RU2778871C2 - Device with solid-state nozzle for endothermal reactions with direct electrical heating - Google Patents

Abstract

FIELD: electrical engineering.

SUBSTANCE: invention relates to the field of electrical engineering, namely to a device with a solid-state nozzle for endothermal reactions with direct electrical heating; it can be used in cracking of oil fractions or hydrocarbon pyrolysis at a temperature between 500 and 1700°C. At least one vertically located pair of electrodes (4, 5) and all electrodes are installed in electroconductive solid-state nozzle (26), while upper and lower sections of the device have specific conductivity from 10⁵ to 10⁸ S/m, a middle section of the device is electrically isolated from the solid-state nozzle, an upper electrode is connected through the upper section of the device, and a lower electrode is connected through the lower section of the device, or each of electrodes is connected through one or several connecting elements (10, 16) electrically contacting with the specified sections, while the ratio of a cross-sectional area of upper and lower electrodes to a cross-sectional area of the corresponding conductive connecting element, or without the use of the connecting element, the ratio of the cross-sectional area of upper and lower electrodes to a cross-sectional area of the corresponding conductive section of the device is from 0.1 to 10.

EFFECT: increase in the efficiency of use of endothermal reaction heat in a heating zone of a reactor, which withstands a pressure drop of more than 0.5 bar.

15 cl, 25 dwg

Description

The present invention relates to a heated device with a packing for endothermic reactions, which can be divided into the upper, middle and lower sections of the device, and the upper and lower sections of the device are electrically isolated from the middle section of the device, with at least one vertically located pair of electrodes, which connected through a pressure-resistant jacket of the device in the upper and lower sections of the device, and with an electrically conductive solid-state nozzle, which is electrically isolated from the side wall of the middle section of the device.

Strongly endothermic reactions are often the beginning of the production chain in the chemical industry, for example, in the cracking of petroleum fractions, the reforming of natural gas or naphtha, the dehydrogenation of propane, the dehydroaromatization of methane to benzene, or the pyrolysis of hydrocarbons. Temperatures between 500 and 1700°C are required to achieve technically and economically attractive yields. The reason for this lies mainly in the thermodynamic limitation of the equilibrium conversion.

Endothermic high temperature reactions pose two main requirements for technical implementation: first, high energy density heat input at the required reaction temperature, and second, integrated heat recovery between product and feed streams. Thanks to the integrated heat recovery, the temperature difference between the storage temperature of the products/starting materials and the desired reaction temperature can be made up with minimal energy consumption.

Fluidized bed reactors are used in the prior art for heat-integrated endothermic processes (Levenspiel, O. (1988), Chemical engineering's grand adventure. Chemical Engineering Science, 43 (7), 1427-1435). Various concepts are used to supply heat to an endothermic reaction.

US 2002/0007594 discloses a process for the parallel production of hydrogen and carbonaceous products in which natural gas is introduced into the reaction space and thermally decomposed in the presence of a carbon rich solid. US 2002/0007594 discloses that the carbonaceous solid is heated in a reactor separate from the thermal decomposition reaction space. Heating occurs by means of exhaust gases arising from the combustion of hydrocarbons or hydrogen. The heated solid is then introduced into the reaction space.

The disadvantage of using a solid as a heat transfer medium is that the solid must be heated above the reaction temperature level in a separate combustion chamber and circulate between the combustion chamber and the reaction chamber. Hot solid operation results in extreme thermal and mechanical stress on the reactor and controls. In addition, the flow of solid particles is associated with the heat demand of the reaction, and a uniform distribution of mass flows across the cross section is a necessary condition to achieve optimal heat integration. Therefore, the ratio between the gas flow and the solids flow can only be controlled within a narrow range.

International application WO 2013/004398 discloses that the thermal energy for the heat transfer medium is generated outside the reaction space and a gaseous heat transfer medium is used which is inert to the decomposition reaction and/or is the product of said reaction. The disadvantage is that the flow of solid particles is associated with the requirements of heat integration. In addition, the decomposition reaction product stream passes through a temperature drop region in which a reverse reaction can take place.

The prior art (eg, US Pat. No. 6,331,283) further discloses autothermal processes in which the heat required for an endothermic reaction is generated from an exothermic co-reaction in the same reaction space. The disadvantage of these autothermal methods is the contamination of the stream of gaseous products with flue gases, for example, in the case of pyrolysis of hydrocarbons, the removal of carbon-containing components into a hydrogen-rich product stream. In addition, losses in the yield of the product are unfavorable, in the case of the pyrolysis of hydrocarbons, a significant loss of pyrolysis carbon.

Therefore, heat can be transferred indirectly, for example recuperatively (eg EP 15168206) or via heat pipes (eg US 4372377) from an exothermic to an endothermic reaction chamber. The disadvantage of this concept is the complex structures in the hot section of the reaction chamber, which put forward high material and structural requirements for sealing and avoiding thermal stresses. In addition, these internal structures interfere with the flow of solid particles. Another problem with this concept is the fouling of the heat exchanger surfaces; for example, in the case of pyrolysis of hydrocarbons, the deposition of pyrolytic carbon preferably occurs on hot surfaces.

US Pat. No. 2,982,622 describes thermally integrated pyrolysis of hydrocarbons in a moving bed of inert materials. Temperatures above 1200°C required for pyrolysis are achieved by electrical heating. In the two figures of US Pat. No. 2,982,622, the electrodes are positioned horizontally. The possibility of a vertical arrangement is disclosed in the description. It can be deduced from the figure of US 2982622 that the electrode inlets are located in the hot zone of the reactor. As a result of this, several disadvantages appear; on the one hand, the electrode bushings form a thermal bridge, which can cause significant heat losses, and on the other hand, the bushing itself is mechanically complex, since it must pass through layers with different thermal expansion, i.e. the reactor wall is made of steel, and the heat-insulating layers are made of mineral materials. As a result, the bushing may experience high bending moments. In addition, the electrode leads must have a high temperature resistance and therefore a certain electrical resistance of the material must be taken into account; usually graphite is used.

US Pat. No. 2,799,640 describes the production of acetylenes in a fluidized bed reactor, with the necessary energy supplied electrically. The electrodes can be placed horizontally or vertically. For vertical arrangement, an annular, spoke-like electrode array is disclosed. It is described that the vertical arrangement provides a good distribution of electric current throughout the space of the reactor. It can be seen from the figures in US Pat. No. 2,799,640 that for both the horizontal and vertical arrangement of the electrodes, the electrode inlets are in the hot zone of the reactor.

Austrian patent AT 175243 describes an electric furnace with two vertical electrodes for transferring current to bulk material, located in the furnace shaft, and the upper electrode is made in the form of a horizontal rectilinear hollow body with internal cooling and is located inside the packing of bulk material. In this disclosure, the electrode entry is also located in the hot zone of the reactor and passes through the lined reactor lid.

Swiss patent CH 278580 discloses a shaft furnace with two vertically arranged ring electrodes for transferring current to bulk material located in the shaft furnace, with the upper electrode located inside the bulk material packing, while the lower electrode is located directly above the gas inlet. In this disclosure, the electrode entry is also located in the hot zone of the reactor and passes through the side wall of the lined reactor.

US Pat. No. 3,259,565 discloses an electrically heated fluidized bed reactor for the pyrolysis of hydrocarbons. The document does not disclose any details about the geometric arrangement and design of the electrodes. Figure 2 of US Pat. No. 3,259,565 shows the entry of power lines through the side wall of the reactor. Therefore, this solution also has the disadvantages mentioned above.

A significant advantage of the horizontal arrangement of the electrodes is that the electrodes do not overlap the cross section of the reactor. In addition, in a horizontal arrangement, by means of vertically separated electrodes, the electric current and therefore the heat output can be distributed purposefully along the direction of flow.

The advantages of a vertical arrangement include the distribution of current over a large cross-sectional area of the reactor, in addition, the parallel orientation of the lines of electric potential in the direction of flow and the possibility of direct current over the entire height of the reactor.

US Pat. Nos. 5,903,591, US 5,406,582 and US 5,974,076 describe an apparatus and method for activating or regenerating carbon in an unpressurized tubular reactor which consists of two or more zones one above the other. The carbon at the upper end is introduced into the upper zone through a feed funnel which is connected to the reactor and is then directed to the respective subsequent zones through the funnel-shaped distributors. The reactor is electrically heated, and the electric current is supplied to the upper zone through the feed funnel, and to the middle zones through funnel-shaped distributors. This does not describe the details of the connections of the hopper, the connecting element and the electrodes. US Pat. No. 5,903,591 respectively discloses both electrode inlets in the hot zone of the reactor and a flat closure through an external hopper in the cold zone. The disadvantage of this invention is that the electric current is distributed to the carbon layer not only through the electrode, but also along the wall of the hopper. Another disadvantage is that the connection of the electrode to the conductive body creates additional contact resistances, which lead to undesirable dissipation of electrical energy into thermal energy. In addition, the interfaces of materials on the connecting elements are weak points for the mechanical stability of the electrodes. Finally, overlapping of the cross section with a graphite electrode formed in the form of a block leads to an uneven distribution of the flow of solids over the cross section of the reactor.

US Pat. No. 5,946,342 describes the production and activation of activated carbon in an electrically heated moving bed. Figure 3 of US Pat. No. 5,946,342 shows ring-shaped electrodes with a large cross-sectional area >50%. The electrodes are made of carbon and have pointed ends parallel to the direction of activated carbon flow. The specific contacting of the electrodes is not described; Figure 3 of US Pat. No. 5,946,342 shows that the contact is not through the reactor cap.

US Pat. No. 7,288,503 also describes the preparation and activation of activated carbon in an electrically heated fixed bed. Use rod electrodes; the electrodes are inserted through the lid and the electrodes are insulated from the lid (see FIG. 3 of US Pat. No. 7,288,503).

Patent application DE 10236019 A1 describes a reactor for carrying out endothermic reactions which is equipped with one or more heating blocks which completely fill the cross section of the reactor and which are electrically insulated from the inner wall of the reactor and optionally from each other, the heating blocks being formed of foam material with open pores. The type and method of contacting the electrodes is not described.

Despite the many advantages of electric heating:

(i) The heating power is basically constant over the entire temperature range and is not limited by the temperature of the heating medium.

(ii) The absence of fuel materials and coolant simplifies the design of the reactor and saves control loops for dosing the appropriate streams of materials in the periphery of the reaction zone. In addition, contamination/dilution of process streams with foreign substances is excluded. As a result, the operational reliability of the reactor is increased.

(iii) The heating power can be achieved in a simple reactor without built-in elements, i.e. with unstructured cross section. As a result, reliable scaling is ensured.

(iv) Heating has no local emission of harmful substances. When using regenerative sources that do not contain CO ₂ , heating is virtually completely free of emissions of harmful substances,

therefore, until now, the decisive disadvantage of heating has been that electricity is more expensive than fossil energy sources. However, this disadvantage should disappear in the next few years due to the transition to alternative energy sources.

In addition, there is still no concept of a reactor for the efficient input and uniform distribution of electrical energy in reactors with packings for endothermic gas-phase or gas-solid reactions at high temperatures. The approaches indicated in the cited prior art for contacting the electrodes through the reactor jacket turn out to be impracticable when implemented in practice. First, the introduction of electrical connections in the hot zone of the reactor is extremely costly and prone to breakage. Secondly, the contact of the electrodes with the current source is almost point-like. This feature has several disadvantages: Electric current is distributed unevenly over the cross section of the nozzle. In addition, the connecting elements that provide electrical contact between the electrodes have a small cross-sectional area and therefore a high electrical resistance. As a result, a significant part of the input electrical energy is dissipated in the connecting elements and in the electrode itself, in particular if it consists of graphite. Consequently, the electrical energy is underused in the reactor packing. In addition, the connecting elements and/or the electrode must be purposefully cooled, which requires an expensive and complex design of the device. Thirdly, the design of the electrodes and associated connectors is not scalable: consequently, the operating conditions in a test reactor with a small cross-sectional area are not representative of a technical device with a large cross-sectional area.

In industry, electrical heating is currently only used in a few large processes; for example, in the chemical gas-phase reaction of ammonia and hydrocarbons to produce hydrocyanic acid at temperatures from 1300 to 1600°C in a fluidized bed reactor of electrically conductive carbon particles, or in the production of calcium carbide in smelting reduction furnaces at temperatures from 2000°C to 2300°C. Figure 2 of US Pat. No. 3,157,468 shows a hydrocyanic acid reactor with vertically arranged rod-shaped electrodes, which has its own inlet for each electrode. Ullmann's encyclopedia, chapter "Calcium carbide", mentions pre-baked carbon electrodes or self-baking Soederberg electrodes. A common type in the prior art are Soderberg-type hollow electrodes. The electrodes work with three-phase alternating current and contact along their circumference with the cooled terminals. Since carbon is the starting material for the production of calcium carbide, the electrodes are consumed and need to be built up. The disadvantages of these designs are the laborious input of individual electrodes through the reactor vessel, since each input must be separately sealed and have electrical contacts, and must also provide the possibility of controlled axial movement of the electrode. In addition, the number of injections required increases in proportion to the cross-sectional area of the reactor.

In industrial reactors, the temperature difference between the central axis and the reactor vessel can be more than 500K. Under these operating conditions, open configurations of electrode arrays that are integral and rigidly fixed around the circumference may crack.

Currently, there is no commercially operated reactor with electrically heated packing for carrying out endothermic reactions in the gas phase or gas-solid-state reactions.

Most traditionally operated high temperature processes are heated using combustion furnaces. These methods cannot do without the export of energy for economically justified work; only about 50% of the heat generated in the process is actually used for the endothermic reaction. Therefore, complete thermal integration is as yet an unattainable goal.

Therefore, the object of the present invention was to demonstrate an adaptable, scalable electrically heated device concept, in particular the concept of a pressurized reactor, for a class of endothermic high temperature processes utilizing a structured space. Another task was to supply electrical energy to the heating zone of the device, in particular the reactor, with small losses. This means that preferably more than 99% of the electrical energy introduced into the device must be released in the heating zone. Another challenge was to ensure that the current flowed as evenly as possible along the entire length of the heating zone; whereby an approximately uniform heating of the packing and hence a linear interaction can be achieved. Another objective was to demonstrate a packed device, in particular a packed reactor, which has as complete thermal integration as possible. Another objective was that the tests in a small cross-sectional area test reactor should be representative of an industrial device, in particular an industrial reactor. In addition, the electrically heated apparatus, in particular the electrically heated reactor, should generally have a simple structure from a hardware point of view.

Unexpectedly, it was possible to demonstrate an electrically heated device with a pressure with a nozzle, in particular a reactor, with an upper (3), middle (1) and lower (3) section of the device, and in the middle section (1) at least one vertical located pair of electrodes (4,5), and all electrodes are installed/immersed in an electrically conductive solid nozzle (26), the upper and lower sections of the device have a conductivity from 10 ⁵ S/m to 10 ⁸ S/m, and the middle section of the device is electrically isolated from a solid nozzle, characterized in that the upper and lower sections of the device are electrically isolated from the middle section of the device, the upper electrode is connected through the upper section of the device, and the lower electrode is connected through the lower section of the device, or each of the electrodes is connected through one or more electrically contacting with the specified sections of the connecting elements (10, 16), and the ratio of the cross-sectional area of the upper and/or, n preferably and, the lower electrode to the cross-sectional area of the corresponding conductive connecting element or, without using a connecting element, the ratio of the cross-sectional area of the upper and/or, preferably, the lower electrode to the cross-sectional area of the corresponding conductive section of the device is from 0.1 to 10.

The device according to the invention is also referred to hereinafter as "reactor".

In the present application, "pressure-resistant device" means a device that can withstand a pressure difference of more than 0.5 bar between its interior and its surroundings.

In the present application, "cap" is understood to mean the end section of the pressure vessel of the reactor.

By "connector" in this application is understood the structural elements of the device, which are connected to the cap with the ability to conduct electricity and which conduct electrical current from the connection points on the cap to the electrodes. The connecting element is, for example, an apron attached to the reactor cap (see Fig. 1a).

The connecting elements are preferably located on the outer circumference of the solid nozzle. The area of the clearance of the cross section of the connecting element, i.e. the area surrounded by the connecting element is preferably more than 90%, preferably more than 95%, in particular more than 98% of the cross-sectional area of the solid nozzle. Particularly preferably, the connecting elements are connected at the same level in the circumferential direction with the edging of the solid nozzle. Advantageously, the connecting elements have a cylindrical or prismatic shape. The connecting elements preferably overlap horizontally less than 10%, preferably less than 5%, in particular less than 2% of the cross-sectional area of the solid nozzle; particularly preferably, the connecting elements do not extend horizontally into the solid nozzle. The connecting elements preferably consist of the same material as the electrodes.

By "cross-section of the connector" in this application is understood the sectional surface between the connector and any horizontal plane with the smallest area that intersects the connector (see Fig. 1b).

In the present application, "electrode cross-section" means the cross-sectional area between the electrode and the conductive connector in contact with the electrode (see Fig. 1c).

By "cross-section of the upper or lower section of the device" in this application is understood the sectional surface between the upper or lower section of the device and any horizontal plane with the smallest area that intersects these sections (similar to the connecting element in Fig. 1b).

By "electrically insulated" in this application is meant an ohmic resistance of more than 1 kΩ, preferably more than 100 kΩ, in particular more than 1 MΩ, between the solid packing and the side wall of the middle section of the reactor, and between the upper and lower sections of the reactor, for example cap, and the side wall of the middle section of the reactor, measured in accordance with DIN VDE 0100-600: 2017-06 (issue date 2017-06).

Under the "side wall of the reactor" in the present application is understood to be essentially a vertically directed section of the reactor vessel (1). Along the side wall, the horizontal sections through the reactor are of substantially the same area (the cross-sectional area of the solid packing).

The ratio of the cross-sectional area of the upper and/or lower electrode, preferably the upper and lower electrode, to the cross-sectional area of the respective conductive connecting element is preferably 0.1 to 10, preferably 0.3 to 3, in particular 0.5 to 2 Preferably, the cross-sectional area of the electrode (for example, the cross-sectional area of all electrode bridges of the electrode in the form of a grid) is in the range from 0.1 cm ² to 10,000 cm ² , preferably from 1 cm ² to 5000 cm ² , in particular from 10 cm ² up to 1000 cm ² . Preferably, the cross-sectional area of one or more conductive connecting elements is in the range from 0.1 cm ² to 10000 cm ² , preferably from 1 cm ² to 5000 cm ² , in particular from 10 cm ² to 1000 cm ² . The calculation of the ratio ( _{electrode cross-sectional area (upper} / _{connector (upper)} cross-sectional area) or respectively ( _{electrode (lower} ) cross-sectional area/ _{connector (lower)} cross-sectional area) is illustrated in Figures 22 and 23.

Without the use of a connecting element (between the electrode and the upper or lower sections of the device, respectively), the ratio of the cross-sectional area of the upper and/or lower electrode, preferably the upper and lower electrodes, to the cross-sectional area of the corresponding conductive section of the device is preferably from 0.1 to 10, preferably from 0.3 to 3, in particular from 0.5 to 2. Preferably, the cross-sectional area of the electrode is in the range from 0.1 cm ² to 10000 cm ² , preferably from 1 cm ² to 5000 cm ² , in particular from 10 cm ² to 1000 cm ² . Preferably, the cross-sectional area of the upper and/or lower section of the device is in the range from 0.1 cm ² to 10000 cm ² , preferably from 1 cm ² to 5000 cm ² , in particular from 10 cm ² to 1000 cm ² .

Preferably between the upper and lower sections of the device, for example between two reactor hoods, a potential difference (voltage) is set from 1 volt to 10000 volts, preferably from 10 volts to 5000 volts, particularly preferably from 50 volts to 1000 volts. The electric field strength between the domes is preferably between 1 V/m and 100000 V/m, preferably between 10 V/m and 10000 V/m, more preferably between 50 V/m and 5000 V/m, in particular between 100 V/m and 1000 V/m.

The electrical conductivity of the solid nozzle is preferably 0.001 S/cm to 100 S/cm, preferably 0.01 S/cm to 10 S/cm, in particular 0.05 S/cm to 5 S/cm.

The solid nozzle advantageously gives an electric current density from 0.01 A/cm ² to 100 A/cm ² , preferably from 0.05 A/cm ² to 50 A/cm ² , in particular from 0.1 A/cm ² to 10 A / cm ² .

The reactor is preferably divided into several zones. Preferably from bottom to top are: particle outlet, gas supply line (12), lower heat transfer zone, lower electrode (5), heating zone, upper electrode (4) with optional side outlet (19), upper heat transfer zone, gaseous product flow outlet (7) and particle flow feed line (6). The bottom heat transfer zone is the vertical section between the top edge of the gas line and the top edge of the bottom electrode. The upper heat transfer zone is the vertical portion between the lower end of the upper electrode and the upper end of the solid packing. The heating zone at each point of the cross section of the reactor is defined as the vertical section between the lower end of the upper electrode and the upper end of the lower electrode.

Advantageously, the bottom side of the top electrode and the top side of the bottom electrode are horizontal across the entire cross section of the reactor. Consequently, the length of the heating zone, in particular the distance between the electrodes, is advantageously the same over the entire cross section of the reactor. The heated reactor cross section is preferably 0.005 m ² to 200 m ² , preferably 0.05 m ² to 100 m ² , particularly preferably 0.2 m ² to 50 m ² , in particular 1 m ² to 20 m ² . The length of the heating zone is preferably between 0.1 and 100 m, preferably between 0.2 and 50 m, particularly preferably between 0.5 and 20 m, in particular between 1 and 10 m. The ratio of length to equivalent diameter of the heating zone is preferably from 0.01 to 100, preferably 0.05 to 20, particularly preferably 0.1 to 10, most preferably 0.2 to 5.

The electrodes are preferably located inside the solid nozzle (see figures 1 and 2). The vertical distance between the top edge of the solid tip (the lowest point in the case of a bevel) and the bottom edge of the electrode plates or, without the use of electrode plates, the bottom edge of the electrode bridges on the top electrode is preferably 10 mm to 5000 mm, preferably 100 mm to 3000 mm, more preferably from 200 mm to 2000 mm. Preferably, said area is from 1 to 50%, preferably from 2 to 20%, particularly preferably from 5 to 30% of the total height of the solid nozzle.

The vertical distance between the top edge of the electrode plates on the bottom electrode and the gaseous feed inlet is preferably 10 mm to 5000 mm, preferably 100 mm to 3000 mm, more preferably 200 mm to 2000 mm. Preferably, said area is from 1 to 50%, preferably from 2 to 20%, particularly preferably from 5 to 30% of the total height of the solid nozzle.

The vertical distance between the particle flow feed line (6) and the top edge of the solid nozzle is preferably 50 mm to 5000 mm, preferably 100 mm to 3000 mm, particularly preferably 20 mm to 2000 mm.

The electrodes may be of any shape known to those skilled in the art. For example, the electrodes are made in the form of a grid (Fig. 12, Fig. 13, Fig. 14) or in the form of rods (Fig. 16).

When rods are used, pointed electrode rods are particularly preferred. The upper and lower electrode rods are preferably pointed on the side facing the heating zone. The tip can be conical (Fig. 16a) or wedge-shaped (Fig. 16b). Accordingly, the end of the rod can be in the form of a point or in the form of a line. In FIG. 17 shows a sketch of a reactor according to the invention, provided with rod-shaped electrodes. Figure 18 shows a detailed drawing of the top reactor hood. Unlike, for example, US Pat. No. 3,157,468 or US Pat. No. 7,288,503, rod electrodes are connected to the dome in an electrically conductive manner and are jointly supplied with electric current through the dome.

Preferably, the electrodes are in the form of a grid. For the lattice shape, various embodiments are possible, examples are cellular lattices of predominantly regular polygons (Fig. 12a), rectangular lattices (Fig. 12b) formed from parallel bridges, spoke lattices (Fig. 13) or lattices of concentric rings ( Fig. 14). Especially preferred are spoke-shaped gratings and gratings of concentric rings.

Particularly preferred is an electrode in the form of a grid, which is rigidly attached to the inside of the upper or respectively lower section of the device, such as a cap, or to a connecting element, such as an apron, attached to the device section.

Rigid fastening is understood as the connection of a rigid body with its environment, with the help of which relative movement between the body and its environment in all directions is not allowed.

For example, the spoke-shaped lattice is preferably formed from webs arranged in the form of a star, which are suspended from the cap or a connecting element fixed to it (Fig. 13a). In addition to the term "bridge", the prior art also uses the terms "spoke", "support", or "tire".

In another embodiment, the spoked array is preferably formed from webs arranged in a star shape, which are suspended from the cap and carry electrode plates protruding perpendicular to them (FIG. 13b). In addition to the term "electrode plate", the prior art also uses the terms "wing", "rib", "side bar" or "side bar".

In another embodiment, the lattice is preferably formed from concentric rings which are connected by radial bridges (FIGS. 14a, 14b). As defined in DE 69917761 T2 [0004], said lattice shape is "fractally scalable".

Electrodes, i.e. electrode jumpers and electrode plates divide the cross section of the reaction section into grid cells. The reaction site is a volume inside the reactor filled with a solid packing. The grid cells are closed or convex segments of the cross-sectional surface of the reactor, limited by the electrode grid. As an example, closed surface features are shown in FIG. 12a; they are formed by a cellular lattice (46) inside the cap (10) or (16). In FIG. 12b the meshes are, for example, strips between two adjacent webs (46) and the corresponding arcuate sections of the cap. In FIG. 12-14, said surfaces represent individual grid cells that are surrounded by continuous or dashed lines. As an example, in FIG. 13a, the cells are delimited by adjacent lattice spokes (4, 5) and, if necessary, by dotted circular lines or a cap (10, 16). As an example, in FIG. 13b, cells are delineated by adjacent bridge electrode plates, the corresponding bridge segment, and a dotted center line between two adjacent arrays. As an example, the cells in Fig. 14a and 14b are closed surface elements that are delimited by adjacent webs and rings, or respectively by the reactor hood.

The lattice cells are characterized by the following parameters: open cross section, equivalent diameter, deviation from circumference and cross section overlap.

The term "open cross-section" in the present invention refers to the cross-sectional area of the cell through which flow can flow. The term "equivalent diameter" in the present invention means the diameter of a circle with the same area as the lattice cell. The term "circumference" in the present invention means the minimum width of the ring between two circles with a common center, which completely surrounds the edge lines of the lattice cell. The deviation from the circle has the dimension of length. The deviation from the circumference of the circle is zero. The term "overlapping of the cross section" in the present invention refers to the proportion of the cross section of the solid nozzle, which is covered by the electrode, in terms of the total cross-sectional area of the solid nozzle (reaction zone).

The open cross-section of the grid cells is preferably 4 cm ² to 10000 cm ² , preferably 20 cm ² to 3000 cm ² , particularly preferably 100 cm ² to 1000 cm ² . Thus, the open cross section is independent of the reactor diameter, and the number of grid cells is approximately proportional to the reactor cross section.

The equivalent grid mesh diameter is preferably between 10 mm and 2000 mm, preferably between 20 mm and 1000 mm, particularly preferably between 50 mm and 500 mm.

The grid cell circumference is preferably between 1 cm and 10 m, preferably between 1 cm and 2 m, particularly preferably between 1 cm and 1 m, in particular between 1 cm and 50 cm. to the equivalent lattice cell diameter. Preferably, the relative circumferential deviation is greater than or equal to 0 and less than 100, preferably greater than or equal to 0 and less than 10, in particular greater than or equal to 0 and less than 5. As an example, the deviation from the circumference of the individual grid cells is shown in the sketches in FIG. 12a, 12b and 13a.

The overlap of the cross section of the electrodes is preferably between 1% and 50%, preferably between 1% and 40%, particularly preferably between 1% and 30%, in particular between 1% and 20%.

The specific surface area of electrodes in the form of a lattice, i.e. the ratio of the circumference of the electrode (i.e. the length of the line of contact between the electrode and the bulk layer in the vertical projection of the reactor) and the cross section of the bulk layer is preferably from 0.01 to 500 m ² /m ³ preferably from 0.1 to 100 m ² /m ³ , more preferably from 1 to 50 m ² /m ³ , in particular from 2 to 20 m ² /m ³ .

The material of the electrodes, i.e. bridges and electrode plates, is preferably iron, cast iron or steel alloy, copper or copper-based alloy, nickel or nickel-based alloy, refractory metal or refractory metal-based alloy and/or electrically conductive ceramic. In particular, the lintels consist of a steel alloy, e.g. material no. material number 2.4816, 2.4642, titanium, in particular alloys with material numbers 3.7025, 3.7035, 3.7164, 3.7165, 3.7194, 3.7235. Among the refractory metals, Zr, Hf, V, Nb, Ta, Cr, Mo, W or their alloys are particularly preferred; preferably Mo, W and/or Nb or their alloys, in particular molybdenum and tungsten or their alloys. In addition, the bridges may contain ceramics, such as silicon carbide and/or carbon, such as graphite, while the ceramics may be a monolithic or fiber-reinforced composite material (for example, a Ceramic Matrix Compound, CMC, or, for example, carbon fiber composite, English Carbon Fiber Composite, CFC).

The material of the electrodes is preferably selected depending on the operating temperature. The steel is preferably chosen for a temperature range of -50 to 1250°C, preferably -50 to 1000°C, more preferably -50 to 750°C, in particular -50 to 500°C. Molybdenum is preferably chosen for the temperature range from -50 to 1800°C, preferably from -50 to 1400°C, in particular from -50 to 1300°C. The carbon fiber-reinforced carbon is preferably chosen for the temperature range -50 to 2000°C, preferably -50 to 1600°C, in particular -50 to 1300°C.

In the case of special applications, the electrodes may also consist of several materials. In the case of using several materials, the electrode is mainly divided along the height into sections of different materials. The choice of material for different zones is mainly based on the following criteria: thermal resistance, electrical conductivity, cost. Segments made of different materials are preferably connected to each other in a force-locked manner or in a permanent manner. Preferably, the connections between the segments are smooth.

The electrodes can advantageously be made in the form of solid electrodes or in the form of hollow electrodes. In the case of solid electrodes, depending on the design, the electrode rods, electrode bridges and/or electrode plates are a solid body. In the case of hollow electrodes, depending on the design, the electrode rods, electrode bridges and/or electrode plates are a hollow body. The cavities within the electrodes may advantageously form channels which can be used to introduce gas streams into the reaction zone or to withdraw gas streams from the reaction zone. The walls of the hollow electrodes are advantageously made of slotted metal sheets, perforated metal sheets, seamless metal grids or mesh materials.

Spoke-shaped grid electrodes according to figures 13a and 13b: The spoke-shaped grid preferably has electrode bridges, preferably 2 to 30 electrode bridges, preferably 3 to 24 electrode bridges, in particular 4 to 18 electrode bridges. Preferably, from 1 to 100 electrode plates are fixed to each of these electrode bridges, preferably from 2 to 50, in particular from 4 to 20.

The length of the webs is preferably between 1 cm and 1000 cm, preferably between 10 cm and 500 cm, in particular between 30 cm and 300 cm. The height of the webs is preferably between 1 cm and 200 cm, preferably between 5 cm and 100 cm, in particular between 10 cm and 50 cm. The thickness of the webs (at its thickest point) is preferably between 0.1 mm and 200 mm, preferably between 1 mm and 100 mm.

The side profile of the bridges and electrode plates is preferably rectangular, trapezoidal or triangular (FIG. 9, FIG. 10), with other geometries, such as rounded ones, being also acceptable. Advantageously, the lower edges of the bridges and plates in the top electrode and the top edges of the bridges and plates in the bottom electrode are horizontal (Fig. 9, Fig. 10).

The cross section of the bridges and electrode plates is preferably lens, diamond or hexagonal (FIG. 11). While the upper and lower ends of the bridges are preferably pointed. The thickness of the bridge or electrode plate at the upper and lower end (point) is preferably between 0.001 mm and 10 mm, preferably between 0.001 mm and 5 mm, in particular between 0.001 mm and 1 mm.

The profile of the jumpers and electrode plates is preferably straight, sawtooth or undulating in plan view. The undulating profiles preferably have a sinusoidal or rectangular shape (FIG. 7). In the case of sawtooth and wavy profiles, the width of the tooth or wave is preferably 1 cm to 200 cm, preferably 1 cm to 100 cm, more preferably 1 cm to 50 cm, the height of the tooth or wave is preferably 1 mm to 200 mm, preferably 1 mm to 100 mm, more preferably 1 mm to 50 mm.

The optional electrode plates are connected to the bridges and are oriented on the reactor plan predominantly perpendicular to the bridges. Preferably, the electrode plates are connected to a bridge either centrally or at one end of the electrode plates. The contact surface between the electrode plate and the bridge advantageously forms a separate rigid attachment for positioning the electrode plate. Accordingly, both ends or one end are free, i.e. it does not have a hard connection with other electrode plates or other jumpers. As a result, the electrode plates can be deformed without causing stress due to thermal expansion.

The distance between adjacent electrode plates on the web is preferably 1 to 2000 mm, preferably 5 to 1000 mm, in particular 10 to 500 mm.

In the case of curved/non-planar electrode plates, the length refers to the circumferential length. The length of the electrode plates preferably decreases linearly along the radius from the outer electrode ring towards the center of the reactor. The length of each plate on the bridge is predominantly proportional to its distance from the center of the reactor cross section; in this case, the length of the electrode plates is understood to be the length of the outermost electrode plate. The length of the electrode plates is preferably 1 cm to 1000 cm, preferably 2 cm to 500 cm, more preferably 5 cm to 200 cm, in particular 10 cm to 100 cm. The height of the electrode plates is preferably 1 cm to 200 cm, preferably 2 cm to 100 cm, more preferably 5 cm to 50 cm, in particular 10 cm to 50 cm. The thickness of the individual electrode plates on the web is constant. The thickness of the electrode plates (at the thickest point), the grating strength, is preferably 0.1 mm to 100 mm, preferably 1 mm to 50 mm. The height to thickness ratio of the electrode plates is preferably 1 to 500, preferably 2 to 250, more preferably 5 to 100, in particular 10 to 50.

In the case of spoke-like arrays, the electrode bridges inside the reactor preferably diverge in the form of a star. The individual electrode bridges are preferably not connected to each other. Preferably, the electrode bridges at their outer end are connected to the reactor hood or to a connecting element on the reactor hood, for example an apron. The other end of the electrode jumpers is predominantly free, i.e. it does not have a hard connection with other electrode bridges. Preferably, the contact surface between the electrode bridge and the upper or lower section of the device, for example a cap, or respectively a connecting element, for example an apron, forms a separate rigid attachment, the so-called rigid attachment, for positioning the electrode bridge. Accordingly, the other end of the electrode bridge is free, so that the electrode bridge can be deformed without causing stress due to thermal expansion.

The upper and lower edges of the jumpers and electrode plates are predominantly offset relative to each other. By offsetting the edges of the webs and plates, nodal points are avoided, which could otherwise lead to stagnation of the bulk layer. In FIG. 15 shows examples of preferred bottom electrode options. In each case, a lattice segment is shown, in which one individual bridge is placed. In the embodiment according to FIG. 15a, the upper edge of the electrode plates is located above the upper edge of the jumper. In the embodiment according to FIG. 15b, the top edge of the electrode plates is located below the top edge of the jumper. The offset between the top edge of the electrode plates and the top edge of the bridges is preferably -500 mm to 500 mm, preferably -200 mm to 200 mm, particularly preferably -100 mm to 100 mm. Negative values mean that the top edge of the electrode plates is below the top edge of the jumpers. The offset between the bottom edge of the electrode plates and the bottom edge of the bridges is preferably -500 mm to 500 mm, preferably -200 mm to 200 mm, particularly preferably -100 mm to 100 mm. Negative values mean that the top edge of the electrode plates is below the top edge of the jumpers.

Fractally scaled array electrodes according to Figures 14a and 14b: The array of concentric rings (fractally scaled electrode) advantageously has electrode bridges that diverge in an approximately star shape and electrode plates that are formed as segments in the shape of a circular arc. The upper and lower edges of the jumpers and electrode plates are predominantly offset in height relative to each other. Bridges on both sides are connected to the electrode plates, the electrode plates being continuous within a circular segment, such as the 1/4 circle in FIG. 14a and 1/6 of the circle in Fig. 14b. The number of jumpers increases from the center to the outside. The jumpers of the outer ring are attached to the reactor cap. The number and location of the bars follows the following rules: The core of the lattice has a diameter of 2*s, has no bars, and is considered ring 1. The recursion formula for constructing further rings is as follows: "Ring i has an outer diameter of 2*i*s and n*i bars , uniformly distributed along the angular coordinate. In every even ring, the bars are offset by π/(n*i) rad clockwise", s denotes the width of the ring, n is a natural number and is denoted as the base of the recursion. The ring width s is preferably 1 to 2000 mm, preferably 5 to 1000 mm, in particular 10 to 500 mm. n is preferably a number from 2 to 30, preferably a number from 2 to 20, in particular a number from 2 to 10. A lattice with base 4 is shown in FIG. 14a, and the grating with base 6 is shown in Fig. 14b. In general, lattice structures that can be scaled when expanded according to the recursion formula are referred to as fractally scalable structures.

In the case of fractally scalable gratings, the electrode bridges inside the reactor predominantly diverge in the shape of a star. Adjacent circular arc-shaped electrode plates are preferably not connected to each other partially or in segments. Thus, the lattice is preferably divided into segments, preferably 2 to 30 segments, preferably 2 to 20 segments. Advantageously, the outer electrode bridges are connected at their outer end to the reactor hood or to a connecting element on the reactor hood, for example a baffle. Preferably, the contact surface between the electrode bridges and the upper or lower section of the device, for example a cap, or respectively a connecting element, for example an apron, forms a separate rigid attachment, the so-called rigid attachment, for positioning the grid segments. Thus, the lattice segment can be deformed without stress, i.e. without touching neighboring lattice segments, as a result of thermal expansion.

The upper and lower sections of the reactor vessel preferably form in each case the contacts for the upper and lower electrodes. The electrodes are preferably in contact through the end sections of the reactor vessel, also referred to as reactor caps (see FIGS. 4 and 5). The reactor caps preferably have one or more electrical connections, (8) and (17), preferably one to three connections, on the outside.

If necessary, the reactor caps may have connecting elements, such as an apron (10), (16), which protrudes into the central section of the reactor; and the term "apron" means the extension of the cap on the inside of the sealing surface to the side wall (11), (18). Preferably, the electrodes are connected to the cap apron. The contact between the reactor cap and the electrode can be made by a permanent connection of materials, such as welding or soldering, by means of a force-locking connection, such as twisting or clamping, or a form-fitting connection, for example, by means of a gear, a groove and a tenon, or a stud and a bolt. The preferred type of connection is determined by the material of the electrode bridges.

The metal electrode bridges are preferably welded or soldered to the cap. The non-metallic electrode bridges are preferably connected to the hood by a combined form-fitting and force-locking connection or a permanent connection of materials, for example a tongue-and-groove connection in combination with a screw connection, a rivet connection or an adhesive connection. In the case of star-shaped gratings and fractally scalable gratings, the electrode bridges are advantageously connected at their outer end to the reactor hood or to the apron of the reactor hood.

The contact surface between the electrode and the upper or lower section of the device, the reactor hood or the connecting element in contact with the hood, for example an apron, is preferably between 0.1 cm ² and 10,000 cm ² , preferably between 1 cm ² and 5000 cm ² , in particular between 10 cm ² and 1000 cm ² . When using a connecting element, such as an apron, the contact surface between the reactor hood and the connecting element in contact with the hood is preferably between 0.05 cm ² and 200,000 cm ² , preferably between 0.5 cm ² and 50,000 cm ² , in particular between 50 cm ² and 10000 cm ² .

Advantageously, the temperature on the contact surface between the top section of the device and the connecting element is preferably less than 600°C, preferably less than 450°C, particularly preferably less than 150°C, preferably in the range from 0 to 600°C, preferably from 10 to 450°C.

The ratio of the cross-sectional area of the connecting element, for example an apron, to the cross-sectional area of the solid nozzle is preferably 0.001 to 0.2 (0.1 to 20%), preferably 0.002 to 0.1 (0.2 to 10%) , particularly preferably from 0.5 to 5%. The ratio of the cross-sectional area of the conductive cap to the cross-sectional area of the solid nozzle is preferably 0.001 to 0.2 (0.1 to 20%), preferably 0.002 to 0.1 (0.2 to 10%), particularly preferably 0.002 to 0.1 (0.2 to 10%). 0.005 to 0.05 (0.5 to 5%).

In the cap-electrode unit, preferably less than 5%, preferably less than 2%, particularly preferably less than 1%, in particular less than 0.1% of the total input electrical energy is dissipated. Preferably, the dissipated energy range is 0 to 5%, preferably 0 to 2%, in particular 0 to 1%. As a result, almost all electrical energy can be used to heat the nozzle between the electrodes. By "dissipated energy" is meant electrical energy converted into thermal energy as a result of the ohmic resistance of the line. Low energy dissipation is achieved due to the low ohmic resistance of the cap-electrode structural unit. The ohmic resistance between any two points of the cap-electrode structural unit is preferably from 10 ^-12 Ω to 10 ^-13 Ω, preferably from 10 ^-12 Ω to 10 ^-5 Ω, in particular from 10 ^-12 Ω to 10 ^-7 Ω. The specified ohmic resistance of the structural unit caps-electrodes is achieved by choosing the material and dimensions of the structural unit caps-electrodes. For the methane pyrolysis reaction system, specific dimensions are described in the example.

The pressure-resistant reactor jacket advantageously consists of an upper reactor section (1), a middle reactor section (2) and a lower reactor section (3). The preferred materials for the reactor jacket are steel alloys, for example with material number 1.4541, 1.4571. The preferred conductivity of the upper and/or lower sections of the device is preferably between 10 ⁵ S/m and 10 ⁸ S/m, preferably between 0.5 x 10 ⁶ S/m and 0.5 x 10 ⁸ S/m. The specific ohmic resistance of the reactor outer pressure jacket is preferably between 10 ^-8 Ωm and 10 ^-5 Ωm, preferably between 2×10 ^-7 Ωm and 2×10 ^-6 Ωm.

By way of example, the top and bottom sections of the reactor comprise an end end of the reactor vessel. The upper section of the reactor is preferably made in the form of a cap. The lower section of the reactor is also preferably made in the form of a hood, in particular in the form of a conical hood (a hood with an outlet cone for solid granulate).

The upper section of the reactor, preferably the reactor hood, preferably has the following connections (see Fig. 4): power supply (8), solids feed line (6) and, if necessary, a distributor (9) (for example, in the form of a cone distributor), one or more outlets for the product flow (7), preferably for the gaseous product flow, inputs for sensors, for example, for temperature measurement, filling level measurement, concentration measurement, pressure measurement.

The lower section of the reactor, preferably a conical reactor hood, has the following connections (see Fig. 5): outlet cone for the product stream (14), preferably for the solid product stream, power supply for the lower electrode (17), at least one inlet for feed streams, (12) preferably for gaseous feed streams, sensor inputs, eg for temperature measurement, concentration measurement, pressure measurement.

The feed stream or, if necessary, several feed streams are preferably introduced through an annular distributor (13) or through several inlets distributed around the circumference on the lower reactor hood. By means of a plate distributor (12) connected thereto, the flow of the starting material can be evenly distributed over the cross section at the feed level. In plan view, the distributor plate, which is optionally present, advantageously has the same shape as the electrodes and is therefore in the same vertical position as the electrodes. Alternatively, the distributor consists of individual elements, each of which is preferably mounted below the electrode elements.

The middle section of the reactor is preferably cylindrical or prismatic (see Fig. 3). Said area is preferably lined with an electrically insulating lining (21) resistant to temperatures up to about 2000°C, preferably up to about 1700°C, preferably up to about 1400°C, preferably up to about 1200°C. This section defines the length of the heating zone. The length of the middle section of the reactor is preferably between 0.25 and 100 m, preferably between 0.5 and 50 m, particularly preferably between 0.75 and 20 m, in particular between 1 and 10 m.

The vertical distance between the top edge of the reactor middle section and the top edge of the solid packing is preferably -2000 mm to 2000 mm, preferably -1000 mm to 1000 mm, particularly preferably -500 mm to 500 mm. Negative values mean that the top edge of the reactor middle section is below the top edge of the solid packing. The vertical distance between the top edge of the middle section of the reactor and the bottom edge of the electrode plates on the top electrode is preferably 10 mm to 5000 mm, preferably 100 mm to 3000 mm, more preferably 200 mm to 2000 mm. The vertical distance between the upper edge of the electrode plates on the lower electrode and the inlet of the gaseous raw materials is preferably 10 mm to 5000 mm, preferably 100 mm to 3000 mm, more preferably 200 mm to 2000 mm.

The electrical insulation performs the following functions: (i) isolate the caps from the side wall of the reactor, i.e. the middle section of the reactor shell, and (ii) isolate the bulk bed from the side wall of the reactor.

Typically, refractory bricks are used for electrically insulating lining, which predominantly contain alumina, zirconium oxide and mixed oxides of aluminium, magnesium, chromium and silicon (see, for example, Patrick Gehre's dissertation: Korrosions-und thermoschockbestandige Feuerfestmaterialien fur Flugstromvergasungsanlagen auf Al ₂ O ₃ -Basis -Werkstoffenwicklung und Korrosionsuntersuchungen (Corrosion and thermal shock resistant refractory materials for entrained flow gasification plants based on Al ₂ O ₃ - material development and corrosion studies.) (TU Freiberg, 2013)).

The middle section of the reactor is preferably electrically isolated from the two caps. For example, in each case, an intermediate ring of electrically insulating material (23) and (25) is used, which is preferably gastightly clamped between the middle section of the reactor and the upper reactor cap (11) or, respectively, the lower reactor cap (18). The intermediate ring is preferably made of enamelled or plastic-coated metal, plastic, such as PTFE or PEEK, or gas-tight ceramic. Alternatively, sealing rings made of an electrically insulating material, such as mica, can be clamped directly between the flanges of the middle section of the reactor and the reactor caps. The thickness of the intermediate ring is preferably 2 mm to 500 mm, more preferably 3 mm to 200 mm, particularly preferably 5 mm to 100 mm.

Preferably, the upper and/or lower section of the device, for example the upper cap, is made of two-shell (see figure 6). The outer shell of the cap (41) preferably surrounds the cap (3 or 31) described above, which is preferably an inner shell. The inner sheath is preferably an electrically conductive connecting element. The outer sheath is preferably electrically isolated from the inner sheath. The outer shell is preferably connected to the middle section (1) of the reactor via a flange (22 or 42). A seal is preferably used between flanges (42) and (22). The seal is preferably a flat seal, a lenticular seal, an O-ring seal, or a welded lip seal. In addition, the outer shell (41) advantageously contains entries (43) for connections (6), (7), (8) that lead to the inner shell of the cap. The inlets are preferably removable, so that the outer shell can be individually flanged onto or off the reactor (see FIGS. 19 and 20).

A preferred embodiment of double-shell cap entries is known to those skilled in the art and is described, for example, in US Pat. No. 7,842,846 B2. In the present invention, the bushing is preferably configured to provide additional electrical insulation between the inner and outer shell. In FIG. 19 shows, as an example, an inlet for a particle flow feed line (6) to the reactor. The flow of solid particles mainly passes through the inlet pipe (58), which is provided with a flange (52). The inlet pipe is preferably made of a metallic material, preferably a metallic pipe, which is coated with an electrically insulating layer, such as enamel. In this case, the inlet preferably contains two concentric cylindrical necks, of which the outer (51) is attached to the outer shell, and the inner (54) is attached to the inner shell of the cap. The inner neck advantageously has a compensator which makes the inner neck flexible in the longitudinal direction. Preferably, the inner neck terminates in a threaded hole plate whose outer circumference is smaller than that of the outer neck. The outer neck advantageously terminates in the flange of the device. The inner and outer flanges are preferably gastightly bonded through an intermediate ring (53). The inner neck and the outer neck are preferably electrically isolated from each other. To do this, an intermediate ring made of metal with flat seals (55) made of an electrically insulating material, such as mica or plastic, is preferably clamped between the inlet pipe flange on one side and the outer neck flange and the inner neck threaded plate on the other side. Sleeves made of an electrically insulating material (57), such as plastic or oxide ceramic, are preferably used between the fixing screws and the intermediate ring.

Alternatively, the intermediate ring may be composed of an electrically insulating material such as plastic, PEEK, or densely sintered oxide ceramic. As an alternative, the intermediate metal ring can be covered with an electrically insulating material, such as enamel or plastic. Preferably, the intermediate ring seal at the outer neck is a flat seal, a lenticular seal, an O-ring seal, or a welded lip seal.

In FIG. 20 shows as an example the entry of a power supply line which leads to the inner shell of the hood. The input contains a pin (63), which is soldered or pressed to the outer side of the inner shell (2). The pin is connected to the connector (64), which is connected to the power supply, using a screw or clamp connection. The connector has a collar at the lower end. The pin fits freely into a ceramic sleeve (65) made of electrically insulating material. The sleeve is preferably made of oxide ceramic. Preferably, the sleeve is made of metal and covered with a layer of enamel. The ceramic sleeve, in turn, enters the socket (61). The specified socket is welded to the outer shell of the cap (27). The socket preferably comprises an expansion joint and a welded flange. The socket (61), the insulating sleeve (65) and the connector (64) are fixed with a loose flange (62). Between the socket (61) and the sleeve (65), as well as between the sleeve (65) and the connector (64), flat seals (66) are inserted. Flat seals are predominantly composed of mica. Alternatively, the seals may be in the form of O-ring seals. Sleeves made of electrically insulating material (67), such as plastic or oxide ceramics, are preferably used between the fixing screws and the outer socket flange.

Preferably, the outer shell of the cap according to FIG. 6 and 7 contains connections for supply (44) and output (45) of an inert gas flow, which contains, for example, nitrogen, argon, carbon dioxide and/or water vapor. By means of an inert gas, the space of the jacket between the inner and outer shell of the cap is blown. Advantageously, the pressure in the jacket space is set slightly higher than the pressure in the immediately adjacent part of the reaction zone. The pressure difference between the jacket space and the immediately adjacent part of the reaction zone is preferably 1 mbar to 500 mbar, preferably 1 mbar to 100 mbar, particularly preferably 1 mbar to 50 mbar. Adjustment of this difference is known to a person skilled in the art, for example, described in international application WO 2013017609 A1.

The dimensions of the reactor depend on the reaction system and the desired throughput. For the methane pyrolysis reaction system, specific dimensions are described in the example.

The packed reactor according to the invention advantageously contains a random bulk layer of solid particles of electrically conductive material. The bulk layer can be homogeneous or structured in height. The homogeneous bulk bed can advantageously form a fixed bed, a moving bed or a fluidized bed, in particular a moving bed. The height-structured layer preferably forms a fixed bed at the bottom and a fluidized bed at the top. Alternatively, the height-structured bed preferably forms a moving bed at the bottom and a fluidized bed at the top. Alternatively, the solid packing preferably comprises structured embedded elements of electrically conductive material, such as honeycomb monoliths, crossed plates such as Sulzer Mellapack packings, static mixers such as Sulzer SMX mixers, or loose particles. The structured embedded elements preferably comprise metal, silicon carbide or carbon and form through electrically conductive paths between the electrodes. If necessary, the hollow volume of the structured built-in elements is completely or partially filled with solid particles. The solid particles advantageously form a fixed bed, a moving bed, a fluidized bed, or a jet bed. The particles may advantageously consist of electrically conductive and/or electrically insulating materials.

As heat-resistant, electrically conductive structured packings, built-in elements made of metal and/or electrically conductive ceramics, such as silicon carbide, carbon and composite materials containing these substances, are suitable.

By "heat integration" in this application is meant countercurrent heat exchange between hot and cold material flow in a process whereby sensible heat from the hot material flow is used to heat the cold material flow. As a result, a change in temperature is achieved in the involved material flows without the transfer of heat flows through the process boundaries.

The reactor according to the invention offers advantageous characteristics for realizing thermal integration mode of operation for endothermic high temperature processes. These characteristics include, in particular, (i) counterflow between the solids stream and the gas stream, and (ii) adjusting the position of the heating zone within the reaction zone, resulting in a heat transfer zone at the upper end for heat exchange between the hot gaseous product and the cold solids stream. particles, and at the lower end a heat transfer zone for heat exchange between the solid product stream and the cold gas supply stream.

The efficiency of heat integration is achieved by minimizing the resistance to heat transfer between the gas and the solid packing due to the favorable ratio of heat capacity flows of gaseous and solid reaction media in the heat transfer zones. An indicator of the effectiveness of thermal integration is the degree of influence of thermal integration: η=(temperature of the reaction zone - temperature of the gas at the outlet of the main stream) / (temperature of the reaction zone - temperature of the solids at the inlet).

The degree of influence of heat integration is preferably more than 60%, preferably more than 65%, even more preferably more than 70%, even more preferably more than 80%, even more preferably more than 90%, in particular more than 95%. The degree of influence of heat integration preferably lies in the range from 60 to 99.5%.

The length of the heat transfer unit is mainly determined by the following parameters: (i) the properties of the particles of the bulk layer, such as particle size, thermal conductivity, emissivity, (ii) the properties of the gas phase, such as conductivity, and (iii) the operating conditions, such as pressure, temperature , throughput.

Thermal resistance during heat exchange between gas and solid packing in heat transfer zones preferably has a length of transfer unit or Height-of-Transfer Units (HTU) of 0.01 to 5 m, preferably 0.02 to 3 m, particularly preferably 0. 05 to 2 m, in particular 0.1 to 1 m. The definition of HTU can be found at http://elib.uni-stuttgart.de/bitstream/11682/2350/1/docu_FU.pdf page 74.

The heat capacity flow is the product of the mass flow and the specific heat of the material flow. The heat capacity flow ratio between the gaseous process stream and the solid process stream is preferably 0.5 to 2, preferably 0.75 to 1.5, particularly preferably 0.85 to 1.2, in particular 0.9 to 1, one. The ratio of heat capacity flows is set via the supply flows and, if necessary, via the lateral supply or lateral discharge of the partial flows.

At the upper end of the reaction zone, in particular at the upper edge of the solid packing, the temperature difference between the outlet temperature of the gaseous product stream and the solids feed stream is preferably 0 K to 500 K, preferably 0 K to 300 K, more preferably 0 K up to 200 K, in particular from 0 K to 100 K.

At the lower end of the reaction zone, in particular at the point where the solid product stream exits the reactor, the temperature difference between the outlet temperature of the solid product stream and the gaseous feed stream is advantageously between 0 K and 500 K, preferably between 0 K and 300 K, more preferably from 0 K to 200 K, in particular from 0 K to 100 K.

The middle section of the reactor preferably has a lateral gas outlet connection. The lateral outlet is advantageously an opening between the moving bed and a gas-permeable region isolated from the moving bed in the reactor, which is connected to a separate opening in the reactor vessel. The side outlet to the reaction zone may preferably be through or divided into segments by means of rigid channels (19). Preferably the rigid channels (19) are integrated into the electrode bridges. The channels can be combined into an annular manifold (20). Through said side outlet, part of the reaction gas can advantageously be withdrawn from the reaction zone.

The side outlet is preferably a height-limited area at the upper end of the heating zone. Particularly preferably, the side arm is positioned in relation to the position of the top electrode as follows: The position of the lower end of the side arm in relation to the lower end of the upper electrode is preferably -2000 to 2000 mm, preferably -1000 to 1000 mm, more preferably 500 to 500 mm , in particular from -500 to 0 mm. Negative values mean that the bottom end of the side arm is below the bottom end of the top electrode. The position of the upper end of the side arm relative to the lower end of the upper electrode is preferably -2000 to 3000 mm, preferably -1000 to 2000 mm, more preferably 500 to 1000 mm, in particular 0 to 1000 mm. Negative values mean that the top end of the side arm is below the bottom end of the top electrode. The position of the upper end of the side arm with respect to the upper end of the middle reaction zone is preferably -3000 to -100 mm, preferably -2000 to -100 mm, more preferably -1000 to -100 mm, in particular -500 to -100 mm. Negative values mean that the top end of the side arm is below the top end of the middle reaction zone.

The proportion of the total volumetric flow which passes through the side outlet is preferably 0 to 100%, preferably 0 to 80%, more preferably 0 to 60%, in particular 0 to 40%.

By means of a side outlet, the heat capacity flow of the gas stream in the upper heat transfer zone is reduced and adapted to the heat capacity flow of the heated solids flow in the moving bed, which flows countercurrently. The side tap influences the position of the upper heat transfer zone, i.e. location of the point with the largest negative temperature gradient in absolute value in the moving layer. The position of the upper heat transfer zone is preferably 10 to 3000 mm, preferably 100 to 2500 mm, more preferably 200 to 2000 mm, in particular 300 to 2000 mm below the upper end of the moving bed.

Another advantage of the side outlet is that the outlet stream temperature is close to the maximum temperature. Due to the high temperature, said stream can be effectively used in various ways. The gas stream from the side outlet can, for example, be used as the reaction gas in the subsequent reaction step (referring to the combination of pyrolysis and the reverse water gas shift reaction).

Another advantage of the side arm is that the electrodes are located above the heating zone in the colder temperature range. Therefore, despite very high temperatures in the heating zone, it is possible to select materials for electrodes that can only be used in the colder temperature range.

The carrier materials of the product formation layer are advantageously heat resistant in the range of 500 to 2000°C, preferably 1000 to 1800°C, more preferably 1300 to 1800°C, particularly preferably 1500 to 1800°C, in particular 1600 to 1800° FROM.

The carrier materials of the product formation layer advantageously have an electrical conductivity in the range between 10 S/cm and 10 ⁵ S/cm.

Suitable heat-resistant carrier materials, especially for methane pyrolysis, are predominantly carbon-containing materials, such as coke, silicon carbide and boron carbide. If necessary, the carriers may be coated with catalytically active materials. Said heat transfer materials may have a different expansion property than the carbon deposited thereon.

The granulate particles have regular and/or irregular geometric shapes. Regularly shaped particles are preferably spherical or cylindrical.

The granules advantageously have a grain size, i. e. equivalent diameter, which is determined by sieving through cells of a certain size, from 0.05 to 100 mm, preferably from 0.1 to 50 mm, more preferably from 0.2 to 10 mm, in particular from 0.5 to 5 mm.

In addition, it is advantageous to use a carbonaceous material, for example in the form of granules. In the present invention, carbon-containing granulate should be understood as a material that mainly consists of hard grains that contain at least 50 wt. -%, preferably at least 80 wt. -%, more preferably at least 90 wt. carbon, in particular at least 98% of the mass. carbon.

Many different carbonaceous granules can be used in the process according to the invention. For example, such a granulate may consist essentially of coal, coke, coke breeze and/or mixtures thereof. In addition, the carbon-containing granulate may contain from 0 to 15 wt. -%, based on the total weight of the granulate, preferably from 0 to 5 wt.%. metal, metal oxide and/or ceramic.

A preferred reactor design according to the invention is a fixed bed catalytic reactor with direct electrical heating. In FIG. 21 shows a sketch of a reactor according to the invention. The reactor is preferably divided into several zones. Predominantly from top to bottom are: gas supply line (73), upper electrode (4), heating zone, lower electrode (5), gaseous product flow outlet (74). The reactor is partially filled with a disordered or structured packing of an electrically conductive material. The nozzle rests on a catalyst support (72) which, in turn, is attached to a connecting element, such as an apron, attached to the lower reactor hood. The top and bottom electrodes (4) and (5) are advantageously located at the top and bottom end of the solid nozzle, respectively.

The term "high temperature processes" includes, inter alia, pyrolysis reactions, dehydrogenation reactions and reforming reactions.

According to the invention, the endothermic high temperature process is preferably a process whose specific volumetric energy consumption in the heating zone is greater than 0.5 MW/m ³ , particularly preferably greater than 1 MW/m ³ , in particular greater than 2 MW/m ³ . For example, the energy consumption in the heating zone may be between 0.5 and 10 MW/m ³ .

In the moving bed reactor according to the invention, the following high temperature reactions are preferably carried out:

• production of synthesis gas by reforming hydrocarbons with steam and/or carbon dioxide, coupled production of hydrogen and pyrolysis carbon by pyrolysis of hydrocarbons. Suitable carrier materials are, in particular, carbon-containing granules, silicon carbide-containing granules, nickel-containing metal granules.

• production of hydrocyanic acid from methane and ammonia or from propane and ammonia. Suitable carrier materials are, in particular, carbonaceous granules.

• production of olefins by cracking hydrocarbons with steam. Suitable carrier materials are, in particular, carbon-containing granules containing silicon carbide granules.

• combination of methane to ethylene, acetylene and benzene.

• production of olefins by catalytic dehydrogenation of alkanes, such as propylene from propane or butene from butane. Suitable carrier materials are, in particular, pellets containing silicon carbide coated with dehydrogenation catalysts or iron-containing shaped articles.

• production of styrene by catalytic dehydrogenation of ethylbenzene. Suitable carrier materials are, in particular, pellets containing silicon carbide coated with dehydrogenation catalysts or iron-containing shaped articles.

• production of diolefins by catalytic dehydrogenation of alkanes or olefins, such as butadiene from butene or from butane. Suitable carrier materials are, in particular, pellets containing silicon carbide coated with dehydrogenation catalysts or iron-containing shaped articles.

• aldehydes via the catalytic dehydrogenation of alcohols, eg anhydrous formaldehyde from methanol. Suitable carrier materials are, in particular, silver-containing granules or dehydrogenation catalyst-coated granules containing silicon carbide, or iron-containing shaped articles.

• production of CO through the Boudouard reaction from CO ₂ and carbon. Suitable carrier materials are, in particular, carbonaceous granules.

• production of hydrogen and oxygen by means of catalytic thermolysis of water on catalytic contacts. Suitable carrier materials are, in particular, silicon carbide-containing granules or iron-containing granules which are coated with a cracking catalyst, for example ferrite.

For preferred embodiments of the process according to the invention, the maximum temperature set point ranges are summarized in a table:

The temperature of the upper electrode is preferably at least 350°C, preferably in the range from 350 to 1900°C.

The contact of the electrodes through the flat end sections of the reactor vessel or a connecting element attached to it and, if necessary, the additional use of refractory metals as electrode material allows the introduction of an electric current into the reaction zone with low losses. Due to the large cross-sectional areas and high electrical conductivity of the reactor caps, as well as, if necessary, connecting elements, the electrical power dissipated in them is negligible. As a result of this connection, the inputs and connections in the specified area are maintained at a moderate temperature level without complex active cooling. Due to the coordinated cross-sectional dimensions of the electrodes and connecting elements, a uniform distribution of the electric current over the cross-section of the solid nozzle is achieved.

The contact of the electrodes around the circumference of the caps and, if necessary, in combination with the lattice geometry of the electrodes, allows a uniform introduction of electric current into the reaction zone. In addition, the lattice geometry of the electrodes makes it possible to structure the cross section of the reactor into small homogeneous regions. As a result, favorable conditions are created for rational scaling and adaptation of the reactor to the required production capacity.

By means of the vertical arrangement of the electrodes, a uniform heat release and a uniform transformation in the heated region of the reaction zone are ensured. A preferred embodiment of electrodes with bar electrode bridges and electrode plates attached thereto has high mechanical strength. Segmentation of the electrodes and one-sided fixation ensure unhindered thermal expansion of the electrodes.

The high degree of flexibility and profiling of the electrode bridges and electrode plates with pointed ends allow solid particles to move freely in the moving bed. As a result, uniform operating conditions are provided throughout the cross section of the reaction zone.

By placing the electrodes inside the packing, above and below the electrically heated area of the packing, two defined heat transfer zones are created in which internal heat transfer can be achieved. As a result, the reactor has the necessary conditions for complete heat integration.

By placing the top edge of the solid packing inside the middle section of the reactor, the high temperature zone is securely limited to a mechanically and thermally stable region of the reactor.

Dividing the vessel into three sections simplifies assembly and disassembly of the reactor. As a result, it is possible to easily replace wear parts as well as to use prefabricated reactor sections for reactor assembly. As a result, the economic efficiency and the quality of the reactor manufacturing are improved.

Figure 1:

In FIG. 1 shows a sketch of a moving bed reactor according to the invention with direct electrical heating.

a. Longitudinal section of the reactor.

b. Cross section of the reactor at the level of the upper electrode. This projection shows the cross section of the connecting element 10.

c. Side view of the development of the apron of the upper electrode. This projection shows the cross section of electrode 4.

Figure 2:

In FIG. 2 shows a sketch of a moving bed reactor according to the invention with direct electrical heating.

Figure 3:

In FIG. 3 shows a detailed drawing of the middle section of the reactor vessel. Figure 4:

In FIG. 4 shows a detailed drawing of the top reactor hood in side view (upper) and in top view (lower).

Figure 5:

In FIG. 5 shows a detailed drawing of the lower reactor hood in side view (lower) and in bottom view (upper).

Figure 6:

In FIG. 6 shows a variant of the reactor according to the invention with a double-shell top reactor hood.

Figure 7:

In FIG. 7 shows a detailed drawing of the top reactor hood in side view (upper) and in top view (lower).

Figure 8:

In FIG. 8 shows the preferred longitudinal profiles of the electrode bridges in the top electrode according to the invention. In each case, identical profiles are used in the bottom electrode.

Figure 9:

In FIG. 9 shows the preferred side profiles of the electrode bridges in the top electrode according to the invention. The bottom of the jumper is horizontal.

Figure 10:

In FIG. 10 shows the preferred side profiles of the jumpers in the bottom electrode according to the invention. The upper part of the jumper is horizontal.

Figure 11:

In FIG. 11 shows preferred cross-sectional profiles of electrode bridges and grid electrode plates according to the invention.

Figure 12:

In FIG. 12 shows a preferred plan view of the grid electrodes.

a. Cell grid. Cells can be regular or irregular polygons. The number of sides is from 3 to 20.

b. Rectangular lattice

Figure 13:

In FIG. 13 shows a preferred plan view of the grid electrodes.

a. Spoke split grille

b. Spoke-shaped split grille with side bars Figure 14:

In FIG. 14 shows a particularly preferred plan view of the grid electrodes. Dashed lines show segment boundaries.

a. Ring "fractally scalable" lattice divided into four segments

b. Annular "fractally scalable" array divided into six segments

Figure 15:

In FIG. 15 shows an electrode segment in the form of a divided grid according to the invention, consisting of an electrode bridge, which is attached to the apron of the reactor hood, and plates located perpendicular to it.

a) The electrode bridge protrudes from the bottom side and the plates protrude from the top side.

b) The electrode bridge protrudes at the top and bottom.

Figure 16:

In FIG. 16 shows rod electrodes according to the invention.

a) Rod electrode with tapered end: Front view (left), side view (right), top view (bottom).

b) Wedge-end rod electrode: Front view (left), side view (right), top view (bottom).

Figure 17:

In FIG. 17 shows a sketch of a moving bed reactor according to the invention with direct electrical heating and a rod electrode.

Figure 18:

In FIG. 18 shows a detailed drawing of the top hood of the rod electrode reactor in side view (upper) and in top view (lower).

Figure 19:

In FIG. 19 shows a sketch of the introduction according to the invention through the outer shell of the upper cap for supplying a stream of solids.

Figure 20:

In FIG. 20 shows a sketch of an inlet according to the invention through the outer shell of a top cap for an electric current busbar.

Figure 21:

In FIG. 21 shows a sketch of a fixed bed reactor according to the invention with direct electrical heating.

Figure 22:

In FIG. 22 is a freehand sketch of the top or bottom section of the device according to the invention to illustrate the calculation of the ratio of the cross-sectional areas of the top or bottom electrode (A _EI ) to the cross-sectional area of the corresponding electrically conductive connector (A _VE ).

Figure 23:

In FIG. 22 is a freehand sketch of a prototype electrode connection similar to the drawings in US Pat. No. 5,903,591 to illustrate the calculation of the ratio of the cross-sectional areas of the top or bottom electrode (A _EI ) to the cross-sectional area of the corresponding electrically conductive connector (A _VE ).

Legend:

1. Middle section of the reactor

2. Upper end section of the reactor / upper reactor hood / upper section of the device

3. Lower end section of the reactor / lower reactor hood / lower section of the device

4. Electrode bridges of the split upper electrode

5. Electrode bridges of the split bottom electrode

6. Solids flow line

7. Output gaseous product flow

8. Connection bus for electric current in the upper hood of the reactor

9. Cone distributor

10. Connector / apron in the upper hood of the reactor for contact with the electrodes

11. Flange on the upper hood of the reactor

12. Plate distributor for the flow of gaseous starting substances

13. Annular distributor of the flow of gaseous starting substances

14. Lower hood of the conical reactor

15. Solid product flow output

16. Connector / apron in the lower hood of the reactor for contact with the electrodes

17. Connection bus for electric current in the lower hood of the reactor

18. Flange on the lower hood of the reactor

19. Channels for lateral removal of the gaseous partial flow from the reaction zone

20. Ring manifold for side outlet

21. Lining of the reactor jacket with refractory, electrically and thermally insulating brickwork

22. Flange at the upper end of the reactor jacket

23. Electrical insulating intermediate ring between the flanges of the upper cap and the reactor jacket

24. Flange at the lower end of the reactor jacket

25. Electrical insulating intermediate ring between the flanges of the upper cap and the jacket of the reactor

26. Heated zone in the bulk layer of particles / in the moving layer

27. Lower heat transfer zone in bulk particle bed / moving bed

28. Upper heat transfer zone in bulk particle bed/moving bed

29. The wall of the middle section of the reactor

30. The wall of the lower hood of the reactor

31. The wall of the upper hood of the reactor

41. Outer shell of the upper hood of the reactor / upper section of the device

42. Flange on the upper hood of the reactor / lower section of the device

43. Electrically insulating, gas-tight bushings in the outer shell of the upper hood of the reactor

44. Flow line for flushing the gap between the inner and outer shell of the top cap

45. Output of the flushing stream from the gap between the inner and outer shell of the top cap

46. Through rigidly clamped in the apron of the reactor cap jumpers of the lattice electrode array

47. Plates or side bridges attached to one side of the electrode bridges of a split electrode

51. Neck on the outer shell with a welded flange

52. Connecting line with welded flange

53. Intermediate ring

54. Neck on the inner shell with a compensator and a welded plate with threaded holes

55. Seals for connecting flanges (51) and (52) with an intermediate ring (53)

56. Seals for the connection between the threaded plate (54) and the intermediate ring (53)

57. Sleeves made of electrical insulating material

58. Inlet pipe for solids flow

61. Neck on the outer shell with a compensator and a welded flange

62. Loose flange

63. Connecting pin for electric current in the lower shell of the cap

64. Connector for electric current as mating part to (63)

65. Sleeves made of electrical insulating material

66. Seals for connecting flanges (61) and (62) with a sleeve (65)

Fig. 67: Sleeve made of insulating material

71. Upper end section of the reactor vessel / upper reactor cap / upper section of the device, made in the form of a toruspherical bottom

72. Catalyst support for supporting the catalytically active fixed bed

73. Feed line for the flow of gaseous starting substances

74. Output gaseous product flow

AEI: Electrode cross-sectional area

AVE: Cross-sectional area of the connecting element

VE: Connector

H: Cap

D: Sealing and insulating ring

SW: Side wall

WD: Thermal insulation / masonry

F1: Flange on cap

F2: Flange on the side wall

EI: Electrode

T: Funnel

ZS: Cylindrical channel

Examples:

Comparative example (similar to US 5,946,342):

Methane pyrolysis should be carried out in a moving bed reactor with direct electrical heating. The volumetric flow of gaseous starting materials is 11000 Nm ³ /h. The thread contains 65 vol. % methane, 15 vol. % hydrogen and about 20 vol. % nitrogen. The flow of solid starting material, which is introduced into the reactor from above, is 11.45 t/h. The particle stream consists of coke with a carbon content of >99.5%. The diameter of the reaction zone is 3400 mm, the height of the electrically heated zone is 2000 mm. Graphite grid electrodes are located at the upper and lower ends of the heating zone, through which the electric current is introduced into the moving bed solid packing. Above the top electrode there is a heat transfer zone with a length of 1000 mm. Similarly, under the lower electrode there is a heat transfer zone with a length of 1000 mm. An electric current of 70,000 A should be introduced into the reactor. The electric current is introduced through twelve cylindrical electrode leads made of graphite, which are arranged in the shape of a star and evenly spaced around the circumference of the reactor jacket at the level of the corresponding electrode. The electrode leads have a diameter of 100 mm and a length of 1000 mm. In the electrode leads, 1000 kW is converted into heat. The specified power corresponds to 12.5% of the required process power. It is entered into the energy balance of the process as wasted power. In addition, the electrical energy dissipated in the form of heat must be removed. The problem is that the specific volumetric release in the electrode leads is 6.2 MW/m ³ . Accordingly, the heat flux density on the surface of the electrode supply is 154 kW/m ² . Without purposeful intensive cooling of the surface of the electrode supply, such a heat flux density can cause a temperature rise of more than 1000 K. With the indicated settings, a methane conversion of more than 94.2% is achieved. The maximum temperature in the reactor is 1230°C. The temperature difference between the solid product stream and the gaseous feed stream at the lower end of the reactor is practically zero, and the temperature difference between the gaseous product stream and the solid feed stream at the upper end of the reactor is 315K. Since excess heat occurs at a moderate temperature level, it can only be converted into mechanical energy with low efficiency.

Example according to the invention:

Methane pyrolysis should be carried out in a moving bed reactor with direct electrical heating. The volumetric flow of gaseous starting materials is 11000 Nm ³ /h. The thread contains 65 vol. % methane, 15 vol. % hydrogen and about 20 vol. % nitrogen. The flow of solid starting material, which is introduced into the reactor from above, is 13.5 t/h. The particle stream consists of coke with a carbon content of >99.5%. The diameter of the reaction zone is 3400 mm, the height of the electrically heated zone is 2000 mm. Molybdenum grid electrodes are located at the upper and lower ends of the heating zone, through which an electric current is introduced into the moving bed solid packing. The electrode is made in the form of a spoke-shaped divided grid with side bridges. It contains 12 electrode bridges (spokes) and eight electrode plates (side bridges) on each electrode bridge. The side profile of the electrode bridges is rectangular, 1600 mm long and 300 mm high. The cross section of the electrode bridges is hexagonal as shown in FIG. 11 Electrode bridges are made in the form of hollow profiles. The covering of the electrode rods consists of a multi-layer mesh fabric (6-layer HAVER & BOECKER POROSTAR STANDARD).

Electrode plates are attached along the electrode bridges at regular intervals of 200 mm. The electrode plates are made of molybdenum. The electrode plates are fixed at right angles and centrally on the electrode bridges as shown in FIG. 13b. The length of the electrode plates increases from the center to the outside. In particular, the length of the electrode plates is (175 mm, 260 mm, 350 mm, 440 mm, 525 mm, 610 mm, 700 mm, 790 mm). The side profile of the electrode plates is rectangular. The height of the electrode plates is the same and is 200 mm. The electrodes are made in the form of solid profiles. The cross section of the electrode plates is hexagonal as shown in FIG. 11, the thickness of the electrode plates is the same and is 20 mm. Electric current is introduced through the reactor caps. The top cap is in the shape of a torospherical bottom and is made of steel 1.4541 with a wall thickness of 20 mm. A cylindrical molybdenum apron 1000 mm long is screwed to the cap. The bottom cap is conical and made of steel 1.4541 with a wall thickness of 20 mm. A cylindrical molybdenum apron 1000 mm long is screwed to the cap. An electric current of 67500 A should be introduced into the reactor. Contact through the cap and twelve electrode jumpers: The heat loss is 19.5 kW, which corresponds to 0.2% of the transmitted power. This power leads to heating of the hoods by about 100 K above the ambient temperature and can be discharged to the environment without any special measures. The electrode bridges also function as conduits for lateral removal of a partial flow from the reaction zone. To do this, the electrode bridges pass through the apron and are open at the outer end. All electrode bridges terminate in an annular channel which functions as a collection channel for the side outlet. As a result, 15% of the gas stream is removed at the upper end of the heating zone of the reaction zone. With these settings, a methane conversion of over 96.5% is achieved. The maximum temperature in the reactor is 1320°C. The temperature difference between the solid product stream and the gaseous feed stream at the lower end of the reactor is 26 K, and the temperature difference between the gaseous product stream and the solid feed stream at the upper end of the reactor is 75 K. This achieves excellent heat integration in the reactor. Excess heat is removed mainly with a side flow at a temperature of 1270°C.

Brief summary:

Claims (15)

1. An electrically heated pressurized device with a nozzle for carrying out endothermic reactions with the upper (2), middle (1) and lower (3) section of the device, with at least one vertically located pair of electrodes (4, 5) embedded in the middle section, and all electrodes are installed in an electrically conductive solid nozzle (26), the upper and lower sections of the device have a specific conductivity of 10 ⁵ to 10 ⁸ S/m, and the middle section of the device is electrically isolated from the solid nozzle, characterized in that the upper and lower sections of the device are electrically isolated from the middle section of the device, the top electrode is connected through the top section of the device, and the bottom electrode is connected through the bottom section of the device or each of the electrodes is connected through one or more connecting elements (10, 16) electrically in contact with the indicated sections and the ratio of the cross-sectional area of the upper and lower electrode to the cross-sectional area corresponding to of the existing conductive connector or, without the use of a connector, the ratio of the cross-sectional area of the upper and lower electrode to the cross-sectional area of the corresponding conductive section of the device is from 0.1 to 10. 2. The device according to claim. 1, characterized in that the ratio of the cross-sectional area of the upper and lower electrode to the cross-sectional area of the corresponding conductive connecting element or, without the use of a connecting element, the ratio of the cross-sectional area of the upper and lower electrode to the cross-sectional area of the corresponding conductive section device is from 0.3 to 3. 3. The device according to claim 1, characterized in that the ratio of the cross-sectional area of the connecting element to the cross-sectional area of the solid nozzle is from 0.001 to 0.2 and/or the ratio of the cross-sectional area of the conductive upper and lower sections of the device to the cross-sectional area of the solid nozzle ranges from 0.001 to 0.2. 4. The device according to claim. 1, characterized in that the electrodes are made in the form of a spoke-like electrode array with 2-30 jumpers arranged in the shape of a star. 5. The device according to claim 1, characterized in that the electrode jumpers at their outer end are connected to at least one connecting element or the upper or lower section of the device and this connection is a separate rigid mount for positioning individual electrode jumpers. 6. The device according to claim. 1, characterized in that the temperature of the upper electrode is at least 350°C. 7. The device according to claim. 1, characterized in that the upper and lower sections of the device are made in the form of caps and can be removed from the middle section of the device. 8. The device according to claim 1, characterized in that the areas of conductive contacts between the electrode and the connecting element are between 0.1 and 10,000 cm ² . 9. The device according to claim. 1, characterized in that the vertical distance between the upper edge of the solid nozzle and the lower edge of the electrodes on the upper electrode is from 10 to 5000 mm, and the vertical distance between the upper edge of the electrodes on the lower electrode and the gaseous feed line is from 10 to 5000 mm. 10. Device according to claim 1, characterized in that the overlap of the cross section of the electrodes is between 1 and 20%. 11. The device according to claim 1, characterized in that the electrode bridges have in each case from 1 to 100 electrode plates attached to them and divide the cross section of the device into grid cells, the equivalent diameter of the grid cells being between 10 and 2000 mm, 12. The device according to at least one of paragraphs. 1-11, characterized in that the upper and/or lower section of the device is made of two shells and the inner shell is a conductive connecting element, and the outer shell is electrically isolated from the inner shell. 13. The method of carrying out endothermic gas-phase or gas-solid-state processes in the device according to one of paragraphs. 1-12, moreover, the carrier material of the solid nozzle is heat-resistant in the range from 500 to 2000 ° C and has an electrical conductivity in the range from 10 to 10 ⁵ S/cm, and carbon-containing materials are used as the carrier material, and the grain size of the carrier material ranges from 0.1 to 50 mm. 14. The method according to p. 13, characterized in that the electrically conductive solid nozzle is made in the form of a layer moving in countercurrent. 15. The method according to claim. 13 or 14, characterized in that at the upper edge of the solid nozzle, the difference between the temperature at the outlet of the gaseous product stream and the flow of solid particles is from 0 to 500 K, and at the lower edge of the solid nozzle, the difference between the outlet temperature solid product flow and gaseous feed flow is from 0 to 500 K.

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