APPARATUS FOR THE INVESTIGATION OF CHEMICAL PROCESSES IN PLATE-SHAPED CELLS

Description

Field of invention

[0001] The present invention relates to an apparatus for investigating chemical processes, a plurality of plate-shaped reaction cells for investigating chemical processes, and a method for investigating chemical processes, with the aid of which process engineering and material-specific optimizations can be carried out simultaneously or in close temporal proximity on a large number of functional elements by varying the process parameters. Background of the invention

[0002] In the field of high-throughput research, there is a continuous need to perform tests and inspections more quickly and efficiently. Particularly in the area of ​​catalyst development and process optimization, it is very time-consuming to integrate the components to be tested into the appropriate apparatus for subsequent testing. For catalyst investigation, devices and procedures, including the necessary software programs, are provided to improve and accelerate research. This makes it possible to replicate technical processes with high accuracy in the laboratory. The large volume of data and the high accuracy help to reduce the number of tests performed at the pilot plant scale. This saves time and energy in product development.

[0003] Devices and methods for investigating chemical processes in the field of high-throughput research have been known in the state of the art for several decades.

[0004] WO-A 2009 / 046944 discloses that tubular reactors can be closed and sealed with a common closure system.

[0005] EP-A 1 256 377 discloses an array with a plurality of vessels, each having a closure element in its outer zone. The closure element is pressed against the outer edge of the vessel. A plurality of vessels are pressurized simultaneously to create a fluid-tight connection.

[0006] CN 11318926 discloses a method for high-throughput screening of catalysts for water electrolysis.

[0007] WO-A 2021 / 048375 discloses a stacking plate reactor used for the investigation of chemical processes, wherein the stacking plate reactor has a plurality of adjacent plate-shaped building blocks.

[0008] WO 2013 / 074551 discloses a capillary flow reactor, also known as a porous flow reactor. These capillary flow reactors, used for chemical and biological multiphase transformations, have a plate-like structure. The reactors can have one or more chambers, with different contacting regions within the chambers for liquids or gases.

[0009] WO 2019 / 0131634 A1 describes electrolysis cells for the electrolysis or co-electrolysis of water or solid oxide fuel cells (SOFCs). Some components of the electrolysis cell are closed with screw connections. In addition to the screw connections, the electrolysis cell also has a piston and a spring or bellows. The piston carries a conduit inside the cell that leads to the reaction chamber. The piston is movable and allows for pressure equalization inside the cell, if required by the reaction processes.

[0010] US Patent 4,756,817 describes an apparatus for pressing and sliding flat, plate-shaped structural elements that include first and second support elements. Side rails are attached to the support elements. The plate-shaped structural elements can be movably arranged and pressed against each other within the apparatus.

[0011] The object underlying the invention is to provide an apparatus and a method to improve electrochemical processes. Summary of the invention

[0012] The present invention provides an apparatus for investigating chemical processes according to the independent claims, wherein further embodiments of the invention are embodied in the dependent claims.

[0013] The tasks mentioned here, and others not mentioned, are solved by the apparatus described below: namely, an apparatus for investigating chemical processes in plate-shaped reaction cells, comprising: a group of plate-shaped reaction cells or a group of stacks of plate-shaped reaction cells, which also include individual plate-shaped reaction cells, and a clamping device that enables independent fixing of the individual plate-shaped reaction cells and stacked plate-shaped reaction cells, wherein the locking system comprises receiving units and a plurality of piston clamping units, the piston clamping units having a common drive system, each plate-shaped reaction cell or each stack of plate-shaped reaction cells having two outer plate surfaces, one outer plate surface being in contact with a receiving unit and the other outer plate surface being in contact with one or more piston clamps of the piston clamping unit, the piston clamping unit being designed toto apply a pressing force to the plate-shaped reaction cells or stacked plate-shaped reaction cells independently of one another, wherein the pressing force acts perpendicular to the plate surface in the direction of the receiving unit, wherein the plate-shaped reaction cells or stacked plate-shaped reaction cells each comprise a plurality of plate-shaped functional elements, wherein the plate-shaped functional elements are catalyst layers, gas diffusion layers, bipolar plates, proton exchange membranes, wherein each plate-shaped reaction cell has at least one inlet for a reactant and at least one outlet for a product, or wherein the stacked plate-shaped reaction cells each have at least one inlet for a reactant and at least one outlet for a product.

[0014] The invention relates to an apparatus for receiving and fixing a plurality of plate-shaped reaction cells by means of a clamping system. The plate-shaped reaction cells each have two outer plate surfaces, one outer surface of which is in contact with a receiving unit and the other outer surface of which is in contact with one or more pistons of a piston clamping element. The movement of the pistons towards the receiving unit exerts a pressing force on the plate-shaped reaction cells, which is directed perpendicular to the plate surface. The receiving unit thus forms a stop against which the plate-shaped reaction cells are pressed.The plate-shaped reaction cells comprise various plate-shaped functional elements, including elements with sealing functions, which are releasably sealed from the environment by pressing force. The interiors of the reaction cells can be supplied with fluids, and electrodes to which a voltage can be applied can also be arranged within these interiors.

[0015] In a preferred embodiment, the piston clamping units have a fluidic drive system, wherein the piston clamping units are connected by lines to a common fluid supply line or to a common fluid supply tank, wherein the common fluid supply line or fluid supply tank is connected to a pressure regulating valve, preferably an equilibar valve, and more preferably a pneumatic or hydraulic fluid, wherein switching valves are arranged in the lines to the common fluid supply line or the common fluid supply tank, and the fluid flow through the fluid line to the piston clamping units can be switched on or off by actuating the switching valves. Switching on means opening the fluid line and switching off means interrupting the fluid line.

[0016] Preferably, the piston compressors are screw-in piston compressors.

[0017] Preferably, the pressure regulator has short settling times. Preferably, the settling times are < 10 seconds, particularly preferably < 1 second, and furthermore preferably < 0.5 seconds. Simultaneously with the short settling times, the pressure regulator has a large dynamic control range in the range of 1 to 500 barg, preferably 5 to 50 barg, wherein the pressure regulator is characterized by high sensitivity and is able to detect pressure changes < 500 mbarg, particularly < 250 mbarg.

[0018] The plate-shaped reaction cells are individually actuated by the pistons of the clamping device. In a preferred embodiment, the pistons of the piston clamping element are moved by a fluidic drive; more preferably, the fluidic drive comprises hydraulic fluid or is a hydraulic actuator. It is preferred that the piston supply lines are equipped with valves. The valve control allows the connection to the supply lines of the individual pistons to be selectively interrupted, thus decoupling the plate-shaped reaction cells from the supply lines. After interruption and decoupling, the selected plate-shaped reaction cells can be removed from the clamping device. The plate-shaped reaction cells can be replaced, or individual elements of the plate-shaped reaction cells can be replaced.Preferably, the fluidic supply lines are connected to a main line equipped with a common pressure regulator, preferably an equilibar pressure regulator. Due to the common pressure regulator, the individual pistons that exert pressing force on the plate-shaped reaction cells are controlled at the same set pressure via the fluidic supply lines connected to the pressure regulator.

[0019] The transmission of the fluidic drive force to the clamps can be structurally implemented via a manifold in which the lines are realized as a sequence of drilled or 3D-printed channels. These channels, together with the valves and screw-in pistons contained within them, form a unit connected to the common supply. Alternatively, the transmission can be implemented as a sequence of pipes connecting the valves and clamps, which are also connected to the common supply. Both variants are functionally equivalent; however, the manifold variant can additionally transmit forces, for example, by forming part of a frame that is necessary in both variants to withstand the fluidically generated force and the resulting counterforces.

[0020] It should be mentioned here that the forces can also be applied electrically through appropriate drives and gearboxes.

[0021] In a preferred embodiment, the fluidic supply lines are fed from a pressure vessel to which a pressure regulator and another fluidic supply line for a compressionally soft fluid are connected. The compressionally soft fluid is, for example, a gas. The advantage of this arrangement is that pressure control can be very precise via the compressionally soft fluid, while the pressing force is exerted via a compressionally stiff fluid, e.g., a liquid. The latter has the further advantage that even the smallest changes in the expansion or compliance of the reaction cell can be detected in the volume of fluid lines filled with the compressionally stiff fluid and sealed off by the switching valves. Thus, pressure measurement in this enclosed volume is also suitable as a detection method for small expansions or compliances, e.g., of the seal closing off the reaction chamber.

[0022] Preferably, the pressing force of the pistons can also be exerted on a stack of plate-shaped reaction cells, making it possible to accommodate multiple stacks of plate-shaped reaction cells in the apparatus. In a further preferred embodiment, the accommodation of several individual plate-shaped reaction cells can be combined with the accommodation of stacks of plate-shaped reaction cells. An advantage is the flexibility of the apparatus in the arrangement of plate-shaped reaction cells. When using plate-shaped reaction cells with predetermined dimensions, a structural modification of the apparatus is very simple, making it easy for the operator to use the apparatus according to the invention for a variety of different processes.Thus, the apparatus according to the invention represents a multifunctional apparatus which is of great technical interest due to its flexibility in handling.

[0023] The plate-shaped reaction cells comprise interchangeable, layered or plate-shaped functional elements. This allows for the particularly easy replacement of elements exhibiting signs of wear. The term "wear" can also refer to the deliberate induction of corrosion, whereby the method is used to replicate or simulate the conditions to which materials are exposed in real-world operation within the laboratory. This includes surface damage to electrodes as well as damage to pipe or container materials, seals, or membranes. Furthermore, the elements of a reaction cell can be combined in various configurations, enabling the performance of a wide range of processes. This also demonstrates the high performance of the apparatus according to the invention. The plate-shaped reaction cells can be operated in parallel or in series.Multi-stage processes can thus be carried out in serially linked reaction cells, or investigations into scaling up processes can be conducted in parallel-linked reaction cells. The apparatus therefore exhibits a very high degree of versatility and efficiency, as modifications and expansions are very easy to handle thanks to the individual seals of the plate-shaped reaction cells. Thus, the apparatus according to the invention is very well suited for screening and optimizing process conditions, surpassing existing apparatuses in terms of ease of handling and flexibility in performance characteristics. The apparatus according to the invention has significant technical benefits, as it provides the basis for 1. optimizing chemical processes based on the use of electric current for the synthesis of chemical compounds, and 2.The aim is to optimize chemical processes in which chemical compounds and molecules are converted into electrical current as fuel. The corrosion that occurs on the electrodes, in the inner walls of the reaction cells, or on the functional elements is part of the electrochemical processes that are subject to targeted investigation and optimization. Improving large-scale processes using renewable energy sources in combination with new process technologies can and will contribute to further reducing CO₂ emissions from the chemical industry. The apparatus according to the invention provides a powerful tool for optimizing these chemical processes.The optimization is time-saving, thanks to modular structural elements in combination with a pressure pressing device that allows individual plate-shaped reaction cells to be sealed and replaced individually, and which is easy to use.

[0024] In a preferred embodiment, the piston tensioning unit of the closure system is characterized in that it comprises one piston tensioner per plate-shaped reaction cell or one piston tensioner per stack of plate-shaped reaction cells. The dimensions and tensioning capacity of the piston tensioner used are matched to the dimensions of the plate-shaped reaction cell in such a way that the apparatus according to the invention has only a small number of piston tensioners, thereby reducing its complexity and improving its handling. Reduced complexity and improved handling are important because the apparatus according to the invention can be used to accommodate a large number of plate-shaped reaction cells.Preferably, the number of plate-shaped reaction cells that can be arranged simultaneously or in parallel in the apparatus and pressed independently with piston clamps is in the range of 2 to 50, more preferably in the range of 2 to 40, and further preferably in the range of 4 to 20.

[0025] Preferably, a force distribution element is arranged at the tip of each piston of the piston clamping device. This force distribution element preferably comprises a ball bearing with at least one ball, which compensates for slight deviations in the parallelism of the piston end face and the outer surface of the reaction cells. The force distribution element offers the advantage that the pressing force is transmitted evenly to the sealing element(s) that seal the interior of the plate-shaped reaction cells from the exterior.

[0026] In a preferred embodiment, the plate-shaped reaction cells are plate-shaped reaction cells for carrying out electrochemical processes, selected from the group consisting of: electrolysis cells, galvanic cells, fuel cells, corrosion tests, current-through batteries, redox flow batteries, e.g., vanadium redox batteries. More preferably, a plate-shaped reaction cell comprises at least two half-cells separated by a partition. Depending on the embodiment, a reaction cell may also have multiple reactant inlets and product outlets.

[0027] A plate-shaped reaction cell, configured as an electrolysis cell or galvanic cell, comprises a separating membrane and electrodes, wherein the reaction cell is divided into half-cells by the separating membrane, and the electrodes are connected to electrical supply lines. Particularly preferably, the plate-shaped reaction cells are configured as electrolysis cells, and it is preferred that the electrodes are connected to current and voltage measuring devices. Furthermore, the apparatus preferably includes online analysis devices from the group of online voltammetry for measuring V / A functions and impedance spectroscopy for measuring high-frequency voltage changes. Very precise measurements can be carried out using the apparatus according to the invention, which is characterized by flexibility and accuracy.Combining electrochemical investigation methods with sensor monitoring of the sealing system of the plate-shaped reaction cells offers synergies. This results from the sensor monitoring's ability to detect changes in the plate-shaped reaction cells that can be correlated with the electrochemical data. This allows for the identification of interfering effects that lead to changes in electrochemical measurement data.

[0028] In a preferred embodiment, each plate-shaped reaction cell has at least one inlet and at least one outlet through which utilities are supplied and product media are discharged. The plate-shaped reaction cell can have a partition in the middle, the partition dividing the cell into half-cells, each half-cell having at least one inlet and at least one outlet.

[0029] In a further embodiment, only one of the two half-cells may have a supply line, while both half-cells have at least one outlet. One of the half-cells may also have two outlets, one for the discharge of liquid fluids and the other for the discharge of gaseous fluids. The outlet may also include a condenser together with a return line, wherein the liquid fluids are separated from the gaseous fluids in the condenser and fed via the return line to the supply line. The returned fluid can then be fed into the interior of the reaction cell together with fresh fluid.

[0030] The plate-shaped reaction cells consist of housing plates that enclose the functional elements. These housing plates include the connections for fluid inlets and outlets, as well as the electrical connections. The connections for the fluid inlets and outlets, as well as the electrical connections, can be routed through the base or the side surfaces of the housing plates. The structural arrangement of the connections depends on the dimensions of the plate-shaped reaction cells and their surrounding environment. Temperature control elements can be present in the vicinity of the plate-shaped reaction cells to enable operation at high temperatures. Cooling elements can also be provided to accelerate the cooling process of the plate-shaped reaction cells.The plate-shaped reaction cells can be equipped with temperature sensors.

[0031] It is preferred that the connections to the fluid supply and return lines are equipped with connection elements that are easy to handle, allowing for the rapid replacement of individual plate-shaped reaction cells. Therefore, it is particularly preferred that the connections be equipped with quick-release couplings. For example, quick-release couplings from Stäubli are especially suitable.

[0032] In a preferred embodiment, the piston or force distribution element is equipped with a sensor that can measure a geometric change in the reaction cell during the reaction. Sensors can be (indirect) force sensors or (direct) measuring sensors such as strain gauges, distance detectors such as ultrasonic or optical barriers, or interference methods. Sensor measurement offers the advantage that the wear of the sealing elements can be monitored and controlled. Direct measurement as a geometric change in the reaction cell has the advantage over the previously described indirect measurement via hydraulic pressure that the measurement can be performed continuously, whereas measuring hydraulic pressure is always linked to the adjustment of the switching valves.

[0033] The parameters influencing long-term performance can be divided into material and process parameters. Material parameters refer to the mechanical and chemical resistance of the functional elements. This includes the surface wettability of the gas diffusion layer, the pressure behavior of the gas diffusion layer, the ionic conductivity of the membrane, and the stability of the sealing elements. Process parameters refer to the process conditions selected for carrying out the process. These include the process pressure, the process temperature, and the fluctuation ranges applied to these process parameters during operation of the reaction cell, as well as the reaction times with which changes in operating conditions occur.In a preferred embodiment of the method, the parallel reaction cells are subjected to a pressing force applied by a common pressure regulator. The pressing force applied to seal each plate-shaped reaction cell must be greater than the internal pressure of each cell. Another advantage is that the individual plate-shaped reaction cells can be used simultaneously under different operating conditions. This allows the individual functional elements to exhibit different wear behavior. In a preferred embodiment, the plate-shaped reaction cells are equipped with force sensors that record the pressing force over time.Equipping the plate-shaped reaction cells with force sensors is advantageous because it makes it possible to control the operation of the individual reaction cells and to register the control data, as well as to perform the investigated process in conjunction with feedback.

[0034] The operating modes of the processes can be divided into break-in and aging process monitoring. These operating modes can be transferred to an automated test system as predefined processes in the form of protocols with a defined processing list. This processing list defines the process engineering and electrical specifications for the test system as a time series. Break-in protocols can be defined so that a desired performance of the reaction cell is achieved after the list has been processed. Process monitoring protocols can be defined so that typical or even rare operating states of a reaction cell are set, and its performance under these operating states is monitored. These operating states can include load changes, such as starting up or shutting down a reaction cell.The long-term behavior of a reaction cell can be investigated under harsher operating conditions, where the protocols used may involve increased operating temperatures or high load cycle frequencies.

[0035] In a preferred embodiment, one or more of the plate-shaped reaction cells have one or more sensors connected to locations within the cell. These sensors are selected from the group consisting of electrochemical dilatometry for characterizing electrode thickness changes, light microscopic characterization, or spectroscopic characterization via optical fibers to electrodes or membranes. Monitoring the interior of the plate-shaped reaction cells during the process is advantageous for ensuring improved process optimization. Synergies arise because the improved monitoring is also coupled with an extended test lifespan, made possible by the individual sealability and resulting interchangeability of the cells.These synergistic effects are also important in high-throughput research, as different process conditions can be tested simultaneously. The plate-shaped reaction cells, which are subjected to particularly demanding process conditions—for example, with regard to temperature or the composition of functional elements—can therefore be individually exchanged.

[0036] In a preferred embodiment of the apparatus, the receiving units are either physically separate units or a single, physically connected unit. If the receiving units are physically separate units, each receiving unit has its own mounting frame, which is connected to a piston clamping unit. If the receiving units are a single, physically connected unit, they share a common mounting frame. Preferably, the piston clamping units are arranged in a common element, with the common mounting frame connecting the receiving units and the common element. The common mounting frame can be advantageous for stabilizing the apparatus. Separate mounting frames can be advantageous for positioning the units at distributed locations.It is also conceivable to combine groups of plate-shaped reaction cells that are present in an apparatus, where the apparatus has, for example, two separate units and one group has a common holding frame.

[0037] In a preferred embodiment of the apparatus, the plate-shaped reaction cells have an inner wetted plate area ranging from 1.5 x 1.5 cm² to 30 x 30 cm², preferably from 2.0 x 2.0 cm² to 25 x 25 cm², and even more preferably from 3.0 x 3.0 cm² to 15 x 15 cm². It should be noted that the dimensions of the plate-shaped reaction cells can also be very small. At the same time, the arrangement is characterized by high accuracy, since the functional elements can be monitored by sensors, allowing for the acquisition of a large number of measurement data. The larger outer plate area is dimensioned to accommodate fluidic and electrical connections.

[0038] When operating individual reaction cells under high load, the functional elements are subjected to greater forces than under low load. In a selected configuration of reaction cells, applying a defined compression or pressing force is important to prevent uncontrolled deformation of the diffusion layer, which could lead to changes in process parameters and the resulting measurement data. Conversely, the behavior of a diffusion layer under different compression levels can be investigated by applying a defined load. Here, suitable cell geometry must ensure that the (in this case constant) sealing force and the (adjustable) compression force of the diffusion layer are decoupled. Forces whose lines of action are perpendicular to each other can be independent of one another.Therefore, a cylindrical reaction cell, sealed similarly to a piston seal on the inside of the cylinder wall, and equipped with a strain gauge on the piston face (perpendicular to the cylinder's inner surface), exhibits strain behavior independent of the sealing force. Another possibility is to measure the strain behavior of an internal diaphragm using a similarly internal sensor. The disadvantage of this method is the external cable routing. A third possibility is to set a negligible internal pressure via appropriately dimensioned inlet, outlet, and discharge lines of the reaction cell. In this case, the negligible internal pressure does not produce any strain changes on the external strain gauge of the reaction cell, which is axially aligned with the clamping device. Strains measured here can only be caused by, for example, swelling behavior of the internal diaphragm.

[0039] Operating the device under a constant pressing force can be significant for the accuracy of the measurement. It is also advantageous that the weakening of the sealing effect can be monitored. Using the apparatus according to the invention, the influence of conditioning and fractures can be recorded and analyzed in the protocol.

[0040] In one example, a plate-shaped reaction cell can be designed as an electrolysis cell. The apparatus, in which several plate-shaped reaction cells are arranged, is then used as an electrolysis cell to investigate the decomposition of water. The separately arranged plate-shaped reaction cells can be in a series or parallel arrangement. A plate-shaped reaction cell designed as an electrolysis cell comprises at least two half-cells separated by a membrane (proton exchange membrane or electrolyte).

[0041] In one embodiment, a plate-shaped reaction cell, acting as an electrolysis cell, can comprise the following functional elements: a partition, catalyst layers, diffusion layers, electrode layers, and sealing elements. Furthermore, the plate-shaped reaction cell includes fluid chambers through which the fluid to be decomposed, in this case water, is passed. The plate-shaped reaction cell comprises at least two housing plates. The fluid chambers can be embedded in the housing plates. In a preferred embodiment, the fluid chambers have a channel-like structure. The channel-like structure improves the residence time behavior of the fluid by guiding each fluid element precisely onto a specific path, preferably one of approximately the same length for all paths. A narrow residence time profile of a reaction mixture is advantageous because it can improve the reaction yield and reduce the proportion of subsequent reactions.The channel-like structure can have one or more channels. The partition is located between the two housing plates, with sealing elements arranged in the edge areas to seal at least the interior from the outside.

[0042] Regarding the term fluid space or supply space, it should be noted that the interiors of the plate-shaped reaction cells can have different structures, which is why they can be referred to as supply spaces or functional spaces.

[0043] The partition wall is bordered on both sides by layers of functional elements, with the partition wall in contact on both sides of the wall surface with the catalyst layer, the diffusion layer, the transport or supply space, and the electrode layers. The sequence of functional elements can vary slightly from reaction cell to reaction cell. For example, functional elements may be grouped together in one layer or merge seamlessly into one another. The catalyst, for instance, may be located in the diffusion layer. The electrode layers may have a mesh-like structure. Furthermore, the electrode layers may also be located on the inner surface of the housing plates.

[0044] In the case of the apparatus with plate-shaped reaction cells for the decomposition of water, at least one half-cell of the plate-shaped reaction cell is equipped with a supply line for water. The protons pass through the partition and are reduced to hydrogen on the cathode side. On the anode side, the water reacts to form oxygen and protons. On the anode side, water is passed through the fluid chamber and a mixture of water and oxygen is passed along the fluid channel. On the cathode side, hydrogen is passed through the fluid chamber.

[0045] In this example, the plate-shaped reaction cells are electrolysis cells for water. The half-cells on the anode side are moistened by the water. The plate-shaped functional elements include catalyst layers, gas diffusion layers, bipolar plates, and proton exchange membranes. A plate reactor comprises at least two housing plates containing plate-shaped functional layers, including sealing elements. The term bipolar plates refers to technical functional elements that spatially separate the reaction cells from the electrical supply to the electrodes, while simultaneously ensuring that the reactants or products are evenly distributed across the surface.

[0046] Preferably, the plate-shaped reaction cells each comprise a plurality of plate-shaped functional elements selected from the group consisting of catalyst layers, gas diffusion layers, bipolar plates, proton exchange membranes, anion exchange membranes, and separation membranes. "Million" means that there are at least two or more functional elements. The number of functional elements depends on the type and configuration of the plate-shaped reaction cell. Embodiments are also possible in which two or more functional elements are present in a single combined element. This means that functional elements within a reaction cell are pre-assembled by a fixed connection.

[0047] Furthermore, embodiments are also possible in which different types of plate-shaped reaction cells are arranged in a modular form. These different types of plate-shaped reaction cells can include electrolysis cells, membrane cells, catalytic membrane cells, and redox cells. These different types of plate-shaped reaction cells can be housed in different receiving units, as can be seen, for example, in the schematic representation of the apparatus shown in Figure 8.a is shown. Furthermore, an embodiment is also possible in which plate-shaped reaction cells are located in the same receiving unit and form a 4-cell configuration. These can be arranged in the apparatus that is in the Figure 11 It is shown on the left-hand side.

[0048] The terms functional elements and functional layers are used synonymously. It should be noted that not all sealing elements have to have a layered structure; sealing rings or rectangular sealing elements can also be used.

[0049] In one embodiment, individual functional elements are integrated into the housing plates. In this embodiment, the gas diffusion layers are permanently bonded to the housing element. This embodiment is considered to exist when the functional elements are used in a defined configuration that remains unchanged and exhibits no significant wear, thus eliminating the need to replace these functional elements. The sealing elements, which are replaceable or reusable, can also be functional elements.

[0050] Since the plate-shaped reaction cells are detachably connected to one another, it is clear that the connections are equipped with sealing elements. The selection and nature of the sealing elements depend on the specific process parameters or conditions under which the reaction cell is used.

[0051] Implementation of the plate reactor as a fuel cell with a proton exchange membrane.

[0052] In one configuration of the apparatus, where each plate-shaped reaction cell is in contact with a force sensor, it is possible to monitor the contact force of the reaction cells and to perform the investigation during dynamic cell operation. The reaction cells can be equipped with an optical connection or access to their interior. Equipping the cell interior with analytical instruments has the advantage of making the cell interior accessible for on-site analyses selected from the group of UV, IR, NIR, MIR, laser diffraction, and optical imaging techniques. For this purpose, the housing surfaces of the plate-shaped reaction cells can have window areas that are transparent to radiation and also feature detection surfaces to capture the reflected radiation signals.

[0053] In one embodiment, the pistons of the piston tensioners are equipped with cylindrical rods, which increase the distance between the plate-shaped reaction cells and the piston tensioner drive. This has the advantage that the plate-shaped reaction cells can also be operated at high temperatures, since the fluidic drive of the piston tensioners exhibits thermal decoupling or the spatial conditions are suitable. The thermal decoupling can be improved by arranging a heat shield below the piston tensioner drive to block radiant heat. The heat shield is made of a material that conducts heat poorly or not at all, such as a ceramic plate.Apart from that, the drive of the piston clamps can be equipped with a cooling device to prevent the transfer of heat from the heating device for the reaction cells to the drive of the piston clamps.

[0054] In a preferred embodiment of the apparatus according to the invention, the pistons of the piston tensioners are equipped with spacer elements; in a preferred embodiment, the spacer elements comprise a heat shield or a cooling device, or a heat shield and a cooling device. The combination of spacer elements in conjunction with a heat shield and a cooling device is advantageous for operating the plate-shaped reaction cells at high temperatures.

[0055] The individual plate-shaped reaction cells are marked with an identifier in the form of a barcode, numerical code, or other character. The system's program control records which cell is used and in which position.

[0056] A further preferred embodiment of the apparatus includes support elements in the form of grooves, recesses, or compartments in which the plate-shaped reaction cells or stacked plate-shaped reaction cells are positioned. Preferably, the support elements include spacers equipped with means for thermal decoupling. The support elements enable high positioning accuracy of the plate-shaped reaction cells.

[0057] In a preferred embodiment, the group of plate-shaped reaction cells or a group of stacks of plate-shaped reaction cells or a group of plate-shaped reaction cells comprising one or more stacks of plate-shaped reaction cells are surrounded by a temperature control device, wherein it is preferred that the device has a heating chamber in which several units of the apparatus are arranged, and the more preferably different units each have separate temperature control devices.

[0058] It should be noted that the embodiment of the apparatus in which the piston clamps are provided with cylindrical rods is particularly preferred when the apparatus for investigating processes involves the plate-shaped reaction cells being ceramic reaction cells. These can be high-temperature electrolysis cells or high-temperature fuel cells, also known as solid-state electrolysis cells or solid-oxide electrolyte cells (abbreviated as SOEC) or as solid-state fuel cells or solid-oxide fuel cells (abbreviated as SOFC).

[0059] In one embodiment, the plate-shaped reaction cells can be designed as fuel cells. In another embodiment, the fuel cells can have individual stacks.

[0060] The apparatus according to the invention can be used to monitor the behavior of the sealing elements under the influence of pressing force as a function of time. This allows for a highly targeted investigation of aging processes. The investigation can focus on the aging processes occurring in the sealing elements or in the functional elements. The investigation of the effect of the pressing force is preferably started once the reaction cells have reached constant operating conditions, so that the temperature-induced linear expansion of the reaction cells is not mistakenly interpreted as expansion or compliance of flexible components (seals, membranes). Therefore, the reaction cells and the pressing apparatus are located in a temperature control chamber or an oven chamber, respectively.

[0061] In one embodiment, the apparatus can be used to carry out the processes that are performed in the plate-shaped reaction cells in a periodic operating mode, whereby individual measurement cycles can also be repeated.

[0062] Aggregate structure and division into functional elements: defined by housing plates, fluid distribution plates, electrodes, and a central membrane assembly with replaceable or reusable sealing elements. The reaction cells can have a stepped design. In this stepped design, the membrane assembly is located in the center of the reaction cells between the two housing plates, and the membrane assembly can be covered with catalyst layers on one or both sides of the membrane. The catalyst-coated membrane assembly constitutes a catalytic membrane assembly. The membrane assembly covered with catalyst layers can be covered on both sides with layers of diffusion elements, preferably gas diffusion elements.Diffusion elements are characterized by having a polarity and a porosity that improve the process, as they partially favor the passage of desired components and promote the discharge of reaction products.

[0063] In one embodiment, the membranes of the reaction cells can be designed as membrane aggregates (abbreviated as MA in this document) or as membrane electrode aggregates (abbreviated as MEA in this document).

[0064] The use of membrane electrode assemblies or membrane assemblies can be advantageous if components can be manufactured cost-effectively as assemblies or if the chemical processes can be carried out particularly efficiently.

[0065] Membrane assemblies are advantageous in applications because they contribute to a frequently desired functional separation into components with active and inactive characteristics, which can be manufactured using different methods. Inactive components include, for example, flow-guiding components or seals. Active components are those that actively participate in chemical reactions, mixing, or separation. Components that participate in chemical reactions include catalytically coated components. Components that alter the material composition include, for example, membranes. These are often functionalized, with functionalization relating to the membrane surfaces, which can, for example, regulate the wetting behavior.The non-active components can be manufactured using production methods such as structuring, cutting, stamping, film extrusion, film casting, etc. Active components can be additionally treated with chemically active components. These include, among others, spray coating, doctor blade coating, sputter coating, CVD coating, sol-gel coating, and impregnation. The finished cell is then assembled from active and non-active components into a membrane assembly.

[0066] Regarding the structural design of membrane aggregates, the membrane is a central component that primarily functions as an ion-conducting layer and, in a preferred embodiment, also includes a catalyst or a catalytic layer on at least one or both sides.

[0067] Plate-shaped reaction cells with housing and sealing elements, connections, supply lines and outlets for gases and liquids, electrical connections.

[0068] To illustrate the invention, structural designs of plate-shaped reaction cells are described, which can be used in conjunction with the apparatus for investigating chemical processes. Various plate-shaped reaction cells can be produced, resulting from different configurations of membrane aggregates.

[0069] In one embodiment, the plate-shaped reaction cell can be configured as a fuel cell (solid-oxide fuel cell or SOFC) that features an ion exchange membrane as its central separation element. The ion exchange membrane is covered on both sides of the separation layer with a porous catalytic layer, which may be covered by diffusion layers.

[0070] In another embodiment, the catalytic layer of fuel cells comprises a carbon-containing or graphite-containing material, or a material that is both carbon-containing and graphite-containing, on whose surface active components or active elements may be deposited. The carbon-containing or graphite-containing material has agglomerates with a size in the range of 40 to 100 nm. The agglomerates may include carbon-containing or graphite-containing primary particles with a size in the range of 10 to 30 nm. The active components or active elements are located on the surface of the primary particles and have a size in the range of 2 to 5 nm. The individual agglomerates may be encapsulated by a polymer membrane. In a preferred embodiment for low temperatures (< 200°C, < 473.15 K), the polymer membrane is a Nafion membrane.Nafion is a trade name for a polymer material from DuPont, specifically a sulfonated tetrafluoroethylene polymer (PTFE). The electrodes can be a wire mesh, which can be located between the porous catalytic layer and the diffusion layer, within the catalytic layer, or between the catalytic layer and the proton exchange membrane. Preferably, the thickness of the proton exchange membrane is in the range of 0.5 mm to 10 mm, and more preferably in the range of 1 mm to 8 mm. Preferably, the thickness of the porous catalytic layer is in the range of 50 µm to 1000 µm, and more preferably in the range of 100 µm to 250 µm. Preferably, the diffusion layer has a thickness in the range of 50 to 250 µm. The fluid space, through which the fuel or working fluids are transported, extends along the surface of the diffusion layer.

[0071] One aspect of the apparatus according to the invention relates to the possibility of scaling up the experimental setup, which can be achieved by very easily increasing the surface area of ​​the membranes. The plate-shaped reaction cells can be available in different dimensions, each of which can be used in the same apparatus with the pressure device. Thus, the plate-shaped reaction cells with smaller dimensions can be exchanged for larger plate-shaped reaction cells. In addition, the individual plate-shaped reaction cells can also be arranged in stacks, with the plate-shaped reaction cells being connected in series so that the membrane areas of the individual cells can be summed to form a total membrane area.This allows data to be collected for upscaling without the need for another device, which is why the use of the apparatus according to the invention makes development in upscaling very efficient and resource-saving.

[0072] In one embodiment, the plate-shaped reaction cell can be used as a solid-state electrolysis cell (so-called SOEC).

[0073] The apparatus according to the invention for investigating plate-shaped reaction cells can be part of a modular platform comprising the following modules: Central control cabinet with supply unit; supply unit for gas and liquids; reaction module with apparatus for receiving and fixing a plurality of plate-shaped reaction cells; concurrent analysis units or online analysis unit; and a control device.

[0074] The invention also relates to a method for investigating plate-shaped reaction cells using the apparatus according to the invention.

[0075] Method for investigating chemical processes in plate-shaped reaction cells using an apparatus that is the subject of this description, wherein the method comprises the following steps: Several plate-shaped reaction cells are positioned with their outer plate surface on the top of receiving units, preferably in such a way that the reaction cells have a horizontal orientation and linear arrangement on the top of the receiving units and are supported by gravity; the plate-shaped reaction cells are pressed together by means of piston clamps, wherein one or more piston clamps per plate-shaped reaction cell exert a pressing force on the outer plate surface of the individual reaction cells, which acts perpendicular to the plate surface in the direction of the stop and thereby seals the interior of the individual reaction cells; connections of the fluid lines to the supply lines and drains are made, optionally connections to the electrical supply lines for the electrodes are made; the plate-shaped reaction cells are operated under the chemical process conditions.

[0076] Preferably, during the execution of the process, one or more process parameters per reaction cell are recorded during the operation of the reaction cells under the chemical process conditions, wherein it is preferred that at least one of these process parameters is the pressing force with which the individual reaction cells are pressed together.

[0077] In carrying out the method, it is further preferred that a comparison of registered process parameters per reaction cell with target parameters is performed; the target parameters can be given by reference data or by process parameters that are registered in neighboring reaction cells; exchange of individual plate-shaped reaction cells by selectively loosening piston clamps and supply lines, wherein it is preferred that the operation of those plate-shaped reaction cells that are not exchanged is continued.

[0078] Furthermore, it is preferred that the method be carried out in combination with an online analysis of the product fluid flows, and it is further preferred that the method be carried out in combination with an inline analysis of the interiors of one or more reaction cells in operation, and in particular, the method is preferably carried out in combination with an online analysis of the product fluid flows and an inline analysis of the interiors of the reaction cells.

[0079] Components of the process may also include conditioning the reaction cells under selected process conditions. Furthermore, analytical characterization studies may be a component of the process. These analytical characterization studies can be performed using online analysis units on the process fluid exiting the plate-shaped reaction cells.Analytical characterization investigations can also be carried out inside the plate-shaped reaction cells, provided the housing plates are equipped with radiation-transparent windows and contain the appropriate elements for radiation excitation and detection. Furthermore, those functional elements of the reaction cell's interior that may be subject to wear or degradation can be subjected to subsequent analytical characterization after removal from the reaction cell. For example, it may be of interest to subject the catalyst layer to subsequent characterization. Subsequent analysis can relate to the determination of the catalyst morphology—a so-called post-process analysis of the catalyst used.All surface analytical methods known to those skilled in the art can be used to perform the autopsy analysis. These methods include, among others: light microscopy, scanning electron microscopy, transmission electron microscopy, EDX, XPS, ICP-OEX, GD-OES, IR, FTIR, SIMS, NMR, XRD, and chromatography. Furthermore, the surface of the catalyst used can also be characterized by laser scanning microscopy, whereby a 3D method with depth resolution can also be employed for the scans. The resolution achieved by laser scanning microscopy is 2–3 µm.

[0080] It is possible to combine laser scanning microscopy with elements from the following group. Laser scanning microscopy can be combined with a camera. This also applies to all other surface analysis methods. By capturing surface structures (pattern recognition) with the camera in combination with a suitable algorithm, it is possible to locate the exact same spatial locations or points from which a desired analysis is performed. This approach allows for the collection of various pieces of information at fixed coordinates. This method can also be carried out with a very precise coordinate system. However, the problem then arises of defining the reference point on the sample so precisely that it can be located again even if the sample is transferred to a different analytical device or instrument.

[0081] The following devices can be used in the procedure: a CCD camera, a confocal laser scanner (< 1µm), laser focus variation, 3D interferometer (< 1 nm).

[0082] The inventive method for investigating chemical processes in plate-shaped reaction cells can be characterized in that the plate-shaped reaction cells can be operated in a temperature range of 298.15 K to 1273.15 K (25°C to 1000°C).

[0083] During the execution The process allows temperature changes to be made in time intervals with temperature steps of up to 60 K / second. The plate-shaped design of the reaction cells offers the advantage of a large external surface area relative to a small internal volume. Therefore, temperature control can be performed very quickly and with high accuracy.

[0084] During the execution of the procedure, a change in fluid composition or a change in gas composition can be carried out at a speed of seconds or at a frequency of 1 Hertz.

[0085] The invention also relates to a program control for controlling an apparatus, which is designed according to the description or the claims and which is used to carry out a method for investigating chemical processes, wherein the program control includes a database in which the measured values ​​are stored. Furthermore, preferably, the method can be carried out using a program control, wherein the program control can include a selection of recipes. The recipes can already be present in the program control as a library. Alternatively, the user can also create their own recipes.

[0086] The procedure can be carried out using online detection methods to characterize the composition of fluid flows. Fast (repeat rate in the range of seconds, with a measurement duration of ≤ 30 seconds per measurement, preferably ≤ 10 seconds per measurement) analytical methods such as FTIR or HFID can be used for online detection – or, for stationary investigations (repeat rate in the range of minutes, with a measurement duration of ≥ 0.5 minutes per measurement, preferably ≥ 1 minute per measurement), gas chromatography can also be used.

[0087] The procedure allows for the simulation of various operating modes, such as those replicating the operation of vehicles. These modes can be based, for example, on the conditions of the New European Driving Cycle (NEDC) for internal combustion engines. The focus is then not on pollutants, but on the efficiency of energy utilization.

[0088] Other examples focus on conditioning the reaction cells to achieve maximum power output. Manufacturers of fuel cell stacks offer varying descriptions of operating modes. The following methods and operating states are also used: Constant Current Hold, Voltage Cycling, Air Braking, Hydrogen Pump, Cathode Oxidant Starvation, Thermal Cycles with Current Cycling, and Combined Temperature and Humidity Cycling. Further details on protocols, including literature examples, can be found, for instance, in the following publication: Current Opinion in Electrochemistry 2022, 31:100843; sciencedirect.com; (https: / / doi.org / 10.1016 / j.coelec.2021.100843).

[0089] To carry out the procedure, it is possible to map individual cycles where the duration of the total cycle is in the range of 20 seconds to 2000 seconds, whereby the temperature fluctuations that occur during the execution of the procedure can be in a range of 273.15 K to 673.15 K (0 to 400 °C).

[0090] To carry out the process, the supply module can be used to supply gases and liquids, which can be provided individually or together.

[0091] Cyclovoltammetry can be used in the accelerated conditioning process, either to activate electrodes or catalysts through conditioning or to further improve performance characteristics during the process. Cyclovoltammetry also allows for the investigation of charge density before and after conditioning under real operating conditions and the correlation of charge density data with performance characteristics. Based on this data, specific structure-activity relationships that lead to improvements or deteriorations in performance can be identified.

[0092] During the procedure, the measurement parameters are at least partially automatically recorded and registered by the program control. Performance characteristic logs are also generated.

[0093] Preferably, a piston compressor from Enerpac Tool Group is used. Piston compressors of this preferred type are described in WO-A 202162224. The compressive force applied by means of the piston compressor is in the range of 10 to 1000 kN per plate-shaped reaction cell, particularly in the range of 20 to 500 kN per plate-shaped reaction cell. In the case of polymeric sealing materials, it is preferred that the specific compressive force acting on the surfaces of the plate-shaped reaction cells is greater than 1 kN per cm²; more preferably, the compressive force acting on the contact surface is greater than 2 kN per cm². The compressive force depends on the material of the sealing element selected. For metallic sealing materials, the compressive force is also in the range of 10 kN per cm² or greater.

[0094] The chemical processes carried out in the plate-shaped reaction cells are performed at temperatures in the range of 273.15 to 1273.15 K, particularly in a range of 298.15 to 1073.15 K, and further, in particular, at a temperature in the range of 373.15 to 873.15 K.

[0095] During the execution of the procedure, the pressures are in the range of 0.05 to 500 bara, particularly in the range of 0.1 to 300 bara, and further pressures particularly in the range of 1 to 250 bara.

[0096] A plate-shaped reaction cell is a reaction cell that exists as a single reaction cell or in the form of stacked plate-shaped reaction cells, wherein the single reaction cell or the stacked reaction cells can be arranged in a position within the receiving unit. If the plate-shaped reaction cells are stacked arrangements, a single stack comprises 2 to 10 plate-shaped reaction cells, in particular a single stack comprises 2 to 6 plate-shaped reaction cells, and more particularly 2 to 4 plate-shaped reaction cells.

[0097] The plate-shaped reaction cells are used in a design selected from the group consisting of membrane reactors, electrochemical reactors in the form of fuel cell reactors, electrochemical reactors in the form of electrolyzers, photocatalytic reactors, and in particular preferably as photocatalytic reactors with integrated LED sources.

[0098] The thickness of a single plate-shaped reaction cell is in the range of 0.5 to 5 cm, in particular 0.8 to 4 cm, and further in the range of 1.5 to 2.5 cm.

[0099] The plate-shaped reaction cells, or individual functional elements of the plate-shaped reaction cells, can have identifiers, for example, in the form of a tag, a barcode, or an RFID chip. This ensures that the plate-shaped reaction cells are positioned at defined receiving positions of the stop. This also allows for monitoring the controlled assembly of the plate-shaped reaction cells. In a preferred embodiment, the assembly is performed at least partially by a robot.

[0100] The sealing elements used to seal the plate-shaped reaction cells are selected based on the process parameters under which the plate-shaped reaction cells are operated. At temperatures exceeding 573.15 K, seals made of a metal or graphite are preferred. At temperatures below 573.15 K, seals made of a material from the Teflon, Kalrez, Viton, or rubber groups are used.

[0101] If multi-stage processes are carried out, it is preferred that these processes be performed in stacked plate-shaped reaction cells, so that the process stages are carried out in the different stages of a layer. This arrangement has the advantage that the adjacent plate-shaped reaction cells, which are not arranged in the same holding position, are not coupled to each other. This allows individual plate-shaped reaction cells to be replaced during operation, while other plate-shaped reaction cells continue to operate.

[0102] In a preferred embodiment, the apparatus according to the invention forms a central module of a multifunctional device, which is composed of several modules and allows for great flexibility with regard to carrying out very different chemical processes and with regard to adding and exchanging individual functional modules. Thus, the invention also relates to a multifunctional device comprising the following modules: one or more supply modules, a central reaction module of an apparatus according to the invention for accommodating plate-shaped reaction cells, an analysis module, and a control module with process control and data acquisition unit.

[0103] These and other characteristics will be explained using the following character description. Brief description of the characters

[0104] Figure 1.a shows the schematic cross-sectional structure of a plate-shaped reaction cell designed as an electrolysis plate reactor or as a plate-shaped electrolysis cell comprising two half-cells separated by a membrane; Figure 1.b shows the schematic structure of a plate-shaped reaction cell as a top view of the inner surface of a housing plate in which a channel structure for fluid passage is provided; Figure 1.c shows the schematic structure of a plate-shaped reaction cell as a top view of the inner surface of a housing plate that does not have a channel structure as shown in the Figure 1.bFigure 2 shows the schematic structure of a piston clamping unit in which a piston clamp is arranged as a screw-in piston clamp, wherein the piston clamping unit has a line for fluid supply; Figure 3a shows a schematic representation of the apparatus according to the invention, which is equipped with four plate-shaped reaction cells, wherein the plate-shaped reaction cells are each fixed between receiving units and pistons of the piston clamping units, wherein the piston clamping units are designed as a common element; Figure 3.Figure b shows a schematic representation of a force distribution element designed as a spherical element and fixed at the tip of a piston; Figure 4 shows a schematic representation of a plate-shaped reactor cell in contact with two piston clamping elements forming a piston clamping unit, wherein the pistons have cylindrical rods extending the distance; Figure 5 shows a schematic representation of an apparatus according to the invention, equipped with three plate-shaped reactor cells, wherein the three piston clamping units are arranged in a common element in which the fluid supply lines for driving the individual piston clamps run, wherein the lines are equipped with valves and the main line has a common pressure regulating valve.The individual reaction cells are equipped with inlets and outlets, the outlets leading to liquid collection vessels; Figure 6 shows a schematic representation of the apparatus, which is located in . Figure 5 The apparatus is shown in a furnace chamber, with the individual assemblies, namely the piston clamping units in a common element, the plate-shaped reaction cells, and the liquid separators, being provided with separate temperature control elements; Figure 7 shows a schematic representation of the apparatus, which is in Figure 6The apparatus is characterized in that the pistons of the piston clamping units are equipped with a temperature control device, and fluids are supplied via a common fluid supply which also includes a temperature control device. The streams exiting the liquid separators can be supplied to an analysis unit. Figure 8a shows a schematic representation of the apparatus equipped with plate-shaped reaction cells, wherein the plate-shaped reaction cells are available as single reaction cells and as stacks of reaction cells. A total of three different groups of plate-shaped reaction cells can be accommodated in the apparatus shown. Figure 8b shows a schematic representation in which the piston clamping units and the receiving units are separate elements, with a holding frame for each pair of piston clamping unit and receiving unit.Figure c shows a schematic representation of piston clamping units connected by fluid lines to a fluid supply tank equipped with a pressure regulator; Figure 8.d shows a schematic representation of the piston clamping units with fluid supply tank located in . Figure 8.cFigure 9 shows a schematic representation of a plate-shaped reaction cell that is fixed in a clamping unit, wherein the piston 25 is pressed against the outer surface of the reaction cell and wherein the piston is simultaneously connected to a sensor element 81 which detects the piston movements; the reaction cell has radiation-transparent windows 83 through which radiation 85 is directed into the interior of the cell; Figure 10a shows a schematic representation of four reaction cells arranged in a parallel arrangement; Figure 10.Figure b shows a schematic representation of four reaction cells arranged in a serial arrangement; Figure 11 shows a schematic representation of two stacks, each with three plate-shaped reaction cells, which in the stack arranged on the left have a serial connection 93 and in the stack arranged on the right have a parallel arrangement 91.Figure 12 shows a schematic representation of a device composed of a group of four modules, the modules being connected to a central control unit; Figure 13 shows a schematic representation of an embodiment of a device composed of several modules, comprising the apparatus according to the invention as a module, which is represented in a plurality of modules that are combined; Figure 14 shows a schematic representation of a module for supplying gases and liquids; Figure 15 shows a schematic representation of a module with online analysis units; Figure 16 shows a schematic representation of an apparatus according to the invention for carrying out chemical processes in plate-shaped reaction cells in a work process for testing production parts that represent functional elements in series products.

[0105] Further features and advantages of the methods and apparatus according to the invention will become apparent from the figures and the accompanying description. It is understood that the features mentioned above and those to be explained below are applicable not only in the combinations shown, but also in other combinations or individually, without departing from the scope of the present invention. Exemplary embodiments of the invention are illustrated in the figures and are described in detail below. Detailed description of exemplary embodiments

[0106] First, a general description of the invention is given based on the entirety of the figures, and then the details of the invention are described with specific reference to the figures.

[0107] Example of the production of catalyst layers.

[0108] An example of the use of the apparatus according to the invention in connection with the development of new and improved catalyst layers, which can be screened using the apparatus in a short time. All methods known in the field of catalyst synthesis can be used to produce the catalyst layers. These are methods for applying catalysts to base plates or to electrodes, or to base plates containing the electrodes. The manufacturing process can include at least one method selected from the group consisting of: chemical immersion, spin coating, dip coating, doctor blade coating, coating with a blade, injection molding, spray coating, screen printing, inkjet printing, aerosol jet atomization, rod deposition, 3D printing, and plasma coating.

[0109] The manufacturing process can utilize special plate-shaped discs selected from the groups of porous ceramic layers, porous metal layers, and composite materials made of ceramic and metal. The ceramic materials can include alumina and steatite.

[0110] In a preferred embodiment, the apparatus according to the invention has a structure that corresponds to the illustrations shown in the Figure 5 and the Figure 8 will be shown. In the representation, which is in Figure 5 As shown, the outer plate surface is pressed towards the stop using two piston clamps (26), whereas in Figure 8The outer plate surface is pressed against the stop only by a piston clamp (26). In both embodiments, a distributor element (23) is visible, in which a common fluid line (30) with fluid lines (27) to the individual piston clamps (26) are provided. Switching valves (57) are arranged in each of the fluid lines (27), and actuating the switching valves (57) interrupts the connection of the fluid line to the fluid supply (50). Thus, by means of the pressure control valve (33) and the pressure regulator connected to the pressure control valve, the pressure values ​​can be determined either as integral pressure values ​​or as a pressure value related to a selected reaction cell, depending on the valve state of the switching valve.If all but one of the switching valves (57) in the individual lines are closed, the pressure value at the pressure regulator refers to the piston clamping unit where the switching valve is open. This allows for selective querying, sampling, or multiplexing of individual measured values.

[0111] The apparatus according to the invention offers a very high degree of flexibility with regard to the chemical processes to be investigated. The apparatus enables the targeted investigation of a large number of process parameters, which are collected in the central database in the form of relational process data. The data registered in the database provide process information that can be used for the experimental design of future experimental configurations. The program control or database evaluation can be equipped with a program that is independently capable of selecting the most favorable process conditions based on the analysis of data sets. This high degree of flexibility, combined with the acquisition of large amounts of data, enables an acceleration of the execution of chemical processes.At the same time, the data quality of the generated process data can also be improved, since, due to a parallel arrangement of plate-shaped reaction cells, it is also possible to carry out the chemical processes in the presence of reference cells, which are equipped with reference materials and which are carried out under selected reference conditions.

[0112] One aspect of the apparatus and device according to the invention relates to the generation of chemical process data that exhibits high and improved data quality compared to conventional devices built without parallel arrangements. This high data quality has the advantage of accelerating the development of chemical processes, as the scope of investigations required for scaling up can be reduced. This conserves resources. Simultaneously, it makes it possible to develop chemical processes that can be applied to smaller-scale applications.

[0113] Another aspect of the invention relates to the use of the apparatus according to the invention for investigating chemical processes in plate-shaped reaction cells in an arrangement to support serial production processes in the energy and automotive sectors. The invention is particularly suitable for use in quality control in serial production and also in carrying out and testing conditioning processes. The schematic representation in Figure 16Figure 1 shows the combination of the apparatus according to the invention with a robot, so that the operation of the apparatus can be at least partially automated; more preferably, the operation of the apparatus is fully automated. Its use in the field of quality control and conditioning is particularly advantageous because the clamping piston units can be individually controlled, the reaction cells can be easily exchanged, and a high throughput is possible. Therefore, production tests (quality control or conditioning, or a combination of quality control and conditioning) can be carried out with the apparatus according to the invention, according to the production capacities of individual factories, with the test capacities being in the range of 10 to 1500 reaction cells per day, preferably in the range of 50 to 1000.The advantages of the invention provide synergistic effects, which are also given by the following properties: the test protocols can be selected in such a way that an accelerated rate can be achieved in the aging of the functional materials and thus in the testing; the execution of the tests is monitored with sensor elements and the registered test data is stored in a database; the fixing of the reaction cells in the apparatus by means of the piston clamping elements is time-saving and can also be automated.

[0114] In a preferred embodiment, the outlet lines of the plate-shaped reaction cells are equipped with a pressure control system, wherein the pressure control system is selected from the group consisting of a pressure control valve arranged directly in the outlet line or a side-flow pressure control device, which is effected by the injection of dilution gases via capillary lines in conjunction with a pressure regulator. In a further preferred embodiment, the pressure control via side-flow line is equipped with an adjustable valve that allows fine control of the gas flow, preferably a Reco control valve.

[0115] Regarding the Figure 1.b and Figure 1.cRegarding the design of the channels 9, it should be noted that the dimensions of the channels depend on the dimensions of the plate-shaped reaction cell. In one embodiment, the channels 9 can have the dimensions of parallel channels, wherein the length of a fluid channel is in the range of 10 to 50 mm and the diameter of a fluid channel is in the range of 50 to 2000 µm, more preferably in the range of 100 to 1000 µm, and furthermore preferably in the range of 100 to 500 µm.

[0116] The choice of material for the seals depends on process parameters such as the type and concentration of the medium, temperature, and pressure. The thickness and shape of the seals depend on the components used. The thickness of the seals can range from 1 to 2 mm, although they can also be 3 mm thick; seals with thicknesses of less than 1 mm can also be used. The thickness of the sealing elements used 4, 4' in the Figure 1.a The surface quality of the flanges against which the gaskets are pressed depends on their area. These flanges are, for example, the inner edge areas of the reaction cell housings, which are pressed against another housing part or a functional element. This is shown schematically for the path of gasket 4 in the Figure 1.b shown. Functional elements such as the membrane 15 in the Figure 1.acan be surrounded by a frame structure, the frame structure forming an edge that is arranged between the housing halves, the frame structure being arranged between the housing halves of the plate reactor. Reference symbol list

[0117] 01 Control device 02 Control cabinet, electrical supply for controller 03 Supply module, gases and liquids 04 Apparatus with plate-shaped reaction cells in a pressing device 04m Module comprising an apparatus 04 05 Analysis module 06 Device composed of a group of four modules 02, 03, 04m and 05 and control device 01 06' Device consisting of a group of modules with multiple modules 04m and further modules 08 System for carrying out quality control on reaction cells or functional elements comprising a device 06 or 06' 1 Plate-shaped reaction cell 3 Electrical supply unit 4, 4' Sealing elements 5 Drain 7 Supply line 8 Supply line 9 Channel in housing element 10 Supply line, drain 11 Housing element 13 Housing element 15 Partition, membrane 16 Diffusion layer 17 Porous catalyst layer 19 Electrode 20 Thread 22 Sealing element 23 Piston tensioning unit 24 Spring 25 Piston of the piston tensioner 26 Piston tensioner 27 Fluid line 28 Seal 30 CommonFluid line 31 Connecting element for receiving units or receiving units 33 Valve, pressure regulating valve 34 Supply line 35 Fluid supply tank 39 Receiving unit(s) for plate-shaped reaction cell(s) 41 Ball element 43 Receptacle for ball element 45 Connecting piece to piston 50 Supply line 51 Spacer in the form of a cylindrical rod 53 Spring element on the piston 54 Outlet line 56 Liquid separator 57 Switching valve 58 Common supply line for inlet 59 Connecting line to the supply line of a reaction cell 60 Housing for temperature control 63 Temperature control device for separator 64 Temperature control device for plate-shaped reaction cells 65 Cooling device for temperature control of the piston tensioners 67 Temperature control device for supply unit 71 Analysis unit 72 Liquid drain line from the separator 73 Switching valve with connection to the analysis unit 78 Mounting frame 81 Sensor for monitoring the piston 83 Radiation-transparent window in the housing of aReaction cell 85 Radiation transmission through transparent window in housing 91 Parallel arrangement of several reaction cells 93 Serial arrangement of several reaction cells 95 Robot 96 Functional elements in test cells 97 Reaction cells in mass-produced products

Claims

1. An apparatus for studying chemical processes in reaction cells in plate form, having: a group of reaction cells in plate form or a group of stacks comprising reaction cells in plate form or else comprising individual reaction cells in plate form, and a closure system that enables independent fixing of the individual reaction cells in plate form and stacked reaction cells in plate form, wherein the closure system comprises receiving units and a multitude of piston clamp units, wherein the piston clamp units have a common drive system, each reaction cell in plate form or each stack comprising reaction cells in plate form has two outer plate surfaces, where one outer plate surface in each case is in contact with a receiving unit and the other outer plate surface with one or more piston clamps of each piston clamp unit, wherein the piston clamp unit is designed to independently subject the reaction cells in plate form or stacked reaction cells in plate form to a compression force, where the compression force acts at right angles to the plate surface in the direction of the receiving unit, wherein the reaction cells in plate form or stacked reaction cells in plate form each comprise a multitude of functional elements in plate form, where the functional elements in plate form are catalyst layers, gas diffusion layers, bipolar plates, proton exchange membranes, wherein each reaction cell in plate form has at least one inlet for a reactant and at least one outlet for a product, or wherein the stacked reaction cells in plate form each have at least one inlet for a reactant and at least one outlet for a product.

2. The apparatus for studying chemical processes according to claim 1, wherein the reaction cells in plate form or stacked reaction cells in plate form each comprise a multitude of functional elements in plate form, selected from the group of catalyst layers, gas diffusion layers, bipolar plates, proton exchange membranes, anion exchange membranes, separation membranes.

3. The apparatus for studying chemical processes according to claim 1 or claim 2, wherein the piston clamp units have a fluidic drive system, wherein the piston clamp units are connected by conduits to a common fluid supply conduit or to a common fluid supply tank, wherein the common fluid supply conduit or the fluid supply tank is connected to a pressure regulator valve, the pressure regulator valve preferably being an Equilibar valve, and the fluid also preferably being a pneumatic or hydraulic fluid, wherein there are switching valves in the conduits to the common fluid supply conduit or the common fluid supply tank, wherein the fluid stream through the fluid conduit can be switched on and off by means of actuation of the switching valves.

4. The apparatus for studying chemical processes according to any of claims 1 to 3, wherein the piston clamp unit of the pressing device is characterized in that the latter has one piston clamp per reaction cell in plate form or one piston clamp per stacked reaction cell in plate form, there is further preferably a force distributor element at the tip of each piston of the piston clamps, and each force distributor element preferably also has a ball bearing.

5. The apparatus for studying chemical processes according to any of claims 1 to 4, wherein the reaction cells in plate form have separation membranes and electrodes and are divided into half-cells, wherein the electrodes are connected to electrical supply conduits, wherein the reaction cells in plate form are configured as electrolysis cells or galvanic cells, and the reaction cells in plate form are especially preferably configured as electrolysis cells, wherein the electrodes are preferably connected to current and voltage measurement devices, and the apparatus further preferably comprises online analysis devices from the group of online voltammetry for measurement of V / A functions, impedance spectroscopy for measurement of high-frequency voltage changes.

6. The apparatus for studying chemical processes according to any of claims 1 to 5, wherein the piston or the force distributor element is equipped with a sensor that can measure a geometric change in the reaction cell during the reaction, sensors being force measurement sensors or measurement sensors selected from the group of expansion measurement strips, distance detectors such as ultrasound barriers and optical light barriers, or interference measurement analyzers.

7. The apparatus for studying chemical processes according to any of claims 1 to 6, wherein one or more of the reaction cells in plate form have one or more sensors connected to sites in the interior of the reaction cells, wherein the sensors are sensors for the performance of in situ test methods selected from the group of electrochemical dilatometry for characterization of the change in thickness of electrodes, light-microscopy or spectroscopy characterization via glass fibers relating to electrodes or membranes.

8. The apparatus for studying chemical processes according to any of claims 1 to 7, wherein the receiving units take the form of physically separate units or of a physically connected unit; if the receiving units take the form of physically separate units, each receiving unit has a dedicated holding frame connected to one piston clamp unit; if the receiving units take the form of a physically connected unit, the receiving elements have a common holding frame, wherein the piston clamp units are preferably arranged in a common element, wherein the common holding frame connects the receiving units and the common element.

9. The apparatus for studying chemical processes according to any of claims 1 to 8, wherein the apparatus is characterized in that the reaction cells in plate form have an inner plate area in the range from 1.5 x 1.5 cm2 to 30 x 30 cm2, the inner plate area is preferably 2.0 x 2.0 cm2 to 25 x 25 cm2, and the inner plate area is further preferably 3.0 x 3.0 cm2 to 15 x 15 cm2.

10. The apparatus for studying chemical processes according to any of claims 1 to 9, wherein the pistons of the piston clamps are equipped with spacer elements, and in a preferred embodiment the spacer elements comprise a heat shield or a cooling device or a heat shield and a cooling device.

11. The apparatus for studying chemical processes according to any of claims 1 to 10, wherein the apparatus (1) has the receiving units carrier elements in the form of grooves, depressions or compartments in which the reaction cells in plate form or stacked reaction cells in plate form are positioned, the carrier elements preferably having spacer elements equipped with means of thermal decoupling.

12. The apparatus for studying chemical processes according to any of claims 1 to 11, wherein the group of reaction cells in plate form or a group of stacked reaction cells in plate form or a group of plate reactors comprising one or more plate reactor stacks is surrounded by a temperature control device, wherein the device preferably has a heat chamber in which two or more components of the device are disposed, and the different components further preferably each have separate temperature control devices.

13. A method of studying chemical processes in reaction cells in plate form by means of an apparatus according to any of claims 1 to 12, wherein the method comprises the following steps: - a plurality of reaction cells in plate form or stacks comprising reaction cells in plate form are positioned with the outer plate surface on the top side of a receiving unit, preferably in such a way that the reaction cells have a horizontal orientation and linear arrangement on the top side of the receiving unit and are supported owing to gravity; - compressing the reaction cells in plate form or the stack comprising reaction cells in plate form by means of piston clamps, where one or more piston clamps per reaction cell in plate form exert a compression force on the outer plate surface of the individual reaction cells that acts at right angles to the plate surface in the direction of the stop and hence closes off the interior of the individual reaction cells in a sealing manner; - establishing the connections of the fluid conduits to the supply conduits and outlets, optionally establishing the connections to the electrical supply conduits for the electrodes; - operating the reaction cells in plate form or the stack comprising reaction cells in plate form under the chemical process conditions, where the reaction cells in plate form in the individual stacks may be connected in series or in parallel.

14. The method of studying chemical processes according to claim 13, wherein, during the operation of the reaction cells under the chemical process conditions, one or more process parameters per reaction cell are registered, and at least one of these process parameters is preferably the compression force with which individual reaction cells are pressed together.

15. The method of studying chemical processes according to claim 13 or claim 14, wherein a comparison of registered process parameters per reaction cell with target parameters is conducted; the target parameters may be given by reference data or by process parameters that are registered in adjacent reaction cells; exchange of individual reaction cells in plate form by selective release of piston clamps and supply conduits, preferably with continuation of operation of those reaction cells in plate form that are not exchanged.

16. The method of studying chemical processes according to any of claims 12 to 15, wherein the method is conducted in combination with an online analysis of the product fluid streams, the method being further preferably conducted in combination with an inline analysis of interiors of one or more reaction cells in operation, and the method being especially preferably conducted in combination with an online analysis of the product fluid streams and an inline analysis of interiors of the reaction cells.

17. A program controller for control of an apparatus according to any of claims 1 to 12 and for performance of a method of studying chemical processes according to any of claims 13 to 16, wherein the program controller comprises a database in which the measurements are stored.