Plasma lysis device, plasma lysis system and method for corona discharge-induced splitting of hydrogen-containing gas

Abstract

Plasma lysis device (100; 100') for corona discharge-induced splitting of hydrogen-containing gases (10) into molecular hydrogen (12) and at least one by-product (14; 14'), comprising: - a gas-tight reaction chamber (18; 18'), - a gas supply line (20) for the hydrogen-containing gas (10) into the reaction chamber (18; 18'), - exactly one plasma electrode (22; 22') for generating corona discharges (32) in the reaction chamber (18; 18') by means of a high-frequency alternating voltage and - a gas outlet (24) for the molecular hydrogen (12) from the reaction chamber (18; 18'), wherein the gas-tight reaction chamber (18; 18') is enclosed by a wall (28) which is configured to electrically insulate the plasma electrode (22; 22') from an outside of the wall (28), and wherein the plasma electrode (22; 22') is connected to a high-frequency generator (200) to generate the high-frequency alternating voltage.

Description

[0001] The invention relates to a plasma lysis device for corona discharge-induced splitting of hydrogen-containing gas into molecular hydrogen and at least one by-product, as well as a plasma lysis system with at least two such plasma lysis devices and a method for corona discharge-induced splitting of hydrogen-containing gas into molecular hydrogen and at least one by-product.

[0002] A plasma-assisted catalytic reforming plant according to US 2012 / 0167464 A1 comprises a feeder, a plasma reactor, a reforming reactor, and a preheater. The first reforming chamber of the reforming reactor is connected to the plasma chamber of the plasma reactor, and the reforming reactor is located within the preheating chamber of the preheater. A preheating pipe of the preheater connects the mixing chamber of the feeder to the plasma chamber and runs partially within the preheating chamber. The first reforming chamber is located within a second reforming chamber of the reforming reactor. One end of a recirculation pipe of the reforming reactor is connected to the opening of the first reforming chamber of the reforming reactor and runs partially within this chamber. The other end of the recirculation pipe passes through the outlet of the second reforming chamber of the reforming reactor and runs partially within the preheating chamber.

[0003] US 2007 / 0267289 A1 describes hydrogen production by plasma-based reforming. Hydrogen production involves introducing a hydrocarbon fluid into the gap between two electrodes, applying a voltage to the electrodes to generate an arc, the arc coming into contact with the hydrocarbon and forming a plasma. This produces a gaseous product consisting of hydrogen and a solid product containing carbon. The gap length is dynamically adjusted to control at least one plasma parameter. Preferably, the gap length is decreased during plasma generation or reforming and increased to boost the hydrogen production rate. The process preferably includes dynamically adjusting the spatial distance between the electrodes and rotating at least one electrode during hydrogen production to reduce the adhesion of solids to the electrodes.Furthermore, the polarity of the electrodes can be periodically reversed, primarily to reduce the adhesion of solids. If the hydrocarbon fluid is a liquid, the process can include controlling the liquid level relative to the electrodes.

[0004] CN 104445059 A discloses a device for generating synthesis gas using an AC plasma burner. The device comprises a reactor consisting of a grounding electrode, an insulating layer, an insulating cover, a gas ring, and a high-voltage electrode. The grounding electrode is shaped like a beer bottle. Its upper and lower ends are each annular with two open ends, the transition between the upper and lower ends being arc-shaped. The insulating cover is connected to the lower end of the grounding electrode. A nozzle is located at the opening in the upper end. The insulating layer is positioned against the inside of the lower end of the grounding electrode. The gas ring is arranged around the circumference of the lower end of the grounding electrode. The high-voltage electrode is mounted on the gas ring and is located on its central axis.

[0005] It is known to separate hydrocarbons, such as methane, natural gas, biogas or heavy oil, into activated carbon and hydrogen using the Kvaerner process in a plasma torch at about 1600 °C.

[0006] Furthermore, Gui-Bing Zhao et al., “Methane conversion in pulsed corona discharge reactors”, Chemical Engineering Journal 125 (2006) 67-79, reported on laboratory scale the conversion of methane into various carbon- and hydrogen-containing gases, such as ethyne, ethane, and ethene, in a coaxial pulsed corona discharge reactor. The corona discharge reactor uses a stainless steel wire as the anode and a stainless steel or niobium cathode surrounding the anode. The anode is arranged along a central axis of the cathode. The anode is positively charged, and the cathode is grounded. Gas flowing through the cathode is converted into a plasma by a high-voltage discharge from the anode. The corona discharge reactor is operated at voltages between 10 kV and 25 kV with pulse frequencies between 0 and 1000 Hz.

[0007] This is where the invention comes in, which provides an improved plasma lysis device for corona discharge-induced splitting of hydrogen-containing gases.

[0008] According to a first aspect, the invention relates to a plasma lysis device for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one byproduct. The plasma lysis device comprises a gas-tight reaction chamber, a gas supply line for the hydrogen-containing gas into the reaction chamber, exactly one plasma electrode for generating corona discharges in the reaction chamber by means of a high-frequency alternating voltage, and a gas outlet for the molecular hydrogen from the reaction chamber. The gas-tight reaction chamber is enclosed by a wall configured to electrically insulate the plasma electrode from an outer surface of the wall. The plasma electrode is connected to a high-frequency generator for generating the high-frequency alternating voltage.

[0009] The invention utilizes a so-called corona discharge, particularly at the tip of the plasma electrode and preferably at a gas nozzle tip of the plasma electrode, which directs the hydrogen-containing gas into the reaction chamber. The corona discharge generates a non-thermal plasma. This can reduce the energy consumption during the splitting of hydrogen-containing gases, as less energy is converted into inefficiently usable thermal energy. Consequently, the costs for the production of molecular hydrogen and the equipment or system for producing the molecular hydrogen can be reduced.

[0010] Furthermore, a higher efficiency can be achieved than with microwave plasma processes such as the Kvaerner process, which operate at an efficiency of approximately 60 percent. For example, an efficiency of 85% can be achieved with the plasma lysis device. This refers to the efficiency in terms of the electrical power required to generate molecular hydrogen. For example, 1 kg of molecular hydrogen can be produced with the plasma lysis device using 10 kWh. The Kvaerner process, for instance, requires 13.75 kWh or 1.25 kWh / m³ for the same amount of energy. 3 molecular hydrogen.

[0011] In contrast to microwave plasma processes, it is also not necessary to work under reduced pressure to produce molecular hydrogen with the plasma lysis device.

[0012] To electrically insulate the plasma electrode from the outside of the reaction chamber wall, the wall is designed such that the electric flux through its surface from the outside to the plasma electrode is zero. For this purpose, an inner surface of the wall opposite the plasma electrode has a floating potential. This allows a stronger electric field to be generated directly at the plasma electrode, thus improving the splitting of the hydrogen-containing gas. The wall can be, for example, an ungrounded, non-metallic wall. Alternatively, it can be a metallic wall with non-metallic insulation on its inner surface opposite the plasma electrode, such as a non-metallic insulating coating.

[0013] The invention recognizes that a corona discharge can be advantageously generated with exactly one plasma electrode. No counter electrode is required; instead, the counter electrode is spontaneously formed by portions of the inner wall of the reaction chamber, thus generating a strong electric field in the reaction chamber between the plasma electrode and these portions of the inner wall. Since only one plasma electrode is used, contamination and potential clogging of the plasma electrode with solid byproducts are reduced.

[0014] The invention is further based on the finding that, by using high-frequency alternating voltage with only one plasma electrode, corona discharge plasmas can be ignited and operated at atmospheric pressure. Operation at atmospheric pressure can reduce the costs for equipment and operation.

[0015] A corona discharge can occur in an electric field strong enough to spatially separate free electrons and ions in a gas after the ionization of an atom, preventing them from immediately recombinating. This can also be used to separate different atoms within molecules by breaking the bonds between them. These atoms can then recombine to form new or differently composed molecules. For example, methane can be split into carbon and hydrogen atoms, which can then recombine to form molecular hydrogen and solid carbon structures.

[0016] A corona discharge can proceed as follows. A first free electron can be generated by field ionization, producing the free electron and a positive ion. In this process, a strong electric field, for example near an electrode tip, alters the potential gradient for an electron bound in an atom, allowing it to overcome or tunnel through the potential barrier. Alternatively, a first free electron can also be generated when a high-energy photon strikes an atom and ionizes it via the photoelectric effect, resulting in the free electron and a positive ion. The high-energy photon can be provided, for example, by a radiation source, such as a UV radiation source, or by a natural event, such as a photon produced by cosmic radiation.

[0017] The strong electric field accelerates oppositely charged particles—the negatively charged free electron and the positively charged ion—in opposite directions, thus separating them spatially. The positively charged ion can be part of a multi-atom molecule, allowing the positively charged molecule to be accelerated. Due to the same amount of charge but a smaller mass, the electron is accelerated much more strongly than the positively charged ion and, upon colliding with another atom, can ionize it and create another free electron. Multiple free electrons can also collide with several atoms of the molecule, potentially splitting the molecule into its constituent atoms. Since each new free electron can create further free electrons, an electron avalanche can occur.

[0018] Some of the free electrons recombine with the positively charged ions, creating neutral atoms and producing a high-energy photon, which in turn can ionize further atoms. These photons are visible as the typical corona glow.

[0019] The electric field strength decreases so significantly at a certain distance from the plasma electrode that the electrons no longer have enough energy to generate further free electrons and positively charged ions. This limits the corona discharge and represents its outer boundary. The positively charged ions can recombine with electrons from the electrode or with free electrons. Furthermore, atoms can recombine with each other to form newly composed molecules.

[0020] Therefore, with the plasma lysis device according to the invention, larger quantities of hydrogen-containing gas can be efficiently split into molecular hydrogen and at least one by-product at lower costs.

[0021] The hydrogen-containing gas can, for example, contain methane. For instance, the hydrogen-containing gas can contain over 75% methane, preferably over 90%, for example, between 90% and 99% methane. In the corona discharge, the methane is split into hydrogen and elemental carbon; in particular, the chemical reaction n CH4 -> n C (s) + 2n H2 takes place, where n C (s) can contain various solid carbon structures, e.g., one or more carbon structures C kwith k less than or equal to n. Carbon structures can be, for example, elemental carbon particles, carbon nanotubes, fullerenes, carbon nanocones, or other carbon structures. The elemental carbon particles can, for example, have a size between 50 µm and 180 µm. Carbon layers can also form. This enables the efficient production of molecular hydrogen and elemental carbon from methane.

[0022] Alternatively or additionally, the hydrogen-containing gas can contain hydrogen sulfide. The hydrogen-containing gas can contain, for example, up to 35% hydrogen sulfide, or between 0% and 35% hydrogen sulfide. During the corona discharge, the hydrogen sulfide is split into hydrogen and elemental sulfur; specifically, the chemical reaction H₂S → H₂ + S(s) takes place. This enables the efficient production of molecular hydrogen and elemental sulfur from hydrogen sulfide.

[0023] The hydrogen-containing gas could be, for example, natural gas. Natural gas can contain, for example, the following substances: - between 30% and 99% methane, e.g. between 75% and 99% methane, especially between 90% and 99% methane, - between 0% and 15% ethane, e.g. between 1% and 15% ethane, especially between 1% and 3% ethane, - between 0% and 10% propane, e.g. between 1% and 10% propane, especially between 0.3% and 0.5% propane, - between 0% and 1% butane, especially between 0.1% and 0.2% butane, - between 0% and 1% ethene, - between 0% and 1% pentanes, especially between 0.01% and 0.03% pentanes - between 0% and 1% hexane, in particular between 0.001% and 0.02% hexane, - between 0% and 35% hydrogen sulfide, - between 0% and 70% nitrogen, e.g. between 0% and 15% nitrogen, especially between 0.5% and 1% nitrogen, - between 0% and 10% carbon dioxide, especially between 0.1% and 0.3% carbon dioxide.

[0024] Natural gas can also contain traces of oxygen, for example between 0.001% and 0.01%. Natural gas can also contain noble gases such as helium, argon, neon, krypton, or xenon, for example, in amounts between 0% and 15%.

[0025] The hydrogen-containing gas can also contain a hydrogen-containing substance that is liquid at room temperature, such as cyclohexane, heptane, toluene, gasoline, JP-8, or diesel, which has been converted into the gaseous state. The hydrogen-containing substance can be converted into the gaseous state, for example, by atomization and / or heating. For this purpose, an atomizer and / or a heating element can be provided, which can atomize and / or heat the liquid to convert it into the gaseous state. The atomizer and / or the heating element can be arranged, for example, upstream of or within the gas supply line that carries the hydrogen-containing gas into the reaction chamber. This also makes it possible to obtain molecular hydrogen from other hydrogen-containing substances that are not gaseous at room temperature.Furthermore, this can enable a significant reduction in carbon dioxide emissions from the transport sector. For this purpose, the plasma lysis device, or multiple plasma lysis devices, can be positioned, for example, between the fuel tank of a vehicle—such as a ship, aircraft, locomotive, railcar, truck, passenger car, or similar—and its propulsion system to convert fossil fuels, such as gasoline, JP-8, diesel, or heavy fuel oil, into molecular hydrogen and elemental carbon. The molecular hydrogen can be used directly as fuel in the vehicle's propulsion system. Alternatively, the molecular hydrogen, along with other gaseous byproducts, can be used as a synthetic fuel, such as synthetic gas. The hydrogen can also be used to power a fuel cell.This can then be used to power an electric motor. This allows vehicles to be adapted for hydrogen or synthetic gas operation. Furthermore, it can enable the continued use of the existing fossil fuel infrastructure while significantly reducing vehicle carbon dioxide emissions. The elemental carbon produced during plasma lysis can be collected in the vehicle. As a result, virtually carbon-neutral transportation using fossil fuels can be achieved if the fossil fuels are converted into molecular hydrogen in the plasma lysis device, which is then used to power the vehicles.

[0026] Advantageous embodiments of the plasma lysis device according to the invention are described below. The additional features of the exemplary embodiments can be combined with one another to form further embodiments, unless they are expressly described as alternatives to each other in the description.

[0027] The plasma lysis device can have a housing. The housing can contain the reaction chamber, the gas inlet, the plasma electrode, and the gas outlet. The reaction chamber can be formed by the housing, so that the wall of the reaction chamber is an outer wall of the housing. Alternatively, the reaction chamber can also be located inside the housing, so that the wall of the reaction chamber and the outer wall of the housing are not identical.

[0028] The high-frequency generator can be part of the plasma lysis device or connected to it as a separate unit. The high-frequency generator can be located inside or outside the housing. Preferably, the high-frequency generator is located outside the housing. In this case, electrical contact can be made externally, i.e., outside the housing.

[0029] The high-frequency generator can have a predetermined output impedance and be connected to the plasma electrode via an impedance matching network to match the impedance of the plasma generated at the plasma electrode by corona discharges and the output impedance of the high-frequency generator. The matching network can be part of the plasma lysis device or part of a separate device containing the high-frequency generator.

[0030] Advantageously, a so-called matching network (also called a matchbox) is used as a link between the high-frequency generator and the plasma generated during the corona discharge. This network matches the resistive and capacitive components of the plasma to an output impedance specified by the high-frequency generator. The plasma impedance depends in particular on the distance between the plasma electrode and the corona discharge, the composition of the hydrogen-containing gas, the properties of the reaction chamber and the housing enclosing the reaction chamber, the temperature in the reaction chamber, and the atmosphere within the reaction chamber.

[0031] The high-frequency generator can include a measuring device for measuring the intensity and power of a forward and a reflected wave. The measuring device can include a directional coupler and two detectors.

[0032] Preferably, the output impedance of the high-frequency generator is 50 ohms and / or the output power of the high-frequency generator is between 30 W and 5000 W. It has been shown that, particularly at this output impedance, a plasma is formed very reliably with a simultaneously good hydrogen yield.

[0033] Preferably, the high-frequency generator is designed to provide a high-frequency alternating voltage with a frequency in the range of 1 MHz to 40 MHz, in particular in the range of 10 MHz to 20 MHz, for example with a frequency of 13.56 MHz.

[0034] Advantageously, the matching network comprises at least one motor-controlled capacitor and at least one variable inductor, for example, two inductors. Together, these form an electrical resonant circuit, allowing the impedance matching to continuously respond to fluctuating loads caused by the plasma. In a further embodiment, the tuning of the capacitors and inductors is performed automatically using a reflection and standing wave control method.

[0035] The high-frequency generator can be configured to provide the alternating voltage in the form of sine waves. This can enable higher energy efficiency for the plasma generated during the corona discharge. Alternatively or additionally, the high-frequency generator can also be configured to provide the alternating voltage in a complex waveform, a rectangular waveform, or another waveform.

[0036] The plasma electrode can be massive.

[0037] The plasma electrode can have one opening. This opening can be connected to the supply line. The plasma electrode can be arranged such that the hydrogen-containing gas is introduced into the reaction chamber through the opening. This allows direct contact between the plasma electrode and the corona discharge plasma. This can reduce energy consumption during the splitting of hydrogen-containing gases, as the gas can be guided precisely through the non-thermal corona discharge plasma. Furthermore, this can enable additional pyrolysis. The plasma electrode can also have multiple openings connected to the supply line. This allows the hydrogen-containing gas to be introduced into the reaction chamber through several openings in the electrode. One or more of the openings can be designed to be opened and closed.For this purpose, flaps can be provided in the openings, or a sliding element can be inserted that can be moved in front of the respective openings to be closed. This can enable improved control of the corona discharge. Alternatively or additionally, the corona discharge can also be controlled, for example, by the amount of hydrogen-containing gas supplied via the gas line.

[0038] The opening of the plasma electrode can be designed as a nozzle for introducing the hydrogen-containing gas into the reaction chamber. Advantageously, this allows the non-thermal plasma generated by the corona discharge to form at the tip of the plasma electrode or the nozzle. Introducing the hydrogen-containing gas through the nozzle can cool the plasma electrode, particularly its tip. This reduces material stress. The nozzle can be in direct contact with the corona discharge plasma. The opening of the plasma electrode can have a variable cross-section between the side of the plasma electrode connected to the supply line and the side connected to the reaction chamber. In particular, the nozzle can taper and / or widen over a section. The nozzle can be, for example, a Venturi nozzle or a Laval nozzle.The nozzle shape and the diameter of the nozzle opening determine the duration of the corona discharge.

[0039] The plasma electrode can, for example, contain stainless steel, brass, and / or aluminum. Alternatively, the plasma electrode can also be made of stainless steel, brass, aluminum, or a combination thereof. Aluminum, for instance, offers good conductivity at a relatively low cost. The plasma electrode can also have different sections, such as a section made of stainless steel and a section made of brass or aluminum. The plasma electrode can be made of a temperature-resistant material that can withstand temperatures up to 800°C, for example. The plasma electrode can contain a catalyst, such as iron, cobalt, and / or nickel.

[0040] Additionally or alternatively, the plasma electrode can have a coating, for example, a catalytic coating such as a nickel, iron, cobalt, or platinum coating. This coating can enable a catalytic effect. Alternatively, the coating can also contain a ceramic material, such as aluminum oxide, nickel oxide, and / or titanium dioxide. The coating can have a thickness of, for example, 200 µm to 1000 µm.

[0041] The plasma electrode can have an outer diameter between 4 mm and 16 mm, for example, 8 mm. The opening of the plasma electrode can have a diameter between 0.1 mm and 1 mm, for example, 0.4 mm. If the plasma electrode has multiple openings, their combined diameter can, for example, be between 0.1 mm and 1 mm. The diameter of the opening of the plasma electrode can vary along its longitudinal axis between the end connected to the gas supply and the end connected to the reaction chamber. The plasma electrode can have a length between 50 mm and 300 mm, for example, 150 mm.

[0042] The opening of the plasma electrode can be threaded. For example, an aluminum turned part can be fitted into the opening. A nozzle can be arranged in the opening of the plasma electrode. The nozzle can, for example, be screwed into the opening, forming a reduced opening of the plasma electrode. For this purpose, the nozzle can, for example, have an external thread. The nozzle can be made of one or more materials, such as brass and stainless steel. The nozzle can be an FDM nozzle, as used, for example, for fused deposition modeling. The material or materials of the nozzle can be temperature-resistant, for example, up to a temperature of 800°C. The nozzle material can contain a catalyst. The nozzle can also have a coating, for example, a catalytic coating.

[0043] The plasma electrode can be electrically connected via a pipe plug.

[0044] The plasma electrode can be designed, for example, to be subjected to a power output in the range between 30 W and 5000 W.

[0045] The plasma lysis device can be configured to emit pulsed gas streams from the plasma electrode opening to remove solid byproducts forming in the reaction chamber. This can prevent the plasma electrode, the opening of the plasma electrode, and / or the reaction chamber from becoming clogged with solid byproducts formed during the corona discharge. The gas streams can be generated using hydrogen-containing gas or another gas, such as an inert gas. The hydrogen-containing gas or the inert gas can be supplied via the gas supply line. Preferably, the plasma lysis device is configured such that no corona discharge occurs during the pulsed gas streams. For this purpose, the supply of the high-frequency voltage to the plasma electrode can be briefly interrupted during the emission of a pulsed gas stream, thus preventing a corona discharge from being generated.

[0046] The plasma lysis device may have a control unit or be connected to one. The control unit may be configured to regulate the emission of pulsed gas pulses. For example, the plasma lysis device may be configured to emit pulsed gas pulses from the plasma electrode opening at timed intervals. Alternatively, the plasma lysis device may be configured to emit pulsed gas pulses from the plasma electrode opening in response to an event. This event may, for example, depend on a power input to the plasma lysis device. In particular, the event may be that a power input threshold is undershot.In this case, the control unit can detect the power input and control the plasma lysis device so that a pulsed gas is released from the plasma electrode opening as soon as the power input falls below the threshold. This can enable more efficient operation of the plasma lysis device. Furthermore, it can prevent the plasma electrode and / or the reaction chamber from becoming clogged with solid by-products.

[0047] Alternatively or additionally, pulsed gas bursts can also be released from other openings and / or nozzles to remove solid byproducts from the reaction chamber. This makes it possible to remove solid byproducts from the reaction chamber and thus clean it.

[0048] The ungrounded, non-metallic wall of the gas-tight reaction chamber can, for example, contain or be formed from a ceramic. Macor, for instance, with a chemical composition of 46% SiO2, 17% MgO, and 16% Al, can be used as the ceramic. z O3, 10% K2O, 7% B2O3, 4% F, in which mica is incorporated into a borosilicate glass matrix. The wall can also be made of or contain quartz glass, for example.

[0049] The wall of the reaction chamber can also have a metallic outer surface and a non-metallic, electrically insulating inner surface. The non-metallic, electrically insulating inner surface can, for example, be made of Teflon.

[0050] The wall can, for example, have a wall thickness of at least 4 mm.

[0051] The cross-section of the reaction chamber can increase in the direction from the gas inlet to the gas outlet. This can reduce the adhesion of solid byproducts to the inner wall. Furthermore, this can reduce turbulence in the reaction chamber and facilitate better removal of molecular hydrogen and byproducts. The reaction chamber can, for example, be funnel-shaped. The opening of the plasma electrode can, for example, be positioned at a midpoint within the reaction chamber.

[0052] The plasma lysis device can be configured to apply a DC voltage to the wall of the reaction chamber. This DC voltage can cause solid byproducts forming in the reaction chamber, such as carbon, to be drawn towards the wall, thus reducing the amount of solid byproduct deposited on the plasma electrode. Preferably, the plasma lysis device is configured such that the DC voltage is applied to the inside of the wall of the reaction chamber. The DC voltage can be, for example, in the range between 0 V and 20 kV, preferably between 5 kV and 15 kV, with a current of 0.01 mA to 250 mA, for example, at 10 kV with a current of 10 mA. The plasma lysis device can be connected to or include a DC voltage source to provide the DC voltage.The DC voltage source can be connected to the wall, in particular the inside of the wall of the reaction chamber, in order to apply the DC voltage to the wall of the reaction chamber.

[0053] The plasma lysis device can have a discharge for at least one solid byproduct from the reaction chamber. Solid byproducts can be in powder form, for example. Discharging the solid byproducts from the reaction chamber can improve process efficiency, as they can no longer interfere with the fission process. For example, solid byproducts can be powdered carbon if the hydrogen-containing gas is methane, and powdered sulfur if the hydrogen-containing gas is hydrogen sulfide.

[0054] The gas outlet for molecular hydrogen can be arranged, for example, in the direction of flow of the hydrogen-containing gas or perpendicular to it. The gas outlet for molecular hydrogen can also be designed to remove gaseous byproducts from the reaction chamber. Furthermore, the gas outlet can be designed to remove solid byproducts, for example, in the form of particles, that are carried along with the gas stream from the reaction chamber.

[0055] The reaction chamber can comprise a main chamber and a secondary chamber. The plasma electrode can be positioned relative to the main chamber such that the corona discharge ignites in the main chamber. The secondary chamber can be located above the main chamber, allowing solid byproducts to flow into it. In this case, the solid byproducts, for example in the form of particles, can be carried away from the reaction chamber by the gas stream formed by the molecular hydrogen and gaseous byproducts. Alternatively, the secondary chamber can be located below the main chamber, allowing solid byproducts to fall into it.

[0056] The secondary chamber can therefore be located further away from or closer to the Earth's center of mass than the plasma electrode during operation of the plasma lysis device. Thus, the secondary chamber can be positioned further away from or closer to the Earth's center of mass than the corona discharge site. Solid byproducts generated during the corona discharge can fall downwards into the secondary chamber due to gravity if the secondary chamber is located closer to the Earth's center of mass than the plasma electrode during operation. If the secondary chamber is located further away from the Earth's center of mass than the plasma electrode during operation, the gas outlet is preferably positioned opposite the opening of the plasma electrode, so that solid byproducts generated during the corona discharge are carried away from the reaction chamber by the gas flow into the gas outlet.This makes it easy to remove solid byproducts from the main chamber so that they cannot interfere with the corona discharge.

[0057] The side chamber can be connected to the drain for at least one solid byproduct in order to remove the solid byproduct from the reaction chamber. This allows the solid byproduct to be taken up by the side chamber and removed from it via the drain. If the solid byproduct is, for example, carbon, the side chamber can serve as a carbon storage tank.

[0058] The secondary chamber, the gas vent, and / or the vent may include a discharge device for removing byproducts. The discharge device may be designed to remove solid byproducts from the reaction chamber in such a way that no gas can enter the reaction chamber through it. The discharge device may, for example, include a flap, an eccentric, a screw conveyor, a rotary valve, or another type of discharge mechanism. Overpressure may be generated in the discharge device to prevent gas from entering it. A pump may be provided for this purpose. This allows the solid byproducts to be removed from the plasma lysis device without allowing gas to enter the reaction chamber from the outside.

[0059] In one embodiment, where the discharge device is a flap, it is preferably arranged at a fork in the gas discharge and configured to direct the gas flow from the reaction chamber either into one of the lines adjoining the fork or into the other. For this purpose, the flap closes one of the lines. The flap can, for example, be arranged on a controllable hinge so that, depending on whether a pulse of gas is emitted from the opening of the plasma electrode, the flap closes one or the other line. This can make it possible to separate solid byproducts, which are discharged from the reaction chamber by a pulse of gas, from the molecular hydrogen produced in the corona discharge.

[0060] Additionally or alternatively, the discharge device can also include one or more pressure-controlled particle filters designed to capture solid byproducts and release them upon an abrupt pressure change. This abrupt pressure change can be generated, for example, by a sudden gas pulse. This can improve the separation of solid byproducts from molecular hydrogen.

[0061] The main chamber and the secondary chamber can be enclosed by different reaction chamber sections. The reaction chamber section enclosing the main chamber can, for example, be made of quartz glass. This reaction chamber section can also be a housing component. This allows for observation of the reaction taking place within the reaction chamber. The reaction chamber section enclosing the main chamber can, for example, have a wall thickness of at least 4 mm.

[0062] The inner surface of the secondary chamber wall can have a higher electrostatic potential than the inner surface of the main chamber wall. This can cause solid byproducts from the main chamber to be attracted towards the secondary chamber.

[0063] The gas outlet for molecular hydrogen can be located above the plasma electrode. Preferably, the gas outlet for molecular hydrogen is located above the plasma electrode when the hydrogen-containing gas is introduced into the reaction chamber through the opening of the plasma electrode. The gas outlet for molecular hydrogen can therefore be located further from the Earth's center of mass than the plasma electrode and thus also further from the Earth's center of mass than the location of the corona discharge. This facilitates the separation of gaseous and solid components generated during the corona discharge. Preferably, the gas outlet for molecular hydrogen is arranged in the direction of flow of the hydrogen-containing gas. This can improve the removal of the resulting molecular hydrogen.This is the case, for example, when the hydrogen-containing gas is introduced into the reaction chamber through the opening of the plasma electrode and the gas outlet for the molecular hydrogen is located opposite the plasma electrode.

[0064] Preferably, the distance between the wall of the reaction chamber and the plasma electrode is at least 40 mm. This distance is defined as the smallest distance between an inner surface of the reaction chamber wall and an outer diameter of the plasma electrode. Alternatively or additionally, the distance between the wall of the reaction chamber and the tip of the plasma electrode is at least 40 mm. Alternatively or additionally, the distance between the gas outlet and the plasma electrode is at least 60 mm. This provides electrical insulation, preventing flashovers between the plasma electrode and other potentials, such as the wall of the reaction chamber or the housing. Furthermore, this reduces the accumulation of solid by-products in the reaction chamber, as sufficient space is provided to collect and remove them.

[0065] The plasma lysis device can be configured to introduce hydrogen-containing gas into the reaction chamber at a flow rate between 1 l / min and 100 l / min, for example, at a flow rate of 2 l / min. The higher the flow rate, the better the plasma lysis device is suited to removing solid, agglomerating structures of the by-product from the reaction chamber. In particular, if the hydrogen-containing gas contains methane, increasing the flow rate allows more solid carbon structures to be removed from the reaction chamber. However, beyond a certain flow rate, a higher flow rate reduces the process efficiency and the yield of molecular hydrogen. The plasma lysis device can be configured to adjust the flow rate to optimize the hydrogen yield.

[0066] The reaction chamber may include a cleaning element for removing solid byproducts. This cleaning element enables the removal of solid byproducts that can accumulate in the reaction chamber during operation of the plasma lysis device. This prevents or at least reduces the disruptive influence of solid byproducts on the corona discharge. During operation of the plasma lysis device, for example, tree-like structures or long rods, such as graphite rods, can grow from the solid byproduct and accumulate on the inner wall of the reaction chamber. These tree-like structures or long rods can, for example, grow at the tip of the plasma electrode and temporarily form part of it. The cleaning element also allows for the mechanical removal of such disruptive solid byproducts that cannot be removed by increasing the gas flow rate.

[0067] The reaction chamber can also include multiple cleaning elements. For example, one cleaning element for removing solid byproducts from the inside of the reaction chamber wall and another for removing solid byproducts from the plasma electrode. This can enable improved removal of solid byproducts from the reaction chamber.

[0068] The cleaning element can be positioned on the inner side of the reaction chamber wall to remove at least one solid byproduct from the reaction chamber. For example, the cleaning element can be movable along the inner side of the reaction chamber wall. This allows for the mechanical removal of solid byproducts that form in the reaction chamber due to the corona discharge and adhere to the inner side of the reaction chamber wall. The cleaning element can have a recess or opening in its center with a larger diameter than the outer diameter of the plasma electrode. This allows the cleaning element to be moved along the entire length or height of the reaction chamber.

[0069] Alternatively or additionally, the cleaning element can also include a rotating element to rotate the plasma electrode relative to the wall of the reaction chamber about a common longitudinal axis. For this purpose, sliding sealing rings can be provided between the walls of the reaction chamber and the plasma electrode. The cleaning element can break up, by rotating, any structures of solid by-product that may extend from the plasma electrode to the inside of the wall of the reaction chamber. By rotating the plasma electrode relative to the wall of the reaction chamber during the corona discharge, the formation of such structures can also be prevented in the first place.

[0070] Alternatively or additionally, the cleaning element can also be arranged on the plasma electrode and be movable around its longitudinal axis relative to the plasma electrode. This can facilitate the removal of solid by-product from the plasma electrode. The cleaning element itself can be movable, and / or the plasma electrode can be rotatable around its longitudinal axis, allowing the cleaning element to move relative to the plasma electrode. The cleaning element can also be fixed in position if the plasma electrode is rotatable around its longitudinal axis. The cleaning element can have a scraper or edge for the mechanical removal of solid by-product. This can facilitate easier mechanical removal of solid by-product.

[0071] The cleaning element can also include one or more nozzles for purging the reaction chamber. The reaction chamber can be purged, for example, with a pulse of gas. For this purpose, the nozzle(s) can be supplied with hydrogen-containing gas or another gas, such as an inert gas. The nozzles can be arranged, for example, in the wall of the reaction chamber, particularly on its inner surface. This can improve the removal of by-products, especially solid by-products, from the reaction chamber. The cleaning element can also include an ultrasonic cleaning device designed to vibrate the gas near solid by-products deposited in the reaction chamber in order to remove them.

[0072] The control unit of the plasma lysis device, or the control unit connected to the plasma lysis device, can be configured to control parameters of the plasma lysis device, such as the flow rate of the hydrogen-containing gas, the temperature of the hydrogen-containing gas, the temperature in the reaction chamber, the temperature of the plasma electrode, the pressure in the reaction chamber, the voltage level of the AC voltage, the frequency of the AC voltage, the frequency of the corona discharges, or other parameters of the plasma lysis device. In particular, the control unit can be configured to control the parameters of the plasma lysis device depending on the composition of the hydrogen-containing gas.

[0073] The plasma lysis device may include a temperature control element, such as a heating element and / or a cooling element, for the reaction chamber to set a temperature within the chamber. Changing the temperature within the reaction chamber can increase the hydrogen yield. Preferably, the reaction chamber is neither cooled nor heated, so that it is generally at ambient temperature before a corona discharge occurs.

[0074] The plasma lysis device can be configured to utilize heat generated in the reaction chamber for pyrolysis. This enables the additional splitting of the hydrogen-containing gas via a pyrolysis reaction. Alternatively or additionally, the heat can also be dissipated. For example, the heat can be removed from the reaction chamber via gas discharge, along with the molecular hydrogen and / or gaseous byproducts. Heat exchangers can then be used for other purposes, such as heating buildings. The heat can, for instance, be used in a heating system.

[0075] The plasma lysis device may additionally or alternatively include an electrode temperature control element, such as an electrode cooling element, for the plasma electrode to set the temperature of the plasma electrode. The plasma electrode can, for example, be set to a temperature in the range between 60°C and 400°C, 60°C and 70°C, or 350°C and 400°C.

[0076] The plasma lysis device may include a pump to adjust the pressure within the reaction chamber. Changing the pressure within the reaction chamber can increase the hydrogen yield. Preferably, the reaction chamber is at ambient pressure before the hydrogen-containing gas is introduced.

[0077] The plasma lysis device can have a supply line for an inert gas. Alternatively, the inert gas can be introduced into the reaction chamber along with the hydrogen-containing gas via the hydrogen-containing gas supply line. The inert gas can contain, for example, nitrogen and / or one or more noble gases, such as helium or argon. The inert gas can increase the reaction rate because more electrons and photons are available for the corona discharge. The inert gas can also aid in cleaning the reaction chamber.

[0078] The wall of the reaction chamber can be made of a temperature-resistant material suitable for temperatures of, for example, at least 800°C. The wall can also consist of several materials, preferably all of which are temperature-resistant up to at least 800°C. The material(s) can also be dimensionally stable. The wall of the reaction chamber can incorporate thermal insulation. This can provide a temperature-resistant and dimensionally stable wall for the reaction chamber.

[0079] The wall of the reaction chamber can be pressure-resistant, for example, up to 10 bar overpressure. Preferably, the wall of the reaction chamber is designed to withstand a continuous overpressure of up to 10 bar. Particularly preferably, the wall of the reaction chamber is designed to withstand even sudden gas pulses with pressures higher than 10 bar.

[0080] The plasma lysis device can incorporate electrical insulation to protect against electrical arcing between the plasma electrode and another potential, such as the wall of the reaction chamber or the housing. This electrical insulation can be achieved, for example, by maintaining a distance between the plasma electrode and the inside wall of the reaction chamber.

[0081] The reaction chamber can contain a catalyst, for example nickel, iron, ruthenium, cobalt or platinum.

[0082] The plasma lysis device can include a particle filter to filter out particles. Preferably, the particle filter is arranged in the gas supply line for the hydrogen-containing gas to filter particles from the hydrogen-containing gas before it enters the reaction chamber. This can reduce impurities from particles in the gas stream, which can lead to unwanted byproducts. The plasma lysis device can also include multiple particle filters. Preferably, one of the particle filters is arranged in the gas outlet to filter particles from the gas stream that is routed from the reaction chamber into the gas outlet.

[0083] The plasma lysis device can include one or more membranes and / or one or more adsorbers to filter gaseous byproducts from a gas stream in the molecular hydrogen outlet. These can be located, for example, within the molecular hydrogen outlet or at one end of it. Polymer membranes, for instance, can be used to separate molecular hydrogen from the gaseous byproduct. Adsorbers can be, for example, ceramic materials with a large surface area and high adsorption capacity for a suitable gaseous byproduct, particularly molecular sieves. Besides zeolites (crystalline aluminosilicates), carbon molecular sieves can also be used. Silica gel or activated aluminum oxide, for example, can be used as adsorbers.Zeolite Socony Mobil-5 (ZSM-5), a synthetic high-silica aluminosilicate zeolite, can also be used as an adsorber. This allows gaseous byproducts to be separated from molecular hydrogen. Furthermore, the gaseous byproduct can be returned to the reaction chamber via the feed line. This can increase the yield of molecular hydrogen.

[0084] Furthermore, the membrane or selective adsorber can also be selectively introduced into the molecular hydrogen gas stream to adjust the composition of the gas flowing through it. For example, depending on the requirements for a methane-hydrogen fuel, methane remaining in the gas stream can be selectively mixed with molecular hydrogen in a predetermined ratio. This can make it possible to provide a synthetic fuel, in particular a synthetic gas.

[0085] The plasma lysis device can include a reservoir. The reservoir can be connected to the gas outlet for the molecular hydrogen. One or more membranes can be arranged in the reservoir. The adsorber can also be located in the reservoir. The adsorber can be arranged, for example, as a packed bed or an open-pore foam. The adsorber for separating molecular hydrogen and gaseous byproducts is advantageously designed such that the gaseous byproducts are preferably bound to it via adsorption. However, combinations of membranes and adsorbers can also be used for different gaseous byproducts. For example, polymer membranes effectively separate CO2, CH4, and N2, but zeolites such as ZSM-5 can also be used.

[0086] The reservoir may include a release device for dissolving the adsorbed gaseous byproduct. This device may, for example, be a heater for thermally dissolving the gaseous byproduct or a vacuum pump for applying negative pressure. Alternatively, the reservoir may have a closable opening through which the loaded absorber can be replaced with an unloaded one after adsorption.

[0087] The plasma lysis device can be used in stationary or mobile structures. Stationary structures include, for example, fixed buildings or facilities such as stationary biogas reactors or stationary wastewater treatment plants. Mobile structures include, for example, mobile buildings, drilling platforms, and vehicles such as airplanes, trucks, cars, trains, or ships, especially cruise ships.

[0088] According to a further aspect, the invention relates to a plasma lysis system for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one byproduct. The plasma lysis system comprises at least two plasma lysis devices according to one of claims 1 to 9 or an embodiment of the plasma lysis device. The plasma lysis devices are arranged in parallel or in series with one another. The plasma lysis devices can, for example, be arranged in series with one other by connecting at least one gas outlet of a preceding plasma lysis device to a gas inlet of a subsequent plasma lysis device. This makes it possible to arrange several plasma lysis devices in series to enable complete splitting of the hydrogen-containing gas. In particular, the reaction chambers of the plasma lysis devices can thus be interconnected.The plasma lysis devices can, for example, also be arranged in a ring, i.e., such that the plasma lysis devices form a ring, with each gas outlet of a preceding plasma lysis device connected to the gas inlet of a subsequent plasma lysis device. The plasma lysis system can provide a gas outlet to remove the molecular hydrogen from the system. In the case of a ring-shaped plasma lysis system, the gas outlet is an additional outlet alongside the existing gas outlet, each connected to the gas inlet of the subsequent plasma lysis device.

[0089] The plasma lysis system enables the scaling of corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one byproduct. Any number of plasma lysis devices can be operated in parallel to obtain large quantities of hydrogen from hydrogen-containing gases.

[0090] The plasma lysis devices of the plasma lysis system can be controlled via a common control unit.

[0091] The common control unit can be configured to control the parameters of the plasma lysis device, in particular depending on the composition of the hydrogen-containing gas.

[0092] The plasma lysis system can include a temperature control unit to set the temperature of the hydrogen-containing gas. The temperature control unit can, for example, include a heat exchanger and / or a cooling unit. This allows pre-tempered hydrogen-containing gas to be introduced into the reaction chamber or gas supply line. Furthermore, hydrogen-containing liquids can be converted into the gaseous state. The temperature control unit can be located outside the plasma lysis devices or be part of one or more of the plasma lysis devices. For example, the temperature control unit can be located in one of the gas supply lines for the hydrogen-containing gas.

[0093] The plasma lysis system may include one or more fans for adjusting the flow rate through the plasma lysis devices.

[0094] The plasma lysis system can incorporate one or more radiation sources, such as ultraviolet (UV) radiation sources. These can enable improved control of the corona discharge ignition. For this purpose, the radiation source can be positioned so that it can direct its radiation precisely to the corona discharge site.

[0095] The plasma lysis system can include one or more high-frequency generators. These can be configured to provide a high-frequency alternating voltage to a plasma electrode of the respective plasma lysis device.

[0096] The plasma lysis system can include a storage tank containing a substance from which hydrogen-containing gas can be produced, for example, a storage tank containing composted materials or a tank containing kerosene, JP-8, heavy fuel oil, gasoline, or diesel. Additionally or alternatively, the plasma lysis system can include a storage tank containing hydrogen-containing gas. Additionally or alternatively, the plasma lysis system can include a power plant for providing energy for the corona-discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one byproduct. Additionally or alternatively, the plasma lysis system can include a hydrogen storage tank for storing the molecular hydrogen. Additionally or alternatively, the plasma lysis system can include a propulsion system that can be powered by molecular hydrogen, for example, a hydrogen combustion engine.Additionally or alternatively, the plasma lysis system can include an energy system that can be operated with molecular hydrogen.

[0097] The hydrogen-containing gas storage tank can be connected to one or more of the plasma lysis devices. In particular, the hydrogen-containing gas storage tank can be connected to a gas supply line of one or more of the plasma lysis devices. The hydrogen-containing gas storage tank can, for example, be connected to or part of a biogas reactor, a wastewater treatment plant, or a natural gas storage facility.

[0098] The power supply system for corona discharge-induced splitting of hydrogen-containing gases can be connected to the high-frequency generator(s) to provide a high-frequency voltage for the plasma electrodes. The power supply system can be a renewable energy source, such as a wind turbine, a solar power plant, a hydroelectric power plant, or a biogas plant.

[0099] The energy system powered by molecular hydrogen can be connected to the hydrogen storage system or to at least one of the plasma lysis devices. The energy system powered by molecular hydrogen can, for example, include a fuel cell or a combined heat and power (CHP) unit. The molecular hydrogen can be used, for example, for heat generation, such as by using it in a hydrogen-powered CHP unit to produce heat.

[0100] The plasma lysis system can enable emission-free energy production. If biogas is used as a hydrogen-containing gas, it can even create a carbon dioxide sink, thus sustainably reducing carbon dioxide in the air and especially in the atmosphere.

[0101] The plasma lysis system can be used in a stationary structure or a mobile structure, especially in a vehicle.

[0102] According to a further aspect, the invention relates to the use of a plasma lysis device according to one of claims 1 to 9 or an embodiment of the plasma lysis device for splitting hydrogen-containing gas into molecular hydrogen and at least one by-product using hydrogen-containing gas provided in an operation of a stationary structure or a mobile structure.

[0103] Instead of one plasma lysis device, several plasma lysis devices or a plasma lysis system according to claim 10 or 11 or another embodiment of the plasma lysis system can also be used to split hydrogen-containing gas into molecular hydrogen and at least one by-product using hydrogen-containing gas provided in an operation of a stationary structure or a mobile structure.

[0104] The hydrogen-containing gas can be supplied, for example, by a stationary structure such as a stationary biogas reactor or a stationary wastewater treatment plant. The plasma lysis device can also be used, for example, to provide molecular hydrogen for a molecular hydrogen-powered energy system, such as a fuel cell or a combined heat and power (CHP) unit. The plasma lysis device can be used, for example, in a hotel, a shopping mall, a store, a factory, or another type of building.

[0105] The hydrogen-containing gas can also be supplied by a mobile structure, such as a vehicle. In other words, the plasma lysis device can also be used in a vehicle. For example, a vehicle, such as a cruise ship, could have a wastewater treatment plant to supply hydrogen-containing gas, e.g., biogas. The hydrogen-containing gas can also be supplied by other vehicles, such as a passenger car or a truck. For this purpose, gasoline or diesel, for example, can be converted into the gaseous state and supplied to the plasma lysis device. The molecular hydrogen can also be stored in a storage system, such as a hydrogen storage tank, to be used as fuel for vehicles, for example, for freight or passenger transport.Furthermore, the plasma lysis device can be used to convert biogas or natural gas into molecular hydrogen and at least one byproduct. The plasma lysis device can be powered, for example, by energy from a renewable energy source, such as a wind turbine, a solar power plant, or a hydroelectric power plant.

[0106] The byproduct formed by splitting hydrogen-containing gas can contain, for example, carbon. This byproduct can contain various carbon structures that have applications in the construction industry, the electronics industry, and lightweight construction. Furthermore, these carbon structures can also be used in paints and coatings, as well as in tire manufacturing.

[0107] According to a further aspect, the invention relates to a method for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product. The method comprises the process steps of - Introducing a hydrogen-containing gas into a gas-tight reaction chamber, - Generating a corona discharge by means of exactly one plasma electrode operated with a high-frequency alternating voltage in the reaction chamber, wherein the gas-tight reaction chamber is enclosed by a wall which is designed to electrically insulate the plasma electrode from an outside of the wall and - Removal of the molecular hydrogen and at least one by-product from the reaction space.

[0108] The hydrogen-containing gas can be introduced into the reaction chamber via a hydrogen gas inlet. The high-frequency alternating voltage can be supplied to the plasma electrode by a high-frequency generator. The molecular hydrogen can be removed from the reaction chamber via a molecular hydrogen outlet.

[0109] The hydrogen-containing gas can be introduced into the reaction chamber through an opening in the plasma electrode.

[0110] The hydrogen-containing gas may contain methane and / or hydrogen sulfide. It may also contain, for example, natural gas and / or biogas. Alternatively or additionally, the hydrogen-containing gas may also contain cyclohexane, heptane, toluene, gasoline, JP-8, and / or diesel fuel converted to the gaseous state. If the hydrogen-containing gas contains biogas, a carbon dioxide sink can be created through process engineering. This can, for example, remove carbon dioxide from the air faster than reforestation.

[0111] The procedure may include the following steps: - Filtering the by-product from a gas stream of molecular hydrogen and by-product.

[0112] The byproduct may contain solid byproducts, for example in the form of particles. Solid byproducts can be filtered, for example, using a particle filter. Furthermore, the byproduct may contain gaseous byproducts. These can be filtered, for example, using a membrane or an adsorber.

[0113] The process may include the following steps: - Collection of gases produced by splitting the hydrogen-containing gas in the gas discharge for molecular hydrogen and / or a reservoir for molecular hydrogen, - Separation of the resulting gases via a multi-stage membrane process and / or via the use of selective adsorption processes.

[0114] This allows for easy separation of the resulting gases and thus also for the collection of molecular hydrogen and gaseous byproducts.

[0115] In a selective adsorption process, for example, the gas produced from splitting the hydrogen-containing gas is passed through a reservoir containing at least one adsorber. One type of gas from a gaseous byproduct can be bound to this adsorber via adsorption. Another type of gas, such as molecular hydrogen, can thus be released initially on its own. The adsorbed gas can then be released from the adsorber in a further step, for example, by pressurization or thermal dissolution.

[0116] The process may involve one step: - Removal of solid by-product from the reaction chamber.

[0117] Solid byproducts can be removed from the reaction chamber, for example, by means of a solid byproduct drain. A discharge device can be provided for this purpose.

[0118] The procedure may include the following steps: - Cleaning the reaction chamber to remove solid by-product from the reaction chamber.

[0119] Cleaning the reaction chamber can include, in particular, the mechanical removal of solid by-product, for example by means of a cleaning element or by blowing out the reaction chamber using gas pulses.

[0120] Examples of embodiments can also be found in the claims.

[0121] Further embodiments of the device and the method are described below with reference to the drawings. The drawings show: Fig. 1 A schematic representation of an embodiment of a plasma lysis device for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product according to the first aspect of the invention; Fig. 2 A photographic representation of a plasma lysis device during operation of the Fig. 1 emerging carbon structure at the tip of the plasma electrode of the plasma lysis device; Fig. 3 A photographic representation of a corona discharge at the plasma electrode in the reaction chamber of the plasma lysis device of the Fig. 1; Fig. 4 A schematic representation of an embodiment of a plasma lysis system for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product according to a further aspect of the invention; Fig. 5 A schematic representation of a flow diagram of an embodiment of a method for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product according to a further aspect of the invention Fig. 6 A schematic representation of a further embodiment of a plasma lysis device for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product according to the first aspect of the invention; Fig. 7 A schematic representation of a further embodiment of a plasma lysis system according to a further aspect of the invention.

[0122] Fig. Figure 1 shows a schematic representation of an embodiment of a plasma lysis device 100 for corona discharge-induced splitting of hydrogen-containing gases 10 into molecular hydrogen 12 and at least one by-product 14. In this embodiment, the by-product 14 is solid. The hydrogen-containing gas 10 can, for example, contain methane, which can be split into molecular hydrogen 12 and solid carbon as by-product 14. In one embodiment, for example, the plasma lysis device can convert methane into elemental carbon and a gas with 80% molecular hydrogen, 10% acetylene, and 10% residual methane. In other embodiments, an almost complete conversion of the methane into carbon and molecular hydrogen is also possible.

[0123] The plasma lysis device 100 has a housing 16 that gas-tightly encloses a reaction chamber 18. Furthermore, the plasma lysis device 100 has a gas inlet 20, exactly one plasma electrode 22, a gas outlet 24, and a discharge 26. The discharge 26 is optional. Instead of the discharge 26, for example, a flap can also be provided in the base of the plasma lysis device to discharge the solid by-product 14 (not shown). In other embodiments, the solid by-product can also be discharged, for example, via the gas outlet.

[0124] The plasma electrode 22 is connected to a high-frequency generator 200. In this embodiment, the high-frequency generator 200 is a separate unit connected to the plasma lysis device 100. In other embodiments, the high-frequency generator can also be part of the plasma lysis device (not shown). The high-frequency generator 200 generates a high-frequency alternating voltage for the plasma electrode 22 and contacts the plasma electrode 22 from outside the housing 16. The high-frequency generator 200 can include a matching network to perform impedance matching (not shown). The matching network can also be part of the plasma lysis device. In this embodiment, the high-frequency generator 200 provides a power output between 30 W and 5000 W and has an output impedance of 50 ohms.The high-frequency generator provides the high-frequency alternating voltage with a frequency in the range of 1 MHz to 40 MHz, especially in the range of 10 MHz to 20 MHz, for example with a frequency of 13.56 MHz.

[0125] In this embodiment, the reaction chamber 18 has a non-grounded, non-metallic wall 28. In this embodiment, the wall is made of quartz glass with a wall thickness of 4 mm. In other embodiments, a different material, for example a ceramic such as Macor, can be used, and a different wall thickness, for example, quartz glass with a minimum thickness of 4 mm, can be used. Furthermore, a metallic wall with non-metallic insulation on its inner surface opposite the plasma electrode, e.g., with a non-metallic insulating coating, can also be provided to electrically insulate the plasma electrode from an outer surface of the wall. An inner surface 30 of the wall 28 of the reaction chamber 18 spontaneously forms a counter electrode during operation of the plasma lysis device 100.Furthermore, the reaction chamber 18 is designed to be gas-tight, so that gas can only be introduced into the reaction chamber 18 via the gas supply line 20 and discharged from the reaction chamber 18 via the gas outlet 24. In this embodiment, a particle filter 21 is additionally arranged in the gas supply line 20, which filters out solid particles from the hydrogen-containing gas 10.

[0126] The plasma electrode 22 is arranged along a central longitudinal axis of the plasma lysis device 100, so that in this embodiment it is opposite the gas outlet 24. The wall 28 of the reaction chamber 18 is arranged coaxially with the plasma electrode 22. The plasma electrode 22 serves to generate corona discharges 32 in the reaction chamber 18 by means of the high-frequency alternating voltage (see Figure 1). Fig. 2) In this embodiment, the plasma electrode 22 has an opening 34 connected to the gas supply line 20. The gas supply line 20 carries the hydrogen-containing gas 10 through the opening 34 of the plasma electrode 22 into the reaction chamber 18. In this embodiment, a nozzle 36 is screwed into the opening 34 of the plasma electrode 22, thus forming part of the plasma electrode 22. The plasma electrode 22 is made of stainless steel and includes a turned aluminum part for screwing in the nozzle 36. The nozzle 36 is an FDM printer nozzle made of brass and stainless steel.

[0127] The plasma lysis device 100 is used for gas processing by means of a non-thermal plasma generated by the corona discharge 32. For this purpose, the hydrogen-containing gas 10 is injected into the reaction chamber 18 through the plasma electrode 22 and its nozzle 36. A high-frequency alternating voltage is applied to the plasma electrode 22, generating a corona discharge 32. The plasma lysis device 100 can, for example, split hydrogen-containing gas 10, which essentially contains methane. Through contact with the non-thermal plasma, the methane is separated—under exclusion of oxygen, i.e., in the gas-tight reaction chamber 18—into elemental, powdered carbon 14 and molecular hydrogen 12. The resulting molecular hydrogen 12 is gaseous, and the carbon 14 precipitates as a solid.

[0128] In this embodiment, the wall 28 of the reaction chamber 18 is simultaneously the outer wall of the housing 16. In other embodiments, the reaction chamber can also be arranged inside the housing, and several walls can be provided between the reaction chamber and the environment.

[0129] The gas outlet 24 serves to remove the molecular hydrogen 12 from the reaction chamber 18. The molecular hydrogen 12 is typically mixed with other gases, such as unconverted methane, since in the corona discharge 32 an incomplete conversion of the hydrogen-containing gas 10 into molecular hydrogen 12 can occur, and thus residual components of the hydrogen-containing gas 10 may be present and further gaseous byproducts may be formed.

[0130] The branch 26 serves to remove the solid by-product 14 from the reaction chamber 18.

[0131] In this embodiment, the reaction chamber 18 is divided into a main chamber 38 and a secondary chamber 40. The plasma electrode 22 is arranged relative to the main chamber 38 such that the corona discharge 32 ignites in the main chamber 38. The secondary chamber 40 is arranged below the main chamber 38 so that solid by-product 14 can fall into the secondary chamber 40. In this embodiment, the secondary chamber 40 contains a discharge device in the form of an eccentric 42, which removes the solid by-product 14 from the reaction chamber 18 without allowing gas to enter the reaction chamber 18 via the eccentric 42. In other embodiments, the discharge device may also include a rotary valve, a screw conveyor, or other discharge elements. The discharge device may also be arranged in the discharge channel, or discharge devices may be arranged in both the secondary chamber and the discharge channel.

[0132] The reaction chamber 18 is designed such that solid by-product from the main chamber 38 can fall into the secondary chamber 40, thereby reducing interference with the corona discharge 32 caused by the solid by-product 14. For this purpose, a distance of at least 40 mm is provided between the wall 28 of the reaction chamber 18 and the plasma electrode 22. This also reduces the risk of flashover. Furthermore, this design allows for a reduction in the temperature on the inner surface 30 of the wall 28. The temperature on the inner surface 30 of the wall 28 can, for example, reach up to 800°C.

[0133] The plasma lysis device 100 is dimensioned such that hydrogen-containing gas 10 can be introduced into the reaction chamber 18 at a flow rate between 1 l / min and 100 l / min. In this embodiment, hydrogen-containing gas 10 is introduced into the reaction chamber 18 at a flow rate between 1 l / min and 2 l / min. In other embodiments, the plasma lysis device can also be operated at a different flow rate.

[0134] The reaction chamber 18 also contains two cleaning elements 44 and 46 for removing the solid by-product 14. The solid by-product 14 can, for example, form solid carbon, carbon structures 48 that extend from the nozzle 36 of the plasma electrode 22 to the inside 30 of the wall 28 of the reaction chamber 18 (see Figure 1). Fig. 3) The carbon structures 48 can, for example, fork at point 50 some distance from the nozzle 36. This is possible, for example, if the plasma of the corona discharge 32 forms a side arm 52 that extends from the plasma electrode 22 towards the inside 30 of the wall 28 of the reaction chamber 18 (cf. Fig. 2) Furthermore, the plasma electrode 22 can be supplemented with a carbon layer 54 or a layer of other solid by-product 14.

[0135] The cleaning element 44 serves to clean the inner surface 30 of the wall 28. For this purpose, the cleaning element 44 is annular in shape, with an opening in its center having a larger inner diameter than the outer diameter of the plasma electrode 22. The cleaning element 44 is movable along a longitudinal axis 56 on the inner surface 30 of the wall 28, so that carbon deposited on the inner surface 30 of the wall 28 can be removed, and the carbon structures 48 can be broken up. In this embodiment, the cleaning element 44 has an edge 58 on its underside for better breaking up carbon structures 48 or other solid by-product 14 deposited on the inner surface 30 of the wall 28. The carbon or other solid by-product that is removed from the main chamber 38 falls into the secondary chamber 40 and can be discharged from there by means of the eccentric 42 and the outlet 26 from the plasma lysis device 100.

[0136] The cleaning element 46 is arranged on the plasma electrode 22 and serves to remove the carbon layer 54 from the plasma electrode 22. The cleaning element 46 has an edge 60 for removing solid by-product 14 and the carbon layer 54 near the nozzle opening 36 of the plasma electrode 22. The cleaning element 46 is also attached to the plasma electrode 22 by a sliding ring 62, so that the cleaning element 46 can be moved relative to the longitudinal axis of the plasma electrode 22 and thus remove the carbon layer 54.

[0137] In this embodiment, the plasma electrode 22 is also provided to rotate relative to the wall 28 about their common central longitudinal axis. For this purpose, sliding sealing rings 64 are provided at the upper and lower ends of the reaction chamber 18, respectively, at the upper end of the main chamber 38 and at the lower end of the secondary chamber 40, which allow the plasma electrode 22 to rotate relative to the wall 28. A drive for automatically rotating the plasma electrode 22 relative to the wall 28 is also provided (not shown). In this embodiment, the plasma electrode 22 is rotated. In other embodiments, the wall 28 can also be rotated around the plasma electrode 22 instead of, or in addition to, the rotation of the plasma electrode 22.

[0138] In this embodiment, the cleaning element 46 is rigidly connected to the wall 28, so that the plasma electrode 22 can rotate relative to it or be moved relative to the cleaning element 46. Alternatively, the cleaning element 46 can be rotatable about the plasma electrode and the plasma electrode 22 fixed (not shown).

[0139] In this embodiment, the plasma electrode has an outer diameter of 8 mm and the nozzle opening has a diameter of 0.4 mm. In other embodiments, the outer diameter of the plasma electrode can also be, for example, between 4 mm and 16 mm, and the nozzle opening of the plasma electrode can have a diameter between 0.1 mm and 1 mm. In this embodiment, the plasma electrode has a length of 150 mm. In other embodiments, the plasma electrode can also have a different length, for example, between 50 mm and 300 mm.

[0140] The reaction chamber 18 is pressure-resistant for pressures up to 1 bar overpressure.

[0141] Fig. Figure 4 shows an embodiment of a plasma lysis system 400 for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product. The plasma lysis system 400 has two plasma lysis devices 100 arranged in series, as shown in Fig. Figure 1 shows the plasma lysis system. In other embodiments, the plasma lysis system can also contain a different number of plasma lysis devices. The plasma lysis devices can also be arranged parallel to one another. The gas outlets of the parallel plasma lysis devices can, for example, lead into a common reservoir or a common gas outlet.

[0142] The plasma lysis system 400 includes a high-frequency generator 200, a gas tank 300, and two reservoirs 600 and 700. In other embodiments, several high-frequency generators may be provided, for example, a separate high-frequency generator for each plasma lysis device.

[0143] A hydrogen-containing gas is supplied in gas tank 300. In this embodiment, natural gas is used as the hydrogen-containing gas. This is fed via the gas supply line into a first plasma lysis device 100, which splits the natural gas into molecular hydrogen and other gaseous and solid byproducts, in particular carbon, as required for Fig. As described in Figure 1, the solid carbon is discharged via the outlet 26 into the reservoir 700 and can be removed from there via an eccentric 42. The molecular hydrogen and the other gaseous byproducts are directed via the gas outlet 24 into the gas supply line 20 of the subsequent plasma lysis device 100. There, the gaseous byproduct is further split into more molecular hydrogen, more gaseous byproduct, and solid byproduct, in particular carbon. The solid byproduct is discharged via the outlet 26' into the reservoir 700. In this case, the outlet 26' is inclined so that solid byproduct from the plasma lysis device 100 can slide down into the reservoir 700.

[0144] The molecular hydrogen and the other gaseous byproduct are discharged into reservoir 600 via gas outlet 24'.

[0145] Reservoir 600 contains a membrane 602 and a selective adsorber 604. Two additional gas outlets 606 and 608 lead out of the reservoir, designed to discharge separate gases from reservoir 600. The reservoir can also be part of a plasma lysis device (not shown). Membranes and selective adsorbers can also be arranged in a gas outlet of a plasma lysis device (not shown).

[0146] In reservoir 600, gaseous byproducts, for example, unconverted methane, are separated from the molecular hydrogen in the gas mixture of molecular hydrogen and gaseous byproducts. In this embodiment, this is achieved via a two-stage process using membrane 602 and selective adsorber 604. Methane cannot pass through membrane 602 and is discharged via gas outlet 606. Further gaseous byproducts are adsorbed by selective adsorber 604, so that essentially only molecular hydrogen is discharged via gas outlet 608. In this embodiment, a polymer membrane is used. ZSM-5, for example, is used as the adsorber. In other embodiments, multiple membranes and / or multiple adsorbers can be used. Other membranes and / or adsorbers can also be used.

[0147] Fig. Figure 5 shows a schematic representation of a flow diagram of an embodiment of a method 500 for corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product according to a further aspect of the invention.

[0148] In step 502, hydrogen-containing gas is introduced into a gas-tight reaction chamber with a non-grounded, non-metallic wall. In other embodiments, a different type of wall may be provided that electrically insulates the plasma electrode from the outside of the reaction chamber wall. In this embodiment, the hydrogen-containing gas is introduced into the reaction chamber through an opening in a plasma electrode. In particular, the plasma electrode has a nozzle through which the hydrogen-containing gas is injected into the reaction chamber.

[0149] In step 504, a corona discharge is generated in the reaction chamber using the plasma electrode. The plasma electrode is supplied with a high-frequency alternating voltage from a high-frequency generator. Exactly one plasma electrode is used, and an inner surface of the reaction chamber wall spontaneously forms a counter electrode during operation, without any electrical current being conducted away; that is, the wall is not grounded.

[0150] In step 506, molecular hydrogen and at least one byproduct are removed from the reaction chamber. In this embodiment, natural gas is used as the hydrogen-containing gas, which mainly contains methane and also, among other things, hydrogen sulfide. In other embodiments, a different hydrogen-containing gas can be used, for example, a hydrogen-containing substance that is liquid at room temperature and has been converted into the gaseous state. Methane is split into molecular hydrogen and powdered carbon as a solid byproduct. The solid byproduct can also contain, for example, elemental carbon, carbon nanotubes, fullerenes, carbon nanocones, or other carbon structures. The molecular hydrogen is gaseous and is removed via a gas outlet. The carbon is removed via a separate outlet.In this embodiment, the carbon falls downwards from the corona discharge point and is then discharged via the exhaust. Alternatively or additionally, carbon particles can also be discharged via the gas exhaust and filtered from the gas stream exiting the reaction chamber in a particle filter.

[0151] In step 508, the reaction chamber is cleaned to remove solid byproducts. Step 508 is optional. During operation, carbon can form carbon structures that extend from the plasma electrode to the inside of the reaction chamber wall. Carbon can also be deposited on the inside of the reaction chamber wall. To address this, the solid byproducts can be removed mechanically using one or more cleaning elements. Alternatively, the flow rate of the supplied hydrogen-containing gas can be increased to break up carbon structures or prevent their formation, thus cleaning the reaction chamber. Furthermore, pulsed gas bursts can be released from the plasma electrode opening to break up carbon structures, particularly tree structures or graphite sticks that form on the plasma electrode.Furthermore, the composition of the hydrogen-containing gas can be adjusted to clean the reaction chamber, or another gas, such as an inert gas, can be used for cleaning.

[0152] The gas discharged from the reaction chamber may contain other gaseous byproducts besides molecular hydrogen. For example, it may contain residual gas from the hydrogen-containing gas originally introduced into the reaction chamber, such as unconverted methane. Solid byproducts, such as carbon, may also be present in the discharged gas.

[0153] In step 510, the gas discharged from the reaction chamber is collected in a reservoir. Alternatively, the gas can also be collected in the gas outlet. Step 510 is optional. Alternatively, the discharged gas can also flow through the reservoir and / or the gas outlet at a substantially unchanged flow rate.

[0154] In step 512, the discharged gas is separated into different gases; in particular, the molecular hydrogen is separated from other gaseous byproducts. Step 512 is optional. In this embodiment, a multi-stage membrane process and a selective adsorption process are used to separate the molecular hydrogen from the other gaseous byproducts. In other embodiments, only a membrane process and / or only a selective adsorption process may be used. In this embodiment, step 512 is carried out in the reservoir. For this purpose, several membranes arranged in series and an adsorber are located in the reservoir. In other embodiments, the separation of the different gases from each other can also be carried out in the gas discharge.If there is still solid by-product, for example carbon, in the exhausted gas, it can be filtered out of the gas, for example by means of a particle filter.

[0155] Fig. Figure 6 shows a schematic representation of a further embodiment of a plasma lysis device 100' for corona discharge-induced splitting of hydrogen-containing gases 10 into molecular hydrogen 12 and at least one by-product. In this embodiment, methane is used as the hydrogen-containing gas 10. The resulting by-products are essentially graphite rods 14' and carbon particles.

[0156] The plasma lysis device 100' is similar to the one in Fig. The plasma lysis device 100 shown in Figure 1 is constructed and has a similar operating principle. The plasma lysis device 100' has a housing 16 that gas-tightly encloses a funnel-shaped reaction chamber 18'. Furthermore, the plasma lysis device 100' has a gas inlet 20, exactly one plasma electrode 22', and a gas outlet 24. A particle filter 21 is arranged in the gas inlet 20 to filter particles from the hydrogen-containing gas 10. A particle filter in the form of a carbon particle filter tube 25 is arranged in the gas outlet 24 to filter carbon particles from the gas discharged from the reaction chamber 18'.

[0157] A key difference is that in operation, the plasma lysis device 100' differs from the one in Fig. 1 plasma lysis device 100 shown instead of solid by-product in the form of tree structures (cf. Fig. 3) Brittle graphite rods 14' form at the tip of the plasma electrode 22', and smaller amounts of carbon particles accumulate in the reaction chamber 18'. The graphite rods 14' form due to a higher gas flow rate and the resulting stronger gas current from an opening 34 of the plasma electrode 22'. The stronger the gas current, the fewer branches of a tree-like structure can form, so that with a sufficiently strong gas current, no branches are formed at all, and only a trunk or rod, namely a graphite rod 14', is formed. In this embodiment, no branches form above a gas flow rate of more than 2 liters per minute (>2 l / min), in which case the gas current is conical. Furthermore, the stronger gas current also makes it easier to carry carbon particles out of the reaction chamber 18' into the gas outlet 24. The graphite rods 14' break off after a certain time.are broken off and fall to the floor of reaction chamber 18'.

[0158] In contrast to the in Fig. In the plasma lysis device 100 shown in Figure 1, a portion of the solid byproduct, namely the carbon particles, is also discharged via the gas outlet 24. These particles can be carried into the gas outlet 24 by the gas stream generated from the opening 34 of the plasma electrode 22' during a corona discharge 32. There, the carbon particles are filtered in the carbon particle filter tube 25 and thus separated from the gas discharged from the reaction chamber 18'.

[0159] Furthermore, in a cleaning mode, the graphite rod 14' can be knocked over and carbon particles deposited in the reaction chamber 18' can be blown out. For this purpose, pulsed gas bursts are emitted from the opening 34 of the plasma electrode 22'. The plasma electrode 22' contains a conical nozzle 36' for this purpose, which is connected to the gas supply line 20 via the opening 34 and the particle filter 21. This makes it possible to easily remove solid byproducts, especially carbon particles, that form in the reaction chamber 18'.

[0160] In this embodiment, a control unit 140 is provided to control the generation of the pulsating gas pulses. The control unit 140 detects a power input to the plasma lysis device 100' and interrupts the supply of high-frequency alternating voltage to the plasma electrode 22', triggering a pulsating gas pulse via the gas supply line 20 when the power input falls below a threshold value. The threshold value is selected to ensure that the opening 34 of the plasma electrode 22' does not become excessively clogged with solid by-product. The control unit 140 can be connected to a gas supply in the gas supply line 20 to briefly increase the gas supply. For example, a valve controllable by the control unit can be arranged in the gas supply line to generate the pulsating gas pulse.In other embodiments, shock-like gas pulses can also be generated on the basis of other events or time-dependently, for example at regular time intervals, in order to remove solid by-product from the reaction chamber 18' and in particular to free the opening 34 of the plasma electrode 22' from solid by-product.

[0161] While the carbon particles can be blown out into the gas outlet 24 with the gas stream, the graphite rod 14' can fall from the plasma electrode 22' to the bottom of the reaction chamber 18'. The gas used in the pulsed gas bursts can be the hydrogen-containing gas 10 or another gas, for example, an inert gas.

[0162] The carbon particles are fed with the gas stream into the gas outlet 24, where they are filtered by the carbon particle filter tube 25. The remaining gas is fed into a reservoir 110. A membrane 102 and a selective adsorber 104 are arranged in the reservoir 110. Additionally, a outlet 106 and another gas outlet 108 lead out of the reservoir 110, designed to remove separated molecular hydrogen and byproducts. Alternatively, membranes and selective adsorbers can also be arranged in the gas outlet of the plasma lysis device (not shown). Other methods can also be used to separate the molecular hydrogen from the solid byproduct particles. For example, only a particle filter or only a membrane can be used.

[0163] In reservoir 110, solid byproducts not filtered out by the carbon particle filter tube 25 and gaseous byproducts, for example, unconverted methane, are separated from the molecular hydrogen in the gas mixture of molecular hydrogen and byproducts. In this embodiment, this is achieved via a two-stage process using membrane 102 and the selective adsorber 104. The solid byproducts and methane cannot pass through membrane 102 and are discharged via the outlet 106. If solid byproducts are absorbed by membrane 102, the membrane 102 can be replaced or cleaned. In this embodiment, membrane 102 is self-cleaning. For this purpose, membrane 102 is connected to a gas collection system (not shown). The gas collection system collects gas and thus builds up pressure, which is released as a gas pulse when a pressure threshold is exceeded. The gas pulse cleans membrane 102.Further gaseous byproducts are adsorbed by the selective adsorber 104, so that essentially only molecular hydrogen is discharged via the gas outlet 108. In other embodiments, it may also be possible to produce a synthetic gas. For this purpose, for example, the methane from the gas outlet 106 can be combined with the molecular hydrogen 12 from the gas outlet 108 in a predefined gas mixture ratio. Alternatively, the membrane and / or the adsorber can also be selected such that a gas mixture of molecular hydrogen and another gaseous byproduct or the methane is produced.

[0164] In this embodiment, a polymer membrane is used. ZSM-5, for example, is used as the adsorber. In other embodiments, multiple membranes and / or multiple adsorbers can be used. Other membranes and / or adsorbers can also be used.

[0165] Furthermore, reaction chamber 18' has a different shape than reaction chamber 18 in Fig. The plasma lysis device shown in Figure 1 has a funnel-shaped form. This increases the cross-section of the reaction chamber 18' in the direction from the gas inlet 20 to the gas outlet 24. This can prevent or at least reduce the adhesion of the carbon particles that are carried away from the reaction chamber 18' with the gas stream.

[0166] In this embodiment, the plasma electrode 22' is screwed into the housing 16 from below and can be removed if necessary, for example, to remove graphite pins 14'. During operation of the plasma lysis device 100', the graphite pins 14' can form at the tip of the plasma electrode 22' near the corona discharge 32. The graphite pin 14' is conductive and can temporarily form part of the plasma electrode 22'. The graphite pin 14' is brittle and therefore typically breaks off after a certain period of operation and falls towards the bottom of the funnel-shaped reaction chamber 18'.

[0167] The plasma electrode 22' is connected to a high-frequency generator 200'. In this embodiment, the high-frequency generator 200' includes an impedance matching network consisting of two coils 202, 204 and a capacitor 206. In this embodiment, the high-frequency generator 200' provides a power output between 30 W and 5000 W and has an output impedance of 50 ohms. The high-frequency generator 200' provides the high-frequency alternating voltage with a frequency in the range of 1 MHz to 40 MHz, particularly in the range of 10 MHz to 20 MHz, for example, with a frequency of 13.56 MHz.

[0168] In this embodiment, the reaction chamber 18 has a non-grounded, non-metallic wall 28. In other embodiments, the reaction chamber can also be enclosed by a different type of wall, which is designed to electrically insulate the plasma electrode from an outer surface of the wall. In this embodiment, the wall 28 is made of quartz glass with a wall thickness of 4 mm. In other embodiments, the wall can also be made of a different material, for example, a ceramic. The wall can also have a different thickness.

[0169] Additionally, a DC voltage generator 130 is connected to the wall 28 of the reaction chamber 18', which applies a DC voltage to it. Specifically, the DC voltage is applied to an inner surface of the wall 28. In this embodiment, the DC voltage is 10 kV at 10 mA. In other embodiments, the plasma lysis device can also be configured to apply a different DC voltage to the wall of the reaction chamber, for example, between 5 kV and 20 kV with 0.01 mA to 200 mA.

[0170] Furthermore, the plasma lysis device 100' includes a transverse nozzle 120 arranged in the wall 28 of the reaction chamber 18' for cleaning the plasma electrode 22', for blowing over the graphite rod 14', and for reducing turbulence. The transverse nozzle 120 is positioned slightly above the tip of the plasma electrode 22'. In other embodiments, the transverse nozzle can also be located elsewhere, for example, protruding from the bottom and in a different orientation relative to the plasma electrode, particularly for cleaning the plasma electrode. The transverse nozzle 120 is connected to a transverse gas supply line 122, which can introduce, for example, an inert gas or additional hydrogen-containing gas into the reaction chamber 18' to clean the plasma electrode 22' with a pulsed gas and, if necessary, to knock over the graphite rod 14' so that it falls to the bottom of the reaction chamber 18'. The transverse nozzle 120 and transverse gas supply line 122 are optional.The gas supply to the transverse nozzle 120 can be controlled by the control unit 140. Alternatively or additionally, the gas supply to the transverse nozzle can also be time-controlled and, for example, introduce a gas pulse into the reaction chamber every 5 minutes.

[0171] Furthermore, the plasma lysis device 100' includes a cleaning element 150 with a pivotable axis 152 and a rod 154. The rod 154 is attached at one end to the pivotable axis 152 and has a brush 156 at the other end, pointing towards the floor. The rod 154 can be, for example, 40 mm or longer. The pivotable axis 152 is located near the wall 28 of the reaction chamber 18' and is driven by an electric motor to pivot the axis 152 and thus the rod 154. The rod 154 can be pivoted so that the brush 156 can be moved over the tip of the plasma electrode 22' to clean it and, if necessary, to help break off graphite pins 14'. In other words, the cleaning element 150 functions similarly to a windshield wiper, wiping over the tip of the plasma electrode 22'.When the brush 154 passes over the tip of the plasma electrode 22', the corona discharge 32 is extinguished for a brief moment. The cleaning element 150 can be controlled by the control unit 140.

[0172] In this embodiment, the reaction chamber 18' is divided into a main chamber 38' and a secondary chamber 40'. In contrast to the one described in Fig. In the plasma lysis device 100 shown in Figure 1, the secondary chamber 40' is arranged above the main chamber 38'. The corona discharge 32 takes place in the main chamber 38', and the molecular hydrogen 12, as well as carbon particles, are discharged in the gas stream via the secondary chamber 40', namely into the gas outlet 24.

[0173] In other embodiments, the gas outlet may have no particle filter, a different type of particle filter, or an additional particle filter to capture the carbon particles. The particle filter could, for example, be a pressure-controlled particle filter. Alternatively or additionally, a controllable flap could be provided. The flap could be located at a junction of the gas outlet to separate gas with a particularly high carbon particle load from the reaction chamber from the molecular hydrogen produced during normal operation when a pulsed gas is released during cleaning mode.

[0174] Other features related to Fig. The plasma lysis device 100 shown in section 1 is not explicitly described again for the plasma lysis device 100', but may optionally be present, such as further cleaning elements.

[0175] Fig.Figure 7 shows a further embodiment of a plasma lysis system 400' for splitting hydrogen-containing gas into molecular hydrogen and at least one byproduct. In this embodiment, the plasma lysis system 400' is connected to a heat supply device in the form of a heater 720 and an energy supply in the form of a fuel cell 730 of a building, in particular a hotel 740. Alternatively, these can also be part of the plasma lysis system 400'. Instead of a hotel, another building or another stationary or mobile structure can also be connected to the plasma lysis system. Instead of a separate heat supply device and energy supply, these elements can, for example, also be combined in a combined heat and power plant (CHP).

[0176] The plasma lysis system 400' contains a storage unit with hydrogen-containing gas in the form of a biogas reactor 702, an energy plant 704 and a plasma lysis unit 710.

[0177] The biogas reactor 702 is additionally connected to a wastewater treatment plant (not shown) and produces a hydrogen-containing gas in the form of biogas from wastewater and waste. This gas consists primarily of methane.

[0178] The energy plant 704 comprises a solar energy plant 706 and a wind energy plant 708. The energy plant 704 serves to provide energy for the corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one by-product. In other embodiments, the energy plant may also include other energy-generating plants, for example, additionally or alternatively, a hydroelectric power plant.

[0179] The plasma lysis unit 710 contains two plasma lysis devices 100' and one high frequency generator 200'.

[0180] The plasma lysis unit 710 is connected to the biogas reactor 702 via the gas supply line 20 and to the energy plant 704 via the power line 705.

[0181] This enables the emission-free generation of heat and molecular hydrogen using green electricity from the energy plant 704 and biogas from the biogas reactor 702. This hydrogen can then be used in the heating system 720 and the fuel cell 730 of the hotel 740. The hotel 740 can thus operate the lighting 742, radiators 744, and hot water system for the shower 746 without producing harmful carbon dioxide 750. Instead, only solid byproducts, such as elemental carbon, and clean water are produced, which can be returned to the water cycle, for example, in the form of clouds 760.

[0182] Alternatively, the generated molecular hydrogen can be stored, for example, in a hydrogen storage system for later use. For instance, the hotel could provide a hydrogen refueling station for vehicles. Other energy systems that can operate on molecular hydrogen could also be supplied with it.

[0183] In one embodiment, the hotel could be part of a cruise ship. The cruise ship could have its own wastewater treatment plant and power plant, providing hydrogen-containing gas and energy to operate the plasma lysis devices. In other embodiments, plasma lysis devices could also be used in other vehicles, such as passenger cars, trucks, railway locomotives, or aircraft, for example, liquefied natural gas (LNG) aircraft or aircraft powered by synthetic gas. In aircraft, for example, kerosene, JP-8, or another conventional fuel could be converted into carbon and LNG or synthetic gas, and this could be used to power the aircraft. This could reduce carbon dioxide emissions from transportation without requiring extensive replacement of the existing infrastructure.

[0184] In summary, the invention relates to the corona discharge-induced splitting of hydrogen-containing gases into molecular hydrogen and at least one byproduct. For this purpose, hydrogen-containing gas is introduced via a gas supply line into a gas-tight reaction chamber containing exactly one plasma electrode. The gas-tight reaction chamber is enclosed by a wall designed to electrically insulate the plasma electrode from its outer surface. The plasma electrode is connected to a high-frequency generator that provides high-frequency alternating voltage and generates corona discharges in the reaction chamber by means of this high-frequency alternating voltage. This splits the hydrogen-containing gas into molecular hydrogen and at least one byproduct. The molecular hydrogen is removed from the reaction chamber via a gas outlet.The hydrogen-containing gas may contain, for example, methane, biogas, natural gas, hydrogen sulfide, or cyclohexane, heptane, toluene, gasoline, JP-8, or diesel converted into the gaseous state.

Claims

[1] Plasma lysis device (100; 100') for corona discharge-induced splitting of hydrogen-containing gases (10) into molecular hydrogen (12) and at least one by-product (14; 14'), comprising: - a gas-tight reaction chamber (18; 18'), - a gas supply line (20) for the hydrogen-containing gas (10) into the reaction chamber (18; 18'), - exactly one plasma electrode (22; 22') for generating corona discharges (32) in the reaction chamber (18; 18') by means of a high-frequency alternating voltage and - a gas outlet (24) for the molecular hydrogen (12) from the reaction chamber (18; 18'), wherein the gas-tight reaction chamber (18; 18') is enclosed by a wall (28) which is configured to electrically insulate the plasma electrode (22; 22') from an outside of the wall (28), and wherein the plasma electrode (22; 22') is connected to a high-frequency generator (200) to generate the high-frequency alternating voltage. [2] Plasma lysis device (100; 100') according to claim 1, wherein the plasma electrode (22; 22') has an opening (34) which is connected to the gas supply line (20) and wherein the plasma electrode (22; 22') is arranged such that the hydrogen-containing gas (10) is introduced through the opening (34) of the plasma electrode (22; 22') into the reaction chamber (18; 18'). [3] Plasma lysis device (100; 100') according to claim 2, wherein the opening (34) of the plasma electrode (22; 22') is designed as a nozzle (36; 36') for introducing the hydrogen-containing gas (10) into the reaction chamber (18; 18'). [4] Plasma lysis device (100; 100') according to claim 2 or 3, wherein the plasma lysis device (100; 100') is configured to emit pulsed gas pulses from the opening (34) of the plasma electrode (22; 22') in order to remove solid by-product (14; 14') forming in the reaction chamber (18; 18') from the reaction chamber (18; 18'). [5] Plasma lysis device (100') according to one of claims 1 to 4, wherein a cross-section of the reaction chamber (18') increases in the direction from the gas supply line (20) to the gas discharge (24). [6] Plasma lysis device (100; 100') according to one of claims 1 to 5, in which a DC voltage is applied to the wall (28) of the reaction chamber (18). [7] Plasma lysis device (100) according to any one of claims 1 to 6, wherein the plasma lysis device (100) has a drain (26) for at least one solid by-product (14) from the reaction chamber (18). [8] Plasma lysis device (100; 100') according to any one of claims 1 to 7, wherein the distance between the wall (28) of the reaction chamber (18; 18') and the plasma electrode (22; 22') is at least 40 mm. [9] Plasma lysis device (100; 100') according to any one of claims 1 to 8, wherein the reaction chamber (18; 18') has a cleaning element (44, 46; 120, 150) for removing solid by-product (14; 14'). [10] Plasma lysis system (400; 400') for corona discharge-induced splitting of hydrogen-containing gases (10) into molecular hydrogen (12) and at least one by-product (14; 14'), comprising at least two plasma lysis devices (100; 100') according to any one of claims 1 to 9, wherein the plasma lysis devices (100; 100') are arranged in parallel or in series with each other. [11] Plasma lysis system (400; 400') according to claim 10, wherein - a storage device containing a substance from which hydrogen-containing gas (10) can be produced, and / or - a storage unit (702) containing hydrogen-containing gas (10), and / or - an energy plant (704) for providing energy for corona discharge-induced splitting of hydrogen-containing gases (10) into molecular hydrogen (12) and at least one by-product (14), and / or - a hydrogen storage device for storing molecular hydrogen (12), and / or - a propulsion system powered by molecular hydrogen (12), and / or - has an energy plant that can be operated with molecular hydrogen (12). [12] Use of a plasma lysis device (100; 100') according to any one of claims 1 to 9 for splitting hydrogen-containing gas (10) into molecular hydrogen (12) and at least one by-product (14; 14') using hydrogen-containing gas (10) provided in an operation of a stationary structure (702) or a mobile structure. [13] Process (500) for corona discharge-induced splitting of hydrogen-containing gases (10) into molecular hydrogen (12) and at least one by-product (14; 14'), comprising the process steps, - Introducing (502) a hydrogen-containing gas (10) into a gas-tight reaction chamber (18; 18'), - Generating (504) a corona discharge (32) by means of exactly one plasma electrode (22; 22') operated with a high-frequency alternating voltage in the reaction chamber (18; 18'), wherein the gas-tight reaction chamber (18; 18') is enclosed by a wall (28) which is designed to electrically insulate the plasma electrode (22; 22') from an outside of the wall (28) and - Removal (506) of the molecular hydrogen (12) and of at least one by-product (14; 14') from the reaction space (18; 18'). [14] Method according to claim 13, wherein the hydrogen-containing gas (10) is introduced through an opening (34) of the plasma electrode (22; 22') into the reaction chamber (18; 18'). [15] Method according to claim 13 or 14, wherein the hydrogen-containing gas (10) contains natural gas, biogas, methane, hydrogen sulfide, and / or cyclohexane, heptane, toluene, gasoline, JP-8 and / or diesel converted into the gaseous state.

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