Structured catalysts

Abstract

A structured catalyst for catalyzing the endothermic reaction of a feed gas to convert it into a product gas is provided.

Description

Technical Field

[0001] Structured catalysts, reactor systems, and processes are provided for conducting endothermic reactions of feed gases, wherein heat for the endothermic reactions is provided by resistive heating. Background Art

[0002] Due to the energy-intensive reactions required to produce it, synthesis gas (synthesis gas) production is typically carried out in large chemical plants. This makes small-scale production difficult. Furthermore, the toxicity of syngas (particularly due to its carbon monoxide content) makes its storage difficult and poses significant risks.

[0003] In smaller plants, synthesis gas is produced on demand. Summary of the Invention

[0004] In a first aspect, a structured catalyst for catalyzing an endothermic reaction of a feed gas to convert it into a product gas is provided, the structured catalyst comprising at least one macroscopic structure of an electrically conductive material and at least one connector attached to the at least one macrostructure, wherein the macrostructure supports catalytically active material, the macrostructure extending in a longitudinal direction from a first end to a second end, wherein the first end forms an inlet for the feed gas to pass into the macrostructure and the second end forms an outlet for the product gas, the macrostructure comprising a circumferential wall surrounding an interior space, wherein the connector comprises a first engagement means for engaging an outer surface of the circumferential wall of the first macrostructure, wherein the engagement means has an inner surface having a shape matching at least a portion of the outer surface of the circumferential wall, wherein the engagement means is attached to the outer surface of the circumferential wall by an interference fit, wherein the structured catalyst comprises at least two macrostructures, wherein the connector comprises at least two engagement means, each engagement means engaging one of the macrostructures, and wherein the inner surfaces of the engagement means are arranged to allow the macrostructures to extend parallel to the longitudinal direction.

[0005] In another aspect, a reactor system for performing an endothermic reaction of a feed gas is provided, the reactor system comprising:

[0006] a) a structured catalyst according to the first aspect;

[0007] b) a pressure housing containing the structured catalyst, the pressure housing comprising an inlet for admitting the feed gas and an outlet for allowing the product gas to exit, wherein the inlet is positioned such that the feed gas enters the structured catalyst at a first end and the product gas exits the catalyst from a second end; and

[0008] c) A heat insulation layer (heat insulation layer) between the structured catalyst and the pressure housing.

[0009] In yet another aspect, there is provided use of the structured catalyst according to the first aspect or the reactor according to the second aspect, wherein the endothermic reaction is selected from the group consisting of steam methane reforming, hydrogen cyanide formation, methanol cracking, ammonia cracking, reverse water gas shift and dehydrogenation.

[0010] Other aspects of the technology are set forth in the following detailed description, accompanying drawings, and appended claims. BRIEF DESCRIPTION OF THE DRAWINGS

[0011] Figure 1a shows a cross-section of an embodiment of a reactor system of the present invention having a structured catalyst comprising an array of macrostructures in cross-section;

[0012] Figure 1b Shown Figure 1a A reactor system wherein the insulation and a portion of the pressure shell are removed;

[0013] Figure 2 is an enlarged view of a portion of the reactor system;

[0014] Figure 3 A structured catalyst comprising six macrostructures and four connectors is shown;

[0015] Figure 4 A connector is shown;

[0016] Figure 5 A connector is shown;

[0017] Figure 6 A structured catalyst comprising a plurality of macrostructures and a plurality of connectors is shown;

[0018] Figure 7a A connector is shown;

[0019] Figure 7b Shown Figure 7a A cross-sectional view of the connector shown in ;

[0020] Figure 8 A connector is shown;

[0021] Figure 9 A connector is shown; and

[0022] Figure 10 A structured catalyst comprising a plurality of macrostructures connected by a plurality of connectors attached to the macrostructures is shown. DETAILED DESCRIPTION

[0023] Electrically heated reactors offer the possibility of producing very compact chemical reactors, as the heat for the reaction is transferred directly to the catalyst zone.

[0024] Compact electroreactors using monolithic catalysts can be easily operated and use easy startup principles to produce gas when needed. This provides a relatively inexpensive plant in which only the required amount of gas can be produced, with little need for gas storage, while also reducing or eliminating gas transportation. The simple reactor equipment and simple operation of the process make gas production attractive in delocalized plants, which reduces the risks of gas handling.

[0025] An embodiment of a compact electroreactor includes a structured catalyst comprising at least one macrostructure and at least one connector attached to the at least one macrostructure. A plurality of macrostructures can be connected in series with one another to provide a desired resistance to match a desired power rating from an associated power source.

[0026] Multiple macrostructures must be electrically connected. Electrical connections in electrical devices must be made carefully to avoid circuit interruptions or localized high contact resistance, a challenge that increases with increasing temperature. Consequently, typical methods for electrical connection are relatively inconvenient, as known methods such as welding or soldering require space around the connection device to ensure good contact.

[0027] To further optimize the size of compact electroreactors, the void space in structured catalysts can be minimized.

[0028] Thus, there is provided a structured catalyst for catalyzing an endothermic reaction of a feed gas to convert it into a product gas, the structured catalyst comprising at least one macrostructure of an electrically conductive material and at least one connector attached to the at least one macrostructure, wherein the macrostructure supports catalytically active material, the macrostructure extending in a longitudinal direction from a first end to a second end, wherein the first end forms an inlet for the feed gas to pass into the macrostructure and the second end forms an outlet for the product gas, the macrostructure comprising a circumferential wall surrounding an interior space, wherein the connector comprises a first engaging means for engaging an outer surface of the circumferential wall of the first macrostructure, wherein the engaging means has an inner surface having a shape matching at least a portion of the outer surface of the circumferential wall, wherein the engaging means is attached to the outer surface of the circumferential wall by an interference fit, wherein the structured catalyst comprises at least two macrostructures, wherein the connector comprises at least two engaging means, each engaging means engaging one of the macrostructures, and wherein the inner surface of the engaging means is arranged to allow the macrostructures to extend parallel to the longitudinal direction.

[0029] The connector can be attached to at least one macrostructure by pressing it onto the at least one macrostructure. Two neighboring macrostructures can be attached to each other by pressing the connector onto the two neighboring macrostructures. This allows for easy assembly of larger arrays of multiple macrostructures that are all electrically connected.

[0030] By pressing the connector onto the at least one macrostructure so that the engagement means is attached to the outer surface of the circumferential wall by an interference fit, the void space in the structured catalyst can be significantly reduced.

[0031] In the context of the present invention, an "interference fit" (also called a press fit or friction fit) is understood to be a tight fit between two tightly fitting mating parts, resulting in a joint held together by friction after the parts are pushed / pressed together. The connector and one or more macro structures can be joined by applying forced pressure, such as from a press, on one part to slide it over / into the other part.

[0032] When the connector is attached to the macrostructure by an interference fit, the engagement means and the circumferential wall mate with each other within 1 mm or less, preferably within 0.1 mm or less, even more preferably within -0.1 mm, in a principal part of the joint, measured perpendicularly to the plane of connection of the connector and the macrostructure. The principal part of the joint refers to at least 50%, preferably at least 75%, even more preferably 100% of the circumference of the joint; i.e. along the inner surface of the engagement means and the outer surface of the circumferential wall. When the engagement means and the circumferential wall mate with each other at a negative distance in the principal part of the joint, deformation of the principal part of the joint is expected; i.e., the circumferential wall or the engagement means of the connector. When the engagement means and the circumferential wall mate with each other at a positive distance in the principal part of the joint, no deformation occurs because the two parts are pressed together without deformation.

[0033] The structured catalyst comprising at least one macrostructure and at least one connector enables an easier production scheme with simple assembly of arrays.

[0034] The macrostructures support catalytically active material, which may be provided at least partially on exposed surface areas of the macrostructures.

[0035] The close proximity between the catalytically active material and the macrostructure enables efficient heating of the catalytically active material by heat conduction from the solid material of the resistively heated macrostructure. Therefore, an important feature of the resistive heating process is that the energy is supplied within the object itself, rather than from an external heat source via heat conduction, convection, and radiation. In addition, the hottest part of the reactor system including the structured catalyst will be within the pressure shell of the reactor system. Preferably, the power supply and the size of the structured catalyst are determined so that at least a portion of the structured catalyst reaches a temperature of 850°C, preferably 900°C, more preferably 1000°C or even more preferably 1100°C. The amount and composition of the catalytically active material can be tailored to the steam reforming reaction under given operating conditions. The surface area of ​​the macrostructure, the fraction of the macrostructure coated with the ceramic coating, the type and structure of the ceramic coating, and the amount and composition of the catalytically active catalyst material can be tailored to the steam reforming reaction under given operating conditions. However, it should be noted that, advantageously, substantially all surfaces of the macrostructure are coated with the ceramic coating, and preferably all or most of the ceramic coating supports the catalytically active material. Preferably, only the parts of the macrostructure which are connected to the one or more connectors are not provided with a ceramic coating.

[0036] As used herein, the term "macrostructure" means a structure that is large enough to be visible to the naked eye without an amplifying device. The size of the macrostructure is typically in the range of tens of centimeters or tens of meters. Advantageously, the size of the macrostructure is at least partially corresponding to the internal dimensions of the pressure shell that accommodates the structured catalyst, thereby saving space for thermal insulation and conductors. In order to provide a macrostructure array with at least one of the external dimensions in the range of several meters (such as 0.5m, 1m, 2m or 5m), two or more macrostructures can be connected. Such two or more macrostructures can be expressed as "macrostructure arrays (an array of macroscopic structures)". In this case, advantageously, the size of the macrostructure array is at least partially corresponding to the internal dimensions of the pressure shell that accommodates the structured catalyst (saving space for thermal insulation). Conceivable macrostructure arrays can occupy 0.1m 3 Up to 10m 3 Or even larger volumes. A "structured catalyst" may comprise a single macrostructure or an array of macrostructures, wherein one or more macrostructures may support a ceramic coating that supports a catalytically active material. If the structured catalyst comprises an array of macrostructures, the macrostructures may be electrically connected to each other; however, alternatively, the macrostructures are not electrically connected to each other. Thus, the structured catalyst may comprise two or more macrostructures positioned adjacent to each other. One or more macrostructures may be extruded and sintered structures. Alternatively, one or more macrostructures may be 3D printed and optionally sintered.

[0037] The physical dimensions of the macrostructures may be of any suitable size; thus, the height of a macrostructure may be smaller than its width, or vice versa.

[0038] The term "first end of the macrostructure" is intended to mean the end of the macrostructure where the feed gas enters the macrostructure, and the term "second end of the macrostructure" is intended to mean the end of the macrostructure where the product gas exits the macrostructure.

[0039] The macrostructure may support a ceramic coating, wherein the ceramic coating may support a catalytically active material. The term "macrostructure supporting a ceramic coating" is intended to mean that the macrostructure is coated with the ceramic coating at least at a portion of the surface of the macrostructure. Thus, the term does not mean that all surfaces of the macrostructure are coated with the ceramic coating; in particular, at least the portion of the macrostructure that is electrically connected to the conductor has no coating thereon. The coating may be a ceramic material having pores in the structure that allow the catalytically active material to be supported on and within the coating. Advantageously, the catalytically active material comprises catalytically active particles having a size in the range of about 5 nm to about 250 nm.

[0040] The macrostructure can be manufactured by extruding a mixture of powdered metal particles and a binder into an extruded structure and then sintering the extruded structure, thereby providing a material with a high geometric surface area per unit volume. Alternatively, the macrostructure can be 3D printed. Preferably, the extruded or 3D printed structure is sintered in a reducing atmosphere (reducing atmosphere). A ceramic coating that may contain catalytically active material can be provided to the macrostructure in an oxidizing atmosphere before a second sintering is performed so as to form a chemical bond between the ceramic coating and the macrostructure. Alternatively, the catalytically active material can be impregnated into the ceramic coating after the second sintering. When a chemical bond is formed between the ceramic coating and the macrostructure, high thermal conductivity between the electrically heated macrostructure and the catalytically active material supported by the ceramic coating can be achieved, thereby providing close and almost direct contact between the heat source and the catalytically active material of the structured catalyst. Due to the close proximity between the heat source and the catalytically active material, heat transfer is efficient, so that the structured catalyst can be heated very efficiently. Thus, a compact reactor system is possible in terms of gas processing per unit volume of the reactor system, and thus the reactor system housing the structured catalyst can be compact.

[0041] As used herein, the terms "3D printing" and "3D printing" are intended to refer to metal additive manufacturing processes. Such metal additive manufacturing processes encompass 3D printing processes in which materials are joined to structures under computer control to create a three-dimensional object, wherein the structures are solidified, for example by sintering, to provide a macrostructure. Furthermore, such metal additive manufacturing processes encompass 3D printing processes that do not require subsequent sintering, such as powder bed fusion or direct energy deposition processes. Examples of such powder bed fusion or direct energy deposition processes are laser beam, electron beam, or plasma 3D printing processes.

[0042] The conductive material comprises Fe, Ni, Cu, Co, Cr, Al, Si or an alloy thereof. Such alloys may include other elements such as Mn, Y, Zr, C, Co, Mo or a combination thereof. Preferably, the conductive material comprises Fe, Cr, Al or an alloy thereof. Such alloys may include other elements such as Si, Mn, Y, Zr, C, Co, Mo or a combination thereof. Preferably, the catalytically active material is a particle having a size of 2 nm to 250 nm. Preferably, the conductor and the conductive material are made of a material different from the conductive material. The conductor can be, for example, iron, nickel, aluminum, copper, silver or an alloy thereof. The ceramic coating is an electrically insulating material and will typically have a thickness in the range of about 100 μm, for example 10 μm to 500 μm.

[0043] The conductive material used for the macrostructure is advantageously a coherent or consistently intra-connected material so that electrical conductivity is achieved throughout the conductive material and thereby thermal conductivity is achieved throughout the structured catalyst, particularly providing heating of the catalyst material. By coherently or consistently intra-connected materials, uniform distribution of current within the conductive material can be ensured, thereby ensuring uniform distribution of heat within the structured catalyst. Throughout this article, the term "coherent" is synonymous with cohesiveness and therefore refers to a material that is consistently intra-connected or consistently coupled. The effect of the structured catalyst being a coherent or consistently intra-connected material is that control of the connectivity within the material of the structured catalyst is obtained, and therefore control of the conductivity of the conductive material is obtained. It should be noted that even if further modifications of the conductive material are made, such as providing slits within portions of the conductive material or implementing insulating materials within the conductive material, the conductive material is still represented as a coherent or consistently intra-connected material.

[0044] At least one macrostructure may include multiple inner walls within the interior space, the multiple inner walls forming multiple flow channels from the first end to the second end. Thus, the macrostructure may have multiple parallel channels, multiple non-parallel channels, and / or multiple labyrinthine channels, wherein the channels have walls defining the channels. Thus, several different forms of macrostructures may be used, as long as the surface area of ​​the structured catalyst exposed to the gas is as large as possible. In a preferred embodiment, the macrostructure has parallel channels because such parallel channels provide the structured catalyst with a very small pressure drop. In a preferred embodiment, the parallel longitudinal channels are inclined in the longitudinal direction of the macrostructure. In this way, gas molecules flowing through the macrostructure will tend to primarily impact the walls within the channels, rather than simply flowing directly through the channels without contacting the walls. In order to provide a macrostructure with sufficient resistivity, the channel size should be appropriate. For example, the channel may be quadratic (as seen in a cross section perpendicular to the channel), with the side length of the square being between 1 mm and 3 mm; however, channels with a maximum cross-sectional extent of up to about 4 cm are conceivable. The wall may for example have a thickness between 0.2 mm and 2 mm, such as about 0.5 mm, and the ceramic coating supported by the wall may have a thickness between 10 μm and 500 μm, such as between 50 μm and 200 μm, such as 100 μm. In another embodiment, the macrostructure of the structured catalyst is cross-corrugated.

[0045] Typically, when macrostructures are extruded or 3D-printed, the pressure drop from the inlet to the outlet of the reactor system can be significantly reduced compared to reactors where the catalyst material is in pellet form.

[0046] The macrostructure includes a circumferential wall surrounding an interior space within which a plurality of channels may extend.

[0047] The connector comprises first engagement means for engaging the outer surface of the circumferential wall of the first macrostructure. To facilitate attachment of the connector to the first macrostructure by interference fit, the engagement means of the connector has an inner surface having a shape matching at least a portion of the outer surface of the circumferential wall.

[0048] When the connector is pressed onto the macrostructure, the outer surface of the circumferential wall may be deformed by an interference fit, thereby ensuring a consistent and durable mechanical connection during use of the structured catalyst.

[0049] The electrical connection between the connector and the macrostructure can be implemented by a deformable material disposed within at least a portion of the circumferential wall. For example, the deformable material can be disposed within a groove on the outer surface of the circumferential wall. Alternatively, the deformable material can be disposed as a layer covering at least a portion of the outer surface of the circumferential wall. In one embodiment, the deformable material can be a foil made of Ag or Sn.

[0050] The electrical connection between the connector and the macrostructure may alternatively or additionally be made by welding or soldering a portion of the macrostructure and the connector along a portion of the interference fit.

[0051] The connector may form an electrical connection with the at least one macrostructure at a temperature exceeding 100°C, preferably 300°C.

[0052] The engagement means may be formed as a through-hole in the connector to allow a portion of the macrostructure to partially extend through the connector when attached by an interference fit. The macrostructure may be attached flush on one side of the connector, for example, with a first end, while a portion of the macrostructure having a second end extends from an opposite side of the connector. In an alternative embodiment, the engagement means may be formed as a cavity in the connector to allow a portion of the macrostructure to be partially inserted into the connector when attached by an interference fit.

[0053] In a preferred embodiment, the at least one macrostructure is substantially square in a cross-section perpendicular to the longitudinal direction. However, it should be understood that the at least one macrostructure may also have other cross-sectional shapes, such as triangle, circle, ellipse, pentagon, hexagon, other polygons, etc.

[0054] In a preferred embodiment, the inner surface of the engaging means forms an engaging space that is substantially square in cross-section perpendicular to the longitudinal direction, thereby matching the preferred shape of the outer surface of the circumferential wall of the macrostructure. However, it should be understood that the inner surface of the engaging means may also form an engaging space having other cross-sectional shapes, such as triangular, circular, elliptical, pentagonal, hexagonal, or other polygonal shapes, to match the shape of the outer surface of the circumferential wall.

[0055] The connector includes at least two engagement devices, such as two engagement devices, three engagement devices, four engagement devices or even more engagement devices. The engagement devices are arranged to allow the macrostructures attached to the connector to extend substantially parallel to each other when each macrostructure is attached to the connector by an interference fit between the inner surface of the engagement device and the outer surface of the circumferential wall. Thus, two macrostructures can be attached and can extend substantially parallel to each other. In an embodiment where the connector includes three engagement devices, three macrostructures can be attached and can extend substantially parallel to each other.

[0056] In one embodiment, the connector is attached to at least two macrostructures at a first distance from the first end, and the additional connector is attached to the outer surface of the circumferential wall of the macrostructures at a second distance from the second end. The distance between the connector and the additional connector is at least twice the first distance and at least twice the second distance. The first distance and / or the second distance can be approximately zero, whereby at least one of the connector and the additional connector is attached to the at least two macrostructures such that at least one of the connector and the additional connector is flush with the first end and the second end, respectively.

[0057] It should be understood that the connector as an example can be attached to a first macrostructure and a second macrostructure of a structural catalyst comprising more than two macrostructures. Additional connectors can also be attached to the first macrostructure and the second macrostructure. However, in an alternative embodiment, additional connectors can be attached to the second macrostructure and the third macrostructure, wherein the numbering of the macrostructures corresponds to the order of the macrostructures arranged in a row perpendicular to the longitudinal direction. Thus, the first macrostructure is arranged adjacent to the second macrostructure, which is arranged between the first macrostructure and the third macrostructure. The fourth macrostructure can be arranged adjacent to the third macrostructure. Two macrostructures arranged adjacent to each other when attached to the connector can be referred to as adjacent macrostructures.

[0058] In a preferred embodiment, the connector is attached to at least one macrostructure at a first end, and the additional connector is attached to at least one macrostructure at a second end.

[0059] The additional connector is formed of a conductive material to form an electrical connection between two adjacent macrostructures.

[0060] The connector can be arranged such that when two macrostructures are attached to the connector by an interference fit, two engagement devices arranged adjacent to each other are arranged with a gap distance in the range of 2 mm to 10 mm to provide a gap in the same range between the two macrostructures. The gap distance can depend on at least one of the size of the macrostructure, the size of the connector, the size of the reactor in which the structured catalyst is used, and the process type, such as the temperature range.

[0061] In addition to attaching a connector to two or more macrostructures so that the macrostructures extend substantially parallel, it is also possible to attach two or more macrostructures to the connector so that the macrostructures extend in a longitudinal direction; that is, to extend the length of one or more macrostructures. This can be achieved by attaching at least two macrostructures to each other in a longitudinal direction via a connector, wherein the connector is attached to a first end of one of the macrostructures and a second end of another of the macrostructures by an interference fit between an inner surface of a coupling device and an outer surface of a circumferential wall of the two macrostructures.

[0062] In a preferred embodiment, the thermal expansion coefficient of the material of the connector is equal to or less than the thermal expansion coefficient of the material of the circumferential wall of the macrostructure. Thus, it is possible to maintain an interference fit at higher temperatures during use of the structured catalyst.

[0063] The connectors may be formed from an alloy comprising one or more substances selected from the group consisting of Fe, Cr, Al, Co, Ni, Zr, Cu, Ti, Mn, and Si. One or more connectors may be coated with a ceramic coating to electrically isolate one connector from another.

[0064] The connector may have a thickness, defined as a dimension of the connector from the inner surface to the outer surface in a direction perpendicular to the inner surface, in the range of 1 mm to 10 mm.

[0065] The connector may have a height, defined as a dimension of the connector along the longitudinal direction, in the range of 3 mm to 50 mm.

[0066] In a preferred embodiment, the conductive material of the macrostructure is an alloy comprising one or more substances selected from the group consisting of Fe, Cr, Al, Co, Ni, Zr, Cu, Ti, Mn and Si.

[0067] The macrostructure may have a length, defined as the dimension of the macrostructure in the longitudinal direction, in the range of 0.1 m to 5 m. In embodiments where two macrostructures are connected in the longitudinal direction by a connector, the extended macrostructure may therefore have a length of up to 10 m.

[0068] A reactor system for performing an endothermic reaction of a feed gas is provided, the reactor system comprising:

[0069] a) a structured catalyst as described above;

[0070] b) a pressure housing containing the structured catalyst, the pressure housing comprising an inlet for admitting a feed gas and an outlet for admitting a product gas, wherein the inlet is positioned such that the feed gas enters the structured catalyst at a first end and the product gas exits the catalyst from a second end; and

[0071] c) A thermal insulation layer between the structured catalyst and the pressure housing.

[0072] It should be understood that the skilled artisan will readily recognize that any of the features described in conjunction with the structured catalyst may also be combined with a reactor system to perform the endothermic reaction of a feed gas, and vice versa.

[0073] The structured catalyst is very suitable for use in a reactor system for carrying out an endothermic reaction of a feed gas. Therefore, the above description of the structured catalyst is also applicable to the reactor system.

[0074] The reactor system layout allows for the introduction of pressurized feed gas into the reactor system at its inlet and directing the gas into the reactor system's pressure housing. Within the pressure housing, a configuration of insulation and inert materials is arranged to direct the feed gas through channels in the structured catalyst, where it comes into contact with the ceramic coating and the catalytically active material supported thereon, which promotes the steam reforming reaction. Furthermore, heating of the structured catalyst supplies the heat required for the endothermic reaction. Product gas from the structured catalyst is directed to the reactor system outlet.

[0075] In a specific embodiment of the present invention, the reactor system includes at least two conductors connected to the structured catalyst to allow connection to a power source. When the pressure housing includes an inlet for admitting process gas and an outlet for allowing product gas to exit, wherein the inlet is positioned so that the feed gas enters the structured catalyst at a first end of the structured catalyst and the product gas exits the structured catalyst at a second end of the structured catalyst, and when the at least two conductors are connected to the structured catalyst at a location on the structured catalyst closer to the inlet than to the outlet, the at least two conductors can be placed in a relatively cooler portion of the reactor system. The first end of the structured catalyst has a lower temperature than the second end of the structured catalyst for the following reasons:

[0076] - the feed gas directed through the inlet can cool the at least two conductors before being heated by the structured catalyst further along the path of the gas through the structured catalyst;

[0077] - the temperature of the feed gas entering the first end of the structured catalyst will be lower than the temperature of the product gas leaving the second end of the structured catalyst due to the heat supplied electrically to the structured catalyst,

[0078] -The endothermic nature of the steam reforming reaction absorbs heat,

[0079] - The structured catalyst is configured to direct an electrical current from one conductor to substantially the second end of the structured catalyst and back to the second of the at least two conductors.

[0080] In one embodiment, at least one of the conductors is connected to a conductor connector. Thus, the conductor connector can include a conductor contact rail for connecting the conductors. In a specific embodiment, the conductor connector includes a first engagement device for engaging the outer surface of the circumferential wall of the first macrostructure. In a specific embodiment, the engagement device has an inner surface having a shape that matches at least a portion of the outer surface of the circumferential wall. In a specific embodiment, the engagement device is attached to the outer surface of the circumferential wall via an interference fit.

[0081] The temperature profile in the structured catalyst can correspond to a substantially continuously increasing temperature along the path of the feed gas through the structured catalyst.

[0082] The reactor system of the present invention does not require a furnace, which significantly reduces the overall reactor size. Furthermore, the advantage is that the amount of synthesis gas produced in a single pressure shell is significantly increased compared to known tubular steam reformers. In standard tubular steam reformers, the amount of synthesis gas produced in a single tube of the tubular steam reformer is as high as 500 Nm 3 / h. In contrast, the reactor system of the present invention is arranged to produce up to or greater than 2000 Nm 3 / h, for example, even up to or greater than 10000 Nm 3 / h (synthesis gas). This can be done with no O2 in the feed gas and with less than 10% methane in the produced synthesis gas. When a single pressure vessel accommodates a 3 / h of synthesis gas, it is no longer necessary to provide a plurality of pressure shells or a device for distributing the feed gas to a plurality of such individual pressure shells.

[0083] Another advantage of the reactor system is that, since the structured catalyst comprises a macrostructure, the flow through the structured catalyst within the reactor system can be upward. Alternatively, the flow through the structured catalyst can be in a horizontal direction or any other suitable direction. This is more difficult in the case of reactors containing pellets due to the risks of fluidization, grinding and blowing out of the particles. Thus, a large amount of piping can be avoided, thereby reducing plant costs. In addition, the possibility of upward or horizontal flow increases the flexibility of plant design.

[0084] Furthermore, it should be noted that the phrase "at least two conductors are connected to the structured catalyst at a location on the structured catalyst that is closer to the first end of the structured catalyst than to the second end of the structured catalyst" is intended to mean that both or all of the at least two conductors are connected closer to the first end of the structured catalyst than to the second end. Preferably, the at least two conductors are connected to the first end of the structured catalyst or within a quarter of the length of the macrostructure closest to the first end.

[0085] Provided is a use of the structured catalyst or the reactor, wherein the endothermic reaction is selected from the group consisting of steam methane reforming, hydrogen cyanide formation, methanol cracking, ammonia cracking, reverse water gas shift and dehydrogenation.

[0086] It should be understood that the skilled person will readily recognize that any features described in conjunction with the structured catalyst and reactor system for carrying out the endothermic reaction of the feed gas are applicable to this use. Therefore, the above description of the structured catalyst and reactor system is also applicable to its use.

[0087] Detailed description of the accompanying drawings:

[0088] The same reference numerals refer to the same elements throughout the drawings.

[0089] Figure 1a A cross-section of an embodiment of a reactor system 100 according to the present invention is shown. The reactor system 100 includes a structured catalyst 10 arranged as an array of macrostructures 5. Each macrostructure 5 in the array is coated with a ceramic coating impregnated with a catalytically active material. The reactor system 100 also includes conductors 40, 40' connected to a power source (not shown in the figure) and connected to the structured catalyst 10 (i.e., the array of macrostructures). The conductors 40, 40' are guided through the wall of the pressure housing 20 containing the structured catalyst via fittings 50 and are guided through the insulating material 30 on the inside of the pressure housing. The conductor 40' is connected to the array of macrostructures 5 by a conductor contact rail 41.

[0090] In one embodiment, the power supply supplies a voltage of 26 V and a current of 1200 A. In another embodiment, the power supply supplies a voltage of 5 V and a current of 240 A. The current is led to the conductor contact rail 41 through the electrical conductors 40, 40', and the current is passed through the structured catalyst 10 from a conductor contact rail 41 (e.g., from Figure 1a The conductor rail (see left in the figure) flows (runs) to another conductor rail 41 (e.g. Figure 1a The current can be either an alternating current, flowing, for example, alternately in two directions, or a direct current, flowing in either direction.

[0091] Macrostructure 5 is made of a conductive material. Kanthal (chrome-aluminum-cobalt-iron) alloy, composed of aluminum, iron, and chromium, is particularly preferred. A ceramic coating (e.g., an oxide) applied to structured catalyst 5 is impregnated with a catalytically active material. Conductors 40, 40' are made of materials such as iron, aluminum, nickel, copper, or alloys thereof.

[0092] During operation, feed gas enters the reactor system 100 from above, as indicated by arrow 11. Product gas exits the reactor system from the bottom of the reactor system, as indicated by arrow 12.

[0093] Figure 1b Shown Figure 1a The reactor system 100 wherein a portion of the pressure shell 20 and the insulation 30 are removed, and Figure 2 is an enlarged view of a portion of the reactor system 100. Figure 1b and Figure 2 The connection ratio between the conductor 40' and the conductor contact rail 41 is Figure 1a . In addition, it can be seen that the conductor 40 is guided through the wall of the pressure housing in the fitting 50 and that one conductor 40 is divided into three conductors 40' within the pressure housing. It should be noted that the number of conductors 40' can be any suitable number, such as less than three or even more than three.

[0094] exist Figure 1a 、 Figure 1b and Figure 2 In the reactor system shown, conductors 40, 40' are guided through the wall of the pressure shell 20 containing the structured catalyst via fittings 50 and are guided through the insulating material 30 on the inside of the pressure shell. As shown by arrow 11, the feed gas for the endothermic reaction enters the reactor system 100 via the inlet on the upper side of the reactor system 100, and as shown by arrow 12, the product gas leaves the reactor system 100 via the outlet at the bottom of the reactor system 100. In addition, one or more additional inlets ( Figures 1a to 2An additional inlet (not shown) is advantageously located adjacent to or in combination with the fitting 50. Such an additional inlet allows cooling gas to flow over, around, near, or within at least one conductor within the pressure housing to reduce heating of the fitting. The cooling gas may be, for example, hydrogen, nitrogen, methane, or a mixture thereof. The temperature of the cooling gas entering the pressure housing may be, for example, approximately 100°C.

[0095] exist Figures 1a to 2 In the reactor system 100 shown, the inert material ( Figures 1a to 2 The inert material (not shown) is advantageously present between the lower side of the structured catalyst 10 and the bottom of the pressure shell. In addition, an inert material is advantageously present between the outer side of the structured catalyst 10 of the macrostructure 5 and the insulating material 30. Thus, one side of the insulating material 30 faces the inner side of the pressure shell 20, and the other side of the insulating material 30 faces the inert material. The inert material is, for example, a ceramic material and can be in the form of particles. The inert material helps control the pressure drop across the reactor system 100 and helps control the flow of gas through the reactor system 100 so that the gas flows on the surface of the structured catalyst 10.

[0096] Figure 3 A structured catalyst is shown comprising six macrostructures 5 and four connectors 60, 60'. The macrostructures 5 extend in a longitudinal direction from a first end to a second end, as indicated by arrows 16. The first end 61 forms an inlet for the feed gas to the macrostructure, and the second end 62 forms an outlet for the product gas.

[0097] The macrostructure 5 comprises a circumferential wall 65 surrounding the interior space. The connector 5 comprises first engagement means 67 for engaging the outer surface of the circumferential wall 65 of the first macrostructure (see e.g. Figure 4 and Figure 5 ). The engagement means 67 are formed as through holes in the connectors 60, 60' to allow a portion of the macrostructure 5 to partially extend through the connector 60 when attached by an interference fit.

[0098] The engagement means 67 has an inner surface having a shape matching at least a portion of the outer surface of the circumferential wall 65. The engagement means 67 is attached to the outer surface of the circumferential wall 65 by an interference fit.

[0099] The additional connector 68 is attached at the second end 62 to the outer surface of the circumferential wall 65 of two adjacent macrostructures 5 .

[0100] The connectors 60 , 60 ′ are attached to the macrostructure 5 at a first distance of approximately 10 mm from the first end. The additional connector 68 is attached to the macrostructure 5 such that the additional connector 68 is flush with the second end 62 .

[0101] To simplify the drawings, Figure 3 The flow channel structure of the macrostructure 5 is omitted.

[0102] Figure 4 An embodiment of a connector 60 is shown. The connector 60 shown comprises two engagement means 67. When each macrostructure 5 is attached to the connector by an interference fit between the inner surface of one of the engagement means 67 and the outer surface of the circumferential wall, the engagement means 67 are arranged substantially parallel to each other in a direction substantially perpendicular to the longitudinal direction, allowing the two macrostructures 5 to extend substantially parallel to each other.

[0103] When two adjacent macrostructures are attached to the connector 60 by interference fit, the connector 60 is provided with a gap distance (as indicated by arrow 17) in the range of 2 mm to 10 mm to provide a gap in the same range between the two adjacent macrostructures.

[0104] The interference fit is facilitated by manufacturing the connector with a tapered lower portion 67A to facilitate guiding the macrostructure into a tight fit position in the connector.

[0105] Figure 5 An embodiment of a connector 60' is shown. The connector 60' shown comprises a single engagement means 67. The engagement means 67 is configured for attaching a single macrostructure 5 by an interference fit between an inner surface of one of the engagement means 67 and an outer surface of the circumferential wall.

[0106] The connector 60' further comprises a flange 69. The flange 69 may comprise conductor contact rails (41, not shown) for connecting conductors (40, 40', not shown).

[0107] The illustrated embodiment of the macrostructure 5 has a substantially square cross section perpendicular to the longitudinal direction. The engagement means 67 is substantially square in a cross section perpendicular to the longitudinal direction, thereby matching the shape of the outer surface of the circumferential wall 65 of the macrostructure 5 .

[0108] The interference fit is facilitated by manufacturing the connector with a tapered lower portion 67A to facilitate guiding the macrostructure into a tight fit position in the connector.

[0109] Figure 6 A structured catalyst 10 is shown that includes a plurality of macrostructures 5 and a plurality of connectors 60, 60', 60". attached to the macrostructures 5. Some of the connectors 60, 60' are connected to the macrostructures 5. Figure 4 、 Figure 5 and Figure 6 The connectors 60, 60' shown in FIG. 5 are identical. An alternative connector 60" for extending the macrostructure 5 is also shown.

[0110] Figure 7a A connector 60" is shown, to which two macrostructures 5 are attached to extend the length of the macrostructures 5 in the longitudinal direction. The two macrostructures 5 are attached to each other in the longitudinal direction via the connector 60", wherein the connector 60" is attached to a first end of one of the macrostructures 5 and to a second end of the other of the macrostructures 5 by an interference fit between an inner surface of a coupling device 67 and an outer surface of a circumferential wall 65 of the two macrostructures.

[0111] Figure 7b Shown Figure 7a A cross-sectional view of the connector 60" is shown in FIG.

[0112] In the embodiment shown, connector 60" connects two macrostructures 5. It will be understood that connector 60 and connector 60" can be combined to provide alternative embodiments of connectors that provide the possibility of extending the length of microstructures while arranging them in parallel and attaching them to each other.

[0113] The interference fit is facilitated by making the connector with a lower portion 67A and an upper portion 67A that are both tapered to facilitate guiding the two macrostructures into a tight fit position in the connector, thereby providing an extended macrostructure.

[0114] Figure 8 Another embodiment of a connector 60A is shown. The connector 60A includes lugs 72, which enable the connector 60A and the structured catalyst to be lifted by using the lugs 72. The macrostructure 5 can be attached to the connector 60A by an interference fit between the engagement means 67 and the outer surface of the circumferential wall of the macrostructure.

[0115] Figure 9 Another embodiment of a connector 60B is shown. Connector 60B includes engagement means 67 for attaching a macrostructure (not shown). Connector 60B includes additional engagement means 67' in the form of engagement angles. When the macrostructure has been inserted into the through-hole of connector 60B, engagement angles 67' can be squeezed to further secure the macrostructure to connector 60B.

[0116] Figure 10 A structured catalyst 10 is shown comprising a plurality of macrostructures 5 connected by a plurality of connectors 60 , 60 ′, 60 ″ attached to the macrostructures 5 . The flange 69 is used to connect to an external power source via a rod 74 and a conductor contact rail (not shown). In addition, the flange 69 is used to connect two adjacent macrostructures 5 via a rod 76 .

Claims

1. A structured catalyst for catalyzing an endothermic reaction of a feed gas to convert it into a product gas, the structured catalyst comprising at least two macrostructures of an electrically conductive material and at least one connector attached to the at least two macrostructures, wherein: The macrostructure supports catalytically active material, and the macrostructure extends in a longitudinal direction from a first end to a second end, wherein the first end forms an inlet for the feed gas to pass into the macrostructure, and the second end forms an outlet for the product gas, the macrostructure includes a circumferential wall surrounding an interior space, wherein the connector includes a joining device for joining the outer surface of the circumferential wall of the macrostructure, wherein the joining device has an inner surface, and the inner surface has a shape that matches at least a portion of the outer surface of the circumferential wall, wherein the joining device is attached to the outer surface of the circumferential wall by an interference fit, wherein the connector includes at least two joining devices, each of the joining devices joins one of the at least two macrostructures to attach the at least two macrostructures to each other, and wherein the inner surface of the joining device is arranged to allow the macrostructure to extend parallel to the longitudinal direction.

2. The structured catalyst according to claim 1, wherein The outer surface of the circumferential wall is deformed by the interference fit.

3. The structured catalyst according to any one of claims 1 to 2, wherein The electrical connection between the connector and the macrostructure is implemented by a deformable material arranged in at least a portion of the circumferential wall.

4. The structured catalyst according to any one of claims 1 to 2, wherein The electrical connection between the connector and the macrostructure is implemented by welding the connector and the macrostructure along a portion of the interference fit.

5. The structured catalyst according to any one of claims 1 to 2, wherein The connector forms an electrical connection with the at least two macrostructures at a temperature exceeding 100°C.

6. The structured catalyst according to any one of claims 1 to 2, wherein The engagement means is formed as a through hole in the connector to allow a portion of the macrostructure to extend partially through the connector when attached by the interference fit.

7. The structured catalyst according to any one of claims 1 to 2, wherein The at least two macrostructures include a plurality of inner walls in the interior space, the plurality of inner walls forming a plurality of flow channels from the first end to the second end.

8. The structured catalyst according to any one of claims 1 to 2, wherein The at least two macrostructures are substantially square in cross section perpendicular to the longitudinal direction.

9. The structured catalyst according to any one of claims 1 to 2, wherein An inner surface of the engaging means forms an engaging space which is substantially square in a cross section perpendicular to the longitudinal direction.

10. The structured catalyst according to any one of claims 1 to 2, wherein The connector is attached to the at least two macrostructures at a first distance from the first end, and wherein an additional connector is attached to the outer surface of the circumferential wall of the macrostructure at a second distance from the second end, wherein the distance between the connector and the additional connector is at least twice the first distance and at least twice the second distance.

11. The structured catalyst according to any one of claims 1 to 2, wherein The engagement means are arranged at a gap distance in the range of 2 mm to 10 mm to provide a gap between the macrostructures in the same range.

12. The structured catalyst according to claim 10, wherein The additional connector is formed of a conductive material to form an electrical connection between two adjacent macrostructures.

13. The structured catalyst according to any one of claims 1 to 2, wherein At least two macrostructures are attached to each other in the longitudinal direction via a connector, which is attached to a first end of one of the macrostructures and a second end of the other of the macrostructures by interference fit between an inner surface of the joining device and an outer surface of a circumferential wall of the two macrostructures.

14. The structured catalyst according to any one of claims 1 to 2, wherein The connector is formed of an alloy including one or more substances selected from the group consisting of Fe, Cr, Al, Co, Ni, Zr, Cu, Ti, Mn and Si.

15. The structured catalyst according to any one of claims 1 to 2, wherein The thermal expansion coefficient of the material of the connector is equal to or smaller than the thermal expansion coefficient of the material of the circumferential wall of the macrostructure.

16. The structured catalyst according to any one of claims 1 to 2, wherein The thickness of the connector is defined as a dimension of the connector from the inner surface to the outer surface in a direction perpendicular to the inner surface, and the thickness is in a range of 1 mm to 10 mm.

17. The structured catalyst according to any one of claims 1 to 2, wherein The height of the connector is defined as a dimension of the connector along the longitudinal direction, and the height is in the range of 3 mm to 50 mm.

18. The structured catalyst according to any one of claims 1 to 2, wherein The conductive material is an alloy including one or more substances selected from the group consisting of Fe, Cr, Al, Co, Ni, Zr, Cu, Ti, Mn and Si.

19. The structured catalyst according to any one of claims 1 to 2, wherein The length of the macrostructure is defined as the dimension of the macrostructure in the longitudinal direction, and the length is in the range of 0.1 m to 5 m.

20. The structured catalyst according to any one of claims 1 to 2, wherein The endothermic reaction is selected from the group consisting of steam methane reforming, hydrogen cyanide formation, methanol cracking, ammonia cracking, reverse water gas shift, and dehydrogenation.

21. A reactor system for performing an endothermic reaction of a feed gas, the reactor system comprising: a) a structured catalyst according to any one of claims 1 to 20; b) a pressure housing containing the structured catalyst, the pressure housing comprising an inlet for admitting the feed gas and an outlet for allowing the product gas to exit, wherein the inlet is positioned such that the feed gas enters the structured catalyst at a first end and the product gas exits the catalyst from a second end; as well as c) A thermal insulation layer between the structured catalyst and the pressure housing.

22. The reactor system of claim 21, wherein: The endothermic reaction is selected from the group consisting of steam methane reforming, hydrogen cyanide formation, methanol cracking, ammonia cracking, reverse water gas shift, and dehydrogenation.

Images