, and to form a byproduct stream from a remaining portion of the mixed gas stream remaining on the feed side. can be configured. The foil-microscreen assembly may additionally include at least one microscreen structure comprising a non-porous planar sheet having a plurality of openings defining a plurality of fluid passageways. A planar sheet may include generally opposed planar surfaces configured to provide support to the permeate side. A plurality of fluid passages may extend between the opposing surfaces. The permeate side of the at least one hydrogen-selective membrane may be metallurgically bonded to the at least one microscreen structure.

1 is a schematic diagram of an example of a hydrogen generating assembly.
2 is a schematic diagram of another example of a hydrogen generating assembly.
3 is a schematic diagram of a hydrogen purification device of the hydrogen generating assembly of FIG. 1;
4 is an exploded isometric view of an example of the hydrogen purification device of FIG. 3;
FIG. 5 is a top view of an example of a foil-microscreen assembly of the hydrogen purification device of FIG. 4;
FIG. 6 is a top view of an example of a microscreen structure of the foil-microscreen assembly of FIG. 5;
7 is a partial view of the microscreen structure of FIG. 6 with another example of an aperture.
8 is a partial view of the microscreen structure of FIG. 6 with another example of an aperture.
9 is a partial view of the microscreen structure of FIG. 6 with additional examples of apertures.
FIG. 10 is a top view of another example of a foil-microscreen assembly of the hydrogen purification device of FIG. 4;
11 is a top view of an example of a microscreen structure of the foil-microscreen assembly of FIG. 10;
12 is a top view of another example of a foil-microscreen assembly of the hydrogen purification device of FIG. 4;
FIG. 13 is a top view of a further example of a foil-microscreen assembly of the hydrogen purification device of FIG. 4;
14 is a partial cross-sectional view of an example of a permeate frame, foil-microscreen assembly, gasket frame, and feed frame of the hydrogen purification apparatus of FIG. 4, shown without a gasket frame between the foil-microscreen assembly and the permeate frame.
FIG. 15 is a top view of the hydrogen purification apparatus of FIG. 4 showing an example of a perimeter shell of the permeation frame and a membrane supporting structure of the permeation frame.
FIG. 16 is a partial cross-sectional view of another example of a peripheral shell of a transmission frame of the hydrogen purification device of FIG. 4 .
17 is an isometric view of an example of a membrane support plate of a membrane support structure of a permeation frame of the hydrogen purification apparatus of FIG. 4;
18 is an isometric view of another example of a membrane support plate of a membrane support structure of a permeation frame of the hydrogen purification device of FIG. 4;
19 is a cross-sectional view of another example of a membrane support structure of the hydrogen purification device of FIG. 4 .
20 is an exploded isometric view of another example of the hydrogen purification device of FIG. 3 .

1 shows an example of a hydrogen generating assembly 20 . Unless specifically excluded otherwise, hydrogen generating assembly 20 may include one or more components of other hydrogen generating assemblies described in this disclosure. The hydrogen generating assembly may include any suitable structure configured to produce product hydrogen stream 21 . For example, a hydrogen generating assembly may include a feedstock delivery system 22 and a fuel processing assembly 24 . The feedstock delivery system may include any suitable structure configured to selectively deliver at least one feed stream 26 to a fuel processing assembly.

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

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

In some embodiments, the feedstock delivery system 22 is a hydrogen-producing fluid 30, comprising a mixture of water and a carbon-containing feedstock miscible with water (such as methanol and/or other water soluble alcohols). It can be configured to deliver. The ratio of water to carbon-containing feedstock in such a fluid stream can be determined by one or more factors, such as the specific carbon-containing feedstock used, user preference, design of the fuel processing assembly, and fuel processing assembly to produce the product hydrogen stream. may vary depending on the mechanism(s) used by the For example, the molar ratio of water to carbon may be from about 1:1 to 3:1. Also, a mixture of water and methanol may be delivered in a 1:1 molar ratio or about a 1:1 molar ratio (37 wt% water, 63 wt% methanol), while a mixture of hydrocarbons or other alcohols may be delivered in a molar ratio greater than 1:1. It can be delivered in a water-to-carbon molar ratio.

When fuel processing assembly 24 produces product hydrogen stream 21 through reforming, feed stream 26 may contain, for example, from about 25 to 75% by volume methanol or ethanol (or other suitable water-miscible liquid). carbon-containing feedstock) and about 25 to 75% by volume of water. In a feed stream comprising at least a substantial amount of methanol and water, such a stream may comprise about 50 to 75 vol % methanol and about 25 to 50 vol % water. A stream comprising ethanol or other water-miscible alcohol may contain about 25 to 60 vol % alcohol and about 40 to 75 vol % water. An example of a feed stream for a hydrogen generating assembly 20 utilizing steam reforming or autothermal reforming includes 69 vol % methanol and 31 vol % water.

Although feedstock delivery system 22 is shown as being configured to deliver a single feed stream 26, the feedstock delivery system may be configured to deliver more than one feed stream 26. These streams may include the same or different feedstocks, and may have different compositions, at least one common component, disjoint components, or the same composition. For example, a first feed stream can include a first component, such as a carbon-containing feedstock, and a second feed stream can include a second component, such as water. Further, although feedstock delivery system 22 may be configured to deliver a single fuel stream 28, in some embodiments, the feedstock delivery system may be configured to deliver more than one fuel stream. The fuel streams may have different compositions, at least one common component, disjoint components, or the same composition. Additionally, the feed stream and fuel stream may be discharged from the feedstock delivery system in different phases. For example, one of the streams may be a liquid stream while the other stream is a gas stream. In some embodiments, both streams may be liquid streams, while in other embodiments both streams may be gas streams. Additionally, although the hydrogen generating assembly 20 is shown as including a single feedstock delivery system 22, the hydrogen generating assembly may include more than one feedstock delivery system 22.

The fuel processing assembly 24 may include a hydrogen-producing region 32 configured to produce an exhaust stream 34 comprising hydrogen gas via any suitable hydrogen-producing mechanism(s). The effluent stream may include hydrogen gas as at least a major component and may include additional gaseous component(s). As such, effluent stream 34 may be referred to as a "mixed gas stream" comprising hydrogen gas as a major component, but also containing other gases.

Hydrogen-producing zone 32 may include any suitable catalyst-containing bed or zone. When the hydrogen-producing mechanism is steam reforming, the hydrogen-producing section is configured to facilitate production of effluent stream(s) 34 from feed stream(s) 26 comprising carbon-containing feedstock and water. A suitable steam reforming catalyst 36 may be included. In such an embodiment, fuel processing assembly 24 may be referred to as a "steam reformer", hydrogen-producing section 32 may be referred to as a "reforming section", and discharge stream 34 may be referred to as a "reform stream". " can be referred to as Other gases that may be present in the reformate stream may include carbon monoxide, carbon dioxide, methane, steam, and/or unreacted carbon-containing feedstock.

When the hydrogen-producing mechanism is autothermal reforming, hydrogen-producing region 32 generates the outlet stream(s) from feed stream(s) 26 comprising water and carbon-containing feedstock in the presence of air ( 34) may include a suitable autothermal reforming catalyst to promote the production. The fuel processing assembly 24 may also include an air delivery assembly 38 configured to deliver the air stream(s) to the hydrogen-producing region.

In some embodiments, fuel processing assembly 24 may include any suitable structure configured to produce at least one hydrogen-rich stream 42 from exhaust (or mixed gas) stream 34. , purification (or separation) region 40 may be included. Hydrogen-enriched stream 42 may include a higher hydrogen concentration than effluent stream 34 and/or a lowered concentration of one or more other gases (or impurities) that were present in that effluent stream. Product hydrogen stream 21 includes at least a portion of hydrogen-rich stream 42. Thus, product hydrogen stream 21 and hydrogen-enriched stream 42 can be the same stream and have the same composition and flow rate. Alternatively, a portion of the purified hydrogen gas in hydrogen-enriched stream 42 may be stored for later use, such as in a suitable hydrogen storage assembly and/or consumed by a fuel processing assembly. The purifying region 40 may also be referred to as a "hydrogen purification unit" or a "hydrogen processing assembly".

In some embodiments, refining zone 40 may produce at least one byproduct stream 44, which may include no or some hydrogen gas. The byproduct stream may be evacuated, passed to a burner assembly and/or other source of combustion, used as a heated fluid stream, stored for future use, and/or otherwise utilized, stored, and/or or discarded. Further, refining zone 40 may discharge the by-product stream as a continuous stream in response to delivery of effluent stream 34, or, for example, in a batch process or a by-product portion of the effluent stream may be transferred into a refining zone. When maintained at least temporarily at , it may emit such a stream intermittently.

The fuel processing assembly 24 includes one or more refining zones configured to produce one or more byproduct streams comprising a sufficient amount of hydrogen gas suitable for use as a fuel stream (or feedstock stream) for a heating assembly for the fuel processing assembly. can include In some embodiments, the byproduct stream may have sufficient fuel value or hydrogen content to enable the heating assembly to maintain the hydrogen-producing region at a desired operating temperature or within a selected temperature range. For example, the by-product stream may contain hydrogen gas, such as 10 to 30 vol % hydrogen gas, 15 to 25 vol % hydrogen gas, 20 to 30 vol % hydrogen gas, at least 10 or 15 vol % hydrogen gas, It may contain at least 20% by volume of hydrogen gas or the like.

Refining zone 40 may include any suitable structure configured to enrich (and/or increase) the concentration of at least one component of effluent stream 21 . In most applications, hydrogen-enriched stream 42 will have a higher hydrogen concentration than vent stream (or mixed gas stream) 34 . The hydrogen-enriched stream may also have a reduced concentration of one or more non-hydrogen components that were present in the effluent stream 34, and the hydrogen concentration of such hydrogen-enriched stream is greater than, equal to, or less than that of the effluent stream. For example, in a typical fuel cell system, even when present at a few ppm, carbon monoxide can damage the fuel cell stack, while other non-hydrogen components that may be present in the exhaust stream 34. , eg water, even when present in much higher concentrations, will not damage the laminate. Accordingly, in such applications, the refining zone may not increase the overall hydrogen concentration, but will lower the concentration of one or more non-hydrogen components that are detrimental or potentially detrimental to the desired application of the product hydrogen stream.

Examples of suitable devices for refining zone 40 include one or more hydrogen-selective membranes 46 , chemical carbon monoxide removal assembly 48 , and/or pressure swing adsorption (PSA) system 50 . Refining region 40 may include more than one type of purification device, and such devices may have the same or different structures and/or may be operated by the same or different mechanism(s). The fuel processing assembly 24 includes, for example, at least one restricting orifice and/or other flow associated with one or more product hydrogen stream(s), hydrogen-rich stream(s), and/or byproduct stream(s). Restrictions may be included downstream of the purifying region(s).

Hydrogen-selective membrane 46 is permeable to hydrogen gas, but at least substantially (or completely) impermeable to other components of effluent stream 34 . Membrane 46 may be formed of any hydrogen-permeable material suitable for use in the operating environment and parameters in which purification region 40 is operated. Examples of suitable materials for the membrane 46 include palladium and palladium alloys, and particularly thin films of such metals and metal alloys. Palladium alloys, especially palladium with 35% to 45% copper by weight, have proven particularly effective. A palladium-copper alloy containing about 40% copper by weight has proven particularly effective, although other relative concentrations and compositions may be used. As three other particularly efficient alloys, palladium with 2% to 20% gold by weight, in particular palladium with 5% gold by weight; palladium having from 3% to 10% indium plus 0% to 10% ruthenium, in particular palladium having 6% indium plus 0.5% ruthenium; and palladium with 20% to 30% silver by weight. When palladium and palladium alloys are used, the hydrogen-selective membrane 46 may sometimes be referred to as a "foil". A typical thickness of the hydrogen-permeable metal foil is less than 25 microns (microns), preferably less than 15 microns, and most preferably between 5 and 12 microns. The foil may be of any suitable dimension, such as 110 mm x 270 mm.

The chemical carbon monoxide removal assembly 48 is a device that chemically reacts the carbon monoxide and/or other undesirable components of the effluent stream 34 to form other potentially harmless compositions. Examples of chemical carbon monoxide removal assemblies include a water-gas shift reactor configured to produce hydrogen gas and carbon dioxide from water and carbon monoxide, a partial oxidation reactor configured to convert carbon monoxide and oxygen (usually from air) to carbon dioxide, and carbon monoxide and hydrogen. A methanation reactor configured to convert to methane and water. The fuel processing assembly 24 may include more than one type and/or number of chemical removal assemblies 48 .

Pressure Swing Adsorption (PSA) is a chemical process by which gaseous impurities are removed from the effluent stream 34 based on the principle that certain gases are more strongly adsorbed onto an adsorbent material than others under appropriate temperature and pressure conditions. Typically, non-hydrogen impurities are adsorbed and removed from effluent stream 34. Adsorption of impurity gases takes place at elevated pressures. When the pressure is reduced, impurities are desorbed from the adsorbent material, thereby regenerating the adsorbent material. Typically, PSA is a cyclic process and requires at least two beds for continuous operation (as opposed to batch). Examples of suitable adsorbent materials that can be used in adsorption beds include activated carbon and zeolites. The PSA system 50 provides an example of an apparatus for use in a refining section 40 where by-products or removed components are not exhausted directly from the refining section as a gas stream concurrent with purification of the effluent stream. Instead, these by-product components are removed when the adsorbent material is regenerated or otherwise removed from the refining zone.

In FIG. 1 , a refining region 40 is shown within a fuel processing assembly 24 . Alternatively, as shown schematically in FIG. 1 by dashed lines, the refining region may be located separately downstream of the fuel processing assembly. Refining region 40 may also include portions within and outside of the fuel processing assembly.

The fuel processing assembly 24 may also include a temperature regulating assembly in the form of a heating assembly 52 . The heating assembly may be configured to produce at least one heated exhaust stream (or combustion stream) 54 from at least one heating fuel stream 28 when combusted, typically in the presence of air. A heated exhaust stream 54 is shown schematically in FIG. 1 as a heated hydrogen-producing region 32 . Heating assembly 52 may include any suitable structure configured to produce a heated exhaust stream, such as a burner or combustion catalyst in which fuel is combusted with air to produce a heated exhaust stream. The heating assembly may include an igniter or ignition source 58 configured to ignite combustion of fuel. Examples of suitable ignition sources include one or more spark plugs, discharge plugs, combustion catalysts, pilot lights, piezoelectric igniters, spark igniters, hot surface igniters, and the like.

In some embodiments, heating assembly 52 may include burner assembly 60 and may be referred to as a combustion-based or combustion-driven heating assembly. In a combustion-based heating assembly, the heating assembly 52 may be configured to receive at least one fuel stream 28 and to combust the fuel stream in the presence of air to provide a hot combustion stream 54 such that The hot combustion stream can be used to heat at least the hydrogen-producing region of the fuel processing assembly. Air may be delivered to the heating assembly through a variety of mechanisms. For example, air stream 62 may be delivered to the heating assembly as a separate stream, as shown in FIG. 1 . Alternatively or additionally, the air stream 62 may be delivered to the heating assembly along with at least one of the fuel streams 28 for the heating assembly 52 and/or from the environment in which the heating assembly is used. can be withdrawn.

Additionally or alternatively, combustion stream 54 may be used to heat fuel processing assemblies and/or other portions of the fuel cell system that are utilized with the heating assembly. Also, other configurations and types of heating assembly 52 may be used. For example, the heating assembly 52 is configured to heat at least the hydrogen-producing region 32 of the fuel processing assembly 24 by generating heat using at least one heating element, such as a resistive heating element. It may be an electrically powered heating assembly. In such an embodiment, the heating assembly 52 may not receive and combust the combustible fuel stream in order to heat the hydrogen-producing region to a suitable hydrogen-producing temperature. An example of a heating assembly is disclosed in US Pat. No. 7,632,322, the entire disclosure of which is incorporated herein by reference for all purposes.

The heating assembly 52 may be housed within a common shell or housing having a hydrogen-producing region and/or a separation region (as further described below). The heating assembly may be disposed separately with respect to the hydrogen-producing region 32, but may be in thermal and/or fluid communication with such a region to provide desired heating of at least the hydrogen-producing region. The heating assembly 52 may be positioned partially or wholly within the common shell, and/or at least a portion (or all) of the heating assembly may be positioned outside of such a shell. When the heating assembly is positioned outside the shell, the hot combustion gases from the burner assembly 60 may be delivered to one or more components within the shell through a suitable heat transfer conduit.

The heating assembly also heats the feedstock delivery system 22, the feedstock feed stream, the hydrogen-producing section 32, the purification (or separation) section 40, or any suitable combination of such systems, streams, and sections. can be configured to Heating the feedstock feed stream may include evaporating a liquid reactant stream or a component of the hydrogen-producing fluid used to produce hydrogen gas within the hydrogen-producing zone. In such an embodiment, the fuel processing assembly 24 may be described as including a vaporization region 64 . The heating assembly may also be configured to heat other components of the hydrogen generating assembly. For example, the heated exhaust stream is configured to heat a pressure vessel and/or other canister containing heating fuel and/or hydrogen-producing fluid forming at least a portion of feed stream 26 and fuel stream 28. It can be.

Heating assembly 52 may achieve and/or maintain any suitable temperature within hydrogen-producing region 32 . Steam reformers are typically operated at temperatures ranging from 200 °C to 900 °C. However, temperatures outside this range are included within the scope of this disclosure. When the carbon-containing feedstock is methanol, the steam reforming reaction will typically operate in the temperature range of about 200 to 500 °C. Exemplary subsets of such ranges include 350 to 450 °C, 375 to 425 °C, and 375 to 400 °C. When the carbon-containing feedstock is a hydrocarbon, ethanol, or other alcohol, a temperature range of about 400 to 900 °C will typically be used for the steam reforming reaction. Exemplary subsets of such ranges include 750 to 850 °C, 725 to 825 °C, 650 to 750 °C, 700 to 800 °C, 700 to 900 °C, 500 to 800 °C, 400 to 600 °C, and 600 to 800 °C. do. Hydrogen-producing region 32 may include two or more zones or sections, each of which may be operated at the same or different temperatures. For example, when the hydrogen-producing fluid comprises a hydrocarbon, hydrogen-producing region 32 may include two different hydrogen-producing portions or regions, one operating at a lower temperature than the other such that A pre-reformation zone may be provided. In such an embodiment, the fuel processing assembly may also be said to include two or more hydrogen-producing regions.

Fuel stream 28 may include any combustible liquid(s) and/or gas(es) suitable for consumption by heating assembly 52 to provide desired heat release. Some fuel streams, as delivered and combusted by heating assembly 52, may be gaseous, while other fuel streams may be delivered to the heating assembly as liquid streams. Examples of suitable heating fuels for fuel stream 28 include carbon-containing feedstocks such as methanol, methane, ethane, ethanol, ethylene, propane, propylene, butane, and the like. Additional examples include low molecular weight condensable fuels such as liquefied petroleum gas, ammonia, light amines, dimethyl ether, and low molecular weight hydrocarbons. Another example includes hydrogen and carbon monoxide. A hydrogen generating assembly comprising a temperature control assembly in the form of a cooling assembly instead of a heating assembly (as may be used when an exothermic hydrogen-producing process - eg, partial oxidation - is used instead of an endothermic process such as steam reforming) In an embodiment of 20, the feedstock delivery system may be configured to supply a fuel or coolant stream to the assembly. Any suitable fuel or coolant fluid may be used.

The fuel processing assembly 24 may also include a shell or housing 66 within which at least the hydrogen-producing region 32 is received, as shown in FIG. 1 . In some embodiments, evaporation region 64 and/or purification region 40 may also be included within the shell. Shell 66 allows components of a steam reformer or other fuel processing mechanism to be moved as a unit. The shell may also protect components of the fuel processing assembly from damage by providing a protective enclosure and/or may reduce the heating demand of the fuel processing assembly as the components may be heated as a unit. there is. Shell 66 may include an insulating material 68 , such as a solid insulating material, a blanket insulating material, and/or an air-filled cavity. The insulating material may be located inside the shell, outside the shell, or both. When the insulating material is outside the shell, the fuel processing assembly 24 may further include an outer cover or jacket 70 outside the insulating material, as shown schematically in FIG. 1 . The fuel processing assembly may include additional components of the fuel processing assembly, such as feedstock delivery system 22 and/or other shells containing other components.

One or more components of fuel processing assembly 24 may extend beyond the shell or may be located outside of the shell. For example, the refining region 40 may be located outside the shell 66, eg remote from the shell, but may be in fluid communication by a suitable fluid-delivery conduit. As another example, a portion of the hydrogen-producing region 32 (e.g., a portion of one or more reforming catalyst beds) may extend beyond the shell, as schematically indicated by dashed lines in FIG. 1 indicating an alternative shell configuration. can Examples of suitable hydrogen generating assemblies and components thereof are described in U.S. Patent Nos. 5,861,137, the entire disclosure of which is incorporated herein by reference for all purposes; 5,997,594; and 6,221,117.

Another example of a hydrogen generating assembly 20 is shown in FIG. 2 and is generally indicated at 72 . Unless specifically excluded otherwise, hydrogen generating assembly 72 may include one or more components of hydrogen generating assembly 20 . Hydrogen generating assembly 72 may include feedstock delivery system 74 , vaporization zone 76 , hydrogen-producing zone 78 , and heating assembly 80 , as shown in FIG. 2 . In some embodiments, hydrogen generating assembly 20 may also include a refining region 82 .

The feedstock delivery system may include any suitable structure configured to deliver one or more feed streams and/or fuel streams to one or more other components of a hydrogen generating assembly. For example, the feedstock delivery system may include a feedstock tank (or container) 84 and a pump 86 . The feedstock tank may include any suitable hydrogen-producing fluid 88, such as water and a carbon-containing feedstock (eg, methanol/water mixture). Pump 86 may have any suitable structure configured to deliver hydrogen-producing fluid to vaporization region 76 and/or hydrogen-producing region 78, such hydrogen-producing fluid comprising water and carbon-containing It may be in the form of at least one liquid-containing feed stream 90 comprising feedstock.

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

Hydrogen-producing section 78 feeds one or more feed streams, such as vapor feed stream(s) 94, into a vaporization section to produce one or more effluent streams 96 comprising hydrogen gas as the main component and other gases. It may include any suitable structure configured to receive from. The hydrogen-producing region may produce an effluent stream through any suitable mechanism(s). For example, hydrogen-producing section 78 may produce effluent stream(s) 96 via a steam reforming reaction. In such an example, hydrogen-producing section 78 may include steam reforming section 97 having a reforming catalyst 98 configured to assist and/or promote a steam reforming reaction. When hydrogen-producing section 78 produces effluent stream(s) 96 via a steam reforming reaction, hydrogen producing assembly 72 may be referred to as a "steam reforming hydrogen producing assembly" and effluent stream 96 ) may be referred to as the “reform stream”.

The heating assembly 80 may include any suitable structure configured to produce at least one heated exhaust stream 99 for heating one or more other components of the hydrogen generating assembly 72 . For example, the heating assembly may heat the vaporization region to any suitable temperature(s), such as at least a minimum vaporization temperature or a temperature at which at least a portion of the liquid-containing feed stream vaporizes to form a vapor feed stream. Additionally or alternatively, the heating assembly 80 may bring the hydrogen-producing region to any suitable temperature(s), such as at least a minimum hydrogen-producing temperature or at least a portion of the vapor feed stream to react to form an exhaust stream. It can be heated to a temperature that produces hydrogen gas for The heating assembly can be in thermal communication with one or more components of the hydrogen generating assembly, such as a vaporization region and/or a hydrogen-producing region.

The heating assembly, as shown in FIG. 2 , may include a burner assembly 100 , at least one air blower 102 , and an igniter assembly 104 . The burner assembly is configured to receive at least one air stream (106) and at least one fuel stream (108) and to combust the at least one fuel stream within a combustion region (110) to produce a heated exhaust stream (99). It may include any suitable structure configured. A fuel stream may be provided by feedstock delivery system 74 and/or refining zone 82 . The combustion region may be housed within the enclosure of the hydrogen generating assembly. Air blower 102 may include any suitable structure configured to generate air stream(s) 106 . The igniter assembly 104 may include any suitable structure configured to ignite the fuel stream(s) 108 .

Refining zone 82 may include any suitable structure configured to produce at least one hydrogen-rich stream 112, which hydrogen-rich stream has a higher hydrogen concentration than vent stream 96 and/or a corresponding vent. It may contain lowered concentrations of one or more other gases (or impurities) that were present in the stream. The refining section can produce at least one byproduct stream or fuel stream 108, which as shown in FIG. 2 can be passed to burner assembly 100 and fuel for that assembly. Can be used as a stream. The refining region 82 may include a flow restriction orifice 111 , a filter assembly 114 , a membrane assembly 116 , and a methanation reactor assembly 118 . A filter assembly (eg, one or more hot gas filters) may be configured to remove impurities from the effluent stream 96 prior to the hydrogen purification membrane assembly.

Membrane assembly 116 is configured to receive a bleed or mixed gas stream(s) 96 comprising hydrogen gas and other gases, and containing a higher concentration of hydrogen gas and/or a lower concentration of other gases than the mixed gas stream. It may include any suitable structure configured to produce permeate or hydrogen-enriched stream(s) 112 that The membrane assembly 116 may include a planar or tubular hydrogen-permeable (or hydrogen-selective) membrane, and more than one hydrogen-permeable membrane may be incorporated into the membrane assembly 116 . The permeate stream(s) may be used for any suitable application, such as for one or more fuel cells. In some embodiments, the membrane assembly may produce a byproduct or fuel stream 108 that includes at least a significant portion of other gases. Methanation reactor assembly 118 may include any suitable structure configured to convert carbon monoxide and hydrogen to methane and water. Although refining zone 82 is shown as including flow restricting orifice 111, filter assembly 114, membrane assembly 116, and methanation reactor assembly 118, the refining zone is an assembly with fewer than all such assemblies. and/or may alternatively or additionally include one or more other components configured to purify effluent stream 96. For example, the purification region 82 may include only the membrane assembly 116 .

In some embodiments, hydrogen generating assembly 72 may include a shell or housing 120 that may at least partially contain one or more other components of the assembly. For example, shell 120 at least partially encloses vaporization region 76, hydrogen-producing region 78, heating assembly 80, and/or purification region 82, as shown in FIG. Acceptable. Shell 120 may include one or more exhaust ports 122 configured to discharge at least one combustion exhaust stream 124 produced by heating assembly 80 .

Hydrogen generating assembly 72 may include control system 126 , which may include any suitable structure configured to control operation of hydrogen generating assembly 72 , in some embodiments. For example, control assembly 126 may include control assembly 128 , at least one valve 130 , at least one pressure relief valve 132 , and one or more temperature measuring devices 134 . Control assembly 128 may detect the temperature within the hydrogen-producing zone and/or refining zone via temperature measuring device 134, which may include one or more thermocouples and/or other suitable devices. Based on the detected temperature, an operator of the control assembly and/or control system may, via valve(s) 130 and pump(s) 86, evaporation section 76 and/or hydrogen-producing section 78 The delivery of feed stream 90 to ) can be adjusted. Valve(s) 130 may include a solenoid valve and/or any suitable valve(s). The pressure relief valve(s) 132 may be configured to ensure that excess pressure in the system is released.

In some embodiments, the hydrogen generating assembly 72 may include a heat exchange assembly 136 comprising one or more heat exchangers configured to transfer heat from one portion of the hydrogen producing assembly to another portion. 138) may be included. For example, heat exchange assembly 136 may transfer heat from hydrogen-enriched stream 112 to feed stream 90 to increase the temperature of the feed stream prior to entry into evaporation zone 76 and Stream 112 may be cooled.

An example of a purification section 40 (or hydrogen purification device) of the hydrogen generating assembly 20 of FIG. 1 is indicated generally at 144 in FIG. 3 . Unless specifically excluded, a hydrogen refinery may include one or more components of the other refining zones described in this disclosure. The hydrogen purifier 40 may include a hydrogen-separation region 146 and an enclosure 148 . The enclosure may define an interior volume 150 having an interior perimeter 152 . The enclosure 148 includes at least a first portion 154 and a second portion 156 coupled together to form a body 149 in the form of a sealed pressure vessel that may include formed inlet and outlet ports. can do. Such ports may form fluid pathways by which gases and other fluids are conveyed into and removed from the interior volume of the enclosure.

First and second portions 154 and 156 may be coupled together using any suitable retaining mechanism or structure 158 . Examples of suitable holding structures include welds and/or bolts. Examples of seals that may be used to provide a fluid-tight interface between the first portion and the second portion may include gaskets and/or welds. Additionally or alternatively, the first and second components are applied such that at least a predetermined amount of compression is applied to the various components forming the hydrogen-separating region within the enclosure and/or other components that may be incorporated into the hydrogen generating assembly. Portions 154 and 156 may be secured together. Applied compression can ensure that various components are held in proper position within the enclosure. Additionally or alternatively, the compression applied to the various components and/or other components forming the hydrogen-separating region may cause, among the various components, among the other components, to form the hydrogen-separating region: and/or provide a fluid-tight interface between the components forming the hydrogen-separation region and other components.

Enclosure 148 may include a mixed gas region 160 and a transmissive region 162 , as shown in FIG. 3 . The mixed gas region and the permeate region may be separated by a hydrogen-separation region 146 . At least one inlet port 164 may be provided through which fluid stream 166 is delivered to the enclosure. Fluid stream 166 may be a mixed gas stream 168 comprising hydrogen gas 170 and other gases 172 delivered to mixed gas region 160 . Hydrogen gas may be the main component of the mixed gas stream. A hydrogen-separation region 146 may extend between the mixed gas region 160 and the permeate region 162 so that gases in the mixed gas region must pass through the hydrogen-separate region to enter the permeate region. As described further below, for example, a gas may be required to pass through at least one hydrogen-selective membrane. The permeate region and mixed gas region may have any suitable relative sizes within the enclosure.

Enclosure 148 may also include at least one product exhaust port 174 through which permeate stream 176 may be received and removed from permeate region 162 . The permeate stream may include at least one of a higher concentration of hydrogen gas and a lower concentration of other gases than the mixed gas stream. Permeate stream 176, in some embodiments, is a carrier gas component or sweep, such as may be delivered as sweep gas stream 178 through sweep gas port 180 in fluid communication with the permeate region. It may at least initially contain a gaseous component. The enclosure may also include at least one byproduct exhaust port 182 through which at least one of a substantial portion of other gases 172 and a reduced concentration of hydrogen gas 170 (relative to the mixed gas stream) A byproduct stream 184 comprising is removed from the mixed gas region.

Hydrogen-separating region 146 has at least a first or mixed gas surface 188 oriented to contact mixed gas stream 168 and a second or permeable surface 190 generally opposite surface 188. It may include one hydrogen-selective membrane 186 . Mixed gas stream 168 may be delivered to the mixed gas region of the enclosure to contact the mixed gas surface of the one or more hydrogen-selective membranes. Permeate stream 176 may be formed from at least a portion of the mixed gas stream passed through hydrogen-separation region to permeate region 162 . Byproduct stream 184 may be formed from at least a portion of the mixed gas stream that does not pass through the hydrogen-separation zone. In some embodiments, byproduct stream 184 may include a portion of the hydrogen gas present in the mixed gas stream. The hydrogen-separation region can also be configured to capture or otherwise retain at least a portion of other gases, which then at least some of the byproduct streams when the separation region is replaced, regenerated, or otherwise recharged. can be removed as

In FIG. 3 , streams 166 , 176 , 178 , and/or 184 may include more than one actual stream flowing into or out of hydrogen refinery 144 . For example, a hydrogen refinery may include a plurality of mixed gas streams 168, a single mixed gas stream 168 that is split into two or more streams prior to being contacted with the hydrogen-separation region 146, passed into the internal volume 150. It can accommodate a single stream, etc. Thus, enclosure 148 may include more than one inlet port 164 , product outlet port 174 , sweep gas port 180 , and/or byproduct outlet port 182 .

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

In some embodiments, a plurality of spaced apart hydrogen-selective membranes 186 may be utilized within the hydrogen-separation region to form at least a portion of the hydrogen-separation assembly 192 . A plurality of membranes, when present, may together form one or more membrane assemblies 194 . In such an embodiment, the hydrogen-separation assembly may extend generally from the first portion 154 to the second portion 156 . Thus, the first and second portions can effectively compress the hydrogen-separation assembly. In some embodiments, sheath 148 may additionally or alternatively include end plates (or end frames) coupled to opposite sides of the body portion. In such embodiments, the end plates can effectively compress the hydrogen-separation assembly (and other components that may be housed within the enclosure) between opposing pairs of end plates.

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

An example of a hydrogen refinery 144 is indicated generally at 196 in FIG. 4 . Unless specifically excluded otherwise, hydrogen refinery unit 196 may include one or more components of other hydrogen refinery units and/or refinery zones described in this disclosure. The hydrogen refinery device 196 may include a shell or enclosure 198 , which may include a first end plate or end frame 200 and a second end plate or end frame 202 . The first and second end plates may be configured to be clamped and/or compressed together to form a sealed pressure vessel having an inner compartment 204 in which a hydrogen-separating region is supported. The first and second end plates may include an inlet port, an outlet port, a sweep gas port, and a byproduct port (not shown), similar to the hydrogen purification device 144 .

The hydrogen purification device 196 may also include at least one foil-microscreen assembly 205 disposed between and/or secured to the first end plate and the second end plate. The foil-microscreen assembly, as shown in FIG. 5 , can include at least one hydrogen-selective membrane 206 and at least one microscreen structure 208 . The hydrogen-selective membrane can be configured to receive at least a portion of the mixed gas stream from the inlet port and separate the mixed gas stream into at least a portion of the permeate stream and at least a portion of the byproduct stream. The hydrogen-selective membrane 206 can include a supply side 210 and a permeate side 212 . At least a portion of the permeate stream is formed from a portion of the mixed gas stream passing from the feed side to the permeate side, and the remaining portion of the mixed gas stream remaining on the feed side forms at least a portion of the byproduct stream.

One or more of the hydrogen-selective membranes may be metallurgically bonded to the microscreen structure 208 . For example, the permeate side of the hydrogen-selective membrane(s) can be metallurgically bonded to the microscreen structure. In some embodiments, one or more of the hydrogen-selective membranes 206 (and/or the permeate side of such membrane(s)) is diffusion bonded to the microscreen structure, so that a solid-state interface between the membrane(s) and the microscreen structure is formed. Diffusion bonds can be formed. For example, by bringing the permeate side of the membrane(s) and the microscreen structure into contact with each other and exposing them to elevated temperature and/or elevated pressure, over time the surface of the membrane(s) and the microscreen structure can self-renew. can be interspersed.

In some embodiments, the microscreen structure may be coated with a thin layer of metal or an intermediate bonding layer to assist diffusion bonding. For example, a low-melting alloy suitable for solid-state diffusion bonding, but (1) not melting below 700 °C to become liquid phase and (2) low-melting point alloy below 700 °C upon diffusion into hydrogen-selective membrane(s). It does not form a thin coating of nickel, copper, silver, gold, or other metal. The thin metal layer is formed by a suitable deposition process (e.g., electrochemical plating, vapor deposition, sputtering, etc.) of a thin coating of an intermediate bonding layer onto the surface of the microscreen structure to be in contact with the hydrogen-selective membrane. can be applied to. In another embodiment, the hydrogen-selective membrane(s) may be secured to at least one membrane frame (not shown), which in turn may be secured to first and second end frames.

Microscreen structure 208 may include any suitable structure configured to support at least one hydrogen-selective membrane. For example, the microscreen structure, as shown in FIG. 6 , is a non-porous planar sheet 213 having generally opposed surfaces 214 and 215 configured to provide support for the permeate side 212. , and a plurality of apertures 216 defining a plurality of fluid passages 217 extending between the opposed surfaces through which the permeate stream can flow through the microscreen structure. Apertures can be formed on the non-porous planar sheet through electrochemical etching, laser drilling, and other mechanical forming processes, such as stamping or die cutting. In some embodiments, as shown in FIG. 6 , one or more apertures (or all apertures) are non-transparent such that the (longitudinal) axis of the aperture or the longitudinal axis of the fluid passageway is perpendicular to the plane of the non-porous planar sheet. - Can be formed on a porous planar sheet. The non-porous planar sheet may be of any suitable thickness, for example between 100 microns and about 200 microns thick.

In some embodiments, the microscreen structure 208 includes one or more perforated regions (or portions) 218 that include a plurality of apertures, and one or more non-perforated regions that do not (or do not have) a plurality of apertures. area (or portion) 219 . Although several apertures 216 are shown in FIG. 6 , apertures 216 are distributed over its entire length and width only at the perforated portion(s). The perforated area(s) may be distinct from or spaced apart from one or more other perforated areas. Non-perforated area(s) 219 may include a perimeter area (or portion) 220 that frames around one or more of the perforated area(s), and/or two or more discrete portions of the perforated area. It may include one or more boundary regions (or portions) 221 that separate or form. In other words, each perforated portion can be spaced from other adjacent discrete perforated portions by at least one boundary portion not having a plurality of apertures.

Aperture 216 may include any suitable pattern(s), shape(s), and/or size(s). In some embodiments, the apertures may be formed in one or more patterns that maximize the combined aperture area while maintaining a sufficiently high stiffness of the microscreen structure to prevent excessive deflection under pressure loading. The opening 216 may be circular (circular) as shown in FIG. 6, may be elongated circular as shown in FIG. 7, may be oval as shown in FIG. 8, and may be oval as shown in FIG. can be hexagonal, such as triangles, squares, rectangles, octagons, and/or other suitable shape(s). In some embodiments, the opening 216 in the puncture area(s) may be of one regular shape. In other embodiments, the apertures 216 in the puncture area(s) may be any suitable combination of two or more different shapes. The apertures may be of any suitable size(s). For example, when the aperture is circular, the diameter may range from about 0.003 inches to about 0.020 inches. Also, when the opening is oval, the radius of the rounded end of the oval can range from 0.001 inch to about 0.010 inch, and the length of the oval can be up to 10 times the radius. In some embodiments, the openings in the puncture area(s) may have one constant size. In other embodiments, apertures 216 in the puncture area(s) may have any suitable combination of two or more different sizes.

The non-porous planar sheet may include any suitable material. For example, the non-porous planar sheet may include stainless steel. Stainless steels include 300-series stainless steels (e.g., stainless steel 303 (aluminum doped), stainless steel 304, etc.), 400-series stainless steels, 17-7PH, 14-8 PH, and/or 15-7 PH can include In some embodiments, the stainless steel may include between about 0.6% and about 3.0% aluminum by weight. In some embodiments, the non-porous planar sheet may include carbon steel, copper or copper alloy, aluminum or aluminum alloy, nickel, nickel-copper alloy, and/or base metal plated with silver, nickel, and/or copper. can The base metal may include carbon steel or one or more of the aforementioned stainless steels.

Hydrogen-selective membrane 206 such that a perimeter portion 222 of the hydrogen-selective membrane is in contact with one or more non-perforated regions 219 of the microscreen structure when the hydrogen-selective membrane is metallurgically bonded to the microscreen structure. It may be of a larger size than the perforated area or portion of this microscreen structure. In some embodiments, as shown in FIG. 5 , a single hydrogen-selective membrane may be metallurgically bonded to a single microscreen structure. In another embodiment, two or more hydrogen-selective membranes 206 may be metallurgically bonded to one microscreen structure 208 . For example, 2, 3, 4, 5, 6, 7, 8, 9, 10 or more hydrogen-selective membranes 206 may be metallurgically bonded to one microscreen structure 208 . 10 shows an exemplary foil-microscreen assembly 205 having six hydrogen-selective membranes 206 metallurgically bonded to one microscreen structure 208 . 12 shows an exemplary foil-microscreen assembly 205 having two hydrogen-selective membranes 206 metallurgically bonded to one microscreen structure 208, while FIG. 13 shows one microscreen An exemplary foil-microscreen assembly 205 is shown having four hydrogen-selective membranes 206 metallurgically bonded to a structure 208 .

When two or more hydrogen-selective membranes 206 are metallurgically bonded to the microscreen structure, the microscreen structure has two or more distinct perforated regions 218 separated by one or more non-perforated regions 219. can include In some embodiments, the puncture area 218 may be the same size as the other puncture areas 218 . For example, FIG. 11 shows six distinct puncture zones 218 of approximately the same size. In other embodiments, one or more fenestration regions 218 may be of a smaller and/or larger size than other fenestration regions 218 . As shown in FIG. 10 , a hydrogen-selective membrane 206 may be metallurgically bonded to each perforation area. Alternatively or additionally, the hydrogen-selective membrane may be metallurgically bonded to two or more distinct perforation zones 218 . The size of the hydrogen-selective membrane(s) 206 is such that, when the membrane is metallurgically bonded to the one or more perforated regions 218, the perimeter portion 222 of the membrane contacts the one or more non-perforated regions 219. can be determined

As shown in FIG. 5 , the microscreen structure 208 can be sized to be accommodated within the open area of the transmission frame (e.g., to be accommodated entirely) and/or to be supported by the membrane support structure within the open area. can In other words, when the microscreen structure and the transmission frame are fixed or compressed relative to the first and second end frames, the microscreen structure may have a size that does not come into contact with the perimeter shell of the transmission frame. Alternatively, the microscreen structure may be supported by and/or secured to a non-porous perimeter wall portion or frame (not shown), for example a perimeter shell of a permeable frame. When the microscreen structure is secured to a non-porous peripheral wall portion, the microscreen structure may be referred to as a "porous central area portion". Examples of other microscreen structures are disclosed in US Patent Application Publication No. 2010/0064887, the entire disclosure of which is incorporated herein by reference for all purposes.

The hydrogen purification apparatus 196 may also include a plurality of plates or frames 224 disposed between and secured to the first and/or second end frames. The frame may comprise any suitable structure and/or may be any suitable shape(s), such as square, rectangular, or circular. For example, as shown in FIG. 4 , the frame 224 may include a perimeter shell 226 and at least one first support member 228 . The perimeter shell may define an open area 230 and a frame plane 232 . Also shown in FIG. 4 , perimeter shell 226 includes first and second opposed sides 234 and 236 , and third and fourth opposed sides 238 and 240 . can do.

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

In some embodiments, frame 224 is any suitable structure configured to support second portion 250 and/or third portion 252 of foil-microscreen assembly 205, as shown in FIG. 4 . It may include a second support member 246 and/or a third support member 248, which may include a structure. For example, the second support members of the plurality of frames can support each other (or other second support members of the plurality of frames) within the second support plane 254 to support the second portion 250 of the foil-microscreen assembly. and) can be co-planar. Additionally, the third support members of the plurality of frames can be connected to each other (or with other third support members of the plurality of frames) within the third support plane 256 to support the third portion 252 of the foil-microscreen assembly. It can be co-planar. In other words, the second support member of each frame of the plurality of frames may be mirror symmetrical with the second support member of another frame of the plurality of frames, while the third support member of each frame of the plurality of frames It may be mirror symmetrical with the third support member of the other frame of the frame. The second and/or third support plane may have any suitable orientation relative to frame plane 232 . For example, as shown in FIG. 4 , the second support plane 254 and/or the third support plane 256 can be perpendicular to the frame plane. Alternatively, the second and/or third support plane may intersect the frame plane 232 but not be perpendicular thereto.

The second support member 246 and/or the third support member 248 can have any suitable orientation relative to the first support member 228 . For example, the first support member 228 can extend into the open area 230 from the third side 238 of the perimeter shell 226; A second support member 246 may extend into the open area from a fourth side 240 (opposite the third side) of the perimeter shell; A third support member 248 may extend into the open area from the third side. Alternatively, the first, second, and/or third support members may extend into the open area from the same side of the perimeter shell, for example from the first, second, third, or fourth side. In some embodiments, first, second, and/or third support members may extend into the open area from a first side and/or a second side (opposite the first side) of the perimeter shell.

The first, second, and/or third support member may be, for example, in the form of one or more protrusions or fingers 258 attached to and/or formed with the perimeter shell. The protrusions may extend from the perimeter shell in any suitable direction(s). The protrusion may span the entire thickness of the perimeter shell or may be less than the entire thickness of the shell. A protrusion of each of the frames 224 may be compressed against the foil-microscreen assembly, thereby locking the assembly in place. In other words, the protrusions of the frame 224 may support the foil-microscreen assembly by stacking the extension(s) of the end frames within the first and second membrane support planes. In some embodiments, the protrusion(s) 258 include one or more receptacles configured to receive at least one fastener (not shown) for securing the frame 224 to the first and/or second end frame, or An opening (not shown) may be included.

As shown in FIG. 4 , the frame 224 may include at least one supply frame 260 , at least one transmission frame 262 , and a plurality of gaskets or gasket frames 264 . The feed frame 260 may be disposed between one of the first and second end frames and at least one foil-microscreen assembly 205 or between two foil-microscreen assemblies 205 . 4, the supply frame comprises a supply frame perimeter shell 266, a supply frame inlet conduit 268, a supply frame outlet conduit 270, a supply frame open area 272, at least one first supply frame. A support member 274 may be included. In some embodiments, the supply frame may include a second supply frame support member 276 and/or a third supply frame support member 278 .

The feed frame perimeter shell 266 may include any suitable structure. For example, as shown in FIG. 14 , the supply frame perimeter shell may include a first section or first perimeter shell 280 and a second section or second perimeter shell 282 . It should be noted that the components of FIG. 14 are exaggerated for illustrative purposes and may not reflect the relative dimensions of such components. The first and second sections may be first and second halves of the perimeter shell, or may be any suitable parts of the perimeter shell. Additionally, the first and/or second section may include channels or grooves (not shown) in any suitable relationship to one another, such as offset from one another. First section 280 and second section 282 can be joined via any suitable method(s) to form an airtight seal between them. For example, a feed frame gasket 284 may be used between such sections. Alternatively, as described in US Patent Application Publication No. 2013/0011301, the first and second sections may be brazed together or layered metal(s) may be used to join the first and second sections. there is. The entire disclosure of the foregoing publication is hereby incorporated by reference for all purposes.

Additionally, the feed frame circumferential shell 266 may include any suitable dimensions configured to support the other components of the hydrogen refinery 196. For example, to support the perimeter shell of the transmission frame(s) 262 and the membrane support structure(s) 286 of such frame(s) along a plurality of supply frame support planes 288, the supply frame perimeter shell size can be determined. For example, as shown in FIG. 14 , the perimeter shell 266 is the perimeter shell of the permeable frame 262 such that at least a portion 294 of the perimeter shell supports a portion 296 of the membrane support structure 286 . It may have a width 290 that is wider than the width 292 of . In other words, the shell around the feed frame can lock the membrane support structure in place and act as a stop for such a support structure. The supply frame support plane may have any suitable orientation relative to the supply frame plane 300 . For example, as shown in FIG. 14 , the supply frame support plane may be perpendicular to the supply frame plane. Alternatively, the supply frame support plane may intersect the supply frame plane 300 but may not be perpendicular thereto.

A feed frame inlet conduit may be formed on the shell around the feed frame and/or configured to receive at least a portion of the mixed gas stream from the inlet port. The feed frame exhaust conduit 270 may be formed on a shell around the feed frame and/or configured to receive a remaining portion of the mixed gas stream remaining on the feed side 210 of the hydrogen-selective membrane 206. . A supply frame open area 272 may be disposed between the supply frame inlet conduit and the supply frame outlet conduit. The supply frame perimeter shell 266 may include a plurality of grooves or channels (not shown) that fluidly connect the inlet and outlet conduits with the supply frame open areas. The channels may be formed on the perimeter shell via any suitable method(s), and/or at any suitable orientation(s), such as an angle that may result in mixing within the supply frame opening area 260. orientation can be formed.

As noted above, the first, second, and/or third feed frame support member may be any suitable structure configured to support the first, second, and/or third portion of the at least one hydrogen-selective membrane. and/or mirror symmetry of the first, second, and/or third support member of the other frame. Additionally, the first, second, and/or third supply frame support member provides a flow direction of at least a portion of the mixed gas stream as it flows across the supply frame opening area between the inlet conduit and the outlet conduit. It may include any suitable structure configured to change the. The first and/or second supply frame support members may also be configured to promote turbulence or mixing within the supply frame open area. For example, in the absence of the first and/or second supply frame support members, the flow of at least a portion of the mixed gas stream across the supply frame opening area between the inlet conduit and the outlet conduit may flow in at least a first direction (not shown). ) can be moved. The first and/or second feed frame membrane support structure may be configured to change the flow of at least a portion of the mixed gas stream from at least a first direction to at least a second direction (not shown) different from the first direction. .

The first, second, and/or third supply frame support member may be, for example, in the form of at least one supply frame protrusion or finger 302 attached to and/or formed with the supply frame circumferential shell. can be The supply frame protrusion(s) may extend from the perimeter shell in any suitable direction(s). For example, the supply frame protrusion(s) may be formed around the supply frame in a direction generally perpendicular (predetermined generally parallel) to the direction in which at least a portion of the mixed gas stream flows from the inlet conduit toward the supply frame opening area. may extend from the shell. For example, if the flow of the mixed gas stream from the inlet conduit to the supply frame opening area is in a generally horizontal direction, the supply frame projection(s) extend from the shell around the supply frame in a generally vertical and/or horizontal direction. It can be.

The transmission frame 262 may be positioned such that at least one foil-microscreen assembly is disposed between one of the first and second end frames and the transmission frame, or between two foil-microscreen assemblies. As shown in FIG. 15 , the transmission frame may include a transmission frame perimeter shell 304 , a transmission frame exhaust conduit 306 , a transmission frame open area 308 , and a membrane support structure 286 .

The perimeter shell of the transmission frame may include any suitable structure. For example, as shown in FIG. 14 , the transmission frame perimeter shell may include a first section or first perimeter shell 310 and a second section or second perimeter shell 312 . The first and second sections may be first and second halves of the perimeter shell, or may be any suitable parts of the perimeter shell. Additionally, the first and/or second section may include channels or grooves (not shown) in any suitable relationship to one another, such as offset from one another. First section 310 and second section 312 can be joined via any suitable method(s) to form an airtight seal between such sections. For example, a permeable frame gasket 314 may be used between such sections. As shown in FIG. 14 and described further below, when the transmission frame 262 is secured to the first and second end frames, the thickness 316 of the shell around the transmission frame is less than the thickness 318 of the membrane support structure. The transmission frame gasket may be configured to be matched or substantially matched (identical or substantially identical).

Alternatively, as described in US Patent Application Publication No. 2013/0011301, the first and second sections may be brazed together or layered metal(s) may be used to join the first and second sections. there is. The entire disclosure of the foregoing publication is hereby incorporated by reference for all purposes.

In some embodiments, as shown in FIG. 16 , the perimeter shell 304 of the transmission frame includes a first section 320, a second section 322, and a third section disposed between the first and second sections. (324). Such sections may be the first, second, and third sections of the perimeter shell, or may be any suitable parts of the perimeter shell. Additionally, the first, second, and/or third section may include channels or grooves (not shown) in any suitable relationship to one another, such as offset from one another. It should be noted that the components of FIG. 16 are exaggerated for illustrative purposes and may not reflect the relative dimensions of such components.

First section 320, second section 322, and third section 324 can be joined via any suitable method(s) to form an airtight seal between such sections. For example, a permeable frame gasket 326 may be used between such sections. 14, when the transmission frame 262 is secured to the first and second end frames, the thickness 316 of the shell around the transmission frame matches or substantially matches the thickness 318 of the membrane support structure. The transmission frame gasket can be configured to be (identical or substantially identical). Alternatively, as described in US Patent Application Publication No. 2013/0011301, the first, second, and/or third sections may be brazed together or the first, second, and/or third sections may be brazed together using layered metal(s). Sections 2 and/or 3 may be combined. The entire disclosure of the foregoing publication is hereby incorporated by reference for all purposes.

An exhaust conduit 306 may be formed on the shell 282 around the permeate frame and/or permeate from the membrane support structure 286, the permeate frame open area 308, and/or the hydrogen-selective membrane(s). It can be configured to accept streams. Perimeter shell 282 may include a plurality of grooves or channels (not shown) that fluidly connect exhaust conduit 284 with the permeate frame opening area and/or membrane support structure. The channels may be formed on perimeter shell 282 via any suitable method(s), and/or may have any suitable orientation(s), such as an angular orientation.

Membrane support structure 286 may include any suitable structure configured to support at least one foil-microscreen assembly, such as first, second, third, and/or other portions of a foil-microscreen assembly. can In some embodiments, the membrane support structure may include first, second, and/or third support members (not shown) similar to one or more of the other frames. Alternatively, membrane support structure 288 may include one or more membrane support plates 328, as shown in FIG. 14 . The membrane support plate(s) may span any suitable portion(s) of the open area, for example over at least a substantial portion of the open area. Further, the membrane support plate(s) can be solid, flat, or planar, can have no perforations or holes (or can have no perforations or holes), and can have no bumps and/or protrusions. (or may be free of bumps and/or protrusions), and/or may be incompressible (or may be substantially incompressible). Additionally, the membrane support plate(s) may not be attached (or may not have attachments) to the shell around the transmission frame. In other words, when the feed frame is secured to the first and second end plates, only the feed frame can lock the membrane support structure in place in the open area of the shell around the permeate frame. Additionally, the membrane support plate(s) may be made of any suitable material(s), for example stainless steel.

Membrane support plate(s) 328 can include a first face (or surface) 330 and a second opposing face (or opposing surface) 332 , as shown in FIG. 14 . As shown in FIG. 17 , either or both sides of the membrane support plate(s) may or may not include any or all grooves, bumps, protrusions, etc. In some embodiments, shown in FIG. 18 , either or both sides of membrane support plate(s) 328 may include any suitable structure that provides one or more flow paths for the permeate stream. As described above, a plurality of fine grooves 334 may be included. When the membrane support plate(s) 328 include surface micro-grooves, such plates may be referred to as “surface-grooved plate(s)”. The microgrooves may have any suitable orientation(s), such as parallel to each other. Further, the fine grooves 334 extend from the first edge 336 to the second opposite edge 338 (or from the third edge to the fourth opposite edge) of the membrane support plate, as shown in FIG. 18 . It can be. Alternatively, one or more fine grooves may be present between the first edge and the second edge, but not including the first edge and the second edge, from the first edge to the second edge, from the second edge to the first edge. etc. can be extended. Also, the fine grooves 334 may be on only the first surface, only on the second surface, or on both the first and second surfaces. Further, microgrooves may be included along the entire length or width of the membrane support plate (as shown in FIG. 18), or any such length or width, such as 25%, 50%, or 75% of the length or width. There may be along suitable part(s) of

Micro grooves 334 can have any suitable dimensions. For example, the microgrooves may have a width of 0.005 inches to 0.020 inches (or preferably 0.010 to 0.012 inches) and a depth of 0.003 to 0.020 inches (or preferably 0.008 to 0.012 inches). The microgrooves may be spaced apart any suitable distance(s), for example 0.003 to 0.020 inches (or preferably 0.003 to 0.007 inches). The microgrooves may be made by any suitable method(s), for example chemical etching, machining, and/or the like.

In some embodiments, the membrane support structure 286 will include one support plate 339 having opposing faces (either or all of which have microgrooves 334), as shown in FIG. 14 . can Alternatively, as shown by dashed lines in FIG. 14 , the membrane support structure may include a first membrane support plate 340 and a second membrane support plate 342 . The first membrane support plate may include a first face 344 and a second opposing face 346 . The second membrane support plate 342 may include a first face 348 and a second opposing face 349 . The first side of the first and/or second membrane support plate may or may not include microgrooves 334 . Also, the second faces of the first and second membrane support plates may face toward each other. In other words, the first and second membrane support plates may be stacked within the membrane support structure such that the second side of the first membrane support plate faces the second side of the second membrane support plate, and/or vice versa. there is. In some embodiments, the second side of the first membrane support plate may contact the second side of the second membrane support plate.

In some embodiments, the membrane support structure may include a third membrane support plate 350 that may be disposed between the first and second membrane support plates, as shown in FIG. 19 . It should be noted that the components of FIG. 19 are exaggerated for illustrative purposes and may not reflect the relative dimensions of such components. The membrane support structure may include first, second, and third membrane support plates stacked such that the third membrane support plate contacts second surfaces of the first and/or second membrane support plates. When the third membrane support plate is disposed between the first and second membrane support plates, the third membrane support plate may sometimes be referred to as the “center plate”. The third membrane support plate may not have fine grooves on either or both of its faces. The first, second, and third membrane support plates may have any suitable dimensions. For example, the first and second membrane support plates may be 0.060 inches, while the third membrane support plate may be 0.105 inches.

As described above, the permeate frame gaskets (314 and/or 326) such that when the permeate frame is secured to and/or compressed against the first and second end frames, the thickness of the permeate frame matches the thickness of the membrane support structure. ) can be configured. Such a gasket may provide a pre-compression thickness that is greater than the thickness of the membrane support structure. When flexible graphite gaskets are used for permeable frame gasket(s) with a compression limit of 15 to 50%, the permeable frame gasket(s) have a thickness prior to compression that results in a desired final thickness within that compression limit. can have When a transmission frame includes such a gasket, the transmission frame may sometimes be referred to as a “self-adjusting transmission frame”. When the self-adjusting permeation frame is compressed during assembly by compression through the feed frame (e.g., under 1000 to 2000 psi compression) to form a hermetic seal between the feed frame and the hydrogen-selective membrane, the feed frame comprises: When in contact with the hydrogen-selective membrane(s), the microscreen structure, and the membrane support structure, which may together form a group or stack of generally incompressible components, the compressive force of the feed frame relative to the permeate frame may be limited. can

As an example, if the membrane support structure has a thickness of 0.257 inches, the transmission frame may ideally have a thickness that is exactly or approximately 0.257 inches. When the perimeter shell of the permeable frame includes two sections, each 0.120 inch thick, for example, the permeable frame gasket should be constructed to be 0.017 inch thick after compression. For example, a permeate frame gasket that is 0.030 inches thick before compression can be compressed to 0.017 inches within its compression limits after compression, which can create a permeate frame thickness that matches the membrane support structure thickness. Although membrane support structure 286 is shown as including membrane support plate 328 , membrane support structure may include wire mesh and/or perforated metal sheet(s) (not shown).

Frame 224 may also include a gasket or gasket frame 264 as shown in FIG. 4 . The gasket frame is formed between other frames, for example between the first and second end plates 200 and 202 and the supply frame 260, between the supply frame 260 and the foil-microscreen assembly 205, Any suitable structure configured to provide a fluid-tight interface between the foil-microscreen assembly and the transmission frame 262 may be included. An example of a suitable gasket for gasket frame 264 is a flexible graphite gasket. Another example of a suitable gasket material is THERMICULITE® 866 sold by Flexitallic LP (Deer Park, Texas). Although frame 224 is shown as including two feed frames 260 and one transmission frame 262, such a frame may include any suitable number of feed frames and transmission frames. Further, although hydrogen purification device 196 is shown as including two hydrogen-selective membranes 206, such a device may include any suitable number of such membranes.

Although one or more of the frames 224 are shown as including protrusions that extend only in a vertical direction or only in a horizontal direction, the frames may additionally or alternatively be positioned in a horizontal, vertical, and/or other suitable orientation, such as For example, it may include a protrusion extending in a diagonal direction or the like. Also, although one or more frames 224 are shown as including three protrusions, a frame may include one, two, four, five or more protrusions. Also, although one or more frames 224 are shown as including co-planar protrusions in the first, second, and/or third support planes, the frame may additionally or alternatively: It may include co-planar protrusions in the fourth, fifth or more support planes.

Another example of a hydrogen refinery 144 is indicated generally at 396 in FIG. 20 . Unless specifically excluded otherwise, hydrogen refinery unit 396 may include one or more components of other hydrogen refinery units and/or refinery zones described in this disclosure.

Hydrogen purification device 396 is similar in many respects to hydrogen purification device 196, but is a different-shaped frame, no support member, and different-sized foil-microscreen assembly, as further described below. , and has a small number of gasket frames. Components or parts of hydrogen purification unit 396 correspond to those of hydrogen purification unit 196 and have the general form "3XX" instead of "1XX" and "4XX" instead of "2XX" in FIG. Denoted by similar reference numbers. Accordingly, features 398, 400, 402, 404, 405, 406, 408, 424, 426, 434, 436, 438, 440, 460, 462, 464, etc., correspond to their respective counterparts in hydrogen refinery 196. It may be identical or substantially identical to portions, ie, features 198, 200, 202, 204, 205, 206, 208, 224, 226, 234, 236, 238, 240, 260, 262, 264, etc.

The hydrogen refinery device 396 may include a shell or enclosure 398 , which may include a first end plate or end frame 400 and a second end plate or end frame 402 . The first and second end plates may be configured to be clamped and/or compressed together to form a sealed pressure vessel having an inner compartment 404 in which a hydrogen-separating region is supported.

The hydrogen purification device 396 can also include at least one foil-microscreen assembly 405 disposed between and/or secured to the first end plate and the second end plate. The foil-microscreen assembly can include at least one hydrogen-selective membrane 406 and at least one microscreen structure 408 . One or more of the hydrogen-selective membranes may be metallurgically bonded to the microscreen structure 408 . For example, one or more hydrogen-selective membranes 406 can be diffusion bonded to the microscreen structure to form a solid-state diffusion bond between the membrane(s) and the microscreen structure. The foil-microscreen assembly 405 is sized to fit the open area of the transmission frame, and thus has a smaller length and width as compared to or compared to the foil-microscreen assembly 205 .

The hydrogen purification device 396 may also include a plurality of plates or frames 424 disposed between and secured to the first and/or second end frames. Frame 424 may include a perimeter shell 426 . The perimeter shell may form an open area 430 . Perimeter shell 426 can also include first and second opposed sides 434 and 436 , and third and fourth opposed sides 438 and 440 . Unlike the frame 224 of the hydrogen purifier 196, the frame 424 does not include any support members.

The frame 424 may include at least one supply frame 460 , at least one transmission frame 462 , and a plurality of gaskets or gasket frames 464 . The feed frame 460 may be disposed between one of the first and second end frames and at least the foil-microscreen assembly 405 , or between two foil-microscreen assemblies 405 . The supply frame may include components at least substantially similar to supply frame 260, such as a supply frame perimeter shell, a supply frame inlet conduit, a supply frame outlet conduit, and/or a supply frame open area.

The transmission frame 462 can be positioned such that at least one foil-microscreen assembly is disposed between one of the first and second end frames and the transmission frame, or between two foil-microscreen assemblies. The transmission frame may include components at least substantially similar to the transmission frame 262, such as a transmission frame perimeter shell, a transmission frame exhaust conduit, a transmission frame open area, and/or a membrane support structure.

Frame 424 may also include a gasket or gasket frame 464 . A gasket frame may be formed between other frames, for example, between first and second end plates 400 and 402 and feed frame 460, and/or feed frame 460 and foil-microscreen assembly 405. It may include any suitable structure configured to provide a fluid-tight interface therebetween. Unlike the hydrogen purifier 196, the hydrogen purifier 396 does not include a gasket frame 464 between the foil-microscreen assembly and the permeate frame 462. Similar to the hydrogen purifier 196, the width of the feed frame and gasket frame is greater than the width of the permeate frame (or the open area of the feed frame and gasket frame is smaller than the open area of the permeate frame), so that the extra width is Covering the edge of the foil-microscreen assembly eliminates or minimizes leakage from the supply side to the permeate side or from the permeate side to the supply side (e.g., the extra width of the supply frame and gasket frame can be applied to the edge of the foil-microscreen assembly). See Figure 14 which shows how to cover). In some embodiments, the extra width corresponds to the width of the peripheral (non-perforated) portion of the microscreen structure of the foil-microscreen assembly.

Hydrogen purification devices and/or components thereof (eg, foil-microscreen assemblies) of the present disclosure may include one or more of the following:

o First and second end frames comprising inlet ports configured to receive a mixed gas stream comprising hydrogen gas and other gases.

o First and second end frames comprising exhaust ports configured to receive a permeate stream comprising at least one of a higher concentration of hydrogen gas and a lower concentration of other gases than the mixed gas stream.

o First and second end frames comprising by-product ports configured to receive a by-product stream comprising at least a substantial portion of another gas.

o at least one foil-microscreen assembly secured thereto disposed between and secured to the first end frame and the second end frame.

o At least one hydrogen-selective membrane disposed between and secured to the first end frame and the second end frame.

o at least one hydrogen-selective membrane having a feed side and a permeate side, wherein at least a portion of the permeate stream is formed from a portion of the mixed gas stream passing from the feed side to the permeate side, and the remaining portion of the mixed gas stream remaining on the feed side is a by-product at least one hydrogen-selective membrane, forming at least a portion of the stream.

o at least one hydrogen-selective membrane metallurgically bonded to at least one microscreen structure.

o the permeate side of at least one hydrogen-selective membrane metallurgically bonded to at least one microscreen structure.

o at least one hydrogen-selective membrane diffusion bonded to at least one microscreen structure.

o Permeate side of at least one hydrogen-selective membrane diffusion bonded to at least one microscreen structure.

o At least one microscreen structure disposed between the at least one hydrogen-selective membrane and the at least one permeation frame.

o At least one microscreen structure configured to support at least one hydrogen-selective membrane.

o At least one microscreen structure includes generally opposed surfaces configured to provide support for the permeate side.

o At least one microscreen structure includes a plurality of fluid passageways extending between the opposed surfaces.

o at least one microscreen structure of a size not in contact with the perimeter shell of the at least one transmission frame.

o At least one microscreen structure and at least one microscreen structure of a size that does not come into contact with the perimeter shell when the at least one transmission frame is secured to the first and second end frames.

o At least one microscreen structure comprising a non-porous planar sheet having a plurality of apertures defining a plurality of fluid passageways.

o A non-porous planar sheet comprising generally opposed planar surfaces configured to provide support to the permeate side.

o A non-porous planar sheet comprising at least one perimeter portion without openings.

o A non-porous planar sheet comprising two or more distinct parts with openings.

o At least one microscreen structure comprising a non-porous metal sheet having a plurality of openings defining a plurality of fluid passageways.

o A non-porous metal sheet in which the openings of the non-porous sheet form a plane including an axis perpendicular to the plane.

o The openings of the non-porous sheet are circular.

o The openings of the non-porous sheet are elongated circular.

o The openings of the non-porous sheet are elliptical.

o The apertures of the non-porous sheet are hexagonal.

o Non-porous metal sheet including stainless steel.

o Non-porous metal sheet comprising 300-series stainless steel.

o Non-porous metal sheet comprising 400-series stainless steel.

o Non-porous metal sheet comprising stainless steel having from about 0.6% to about 3.0% aluminum by weight.

o Non-porous metal sheet comprising one or more nickel alloys.

o Non-porous metal sheet comprising one or more nickel alloys having a plated nickel surface.

o Non-porous metal sheet comprising one or more alloys of nickel with copper.

o One or more distinct parts separated from adjacent distinct parts by at least one boundary part not having an aperture.

o Different hydrogen-selective membranes are metallurgically bonded in discrete parts.

o The hydrogen-selective membrane is of a larger size than the discrete portions such that the perimeter portion of the membrane is in contact with at least one portion of the non-porous planar sheet that does not contain openings.

o A plurality of frames disposed between the first and second end frames and the at least one hydrogen-selective membrane and secured to the first and second end frames.

o A plurality of frames comprising at least one permeable frame disposed between the at least one hydrogen-selective membrane and the second end frame.

o at least one transmission frame comprising a perimeter shell.

o at least one permeate frame comprising an exhaust conduit formed on the perimeter shell and configured to receive at least a portion of the permeate stream from the at least one hydrogen-selective membrane.

o at least one transmissive frame comprising an open area surrounded by a perimeter shell.

o At least one transmission frame comprising at least one membrane support structure.

o at least one membrane support structure spanning at least a substantial portion of the open area.

o At least one membrane support structure configured to support at least one hydrogen-selective membrane.

o At least one membrane support structure comprising a membrane support plate comprising a first face and a second face opposite the first face.

o The first and/or second face has a plurality of microgrooves configured to provide flow channels for at least a portion of the permeate stream.

o The first and/or second side is free of microgrooves.

o At least one membrane support structure comprising first and second membrane support plates.

o The first and second membrane support plates do not have perforations.

o First and second membrane support plates having a first face with a plurality of fine grooves configured to provide flow channels for at least a portion of the permeate stream.

o First and second membrane support plates having a second face opposite to the first face.

o First and second membrane support plates laminated within at least one membrane support structure.

o First and second membrane support plates laminated within at least one membrane support structure such that the second side of the first membrane support plate faces the second side of the second membrane support plate.

o First and second non-compressible membrane support plates.

o Flat first and second membrane support plates.

o At least one feed frame disposed between the first end frame and the at least one hydrogen-selective membrane.

o At least one feed frame comprising a perimeter shell.

o at least one supply frame comprising an inlet conduit formed on a perimeter shell of the at least one supply frame.

o At least one feed frame comprising an inlet conduit configured to receive at least a portion of the mixed gas stream from the inlet port.

o At least one supply frame comprising a discharge conduit formed on a peripheral shell of the at least one supply frame.

o at least one supply frame comprising a discharge conduit configured to receive a remaining portion of at least a portion of the mixed gas stream remaining on the supply side of the at least one hydrogen-selective membrane.

o at least one feed frame comprising a feed frame open area surrounded by a perimeter shell of the feed frame and disposed between the inlet conduit and the outlet conduit.

o the peripheral shell of the at least one feed frame is dimensioned such that the peripheral shell of the at least one feed frame supports the peripheral shell of the at least one permeable frame and a portion of the at least one membrane support structure.

o so that along a plurality of support planes perpendicular to the frame plane of each frame of the plurality of frames, the circumferential shell of the at least one feed frame supports the circumferential shell of the at least one transmission frame and a portion of the at least one membrane support structure. A peripheral shell of at least one supply frame having a size of

o At least one membrane support structure comprising a third membrane support plate.

o A third membrane support plate disposed between the first and second membrane support plates.

o Non-compressible third membrane support plate.

o Flat third membrane support plate.

o Third membrane support plate without perforations.

o Third membrane support plate without fine grooves.

o Perimeter shell of the transmission frame comprising first and second perimeter shells.

o Perimeter shell of the transmission frame comprising a gasket disposed between the first and second perimeter shells.

o A gasket configured such that the thickness of the shell around the permeation frame matches the thickness of the membrane support structure.

o A gasket configured such that when the permeate frame is secured to the first and second end frames, the thickness of the shell around the permeate frame matches the thickness of the membrane support structure.

o A permeable frame perimeter shell comprising first, second and third perimeter shells.

o A permeable frame perimeter shell comprising a first gasket disposed between the first and second perimeter shells.

o A permeable frame perimeter shell comprising a second gasket disposed between the second and third perimeter shells.

o First and second gaskets configured such that the thickness of the permeable frame perimeter shell matches the thickness of the membrane support structure.

o First and second gaskets configured so that the thickness of the shell around the permeation frame matches the thickness of the membrane support structure when the permeate frame is secured to the first and second end frames.

o First and second membrane support plates each having first and second opposed edges.

o A plurality of fine grooves extending from the first edge to the second edge.

o Multiple parallel microgrooves.

The present disclosure, including hydrogen purification devices and components of such devices, may be applied to fuel-processing and other industries in which hydrogen gas is purified, produced, and/or utilized.

The foregoing disclosure includes many other inventions with independent facilities. Although each of these inventions has been disclosed in its preferred form, the specific embodiments disclosed and illustrated herein should not be regarded in a limiting sense, as numerous modifications may be made. Inventive subject matter includes all novel and nonobvious combinations and subcombinations of the various elements, features, functions and/or properties disclosed herein. Similarly, where in any claim the indefinite article ("a") or the "first" element or its equivalents are recited, such claim does not require and exclude two or more such elements, and does not preclude one or more. It should be understood to include the integration of such elements.

The invention, embodied in various combinations and sub-combinations of features, functions, elements and/or properties, may be claimed by providing new claims in related applications. Such new claims, whether to a different invention or to the same invention, whether of a broader, narrower or equivalent scope different from the original claims, are intended to be included within the claimed subject matter of the present disclosure. is considered

Claims (19)

a foil-microscreen assembly;
at least one hydrogen-selective membrane having a feed side and a permeate side; and
At least one non-porous planar sheet having a plurality of apertures, the plurality of apertures being formed on the non-porous planar sheet through one of chemical etching, laser drilling, stamping, or die cutting, the plurality of apertures comprising a plurality of fluid wherein the at least one non-porous planar sheet comprises opposed planar surfaces configured to provide support to the permeate side, a plurality of fluid passageways extending between the opposing surfaces, and wherein the at least one hydrogen- The permeate side of the selective membrane is metallurgically bonded to at least one non-porous planar sheet, the non-porous planar sheet comprising at least two distinct portions having a plurality of apertures. A foil-microscreen assembly comprising: 2. The method of claim 1, wherein each distinct portion of the two or more distinct portions is spaced from adjacent distinct portions of the two or more distinct portions by at least one border portion not having a plurality of apertures. , Foil-microscreen assembly. 2. The method of claim 1, wherein at least one hydrogen-selective membrane comprises two or more hydrogen-selective membranes, and the other hydrogen-selective membranes of the two or more hydrogen-selective membranes are each distinct portion of the two or more distinct portions. A foil-microscreen assembly, metallurgically bonded to the part. 4. The method of claim 3, wherein each hydrogen-selective membrane of the at least two hydrogen-selective membranes is such that a peripheral portion of the hydrogen-selective membrane is in contact with at least one portion of a non-porous planar sheet that does not include a plurality of apertures. A foil-microscreen assembly having a larger size than the corresponding segmented part. The foil-microscreen assembly of claim 1 , wherein the at least one hydrogen-selective membrane is diffusion bonded to at least one non-porous planar sheet. 2. A foil-microscreen assembly according to claim 1, wherein the non-porous planar sheet forms a plane and a longitudinal axis of at least one of the plurality of apertures is perpendicular to the plane. 7. A foil-microscreen assembly according to claim 6, wherein a longitudinal axis of every aperture of said plurality of apertures is perpendicular to said plane. The foil-microscreen assembly of claim 1 wherein the thickness of the non-porous planar sheet is between 100 microns and 200 microns. A method of making a foil-microscreen assembly;
providing at least one hydrogen-selective membrane having a feed side and a permeate side;
providing at least one non-porous planar sheet having a plurality of apertures, wherein the plurality of apertures are formed on the at least one non-porous planar sheet through one of chemical etching, laser drilling, stamping, or die cutting; The plurality of apertures define a plurality of fluid passageways, the at least one non-porous planar sheet comprising opposing planar surfaces and a plurality of fluid passageways extending between the opposing surfaces, the non-porous planar sheet comprising a plurality of apertures. providing at least one non-porous planar sheet comprising two or more discrete portions having and
metallurgically bonding the permeate side of at least one hydrogen-selective membrane to at least one non-porous planar sheet. 10. The method of claim 9, wherein the step of metallurgically bonding the permeate side of the at least one hydrogen-selective membrane to the at least one non-porous planar sheet comprises: diffusion bonding to a porous planar sheet. 11. The method of claim 10, wherein the permeate side of the at least one hydrogen-selective membrane is diffusion bonded to the at least one non-porous planar sheet, wherein the at least one non-porous layer is a thin metal layer or intermediate bonding layer that assists in the diffusion bonding. A method comprising coating a planar sheet. 12. The method of claim 11, wherein coating the at least one non-porous planar sheet with an intermediate bonding layer or a thin layer of metal that aids diffusion bonding comprises, via a deposition process, coating the at least one non-porous planar sheet with a thin layer of metal or an intermediate bonding layer. and applying an intermediate bonding layer. delete 10. The method of claim 9, wherein the non-porous planar sheet defines a plane, and forming a plurality of apertures on the non-porous planar sheet via one of electrochemical etching, laser drilling, stamping, or die cutting comprises: forming a plurality of apertures on the non-porous planar sheet through one of chemical etching, laser drilling, stamping, or die cutting such that a longitudinal axis of at least one of the plurality of apertures is perpendicular to the plane; , method. 10. The method of claim 9, wherein the non-porous planar sheet defines a plane, and forming a plurality of apertures on the non-porous planar sheet via one of electrochemical etching, laser drilling, stamping, or die cutting comprises: forming a plurality of apertures on the non-porous planar sheet through one of etching, laser drilling, stamping, or die cutting such that longitudinal axes of all apertures of the plurality of apertures are perpendicular to the plane. The foil-microscreen assembly of claim 1 , wherein the at least one hydrogen-selective membrane is comprised of one or more palladium alloys. 17. The foil-microscreen assembly of claim 16, wherein the at least one palladium alloy has from 35% to 45% copper by weight. 17. The foil-microscreen assembly of claim 16, wherein the at least one palladium alloy has from 20% to 30% silver by weight. 2. A foil-microscreen assembly according to claim 1, wherein the at least one non-porous planar sheet is coated with a thin layer of metal consisting of at least one of silver, copper, or nickel.