WO2024079322A1 - Ensemble d'électrodes à plasma et dispositif d'analyse de plasma - Google Patents

Ensemble d'électrodes à plasma et dispositif d'analyse de plasma Download PDF

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Publication number
WO2024079322A1
WO2024079322A1 PCT/EP2023/078500 EP2023078500W WO2024079322A1 WO 2024079322 A1 WO2024079322 A1 WO 2024079322A1 EP 2023078500 W EP2023078500 W EP 2023078500W WO 2024079322 A1 WO2024079322 A1 WO 2024079322A1
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Prior art keywords
electrode
plasma
gas
ignition
arrangement
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PCT/EP2023/078500
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German (de)
English (en)
Inventor
Jens Hanke
Sascha Knist
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Graforce Gmbh
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Priority claimed from DE102022126660.5A external-priority patent/DE102022126660A1/de
Application filed by Graforce Gmbh filed Critical Graforce Gmbh
Publication of WO2024079322A1 publication Critical patent/WO2024079322A1/fr

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    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00—Generating plasma; Handling plasma
    • H05H1/24—Generating plasma
    • H05H1/48—Generating plasma using an arc
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00—Generating plasma; Handling plasma
    • H05H1/24—Generating plasma
    • H05H1/26—Plasma torches
    • H05H1/32—Plasma torches using an arc
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0809—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes employing two or more electrodes
    • B01J2219/0811—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes employing two or more electrodes employing three electrodes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0824—Details relating to the shape of the electrodes
    • B01J2219/0826—Details relating to the shape of the electrodes essentially linear
    • B01J2219/083—Details relating to the shape of the electrodes essentially linear cylindrical
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0837—Details relating to the material of the electrodes
    • B01J2219/0839—Carbon
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0869—Feeding or evacuating the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0873—Materials to be treated
    • B01J2219/0875—Gas
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0405—Purification by membrane separation
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/042—Purification by adsorption on solids
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/062—Hydrocarbon production, e.g. Fischer-Tropsch process
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/066—Integration with other chemical processes with fuel cells
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/068—Ammonia synthesis
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0861—Methods of heating the process for making hydrogen or synthesis gas by plasma
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
    • C01B2203/84—Energy production
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H2245/00—Applications of plasma devices
    • H05H2245/10—Treatment of gases

Definitions

  • the invention relates to a plasma electrode arrangement and a plasma lysis device with such a plasma electrode arrangement.
  • Kvaerner uses a hollow inner electrode arranged within an outer electrode to generate the plasma, as shown for example in WO 93/20152.
  • the invention relates to a plasma electrode arrangement comprising a cylindrical hollow outer electrode, an annular ignition electrode which is electrically insulated from the outer electrode and arranged at a distance therefrom, and an inner electrode arranged at a distance therefrom within the outer electrode and the ignition electrode, wherein the ignition electrode can be connected to a high-voltage source.
  • the invention includes the finding that the use of a separate ignition electrode allows the distance between the inner and outer electrodes to be increased and thus allows a higher performance of a plasma lysis device equipped with the plasma electrode arrangement.
  • the invention is based on the finding that the use of an ignition electrode also allows the use of different plasma gases.
  • an arc is built up between the ignition electrode and the inner electrode during ignition, which extends into a plasma gap between the inner and outer electrodes and initiates the formation of a plasma between the inner and outer electrodes.
  • the inner electrode forms a counter electrode to the outer electrode and the ignition electrode.
  • Nitrogen and/or hydrogen are preferred as plasma gases.
  • gases such as ammonia or noble gases or gas mixtures is also possible.
  • the ignition electrode is flattened on a side facing the outer electrode. This structure facilitates the extension and movement of the arc into a plasma gap between the inner and outer electrodes.
  • the thickness of the ignition electrode decreases from a side facing away from the outer electrode to a side facing the outer electrode.
  • This structure also promotes an extension of the arc into a plasma gap between the inner and outer electrodes.
  • the ignition electrode is essentially designed as a hollow truncated cone. This ensures both the decreasing thickness of the ignition electrode in a geometry that is easy to produce and the accommodation of the inner electrode in the cavity of the ignition electrode.
  • the ignition electrode has a fastening area with which it is mechanically connected to the outer electrode via insulating spacers. This enables simple assembly of the plasma electrode arrangement, with the insulating spacers ensuring both insulation and maintaining a distance between the ignition and outer electrodes.
  • an ignition gap between the ignition electrode and the inner electrode has a width in the range of 4 to 20 mm.
  • a plasma gap between the outer and inner electrodes preferably has a width of more than 20 mm. With such a large distance, a higher voltage is possible when maintaining the plasma and thus a higher yield.
  • the outer electrode and/or the ignition electrode and/or the inner electrode comprise graphite or consist of graphite.
  • Graphite is particularly suitable as an electrode material because it has good conductivity values and is easy to form.
  • graphite electrodes are used in the processes underlying this, contamination of the carbon produced is avoided even when the electrodes wear out.
  • the plasma electrode arrangement further comprises a gas guide device arranged on a side of the ignition electrode facing away from the outer electrode and spaced therefrom, wherein the gas guide device comprises channels and/or grooves for guiding gas and the channels and/or grooves are arranged in particular concentrically.
  • a flow of the incoming plasma gas directed with the aid of the gas guide device in addition to the annular ignition electrode promotes an extension of the ignition arc into a plasma gap between the inner and outer electrodes and offers support in the formation of the plasma in the form of an arc or a torch.
  • the gas guiding device comprises at least one gas guiding ring with channels and/or grooves, which is arranged in a housing, preferably a ceramic tube.
  • the inner electrode is preferably hollow. This means that both plasma gas and, in certain applications, a starting material gas to be processed can be fed through the inner electrode.
  • the plasma electrode arrangement preferably comprises an electrode changing system comprising a plurality of inner electrodes in a drum arrangement of a turret system, wherein the electrode changing system is designed to lower exactly one inner electrode into an interior of the outer electrode and, after a predetermined time or in response to a control signal, to raise the lowered inner electrode, to rotate the drum by at least one position and to lower another inner electrode into the interior.
  • the inner electrodes which regularly wear out during the process, can be easily replaced.
  • Such an electrode changing system can also be used in plasma electrode arrangements without an ignition electrode.
  • the plasma electrode arrangement comprises a bayonet connection for connection to a bayonet base in an opening of a reaction chamber, wherein the outer electrode and ignition electrode are mechanically connected to the bayonet connection.
  • the invention relates to a plasma lysis device for splitting a starting material into at least one product gas and at least one by-product, comprising a plasma electrode arrangement according to the first aspect of the invention at least partially arranged in a reaction chamber and at least one starting material feed in the reaction chamber and a direct current source connected to the external electrode.
  • a plasma lysis device can also be referred to as an electrolysis or plasma electrolysis device.
  • the starting material can be gaseous, solid or liquid. It can also be a mixture of different starting materials.
  • the starting material preferably comprises at least one hydrocarbon and is preferably split into at least molecular hydrogen and solid carbon.
  • the solid or liquid starting material can also Contain oxygen compounds, which then also promote the formation of carbon monoxide or carbon dioxide, if desired.
  • the starting material can contain methane, for example.
  • the starting material can contain over 75% methane, preferably over 90% methane, for example between 90% and 99% methane.
  • the methane is split in the plasma 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 Ck with 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
  • hydrocarbon-containing starting materials are naphtha, flare gas, landfill gas and pure hydrocarbons such as pure propane.
  • the starting material can be, for example, natural gas.
  • Natural gas can, for example, contain the following substances: between 30% and 99% methane, e.g. between 75% and 99% methane, in particular between 90% and 99% methane, between 0% and 15% ethane, e.g. between 1% and 15% ethane, in particular between 1% and 3% ethane, between 0% and 10% propane, e.g.
  • Natural gas can also contain traces of oxygen, e.g. between 0.001% and 0.01% oxygen. Natural gas can also contain noble gases such as helium, argon, neon, krypton or xenon, for example with a respective proportion between 0% and 15%.
  • noble gases such as helium, argon, neon, krypton or xenon
  • biogas Another preferred starting material is biogas. This can be used in particular to produce syngas. For example, with a biogas composition of 50% CH4 and 50% CO2, a feed of 1:14 H2 and CO can be produced.
  • waste from which hydrogen and usable by-products can be obtained cost-effectively and, in addition, the load of waste to be landfilled can be significantly reduced or even eliminated entirely.
  • waste from which hydrogen and usable by-products can be obtained cost-effectively and, in addition, the load of waste to be landfilled can be significantly reduced or even eliminated entirely.
  • sewage sludge biomass such as food scraps, manure, household waste, pharmaceutical waste, car tires, plastic waste, packaging waste, industrial waste
  • RESH bustible, shredded waste from the automotive industry RESH consists of the following material groups, although the exact composition can vary: plastics 62% (including 29% elastomers), car glass, sand 16%, paint dust, rust etc.
  • waste products comprising glass fiber reinforced carbons such as glass fiber cables or rotor blades, for example from wind turbines
  • Municipal or industrial waste water wood gas condensate water, grease water, cellulose water, vapour water, centrate water, press water, process water from sewage sludge treatment, landfill leachate, wash water, for example from flue gas cleaning, oily water, mining waste water, waste water from oil production (for example from fracking, from drilling platforms), ammonia water, liquid manure (for example pig, cattle or poultry manure), liquid fermentation residues or products obtained from these.
  • Process water can be used as a starting material.
  • renewable raw materials such as biomass from plants or parts of plants can also be used as starting materials, or hydrogen-containing liquids such as cyclohexane, heptane, toluene, petrol, JP-8 or diesel.
  • Particularly preferred starting materials are those which, as hydrogen-containing solids and/or liquids, comprise those which contain hydrocarbon compounds.
  • Solid carbon (C(s)) is then formed during plasmalysis, where C(s) can contain various solid carbon structures, e.g. one or more carbon structures.
  • Carbon structures can be, for example, elementary carbon particles, carbon nanotubes, fullerenes, carbon nanocones or other carbon structures.
  • the elementary carbon particles can, for example, have a size between 50
  • Carbon layers can also form. This enables efficient production of molecular hydrogen and elemental carbon from the starting materials. In particular, this creates a cost- and energy-efficient way of producing high-quality hydrogen and elemental carbon from waste products.
  • the plasma lysis device preferably comprises a separate high-voltage source connected to the ignition electrode.
  • the high-voltage source can be either a high-frequency or a low-frequency voltage source.
  • the high-voltage source is preferably a generator that is connected to the ignition electrode via a matching network. This enables long arcs and stabilizes the direct current plasma arc when the plasma lysis device is started until the outer electrode and the atmosphere surrounding it are hot (e.g. 3 s).
  • a transformer is used as a low-frequency source together with the generator. To set a suitable arc length, a transformer with at least 6 kV is preferably used.
  • the ignition electrode is connected to the high-voltage source via a contacting device, for example a wire or graphite rod.
  • the plasma lysis device comprises a plasma gas supply line for plasma gas connected to the gas guide device.
  • the plasma lysis device further comprises a magnetic coil which is arranged outside the reaction chamber and is designed to generate a magnetic field in which at least one end of the outer electrode facing away from the ignition electrode is arranged.
  • the spread of the plasma can be influenced via such a magnetic field and in particular a flashover of the plasma onto a wall of the reaction chamber can be prevented.
  • a feedstock feed is preferably arranged in the reaction chamber below the plasma electrode arrangement. This enables uniform treatment of the feedstock. Furthermore, in the case of gaseous feedstocks, the feedstock feed below the plasma electrode enables special gas guides to ensure a residence time of the gaseous feedstock, simultaneous cooling of the reactor inner wall and also a preferred flow velocity of more than 18 m/s at the gas outlet. This prevents sooting of the chamber and downstream systems such as pipes and heat exchangers up to a possible carbon separator.
  • the reaction space is divided into a plasma generation area and a fission area, with both areas being separated from one another by a constriction. It is particularly advantageous if the feed of starting material is arranged in the fission area.
  • the separation into the two areas does not mean that fission necessarily takes place exclusively in the fission area; rather, it can also occur partially in the plasma generation area.
  • the plasma lysis device preferably has at least one gas outlet for a product gas produced, in particular for molecular hydrogen and gaseous byproducts, as well as an outlet for at least one solid byproduct from the reaction chamber.
  • Solid byproducts such as solid carbon
  • Solid byproducts can be in powder form, for example. The removal of the solid byproducts from the reaction chamber improves the process efficiency, since they can no longer interfere with the splitting process and ensures a continuous process. Solid byproducts can be powdered carbon in different modifications, for example if the starting material is methane.
  • a carbon separator can preferably be connected to the gas outlet, for example a cyclone or filter bags. This can be used in the gas stream existing carbon must be separated from the product gas to prevent clogging of subsequent membranes or adsorbers.
  • the plasma lysis device can have one or more membranes and/or one or more adsorbers to filter out gaseous by-products from a gas stream of the gas outlet for the molecular hydrogen. These can be arranged, for example, within the gas outlet for the molecular hydrogen or at one end of the gas outlet for the molecular hydrogen.
  • polymer membranes can be used to separate molecular hydrogen and gaseous by-products.
  • Ceramic materials with a large surface area and high adsorption capacity for a corresponding gaseous by-product, in particular so-called molecular sieves can be used as adsorbers.
  • zeolites i.e. crystalline aluminosilicates
  • these can also be carbon molecular sieves.
  • silica gel or activated aluminum oxide can be used as adsorbers.
  • Zeolite Socony Mobil-5 ZSM-5
  • a synthetic high-silica aluminosilicate zeolite can also be used as adsorbers. This makes it possible to separate gaseous by-products from molecular hydrogen. Furthermore, the gaseous byproduct can be fed back into the reaction chamber via the feed line. This can increase the yield of molecular hydrogen.
  • the membrane or the selective adsorber can also be selectively introduced into the gas outlet for the molecular hydrogen in order to adjust a composition of the gas stream flowing through the gas outlet for the molecular hydrogen.
  • methane remaining in the gas stream can be specifically mixed with the molecular hydrogen in a predetermined ratio. This can make it possible to provide a synthetic fuel, in particular a synthetic gas.
  • solid by-products with small particle sizes such as elemental carbon
  • solid by-products with small particle sizes such as elemental carbon
  • the invention relates to a use of the product gas produced by the plasmalysis device according to one of claims 12 to 16 or another embodiment of the plasmalysis device, in particular molecular hydrogen and/or the at least one by-product, for producing subsequent products.
  • Which subsequent products can be produced on the basis of the product gas produced by the plasmalysis device and/or the at least one by-product depends, among other things, on which by-products and product gases are produced.
  • the hydrogen-containing gas can contain carbon in addition to hydrogen.
  • the hydrogen-containing gas can also contain nitrogen or noble gases. Nitrogen or a noble gas can also be introduced into the reaction chamber in addition to the hydrogen-containing gas, for example via one of the other gas supply lines.
  • a solid or liquid starting material can contain hydrocarbons and thus carbon as well as hydrogen.
  • the hydrogen-containing gas can contain methane (CH4), for example.
  • the at least one by-product can contain carbon structures, for example carbon agglomerates. If methane is passed through the plasma, high-quality carbon structures can be produced. The quality of the carbon structures also depends on the parameters of the plasma lysis device during the production process. With lower energy input, for example, smaller carbon agglomerates are produced and a higher hydrogen yield is achieved. Smaller carbon agglomerates are carbon structures with smaller particle sizes of the agglomerates, for example in the range of particle sizes below 200
  • the hydrogen yield is reduced, for example to 20% compared to a maximum hydrogen yield.
  • the properties of the carbon agglomerates depend, among other things, on the particle size of the primary particles as well as on the particle size of the carbon agglomerates formed by the primary particles. As the particle size of the primary particles decreases, the viscosity increases, the dispersibility decreases, the electrical conductivity decreases, the color strength increases, and the color tone becomes browner. As the particle size of the carbon agglomerates decreases, the viscosity decreases, the dispersibility decreases, the electrical conductivity decreases, the color strength increases, and the color tone becomes browner.
  • the power depends on the current and voltage.
  • the average particle size for example, depends particularly strongly on the current at a fixed voltage.
  • the by-product can, for example, contain more than 95% by weight of carbon particles.
  • the average particle size of the carbon agglomerates can, for example, be between 7.7 ⁇ m and 105 ⁇ m.
  • the carbon particles can form carbon agglomerates which together can form a porous solid.
  • the porous solid can, for example, have pore radii between 0.18 nm and 1.7 nm. Pore volumes can, for example, be between 0.016 and 0.037 cc/g.
  • the by-product can be in the form of a porous solid.
  • the by-product can have a surface area of between 50 m 2 /g and 2000 m 2 /g, determined by BET measurement.
  • the by-product can contain, for example, carbon black, in particular industrial carbon black.
  • the carbon black can, for example, have a dibutyl phthalate absorption (DBPA) measured according to DIN 53601: 1978-12 of between 30 and 130 ml/100g and an iodine number of 10 to 160 mg/g.
  • DBPA dibutyl phthalate absorption
  • a cascaded separation process can be carried out in which the starting material is split in several successive stages and the resulting gases and by-products are separated from each other.
  • the product gas produced and the at least one by-product can also be passed through several plasma lysis devices, for example with different parameters of the plasma lysis device.
  • the different plasma lysis devices can have different temperatures in the reaction space and/or the plasmas can have different temperatures.
  • molecular hydrogen that is passed through the plasma can increase the temperature and create a hot hydrogen plasma.
  • the changed temperatures can be used to achieve different hydrogen yields and produce by-products, for example with higher quality structures.
  • gas streams that are discharged from a first plasmalysis device can also be separated in such a way that only a portion of the gas streams are fed to a subsequent second plasmalysis device.
  • the at least one by-product as a carbon structure in the form of soot can have the following different ASTM grades depending on the intended application or purpose of use: N110, N115, N121, N220, N234, N330, N326, N339, N347, N375, N539, N550 or N650.
  • the downstream products of molecular hydrogen can include, for example, ammonia, acetylene or synthetic gas, such as a syngas HCO mixture.
  • the downstream products of molecular hydrogen can in turn be further processed in other applications to produce subsequent downstream products.
  • ammonia can be used to produce fertilizer.
  • Molecular hydrogen can also be used, for example, to generate energy, store energy, as fuel or to desulfurize fuels.
  • the downstream products of molecular hydrogen can include, for example, ammonia, acetylene or synthetic gas, such as a syngas HCO mixture.
  • the downstream products of molecular hydrogen can in turn be further processed in other applications to produce subsequent downstream products.
  • ammonia can be used to produce fertilizer.
  • Molecular hydrogen can also be used, for example, to generate energy, store energy, as fuel or to desulfurize fuels.
  • the secondary products of the at least one by-product also depend on the starting material.
  • the at least one by-product produced in addition to the molecular hydrogen depends on various parameters of the plasma lysis device during the production process.
  • a surface size and a clustering of carbon chains can be adjusted, among other things, in order to produce different carbon structures, for example different types of soot.
  • the carbon structures can also be produced, for example, with a plasma,
  • the plasma of the plasma lysis device can be post-treated to produce new crystalline structures.
  • several plasma lysis devices can be arranged in series so that the carbon structures produced in the first plasma lysis device can be post-treated in a second plasma lysis device. Different carbon structures in different shapes can therefore be produced.
  • the parameters of the plasma lysis device can be optimized during the production process, for example, so that a specific by-product is produced, e.g. with a specific carbon structure that is optimized for a specific application or further processing into a subsequent product.
  • Downstream products that can be made from the carbon structures or to which the carbon structures can be added as an additive can include, for example, compostable products such as coffee capsules and containers, or also feed additives, ceramics, improved manure, activated carbon for wastewater treatment, coal for the extraction of phosphorus and other chemical bases in sewage sludge, improved soil for improved storage of nutrients, carbon binder mixtures for example as a building material substitute or plastics substitute, carbon polymer mixtures, carbon biopolymers, carbon silicates, coke, asphalt mixtures, cement mixtures, concrete mixtures, tires, paints, varnishes, black surfaces, batteries, coatings, toner, ink, conductive ink, mechanical rubber products, conveyor belts, casings, closures, plastics, cables and containers. Certain downstream products can be used, for example, for insulation, filtration, packaging or lightweight construction.
  • Another downstream product can be, for example, a methane-carbon dioxide mixture (CH4 + CO2), which can be used as a precursor for the Fischer-Tropsch process to produce kerosene.
  • Downstream products can also contain synthetic fuels that can be synthesized on the basis of the gas streams produced by the plasmalysis device. Synthesis can also be carried out in the plasmalysis device itself, for example at 50 bar. Fission steps can also be combined with synthesis steps.
  • the invention relates to a use of molecular hydrogen produced in a plasma lysis device according to one of claims 12 to 16 or another embodiment of the plasma lysis device for the following applications: as fuel, for producing a hydrogen combustion product, as a propulsion agent, for operating a hydrogen-powered vehicle, for mixing with liquefied gas, for mixing with liquefied natural gas (LNG), for mixing with liquid biomethane (LBM), for mixing with natural gas, for mixing with methane, for producing synthesis gas, for producing synthetic fuel, for producing ammonia which can be further used for fertilizer production, for refining petroleum, for hydrogenating chemical compounds, for operating a hydrogen turbine, for operating a fuel cell, for operating a combined heat and power (CHP) plant, for operating a cogeneration plant, for generating energy by means of a fuel cell, for generating energy and/or heat by means
  • the invention relates to a use of by-product produced in a plasmalysis device according to one of claims 12 to 16 or another embodiment of the plasmalysis device for the following applications: as a reducing agent in the production of steel, as a fuel, as an adsorbent, for example in chemistry, medicine, drinking water treatment, waste water treatment, ventilation technology or air conditioning technology, as a carrier material for catalysts for heterogeneous catalysis, as a base material for the production of carbon structures, - as an additive for the production of asphalt, as an additive for the production of cement, as an additive for the production of concrete, as an ingredient of a thermal conductivity agent, for example a thermal paste, as activated carbon for waste water treatment, - as a feed additive, as an additive to a binder, as an additive to soil for improved storage of nutrients, as coal for the extraction of phosphorus and other chemical base substances in sewage sludge, - as an additive in building materials, as an additive in plastics, for insulation, for filtration, for packaging
  • the by-product can also be used, for example, in the steel industry, for example in blast furnaces or cupola furnaces. Protection is only claimed for by-product actually produced with the plasmalysis device. In other words, this concerns exactly the situation in which the by-product is produced in the plasmalysis device and then exploited, for example by being used for a specific application.
  • FIG. 1 A schematic representation of an embodiment of a plasma electrode arrangement according to the first aspect of the invention in a sectional view;
  • FIG. 2 A schematic representation of the embodiment of a plasma electrode arrangement according to Fig. 1 in a perspective view;
  • FIG. 3 A schematic representation of an embodiment of a plasmalysis device according to the second aspect of the invention.
  • Fig. 1 shows a schematic representation of an embodiment of a plasma electrode arrangement 1000.
  • This comprises a cylindrical hollow outer electrode 200, an ignition electrode 100 and an inner electrode (not shown here).
  • the inner electrode is arranged at a distance within the outer electrode 200 and the ignition electrode 100 and is preferably also hollow.
  • the inner electrode forms a counter electrode to the outer electrode and the ignition electrode.
  • the ignition electrode 100 is ring-shaped and is electrically insulated and spaced apart from the outer electrode 200.
  • the ignition electrode 100 can also be connected to a high-voltage source, here via a contacting device 120.
  • the ignition electrode 100 is flattened on a side facing the outer electrode 200 and its thickness decreases from a side facing away from the outer electrode 200 to a side facing the outer electrode.
  • the ignition electrode 100 is therefore essentially designed as a hollow truncated cone, to which a fastening region 110 adjoins.
  • the ignition electrode is mechanically connected to the outer electrode 200 via the fastening region 110 via insulating spacers 210.
  • the ignition electrode 100, outer electrode 200 and inner electrode 300 are preferably made of graphite here.
  • Two gas guide rings 410 of a gas guide device 400 are arranged above the ignition electrode 100 via further insulating spacers.
  • the gas guide rings 410 and with them the gas guide device 400 have channels for guiding gas. These are discussed in more detail in Fig. 2.
  • the gas guide rings 410 are arranged here in a housing 450 having a ceramic tube.
  • the plasma electrode arrangement 1000 further comprises a bayonet connection 500 for connection to a bayonet base in an opening of a reaction chamber.
  • the bayonet connection 500 has bayonet pins 510 for engaging in corresponding openings of the bayonet base.
  • the outer electrode 200 and the ignition electrode 100 are mechanically connected to the bayonet connection 500. In the embodiment shown, the outer electrode extends within the bayonet connection and from there further into the reaction chamber, which is only indicated here.
  • Fig. 2 additionally shows, in a schematic representation, the embodiment of a plasma electrode arrangement 1000 according to Fig. 1 in a perspective view.
  • the channels 420 of the gas guide device 400 can be clearly seen, which are arranged concentrically around an inner opening through which the inner electrode can be guided.
  • Fig. 3 shows a schematic representation of an embodiment of a plasma lysis device 2000 according to the second aspect of the invention.
  • the plasma lysis device 2000 for splitting a starting material into at least one product gas and at least one by-product comprises a plasma electrode arrangement 1000. This is located at least partially in a reaction chamber 2005, which is divided here into a plasma generation region 2010 and a splitting region 2020, with both regions being separated from one another by a constriction 2015.
  • the separation into both regions does not mean that a Fission necessarily takes place exclusively in the fission region, but it can also occur partially in the plasma generation region.
  • the plasma electrode arrangement 1000 here comprises an ignition electrode 100, an outer electrode 200 and an inner electrode 300. Furthermore, it comprises a gas guide device 400. A plasma gas can be supplied via the plasma gas supply line 2800, which is connected to the gas guide device.
  • a starting material feed 2100 is arranged here in the fission region 2020, i.e. below the plasma electrode arrangement 1000.
  • the plasma lysis device 2000 further comprises an alternating current source 2400 connected to the outer electrode 200.
  • the ignition electrode 100 is connected to a separate high-voltage source 2300.
  • the high-voltage source 2300 can be either a high-frequency or a low-frequency voltage source.
  • the plasma lysis device 2000 further comprises a magnetic coil 2600 which is arranged outside the reaction chamber 2005 and is designed to generate a magnetic field in which at least one end of the outer electrode 200 facing away from the ignition electrode 100 is arranged.
  • the plasma lysis device 2000 here also has a gas discharge line 2200 for a generated product gas, in particular for molecular hydrogen and gaseous by-products, as well as a discharge line 2700 for at least one solid by-product from the reaction space.
  • the plasma electrode arrangement 1000 has an electrode changing system 2500 comprising a plurality of inner electrodes 300 in a drum arrangement of a revolver system.
  • the electrode changing system 2500 is designed to lower exactly one inner electrode into an interior of the outer electrode 200 and, after a predetermined time or in response to a control signal, to raise the lowered inner electrode 300, to rotate the drum by at least one position and to lower another inner electrode into the interior.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • Plasma & Fusion (AREA)
  • Chemical & Material Sciences (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Organic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

L'invention concerne un ensemble d'électrodes à plasma qui comprend une électrode externe creuse cylindrique, une électrode d'amorçage annulaire qui est électriquement isolée et espacée de l'électrode externe, et une électrode interne qui est disposée à l'intérieur de l'électrode externe et de l'électrode d'amorçage à distance de celles-ci, l'électrode d'amorçage (100) pouvant être connectée à une source de haute tension.
PCT/EP2023/078500 2022-10-13 2023-10-13 Ensemble d'électrodes à plasma et dispositif d'analyse de plasma WO2024079322A1 (fr)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
DE102022126660.5 2022-10-13
DE102022126660.5A DE102022126660A1 (de) 2022-10-13 2022-10-13 Plasmaelektrodenanordnung und Plasmalysevorrichtung
DE102023110741 2023-04-26
DE102023110741.0 2023-04-26

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1019848A (en) * 1963-10-29 1966-02-09 Ass Elect Ind Improvements relating to plasma arc torch assemblies
WO1993020152A1 (fr) 1992-04-07 1993-10-14 Kvaerner Engineering A.S. Reacteur de decomposition
US5486674A (en) * 1991-12-12 1996-01-23 Kvaerner Engineering As Plasma torch device for chemical processes
CN109162853A (zh) * 2018-10-26 2019-01-08 大连民族大学 一种双放电模式等离子体点火器
CN109253029A (zh) * 2018-10-26 2019-01-22 大连民族大学 一种具有渐扩接地电极出口结构的等离子体点火器
CN109488510A (zh) * 2018-10-26 2019-03-19 隆成利达（大连）科技有限公司 具有环-柱双阳极结构的双电离模式等离子体点火器

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB1019848A (en) * 1963-10-29 1966-02-09 Ass Elect Ind Improvements relating to plasma arc torch assemblies
US5486674A (en) * 1991-12-12 1996-01-23 Kvaerner Engineering As Plasma torch device for chemical processes
WO1993020152A1 (fr) 1992-04-07 1993-10-14 Kvaerner Engineering A.S. Reacteur de decomposition
CN109162853A (zh) * 2018-10-26 2019-01-08 大连民族大学 一种双放电模式等离子体点火器
CN109253029A (zh) * 2018-10-26 2019-01-22 大连民族大学 一种具有渐扩接地电极出口结构的等离子体点火器
CN109488510A (zh) * 2018-10-26 2019-03-19 隆成利达（大连）科技有限公司 具有环-柱双阳极结构的双电离模式等离子体点火器

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