WO2023099005A1 - Méthode et dispositif de craquage à basse température d'un matériau de départ contenant des hydrocarbures - Google Patents

Méthode et dispositif de craquage à basse température d'un matériau de départ contenant des hydrocarbures Download PDF

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Publication number
WO2023099005A1
WO2023099005A1 PCT/EP2021/084032 EP2021084032W WO2023099005A1 WO 2023099005 A1 WO2023099005 A1 WO 2023099005A1 EP 2021084032 W EP2021084032 W EP 2021084032W WO 2023099005 A1 WO2023099005 A1 WO 2023099005A1
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Prior art keywords
starting material
hydrocarbon
reactor
gas
hydrogen
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PCT/EP2021/084032
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German (de)
English (en)
Inventor
Sahabi BEHZAD
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Behzad Sahabi
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Priority to PCT/EP2021/084032 priority Critical patent/WO2023099005A1/fr
Publication of WO2023099005A1 publication Critical patent/WO2023099005A1/fr

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
    • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
    • C10K3/001—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by thermal treatment
    • C10K3/003—Reducing the tar content
    • 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
    • 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
    • C01B2203/0465—Composition of the impurity
    • C01B2203/049—Composition of the impurity the impurity being carbon
    • 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
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/12—Heating the gasifier
    • C10J2300/123—Heating the gasifier by electromagnetic waves, e.g. microwaves
    • C10J2300/1238—Heating the gasifier by electromagnetic waves, e.g. microwaves by plasma

Definitions

  • the invention relates to a method and a device for the low-temperature cracking of a hydrocarbon-containing starting material.
  • hydrocarbons are produced that cannot be put to any meaningful use.
  • Gases containing hydrocarbons are often flared off using gas flares, e.g. associated gases in oil production, unusable quantities of gas in biogas production, landfill gas and unusable parts of sewage gas in sewage treatment plants.
  • the gases to be flared are therefore also called flare gases or flare gases.
  • hydrocarbons that cannot be used can also come from waste plastics, for example from landfills, plastic waste that can no longer be mechanically recycled, bilge oil or natural gas.
  • microwave technology for the pyrolysis of organic material, in particular used tires or similar rubber mixtures, is proposed in DE 3880155 T2.
  • the organic material is preheated by a stream of hot gas and the preheated material is introduced directly into a microwave discharge zone in a substantially oxygen-free superatmospheric gas atmosphere. Solid fission products containing elemental carbon and gaseous by-products are formed.
  • DE 10 2015 218 098 A1 discloses a method and a device for the thermal cracking of hydrocarbons, thermal energy being generated by an arc in a plasma gas between at least two electrodes.
  • the heated plasma gas is mixed with the hydrocarbons to be split, the hydrocarbons being at a temperature heated by more than 600 °C.
  • a mixture of carbon and hydrogen is formed.
  • EP 1643001 A1 discloses a method and a device for the thermal cracking of hydrocarbons, in which the plasma of a microwave discharge is used for cracking and which serves to produce polycrystalline diamond layers.
  • WO 2004033368 A1 discloses a device for fuel reforming, with which a reformed fuel gas containing hydrogen and which is free of carbon monoxide is to be generated.
  • a mixture of hydrocarbon fuel is passed through a first reformer unit.
  • the reformed gas stream is then passed through a non-thermal plasma generated in a microwave reactor to convert any remaining carbon monoxide. Thereafter, the fuel can be supplied to a fuel cell.
  • WO 2019032554 A1 discloses a method and a device of the type mentioned at the outset, according to which microwave radiation from a radiation source is fed via a waveguide to a resonator which includes a reaction space.
  • Plasma-generating material is fed into the reaction space from a first material source and a starting material containing hydrocarbons is fed from a second source.
  • the hydrocarbon-containing starting material is thermally split, resulting in a carbon-enriched intermediate product and a hydrogen-enriched intermediate product.
  • the carbon in the form of graphite or graphene can be separated from the resulting split material.
  • sponge iron also known as DRI (“direct reduced iron”) for short, by reducing iron ore by adding hydrogen (US 2018/0221947 A1).
  • hydrogen used for iron reduction to thermally decompose a hydrocarbon-containing gas, for example methane, in particular using a high-temperature bubble column reactor in which the hydrocarbon-containing gas is passed through molten metal Hydrogen is collected in gaseous form, while the carbon is deposited as a solid in the molten metal (https://www.chemie.de/news/142290/wasserstoff-aus-methan-ohne-co2-ausstoss.html, online on June 27th. 2019; Tobias Günter G complicatler, "Methane pyrolysis in a liquid metal bubble column reactor (process engineering)", ISBN-10: 3843933448).
  • the invention is based on the object of providing a more efficient use or treatment of hydrocarbon-containing starting materials.
  • Starting materials in particular flare gases or flare gases, which have hitherto not been used or used little for economic or technical reasons, should preferably be put to an economically reasonable use.
  • the object is achieved by a method for low-temperature cracking, in particular for non-thermal cracking, of a hydrocarbon-containing starting material, having the following steps:
  • a core idea of the invention is to use a non-thermal plasma to split the hydrocarbon-containing starting material.
  • the starting material is split into a carbon portion and a hydrogen portion.
  • a non-thermal plasma is understood to mean a plasma in which there is no thermal equilibrium between the electrons excited by the plasma and the hydrocarbon-containing starting material at the macroscopic level.
  • the non-thermal plasma is also referred to as non-thermal microwave plasma in the context of the present invention.
  • an excitation frequency in a range between 900 MHz and 2.5 GHz, for example an excitation frequency of 2.45 GHz, can be selected.
  • Vibrational excitation of the electrons in the hydrocarbon-containing starting material preferably occurs at these excitation frequencies. This leads to a significant mismatch between the temperature of the excited electrons and associated ions of the hydrocarbonaceous feedstock.
  • the aforementioned thermal imbalance between the excited electrons and the hydrocarbon-containing starting material can thus be generated in order to obtain a non-thermal plasma.
  • the macroscopic ambient temperature of the non-thermal plasma is far below the temperature of thermal plasmas and usually does not exceed approx. 150°C if the process is carried out efficiently.
  • the generation of the non-thermal plasma can take place without using an additional plasma-generating substance. This makes the process particularly efficient and economical. After splitting in the non-thermal plasma, the carbon content and the hydrogen content are separated from one another in a separating process.
  • no working gas is used to generate the non-thermal plasma.
  • no feed for a working gas is required in the device for low-temperature cracking described below.
  • the inventive method for the cleavage of the hydrocarbonaceous feedstock no pyrolysis of the hydrocarbonaceous feedstock. Rather, the generation of the non-thermal plasma causes a chemical-physical splitting of the hydrocarbon-containing starting material.
  • the hydrocarbonaceous feedstock is not preheated prior to the generation of the non-thermal plasma. This increases the efficiency of the method according to the invention and the device according to the invention.
  • the at least one process parameter is preferably selected from the following list: pressure, volume throughput and/or temperature of the gaseous, hydrocarbon-containing starting material before the microwave plasma is generated, for example directly before the microwave plasma is generated, pressure and/or temperature at the microwave plasma generation site, amount of substance and/or composition of matter after the separation of the carbon fraction and the hydrogen fraction, pressure, volume flow rate and/or temperature of the carbon fraction and/or the hydrogen fraction after the separation.
  • Conventional sensors can be used to monitor the process parameters.
  • the non-thermal plasma is preferably generated by means of microwave radiation acting on the hydrocarbon-containing starting material.
  • a non-thermal plasma in this case a non-thermal microwave plasma—is generated from at least a portion of the hydrocarbon-containing starting material.
  • the microwave radiation is generated in a microwave plasma device.
  • the frequency of the microwaves is preferably in a range between 900 MHz and 2.5 GHz and is particularly preferably 2.45 GHz.
  • the microwave plasma device is preferably operated at pressures between 1 bar and 8 bar.
  • the method step for generating the non-thermal plasma involves generating a non-thermal microwave plasma from (at least a proportion of the gas or vapor present or brought into gas or vapor form or from) the hydrocarbon-containing starting material by means of the starting material acting microwave radiation in a microwave plasma device for splitting the hydrocarbon-containing starting material into a carbon portion and a hydrogen portion.
  • the carbon portion and the hydrogen portion are separated in a separating process outside of the microwave plasma device.
  • the invention is not limited to the generation of a non-thermal microwave plasma for fission. Generation of the non-thermal plasma can also be accomplished by other means. The only decisive factor is that a non-thermal plasma is used for the cleavage, which enables the low-temperature cleavage according to the invention.
  • the hydrocarbon-containing starting material can already be present in the gas phase and can be formed, for example, by a hydrocarbon-containing gas and/or hydrocarbon-containing vapor. Likewise, the starting material can initially be in the liquid phase and brought into the gaseous phase before or during the generation of the non-thermal microwave plasma.
  • the hydrocarbon-containing starting material preferably comprises associated gas or is generated from this. This provides an alternative to the usual flaring of associated gas.
  • Other hydrocarbon-containing raw materials intended for flaring can also be used as starting material.
  • the use of these gases, which are otherwise used as flare gases or flare gases, is environmentally friendly because on the one hand the emission of CO2 is reduced and on the other hand energy can be generated.
  • the hydrocarbon-containing starting material can include liquefied plastic, in particular from waste plastic, or bilge oil, from petroleum, from biogas or natural gas or can be generated from these substances.
  • the hydrocarbon-containing starting material can in particular come from waste plastics, for example from landfills, plastic waste that can no longer be mechanically recycled, biomass, biogas, clathrates, biogenic methane, bilge oil, crude oil or natural gas.
  • the invention can also be used in the utilization of conventional hydrocarbon-containing starting materials, in particular crude oil or natural gas.
  • the advantage of the invention lies in the very high energy efficiency of the process, which enables gentle handling of the bottleneck resource of the CCh-neutral electricity.
  • the starting material is preferably in a purified form.
  • the associated petroleum gas used or the other hydrocarbon-containing base material can be subjected to purification, e.g. desulfurization and possibly further purification measures.
  • Suitable cleaning processes are known from the prior art, e.g. for various gases containing hydrocarbons, e.g. digester gas, landfill gas, gases from anaerobic industrial wastewater treatment and natural gas.
  • the starting material can be reacted with iron oxide hydroxide (FeO(OH)), e.g. in a fixed bed absorber or a fluidized bed absorber.
  • the method therefore preferably comprises a purification of the hydrocarbon-containing starting material.
  • the purification of the hydrocarbon-containing starting material is particularly preferably carried out by passing the hydrocarbon-containing starting material through an absorption reactor is passed to be reacted with iron oxide hydroxide (FeO(OH)).
  • passing the hydrocarbonaceous feedstock through the absorption reactor comprises passing the hydrocarbonaceous feedstock through one or more fractals.
  • passing the hydrocarbonaceous feedstock through the absorption reactor comprises passing the hydrocarbonaceous feedstock through one or more fractals.
  • the iron oxide hydroxide is preferably provided as a bed in the absorption reactor.
  • the hydrocarbon-containing starting material is preferably passed through the bed of iron oxide hydroxide in the absorption reactor.
  • sulfur is eliminated from the hydrocarbonaceous feedstock. This produces iron sulfide (FeS/FezSs).
  • the purification step comprises feeding iron oxide hydroxide, preferably continuously, into the absorption reactor (e.g. by means of a feed screw conveyor) and removing iron sulphide from the absorption reactor, preferably continuously (e.g. by means of a discharge screw conveyor).
  • the cleaning step by means of suitable sensors, for example by recording the volume throughput of the hydrocarbon-containing starting material that is fed into the absorption reactor and/or the volume throughput of the cleaned hydrocarbon-containing starting material that is discharged from the absorption reactor. This information can be used, for example, to adjust the amount of iron oxide hydroxide fed to the absorption reactor.
  • the cleaning step can be carried out before and/or after the generation of the non-thermal microwave plasma.
  • the separation process includes a separation of at least part of the carbon content.
  • the deposition can e.g. B. as graphite and / or graphene.
  • at least one electrostatic separator in particular a corona reactor, can be used, alternatively, a centrifugal separator, z. B. in the form of a cyclone device, or for example a molten metal can be used.
  • the invention also provides for the method according to the invention to be used to carry out a method for reducing a solid, in particular silicon dioxide or one or more iron oxides, e.g. as they occur in iron ores, such as FezCh or FeaO, using at least one for the reduction process Part of the hydrogen generated during thermal cracking is used.
  • part of the hydrogen generated during thermal cracking can be used to generate energy.
  • the object of the invention is also achieved by a device for low-temperature cracking, in particular for non-thermal cracking, of a starting material containing hydrocarbons, having a microwave plasma device with a reactor chamber and a microwave source, a separating device connected to the reactor chamber via a discharge line, and at least one sensor for measuring or monitoring a process parameter, the microwave plasma device being set up to generate a non-thermal plasma from at least part of the hydrocarbon-containing starting material located in the reactor chamber for non-thermal cracking or low-temperature cracking of the hydrocarbon-containing starting material into a carbon component and a hydrogen component produce, and wherein the separating device is set up to separate the carbon content from the hydrogen content.
  • the same advantages can be achieved that were described above in relation to the method according to the invention.
  • Features of the device in particular functional features of the structural elements of the device, can be transferred as method steps to the method according to the invention.
  • features of the method according to the invention can be transferred to the device according to the invention by configuring the device in such a way that it is used for Execution of the corresponding process features is trained and suitable.
  • the device according to the invention is preferably designed and used for carrying out the method according to the invention described above, it is preferred that the method according to the invention is carried out with a device according to the invention.
  • the present invention also includes the use of the device according to the invention for carrying out the method according to the invention.
  • the device has a feed line for the hydrocarbon-containing starting material to the reactor space.
  • the hydrocarbonaceous feedstock is provided in the gas phase.
  • the feed line is designed as a gas (pipe) line.
  • the device has a plasma device with a reactor space and plasma source, a separating device and a sensor.
  • a microwave source is preferably used to generate the plasma.
  • one or more of these elements may be provided multiple times in the device.
  • a larger number of microwave plasma devices can be provided as separating devices in the device, so that several microwave plasma devices are assigned to one separating device.
  • the device has at least one sensor for measuring or monitoring at least one process parameter.
  • the at least one sensor is preferably designed to measure the process parameter to be monitored continuously or at predetermined time intervals.
  • the at least one sensor is preferably a pressure sensor, a temperature sensor, a volume flow sensor, a particle counter and/or a particle analyzer, for example a gas chromatograph.
  • a pressure, temperature or volumetric flow sensor is preferably arranged in front of the reactor chamber, for example on the supply line, or on or in the discharge line. If the sensor is formed by a particle counter and/or a particle analyzer, it is preferable to arrange the sensor after the reactor space in order to detect the fission products from be able to characterize or quantify the values obtained in the reactor space.
  • the measured values determined with the at least one sensor can also be used to control the device.
  • the at least one separating device or at least one of the separating devices comprises a separating unit.
  • the separating unit can include an electrostatic separator such as a corona reactor and/or a centrifugal separator. It is also possible that the at least one separating device or at least one of the separating devices comprises a molten metal washer.
  • the device has a reduction unit which is connected to the at least one separating device or to at least one of the separating devices via an intermediate line and is set up to reduce a substance by means of the hydrogen content.
  • the device has at least one absorption reactor which is designed to clean the hydrocarbon-containing starting material, in particular to separate sulfur-containing components.
  • the at least one absorption reactor can be arranged before and/or after the at least one microwave plasma device.
  • the absorption reactor preferably has a closed reaction space which is designed to carry out the reaction required for purification.
  • the absorption reactor preferably also has at least one gas inlet for connection to a gas supply line.
  • the at least one gas inflow is preferably formed in a lower region of the absorption reactor.
  • the absorption reactor preferably also has at least one gas outlet for connection to a gas outlet.
  • the at least one gas outlet is preferably formed in an upper region of the absorption reactor.
  • the reaction material in the absorption reactor is preferably formed by iron oxide hydroxide.
  • the reaction reactor preferably has at least one fractal, which is arranged at the at least one gas inflow and is designed to homogenize the flow of the supplied hydrocarbon-containing starting material and to distribute it over a broader cross section.
  • a fractal is to be understood as meaning an element through which gas can flow, which enables a targeted distribution and homogenization of the gas flow over a large flow area.
  • the structure of such a fractal with at least two successive inflow layers with a large number of flow openings is particularly advantageous, with successive inflow layers having an increasing number of flow openings with a decreasing cross-sectional area of the individual flow openings.
  • the gas flowing through the fractal can be successively distributed over a larger number of flow openings with decreasing cross-sections as it flows through the successive layers. In this way, a targeted distribution and homogenization of the gas flow over a large flow area is achieved.
  • the absorption reactor has a feed means for feeding reaction material.
  • the feeding means is arranged in the upper part of the absorption reactor. Reaction material that is fed in then falls into the absorption reactor due to gravity and can be accumulated there to form a bed.
  • the feeding means comprises an infeed auger.
  • the absorption reactor has a discharge means for discharging spent reaction material after reaction with the hydrocarbonaceous feedstock has taken place.
  • the discharge means is located in the lower part of the absorption reactor. Consumed reaction material falling down in the reaction reactor can then be discharged from the reaction reactor.
  • the discharge means preferably has a discharge screw conveyor.
  • the invention also provides for the use of the device according to the invention described above for low-temperature cracking, in particular for the non-thermal cracking of hydrocarbon-containing starting materials, in particular flare gas.
  • advantageous exemplary embodiments of the method according to the invention possible uses of the method and the device according to the invention are presented using figures.
  • FIG. 2 shows a schematic representation of a first unit (upper level) of a device according to the invention in an oblique view
  • FIG. 3 shows a schematic representation of a second unit (lower level) of the device according to the invention in an oblique view
  • FIG. 6 shows a schematic cross-sectional view of an absorption reactor according to an embodiment of the present invention.
  • FIG. 1 shows a flow chart of an exemplary variant of the method according to the invention, not all of the method steps shown being obligatory, but possibly also being replaced by alternative method steps or else being omitted.
  • hydrocarbons for example natural gas, bilge oil, oil from plastics processing or conventional hydrocarbon-containing starting materials
  • the starting material should be brought into a state suitable for the process, in particular a state of aggregation if necessary, cleaned and/or free from undesirable substances, for example sulphur.
  • the starting material is conveyed from a starting material source 1, optionally via a heat-supplying unit, preferably via a heat exchanger 2, and optionally via a feed pump 3, to a microwave plasma unit 4, hereinafter referred to as MWP unit 4 for short, in which the starting material a non-thermal plasma, in the present exemplary embodiment a non-thermal microwave plasma, is generated.
  • the feed pump can be dispensed with if the starting material is introduced into a device carrying out the process with sufficient pressure.
  • the non-thermal plasma the hydrocarbon of the starting material is split into a carbon portion and a hydrogen portion.
  • the mixture of carbon content and hydrogen content is then fed to an electrostatic separator 5, which serves as a separating device for separating the carbon content from the hydrogen content.
  • the carbon can essentially occur in nanoform, for example as graphene. However, the carbon can also occur as graphite or in some other form.
  • the carbon is collected separately and can be used for other purposes.
  • separating devices can also be used, e.g. a device based on centrifugal force, for example a cyclone separator or a metal melt, through which the hydrogen-carbon mixture is passed. Separating or separating devices of this type are known from the prior art.
  • the hydrogen can be used for various purposes, e.g. in particular SiCh, with which pure silicon 9 can be produced.
  • SiCh silicon carbide
  • water 10 is produced in addition to the reduced material obtained.
  • a further optional alternative or further use of the hydrogen produced can be the operation of a combined heat and power plant 11 , in which water 10 is obtained and used to produce electricity 12 and heat 13 can be.
  • the heat 13 and/or the current 12 can be used in full or in part for the device according to the invention, e.g. B. for the optional heat exchanger 2 or for the optional feed pump 3 or for the MWP unit 4.
  • At least one process parameter is monitored while the method is being carried out.
  • process steps and transitions that are particularly suitable for this purpose are marked with an asterisk.
  • the parameters affected in the respective method step are particularly suitable as process parameters for monitoring during the method steps.
  • the quantity characterised, for example, by the volume throughput
  • parameters such as the pressure and/or temperature of the process gas.
  • the sensors required for this are inexpensive to purchase, easy to attach and robust in operation
  • these process parameters provide relevant information about the process sequence, which allows both control of the process and targeted error analysis during operation.
  • FIGS. 2 and 3 show two sub-systems of an exemplary embodiment of the device according to the invention, namely FIG. 2 a first sub-system 14 and FIG .
  • both subsystems 14 and 15 work together, with the first subsystem 14 being arranged above the second subsystem 15, for example.
  • a raw material here for example flare gas
  • a cleaning unit here for example consisting of two absorption reactors 17, where the flare gas is freed from foreign substances, e.g. sulfur, as far as possible .
  • the absorption reactors 17 can be, for example, fixed-bed absorbers or acting fluidized bed absorber.
  • the flare gas to be cleaned can be reacted in the absorption reactors 17, for example with iron oxide hydroxide FeO(OH).
  • the cleaned flare gas is optionally fed as starting material via a second pipe system 18 to a distributor unit 19, which preferably can have a fractal (not visible here) and supplies the starting material via distributor pipe systems 20 to microwave plasma reactors 21, hereinafter referred to as MWP reactors 21.
  • MWP reactors 21 microwave plasma reactors 21, hereinafter referred to as microwave plasma reactors 21, hereinafter referred to as MWP reactors 21.
  • MWP reactors 21 For the sake of clarity, only one distributor pipe system 20 and two MWP reactors 21 are provided with reference numbers. 2 shows a total of six MWP reactors 21. However, MWP reactors 21 can also be provided in a smaller or larger number and/or in a different arrangement.
  • the MWP reactors 21 are each fed by a microwave source 22 that preferably has a controller.
  • sensors 51 are also shown schematically at various points in the device, which allow process parameters to be monitored while the method is being carried out.
  • the sensors in the pipe systems are preferably pressure, temperature and/or volume flow sensors.
  • Fig. 4 shows a MWP reactor 21 schematically in cross section with a reactor inlet 23, which is followed in the flow direction symbolized by the arrow by a distribution device 24, which preferably has a fractal causing a uniform distribution of the cleaned starting material over the reactor cross section, as indicated here.
  • a reactor space 25 is preferably delimited by a reactor space wall 26, for example made of quartz glass, and surrounded by a microwave waveguide 27, which is fed by the microwave source 22 (see FIG. 2), not shown in FIG.
  • a non-thermal microwave plasma is generated with the feedstock. Other additives are not required to generate the plasma.
  • the generation of the non-thermal plasma causes the hydrocarbons in the starting material to be split into hydrogen and carbon at comparatively low temperatures.
  • the fission products hydrogen and carbon are present as a mixture.
  • the hydrogen/carbon mixture leaves the MWP reactor 21 in the flow direction (arrow) through the reactor outlet 28 into a reactor outlet pipe 29, not shown in Fig. 4.
  • the reactor outlet pipes 29 connected to the reactor outlets 28 of the MWP reactors 21 when the overall system is complete are shown with open ends in FIG. 3, which connect to the reactor outlets 28 (FIG. 4) in the overall system.
  • reference numeral 51 again indicates sensors which are designed to monitor process parameters.
  • the sensor 51 at the reactor inlet 23 is designed to measure properties of the inflowing reaction gas and preferably comprises a pressure, temperature and/or volume flow sensor. The same applies to the sensor 51 at the reactor outlet 28.
  • the sensor 51 inside the reactor space 25 is designed to characterize the non-thermal plasma and detects at least one process variable of the plasma, such as its temperature.
  • the hydrogen/carbon mixture passes via the reactor outlet pipes 29 into a second distribution pipe system 30, which leads the hydrogen/carbon mixture to six outer electrostatic precipitators 5a (only three of which are provided with a reference number) and a central electrostatic precipitator 5z.
  • the outer electrostatic separators 5a are each assigned to a MWP reactor 21.
  • the central electrostatic separator 5z serves as a backup separator, which is then served with the hydrogen/carbon mixture of one of the MWP reactors 21 when the outer electrostatic separator 5a assigned to this MWP reactor 21 is removed from the process for cleaning or maintenance purposes.
  • the hydrogen/carbon mixture can be controlled, for example, via a three-way valve (not shown here) assigned to the corresponding outer electrostatic separator 5a.
  • the terms "outer electrostatic separator 5a" and "central electrostatic separator 5z” describe the exemplary spatial arrangement given in the figures. Of course, other spatial arrangements are possible.
  • a backup separator can also be dispensed with, or multiple backup separators can be provided.
  • An electrostatic precipitator 5a or 5z is shown in Fig. 5 schematically in cross section. The hydrogen/carbon mixture reaches the electrostatic separator 5a or 5z via a separator inlet 31 and rises there in a separator tower 32 .
  • the carbon On the way through the separator tower 32, the carbon is electrostatically separated from the hydrogen/carbon mixture by means of a discharge electrode 34 and a collecting electrode 35, between which a voltage is built up, and strikes the collecting electrode 35, which at the same time forms the inner peripheral wall of the separator tower 32 is, and at the discharge electrode 34 down.
  • the carbon is shown here as carbon mass 36 .
  • the carbon 36 is thrown off by vibration, e.g. by hitting the separator tower 36, and leaves the separator 5 via a chute 37. It passes through a carbon collection pipe system 38 (Fig. 3) and, if necessary, by means of propulsion means, such as at least one screw conveyor, not shown here the carbon from all separators 5a or 5z into a solids collection container 39 and can be supplied with or from it for further uses.
  • a sensor 51 on the power supply of the electrostatic precipitator 5a, 5z is designed as a current and/or voltage sensor in order to detect the operating properties of the electrostatic precipitator 5a, 5z.
  • a further sensor 51 for detecting the volume throughput, pressure and/or temperature of the outflowing gas is arranged at the separator outlet 33 . It is also possible to use a sensor 51 (not shown) at the separator inlet 31 in order to record the properties of the gases supplied, such as volume throughput, pressure and/or temperature.
  • sensors can be provided both at the separator inlet 31 and at the separator inlet 33, which sensors can determine the material composition of the gases flowing through. This can be used to monitor whether the splitting and separating processes are working properly.
  • the hydrogen from the hydrogen/carbon mixture separated in the separator tower 36 continues to rise and leaves the electrostatic generator 5a or 5z via a separator outlet 33 and reaches a hydrogen collection container via a hydrogen distribution pipe system 40 41.
  • the hydrogen can also be used directly or indirectly for other uses, such as e.g. B. a combined heat and power plant or a plant for the reduction of a material such as iron oxide or silicon oxide or silicon dioxide.
  • FIG. 6 shows a schematic view of an absorption reactor 17 according to an exemplary embodiment of the present invention.
  • the absorption reactor 17 has an essentially closed housing which delimits a reactor interior 46 .
  • the absorption reactor 17 At the upper end of the absorption reactor 17 there is a feed screw conveyor 42 which is used to feed reaction material.
  • the absorption reactor is used to clean sulfur-containing flare gases.
  • iron oxide hydroxide provided as granules as the reaction material.
  • Granular iron oxide hydroxide is fed in as reaction material by means of the feed screw conveyor 42 and is shown schematically by unfilled circles and accumulates in the absorption reactor 17 to form an iron oxide hydroxide bed 49 with a certain filling level in the reactor interior 46 .
  • Gases to be cleaned are fed to the absorption reactor 17 via gas supply lines 44 .
  • the gas supply lines 44 are connected to the absorption reactor 17 via gas inlets (not specifically shown) which are arranged at a lower end of the absorption reactor 17 and are in direct fluid connection with the reactor interior 46 or are arranged in this.
  • the flare gas In order to maximize the efficiency of the absorption reactor 17, it is desirable for the flare gas to be cleaned to flow through the iron oxide hydroxide bed 49 as uniformly as possible over as large an area as possible.
  • fractals 48 are provided at the lower end of the absorption reactor 17, which are configured and arranged in such a way that introduced gases to be cleaned flow through the fractals 48.
  • the gas flow introduced is homogenized and distributed over as wide a cross-section as possible. In this way it can be ensured that essentially the entire cross-sectional area of the absorption reactor 17 is covered by gas to be cleaned is flowed through and thus the entire existing reaction material is used.
  • reaction material in the bed 49 binds sulfur from the flare gas.
  • the resulting reaction product is iron sulfide. Due to the tapering shape of the lower part of the absorption reactor 17, the reaction material that has reacted to form iron sulfide collects at the lowest point of the absorption reactor 17.
  • a discharge screw conveyor 43 is arranged there, which removes the iron sulfide from the reactor interior 46.
  • the reaction material is conveyed directly into the reactor interior 46 .
  • the reaction material in the reactor interior 46 is filled up to a predetermined bed height, with the reaction material 46 being poured directly onto the fractals 48 .
  • the bed height is maintained by conveying reaction material at a predetermined rate per unit time via the feed screw conveyor 42 into the reactor interior 46, while the same rate per unit time of reaction material reacted with the gas is at the bottom of the absorption reactor 17 is deducted via the discharge screw conveyor 43.
  • the schematically illustrated sensors 51 can be provided in the gas supply line 44, which can characterize the kinetic and thermodynamic properties of the supplied gas (for example volume throughput, pressure and/or temperature) and/or its material composition.
  • at least one sensor 51 is provided on the gas discharge line 45, which is designed to characterize kinetic and thermodynamic properties of the discharged, cleaned gas (e.g. volume throughput, pressure and/or temperature) and/or its material composition.
  • the reaction in the absorption reactor 17 can thus be monitored easily.
  • the material composition of the discharged, cleaned gas can also be used to determine whether further reaction material should be introduced into the absorption reactor 17 and in what quantities. reference list

Abstract

L'invention concerne une méthode de craquage à basse température, en particulier un craquage non thermique, d'un matériau de départ contenant des hydrocarbures, comprenant les étapes suivantes : la fourniture du matériau de départ contenant des hydrocarbures dans la phase gazeuse ; la génération d'un plasma non thermique à partir du matériau de départ contenant des hydrocarbures afin de craquer le matériau de départ contenant des hydrocarbures en un composant carboné et un composant hydrogène ; et la séparation du composant carboné et du composant hydrogène ; au moins un paramètre de processus étant surveillé tandis que la méthode est mise en œuvre, de préférence à l'aide de mesures de capteur. L'invention concerne en outre l'utilisation de la méthode pour la mise en œuvre d'une méthode de réduction d'un matériau solide, à un dispositif de craquage à basse température, en particulier pour un craquage non thermique, d'un matériau de départ contenant des hydrocarbures, ainsi que l'utilisation du dispositif pour un craquage à basse température, en particulier pour un craquage non thermique, de gaz de torche.
PCT/EP2021/084032 2021-12-02 2021-12-02 Méthode et dispositif de craquage à basse température d'un matériau de départ contenant des hydrocarbures WO2023099005A1 (fr)

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DE3880155T2 (de) 1987-11-11 1993-07-29 Kenneth Michael Holland Pyrolyses von organischem material.
WO2004033368A1 (fr) 2002-10-08 2004-04-22 Hrl Laboratories, Llc Appareil a reformage de combustible pour la production d'un gaz combustible hydrogene reforme exempt de monoxyde de carbone
US20040148860A1 (en) * 2001-07-25 2004-08-05 Fletcher David E. Production of hydrogen and carbon from natural gas or methane using barrier discharge non-thermal plasma
EP1643001A1 (fr) 2002-09-30 2006-04-05 Institute of Applied Physics RAS Procede haute vitesse de depot de films de diamants en phase gazeuse dans le plasma d'une decharge thf et reacteur a plasma correspondant
US20110289845A1 (en) * 2005-04-12 2011-12-01 Ze-Gen, Inc. Method for controlling syngas production in a system with multiple feed materials using a molten metal bath
US20160244683A1 (en) * 2013-10-10 2016-08-25 Plasco Energy Group Inc. A Non-Equilibrium Plasma-Assisted Method and System for Reformulating and/or Reducing Tar Concentration in Gasification Derived Gas Product
DE102015218098A1 (de) 2015-09-21 2017-03-23 Deutsche Lufthansa Ag Verfahren zur thermischen Spaltung von Kohlenwasserstoffen und korrespondierende Vorrichtung
US20180221947A1 (en) 2016-08-03 2018-08-09 Reid Reactors Llc Method and apparatus for producing metallic iron from iron oxide fines
WO2019032554A1 (fr) 2017-08-08 2019-02-14 H Quest Vanguard, Inc. Conversion non thermique par plasma d'hydrocarbures
EP3878807A1 (fr) * 2020-03-13 2021-09-15 Clariant International Ltd Procédé de production de gaz de synthèse par gazéification allothermique à réduction de dioxyde de carbone contrôlée

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3880155T2 (de) 1987-11-11 1993-07-29 Kenneth Michael Holland Pyrolyses von organischem material.
US20040148860A1 (en) * 2001-07-25 2004-08-05 Fletcher David E. Production of hydrogen and carbon from natural gas or methane using barrier discharge non-thermal plasma
EP1643001A1 (fr) 2002-09-30 2006-04-05 Institute of Applied Physics RAS Procede haute vitesse de depot de films de diamants en phase gazeuse dans le plasma d'une decharge thf et reacteur a plasma correspondant
WO2004033368A1 (fr) 2002-10-08 2004-04-22 Hrl Laboratories, Llc Appareil a reformage de combustible pour la production d'un gaz combustible hydrogene reforme exempt de monoxyde de carbone
US20110289845A1 (en) * 2005-04-12 2011-12-01 Ze-Gen, Inc. Method for controlling syngas production in a system with multiple feed materials using a molten metal bath
US20160244683A1 (en) * 2013-10-10 2016-08-25 Plasco Energy Group Inc. A Non-Equilibrium Plasma-Assisted Method and System for Reformulating and/or Reducing Tar Concentration in Gasification Derived Gas Product
DE102015218098A1 (de) 2015-09-21 2017-03-23 Deutsche Lufthansa Ag Verfahren zur thermischen Spaltung von Kohlenwasserstoffen und korrespondierende Vorrichtung
US20180221947A1 (en) 2016-08-03 2018-08-09 Reid Reactors Llc Method and apparatus for producing metallic iron from iron oxide fines
WO2019032554A1 (fr) 2017-08-08 2019-02-14 H Quest Vanguard, Inc. Conversion non thermique par plasma d'hydrocarbures
EP3878807A1 (fr) * 2020-03-13 2021-09-15 Clariant International Ltd Procédé de production de gaz de synthèse par gazéification allothermique à réduction de dioxyde de carbone contrôlée

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TOBIAS GÜNTER GEISSLER, METHANPYROLYSE IN EINEM FLÜSSIGMETALL-BLASENSÄULENREAKTOR (VERFAHRENSTECHNIK, ISBN: 10: 3843933448

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