Apparatus and method for producing hydrogen and solid carbon from C1- to C4-alkane-containing gas

Abstract

The present invention relates to an apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, a method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, and an application of the apparatus for use in a method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using the method of the present invention.

Description

Technology Field

[0001] The present invention relates to an apparatus, a method, and an application of the apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using a thermal plasma that uses at least one reactor that generates a thermal plasma using an electric arc. Background Technology

[0002] There is increasing demand for the production of clean and storable energy sources with a reduced CO2 footprint during production and consumption processes. However, these energy sources will ultimately penetrate the market only if production-related costs are sufficiently low. This is particularly true for energy sources in the mobility, heat production, chemical, steel, and oil refining sectors.

[0003] The use of hydrogen for direct combustion, for use in fuel cells, or to produce synthetic fuels such as methanol, dimethyl ether, synthetic natural gas, synthetic gasoline, synthetic diesel, or synthetic kerosene using carbon dioxide (CO2) as a carbon source, for example, has been investigated for some time. Typically, hydrogen is produced from coal or from liquid / gaseous hydrocarbons through gasification or reforming reactions. These conversions occur at high temperatures and entail significant CO2 emissions during the reaction process and in the process of generating the heat required to drive these reactions.

[0004] Several routes have been investigated and are currently under development for hydrogen production that emits only low or reduced amounts of CO2. For example, one option is to capture CO2 from the exhaust gases of a conventional hydrogen production plant and then compress and sequester the CO2. Logistics costs can be enormous, especially if the hydrogen production site is far from the sequestering site. Another option is, for example, electrolysis, which decomposes water into oxygen and hydrogen. Here, a large amount of energy (electric current) is required to drive the reaction (water decomposition, see reaction (1)) in the electrolysis method. Here, standard molar enthalpies for various reactions are given, based on 298 K unless otherwise specified.

[0005]

[0006] Since electrolysis requires a significant amount of electrical energy, total CO2 emissions are closely related to the CO2 emissions associated with the production of the consumed electricity. Today, in many parts of the world, the penetration of renewable power generation is insufficient, so the average CO2 emissions from power production are too high to make electrolysis ecologically meaningful within grid mix electricity. On the other hand, if electrolysis is performed solely or primarily with renewable electricity, the corresponding annual full load hours will frequently be too low to enable economic operation.

[0007] Since the bond energy of hydrogen-carbon bonds in hydrocarbons such as methane is significantly lower than that of hydrogen-oxygen bonds in water, the specific separation energy requirement for said hydrocarbons is correspondingly lower. Therefore, theoretically, it is possible to produce hydrogen with less energy than the electrolysis method by separating hydrocarbons into hydrogen and carbon.

[0008] Various technologies are being investigated and developed to take advantage of these benefits. For example, WO2013 / 004398 A2 (Linde and BASF) describes a method for separating hydrocarbons in the presence of carbon-rich granules forming a moving bed. The heat required to bring about said separation is provided by the combustion of a fuel containing said hydrocarbons and some of said hydrogen. A disadvantage of this technology is that it requires a significantly high specific expenditure, particularly on a small scale.

[0009] Another plasma-based partial hydrocarbon splitting process, though one that is often overlooked when high hydrogen yields and pure carbon production are required, is plasma-based acetylene (C2H2) production starting from C1- to C4-alkanes, such as methane (CH4), or hydrocarbons with much higher molecular weights. Acetylene is a highly valuable compound because it can serve as a feedstock in some chemical syntheses. Although hydrogen is produced as a byproduct during the process, some of the hydrogen from the feedstock remains in the target product, acetylene (see Chemical Formula (2), which illustrates methane conversion as an example of hydrocarbon conversion).

[0010]

[0011] One example of such a method is the commercially implemented "Huels arc process." In this process, after a one-step conversion of low molecular weight hydrocarbons (e.g., methane) to acetylene using an electric arc, a so-called quenching step is performed to stabilize the highly reactive acetylene by extremely rapidly cooling the hydrocarbon-derived plasmaeous plasma gas; optionally, this is performed in two steps using various fluids. This prevents the formation of derivatives, such as high molecular weight hydrocarbon compounds, from acetylene (see Acetylene, Paessler et al., Ullmann's Encyclopedia of Industrial Chemistry, doi:10.1002 / 14356007.a01_097.pub4, 2011). Given the extensive hydrogen production, its application may be limited due to the need to find sufficient demand for acetylene. This complicates the commercialization of the above process and may limit its hydrogen production potential.

[0012] Another recent example of an electric arc-based method for the incomplete separation of hydrocarbons is described in WO2015 / 140058 A1 (BASF). In this method, a methane-containing gas is converted into acetylene using an electric arc. Immediately thereafter, to increase the acetylene yield, the acetylene-containing mixture is rapidly cooled (quenched) with additional methane-containing gas. Subsequently, the acetylene is mixed with another hydrocarbon-containing feedstock and maintained at a lower temperature so that one or more hydrogen- and carbon-containing products having a boiling point of 15°C or higher can be obtained through reaction with the additional feedstock. The reactor described herein has three to four different sections of a predetermined length. In each section, a gaseous medium or a liquid medium is introduced through at least one inlet for the respective medium. Thus, the method of WO2015 / 140058 A1 ensures the formation of one or more hydrogen- and carbon-containing organic compounds having a boiling point of 15°C or higher. The inventors have found that neither the reactor nor the method described herein enables an energy-efficient and cost-effective method of producing hydrogen and solid carbon from C1- to C4-alkane-containing gases, while producing said hydrogen in high yield. Furthermore, the method presents the need to find applications for the chemicals produced along with the hydrogen, which can limit the hydrogen production potential by complicating the commercialization of the method.

[0013] One junction method for the production of hydrogen and solid carbon by plasma-based hydrocarbon separation is described in the document WO93 / 12030 A1 (Kvaener). In this case, interlocked tubular electrodes are mounted in a concentric arrangement in a massive reactor. An electric arc is set at the electrode ends facing the reactor volume to generate a plasma gas from hydrogen, which is then mixed with methane in the second stage. This process is specifically designed to obtain carbon particles having specific characteristics, such as particle size and shape. The inventors have found that this two-stage process for hydrogen production is inefficient and costly overall because it requires a large reactor volume and results in separate reactor zones for process conditions, such as temperature and gas composition.

[0014] An alternative method for producing hydrogen from plasma-based hydrocarbon separation is described in WO01 / 46067 A1 (Bechtel). The key to this process is the use of a laval-type nozzle in the reactor. Similar to WO2015 / 140058 A1, methane is converted to acetylene using an electric arc that generates a plasma gas from hydrogen or an inert gas. Acetylene is produced by feeding methane into the plasma gas. Subsequently, the mixture is delivered downstream through the nozzle. Due to specific gas dynamics, the nozzle induces a relatively high pressure drop of the gas exiting downstream of the nozzle. At the same time, the average temperature is significantly lowered. WO01 / 46067 A1 emphasizes that the described process and reactor parameters, such as the location of the feed inlets and the diameter of the reactor chamber, are critical in achieving the desired gas expansion and separating hydrocarbons into the target products, hydrogen and carbon. Therefore, sensible heat from the upstream high-temperature process gas of the nozzle is not significantly utilized to achieve high efficiency in the separation process. Furthermore, high pressure drop is generally undesirable because most hydrogen downstream processes or logistics require correspondingly greater recompression. Overall, the process features a very specific design requiring controlled process conditions and high specific energy costs, which is disadvantageous in light of the requirement for energy-efficient processes to be provided for hydrogen and solid carbon production.

[0015] Therefore, the aforementioned processes have limitations in relation to the goal of producing hydrogen and solid carbon in an economical, clean, environmentally friendly, and energy-efficient manner. In particular, these processes have high investment and operating costs, and / or low energy efficiency.

[0016] The present invention relates to an apparatus, a method, and a use of said apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using a thermal plasma as defined in the appended claims.

[0017] More specifically, in the first aspect, the present invention relates to an apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the apparatus comprises at least one reactor that generates thermal plasma using an electric arc, and wherein the reactor comprises a plasma section and a second reactor section.

[0018] i) The above plasma section is,

[0019] · An anode and a cathode for generating an electric arc - said arc extends within said plasma section -, and

[0020] · At least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor

[0021] Includes,

[0022] · The anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface—an outlet in the flow direction of the main stream of the plasma gas—the outlet forms an open end of the anode in the flow direction of the main stream—and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing opposite the flow direction of the main stream—and the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing opposite the flow direction of the main stream and the open end of the anode in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and

[0023] · The anode and the cathode are arranged so that a plasmaeous plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode, and

[0024] ii) The second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream, the second reactor section,

[0025] · A first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and

[0026] · Outlet means for recovering components from the reactor above - said outlet means are located at the end of the second reactor section in the direction of flow of the main stream -

[0027] Includes,

[0028] · The first subsection includes at least one second supply line for introducing a C1- to C4-alkane-containing gas into the second reactor section, and

[0029] · The at least one second supply line is arranged so that the C1- to C4-alkane-containing gas introduced into the reactor through the at least one second supply line is introduced into the plasma-like plasma gas at a downstream location of the foot points of the electric arc in the flow direction of the main stream, thereby allowing a mixture to be formed from the plasma-like plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line in the first subsection of the second reactor section downstream of the at least one second supply line.

[0030] · The location of the at least one second supply line along the flow direction of the main stream defines the beginning of the second reactor section and its first subsection, and

[0031] · The volume of the plasma section from the uppermost upstream position, where the inner surface of the hollow channel of the anode faces the electric arc, to the end of the plasma section of the reactor is 0.0001 to 0.4 m3 The range of, preferably 0.001 to 0.2 m 3 It is a volume within the range, defines a reference volume, and

[0032] · The volume of the first subsection of the second reactor section is in the range of 10 to 200 times the reference volume, preferably in the range of 20 to 100 times the reference volume, and

[0033] · The total volume of the second reactor section is in the range of 20 to 2000 times the reference volume, preferably in the range of 40 to 1000 times the reference volume, and

[0034] · The reactor comprises, at least at one point within the first subsection of the second reactor section and / or within the plasma section, a flow cross-section across the main stream flow direction that is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the main stream flow direction in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode, wherein if included within the plasma section, it is included within the region of the end of the plasma section as downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the main stream flow direction.

[0035] In a second aspect, the present invention relates to a method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, characterized by comprising the following steps.

[0036] a) a step of extracting C1- to C4-alkane-containing plasma gas from a C1- to C4-alkane-containing gas supply device;

[0037] b) a step of introducing the C1- to C4-alkane-containing plasma gas extracted from the device for extracting the C1- to C4-alkane-containing plasma gas into at least a first reactor;

[0038] Here, the reactor is a reactor that generates thermal plasma using an electric arc, and the reactor includes a plasma section and a second reactor section, and

[0039] i) The above plasma section is,

[0040] · An anode and a cathode for generating an electric arc - said arc extends within said plasma section -, and

[0041] · At least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor

[0042] Includes,

[0043] · The anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface—, an outlet in the flow direction of the main stream of the plasma gas—the outlet forms an open end of the anode in the flow direction of the main stream—, and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing in the opposite direction of the flow direction of the main stream—the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing in the opposite direction of the flow direction of the main stream and the open end of the anode in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and

[0044] · The anode and the cathode are arranged so that a plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode, and

[0045] ii) The second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream, the second reactor section,

[0046] · A first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and

[0047] · Means for an outlet for recovering components from the reactor above - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream -

[0048] Includes,

[0049] · The first subsection comprises at least one second supply line for introducing a C1- to C4-alkane-containing gas into the second reactor section, and the location of the at least one second supply line along the flow direction of the main stream defines the inlet of the second reactor section and its first subsection, and

[0050] The C1- to C4-alkane-containing plasma gas is introduced into the reactor through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section of the reactor;

[0051] c) a step of generating an electric arc that expands within the plasma section of the reactor to the anode and cathode;

[0052] d) a step of forming a plasma gas from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section using the electric arc in the plasma section of the reactor;

[0053] e) introducing a C1- to C4-alkane-containing gas into the first subsection of the second reactor section through the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section, wherein

[0054] · The C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line is introduced into the plasma gas downstream of the foot points of the electric arc generated by the anode and cathode in the direction of flow of the main stream, so that a mixture can be formed in the first subsection of the second reactor section downstream of the at least one second supply line from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line.

[0055] · At the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas has an average temperature in the range of 1200 to 3000 ℃ and contains acetylene, so that the mixture formed by the introduction of the C1- to C4-alkane-containing gas into the plasma gas through the at least one second supply line has an average temperature of 850 ℃ or higher, preferably 1050 ℃ or higher, and less than 3000 ℃ in the region range from the at least one second supply line to the end of the first subsection of the second reactor section;

[0056] f) a step of moving the mixture downstream in the direction of flow of the main stream through the second reactor section, wherein

[0057] · The movement is carried out such that the average residence time of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the first subsection of the second reactor section is in the range of 100 ms to 2000 ms, preferably in the range of 200 ms to 1000 ms, and

[0058] · The movement is carried out such that the average residence time of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the entire second reactor section is in the range of 200 ms to 20,000 ms, preferably in the range of 400 ms to 10,000 ms, and

[0059] At least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and preferably, at least 10% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line There is a deviation of 10% or more, and more preferably, a deviation of 15% or more, even more preferably 20% or more from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and

[0060] · Hydrogen and solid carbon are produced by reactions occurring in the mixture within the second reactor section and, preferably, in the plasma section;

[0061] g) a step of controlling the average temperature of the mixture within the second subsection of the second reactor section to 650°C or higher, preferably 750°C or higher, more preferably 850°C or higher, and less than 1500°C - wherein the average temperature at the end of the second reactor section of the mixture of the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line is controlled to an average temperature of 200K or higher, preferably 400K or higher, more preferably 600K or higher, but lower than the average temperature of the plasma gas at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line -; and

[0062] h) A step of recovering the mixture at the end of the reactor through an outlet means for recovering the mixture from the reactor - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream -.

[0063] In a third aspect, the present invention relates to the use of an apparatus for use in the method of the present invention for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the apparatus comprises at least one reactor that generates thermal plasma using an electric arc, and said reactor comprises a plasma section and a second reactor section.

[0064] i) The above plasma section is,

[0065] · An anode and a cathode for generating an electric arc - said arc extends within said plasma section -, and

[0066] · At least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor

[0067] Includes,

[0068] · The anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface—an outlet in the flow direction of the main stream of the plasma gas—the outlet forms an open end of the anode in the flow direction of the main stream—and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing opposite the flow direction of the main stream—and the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing opposite the flow direction of the main stream and the open end of the anode in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and

[0069] · The anode and the cathode are arranged so that a plasmaeous plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode, and

[0070] ii) The second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream, the second reactor section,

[0071] · A first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and

[0072] · Outlet means for recovering components from the reactor above - said outlet means are located at the end of the second reactor section in the direction of flow of the main stream -

[0073] Includes,

[0074] · The first subsection includes at least one second supply line for introducing a C1- to C4-alkane-containing gas into the second reactor section, and

[0075] · The at least one second supply line is arranged so that the C1- to C4-alkane-containing gas introduced into the reactor through the at least one second supply line is introduced into the plasma-like plasma gas at a downstream location of the foot points of the electric arc in the flow direction of the main stream, thereby allowing a mixture to be formed from the plasma-like plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line in the first subsection of the second reactor section downstream of the at least one second supply line.

[0076] · The location of the at least one second supply line along the flow direction of the main stream defines the beginning of the second reactor section and its first subsection, and

[0077] · The volume of the plasma section from the uppermost upstream position, where the inner surface of the hollow channel of the anode faces the electric arc, to the end of the plasma section of the reactor is 0.0001 to 0.4 m 3 The range of, preferably 0.001 to 0.2 m 3 It is a volume within the range, defines a reference volume, and

[0078] · The volume of the first subsection of the second reactor section is in the range of 10 to 200 times the reference volume, preferably in the range of 20 to 100 times the reference volume, and

[0079] · The total volume of the second reactor section is in the range of 20 to 2000 times the reference volume, preferably in the range of 40 to 1000 times the reference volume, and

[0080] · The reactor comprises, at least at one point within the first subsection of the second reactor section and / or within the plasma section, a flow cross-section across the main stream flow direction that is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the main stream flow direction in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode, wherein if included within the plasma section, it is included within the region of the end of the plasma section as downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the main stream flow direction. Brief explanation of the drawing

[0081] FIG. 1 shows an embodiment of the apparatus (10) of the present invention, which is suitable for use in the method according to the present invention as an apparatus for producing hydrogen and solid carbon from C1- to C4-alkane-containing gases. The method of the present invention can be implemented using this apparatus. FIG. 2 shows another embodiment of the apparatus (10) of the present invention, which is suitable for use in the method according to the present invention as an apparatus for producing hydrogen and solid carbon from C1- to C4-alkane-containing gases. The method of the present invention can be implemented using this apparatus. Here, the most upstream point, which is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream (71) in the range of foot points of the electric arc on the inner surface of the hollow channel of the anode, is located upstream of the first subsection of the second reactor section in the flow direction of the main stream. Specific details for implementing the invention

[0082] Together with the accompanying drawings, the detailed description of the present invention describes the technical content of the present invention according to preferred embodiments, which are not intended to limit the scope of the present invention. Any equivalent modifications and variations made according to the appended claims fall within the scope of the claims of the present invention.

[0083] As outlined above, the present invention relates to three aspects for the production of hydrogen and solid carbon, namely, an apparatus, a method, and a use of the apparatus. With respect to these three aspects, the disclosures set forth in this application are interchangeably applicable and disclosed herein.

[0084] Surprisingly, it has been found that when using conventional devices and processes, a significant portion of the hydrocarbons undergo uninhibited formation of acetylene or other highly unsaturated compounds, or the process parameters required to operate the process cause inefficient operation due to low space-time yield or large pressure drop, or the molecular hydrogen yield is reduced due to the formation of hydrogen-containing high molecular weight components such as high molecular weight hydrocarbons.

[0085] Acetylene can react with benzene (C6H6) and highly aromatic compounds. These compounds can cause tar formation, which can be deposited on the walls of the reactor or subsequent equipment (e.g., heat exchangers). It has been found that conventional hydrogen production equipment does not adequately control the conversion of acetylene into carbon and hydrogen, for example, by controlling concentration, residence time, and temperature along the path through the reactor. This results in the formation of corresponding hydrogen-containing byproducts, the deposition of higher molecular compounds, and inevitable interruptions in process operations for equipment cleaning. The present invention prevents this, reduces the amount of hydrocarbon byproducts in the resulting mixture, and facilitates the continuous production of hydrogen and solid carbon.

[0086] In other words, the inventors of the present invention have surprisingly discovered that hydrogen can be produced from C1- to C4-alkane-containing gases at a target yield more efficiently, particularly at lower specific energy expenses and lower capital expenditures, through specific modifications to the apparatus of the prior art, in particular to a thermal plasma reactor in which thermal plasma is generated by an electric arc, and through specific modifications to the process of the prior art. In particular, by controlling the trends of concentration, average residence time, residence time distribution, and average temperature ranges along the flow path of the main stream passing through the reactor, the generation of undesirable byproducts can be reduced and the conversion of the feedstock can be increased to a high space-time yield. This is partly because the acetylene generated in the plasma gas is diluted by the C1- to C4-alkane-containing gas introduced into the plasma gas in the first subsection of the second reactor section. This applies equally to the apparatus of the present invention, which ensures a proper mixing of the feedstocks, a specified residence time distribution of the atoms of the reaction components, and a specified average residence time. The inventors have discovered that hydrogen and solid carbon, particularly carbon black, can be efficiently produced through specific modifications to the apparatus and process of the prior art for acetylene production. Accordingly, the present invention enables the implementation of a commercially attractive process for producing hydrogen and carbon. This addresses the long-standing demand for energy-efficient, economical, and environmentally friendly hydrogen production without the aforementioned problems and limitations. Furthermore, the byproduct carbon black is used in many industrial sectors, for example, the printing industry, and can therefore be commercialized. Additionally, undesirable byproducts in the resulting product gas mixture are largely excluded.

[0087] The component according to the present invention may be in a gaseous, liquid, or solid state at 273.15 K and 1.01325 bar, unless otherwise specified herein. The component may be an atom, a molecule, an oligomer, a polymer, a radical, or an ion. Radicals and ions are specific species of the corresponding atom.

[0088] The device of the present invention comprises at least one reactor. Accordingly, the device may comprise only one reactor. Alternatively, the device of the present invention may comprise two or more reactors. These may be operated in parallel. Operating two or more reactors in parallel is advantageous in that it provides improved flowability. For example, if one reactor is subject to maintenance, the other reactor(s) can continue operations. Thus, this prevents the entire plant from shutting down. Additionally, two or more reactors installed in parallel increase the range of loads that can operate a single plant. This can be beneficial, for example, when grid services such as control power need to be provided by operating the plant with flexible loads.

[0089] Herein, the term "at least one" means 1, 2, 3, 4, 5, and a number greater than or equal to these. In some embodiments, "at least one" means one. In other embodiments, "at least one" means two or more.

[0090] The terms "in the range of" or "in the range from" refer to a range. According to the present invention, endpoints of a specified area are considered to be part of the range unless otherwise specified.

[0091] FIGS. 1 and 2 illustrate reactors having a vertical orientation, but reactors having a horizontal orientation or any other orientation are also included.

[0092] The term "reactor" as used in the present invention refers to a chemical reactor. The reactor comprises a reactor space where a chemical reaction takes place. It may be introduced into or recovered from the reactor space through an inlet and an outlet. Here, the reactor is a sealed vessel suitable for carrying out the method for producing hydrogen and solid carbon according to the present invention based on a thermal plasma process, wherein the thermal plasma is generated by an electric arc. A general example of a reactor is the so-called Huels reactor (see Acetylene, Paessler et al., Ullmann's Encyclopedia of Industrial Chemistry, doi:10.1002 / 14356007.a01_097.pub4, 2011). This reactor is used for the production of acetylene. The apparatus of the present invention comprises an electric arc reactor having special features different from those of a Huels reactor, said special features being advantageous for implementing the method of the claim. The apparatus of the claim including said electric arc reactor may be used to carry out the method of the claim.

[0093] The term "plasmaeous plasma gas" used in this invention refers to a gas existing in a plasma state. Gases that are introduced into, are introduced into, or are scheduled to be processed within a reactor for generating thermal plasma using an electric arc, but do not exist in a plasma state or are not yet in a plasma state, are not included in the definition of plasmaeous plasma gas. Likewise, gases that exist in the reactor for generating thermal plasma using an electric arc but do not exist in a plasma state or no longer exist in a plasma state are not included in the definition of plasmaeous plasma gas.

[0094] According to A. Fridman (Plasma Chemistry, Cambridge University Press, 2009), a gas existing in a plasma state is generally defined as an ionized gas, that is, a gas containing at least one electron that is not bound to atoms or molecules and converts said atoms or molecules into positively charged ions. Preferably, a gas existing in a plasma state contains electrically charged particles, in an amount sufficient to influence the electrical properties and behavior of the gas and alter them relative to a standard gaseous state. An example of an electrical property is electrical conductivity. Electrical conductivity increases when the gas is in a plasma state, particularly when the plasma state is adopted at an elevated temperature. Conceptually, the relationship between electrical conductivity, the plasma state, and gas temperature can be explained as follows: It is known that the degree of ionization increases with increasing temperature (e.g., shown in the tabulated data regarding hydrogen, nitrogen, oxygen, air, and selected inert gases in MI Boulos, *Thermal Plasmas, Fundamentals and Applications, Vol. 1, 1994*). Due to the enhanced mobility of opposite charges, an increase in the degree of ionization is accompanied by an increase in electrical conductivity.

[0095] Furthermore, in aspect of the present invention, the plasma gas is preferably characterized in that the electrical conductivity of each plasma gas at a predetermined density is at least one order of magnitude greater than the electrical conductivity of a corresponding gas at room temperature and the same density, preferably at least two orders of magnitude greater, and more preferably at least four orders of magnitude greater.

[0096] A non-plasma state gas at room temperature (i.e., without external electrical or other stimuli) is 10 -22While having an electrical conductivity of less than S / m, the plasma state gas according to the present invention is 10 -21 S / m or more, preferably 10 -20 S / m or more, more preferably 10 -18 It is characterized by electrical conductivity of S / m or higher.

[0097] In this regard, those skilled in the art can measure the electrical conductivity of a gas by a technique similar to the flame ionization detection method.

[0098] It is preferable to generate a gas existing in a plasma state by using electrical energy, for example, by applying a strong electromagnetic field to the gas (for example, an electromagnetic field generated around an electric arc).

[0099] Plasma gas, that is, gas existing in a plasma state, can be encountered at least at one point in the flow cross-section crossing the flow direction of the main stream within the reactor.

[0100] C1- to C4-alkane-containing gas means a gas comprising methane, ethane, propane, butane, 2-methylpropane, or a mixture thereof. The sum of the C1- to C4-alkane(s) in the gas is 10 vol.% or more, preferably 25 vol.% or more, more preferably 50 vol.% or more, even more preferably 75 vol.% or more, and even more preferably 90 vol.% or more. In some embodiments, the C1- to C4-alkane-containing gas is natural gas. In some embodiments, the C1- to C4-alkane-containing gas contains methane and / or propane. This is advantageous in that both gases can be obtained in large quantities, for example, methane can be obtained from natural gas and propane can be obtained from the production of hydrogenated vegetable oils. Most preferably, the C1- to C4-alkane-containing gas is natural gas or methane-containing gas. This means that natural gas can be used as either a gas containing methane or another gas containing methane. Most preferably, the C1- to C4-alkane-containing gas contains methane, in particular 25 vol.% or more methane, more preferably 50 vol.% or more methane, even more preferably 75 vol.% or more methane, most preferably 90 vol.% or more methane. This applies equally to the C1- to C4-alkane-containing plasma gas and equally to the use of the method and reactor of the present invention. In some embodiments, the C1- to C4-alkane-containing gas introduced into the plasma section through at least one first supply line and the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through at least one second supply line are withdrawn from the same C1- to C4-alkane-containing gas supply device. Preferably, both are withdrawn from the same natural gas supply device.Accordingly, the apparatus of the present invention may include C1- to C4-alkane-containing gas sources connected to the at least one first supply line and the at least one second supply line. Preferably, both supply lines are connected to the same C1- to C4-alkane-containing gas supply device. More preferably, the gas supply device comprises natural gas. Nevertheless, the gas from the gas supply device may be further mixed with another component, for example, a hydrocarbon, before being introduced into the reactor, for example, with an acetylene-containing gas or a hydrogen-containing gas. In relation to the apparatus of the present invention, this means that the at least one first supply line and / or the at least one second supply line may be connected to another supply line for introducing an additional component into the gas from the gas supply device.

[0101] The term "at least one first supply line" means one, two, three, four, five, or more first supply lines. In some embodiments, the at least one first supply line is a single first supply line. In other embodiments, the at least one first supply line means two or more first supply lines.

[0102] The term "at least one second supply line" means one, two, three, four, five, or more second supply lines. In some embodiments, the at least one second supply line is one second supply line. In other embodiments, the at least one second supply line means two or more second supply lines.

[0103] The term "at least one third supply line" means one, two, three, four, five, or more third supply lines. In some embodiments, at least one third supply line is one second supply line. In other embodiments, at least one third supply line means two or more third supply lines.

[0104] In addition to the above at least one third supply line, the apparatus, method, and use of the present invention may include a reactor having at least one fourth supply line downstream of the at least one third supply line in the direction of flow of the main stream.

[0105] C1- to C4-alkane-containing gases are higher boiling point components, e.g., C5-alkanes, olefins, aromatic compounds such as benzene, and mixtures thereof, or even components containing small amounts of oxygen (e.g., C 12 H 24 Mixtures with long-chain aldehydes such as O may also be included. For example, C1- to C4-alkane-containing gases may contain higher boiling point components in the range of 0.1 to 50 vol.%, preferably in the range of 0.5 to 30 vol.%, and more preferably in the range of 1 to 10 vol.%. Depending on the selected feedstock, design parameters and operating parameters may need to be adjusted.

[0106] In some embodiments, the C1- to C4-alkane-containing gas comprises less than 5 vol.% O2, preferably less than 2 vol.% O2, most preferably less than 1 vol.% O2, less than 10 vol.% CO, preferably less than 5 vol.% CO, most preferably less than 2.5 vol.% CO, less than 10 vol.% CO2, preferably less than 5 vol.% CO2, most preferably less than 2.5 vol.% CO2, and / or less than 10 vol.% N2, preferably less than 5 vol.% N2, most preferably less than 1 vol.% N2. Such and the above-described definitions for the C1- to C4-alkane-containing gas apply to both the plasma gas and the gas introduced into the reactor through the at least one second supply line. One embodiment also applies to the use of the method and apparatus of the present invention.

[0107] Most of the devices and processes of the prior art involve the use of a plasma gas or, as the main component of said plasma gas, hydrogen, nitrogen, or an inert gas, such as helium (He), neon (Ne), argon (Ar), krypton (Kr), or xenon (Xe), or a mixture of hydrogen, nitrogen, and / or inert gas. However, the inventors of the present invention have discovered that using hydrogen (H2), nitrogen, or an inert gas as the plasma gas results in a much higher specific energy requirement than that of the present invention. Furthermore, it requires significant effort to separate the produced hydrogen from the untreated byproduct gas.

[0108] Nevertheless, in some embodiments of the present invention, the C1- to C4-alkane-containing gas comprises H2 in an amount from 0.1 vol.% to 25 vol.%, preferably from 0.5 vol.% to 15 vol.%, and more preferably from 1 vol.% to 5 vol.%. In particular, the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line may comprise H2 in an amount from 0.1 vol.% to 25 vol.%, preferably from 0.5 vol.% to 15 vol.%, and more preferably from 1 vol.% to 5 vol.%. The C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line may contain H2 in an amount from 0.1 vol.% to 25 vol.%, preferably from 0.5 vol.% to 15 vol.%, more preferably from 1 vol.% to 5 vol.%. The C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line may contain acetylene in an amount from 0.1 vol.% to 10 vol.%, preferably from 0.5 vol.% to 7 vol.%, more preferably from 1 vol.% to 5 vol.%.

[0109] The following main target reaction [see Reaction Scheme (2), to be revisited later] and main side reaction [see Reaction Scheme (3)] take place in a plasma section using a plasma gas containing C1- to C4-alkanes:

[0110] Target Response:

[0111]

[0112] Major side reaction (endothermic):

[0113]

[0114] As indicated by the positive enthalpy difference, a significant amount of energy is required to operate hydrogen production. The inventors have, surprisingly, found that the apparatus, method, and use of the claim are advantageous in that they can reduce the formation of undesirable high molecular weight hydrocarbons, such as tars, by inducing the exothermic acetylene decomposition reaction (4) in a controlled manner in the second reactor section. At the same time, this reaction increases absolute hydrogen and solid carbon yield and lowers overall specific electric energy expenses by enabling the additional addition and separation of C1- to C4-alkane-containing feedstocks. The energy required to separate more C1- to C4-alkane-containing gases into hydrogen and solid carbon can be provided by the decomposition of acetylene. Thus, it is possible to increase the capacity of the plasma reactor and reduce the total specific electricity demand required for the separation of C1- to C4-alkane-containing gases.

[0115] Main exothermic reaction:

[0116]

[0117] Generally, the pathway of a continuous acetylene reaction is complex. For example, it is known that acetylene undergoes combination to form benzene, from which higher aromatics and tar are formed. The latter can cause undesirable deposition on the reactor walls and may necessitate suspending process operations for reactor cleaning. The additional addition of C1- to C4-alkane-containing gases in the reaction pathway under the boundary conditions disclosed in this invention results, first, in a controlled reduction of the average temperature of the plasma gas, thereby reducing reactivity, and second, in the dilution of acetylene. Both of these are intended to suppress the aforementioned undesirable tar formation and prevent undesirable continuous reactions of acetylene. The inventors have discovered that the heat of acetylene decomposition can be used to separate additional C1- to C4-alkanes contained in the feedstock into hydrogen and carbon black. Accordingly, the reactor, the use, and the method are designed such that the oligomerization of acetylene in the second reactor section is reduced and rather the acetylene is made as unstable as possible, while the decomposition of acetylene reliably leads to the conversion of the injected C1- to C4-alkanes into hydrogen and carbon black. Surprisingly, it was found that this is ensured, for example, by the average residence time and average temperature profile of the claim, as well as by the residence time distribution. This is also established by the design of a special apparatus. The average residence time and residence time distribution defined herein relate to the atoms of the mixture. Thus, they relate only to the atoms of the plasma gas and the C1- to C4-alkane-containing gas injected through the at least one second supply line.

[0118] For a substance flowing through a volume, the residence time of a single atom is a measure of how long the atom spends within it. A single atom, including atoms contained in molecules, oligomers, polymers, or particles, has a single residence time; however, a mixture of multiple atoms, including atoms contained in molecules or particles, has a residence time distribution (RTD) because individual flow paths and velocities may generally differ. Accordingly, the present invention refers to an average residence time to define the average residence time of all atoms of the mixture passing through a second reactor section. The average residence time and residence time distribution can be measured, for example, by introducing a non-reactive tracer into the reactor at the inlet.

[0119] Importantly, the inventors have surprisingly discovered that it is advantageous to avoid the stabilization of acetylene, which is a key element in the processes of the invention. In other words, the inventors have discovered that it is advantageous to omit extensive quenching of the mixture in the reactor, as this is intended to stabilize the acetylene. Accordingly, the apparatus, method, and use of the present invention avoid such measures.

[0120] Accordingly, the energy required to separate C1- to C4-alkane-containing gases into hydrogen and solid carbon (e.g., carbon black) is partially provided by the decomposition of acetylene due to specific features of the apparatus, method, and use of the claim. Thus, it is possible to increase the capacity of the plasma reactor and reduce the specific power requirement for the separation of C1- to C4-alkane-containing gases.

[0121] The device of the present invention may be an industrial plant, a distributed small-scale plant, a laboratory-scale facility, or a pilot plant for the production of hydrogen and solid carbon. The device may include one or more reactors for generating thermal plasma using an electric arc. Accordingly, the device may include multiple reactors operating in parallel or alternately.

[0122] The term average temperature used here refers to the average temperature across the region traversing the flow direction of the main stream, where the local temperature is weighted by the corresponding mass flow and average heat capacity.

[0123] The conditions and process parameters defined and mentioned herein should be understood as relating to the steady state of the reactor, unless otherwise explicitly specified.

[0124] The term "mixture" as used herein refers to a mixture of components obtained by mixing a plasma gas exiting a plasma section with a C1- to C4-alkane-containing gas introduced into the plasma gas in a first subsection of a second reactor section through at least one second supply line. The composition of the mixture may vary as the components react while passing through the second reactor section and any subsequent devices. The components of the mixture may be in a gaseous, liquid, and / or solid state.

[0125] The reactor comprises a plasma section and a second reactor section located downstream immediately after the plasma section of the reactor in the direction of the main stream flow. The plasma section is part of the reactor. A C1- to C4-alkane-containing plasma gas is introduced into the plasma section through at least one first supply line. The plasma section further comprises an anode and a cathode that generate an electric arc extending within the plasma section. To form a plasma-like plasma gas within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line, the electric arc heats the plasma gas. This causes reactions of the components of the plasma gas, including the formation of ions and radicals, due to the high temperature. Thus, the plasma-like plasma gas is rich in ionized particles and / or radicals derived from the C1- to C4-alkane-containing plasma gas.

[0126] The anode has a hollow channel along the flow direction of the main stream of the plasma gas, an outlet in the flow direction of the main stream of the plasma gas, and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through the at least one first supply line, wherein the hollow channel has an inner surface, the outlet forms an open end of the anode in the flow direction of the main stream, and the inlet forms an open end of the anode facing in the opposite direction of the flow direction of the main stream. The anode is configured so that the plasma gas can flow along the hollow channel through the open end of the anode facing in the opposite direction of the flow direction of the main stream and the open end of the anode facing in the flow direction of the main stream, and the plasma gas comes into contact with the inner surface of the hollow channel of the anode when passing through the anode. The foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode. Preferably, the anode has a cylindrical shape having a coaxial hollow channel.

[0127] In some embodiments, the corresponding anode and cathode do not overlap at least partially in the direction of flow of the main stream. Thus, the anode and cathode are not nested. This is illustrated in FIGS. 1 and 2.

[0128] The expression "the anode and cathode do not overlap at least partially" used in this invention means that the anode and cathode are separated from each other in the main flow direction.

[0129] In preferred embodiments, the anode and / or cathode are cooling electrodes that are preferably cooled by liquid cooling, more preferably by water cooling. This reduces corrosion of the electrodes and ensures that the electrodes operate continuously for a long time. In other embodiments, the anode and / or cathode are formed from a material containing less than 10 wt.% graphite or other solid carbon material. Reactors containing graphite-based or solid carbon-based electrodes are generally more expensive and exhibit a higher degradation rate than metal-based electrodes. Therefore, in preferred embodiments, the anode and cathode of the reactor are metal electrodes.

[0130] In additional embodiments, the anode and cathode are concentric, and the cathode also has a hollow channel having a main axis extending along the flow direction of the main stream, the hollow channel having two opposite ends, the end facing opposite the flow direction of the main stream being closed, and the end facing the flow direction of the main stream being open. Preferably, this open end facing the flow direction of the main stream of the plasma gas is located upstream of the open end of the anode facing opposite the flow direction of the main stream and is concentric with the open end of the anode. With respect to the end of the hollow channel of the cathode facing the direction of flow of the main stream, the term "closed" means that the end of the channel is completely closed or that the flow cross-section across the direction of flow of the main stream is reduced by more than 90% based on the area of ​​the flow cross-section of the cathode across the direction of flow of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the cathode.

[0131] In these embodiments, the anode and the cathode are arranged such that the foot points of the electric arc contact the inner surface of the cathode and the inner surface of the anode, respectively. In preferred embodiments, the anode and the cathode are arranged such that a gap exists in the direction of the main stream between the end of the cathode facing the direction of the main stream flow and the end of the anode facing the opposite direction of the main stream flow. The length of the gap is preferably at least 0.3 times, more preferably at least 0.5 times, the average inner diameter of the hollow channel of the anode within the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode. In some embodiments, the at least one first supply line is arranged so that the plasma gas can be introduced into the plasma section of the reactor through the gap between the anode and the cathode.

[0132] The shape and location of the foot points of the electric arc on the cathode and / or anode change over time during operation, changing not only during ramp-up, shutdown, and load changes but also during steady-state operation. In particular, in the case of an anode having a hollow channel where the foot points of the electric arc are located on the inner surface of the hollow channel of the anode, the location of the foot points may change along the circumference of the anode over time, even during steady-state operation, as well as change upward and downward in the direction of the main stream flow within at least a limited range. The range of the location of the foot points on the inner surface of the hollow channel of the anode in the direction of the main stream flow generally depends on the current mode of operation. For example, if all other process parameters are kept constant, an increase in the electric load causes the electric arc to lengthen, shifting the positional range of the foot points on the inner surface of the hollow channel of the anode to a region further downstream from the direction of the main stream flow on the surface of the hollow channel of the anode. In the context of the present invention, with respect to the inner surface of the hollow channel of the anode, the term "foot points" refers to the location of the foot points that is most downstream in all continuous reactor operating modes. The most extended range of the foot points can be identified, for example, based on a material corrosion analysis on the inner surface of the hollow channel of the anode when modifying the anode after operation. During operation, the material corrosion is higher in the inner surface portion in contact with the foot points compared to the surface section not reached by the arc. The foot points define the region where the electric arc contacts the anode. Likewise, the area where foot points are located on the inner surface of the hollow channel of the cathode during operation can be identified when modified after operation.

[0133] Generally, in the case of the method disclosed in the present invention, the electrical energy input to the plasma section by the electric arc is a normal cubic meter (1 m²) of C1- to C4-alkane-containing supply plasma gas. N 3 0.5 to 10 kWh per el It is the range. For the purposes of the present invention, a normal cubic meter is 1 cubic meter (1 m²) at 1.01325 bar and 273.15 K. 3 It is the amount of gas contained in the volume of ) (DIN 1343, version 1990-01).

[0134] The above apparatus and the reactor thereof may be operated at a variable load, for example, a variable load in the range of 50 to 100% of the design load. The load may be controlled according to a specific signal received by a control unit. The signal received by the control unit and used to control the apparatus and method of the present invention may be a signal derived from factors that influence the determination of the process load. These factors may include electricity costs, the current carbon footprint of electricity consumption, and / or requests for grid service provision, such as control power.

[0135] The term "anode" used for the definition of the present invention is understood narrowly. The anode extends to the beginning of the second reactor section, which is identical to the beginning of the first subsection of the second reactor section, that is, to the location of the at least one second supply line along the flow direction of the main stream (although the portion beyond the beginning of the first subsection of the second reactor section may have the same potential as the anode). Other portions of the plasma section, such as magnetic devices or devices that hydrodynamically induce swirling of the plasma gas, do not belong to the anode defined according to the present invention, even if they may have the same potential as the anode. Accordingly, in some embodiments, at the open end of the anode facing the direction of flow of the main stream or at the location where the foot points of the electric arc contact the inner surface of the hollow channel of the anode, the flow cross-section of the reactor across the direction of flow of the main stream does not change along the length of the anode and / or along the transition from the anode to the second reactor section. In other words, the flow cross-section across the direction of flow of the main stream can remain essentially the same at the anode and at the transition from the anode to the second reactor section. Thus, in some embodiments, the flow cross-section across the direction of flow of the main stream at the open end of the anode opposite to the direction of flow of the main stream can be essentially the same as the flow cross-section across the direction of flow of the main stream at the beginning of the first subsection of the second reactor section.

[0136] The fact that the reactor includes a second reactor section (30) immediately after the plasma section (20) of the reactor means that the two reactor sections are directly connected to each other. The second reactor section has a first subsection (31) and a second subsection (32), the second subsection being immediately after the first subsection in the direction of the main stream flow. At the end of the second subsection in the direction of the main stream flow, an outlet means (33) for recovering the mixture from the reactor is configured. This may be one or more lines or valves for recovering the mixture from the reactor.

[0137] The statement that the outlet means is located at the end of the second reactor section means that the outlet means is located at or near the end of the second reactor section, suitable for recovering the mixture from the reactor.

[0138] The term flow direction of the main stream of gas (23), or more specifically, flow direction of the main stream of plasma gas, as used herein, refers to the entire stream of said gas or said plasma gas passing through the reactor until it is injected into the plasma section of the reactor and then recovered through the outlet means (33) at the end of the second reactor section. Generally, the flow direction of the main stream of plasma gas refers to the gas flowing through the plasma section. With respect to the second reactor section and the mixture, it is usually referred to as the flow direction of the main stream of the mixture. During the process, the plasma gas reacts and mixes with other components. Although the flow direction of the main stream of gas may change along the path of said main stream passing through the reactor, said flow direction of the main stream is nevertheless a means for defining the location and orientation of features of the method, apparatus, and use of the present invention as illustrated in the drawings. As an example, there is a flow cross-section that crosses the flow direction of the main stream.

[0139] The first subsection (31) includes at least one second supply line (70) for introducing a C1- to C4-alkane-containing gas into the first subsection (31) of the second reactor section (30). The key aspect of the invention is that both the plasma gas introduced through the at least one first supply line and the gas introduced into the reactor through the at least one second supply line are C1- to C4-alkane-containing gases. As the C1- to C4-alkane-containing gas introduced through the at least one second supply line is introduced as a plasma gas at a downstream location of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the direction of flow of the main stream, a mixture comprising the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas introduced through the at least one second supply line is formed in the first subsection of the second reactor section downstream of the at least one second supply line.

[0140] The reactor comprises, at least one point within the first subsection of the second reactor section and / or within the plasma section, a flow cross-section across the main stream flow direction that is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the main stream flow direction in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode, wherein if included within the plasma section, it is included within the region of the end of the plasma section as downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the main stream flow direction. Accordingly, the at least one point where the flow cross-section across the main stream flow direction is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the main stream flow direction in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode is upstream or downstream of the at least one second supply line in the main stream flow direction. In some embodiments, the most upstream point in the direction of flow of the main stream is located in the plasma section, which is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode in the direction of flow of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the direction of flow of the main stream, whereas in other embodiments, it is located in the first subsection of the second reactor section.

[0141] The location of the at least one second supply line along the flow direction of the main stream defines the inlet of the second reactor section and its first subsection. The second reactor section and its first subsection begin on a plane passing through the uppermost upstream point of the at least one second supply line in the flow direction of the main stream. The plane is perpendicular to the flow direction of the main stream of the plasma gas at the uppermost upstream point of the at least one second supply line.

[0142] This is illustrated in FIG. 1 and FIG. 2, where the at least one second supply line (70) defines the inlet of the second reactor section (30). In FIG. 2, a point in the flow direction of the main stream (71) that is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode in the flow direction of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode is upstream of the inlet of the second reactor section (30) in the flow direction of the main stream, i.e., upstream of the at least one second supply line, and thus located in the plasma section, but downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the flow direction of the main stream.

[0143] In preferred embodiments, the reactor comprises at least one sudden expansion located between the foot points of the electric arc on the inner surface of the hollow channel of the anode and the top upstream point in the flow direction of the main stream, wherein the top upstream point is a point where the flow cross-section across the flow direction of the main stream (71) is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode. The sudden expansion is a sudden expansion of the flow cross-section across the flow direction of the main stream, wherein the sudden expansion has an opening angle of at least 20°, preferably at least 45°, more preferably at least 75° with respect to the axis of the main stream in the flow direction of the main stream. The configuration of such a reactor helps to mix the C1- to C4-alkane-containing gas introduced into the reactor through the at least one second feed line with the plasma gas and to broaden the residence time distribution of atoms in the mixture. In particular, the rapid expansion section enhances the reverse mixing of some of the carbon-rich solid particles, the surface of which exerts a catalytic effect on hydrocarbon decomposition, and which may grow to a larger size through reverse mixing. Additionally, the residence time distribution may be further broadened and the apparatus and method of the present invention further improved through additional means, such as means for inducing turbulence and / or reverse mixing. Accordingly, in some embodiments, the second reactor section includes at least one additional device for inducing additional turbulence and / or reverse mixing of the mixture, which is preferably located downstream of the at least one second feed line in the direction of the main stream flow.In some embodiments, the at least one additional device is located downstream of the top upstream point in the flow direction of the main stream, the top upstream point being a point where the flow cross-section across the flow direction of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode. In these embodiments, the at least one additional device may be located downstream of the at least one second supply line in the flow direction of the main stream. The at least one additional device for inducing turbulence and / or reverse mixing of the mixture may be selected from the group consisting of a passive grid, a static mixer, a bend of the reactor, and combinations thereof, preferably, the bend of the reactor inducing the flow direction of the mixture to change by at least 80°, preferably at least 135°, with respect to the flow direction of the main stream. In some embodiments of the present invention, the reactor comprises two or more rapid expansion sections, preferably in the second reactor section, and more preferably in the first and / or second subsection of the second reactor section.

[0144] In preferred embodiments, at least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line.

[0145] Unless otherwise specified, the residence time, average residence time, and residence time distribution within the second reactor section refer to the residence time, average residence time, and residence time distribution throughout the entire second reactor section.

[0146] The term "deviation of more than 5% in absolute number from the average residence time" means that the atoms have a residence time of 95% or less or 105% or more compared to the average residence time.

[0147] Preferably, at least 10% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 10% in absolute number from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and more preferably, have a deviation of at least 15%, and even more preferably at least 20%, from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line.

[0148] In other embodiments, the flow cross-section across the flow direction of the main stream in the range of the area from the foot points of the electric arc on the inner surface of the hollow channel of the anode to the top upstream point in the flow direction of the main stream is, at any point, 60% or more, preferably 80% or more, more preferably 90% or more compared to the average flow cross-section across the flow direction of the main stream at the foot points of the electric arc on the inner surface of the hollow channel of the anode, wherein the flow cross-section across the flow direction of the main stream is 5 times or more, preferably 10 times or more, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode. This ensures that even if there is a reduction in the flow cross-section between the foot points of the electric arc on the inner surface of the hollow channel of the anode and the point where the flow cross-section across the flow direction of the main stream is expanded, there is only a limited reduction. This prevents undesirable pressure drop and material stress within this zone of the reactor.

[0149] To define the required residence time of the atoms of the mixture, the device is characterized by a specific volume ratio of individual sections. The reference is the volume of the plasma section, which is the volume from the top upstream position where the inner surface of the hollow channel of the anode faces the electric arc to the end of the plasma section of the reactor. The term “volume of the plasma section from the top upstream position where the inner surface of the hollow channel of the anode faces the electric arc to the end of the plasma section of the reactor” refers to the internal volume of the hollow channel of the anode that starts at the top upstream point of the hollow channel of the anode facing the electric arc in a plane perpendicular to the inner surface of the anode at this point—where said plane is perpendicular to the flow direction of the main stream at the top upstream point of the anode—and ends at a plane perpendicular to the flow direction of the main stream at the end of the plasma section of the reactor. This volume is indicated by reference numeral (22) in FIGS. 1 and 2. The above reference volume is 0.0001 to 0.4 m 3 The range of, preferably 0.001 to 0.2 m 3 It has a volume in the range of. The volume of the first subsection of the second reactor section and the total volume of the second reactor section are defined in relation to the reference volume. The volume of the first subsection of the second reactor section is in the range of 10 to 200 times the reference volume, preferably in the range of 20 to 100 times the reference volume, while the total volume of the second reactor section is in the range of 20 to 2000 times the reference volume, preferably in the range of 40 to 1000 times the reference volume.

[0150] The term "volume" used herein refers to the internal volume of an object. With respect to the reference volume, it means that the reference volume relates to the internal volume of the hollow channel of the anode filled with plasma gas. Accordingly, cooling means that may be connected to or contained in the anode, or the walls of the hollow channel of the anode, are not included. With respect to the volume of the second reactor section, it means that the volume used herein relates to the internal volume of the second reactor section, the internal volume of the second reactor section extending from a plane perpendicular to the flow direction of the main stream at the transition point from the plasma section to the second reactor section to the end of the second reactor section, and is filled with the plasma gas exiting the plasma section and the components of the C1- to C4-alkane-containing gas of the at least one second supply line. With respect to the volume of the first subsection of the second reactor section, it means that the volume used herein relates to the internal volume of the first subsection of the second reactor section, wherein the internal volume of the first subsection of the second reactor section extends from a plane perpendicular to the flow direction of the main stream at the transition point from the plasma section to the second reactor section to the end of the first section of the second reactor section, and is filled with the plasma gas exiting the plasma section and the components of the C1- to C4-alkane-containing gas of the at least one second supply line.

[0151] Preferably, the C1- to C4-alkane-containing gas is introduced into the plasma-like plasma through the at least one second supply line across the flow direction of the main stream at a location downstream from the foot points of the electric arc on the inner surface of the hollow channel of the anode in the flow direction of the main stream. Accordingly, the at least one reactor may be configured such that the at least one second supply line can introduce the C1- to C4-alkane-containing gas into the plasma-like plasma gas across the flow direction of the main stream. The cross-flow includes an inflow at an angle in the range of 80 to 100°, preferably in the range of 85 to 95°, with respect to the axis of the main stream. This further enhances the mixing of the plasma-like plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line.

[0152] The absolute flow rate of the above plasma gas is generally 2 m 3 / h to 40,0000 m 3 The range is / h. It is evident that the specific flow rate is set according to the details of the selected reactor design. Therefore, the specified maximum flow rate is 0.0001 m 3 It will not be combined with the reference volume of the plasma section. Therefore, the ranges of parameters described herein should be understood as the ranges within which a person skilled in the art selects appropriate parameter settings to operate the apparatus of the present invention and implement the method of the present invention.

[0153] Preferably, the ratio of the flow rate of the second supply gas to the flow rate of the supply plasma gas in units of normal cubic meters per hour is set to be within the range of 0.1 to 1.5. Preferably, the temperature of the plasma gas introduced into the plasma section through the at least one first supply line is in the range of 20°C to 600°C before being injected into the first reactor section. This may include the step of heating the plasma gas, for example using a heat exchanger, before the plasma gas is introduced into the plasma section. Also preferably, the temperature of the C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line may be in the range of 20°C to 1000°C. Here, too, a heat exchanger may be used to heat the gas to a temperature within this range. The ratio of the streams and the temperatures of the streams after preheating are means for adjusting the temperature profile of the mixture within the second reactor section. Other means include, for example, a specific energy input of the electric arc in units of kilowatt-hours of electric energy per normal cubic meter of plasma gas, and the composition of the C1- to C4-alkane-containing gas and the supply plasma gas introduced through the at least one second supply line.

[0154] If the device includes a heat exchanger, the heat exchanger may receive heat from the mixture exiting the reactor. Thus, in some embodiments, the outlet means of the second reactor section is connected to the heat exchanger (120). Alternatively, the heat exchanger may receive heat from steam or from at least one burner. Preferably, the burner is fueled using a fuel containing a portion of the hydrogen that was produced immediately before in the reactor of the device of the present invention.

[0155] Alternatively, the device comprises two heat exchangers capable of receiving the mixture or at least a portion of the mixture exiting the reactor. In a preferred embodiment, both heat exchangers are connected in parallel to the outlet means of the reactor. In another preferred embodiment, the heat exchangers are connected in series (i.e., one heat exchanger is directly connected to the outlet means of the reactor and the other heat exchanger is connected to the outlet of the first heat exchanger). Thus, the plasma gas injected into the plasma section through the at least one first supply line can be preheated by one heat exchanger together with the C1- to C4-alkane-containing gas introduced through the at least one second supply line. Alternatively, the plasma gas injected into the plasma section through the at least one first supply line may be preheated separately from the C1- to C4-alkane-containing gas introduced through the at least one second supply line by one of the two heat exchangers connected in parallel or in succession to the outlet means of the reactor, and the C1- to C4-alkane-containing gas introduced through the at least one second supply line may be preheated by the other of the two heat exchangers connected in parallel or in succession to the outlet means of the reactor. When the two heat exchangers are connected in succession, the first heat exchanger connected to the stream recovered through the outlet (33) may also be connected to the at least one first supply line (60) to transfer heat to the plasma gas before the plasma gas is introduced into the plasma section through the at least one first supply line (60).A second heat exchanger may be connected to at least one second supply line (70) to transfer residual heat from a stream exiting the first heat exchanger to the gas flowing into the first subsection of the second reaction section through at least one second supply line (70).

[0156] In a preferred embodiment, the device comprises a heat exchanger connected to the outlet means of the reactor to receive the mixture or at least a portion of the mixture exiting the reactor and to simultaneously cool the mixture. In a further preferred embodiment, the device comprises one heat exchanger for steam generation and both of the one or two heat exchangers for preheating the plasma gas injected into the plasma section through the at least one first supply line and / or the C1- to C4-alkane-containing gas introduced through the second supply line. In a preferred process, the heat exchangers are operated at various loads depending on the circumstances, for example, depending on the availability of renewable electricity and / or the demand for heat and / or electricity rates. More specifically, in a preferred process, depending on the circumstances, for example, when the availability of renewable electricity is high and / or there is a demand for heat, a larger portion or all of the mixture exiting the reactor will be used for heat generation for external heat utilization. Where the availability of renewable electricity is low and / or the demand for heat is low, little or no heat for external use will be generated from the mixture, and instead, in order to reduce specific electrical energy consumption for the production of hydrogen and solid carbon in the reactor, the mixture will be used to preheat the plasma gas injected into the plasma section through the at least one first supply line and / or the C1- to C4-alkane-containing gas introduced through the second supply line.

[0157] In some embodiments, the apparatus according to the present invention for hydrogen and solid carbon further comprises at least one device for concentrating a solid component (preferably carbon black) formed in the reactor, wherein the at least one device for concentrating the solid component (preferably carbon black) concentrates the solid component (preferably carbon black) of the mixture by separating a gaseous component from the solid component (preferably carbon black) of the mixture, and the at least one device for concentrating the solid component (preferably carbon black) has a) fluidly communicating with the outlet means of the reactor, b) at least one outlet for a stream containing a solid component (preferably carbon black) at a concentration concentrated relative to the mixture that flows into the at least one device for concentrating the solid component (preferably carbon black), and c) at least one outlet for a stream containing a solid component (preferably carbon black) at a concentration reduced relative to the mixture and a gaseous component of the mixture that flows into the at least one device for concentrating the solid component (preferably carbon black). have.

[0158] In some embodiments, the at least one device for concentrating the solid component of the mixture is selected from the group consisting of a cyclone (particularly a high-temperature cyclone), a filter (preferably a high-temperature filter), a device having a fixed bed or a fluid bed of solid particles, a scrubber (preferably a scrubber using a moisture-containing scrubbing medium or an oil-based scrubbing medium), and combinations thereof.

[0159] In some embodiments, the total volume of the second reactor section, extending from the point of transition from the plasma section to the second reactor section in a plane perpendicular to the flow direction of the main stream to the end of the second reactor section, and the volume of the device for concentrating the solid component of the mixture, is in the range of 20 to 2000 times the reference volume, preferably in the range of 40 to 1000 times the reference volume.

[0160] The solid carbon of the present invention preferably comprises carbon black or is carbon black. Generally, industrial carbon black comprises aggregates of primary particles having a particle size in the range of several nanometers to 500 nm or is said aggregates. For example, different types of carbon black exist that differ in terms of particle size and / or specific surface area. The term solid carbon refers to carbon within the reactor space that is solid under reaction conditions. An example of solid carbon is an aggregate of carbon atoms.

[0161] In other embodiments, the apparatus of the present invention comprises at least one device for concentrating a solid component connected to an outlet of the second reactor section, wherein a heat exchanger is connected to an outlet of the at least one device for concentrating a solid component, said heat exchanger is connected to an outlet for a mixture having a lower solid concentration than the feed of the at least one device for concentrating solid carbon black.

[0162] In some embodiments, the apparatus for producing hydrogen and solid carbon comprises, in addition to the at least one device for concentrating a solid component (preferably carbon black), at least one device for concentrating hydrogen from a stream comprising a solid component (preferably carbon black) at a reduced concentration relative to the mixture and a gaseous component of the mixture, wherein the at least one device for concentrating hydrogen comprises: a) fluidly communicating with an outlet of the at least one device for concentrating the solid component (preferably carbon black) of the mixture for a stream comprising the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black); b) having at least one outlet for a stream comprising hydrogen at a concentrated concentration relative to the stream comprising the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black) for concentrating hydrogen; and c) the gaseous component of the mixture and a reduced concentration of the solid component of the mixture for concentrating hydrogen for concentrating hydrogen It has at least one outlet for a stream containing hydrogen at a reduced concentration compared to the stream containing a component (preferably carbon black).

[0163] In some embodiments, the at least one outlet for a stream containing hydrogen at a reduced concentration compared to the stream containing the gaseous component of the mixture and the reduced concentration of the solid component (preferably carbon black) introduced into the at least one device for hydrogen enrichment is connected to a storage vessel, preferably a pressure vessel having a pressure higher than the original pressure of the stream. The gas stored therein may include unsaturated hydrocarbons such as ethylene and acetylene and may be useful as fuel.

[0164] In a preferred embodiment, the at least one outlet for a stream containing hydrogen at a reduced concentration compared to the stream containing a gaseous component of the mixture and a reduced concentration of a solid component (preferably carbon black) introduced into the at least one device for hydrogen concentration is connected to a burner so as to burn at least a portion of this gas.

[0165] In other embodiments, at least a portion of the stream containing hydrogen at a reduced concentration compared to the stream containing the gaseous component of the mixture and the reduced concentration of the solid component (preferably carbon black) introduced into the at least one device for hydrogen concentration is used as a feedstock and is preferably fed back to the reactor through the at least one first feed line, the second feed line, and / or the third feed line (if available), more preferably through the at least one second feed line. Preferably, use as a feedstock varies over time and depends on the reactor operating mode and / or specific boundary conditions. For example, preferably, when the electricity rate is equal to or exceeds a threshold to be determined in the future, the stream may be used as a feedstock in the reactor. In a preferred embodiment, the outlet for a stream containing hydrogen at a reduced concentration compared to the stream containing the gaseous component of the mixture and the reduced concentration of the solid component (preferably carbon black) introduced into the at least one device for hydrogen enrichment is also connected to a flare and / or burner to generate process heat. Thus, at least some of the oxygen-containing components, such as carbon monoxide that may be formed from CO2 in natural gas, or other oxygen-containing components in the feedstock, as well as inert gases such as N2 in the C1- to C4-alkane-containing gas introduced through the at least one first supply line and / or the at least one second supply line, can be removed.

[0166] In other embodiments, the apparatus according to the present invention for hydrogen and solid carbon production comprises a reactor having means for detachably connecting an anode or a portion of said anode to the remainder of the reactor, preferably two distinct means. Preferably, one of the two distinct means is located upstream of the foot points of an electric arc on the inner surface of a hollow channel of said anode in the direction of flow of said main stream, and the other of the two distinct means is located downstream of the foot points of an electric arc on the inner surface of a hollow channel of said anode in the direction of flow of said main stream. The means for detachably connecting the anode or a portion of said anode to the remainder of the reactor is located upstream of said at least one second supply line in the direction of flow of said main stream. In some embodiments, an upper upstream point exists in the range of areas from downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the flow direction of the main stream to upstream of the at least one second supply line in the flow direction of the main stream, wherein the upper upstream point is a point where the flow cross-section across the flow direction of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode. This means that the point (extension of the flow cross-section) where the flow cross-section across the flow direction of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode may already exist in the space between the foot points of the electric arc and the second supply line.More preferably, a rapid expansion portion of the flow cross-section across the flow direction of the main stream is additionally present upstream of the top upstream point, in which the flow cross-section across the flow direction of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of foot points of the electric arc on the inner surface of the hollow channel of the anode. In this situation, the means located downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the direction of flow of the main stream is located upstream of the uppermost upstream point, where the flow cross-section crossing the direction of flow of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode crossing the direction of flow of the main stream in the area of ​​the foot points of the electric arc on the inner surface of the hollow channel of the anode, and even more preferably, is located upstream of the rapid expansion portion of the flow cross-section crossing the direction of flow of the main stream. This enables a quick, easy, and efficient anode replacement if necessary. In particular, the downtime of the reactor does not need to be extended, and the reactor does not need to be substantially disassembled for anode replacement.

[0167] In some embodiments, the apparatus according to the present invention for producing hydrogen and solid carbon comprises a reactor having means for detachably connecting a cathode or a portion of said cathode to the remainder of the reactor, preferably two distinct means. The means for detachably connecting the cathode or a portion of said cathode to the remainder of the reactor is located upstream of said at least one second supply line in the direction of flow of said main stream. Preferably, said cathode has a hollow channel in which the electric arc extends, and foot points of said electric arc contact the inner surface of the hollow channel of said cathode. In this situation, one of said two distinct means may be located upstream of the foot points of said electric arc on the inner surface of the hollow channel of said cathode in the direction of flow of said main stream, and the other of said two distinct means may be located downstream of the foot points of said electric arc on the inner surface of the hollow channel of said cathode in the direction of flow of said main stream.

[0168] In preferred embodiments, the inner surface of the hollow channel of the anode lies in the same plane as the inlet of the inner surface of the second reactor section in the direction of the main stream flow at its end in the direction of the main stream flow (see FIG. 1 and FIG. 2). Thus, in both embodiments, at the point where the anode transitions to the second reactor section in the direction of the main stream flow, there is no portion of the anode wall that is in contact with the process gas coming from the opposite side. Preferably, a certain passage exists from the inner surface of the hollow channel of the anode and the inner surface of the first subsection of the second reactor section. This enables improved control of flow and reaction within the reactor and prevents the deposition of undesirable tar or solids.

[0169] In this situation, the reactor may block the path of the plasma gas to the second reactor section by including a flow channel blocking means under the detachable anode. Preferably, the means for blocking the connection is located between the anode and the inlet of the second reactor section. Preferably, the blocking means is a valve or a slide. In a more preferred embodiment, the blocking means is preferably cooled with a liquid, and more preferably with water.

[0170] In some embodiments, the at least one reactor has at least one third supply line for introducing a C1- to C4-alkane-containing gas into the second reactor section, the at least one third supply line for introducing the C1- to C4-alkane-containing gas is positioned downstream of the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section in the direction of the flow of the main stream, and more preferably, the position of the at least one third supply line defines the inlet of the second subsection (32) of the second reactor section. Introducing the C1- to C4-alkane-containing gas through the at least one third supply line downstream of the at least one second supply line is advantageous in that the temperature and reaction can be better controlled along the path of the main stream.

[0171] The mixture produced by the apparatus and method of the present invention, containing hydrogen and solid carbon recovered through the outlet means (33), may be stored. The storage may be temporary storage at an intermediate stage (e.g., for buffer purposes in an integration process) or storage for a longer period. For example, the mixture may be stored in a pressurized vessel. Such a pressurized vessel may store gas at an elevated pressure of up to 200 bar. In some embodiments, the amount of solid carbon is first reduced. Subsequently, the remaining mixture containing raw materials (containing solid carbon and / or additional components in reduced amounts) or purified hydrogen may be stored in the vessel.

[0172] A method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma is characterized by comprising at least steps a) to h) defined in the appended claims. In step a), the C1- to C4-alkane-containing plasma gas is withdrawn from a C1- to C4-alkane-containing gas supply device. Such a device is also disclosed herein as a device for supplying C1- to C4-alkane-containing gas. In preferred embodiments, the method uses a device and a reactor according to the present invention.

[0173] In step e), the C1- to C4-alkane-containing gas is introduced into a first subsection of the second reactor section through at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section, wherein the C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line is introduced into the plasma-like plasma gas downstream of the foot points of the electric arc generated by the anode and cathode in the direction of flow of the main stream, so that a mixture can be formed in the first subsection of the second reactor section downstream of the at least one second supply line from the plasma-like plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line.

[0174] At the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas has an average temperature in the range of 1200 to 3000 ℃, preferably in the range of 1500 to 2800 ℃. This means the average temperature that the plasma gas would have had at the said location if the C1- to C4-alkane-containing gas had not been introduced into the plasma gas through the at least one second supply line.

[0175] The key point is that the plasma gas contains acetylene before the C1- to C4-alkane-containing gas is introduced and injected into the plasma gas through the at least one second supply line. Preferably, at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas contains 2 vol.% or more, preferably 4 vol.% or more, more preferably 6 vol.% or more, and most preferably 8 vol.% or more of acetylene.

[0176] A mixture is formed by introducing a C1- to C4-alkane-containing gas into the plasma gas through the at least one second supply line. The mixture has an average temperature of 850°C or higher, preferably 1050°C or higher, and less than 3000°C, preferably less than 2800°C, in the region range from the at least one second supply line to the end of the first subsection of the second reactor section.

[0177] The average temperature of the mixture in the second subsection of the second reactor section is 650°C or higher, preferably 750°C or higher, more preferably 850°C or higher, and less than 1500°C, preferably in the range of 700°C to 1400°C, more preferably in the range of 800°C to 1300°C, most preferably in the range of 800°C to 1200°C, and the average temperature at the end of the second reactor section of the mixture obtained from the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line is 200K or higher, preferably 400K or higher, more preferably 600K or higher, and is lower than the average temperature of the plasma gas at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line. This average temperature is much higher than that used in conventional reactors and processes for acetylene production, further improving process efficiency. This also applies to the method and reactor applications of the present invention.

[0178] Step f) comprises moving the mixture downstream in the flow direction of the main stream through the second reactor section, wherein the moving is performed such that the average residence time of atoms in the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line in the first subsection of the second reactor section is in the range of 100 ms to 2000 ms, preferably in the range of 200 ms to 1000 ms, more preferably in the range of 400 ms to 900 ms, and even more preferably in the range of 500 ms to 800 ms. Accordingly, the average temperature of the mixture and the average residence time of its atoms in the first subsection of the second reactor section are essential for the efficient operation of the method. Step f) further specifies that the transfer is made such that the average residence time of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the entire second reactor section (including the second subsection of the second reactor section) is in the range of 200 ms to 20000 ms, preferably in the range of 400 ms to 10000 ms, more preferably in the range of 600 ms to 9000 ms, even more preferably in the range of 800 ms to 8000 ms, and even more preferably in the range of 1000 ms to 7500 ms. Additionally, in the entire second reactor section including the second subsection of the second reactor section, the average temperature of the mixture and the average residence time of the atoms are essential for the efficient operation of the method.

[0179] Additionally, in step f), at least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and preferably, at least 10% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line. It is specified that there is a deviation of at least 10% in absolute number from the average residence time, and more preferably, a deviation of at least 15%, even more preferably at least 20%, from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line. Accordingly, the residence time distribution as well as the average residence time of the atoms of the mixture are significant and controlled. Thus, hydrogen and solid carbon (preferably carbon black) are also produced in the second reactor section.Hydrogen and solid carbon (preferably carbon black) are produced in the reactor at a lower overall energy cost, because the process and apparatus parameters are defined such that the use of acetylene decomposition heat can be maximized to provide the energy required for the conversion of C1- to C4-alkane-containing gases into hydrogen and solid carbon in the second reactor section.

[0180] In relation to the apparatus of the present invention, the method of the present invention disclosed above and in the appended claims may include steps of concentrating solids and hydrogen from the mixture. Accordingly, the method may further include step i) of processing the mixture recovered through the outlet means into at least one device for concentrating the solid component of the mixture (preferably carbon black) in order to generate a stream containing a concentrated concentration of the solid component of the mixture (preferably carbon black) and a stream containing a gaseous component of the mixture and a reduced concentration of the solid component of the mixture (preferably carbon black). Preferably, step i) is performed in at least one device for concentrating a solid component (preferably carbon black) formed in the reactor, and the at least one device for concentrating the solid component (preferably carbon black) is used to separate a gaseous component from the solid component (preferably carbon black) of the mixture in order to concentrate the solid component (preferably carbon black) of the mixture, and the at least one device for concentrating the solid component is fluidly connected to the outlet means of the reactor and has at least one outlet for a stream containing a solid component (preferably carbon black) at a concentration concentrated relative to the mixture that flows into the at least one device for concentrating the solid component (preferably carbon black), and at least one outlet for a stream containing a solid component (preferably carbon black) at a concentration reduced relative to the mixture and a gaseous component of the mixture that flows into the at least one device for concentrating the solid component (preferably carbon black). Preferred examples of such a device are disclosed herein.

[0181] In some embodiments, the average residence time of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line is in the range of 200 ms to 20000 ms, preferably in the range of 400 ms to 10000 ms, more preferably in the range of 600 ms to 9000 ms, even more preferably in the range of 800 ms to 8000 ms, and even more preferably in the range of 1000 ms to 7500 ms. This is because, through the temperature profile defined in the method of the present invention, under certain circumstances, the C1- to C4-alkane-containing gas can be further converted into hydrogen and solid carbon when the mixture passes from the outlet of the second reactor section to the place containing the device for concentrating the solid component (preferably, carbon black). The sum of the internal volume of the device for concentrating the solid component filled by the mixture exiting the second reactor section and the internal volume of the connection portion of the device for concentrating the solid (preferably, carbon black) to the outlet of the second reactor section may be in the range of 10 to 1800 times the reference volume specifically described above, preferably in the range of 20 to 800 times the reference volume.

[0182] The method of the present invention, comprising the device for concentrating the solid component, may further include step j) of processing the stream comprising the gaseous component of the mixture and the solid component of the mixture at a reduced concentration (preferably carbon black) using at least one device for generating a stream having a concentrated concentration of hydrogen compared to the stream comprising the gaseous component of the mixture and the solid component of the mixture at a reduced concentration (preferably carbon black). Preferably, step j) is performed in at least one device for concentrating hydrogen from a stream comprising a solid component (preferably carbon black) at a reduced concentration relative to the mixture flowing into at least one device for concentrating a solid component (preferably carbon black) and a gaseous component of said mixture, and the at least one device for concentrating hydrogen is fluidly connected to at least one outlet of the at least one device for concentrating a solid component (preferably carbon black) of said mixture for a stream containing a solid component (preferably carbon black) at a reduced concentration relative to the stream containing a gaseous component of said mixture and a solid component (preferably carbon black) at a reduced concentration relative to said stream flowing into at least one device for concentrating hydrogen, and has at least one outlet for a stream containing a hydrogen at a reduced concentration relative to said stream containing a solid component (preferably carbon black) at a reduced concentration relative to said stream flowing into at least one device for concentrating hydrogen.

[0183] In some embodiments, the method is carried out such that the reactor includes, at least 5 times, preferably at least 10 times, a flow cross-section across the main stream flow direction that is greater than the average flow cross-section of the anode across the main stream flow direction in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode at at least one point within the first subsection of the second reactor section and / or within the plasma section, wherein if included within the plasma section, it is included within the range of the range up to the end of the plasma section as downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the main stream flow direction. Preferably, the pressure immediately upstream (in the direction of flow of the main stream) immediately preceding the top upstream point, where the flow cross-section across the main stream flow direction is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the main stream flow direction in the range of foot points of the electric arc on the inner surface of the hollow channel of the anode, is in the range of 0.5 to 30 bar overpressure or bar gauge.

[0184] In another embodiment of the method of the present invention, the wall of the second reactor section is cooled, preferably cooled with a fluid, more preferably cooled with a liquid, and even more preferably cooled with a liquid at a temperature of up to 450°C. This applies to the apparatus of the present invention as well, and thus the apparatus may include a reactor having a second reactor section having a cooled wall, preferably a wall cooled with a liquid, more preferably a wall cooled with a liquid at a temperature of up to 450°C.

[0185] In some embodiments of the above method, a C1- to C4-alkane-containing gas is introduced into the plasma gas through the second supply line across the flow direction of the main stream. This improves the mixing of the mixture.

[0186] Additionally, the method may include performing at least a third inflow of a C1- to C4-alkane-containing gas into the second reactor section, wherein the third inflow is performed through at least one third supply line positioned downstream of the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section in the direction of flow of the main stream, and preferably, the location of the at least one third supply line defines the inlet of the second subsection of the second reactor section.

[0187] To further improve the above method, the method may preferably include introducing into the second reactor section a carbon black that is a part of the solid carbon (preferably carbon black) produced and separated according to the method of the present invention, preferably carbon black, which is preferably dispersed in a hydrogen and / or C1- to C4-alkane-containing gas, preferably carbon black, which is preferably a part of the solid carbon (preferably carbon black) produced and separated according to the method of the present invention, preferably having different average physical properties (e.g., different average particle size or specific surface area) compared to the total of the solid carbon (preferably carbon black) produced in the method. Through the fractionation of the solid carbon material (preferably carbon black material), solid carbon (preferably carbon black) having a specific average particle size or specific surface area can be obtained. The dispersed carbon black may be a part derived from the carbon black produced in the method according to the present invention, which includes the separation of carbon black. Solid carbon (preferably carbon black) dispersed in hydrogen and / or a C1- to C4-alkane-containing gas is introduced into the second reactor section by being introduced directly into the second reactor section or, preferably, into the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the first subsection of the second reactor section. Preferably, the solid carbon (preferably carbon black) is introduced into the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the first subsection of the second reactor section.

[0188] If the above solid carbon-containing (preferably carbon black-containing) gas stream is introduced directly into the second reactor section, 1 g / m² immediately before the point of introduction into the second reactor section N 3 Up to 100 g / m² N 3The solid carbon (preferably, carbon black) concentration may be within a range. Preferably, when the solid carbon-containing (preferably, carbon black-containing) gas stream is directly introduced into the second reactor section, the ratio of the flow rate of the solid carbon-containing (preferably, carbon black-containing) gas stream immediately before entering the second reactor section to the sum of the flow rate of the C1- to C4-alkane-containing plasma gas stream and the flow rate of the C1- to C4-alkane-containing gas stream of the at least one second supply line is m N 3 The range is 0.01% to 10% in / h units, preferably 0.1% to 5%.

[0189] And, when the solid carbon-containing (preferably, carbon black-containing) gas stream is introduced into the at least one second supply line for introducing a C1- to C4-alkane-containing gas into the first subsection of the second reactor section, 1 g / m² immediately before the point in time when the C1- to C4-alkane-containing gas is introduced into the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the first subsection of the second reactor section N 3 Up to 100 g / m² N 3The solid carbon (preferably, carbon black) concentration may be within a range. Preferably, when the solid carbon-containing (preferably, carbon black-containing) gas stream is introduced into the at least one second supply line for introducing a C1- to C4-alkane-containing gas into the first subsection of the second reactor section, the ratio of the flow rate of the solid carbon-containing (preferably, carbon black-containing) gas stream immediately before entering the at least one second supply line to the sum of the flow rate of the C1- to C4-alkane-containing plasma gas stream and the flow rate of the C1- to C4-alkane-containing gas stream of the at least one second supply line is m N 3 The range is 0.01% to 10% in / h units, preferably 0.1% to 5%.

[0190] The above solid carbon (preferably, carbon black) is 1 to 1000 m 2 Range of / g, preferably 10 to 800 m 2 The range of / g, and most preferably 50 to 600 m 2It has a specific surface area in the range of / g. The said specific surface area is determined using the BET NSA method described in ASTM D6556-14 (approved June 1, 2014; published July 2014; 10.1520 / D6556-14), which is incorporated herein by reference. Carbon black can act as a catalyst for various reactions within the reactor (e.g., the separation of natural gas into hydrogen and carbon) and can further improve yield and / or reaction kinetics. Additionally, the introduction of carbon black particles helps to promote the concentration of the solid component of the mixture by increasing the average particle size of the solid carbon in the device that concentrates the solid component (preferably, carbon black) from the mixture. Accordingly, the method of the present invention may include the step of introducing solid carbon (preferably, carbon black) into the second reactor section, wherein, preferably, the solid carbon (preferably, carbon black) has the concentration and characteristics defined above. g / m² N 3 The above definition of the concentration of solid carbon (preferably carbon black) using units refers to grams per normal cubic meter.

[0191] As already described above, at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas contains 2 vol.% or more, preferably 4 vol.% or more, more preferably 6 vol.% or more, and even more preferably 8 vol.% or more of acetylene.

[0192] To further improve the above method, the electric arc generated by the anode and cathode can be rotated around an axis extending from the cathode to the anode. This can be advantageous in terms of energy input to the plasma gas and for improving the lifespan of the electrodes. Preferably, as shown in, for example, Acetylene, Paessler et al., Ullmann's Encyclopedia of Industrial Chemistry, doi:10.1002 / 14356007.a01_097.pub4, 2011, the electric arc rotation is caused by means selected from the group consisting of a magnetic device (preferably located along the cathode and / or anode) or a device that induces swirling in the C1- to C4-alkane-containing plasma gas immediately before it enters the plasma section [e.g., a so-called vortex chamber], and preferably, the electric arc rotates about an axis oriented in the direction of flow of the main stream. In preferred embodiments, the electric arc rotates about the axis for 0.1 s -1 Ideally, more preferably 0.2 s -1 Ideally, and even more preferably 0.5 s -1 It rotates at a frequency above. Preferably, the rotation of the electric arc is induced by a device that induces a vortex in the C1- to C4-alkane-containing plasma gas immediately before it is introduced into the plasma section.

[0193] Preferably, the method is characterized in that additional turbulence and / or backmixing in the mixture is induced in the second reactor section, in particular, additional turbulence in the mixture is induced downstream of the at least one second supply line in the direction of flow of the main stream, preferably using at least one device for inducing turbulence and / or backmixing of the mixture, which is preferably selected from the group consisting of a passive grid, a static mixer, a bend of the reactor, and combinations thereof.

[0194] In a more preferred embodiment of the method of the present invention, the anode and cathode of the at least one reactor are concentric, and the cathode has a hollow channel having a main axis extending along the flow direction of the main stream, and the hollow channel has two opposite ends, the end facing opposite the flow direction of the main stream is closed, and the end facing the flow direction of the main stream of the plasma gas is open and is located upstream of the open end of the anode facing opposite the flow direction of the main stream and is concentric with the open end of the anode, and the anode and cathode are arranged such that the foot points of the electric arc contact the inner surface of the hollow channel of the anode and the inner surface of the hollow channel of the cathode, respectively. Preferably, the anode and the cathode are arranged such that a gap exists in the direction of the main stream between the end of the cathode facing the direction of flow of the main stream and the end of the anode facing the opposite direction of flow of the main stream, and the length of the gap is preferably at least 0.3 times, more preferably at least 0.5 times, the average inner diameter of the hollow channel of the anode in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode. Preferably, the plasma section is designed so that the plasma gas can be introduced into the gap between the anode and the cathode when the plasma gas is introduced into the plasma section of the reactor through the at least one first supply line.

[0195] According to another embodiment of the method of the present invention, the C1- to C4-alkane-containing plasma gas and / or the gas introduced through the at least one second supply line is a gas containing methane or natural gas. Accordingly, in some embodiments, natural gas may be introduced into the reactor through both the at least one first supply line and the at least one second supply line. Alternatively, in some embodiments, methane may be introduced into the reactor through both the first supply line and the at least one second supply line.

[0196] As an independent aspect, the invention disclosed below may be included in the invention defined by the appended claims, and vice versa.

[0197] The inventors have surprisingly discovered that introducing an acetylene-containing gas into the first subsection of the second reactor section, accompanied by a C1- to C4-alkane-containing gas through the at least one second supply line, thereby introducing a plasma gas derived from the C1- to C4-alkane-containing gas is advantageous for the production of hydrogen and solid carbon. The introduced acetylene is decomposed in the second reactor section to generate heat, which helps to increase the temperature of the C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line more rapidly and further promotes the conversion of the C1- to C4-alkane-containing gas into hydrogen and solid carbon (production of hydrogen and solid carbon). Thus, compared to the prior art, the energy consumption of the method can be reduced and / or the capacity of the reactor can be increased.

[0198] The above independent aspects relate to a method, apparatus, and use having additional features as described below.

[0199] Embodiment 1: A method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, characterized by comprising the following steps.

[0200] a) a step of extracting C1- to C4-alkane-containing plasma gas from a C1- to C4-alkane-containing gas supply device;

[0201] b) a step of introducing the C1- to C4-alkane-containing plasma gas extracted from the device for extracting the C1- to C4-alkane-containing plasma gas into at least a first reactor;

[0202] Here, the reactor is a reactor that generates thermal plasma using an electric arc, and the reactor includes a plasma section and a second reactor section, and

[0203] i) The above plasma section is,

[0204] · An anode and a cathode for generating an electric arc - said arc extends within said plasma section -, and

[0205] · At least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor

[0206] Includes,

[0207] · The anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface—, an outlet in the flow direction of the main stream of the plasma gas—the outlet forms an open end of the anode in the flow direction of the main stream—, and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing in the opposite direction of the flow direction of the main stream—the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing in the opposite direction of the flow direction of the main stream and the open end of the anode in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and

[0208] · The anode and the cathode are arranged so that a plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode, and

[0209] ii) The second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream, the second reactor section,

[0210] · A first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and

[0211] · Means for an outlet for recovering components from the reactor above - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream -

[0212] Includes,

[0213] · The first subsection includes at least one second supply line for introducing gas into the second reactor section, and the location of the at least one second supply line along the flow direction of the main stream defines the second reactor section and the inlet of its first subsection, and

[0214] The C1- to C4-alkane-containing plasma gas is introduced into the reactor through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section of the reactor;

[0215] c) a step of generating an electric arc that expands within the plasma section of the reactor to the anode and cathode;

[0216] d) a step of forming a plasma gas from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section using the electric arc in the plasma section of the reactor;

[0217] e) introducing a gas mixture comprising C1- to C4-alkanes and acetylene into a first subsection of the second reactor section through the at least one second supply line for introducing gas into the second reactor section, wherein

[0218] · The gas mixture comprising C1- to C4-alkanes and acetylene introduced into the second reactor section through the at least one second supply line is introduced into the plasma gas at the downstream of the foot points of the electric arc generated by the anode and cathode in the flow direction of the main stream, thereby forming a mixture from the plasma gas exiting the plasma section and the gas mixture comprising C1- to C4-alkanes and acetylene introduced into the first subsection of the second reactor section through the at least one second supply line, and the gas mixture introduction is performed so as to be formed in the first subsection of the second reactor section downstream of the at least one second supply line.

[0219] f) a step of moving the mixture downstream in the direction of flow of the main stream through the second reactor section, wherein

[0220] · Hydrogen and solid carbon are produced by reactions occurring in the mixture within the second reactor section and, preferably, in the plasma section; and

[0221] g) A step of recovering the mixture at the end of the reactor through an outlet means for recovering the mixture from the reactor, wherein the outlet means is located at the end of the second reactor section in the direction of flow of the main stream, and preferably, the recovered mixture comprises acetylene in the range of 0.01 to 4 vol.%, preferably in the range of 0.1 to 1 vol.%.

[0222] Embodiment 2: A method according to Embodiment 1 for producing hydrogen and solid carbon, wherein the method is executed continuously and further comprises the following steps.

[0223] Step h) of processing the mixture recovered through the outlet means using at least one device for concentrating a solid component (preferably carbon black) formed within the reactor, wherein the at least one device for concentrating a solid component (preferably carbon black) separates a gaseous component from the solid component (preferably carbon black) of the mixture to concentrate the solid component (preferably carbon black) of the mixture, and wherein the at least one device for concentrating a solid component (preferably carbon black) fluidly communicates with the outlet means of the reactor to obtain a stream containing solid carbon (preferably carbon black) at a concentration concentrated relative to the mixture flowing into the at least one device for concentrating a solid component, and a stream containing solid components and gaseous components of the mixture at a reduced concentration relative to the mixture flowing into the at least one device for concentrating a solid component.

[0224] Step i) of processing the stream comprising a solid component (preferably carbon black) at a reduced concentration compared to the mixture and a gaseous component of the mixture into the at least one device for concentrating the solid component (preferably carbon black) and the at least one device for concentrating the solid component (preferably carbon black) at a reduced concentration compared to the mixture and a gaseous component of the mixture into the at least one device for concentrating the solid component (preferably carbon black) at a reduced concentration compared to the mixture and the at least one device for concentrating the solid component (preferably carbon black) at a reduced concentration compared to the mixture and the at least one device for concentrating the hydrogen from the other gaseous components to obtain a stream comprising hydrogen at a concentrated concentration compared to the mixture into the at least one device for concentrating the hydrogen and a stream comprising hydrogen and acetylene (preferably acetylene at a concentrated concentration compared to the mixture into the at least one device for concentrating the hydrogen) at a reduced concentration compared to the mixture into the at least one device for concentrating the hydrogen -; and

[0225] Step j) introducing a stream or at least a portion thereof comprising hydrogen and acetylene at a reduced concentration compared to the mixture introduced into the at least one device for hydrogen concentration (preferably, acetylene at a concentrated concentration compared to the mixture introduced into the at least one device for hydrogen concentration), into the at least one second supply line used to introduce the gas mixture comprising C1- to C4-alkanes and acetylene in step e) into the first subsection of the second reactor section.

[0226] Embodiment 3: A method according to Embodiment 1 or 2 for the production of hydrogen and solid carbon, wherein the acetylene concentration of the gas mixture of step e) comprising C1- to C4-alkanes and acetylene is 2 vol.% or more, preferably 4 vol.% or more, more preferably 6 vol.% or more, most preferably vol.% or more acetylene.

[0227] Embodiment 4: A method according to any one of Embodiments 1 to 3 for the production of hydrogen and solid carbon, wherein the method further comprises the features of the method described in the appended claims and in this description.

[0228] Embodiment 5: An apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the apparatus comprises at least one reactor that generates thermal plasma using an electric arc, and wherein the reactor comprises a plasma section and a second reactor section.

[0229] i) The above plasma section is,

[0230] · An anode and a cathode for generating an electric arc - said arc extends within said plasma section -, and

[0231] · At least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor

[0232] Includes,

[0233] · The anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface—, an outlet in the flow direction of the main stream of the plasma gas—the outlet forms an open end of the anode in the flow direction of the main stream—, and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing in the opposite direction of the flow direction of the main stream—the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing in the opposite direction of the flow direction of the main stream and the open end of the anode in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and

[0234] · The anode and the cathode are arranged so that a plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode, and

[0235] ii) The second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream, the second reactor section,

[0236] · A first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and

[0237] · Means for an outlet for recovering components from the reactor above - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream -

[0238] Includes,

[0239] · The first subsection comprises at least one second supply line for introducing a gas mixture including C1- to C4-alkanes and acetylene into the second reactor section, wherein the position of the at least one second supply line along the flow direction of the main stream defines the inlet of the second reactor section and the first subsection, and

[0240] · The at least one second supply line is arranged so that the gas mixture containing C1- to C4-alkanes and acetylene introduced into the reactor through the at least one second supply line is introduced into the plasma gas at a downstream location of the foot points of the electric arc in the direction of flow of the main stream, thereby forming a mixture from the plasma gas exiting the plasma section and the gas mixture containing C1- to C4-alkanes and acetylene of the at least one second supply line, which can be formed in the first subsection of the second reactor section downstream of the at least one second supply line, and the at least one second supply line for introducing the gas mixture containing C1- to C4-alkanes and acetylene into the second reactor section is fluidly connected to an acetylene-containing gas supply device.

[0241] Embodiment 6: An apparatus according to Embodiment 5 for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the at least one second supply line for introducing the gas mixture comprising C1- to C4-alkane and acetylene is fluidly connected to a C1- to C4-alkane-containing gas supply device.

[0242] Embodiment 7: An apparatus according to Embodiment 5 or 6 for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, said apparatus comprising:

[0243] iii) at least one device for concentrating a solid component (preferably carbon black) formed in the reactor above—the at least one device for concentrating a solid component (preferably carbon black) concentrates the solid component (preferably carbon black) of the mixture by separating a gaseous component from the solid component (preferably carbon black) of the mixture, and the at least one device for concentrating a solid component (preferably carbon black) concentrates,

[0244] · Fluidly communicating with the discharge means of the above reactor, and

[0245] · having at least one outlet for a stream containing a solid component (preferably carbon black) at a concentration concentrated compared to the mixture introduced into the at least one device for concentrating the solid component (preferably carbon black), and

[0246] · having at least one outlet for a stream comprising a solid component (preferably carbon black) at a reduced concentration compared to the mixture and a gaseous component of said mixture, which is fed into said at least one device for concentrating the solid component (preferably carbon black) -; and

[0247] iv) at least one device for concentrating hydrogen from a stream comprising a solid component (preferably carbon black) at a reduced concentration compared to the mixture flowing into the at least one device for concentrating a solid component (preferably carbon black) and a gaseous component of the mixture—the at least one device for concentrating hydrogen,

[0248] · Fluidly communicating with the outlet of the at least one device for concentrating the solid component (preferably carbon black) of the mixture for a stream comprising the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black), and

[0249] · having at least one outlet for a stream containing hydrogen at a concentrated concentration and, preferably, acetylene at a reduced concentration, compared to a stream containing a gaseous component of the mixture and a reduced concentration of a solid component (preferably, carbon black) introduced into at least one device for hydrogen concentration, and

[0250] · having at least one outlet for a stream comprising hydrogen and acetylene at a reduced concentration compared to a stream comprising a gaseous component of the mixture and a reduced concentration of a solid component (preferably carbon black) introduced into the at least one device for hydrogen concentration [preferably acetylene at a concentrated concentration compared to a stream comprising a gaseous component of the mixture and a reduced concentration of a solid component (preferably carbon black) introduced into the at least one device for hydrogen concentration], and the stream or a portion thereof is introduced through an inlet of the at least one second supply line of the reactor to introduce the gas mixture comprising C1- to C4-alkanes and acetylene into a first subsection of the second reactor section.

[0251] Includes

[0252] Embodiment 8: An apparatus according to Embodiment 7 for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the apparatus comprises a device for concentrating the acetylene concentration of a stream containing acetylene with a reduced concentration of hydrogen relative to a stream containing a gaseous component of the mixture and a reduced concentration of a solid component (preferably, carbon black), and the apparatus comprises,

[0253] · having an inlet for an acetylene-containing gas that fluidly communicates with the outlet of the device for hydrogen enrichment for a stream containing hydrogen and acetylene at reduced concentrations compared to the stream containing the gaseous component of the mixture and the solid component at reduced concentration,

[0254] · The device for acetylene concentration has an outlet for a stream having a reduced acetylene concentration compared to the stream flowing into the inlet of the device, and

[0255] · It has an outlet for a stream having a concentrated acetylene concentration compared to the stream introduced through the inlet, the outlet being fluidly connected to the inlet of the at least one second supply line for introducing a gas mixture containing C1- to C4-alkanes and acetylene into the first subsection of the second reactor section.

[0256] Embodiment 9: A method according to any one of Embodiments 5 to 8 for the production of hydrogen and solid carbon, wherein the apparatus further comprises the features of the apparatus described in the appended claims and in this description.

[0257] Example 10: Use of a reactor described in any one of Examples 5 to 9 in the method described in any one of Examples 1 to 4.

[0258] In some embodiments, there is a storage tank for an acetylene-containing gas from a stream containing hydrogen and acetylene at reduced concentrations compared to a stream containing a gaseous component of the mixture and a reduced concentration of a solid component (preferably carbon black).

[0259] Additionally, the device may include a control unit for controlling the flow rate to the inlet of the at least one second supply line of the stream containing hydrogen and acetylene at reduced concentrations compared to the stream containing the gaseous component of the mixture and a reduced concentration of the solid component (preferably, carbon black), wherein the at least one second supply line is intended to introduce the gas mixture containing C1- to C4-alkanes and acetylene into the first subsection of the second reactor section. In some embodiments, the control unit controls the flow rate according to selected boundary conditions [e.g., electricity rates (if electricity rates are high, more acetylene is supplied to the reactor)] or according to process stages. For example, a higher flow rate is selected at the start stage (when more energy is required to raise the temperature). Lower flow rates may be selected at other process stages. If necessary, other parameters such as the flow rate of the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the second supply line, the flow rate of the plasma gas, or specific electrical energy are also adjusted accordingly. This also applies to the method of this aspect, and thus the method may include the step of controlling the flow rate of the stream or a portion thereof containing hydrogen and acetylene at reduced concentrations relative to the stream containing the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black) to the inlet of the at least one second supply line, said at least one second supply line is intended to introduce the gas mixture containing C1- to C4-alkane and acetylene into the first subsection of the second reactor section. Such flow rate control is performed by the control unit described above.

[0260] An apparatus for acetylene concentration includes, for example, an absorption column and a desorption column, but is not limited thereto. In the absorption column, acetylene is washed away from the gas stream, and the desorption column recovers the scrubbing medium and releases the previously absorbed acetylene at a higher concentration.

[0261] The invention and independent aspects defined in the appended claims are further illustrated in a non-limiting manner by the following embodiments and drawings.

[0262] Examples

[0263] Drawing symbols have the following meanings:

[0264] 10: Device of the present invention

[0265] 15: Thermal plasma reactor

[0266] 20: Plasma section of the reactor

[0267] 21: Electric arc

[0268] 22: A part of the plasma section volume that defines the reference volume, starting from the uppermost upstream position where the inner surface of the anode's hollow channel faces the electric arc to the end of the plasma section of the reactor.

[0269] 23: Direction of Mainstream Flow

[0270] 24: In the direction of the main stream flow, the gap between the cathode end facing the direction of the main stream flow (lower end of the cathode) and the anode end facing the opposite direction of the main stream flow (upper end of the anode).

[0271] 30: Second Reactor Section

[0272] 31: First subsection of the second reactor section

[0273] 32: Second subsection of the second reactor section

[0274] 33: Means of outlet of the second reactor section

[0275] 40: Cathode (metal-based and water-cooled)

[0276] 50: Anode (metal-based and water-cooled)

[0277] 60: First supply line

[0278] 70: 2nd supply line

[0279] 71: The uppermost upstream point in the direction of flow of the main stream, wherein the flow cross-section across the direction of flow of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the direction of flow of the main stream within the area of ​​the foot points of the electric arc on the inner surface of the hollow channel of the anode.

[0280] 72: Inlet for line 144 connecting outlet 142 to the second supply line (70)

[0281] 80: Third supply line

[0282] 90: C1- to C4-alkane-containing gas supply unit (natural gas supply)

[0283] 100: Electrical insulator

[0284] 110: Device for inducing a vortex of C1- to C4-alkane-containing plasma gas before it enters a plasma section

[0285] 120: Heat exchanger

[0286] 130: Device for concentrating solid components (preferably, carbon black)

[0287] 131: Inlet of device 130

[0288] 132: Outlet for a stream having a concentrated solid component (preferably, carbon black).

[0289] 133: Outlet for a stream having a reduced concentration of solid components (preferably, carbon black).

[0290] 140: Device for hydrogen enrichment

[0291] 141: Inlet of device 140

[0292] 142: Outlet for streams containing acetylene and reduced concentration hydrogen

[0293] 143: Outlet for streams having concentrated hydrogen

[0294] 144: A line connecting an outlet for a stream having acetylene and reduced concentration of hydrogen to a second supply line (70).

[0295] 145: Branch of line 144

[0296] The dashed arrows are intended to illustrate the flow of different gas streams. For example, the arrow extending from supply line 60 illustrates the flow of plasma gas into the gap between the anode (50) and the cathode (40). The same applies to the second supply line (70) and the third supply line (80) and their corresponding dashed arrows. The dashed arrow 23 illustrates the flow of the main stream passing through the reactor. As is evident from FIGS. 1 and 2, the gas introduced through the second and third supply lines is injected to cross the flow direction of the main stream.

[0297] FIG. 1 shows one embodiment of an apparatus (10) of the present invention for producing hydrogen and solid carbon from natural gas. The apparatus (10) includes a reactor (15) that generates a thermal plasma using an electric arc. The apparatus further includes a C1- to C4-alkane-containing gas supply device (natural gas supply) (90), a heat exchanger (120), a solid component concentration device (130), and a hydrogen concentration device (140). The C1- to C4-alkane-containing gas (here, natural gas) supply means (90) provides natural gas to the reactor. An exemplary natural gas composition has the following composition: Natural gas consisting of about 98 vol.% methane, 1 vol.% another alkane (ethane, propane, butane, pentane), and 1 vol.% inert gas. (CIS countries).

[0298] The reactor (15) comprises a plasma section (20) and a second reactor section (30), wherein the second reactor section (30) is located immediately after the plasma section of the reactor in the flow direction of the main stream (23). The plasma section (20) comprises an anode (50) and a cathode (40) for generating an electric arc, wherein the arc expands within the plasma section and rotates about its axis by a vortex of C1- to C4-alkane-containing plasma gas induced by a device (110) that induces a vortex of C1- to C4-alkane-containing plasma gas before it is introduced into the plasma section. Additionally, the plasma section comprises at least one first supply line (60) for introducing C1- to C4-alkane-containing plasma gas into the plasma section of the reactor. The above cathode (40) is cylindrical and has a hollow channel having a main axis that extends along the flow direction of the main stream (23) in the plasma section.

[0299] The anode is cylindrical and has a hollow channel along the flow direction of the main stream of the plasma gas. The hollow channel has an inner surface. Additionally, the channel has an outlet in the flow direction of the main stream of the plasma gas, which forms an open end of the anode in the flow direction of the main stream. Furthermore, the channel has at least one inlet for receiving a C1- to C4-alkane-containing plasma gas (here, natural gas) introduced into the plasma section of the reactor through at least one first supply line, which forms an open end of the anode facing in the opposite direction of the flow direction of the main stream. The anode is configured so that the plasma gas can flow along the hollow channel through the open end of the anode facing in the opposite direction of the flow direction of the main stream and the open end of the anode facing in the flow direction of the main stream, and the plasma gas comes into contact with the inner surface of the hollow channel of the anode when passing through the anode.

[0300] The anode and cathode are concentric. The hollow channel of the cathode has two opposite ends, the end facing opposite the direction of flow of the main stream is closed, and the end facing the direction of flow of the main stream of the plasma gas is open and is located concentrically upstream of the open end of the anode facing opposite the direction of flow of the main stream. The cathode is located upstream of the open end of the anode facing opposite the direction of flow of the main stream, and the anode and cathode are arranged so that the foot points of the electric arc (21) contact the inner surface of the hollow channel of the anode and the inner surface of the hollow channel of the cathode, respectively. Through this, the generated electric arc is formed in the plasma section, thereby forming a plasma gas in the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line. As illustrated in FIG. 1, the anode and the cathode are arranged such that a gap (24) exists in the direction of the main stream between the end of the cathode (the lower end of the cathode) facing the direction of the flow of the main stream and the end of the anode (the upper end of the anode) facing the opposite direction of the flow of the main stream. The length of the gap (24) is preferably at least 0.3 times, more preferably at least 0.5 times, the average inner diameter of the hollow channel of the anode in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode.The above at least one first supply line is arranged so that the plasma gas can be supplied into the volumes of the hollow cathode and anode through the vertical gap between the anode and the cathode when the plasma gas is introduced into the plasma section of the reactor through a device (110) that induces a vortex of the C1- to C4-alkane-containing plasma gas before it is introduced into the plasma section.

[0301] The second reactor section (30) comprises a first subsection (31) and a second subsection (32), the second subsection being located downstream immediately after the first subsection in the direction of flow of the main stream. Additionally, the second reactor section comprises an outlet means (33) for recovering components from the reactor, the outlet means being located at the end of the second reactor section in the direction of flow of the main stream. The first subsection comprises at least one second supply line (70) for introducing a C1- to C4-alkane-containing gas into the second reactor section, the at least one second supply line being arranged so that the C1- to C4-alkane-containing gas introduced into the reactor through the at least one second supply line is introduced into the plasma gas such that it crosses the direction of flow of the main stream at a downstream location of the foot points of the electric arc in the direction of flow of the main stream. Accordingly, a mixture is formed in the first subsection of the second reactor section from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line. Additionally, the first subsection of the second reactor section includes a flow cross-section across the flow direction of the main stream that is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the flow direction of the main stream in the range of foot points of the electric arc on the inner surface of the hollow channel of the anode at at least one point.

[0302] At the upstrip immediately preceding point 71, there is a rapid expansion of the flow cross section that crosses the flow direction of the main stream, which has an opening angle of about 90° with respect to the flow direction of the main stream. In the region from the foot points of the electric arc on the inner surface of the hollow channel of the anode to the expansion at the upstrip immediately preceding point 71, the flow cross section that crosses the flow direction of the main stream remains essentially the same. The rapid expansion causes back-mixing and vortices of the components as they pass through the second reactor section, particularly immediately after the rapid expansion. As a result, the residence time distribution of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line is widened.At least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and preferably, at least 10% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line There is a deviation of more than 10% in the number of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and more preferably, a deviation of more than 15%, and even more preferably more than 20% in the average residence time of all atoms of the mixture in the second reactor section.

[0303] In FIG. 1, the at least one second supply line (70) is upstream of the top upstream point (71) in the direction of flow of the main stream, where the flow cross-section across the direction of flow of the main stream is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode across the direction of flow of the main stream in the area of ​​the foot points of the electric arc on the inner surface of the hollow channel of the anode. The at least one second supply line (70) defines the inlet of the second reactor section (30) and its first subsection (31).

[0304] The volume of the plasma section from the uppermost upstream position, where the inner surface of the hollow channel of the anode (50) faces the electric arc (21), to the end of the plasma section of the reactor is 0.0001 to 0.4 m 3 The range of, preferably 0.001 to 0.2 m 3The volume is of the range, and a reference volume (22) is defined. The volume of the first subsection (31) of the second reactor section is in the range of 10 to 200 times the reference volume, preferably in the range of 20 to 100 times the reference volume. The total volume of the second reactor section is in the range of 20 to 2000 times the reference volume, preferably in the range of 40 to 1000 times the reference volume. At the location where the C1- to C4-alkane-containing gas of the at least one second supply line is introduced into the plasma gas, the plasma gas has an average temperature in the range of 1200 to 3000 ℃, preferably in the range of 1500 to 3000 ℃ and contains acetylene, and the mixture formed by introducing the C1- to C4-alkane-containing gas into the plasma gas through the at least one second supply line has an average temperature of 850 ℃ or higher, preferably 1050 ℃ or higher, and less than 3000 ℃ in the region range from the at least one second supply line to the end of the first subsection of the second reactor section, the second reactor section is configured such that the mixture has an average temperature of 850 ℃ or higher, preferably 1050 ℃ or higher, and less than 3000 ℃.

[0305] In addition, the second reactor section is configured such that the average temperature in the second subsection of the mixture obtained from the mixing of the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line and the reaction thereof is 650°C or higher, preferably 750°C or higher, more preferably 850°C or higher, and less than 1500°C at any point along the flow direction of the main stream, and the average temperature at the end of the second reactor section of the mixture obtained from the mixing of the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line and the reaction thereof is 200K or higher, preferably 400K or higher, more preferably 600K or higher, but lower than the average temperature of the plasma gas at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line.

[0306] In this embodiment, the reactor (15) includes at least one third supply line (80) for introducing additional C1- to C4-alkane-containing gas (natural gas) into the mixture. A cascade-like arrangement of these second and third supply lines improves temperature control along the path of the main flow.

[0307] Finally, the mixture is recovered to the reactor (15) through the outlet means (33). The mixture recovered from the reactor through the outlet means (33) contains acetylene in the range of 0.01 to 4 vol.%, preferably in the range of 0.1 to 1 vol.%. In this embodiment, the outlet means (33) of the reactor is connected to a heat exchanger (120) used to preheat the gas entering the reactor through the supply lines (60, 70, 80). Preheating the gas entering the reactor reduces the overall electrical energy cost and improves the reactor production capacity.

[0308] The mixture recovered through the above-mentioned outlet means (33) and passed through the heat exchanger (120) is introduced through the inlet (131) into a device (130) for concentrating the solid component (preferably carbon black) of the mixture. The device (130) may be a high-temperature cyclone. The device separates the gaseous component from the solid component of the mixture to concentrate the solid component of the mixture. The device (130) is in fluid communication with the outlet means (33) of the reactor. The device (130) has an outlet (132) for discharging a stream containing a solid component (preferably carbon black) at a concentration higher than that of the mixture introduced into the device for concentrating the solid component (preferably carbon black), and an outlet (133) for a stream containing a solid component (preferably carbon black) at a reduced concentration compared to the mixture introduced into the device for concentrating the solid component (preferably carbon black) and a gaseous component of the mixture. At least a portion of the solid component (preferably carbon black) produced in the reactor is discharged through the outlet (132) along with a stream containing a solid component (preferably carbon black) at a concentration higher than that of the mixture introduced into the solid component (preferably carbon black) concentration device.

[0309] The outlet (133) is fluidly connected to a device (140) for concentrating hydrogen from a stream containing the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black). This device increases the hydrogen content of the stream entering the device through the inlet (141). Additionally, the device has an outlet (143) for a stream containing hydrogen at a concentrated concentration and an outlet (142) for a stream containing hydrogen at a reduced concentration compared to the stream containing the gaseous component of the mixture and a reduced concentration of the solid component (preferably carbon black) entering the hydrogen concentrating device. The stream recovered from outlet 143 may be supplied to a hydrogen storage container (not shown). The stream exiting outlet 142 contains acetylene at an increased concentration compared to the stream recovered from outlet 143 and is supplied into the at least one second supply line (70) through line (144). The stream recovered from outlet 143 can be supplied to a storage container (not shown). Acetylene supplied into the first subsection of the second reactor section allows the C1- to C4-alkane-containing gas introduced into the second reactor section by the at least one second supply line to be heated more quickly through the heat release from the decomposition of acetylene. Additionally, the total electrical energy consumption can be reduced.

[0310] As can be seen from FIG. 1, the reactor does not include means for supplying a liquid medium into the second reactor section to quench the mixture. By not performing a quenching step in the second reactor section and recovering the mixture at a correspondingly higher temperature, more efficient preheating of the supply gas is possible and the overall energy balance of hydrogen and solid carbon production can be improved.

[0311] FIG. 2 shows an alternative embodiment of the present invention. This differs from the embodiment shown in FIG. 1 in that the uppermost upstream point (71) in the direction of flow of the main stream, which is at least 5 times, preferably at least 10 times, larger than the average flow cross-section of the anode in the area of ​​the foot points of the electric arc on the inner surface of the hollow channel of the anode, is located upstream of the inlet of the second reactor section.

[0312] The method of the present invention for producing hydrogen and solid carbon from C1- to C4-alkane-containing gases using thermal plasma can be carried out using the apparatus (10) described above. The method comprises the following steps:

[0313] a) a step of extracting C1- to C4-alkane-containing plasma gas from a C1- to C4-alkane-containing gas supply device (90); and

[0314] b) a step of introducing the C1- to C4-alkane-containing plasma gas extracted from the device (90) for extracting the C1- to C4-alkane-containing plasma gas into at least a first reactor (15) - the reactor is a reactor that generates thermal plasma using an electric arc, and the C1- to C4-alkane-containing plasma gas is introduced into the reactor through at least one first supply line (60) for introducing the C1- to C4-alkane-containing plasma gas into the plasma section (20) of the reactor (15) -; and

[0315] c) A step of generating an electric arc (21) extending within the plasma section (20) of the reactor to the anode (50) and cathode (40)—wherein the foot points of the electric arc contact the inner surface of the hollow channel of the anode and the inner surface of the hollow channel of the cathode, respectively. The rotation of the electric arc is induced through a device (110) that induces a vortex of the C1- to C4-alkane-containing plasma gas before it is introduced into the plasma section through the at least one first supply line (60). The axis of rotation of the electric arc is oriented in the direction of flow of the main stream (23). The rotation frequency of the electric arc around its axis is 0.1 s. -1 Ideally, more preferably 0.2 s -1 Ideally, and even more preferably 0.5 s -1 Lee Sang-im -; and

[0316] d) forming a plasma gas from a C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line (60) for introducing a C1- to C4-alkane-containing plasma gas into the plasma section (20) using the electric arc (21) in the plasma section (20) of the reactor; and

[0317] e) a step of introducing a C1- to C4-alkane-containing gas into the first subsection (31) of the second reactor section (30) through the at least one second supply line (70) for introducing the C1- to C4-alkane-containing gas into the second reactor section - the location of the at least one second supply line along the flow direction of the main stream defines the inlet of the second reactor section and its first subsection, where,

[0318] · The C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line is introduced laterally into the plasma gas at the downstream of the foot points of the electric arc (21) generated by the anode and cathode in the flow direction of the main stream (23), so that a mixture can be formed in the first subsection of the second reactor section downstream of the at least one second supply line from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line (70).

[0319] · At the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line (70), the plasma gas has an average temperature in the range of 1200 to 3000 ℃ and contains acetylene, so that the mixture formed by the introduction of the C1- to C4-alkane-containing gas into the plasma gas through the at least one second supply line has an average temperature of 850 ℃ or higher, preferably 1050 ℃ or higher, and less than 3000 ℃ in the region range from the at least one second supply line (70) to the end of the first subsection of the second reactor section -; and

[0320] f) a step of moving the mixture downstream in the flow direction of the main stream (23) through the second reactor section above - where,

[0321] · The movement is performed such that the average residence time of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the first subsection (31) of the second reactor section is in the range of 100 ms to 2000 ms, preferably in the range of 200 ms to 1000 ms, and

[0322] · The movement is performed such that the average residence time of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the entire second reactor section (30) is in the range of 200 ms to 20000 ms, preferably in the range of 400 ms to 10000 ms, and

[0323] At least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and preferably, at least 10% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line There is a deviation of 10% or more, and more preferably, a deviation of 15% or more, even more preferably 20% or more from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line, and

[0324] · Hydrogen is generated by reactions occurring in the mixture within the second reactor section and, preferably, also in the plasma section -; and

[0325] g) a step of controlling the average temperature of the mixture within the second subsection of the second reactor section to 650°C or higher, preferably 750°C or higher, more preferably 850°C or higher, and less than 1500°C - wherein the average temperature at the end of the second reactor section of the mixture of the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line is controlled to an average temperature of 200K or higher, preferably 400K or higher, more preferably 600K or higher, but lower than the average temperature of the plasma gas at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line -; and

[0326] h) recovering the mixture from the reactor through an outlet means (33) for recovering the mixture from the reactor and passing the mixture through a heat exchanger (120) - the outlet means (33) is located at the end of the second reactor section in the direction of flow of the main stream -; and

[0327] i) a step of treating the mixture exiting the heat exchanger (120) with a device (130) for concentrating the solid component (particularly carbon black) of the mixture, in order to generate a stream containing the solid component (particularly carbon black) of the mixture at a concentrated concentration and a stream containing the gaseous component of the mixture and the solid component (particularly carbon black) of the mixture at a reduced concentration; and

[0328] j) A step of processing a stream comprising a gaseous component of the mixture and a reduced concentration of a solid component of the mixture (preferably carbon black) using at least one device for generating a stream comprising a gaseous component of the mixture and a reduced concentration of a solid component of the mixture (preferably carbon black)—the stream having a reduced concentration of hydrogen is recovered at outlet 143, and the stream recovered at outlet 142 contains hydrogen at a reduced concentration compared to the stream comprising a gaseous component of the mixture and a reduced concentration of a solid component of the mixture (preferably carbon black). Stream 142 contains acetylene at a reduced concentration compared to stream 143.

[0329] The heat exchanger (120) is used to heat the stream from the supply device (90) before introducing it into the reactor through the inlets (60, 70, 80). Device 130 is used to concentrate the solid carbon (preferably carbon black) formed through the reaction in the reactor. Additionally, device 140 is used to concentrate the hydrogen of the mixture. A stream containing hydrogen at a concentrated concentration can be recovered through outlet 143 and supplied to a storage container. A stream recovered through outlet 142, containing hydrogen at a reduced concentration compared to a stream containing the gaseous component of the mixture and the solid component of the mixture at a reduced concentration, contains acetylene, preferably at an increased concentration compared to the stream entering through the inlet (141). A stream containing acetylene recovered through outlet 142 can be supplied to an inlet (72) of the at least one second supply line (70) via line (144). In another preferred embodiment, the stream recovered through outlet 142 is supplied via line (144) to an acetylene concentration enrichment device (not shown) fluidly connected to the inlet (72). The acetylene concentration enrichment device has an outlet for a stream containing acetylene at an increased concentration relative to the supply stream of the device fluidly connected to the inlet (72). This stream can be supplied into the at least one second supply line (70) via the inlet (72).

[0330] In another embodiment of the device and method described herein, an additional heat exchanger (not shown in FIG. 1 and FIG. 2) is placed between the heat exchanger (120) and the separation device (130) and is used for steam generation.

[0331] In some embodiments, a heat exchanger (120) is connected so that heat from the mixture recovered through the outlet (33) is transferred to a stream transferred through the line (144) to the inlet (72), thereby allowing the stream to be heated before being injected into a stream flowing into the first subsection of the second reactor section through the at least one second supply line (70).

[0332] In addition, the above-described device can be used for the method of the present invention, particularly for the process of the above-described method.

Claims

Claim 1 An apparatus for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, wherein the apparatus comprises at least one reactor that generates thermal plasma using an electric arc, and wherein the reactor comprises a plasma section and a second reactor section, i) wherein the plasma section comprises: an anode and a cathode for generating an electric arc—the arc extending within the plasma section—, and at least one first supply line for introducing a C1- to C4-alkane-containing plasma gas into the plasma section of the reactor, wherein the anode comprises a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel having an inner surface—an outlet in the flow direction of the main stream of the plasma gas—the outlet forming an open end of the anode in the flow direction of the main stream—and a method for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through the at least one first supply line. It includes at least one inlet—said that the inlet forms an open end of the anode facing opposite to the flow direction of the main stream—and the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing opposite to the flow direction of the main stream and the open end of the anode facing in the flow direction of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and· The anode and the cathode are arranged such that a plasmaeous plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode; ii) the second reactor section located downstream immediately after the plasma section of the reactor in the direction of the flow of the main stream comprises: · a first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of the flow of the main stream -, and · outlet means for recovering components from the reactor - the outlet means is located at the end of the second reactor section in the direction of the flow of the main stream -, · The first subsection comprises at least one second supply line for introducing a C1- to C4-alkane-containing gas into the second reactor section, and · the at least one second supply line is arranged such that the C1- to C4-alkane-containing gas introduced into the reactor through the at least one second supply line is introduced into the plasma-containing plasma gas at a downstream location of the foot points of the electric arc in the flow direction of the main stream, thereby allowing a mixture to be formed from the plasma-containing plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line in the first subsection of the second reactor section downstream of the at least one second supply line.· The location of the at least one second supply line along the flow direction of the main stream defines the beginning of the second reactor section and its first subsection, and · The volume of the plasma section from the uppermost upstream position, where the inner surface of the hollow channel of the anode faces the electric arc, to the end of the plasma section of the reactor is 0.0001 to 0.4 m, 3 An apparatus for producing hydrogen and solid carbon, comprising: a volume of the range of, defining a reference volume; wherein the volume of the first subsection of the second reactor section is in the range of 10 to 200 times the reference volume; wherein the total volume of the second reactor section is in the range of 20 to 2000 times the reference volume; and wherein the reactor comprises, at least one point within the first subsection of the second reactor section and / or within the plasma section, a flow cross-section across the main stream flow direction that is at least 5 times larger than the average flow cross-section of the anode across the main stream flow direction in the range of the foot points of the electric arc on the inner surface of the hollow channel of the anode, wherein, if included within the plasma section, the flow cross-section is included within the range of the area downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the main stream flow direction to the end of the plasma section. Claim 2 An apparatus for producing hydrogen and solid carbon, wherein, in claim 1, the apparatus further comprises at least one device for concentrating a solid component formed within the reactor, the at least one device for concentrating a solid component concentrates the solid component of the mixture by separating a gaseous component from the solid component of the mixture, and the at least one device for concentrating a solid component is fluidly connected to the outlet means of the reactor, and has at least one outlet for a stream containing a solid component at a concentration concentrated relative to the mixture that flows into the at least one device for concentrating a solid component, and at least one outlet for a stream containing a solid component at a concentration reduced relative to the mixture and a gaseous component of the mixture that flows into the at least one device for concentrating a solid component. Claim 3 In paragraph 2, the apparatus further comprises at least one device for concentrating hydrogen from a stream comprising a solid component at a reduced concentration relative to the mixture and a gaseous component of said mixture, wherein the at least one device for concentrating hydrogen comprises: · fluidly communicating with the outlet of the at least one device for concentrating the solid component of said mixture for a stream comprising the gaseous component of said mixture and a reduced concentration of the solid component of said mixture; · having at least one outlet for a stream comprising hydrogen at a concentrated concentration relative to the stream comprising the gaseous component of said mixture and a reduced concentration of the solid component of said mixture for concentrating the hydrogen; and · having at least one outlet for a stream comprising hydrogen at a reduced concentration relative to the stream comprising the gaseous component of said mixture and a reduced concentration of the solid component of said mixture for concentrating the hydrogen for concentrating the hydrogen. Claim 4 In any one of claims 1 to 3, · between the foot points of the electric arc on the inner surface of the hollow channel of the anode and the uppermost upstream point in the flow direction of the main stream, there exists one or more rapid expansion portions of the flow cross-section crossing the flow direction of the main stream - the flow cross-section crossing the flow direction of the main stream at the uppermost upstream point is at least 5 times larger than the average flow cross-section of the anode crossing the flow direction of the main stream within the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode, and the rapid expansion portion has an opening angle of at least 20° with respect to the axis of the main stream in the flow direction of the main stream -; and / or · the flow cross-section across the flow direction of the main stream in the area range from the foot points of the electric arc on the inner surface of the hollow channel of the anode to the top upstream point in the flow direction of the main stream, at any point, is 60% or more of the average flow cross-section across the flow direction of the main stream at the foot points of the electric arc on the inner surface of the hollow channel of the anode - the flow cross-section across the flow direction of the main stream at the top upstream point is 5 times or more larger than the average flow cross-section of the anode across the flow direction of the main stream in the area range of the foot points of the electric arc on the inner surface of the hollow channel of the anode -, apparatus for producing hydrogen and solid carbon. Claim 5 In paragraph 4, the reactor comprises means for detachably connecting the anode or a portion of the anode to the remainder of the reactor; and / or the corresponding anode and cathode do not overlap at least partially in the direction of flow of the main stream; and / or the anode and / or cathode are cooling electrodes, an apparatus for producing hydrogen and solid carbon. Claim 6 An apparatus for producing hydrogen and solid carbon according to any one of claims 1 to 3, wherein the anode and the cathode are concentric, the cathode has a hollow channel having a main axis extending along the flow direction of the main stream, the hollow channel has two opposite ends, the end facing opposite the flow direction of the main stream is closed, and the end facing the flow direction of the main stream of the plasma gas is open and is located upstream of the open end of the anode facing opposite the flow direction of the main stream and is concentric with the open end of the anode, and the anode and the cathode are arranged such that the foot points of the electric arc contact the inner surface of the hollow channel of the cathode and the inner surface of the hollow channel of the anode, respectively. Claim 7 An apparatus for producing hydrogen and solid carbon, wherein, in any one of claims 1 to 3, the at least one reactor is configured such that the at least one second supply line introduces the C1- to C4-alkane-containing gas into the plasma gas, such that the supply line is introduced across the flow direction of the main stream; and / or, the at least one reactor has at least one third supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section, and the at least one third supply line for introducing the C1- to C4-alkane-containing gas is positioned downstream of the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section in the flow direction of the main stream; and / or, the second reactor section comprises at least one device for inducing turbulence and / or backmixing of the mixture. Claim 8 An apparatus for producing hydrogen and solid carbon according to any one of claims 1 to 3, wherein at least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line. Claim 9 A method for producing hydrogen and solid carbon from a C1- to C4-alkane-containing gas using thermal plasma, comprising: a) withdrawing a C1- to C4-alkane-containing plasma gas from a C1- to C4-alkane-containing gas supply device; b) introducing the C1- to C4-alkane-containing plasma gas withdrawn from the C1- to C4-alkane-containing gas supply device into at least a first reactor; wherein the reactor is a reactor that generates thermal plasma using an electric arc, and the reactor comprises a plasma section and a second reactor section, and i) the plasma section comprises: an anode and a cathode for generating an electric arc—the arc extends within the plasma section—and at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section of the reactor, wherein the anode is a hollow channel along the flow direction of the main stream of the plasma gas—the hollow channel has an inner surface The apparatus comprises: an outlet facing the direction of flow of the main stream of the plasma gas—the outlet forms an open end of the anode facing the direction of flow of the main stream—and at least one inlet for receiving the C1- to C4-alkane-containing plasma gas introduced into the plasma section of the reactor through at least one first supply line—the inlet forms an open end of the anode facing the opposite direction of flow of the main stream—the anode is configured such that the plasma gas can flow along the hollow channel through the open end of the anode facing the opposite direction of flow of the main stream and the open end of the anode facing the direction of flow of the main stream, and the plasma gas contacts the inner surface of the hollow channel of the anode when passing through the anode, and· The anode and the cathode are arranged such that a plasma gas can be formed within the plasma section from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line by the arc generated by them being formed within the plasma section, and the foot points of the electric arc in contact with the anode are located on the inner surface of the hollow channel of the anode; ii) the second reactor section located downstream immediately after the plasma section of the reactor in the direction of flow of the main stream comprises: · a first subsection and a second subsection - the second subsection is located downstream immediately after the first subsection in the direction of flow of the main stream -, and · an outlet means for recovering components from the reactor - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream -, wherein · the first subsection is for the C1- to C4-alkane-containing gas to the second reactor c) a step of generating an electric arc extending within the plasma section of the reactor to the anode and cathode; d) using the electric arc in the plasma section of the reactor, wherein the position of the at least one second supply line along the flow direction of the main stream defines the inlet of the second reactor section and its first subsection, and the C1- to C4-alkane-containing plasma gas is introduced into the reactor through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section of the reactor; c) a step of generating an electric arc extending within the plasma section of the reactor to the anode and cathode; and d) using the electric arc in the plasma section of the reactor,A step of forming a plasma gas from the C1- to C4-alkane-containing plasma gas introduced into the plasma section through the at least one first supply line for introducing the C1- to C4-alkane-containing plasma gas into the plasma section; e) a step of introducing the C1- to C4-alkane-containing gas into the first subsection of the second reactor section through the at least one second supply line for introducing the C1- to C4-alkane-containing gas into the second reactor section, wherein the C1- to C4-alkane-containing gas introduced into the second reactor section through the at least one second supply line is introduced as the plasma gas downstream of the foot points of the electric arc generated by the anode and cathode in the flow direction of the main stream, thereby allowing the mixture to exit the plasma section at the first subsection of the second reactor section downstream of the at least one second supply line. The inflow is performed so as to be formed from the gas and the C1- to C4-alkane-containing gas introduced into the first subsection of the second reactor section through the at least one second supply line, and at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas has an average temperature in the range of 1200 to 3000 ℃ and contains acetylene,A mixture formed by introducing the C1- to C4-alkane-containing gas into the plasma gas through the at least one second supply line has an average temperature of 850°C or more and less than 3000°C in the region from the at least one second supply line to the end of the first subsection of the second reactor section; f) a step of moving the mixture downstream in the flow direction of the main stream through the second reactor section, wherein · the movement is performed such that the average residence time of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the first subsection of the second reactor section is in the range of 100 ms to 2000 ms, and · the average residence time of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within the entire second reactor section The above movement is performed so as to be in the range of 200ms to 20,000ms, and at least 5% of the atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line have a residence time in the second reactor section that deviates by at least 5% in absolute numbers from the average residence time in the second reactor section of all atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line.· Hydrogen and solid carbon are produced by reactions occurring in the mixture within the second reactor section; g) a step of controlling the average temperature of the mixture within the second subsection of the second reactor section to 650°C or higher - the average temperature at the end of the second reactor section of the mixture of the plasma gas and the C1- to C4-alkane-containing gas introduced through the at least one second supply line is controlled to an average temperature of 200K or higher, but lower than the average temperature of the plasma gas at the location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line -; and h) a step of recovering the mixture at the end of the reactor through an outlet means for recovering the mixture from the reactor - the outlet means is located at the end of the second reactor section in the direction of flow of the main stream - comprising, a method. Claim 10 In claim 9, the method further comprises the step of i) treating the mixture recovered through the outlet means with at least one device for concentrating the solid component of the mixture in order to generate a stream containing the solid component of the mixture at a concentrated concentration and a stream containing the gaseous component of the mixture and the solid component of the mixture at a reduced concentration; and the average residence time of atoms of the mixture formed from the plasma gas exiting the plasma section and the C1- to C4-alkane-containing gas of the at least one second supply line within a region range from the beginning of the second reactor section to the device for concentrating the solid component of the mixture is in the range of 200 ms to 20000 ms. Claim 11 In claim 10, the method further comprises the step of j) processing the stream comprising the gaseous component of the mixture and the solid component of the mixture at a reduced concentration using at least one device for generating a stream having a concentrated concentration of hydrogen compared to the stream comprising the gaseous component of the mixture and the solid component of the mixture at a reduced concentration. Claim 12 A method according to any one of claims 9 to 11, wherein the reactor comprises, at least 5 times larger than the average flow cross-section of the anode across the flow direction of the main stream in the region of the foot points of the electric arc on the inner surface of the hollow channel of the anode, a flow cross-section across the flow direction of the main stream at least at one point within the first subsection of the second reactor section and / or within the plasma section, wherein if included within the plasma section, the flow cross-section is included within the region of the end of the plasma section as downstream of the foot points of the electric arc on the inner surface of the hollow channel of the anode in the flow direction of the main stream. Claim 13 A method according to any one of claims 9 to 11, wherein the C1- to C4-alkane-containing gas is introduced into the plasma plasma gas through the at least one second supply line so as to cross the flow direction of the main stream; and / or at least a third inflow is performed to introduce the C1- to C4-alkane-containing gas into the second reactor section, wherein the third inflow is performed through at least one third supply line positioned downstream of the at least one second supply line to introduce the C1- to C4-alkane-containing gas into the second reactor section in the flow direction of the main stream. Claim 14 A method according to any one of claims 9 to 11, wherein: · solid carbon dispersed in a hydrogen and / or C1- to C4-alkane-containing gas is directly introduced into the second reactor section; and / or · at a location where the C1- to C4-alkane-containing gas is introduced into the plasma gas through the at least one second supply line, the plasma gas comprises 2 vol.% or more of acetylene; and / or · the electric arc generated by the anode and cathode rotates about an axis extending from the cathode to the anode. Claim 15 A method according to any one of claims 9 to 11, wherein additional turbulence and / or backmixing in the mixture is induced in the second reactor section. Claim 16 A method according to any one of claims 9 to 11, wherein the anode and cathode of the at least first reactor are concentric, the cathode has a hollow channel having a main axis extending along the flow direction of the main stream, the hollow channel has two opposite ends, the end facing opposite the flow direction of the main stream is closed, and the end facing the flow direction of the main stream of the plasma gas is open and is located upstream of the open end of the anode facing opposite the flow direction of the main stream and is concentric with the open end of the anode, and the anode and cathode are arranged such that the foot points of the electric arc contact the inner surface of the hollow channel of the anode and the inner surface of the hollow channel of the cathode, respectively; and / or the C1- to C4-alkane-containing gas of the plasma gas and / or the at least one second supply line is a gas containing methane or natural gas. Claim 17 delete

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