Reactor with microstructure arrangement

Abstract

The invention relates to a reactor with a multilayer structure. According to the invention, the multilayer structure has a required number of individual segments which are arranged one above the other and / or adjacent to one another and are connected to one another, which segments are produced from a diffusion-welded stack of microstructured metal sheets, the distribution channel for the cooling medium being deflectable at least twice, and wherein the coolant is initially introduced only laterally into the end metal plates of the stack in a transverse flow manner transverse to the flow direction of the process fluid, after which the cooling fluid is deflected in the direction of the stack and distributed onto a plurality of reaction regions within a segment; the invention also relates to a method for producing a reactor, preferably a (micro) structured reactor, comprising a layer for the flow of a reaction medium and for the flow of a heat transfer medium.

Description

[0001] All documents cited in this application are incorporated herein by reference in their entirety.

[0002] The present invention relates to a reactor having a multilayer structure, the multilayer structure having a desired number of individual segments stacked one above the other and / or adjacent to one another and connected to one another, the individual segments being made of a diffusion-welded stack of microstructured metal plates, wherein the distribution channels for the coolant are preferably deflected at least twice, and wherein preferably the coolant is initially introduced laterally only in a transverse flow manner perpendicular to the flow direction of the process fluid into the region produced by the end metal plates of the stack, and subsequently the coolant is deflected in the stack direction and distributed over a number of reaction zones of a segment; the present invention also relates to a method for producing a reactor, preferably a (micro)structured reactor, which comprises layers for the flow of the reaction medium on the one hand and for the flow of the heat transfer medium on the other hand. Background Art

[0003] In a (micro)structured reactor, a solid catalyst can be introduced as a layer or as a particulate packing. Such reactors are typically used for fast, highly exothermic reactions in order to ensure effective heat supply or heat dissipation by means of a layer structure (i.e., by alternatingly arranging layers of the reaction medium flow and layers of the heat transfer medium flow), so that the reaction can be operated as close as possible to the temperature setpoint.

[0004] When applying such microstructured reactors, it is known to be important that all structures, whether in the form of grooves or channels, achieve a uniform flow field. In addition to the influence of manufacturing tolerances on the effective hydraulic diameter, which significantly affects the flow resistance and thus directly affects the volumetric flow rate in corresponding parallel structures in the case of a common inlet and outlet (Pfeifer et al., Characterization of flow distribution in microchannel reactors, AIChE J, pp. 418 - 425, 2004), the flow conditions of multiple structures are also related to the uniform application of the working fluid (Pfeifer et al., Hot-wire anemometry for experimental determination of flow distribution in multilayer microreactors, Chemical Engineering J 135S (2008), pp. 173 - 178). If the parallel structures are filled with catalytically active material, as narrow a particle size distribution as possible is advantageous so that the local porosity in the entire particle bed is as uniform as possible during filling, and thus a uniform distribution of the mass flow rate over the parallel structures can be achieved. In the case of a corresponding high pressure drop in the particle bed, the influence of the external flow conditions on the uniform distribution is almost negligible.

[0005] This is also described in US Patent US10335759 B1, where ultrasonic waves and the fluidized state of the particle bed are used to achieve the most uniform distribution of catalyst particles possible. However, in addition, the size of the channels into which the particles are introduced is equally important for the uniform distribution of the material flow, as are the channels running in parallel for cooling or heating the reaction. In channels filled with particles, the ratio of the volume in which the particles are in contact with the walls to the volume in which there is particle-to-particle contact increases as the channels become smaller. This applies in particular to channel-particle size ratios of 2 - 10, which may be the case in microchannels. This means that even under conditions where the particle structure is the main influencing factor, the dimensional tolerances of the channels themselves have an impact on the uniform distribution. This applies in particular to very fast reactions, in which very short residence times are required and the length of the catalyst bed is quite small. If the size of some of the adjacent channels used for cooling or heating the reaction is smaller than that of the other channels, this will result in a lower mass flow rate for isothermal reactions at these locations, which will have a negative impact on the temperature or temperature distribution required in the reactor.

[0006] When manufacturing a microstructured reactor, the parallelization of channels optimized for heat and mass transfer increases the production rate. Ideally, the production rate increases with the number of channels as long as the mass flow rate is uniformly distributed. Obviously, when the channels are parallelized, the heat transfer between adjacent channels must always be considered, since media must also be supplied to these channels. A cross-flow design is generally most suitable for this purpose, since connections are possible at the sides of the reactor in this design. Corresponding designs are known from many patents, see also German Patent DE 10 2005 022 985 and US Patent US 5249359. Supplying the coolant in a countercurrent or cocurrent arrangement geometrically forces a relatively large area of the channels to operate in a cross-flow manner, at which point heat transfer already occurs. This increases the coolant temperature from the inlet of the heat transfer medium to the location where the countercurrent or cocurrent region is located. In this case, the supply of isothermal coolant for countercurrent or cocurrent depends on the number of lateral reaction channels in the design. This is particularly disadvantageous for very fast reactions with a high heat of reaction. This problem is made more complex by deliberately reducing the pressure loss in the microchannels by shortening the length of the packed bed in the microchannels (and thus also shortening the heat exchange zone). In this regard, the expansion of the external dimensions of a plate stack with microchannels for reaction and integrated cooling is severely restricted both in width and length.

[0007] Since there are also height restrictions for the plattenpakets, the parallelization of reactor modules is generally proposed. This limitation results from the connection technology of the modules, either due to the increasing stress when welding multi-layer stacks of metal plates using a sandblasting process or due to the buckling of the material of the metal plate stack and possible shear failure caused by applying forces to the stack during diffusion welding.

[0008] The need to use multiple reactor modules to achieve high plant capacity results in disadvantages in terms of the required piping and the distribution of flow to the individual reactor modules. Due to the cost advantages of pumps or compressors scaling with throughput, centralized supply to the individual modules is advantageous. Therefore, US Patent US2014 / 0357738A1 proposes integrating the individual metal reactor modules into the same pressure vessel, in which the individual connection areas of the channels are internally sealed relative to the distribution chamber.

[0009] When manufacturing the individual reactor modules and producing microchannels by sheet metal processing or drilling, especially when using individual plates, dimensional tolerances are expected due to the rolling of the plates and due to joining the plates by individual diffusion welding processes. As described above, this can lead to uneven distribution of the process fluid or coolant.

[0010] EP 3 463 642 B1 (wherein, if several reactors are used, they are connected in series), DE 103 39972A1 (wherein the connection is achieved by laser welding) can be considered as further prior art; alternatively, there may also be (with a weaker technical relevance) DE 60 2004 009 360 T2, DE 103 18257A1, EP 1 352 686 A1, DE 10 2004037 059 B4.

[0011] In this regard, based on the known prior art, there is still a considerable need to improve the original prior art.

[0012] Objective:

[0013] Therefore, the object of the present invention is to overcome the disadvantages of the above-mentioned prior art and to provide a reactor in which these problems no longer exist or at least exist only to a rather small extent.

[0014] A reactor design should be sought that avoids the disadvantages of the prior art and improves the known reactors.

[0015] In addition, a manufacturing process should be sought that allows the relatively easy, safe, and economical production of such a reactor.

[0016] Further objects will occur to those skilled in the art when considering the claims and the following description.

[0017] Solution:

[0018] These and other objects, which are obvious to those skilled in the art from this specification, are solved by the subject matter presented in the claims, and the dependent claims represent preferred and particularly advantageous embodiments.

[0019] In the context of the present invention, the front side of the reactor is understood to be the side where the reaction medium / fluid is supplied to the reactor, and the rear side of the reactor is understood to be the side where the reaction medium / fluid is discharged from the reactor.

[0020] Description:

[0021] In particular, the subject matter of the present invention is a method for producing a reactor, preferably a (micro)structured reactor, which reactor comprises layers for the flow of a reaction medium on the one hand and for the flow of a heat transfer medium on the other hand.

[0022] For this purpose, in step a), structured metal plates having the same width and the same depth for each layer are first stacked on top of each other. Preferably, the side lengths of the metal plates are 20 cm to 200 cm. In a preferred embodiment, the metal plates have a thickness of 0.3 mm to 12 mm.

[0023] In an alternative embodiment which is preferred in some variants, structured or unstructured metal plates are also stacked as the topmost and / or lowermost end metal plates (sometimes referred to as end metal plates or end plates).

[0024] The orientation of the metal plates, in particular the classification of the front side and the rear side of each individual metal plate or the classification of both sides, is determined by the structure of the metal plates, and the reactor structure itself is formed by the reaction channels or groups of reaction channels provided. This is because the reaction medium flows through the reactor structure (reaction channels) from one side (front side) to the other side (rear side). The orientation of the other metal plates is necessarily determined by the metal plates containing the reactor structure. This is readily apparent to those skilled in the art.

[0025] In the next process step b), the plates stacked in this way are joined together by diffusion welding.

[0026] In a preferred embodiment of the present invention, in this case the height of the plate stack is at most 1.5 times greater than the length of the longest side (for example, if the side length is 20 cm, the height of the stack is at most 30 cm).

[0027] Next, in step c), the diffusion-welded stack obtained in this way is separated in the width direction into individual segments of the same depth. In some preferred embodiments of the invention, the depth of the individual segments is between 3 cm and 30 cm, and in other embodiments, the depth is between 3.5 cm and 32 cm. It should be noted here that the reaction medium can also be deflected (umgelenkt) between these two sides and does not necessarily flow in a straight line between the two sides. In addition to strictly straight reaction channels, other configurations of reaction channels (preferably zigzag, wavy or meandering) with annular structures are also conceivable. However, a straight reaction channel is most preferred, especially for reactions with short residence times.

[0028] In some embodiments, the depth of the segment is equal to the distance between the front and rear sides of the reactor.

[0029] – This applies in particular to the case of using the following structured metal plates, in which: the reaction channels extend to the edges of the plate.

[0030] – This also applies to the case of using the following structured metal plates, in which: the reaction channels do not extend to the edges of the plate, and after production, the front or rear side of the segment must first be milled until the reaction channels are reached, but milling is not carried out in the edge region and the circumferential edge remains unprocessed (this improves stability and is very suitable for carrying flange connections for jointly supplying the reaction medium). According to the invention, this method is preferred because, among other things, it achieves a good balance between ease of manufacture, stability and functionality. This milling can optionally be carried out before or after the following step d). In some embodiments, it is useful and therefore preferred to carry out the milling after step d) because any unevenness in the segment connection can be eliminated.

[0031] - However, this does not apply to the case where the following structured metal plates are used, in which the reaction channels do not extend to the edges of the plate, and after production, the front and rear sides of the segment must first be milled until the reaction channels are reached, and the surface is completely milled without leaving a circumferential edge.

[0032] Then, in the next process step d), the required number of individual segments obtained in the previous steps are stacked on top of each other and / or adjacent to each other and connected to each other. Preferably, if the order of the plates in the stack is symmetric, i.e., the order when viewed from bottom to top is the same as the order when viewed from top to bottom, the lower end plate of one segment is arranged on the upper end plate of another segment. In other variants, the upper end plate can be arranged on the upper end plate of another segment, or the lower end plate can be arranged on the lower end plate of another segment; there are differences if the order of the plates in the stack is different. In some preferred embodiments, only the stacked arrangement is used. The connection can be carried out by any method, preferably selected from threaded connection, clamping, gluing or circumferential welding, especially circumferential welding.

[0033] Thus, "stacked on top of each other" means that the segments are arranged in an end plate to end plate manner, and "adjacent to each other" means side by side.

[0034] It should be noted that in the case of manufacturing the individual segments by diffusion welding, due to process reasons, it is almost impossible to achieve a maximum height three times the depth of the segment (i.e., a reactor that is no longer usable will be produced), or it will result in severe buckling of the segment. If the height of the plate stack is 1.5 times greater than their width as the maximum side length, and for example, 5 segments are stacked on top of each other in step d), the resulting maximum height of the assembled reactor relative to its width is 7.5.

[0035] In a preferred embodiment of the present invention, before step c) or simultaneously with step c), preferably before step a), grooves are incorporated in the metal plate or the stack, and then in step c) the splitting is carried out along the grooves. Preferably, these grooves can be generated by etching, milling, blanking or other means; in some (additional) preferred variants, they are generated by blanking.

[0036] Therefore, the position of this row of grooves defines the depth of the segments in the finished product.

[0037] In some preferred variants of the present invention, blanking openings are introduced on the side of the metal plate or on the side of the stack at the same height as the grooves. This makes it easier to separate into segments.

[0038] To make separation easier, the grooves are preferably as long and narrow as possible, but should not exceed a certain length. The maximum length is based on the required width of the respective reactor section (i.e., the corresponding group of reaction channels, which can also be referred to as (reactor) modules, even if they only relate to a single structured metal plate), i.e., the width of the corresponding reactor openings (corresponding group of reaction channels) specified in the metal plate. In this case, it is preferred that, when considered individually, the reaction zones generated by the reactor sections in the finished reactor can still achieve efficient cooling in parallel or co-current mode. In some variants, the length of each groove is less than twice the segmentation depth. In a particularly preferred embodiment, the length of the groove is in the range of 1.5 to 15 cm. Thus, in a preferred embodiment of the present invention, one or more preferably two or several such grooves are incorporated in the metal plate or stack, and the ratio of the sum of the lengths of the grooves to the total width of the metal plate is preferably 60% to 90%, more preferably 30% to 70%. In some preferred variants, two or at least two grooves are incorporated, because in these variants, the parallel connection problem of the individual reactor modules integrated in the plate can also be achieved.

[0039] In a preferred embodiment of the present invention, the ratio of the segmentation depth to the groove length (= width of the reactor module) is maintained at 2 to 8. It is also preferred that the reaction zone length (length of the reaction channel) is greater than the length of a single groove, i.e., the corresponding width of the reactor section. In some preferred embodiments, at least one groove area in the corresponding metal plate is located "above" each reaction area. The groove is preferably long enough for all the channels of the reactor module to be located within the groove, i.e., the length of the groove is greater than the width of the area where the channel exits (i.e., greater than the width of one module). However, due to the number of reaction zones in the segmentation (section), especially if the segmentation (section) has more than two grooves or reactor modules, the total width as the sum of all grooves and intermediate areas is significantly greater than the reaction zone length.

[0040] In a preferred embodiment of the present invention, the metal plate used in step a) is approximately square, preferably exactly square. Approximately square means that the aspect ratio is from 1:2 to a maximum of 2:1, preferably from 1:1.3 to 1.3:1, more preferably from 1.15:1 to 1:1.15, particularly preferably from 1.1:1 to 1:1.1, and particularly preferably the exact aspect ratio is 1:1. Of course, manufacturing tolerances may result in slightly different aspect ratios.

[0041] In a further preferred embodiment of the present invention, in the case of using circumferential seam welding in step d), preferably by milling the formed weld seams, the connecting parts of the respective segments obtained in step d) are planarized to form a planar sealing edge.

[0042] In a further preferred embodiment of the present invention, the structured metal plate has edges around its structuring (among other things, such that less deformation occurs during diffusion welding), and after step c) or after step d), preferably after step d), step f) is carried out ("f" stands for milling ), in which the segmented front and rear sides are milled to the openings of the reaction channels. The milling can be carried out over the entire surface or in such a way that a circumferential edge is retained in the formed reactor. The circumferential edge is preferably slightly thinner than the side edges of the structured metal plate (there is still a (small) gap between the corresponding structured side ends and the inside of the circumferential edge).

[0043] In a still further preferred embodiment of the present invention, the flat sealing edges are each adapted to the flange, either in whole or in part.

[0044] In a preferred embodiment of the present invention, the end metal plates are selected and designed such that the coolant can be introduced into their interior in a transverse flow manner transverse to the flow direction of the process fluid. The coolant channels in the end metal plates are further configured such that the coolant is deflected parallel to the stacked height of the segments.

[0045] It is further preferred that the coolant is deflected at least twice in the distribution channels in the reactor. In a particularly preferred exemplary embodiment, the first transverse flow region is achieved by channels with a size of 5 mm to 20 mm. In these embodiments, the secondary distribution in the stacking direction (seen spatially close to each reactor module) is achieved by channels with a size of 2 mm to 10 mm, and after the second deflection back to the transverse flow, it is achieved by channels with a size of 2 mm to 5 mm. In these designs, the actual temperature control channels arranged parallel to the reaction channels usually have a diameter and / or side length of less than 2 mm.

[0046] In a preferred embodiment of the present invention, the end metal plates are selected such that the coolant can flow through regions not close to the reaction channels in a transverse flow manner. The term "close" preferably means a distance of at least 5 mm, preferably between 5 mm and 10 mm here.

[0047] In a preferred embodiment of the present invention, the thickness of the end metal plates (if present) is equal to or greater than 5 mm, preferably 10 mm, and / or less than 80 mm, preferably 70 mm; more preferably between 10 mm and 70 mm, and in some other embodiments between 10 mm and 40 mm; the end metal plates also have inlet openings for the coolant. In some preferred embodiments, these inlet openings can have a diameter of 5 to 20 mm (of course, the diameter of the inlet openings will be adjusted according to the thickness of the plate so that the plate and the opening or channel are stable and closed; this is obvious and achievable for those skilled in the art).

[0048] A further preferred embodiment is that the end metal plates have drilled holes at the same positions.

[0049] In some preferred embodiments, the heating elements are also inserted in the stacking direction. For this purpose, in the preferred embodiments, circular grooves have been provided in the end plates and the plate elements, which can be further drilled after diffusion welding and after connecting the segments if required, in order to achieve a high fitting accuracy between the heating elements and the metal plates in the case of deformation of the openings due to diffusion welding and possible offsets during connecting the segments. Alternatively, but generally less preferred, within the scope of the present invention, continuous drilling can also be carried out only after connecting the segments. In each case, the circular grooves are arranged such that they are located beside or between the reactor zones, i.e., such that no connection is made with the branches of the cooling channels.

[0050] In particular, another subject matter of the present invention is a reactor, characterized in that the reactor has a required number of individual segments, which are stacked on top of each other / or adjacent to each other and connected to each other, in particular stacked on top of each other, wherein the lower end plate of one segment is arranged on the upper end plate of another segment, the segments are made of a diffusion-welded stack of microstructured metal plates, wherein the distribution channels for the coolant are deflected at least twice, and wherein,

[0051] - the coolant is initially introduced laterally only into the end metal plates of the stack in a lateral flow manner transversely to the flow direction of the process fluid, and

[0052] – subsequently, the coolant is deflected in the end metal plates in the stacking direction and distributed over a number of reaction zones within a segment.

[0053] Preferably, the reactor according to the present invention is produced according to the above method.

[0054] Equally important is the use of the reactor according to the present invention or the reactor produced by the method according to the present invention for the Fischer-Tropsch reaction or the methanation reaction, in particular the subject matter of the present invention.

[0055] Regarding the present invention and its advantages, the following can be stated:

[0056] The increase in the plate size and thus the entire welded body, as compared to a number of small individual modules, is advantageous in order to reduce the influence of tolerances resulting from the rolling process of the plate substrate as compared to a number of individual diffusion welding processes for the individual modules. However, due to size limitations, this is not easily achievable. Since for a very rapid reaction, the reactor width must generally be significantly greater than the reactor length, the shape of the individual segments is rectangular. According to the invention, a number of such shapes are arranged in a row until an approximately square shape for diffusion welding is achieved, and then separated into individual parts after the diffusion welding process. Due to the square shape, the plate stack can be higher than in the rectangular shape (reduced risk of shear), which is advantageous for the number of reactor modules. By rotating the individual cut segments by 90° relative to each other, a greater stacking height can be achieved by arranging them and performing a corresponding circumferential seam welding on the contact surfaces, whereby the process fluid can enter or leave the exposed channels at the formed end faces. The invention also includes providing a blanking notch at the location where the welded body is separated in order to facilitate separation. The notch should be as narrow and long as possible; ideally, the ratio of the notch length to the total width of the plate should be 30 - 70%. In addition, it is preferred to have at least two notches instead of a single notch. It has been shown that a ratio of 2 to 8 between the reaction zone length and the notch length is particularly suitable for preventing the plate stack from buckling in the notch. Since all segments are made from a single plate stack, the tolerances during the rolling process and those resulting from the diffusion welding process are reduced. Even if different deformations of the individual plate stacks are obtained when using the same welding parameters (inaccurate temperature measurement at high temperatures, deviations in the steel structure, etc.), the resulting entire body can, due to the circumferential seam welding, be adapted to a flange on its end face after the weld seams have been milled to produce a flat sealing edge, such that the cost required for connection is significantly reduced as compared to a number of individual modules.

[0057] In order to achieve as wide a reactor width as possible, the invention allows the coolant to be deflected at least twice in as wide a distribution channel as possible, whereby the coolant is initially introduced laterally (lateral flow) only into the end metal plates transversely to the flow direction of the process fluid. Then, it is deflected in the stacking direction and distributed to a number of reaction zones within the separated reactor segments. The channel arrangement in the end metal plates, which preferably has a thickness of 10 mm to 40 mm, and the channel arrangement in the region without reaction channels in the direction of the plate stack prevent significant heat exchange of the coolant before it enters each plate of the cooling channels. Finally, a sufficiently high ratio of the length of the catalyst bed to the width of the reaction zone ensures the maximization of the countercurrent / cocurrent flow zones. If the end metal plates of the reactor segments are placed side by side as described above, the heat introduced into the coolant supply line is minimal.

[0058] For the present invention, the reactor size can be maximized with very short reaction channels having lengths in the range of 2.5 cm to 28 cm or 3 cm to 30 cm (these dimensions are related to the depth of each of the above-mentioned segments and depend on whether (and to what extent) milling has to be carried out; if milling is necessary, the segment depth is slightly greater than the reactor channel length).

[0059] Thus, the present invention is in particular based on an optimized manufacturing process for paralleling a plurality of modules, which cannot be obtained from the prior art, and it is thus particularly surprising that the method (and the product formed) of the present invention achieves excellent results.

[0060] By means of the present invention, for reactions with very short residence times, i.e., very short reaction zones, the limitations on the reactor size with respect to the reactor width and the stack height are significantly reduced. At the same time, the distribution of the coolant flow is optimized and the uniform distribution of the process fluid is optimized.

[0061] In the case of the present invention, in particular in the preferred embodiments, the paralleling of several modules is achieved with very short residence times without the use of control fittings or residence elements. The present invention (i.e., in particular the paralleling of the modules, which originally results from the segmentation of the plate stack and by rotating one of the material flows by 90° and distributing it to the individual modules by means of connection techniques) avoids or eliminates the fundamental difficulties (see above) in the overall construction of large devices with very short side lengths. The manufacturing "trick" according to the present invention brings significant economic advantages for plant engineering in terms of saving such fittings.

[0062] A person skilled in the art can precisely design the details of the device (such as dimensions, wall thickness, materials, etc.) that are not explicitly described in this specification within the scope of their general professional knowledge according to the specific reaction conditions to meet the requirements of a specific reaction.

[0063] If, in the description of the device according to the present invention, part or the whole of the device is marked as "consisting of...", this is to be understood as referring to the necessary parts mentioned. Obvious or inherent parts are not excluded, such as pipes, valves, screws, housings, measuring devices, storage containers for segregates / products, etc.

[0064] Unless explicitly described otherwise, the individual parts of the device are operatively connected to one another in a generally known manner.

[0065] The various embodiments of the present invention, for example but not limited to the embodiments of the various dependent claims, can be combined with one another in any way as long as such a combination is not mutually contradictory.

[0066] The present invention will now be explained in more detail with reference to the accompanying drawings. The drawings should not be construed as restrictive and are not drawn to scale. The drawings are schematic and do not include all the features present in conventional devices, but are simplified to the features necessary for the present invention and understanding thereof; for example, screws, connections, etc. are not shown or are not shown in detail.

[0067] In the drawings, the specification and the claims, the same reference numerals denote the same features.

[0068] In the following description, some variants or advantageous and preferred variants / embodiments are also shown, which, unless otherwise stated, are not limited to the corresponding described drawings, but are preferred variants of the present invention itself (unless contradictory).

[0069] Figure 1 There is shown a reactor 1a according to the present invention, the reactor 1a being in the form of a stack 2 of structured metal plates, these metal plates being stacked one above the other, and metal end plates 3 being located at the top and bottom. All these plates are diffusion-welded into a unit. The reactor is shown before being separated into individual segments 6 (in the example shown having three segments). Also visible is the blanking notch 4 along which the segments 6 are separated from one another; the grooves 5 also intended for separation are not visible here, since these grooves do not exist in the cover plates, but only in the intermediate stacked plates (metal plates) (see also Figure 4 and 5 ). Also shown are the reactor openings 10 in the individual structured metal plates. If desired, a catalyst can be placed in these openings during reactor operation. In addition, holes 7 for heating elements are shown in the metal end plates. Also visible are the inlet openings 8 for the coolant, these inlet openings 8 being located laterally here in the end plates 3.

[0070] It should be noted that Figure 1 there is shown an embodiment in which structured metal plates are used for the stack 2, these structured metal plates having reactor openings 10 on the front side (and on the rear side, not shown in the figure). However, in terms of production technology, it is sometimes advantageous if these structures do not extend to the edges, but the edges of the metal plates are continuous (which results in a reduction in deformation during diffusion welding, or allows a higher pressure to be applied to the edges / different precision requirements for the edges during diffusion welding), and is therefore preferred in a variant of the present invention.

[0071] Although it is preferred according to the present invention to separate the individual segments 6 from one another, rearrange them and then use the new arrangement as a reactor, the reactor 1a shown here can also be used in this form; compared with the more preferred embodiments according to the present invention, such a reactor will have a relatively long or deep reactor (in the example shown, three times as long as when the segments are separated).

[0072] Figure 2 shows the reactor 1b according to the present invention, in which the individual segments 6 are separated from each other at the punching opening 4 (and the groove 5 not shown) in the reactor 1a, and then stacked on top of each other again. For the sake of distinction, these segments shown here as being horizontally placed are now referred to as segments 6' (but they are the same segments, just separated from each other). It can be clearly seen that the rearrangement of the segments results in more reaction channels (reactor openings 10) being obtained from the reactor 1a. For reactors with rapid reactions, a relatively shallow depth with correspondingly shorter reaction channels is usually sufficient. The holes 7 for the heating elements can also be seen again here. The inlet opening 8 for the coolant can also be seen again. In the reactor of the present invention, the channels for the reaction medium naturally run through the entire reactor 1a / 1b and do not merely represent holes in the end metal plates 3 of the metal. In Figure 2 In, 3' represents the inner surface of the stack 2 after milling, and in Figure 2 it can be seen that the edges (the edges in the upper left and lower right corners of the figure) are left unprocessed in order to obtain a circumferential edge in which screw holes 9 have been machined (flanges etc. can be attached; for example, a flange for a reaction fluid supply device can be attached). Since it is manufactured by diffusion welding, the end metal plates 3 in this figure can no longer be clearly distinguished from the surrounding edges (the transition part cannot be recognized). It is also clearly visible that various preparation structures 15 designed here as screw holes or notches. These structures can be used to connect the individual segments 6' to each other, or to connect the finished reactor 1b to other workpieces.

[0073] It should be noted that Figure 2 shows a variant of the present invention, in which the individual metal plates of the stack 2 initially and during connection by diffusion welding have no structures at the edges; only after tilting (and preferably after joining), the individual stack segments 6' are milled to the depth of the reactor opening 10, leaving a circumferential edge (i.e., it is not milled on the outside), and then, for example, screw holes 9 (or the like) can be machined into this circumferential edge (as shown here). In this way, the previous diffusion welding can be carried out more easily / effectively, and a uniform surface 3' can be obtained by subsequent milling, so that the arrangement of the supply nozzles can thus be better and / or more precise, and / or the distribution of the reaction medium can be more uniform; in this regard, this is a preferred variant of the present invention.

[0074] Figure 3 shows the reactor 1c according to the present invention, which is very similar to Figure 2 but has slightly different details or representations. Compared with Figure 2, here the end of the heating element as 7a can be seen, and the heating element has been pushed through the reactor (i.e., through the hole 7 for the heating element). In Figure 3 , at the protruding end 7a of the heating element as can be seen, for example, depending on the design of the heating element, a power connection can be provided as the heating element may be electrically powered. Additionally, in an embodiment according to Figure 3 , a common flat sealing surface 21 is placed on three respective segments, which are placed on the edge of the previously machined (milled on the inside) segment surface 3'. In this common flat sealing surface 21, screw holes 9 can again be seen, and these screw holes 9 of course match the screw holes 9 arranged below them, and these lower screw holes 9 have been machined into the side of the partial / end metal plate or segment 6'. This sealing surface 21 can be made of substantially the same material as the metal plate of the reactor, or can be made of other materials (specially) suitable for sealing. In this regard, it is very likely to use materials such as Teflon for this purpose. Furthermore, this figure shows the following variant, wherein: the inlet openings 8 for the coolant (thus no longer visible in this figure) are connected to each other by (e.g., welded) half-pipes 13. In this way, for example, two coolant inlet openings at the same height on one segment can be supplied by a single coolant supply source. For this purpose, for example, the (screw) connection 14 for coolant supply shown here can be used. Although Figure 3 shows three half-pipes 13, which are stacked on top of each other in each segment and have corresponding (screw) connections 14 for coolant supply, these half-pipes can also be replaced by other configurations. For example, instead of three separate half-pipes 13, a kind of cover can be provided only on the side of each segment 6', where the cover, for example, covers all the inlet openings 8 for the coolant, and the cover is provided only with the (screw) connection 14 for coolant supply. Corresponding other configurations are also feasible. In addition to the reactor opening 10 that can be seen again in this figure, the connection parts between the respective segments 6' can also be seen, which are indicated here by the reference numeral 12. In this case, they represent the surrounding welded connection parts that connect the respective segments 6'. Of course, these surrounding welded connection parts 12 have been leveled by milling the stack surface. In the case where the surface is not milled, it is preferred to mill or level such surrounding welded connection parts in order to obtain as flat a surface as possible (which is beneficial for further processing, operating safety, or distribution of the reaction medium).

[0075] Figure 4 An example of a structured metal plate 16 is shown in a plan view. This is an exemplary structured metal plate that can be used in the manufacture of, for example, reactors 1a, 1b, or 1c, except that, for simplicity, Figure 4 , only two segments 6 are shown instead ofFigure 1 、 2And the three segments in 3. Of course, the present invention is not limited to two or three segments 6, but reducing to two or three segments 6 is merely for simplifying the illustration. However, in various preferred variants of the present invention, two segments 6' or three segments 6 are preferably used. This figure shows various drill holes in the structured metal plate 16. These drill holes have two different diameters. The smaller diameter is denoted by the number 7 and correspondingly represents the holes for the heating elements 7, where 12 holes of the smaller diameter can be seen in each segment (divided into three groups of four each). Thus, these holes pass through all the structured metal plates that are to be stacked one above the other in the same position; if the heating elements are to pass through the reactor, the corresponding structured metal plates 16 (and others) to be used have to be manufactured accordingly and it has to be ensured that the drill holes overlap. In this context, it should be noted that in the context of the present invention, it is not mandatory for the heating elements to pass through the reactor; this is merely one of (many possible) variants, and within the context of the present invention, the drill holes / holes 7 are optional and are only absolutely necessary when heating elements are to be used. However, whether or not heating elements are actually used, in some variants it is preferred to provide the holes 7 in order to achieve flexibility in the use of the heating elements (in addition, in some variants, (heated) air can simply pass through the holes or the channels formed by the holes). The additional larger drill holes with the reference numeral 11a represent the openings for the coolant channels perpendicular to the plane layer; when several structured plates that are not necessarily the same are stacked one above the other, the channels themselves are formed, and in this regard as well, it must be ensured that the plates placed one above the other match or adapt to each other in terms of the structure for the coolant (channels) (this is obvious to a person skilled in the art). Then, the coolant can flow through these openings 11a (applications where the coolant does not need to pass through can also be envisioned, and the reactor according to the present invention can of course also be used for such applications). The blanking openings 4 and the grooves 5 are also shown in this figure, and the two segments 6 can be separated from each other along the blanking openings 4 and the grooves 5. The groove 5 has a corresponding groove length A, which in the shown example (preferred embodiment) substantially corresponds to the width B of a single reactor module, i.e., the width of the corresponding reactor channels arranged adjacent to each other within the same segment. In this figure, the reaction zone length of the corresponding reactor module is also shown, denoted by R. In addition, T represents the depth of the corresponding segment 6. This figure shows the structured metal plate 16, where the structuring does not extend to the edges (the upper and lower edges in the figure) (the depth T of the segment 6 is significantly greater than the reaction zone length R of each reactor module), such that after the individual segments 6 are separated from each other (tilted 90°) and joined, the surface of the stack has to be milled until the reactor opening is reached. This is the preferred embodiment of the present invention, but (as already mentioned) within the scope of the present invention, it is entirely possible to extend the structure of each reactor module in the structured metal plate to the corresponding edges of the metal plate, in which case milling will no longer be required.

[0076] It should be noted that, in the context of the present invention, it is not mandatory to machine the surface of the segment 6' by milling to reach the opening of the reactor module. Other known surface removal methods can also be used. However, for practical reasons, milling is generally preferred.

[0077] Figure 5 A top-down perspective view shows how various structured metal plates (16, 17, 18, 19, 20) are stacked on top of each other to form a stack 2 (a part) made of structured metal plates. The structured metal plate 16 corresponds to Figure 4 the metal plate shown. In Figure 5 the case of, the structured metal plate 16 with L' is also shown, where the reaction fluid will flow along L' (in the finished reactor, from the bottom to the top along the linear reactor module structure). Here, among the various structured metal plates, the grooves 5 and the notches 4 are also shown, and the respective segments 6 are then separated from each other along the grooves 5 and the notches 4. The structured metal plate 20 represents a transition plate, which can be structured differently as needed, so that in this example, the exact structure is not shown. The drilled holes or coolant channels 11a perpendicular to the respective plate layers are shown again. In addition, the coolant channels 11b in the respective plate layers are shown. In the structured metal plate 19, the coolant channels 11a perpendicular to the plate layer are connected to the coolant channels 11b located in the plate layer. In this way, the coolant can enter the layer through the coolant channels 11a and then flow along the coolant channels 11b in the layer. Via the coolant channels 11b, the coolant can then enter the next layer, in this case the structured metal plate 18 (in the shown variant, the corresponding structure located in the plate layer is also provided in the metal plate 18, but this is not always the case). Then, in the following structured metal plate 17, the longitudinal flow region of the coolant is denoted by L, that is, in this plate, the coolant is deflected and then flows vertically, for example, in the plate layer. In this regard, by appropriately designed structured metal plates, the coolant can be introduced into the stack 2 of structured metal plates from the bottom side (or the top side) of the reactor, and then deflected in different directions through various deflection mechanisms in the respective plate layers in order to achieve as optimized a coolant distribution as possible. By operating in this way, (partial) cross-flow can be provided, and the cross-flow region is denoted by K here. It should be noted that the schematic order of the structured metal plates shown here or the exact structure of the metal plates is only exemplary, and the present invention is of course not limited to the order of the structured metal plates shown here and the shown structure.

[0078] List of reference signs:

[0079] 1a Reactor (before segment separation)

[0080] 1b Reactor (after segmented separation and rearrangement)

[0081] 1c Reactor (after segmented separation and rearrangement; other design)

[0082] 2 Stack of structured metal plates

[0083] 3 Metal end metal plate (unstructured, only provided with inlet openings for coolant)

[0084] 3' Milled surface of the stack

[0085] 4 Blanking opening

[0086] 5 Groove

[0087] 6 Segment

[0088] 6' Segment, horizontal (after separation)

[0089] 7 Hole for heating element

[0090] 7a Heating element (visible part)

[0091] 8 Inlet opening for coolant

[0092] 9 Screw hole (for attaching flange)

[0093] 10 Reactor opening

[0094] 11a Coolant channel perpendicular to the plate layer

[0095] 11b Coolant channel in the plate layer

[0096] 12 Surrounding welded joint

[0097] 13 Half pipe (welded, connecting the inlet opening for coolant)

[0098] 14 (Screw) connection for coolant supply

[0099] 15 Provide connection (screw hole; notch, etc.)

[0100] 16 Structured metal plate

[0101] 17 Structured metal plate

[0102] 18 Structured metal plate

[0103] 19 Structured metal plate

[0104] 20 Structured metal plate

[0105] 21 Common planar sealing surface (with screw hole 9)

[0106] A Groove length

[0107] Width of the B reactor module

[0108] K Transverse flow cross-section

[0109] L Longitudinal flow of the coolant

[0110] L' Longitudinal flow of the reaction fluid

[0111] R Reaction zone length

[0112] Depth of section 6.

[0113] Example:

[0114] The present invention will now be further explained with reference to the following non-limiting examples.

[0115] A reactor according to the present invention is produced, wherein before segment separation, the segment width of the welded reactor plate stack is 530 mm, the depth of a total of three segments is 580 mm, and the stack height of the end plates is 277 mm. In this case, end plates (3) with a thickness of 50 mm are used. Four reactor modules are integrated into each segment, and after milling, it has a heat transfer area that is 70 mm wide and 120 mm long. Considering the punching notches (4) at the plate edges, the length of each of the four grooves (5) in each segment is 72 mm, making the ratio of the groove to the segment width approximately 60%. The width of the groove is 5 mm. The arrangement of the plates is regular such that the upper and lower end plates can be selectively combined for welding by electron beam welding. In each of the two end plates, three inlet openings (8) with a diameter of 11.3 mm are provided for each segment, and they are 5.3 mm away from the plate stack. From there, the cooling water flow is distributed to the coolant channels with a diameter of 9 mm perpendicular to the plate layer (11a). The coolant channels in the plate layer (11b) are 3 mm wide and 3 mm deep. The coolant channels running in parallel with the reaction channels are 1.5 mm wide and 0.5 mm deep. The reaction channels are 4×4 mm. The diameter of the prefabricated holes for the heating elements (heating cylinders) (7) is 6 mm, and the prefabricated holes are drilled into holes with a diameter of 10 mm. After diffusion welding, the plate stack is only approximately 270 mm high. Therefore, after arranging the segments in a rotating state, the total height of the finished reactor (three times that of segment 6') is 810 mm, and the known width of the segment is 530 mm. During assembly, after rearranging the segments, the distance between the front and rear sides of the segment is approximately 193 mm (the depth of segment 6). Therefore, the ratio of the stack height to the segment depth finally present in the finished reactor is approximately 5.2. Finally, both sides of the reactor are milled over its entire surface such that the maximum depth of the finished reactor is 170 mm. To open the reaction channels, an additional 25 mm is milled on both sides, making the total length of the reaction channels 120 mm. The circumferential edge is used to fix the stud bolts of the continuous flange. The reactor is filled with nickel catalysts with a particle diameter of 300 - 400 μm and is used for the methanation reaction under full-distilled water cooling.

Claims

1. A method for producing a reactor, preferably a (micro)structured reactor, the reactor comprising layers for the flow of a reaction medium on the one hand and for the flow of a heat transfer medium on the other hand, wherein, a) Structured metal plates having the same width and the same depth for each layer are stacked on top of each other; a1) Optionally, one or two structured or unstructured end metal plates are also stacked as the uppermost and / or lowermost end plates; b) The plates stacked in this way are joined to each other by diffusion welding; c) The diffusion-welded stack thus obtained is separated in the width direction into individual segments having the same depth respectively; and d) The required number of individual segments obtained in step c) are placed and joined together in a manner of being stacked on top of each other and / or adjacent to each other.

2. The method according to claim 1, wherein Before or simultaneously with step c), grooves are incorporated in the metal plates or the stack, and then separation is carried out along the grooves in step c).

3. The method according to any one of claims 1 or 2, characterized in that, One or several grooves are incorporated in the metal plates or the stack, wherein the ratio of the sum of the lengths of the grooves to the total width of the metal plates is preferably 60% to 90%.

4. The method according to any one of the preceding claims, in particular claim 1, characterized in that, The ratio of the segment depth to the groove length is maintained at 2 to 8.

5. The method according to any one of the preceding claims, in particular claim 1, characterized in that The metal plates used in step a) are approximately square.

6. The method according to any one of the preceding claims, in particular claim 1, characterized in that, In the case of using circumferential seam welding in step d), preferably by milling the formed weld seams, the connecting parts of the individual segments obtained in step d) are planarized with each other to form planar sealing edges.

7. The method according to claim 7, wherein The planar sealing edges are adapted to flanges.

8. The method according to any one of the preceding claims, in particular claim 1, characterized in that The metal plates are selected and structured such that the coolant in the formed reactor can flow at least partially in a transverse flow manner transverse to the flow direction of the process fluid, and preferably, the coolant can be deflected at least twice within the distribution channels.

9. The method according to any one of the preceding claims, in particular claim 1, characterized in that, The metal plates are selected and structured such that the coolant in the formed reactor can flow in a transverse flow manner through areas not close to the reaction channels.

10. The method according to any one of the preceding claims, in particular claim 1, characterized in that The structured or unstructured end metal plates, if present, have a thickness equal to or greater than 10 mm and preferably have inlet openings for the coolant on the sides.

11. The method according to any one of the preceding claims, in particular claim 1, characterized in that, After step c) or after step d), preferably after step d), f) The front and rear sides of the segments are milled to the openings of the reaction channels.

12. A reactor manufactured according to any one of claims 1 to 11, characterized in that, The reactor has the required number of individual segments, the individual segments are stacked on top of each other and / or adjacent to each other and connected to each other, the individual segments are made of a diffusion-welded stack of microstructured metal plates, and the distribution channels for the coolant are deflected at least twice, and wherein, - The coolant is initially laterally introduced only into the area generated by the end metal plates of the stack in a transverse flow manner transverse to the flow direction of the process fluid, and - Subsequently, the coolant is deflected in the stacking direction and distributed over a number of reaction areas within a segment.

13. Use of the reactor according to claim 12 or a reactor produced by the method according to any one of claims 1 to 11, in particular claim 1, for a Fischer-Tropsch reaction or a methanation reaction.

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