Reactor and method for carrying out chemical reactions

The reactor design addresses safety and efficiency issues in electrically heated reactors by using electrical heating and inert gas supply to prevent explosions and control pressure, ensuring stable operation for endothermic reactions.

JP7731369B2Active Publication Date: 2025-08-29LINDE AG +1
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Patent Information

Application Number
JP2022564632
Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
Priority Date
2020-04-23
Filing Date
2021-04-22
Publication Date
2025-08-29
Estimated Expiration
2041-04-22

AI Technical Summary

Technical Problem

Existing chemical reactors face challenges in efficiently heating strongly endothermic reactions while minimizing carbon dioxide emissions and ensuring safety, particularly in electrically heated reactors where flammable gases can accumulate and pose explosion risks.

Method used

The reactor design incorporates electrical heating of reaction tubes as resistors, uses a star circuit for potential equalization, and supplies an inert gas atmosphere with discharge orifices to maintain a controlled environment, reducing the risk of explosions and pressure increases.

Benefits of technology

This approach enhances safety by preventing combustion of flammable gases, controlling pressure, and maintaining a non-flammable atmosphere, thus ensuring stable operation of electrically heated reactors.

✦ Generated by Eureka AI based on patent content.

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Abstract

The present invention relates to a reactor (100, 200) for carrying out chemical reactions, comprising a reaction vessel (10), one or more reaction tubes (20), and means (40) for electrical heating of the reaction tube(s) (20). The reaction vessel (10) has one or more discharge orifices (61, 62) that are permanently open or open above a set pressure level, and is provided with gas supply means (50) configured to supply an inert gas into the interior of the reaction vessel (10). A corresponding method is also the subject of the present invention.
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Description

[Technical Field]

[0001] The present invention relates to a reactor and a method for carrying out chemical reactions according to the preambles of the independent claims. [Background technology]

[0002] Many processes in the chemical industry use reactors in which one or more reactants pass through heated reaction tubes, where they react catalytically or non-catalytically. Heating serves, among other things, to overcome the activation energy required for the ongoing chemical reaction. The reaction may proceed entirely endothermically or, after the activation energy has been overcome, exothermically. The present invention is particularly concerned with strongly endothermic reactions.

[0003] Examples of such processes are steam cracking, various reforming processes, in particular steam reforming, dry reforming (carbon dioxide reforming), mixed reforming processes, alkane dehydrogenation processes, etc. In steam cracking, the reaction tubes are guided through the reactor in the form of a coil with at least one U-shaped bend in the reactor, while tubes extending through the reactor without a U-shaped bend are usually used in steam reforming.

[0004] The present invention is suitable for all such processes and reactor tube designs. The articles "Ethylene", "Gas Production", and "Propene" in the Ullmann Encyclopedia of Industrial Chemistry, for example, in the April 15, 2009 publication, DOI: 10.1002 / 14356007.a10_045.pub2, the December 15, 2006 publication, DOI: 10.1002 / 14356007.a12_169.pub2, and the June 15, 2000 publication, DOI: 10.1002 / 14356007.a22_211, are referenced here purely for illustrative purposes.

[0005] The reaction tubes of the corresponding reactor are conventionally heated using burners, in which case the reaction tubes are passed through a combustion chamber in which the burners are also arranged.

[0006] However, as described, for example, in DE 10 2015 004 121 A1 (as well as EP 3 075 704 A1), there is currently an increasing demand for synthesis gas and hydrogen, for example, produced with or without reduced local carbon dioxide emissions. However, this demand cannot be met by processes that typically use combustion reactors, typically by burning fossil energy carriers. Other processes are ruled out, for example, due to high costs. The same applies to the production of olefins and / or other hydrocarbons by steam cracking or dehydrogenation of alkanes. Even in such cases, methods that release less carbon dioxide in situ are desirable.

[0007] Against this background, the aforementioned DE 10 2015 004 121 A1 proposes electrical heating of a steam reforming reactor in addition to combustion. In this case, for example, one or more voltage sources are used, providing three-phase AC voltage to three external conductors. Each external conductor is connected to a reactor tube. A star circuit is formed, with a star point realized by a collector, to which the pipeline opens and the reactor tube is electrically connected. In this way, the collector ideally remains potential-free. The collector is positioned below and outside the combustion chamber, preferably extending transversely, i.e., horizontally, relative to the vertical line. WO 2015 / 197181 A1 also discloses a reactor in which the reactor tubes are arranged in a star point circuit.

[0008] In addition to direct heating of the reactor tubes, in which an electric current flows through the reactor tubes, there are a variety of concepts for indirect electrical heating of the reactor tubes. Indirect electrical heating can take the form of external electrical heating, as described, inter alia, in WO 2020 / 002326 A1. Internal heating is also possible, as disclosed, for example, in WO 2019 / 228798 A1. In addition to resistive or impedance heating, inductive electrical heating of the reactor tubes or catalyst bed can be performed, as described in WO 2017 / 072057 A1. Induction heating can be achieved, for example, by heating internal or external heating elements or the reactor tube itself. Direct (non-inductive) heating of the reactor tubes is also disclosed in DE 10 2015 004 121 A1. The basic concept for heating can be realized with multi-phase or single-phase alternating current or direct current. In the case of direct heating of the reactor with direct current or single-phase alternating current, a star circuit with a potential-free star point cannot be realized, but the power input can in principle be realized in the same way as in the case of polyphase direct current. The invention is suitable for all variants of electric heating.

[0009] WO 2004 / 091773 A1 describes an electrically heated reactor for carrying out gas reactions at high temperatures. The reactor is composed of a reactor block, one or more monolithic modules of a material suitable for electrical heating, surrounded by a housing with channels extending through the modules and designed as reaction channels, and a device for conducting or inducing electric current in the reactor block. The safety during operation of such a reactor is enhanced in that the housing of the reactor block has a double-walled jacket that hermetically seals the reactor block and at least one device for supplying an inert gas to the double-walled jacket.

[0010] As will also be explained below, in the case of electrically heated reactors, special safety-related aspects must be observed. The aim of the present invention is to take these aspects into account and thus to identify measures which allow advantageous operation of electrically heated reactors. [Prior art documents] [Patent documents]

[0011] [Patent Document 1] DE 10 2015 004 121 A1 [Patent Document 2] EP 3 075 704 A1 [Patent Document 3] WO 2015 / 197181 A1 [Patent Document 4] WO 2020 / 002326 A1 [Patent Document 5] WO 2019 / 228798 A1 [Patent Document 6] WO 2017 / 072057 A1 [Patent Document 7] WO 2004 / 091773 A1 [Non-patent literature]

[0012] [Non-Patent Document 1] Ullman Encyclopedia of Industrial Chemistry, DOI:10.1002 / 14356007.a10_045.pub2, April 15, 2009 [Non-patent document 2] Ullman Encyclopedia of Industrial Chemistry, DOI:10.1002 / 14356007.a12_169.pub2, December 15, 2006 [Non-patent document 3] Ullman Encyclopedia of Industrial Chemistry, DOI:10.1002 / 14356007.a22_211, June 15, 2000 Summary of the Invention

[0013] Against this background, the present invention proposes a reactor and a method for carrying out chemical reactions according to the preambles of the independent claims. Embodiments are the subject of the dependent claims and the following description.

[0014] In the electrified furnace concept underlying the present invention (the term "furnace" is generally understood to denote the corresponding reactor or at least its insulated reaction space), for example, the reaction tubes or corresponding tube segments (hereinafter also referred to as "tubes" for short) themselves are used as electrical resistors for generating heat. This direct approach has the advantage of being more efficient and allowing a higher achievable heat flux density compared to indirect heating by external electrical heating elements. However, as mentioned above, it is also possible within the framework of the present invention to carry out any other type of electrical heating (direct or indirect, as resistance, impedance or induction heating, in the form of single-phase or multi-phase alternating current or by direct current), if said heating proves to be advantageous.

[0015] When heating with multiphase alternating current, power is supplied to the directly heated reactor tubes via M separately connected phases. The conductive reactor tubes connected to the M phases can also be electrically connected at their other ends to a star point. The number of phases M is preferably 3 and corresponds to the number of phases in a conventional three-phase current power supply or network. However, in principle, the invention is not limited to the use of three phases and can also be used with a greater number of phases, for example 4, 5, 6, 7 or 8. The phase offset is therefore preferably 360° / M, i.e. 120° for a three-phase current.

[0016] In electrical heating with multiphase alternating current, the equalization of potentials between the phases is achieved at the star point by a star circuit, which ideally eliminates the need for electrical insulation of the connected pipelines. This represents a particular advantage of such furnace concepts, since the destruction of metal reactor tubes to insulate certain sections is undesirable, especially at the high temperatures used and the high material and construction costs involved.

[0017] However, the measures proposed by the present invention and described below are equally suitable for use with single-phase AC and DC current, and the present invention can be used in both AC-heated and DC-heated reactors, or in corresponding mixed configurations. As mentioned above, the present invention is also suitable for use with indirectly heated reactor tubes. In the case of a DC configuration, only the type of current source and the power input or the area of ​​the reactor tube facing the corresponding section to which current is supplied differ from the AC configuration, for example. In the latter, electrical connections between different tube sections are only performed optionally. Since no potential-free star points exist in the DC configuration, it is necessary to provide appropriate current discharge elements that safely return the current flow to the outside. The latter can be designed in the same way as the power input, as described below.

[0018] The present invention relates to the protection of electrically heated reactors of the type described, which is necessary in particular in the event of damage to the reactor tubes ("coil shredders"). In the event of such damage, in particular one or more reactor tubes may be completely severed, whereas the present invention advantageously provides for a less severe leakage. In the event of such damage, a sudden or gradually progressing leakage of flammable gas occurs into the reactor vessel, which is largely sealed for thermal insulation purposes.

[0019] Such damage is less of a safety concern in conventional combustion reactors than in purely electrically heated reactors, particularly those used according to the present invention. This is because flammable gases, e.g., in the form of hydrocarbon-steam mixtures, emanating from the reaction tubes in a combustion reactor can react immediately and continuously through combustion occurring in the reaction vessel or corresponding combustion chamber, or because combustion has already substantially "inerted" the gas space surrounding the reaction tubes, with a significantly reduced oxygen content. In contrast, in the case of purely electrical heating, the corresponding flammable gases can accumulate in the reaction vessel, where they can reach the limit of explosion or detonation, e.g., with the normal oxygen content of air and temperatures exceeding the autoignition temperature. Even in the case of combustion without explosion or detonation, the energy input from complete or incomplete combustion can lead to overheating. The complete or incomplete combustion itself, together with the volume of gases escaping from the reaction tubes, can result in a particularly significant pressure increase. The present invention reduces this pressure increase because combustion of the gas mixture is avoided.

[0020] In the terms of the claims, the present invention relates to a reactor for carrying out chemical reactions, the reactor comprising a reaction vessel (i.e., an insulated or at least partially insulated region), one or more reaction tubes, and means for electrical heating of the reaction tube(s). The reactor proposed by the present invention is set up to carry out chemical reactions at the temperature levels described below, in particular for high-temperature reactions. The reaction tubes are guided through the reactor with at least one U-shaped bend or extend through the reactor without any U-shaped bend. The means for electrical heating can be designed as broadly described above. On the one hand, this means can be means for supplying power to the reaction tube(s). This means bringing about a current flow and corresponding heating in the reaction tube(s), for example rigid current rods guided in the reactor, but the means can also be means for indirect heating, such as resistance and / or induction heating devices that transfer heat conductively and / or by thermal radiation to the reaction tube(s) or tubes, or that generate eddy currents in the reaction tube(s) or the catalyst bed, and thus generate heat.

[0021] Within the framework of the present invention, the reaction vessel has one or more discharge orifices that are permanently open or that are set to open above a set pressure level, and is provided with gas supply means that are set to supply an inert gas into the interior of the reaction vessel.

[0022] In the following, reactors designed according to the invention or according to different embodiments of the invention will mainly be described, with the corresponding descriptions in each case also applying to the corresponding methods, by means of which correspondingly configured means in each case carry out the specified method steps.

[0023] To supply the inert gas, the gas supply means may comprise, for example, a supply nozzle or an opening opening into the reactor, together with a line and a gas reservoir connected to the line, so that the inert gas can be supplied to the interior of the reactor. The reactor is in particular a chamber surrounded by a large portion, i.e., at least 90, 95, or 99%, of the interior by an insulating wall. The interior of the reactor is the area in which the reaction tubes are arranged and surrounded by the reactor wall. For example, the wall of a double-walled reactor is not part of the interior.

[0024] In all embodiments of the present invention, the inert gas can be a gas or gas mixture having a superatmospheric content of nitrogen, carbon dioxide, and / or argon, respectively, or the gas supply means can be configured to provide the corresponding inert gas, for example, by retaining the corresponding inert gas available or by mixing a pure gas, i.e., mixing a pure gas with air. In particular, the content of non-flammable gas can exceed 50%, 60%, 70%, 80%, or 90%. Thus, the inert gas does not need to be a pure "inert gas" in the traditional sense; rather, it is sufficient if the inert gas, particularly the content of non-flammable gas, at least partially reduces the flammability range of the mixture, i.e., reduces the risk of fire, explosion, or implosion. Inert gases for use within the framework of the present invention can in particular have a reduced oxygen content, e.g., an oxygen content of less than 10%, 5%, 1%, 0.5%, or 0.1%. In particular, the inert gas can also be (completely or substantially) oxygen-free.

[0025] The proposed measures provide a controlled atmosphere containment for the thermal insulation and safety-related protection of electrically energized high-temperature reactors. Within the scope of the present invention, in particular, fully electric heating can be provided. That is, the heating of the reaction tubes, at least within the reaction vessel, is preferably carried out predominantly or exclusively by thermal heating, i.e., in particular, at least 90, 95, or 99% of the total heat introduced therein is carried out by electrical heating means. Since heat input via the gas mixture conducted through the reaction tube(s) remains ignored here, this proportion particularly relates to the heat transferred from the outside to the wall(s) of the reaction tube(s) in the reaction vessel or generated within the reaction vessel at this wall or catalyst bed.

[0026] Thus, in its most general form, the invention describes a confinement for a high-temperature reactor (wherein the term "high-temperature reaction" refers in particular to reactions proceeding at temperatures above 500°C, especially between 700 and 1000°C) equipped with electrical heating and fed with hydrocarbons, which confinement 1. provides an inert atmosphere around the tubes and 2. is not permanently sealed. Particularly preferred is the application to electrically heated reactors where the process gas temperature is close to or exceeds the autoignition temperature of the hydrocarbons contained in the process gas. The term "process gas" refers to the gas or gas mixture flowing through the reaction tube or tubes.

[0027] Embodiments of the invention differ in particular by the embodiment of one or more discharge orifices, which are permanently open or are set to open above a set pressure level, although combinations of correspondingly designed discharge orifices are also possible in principle.

[0028] In a group of embodiments, hereinafter referred to as "first group," the discharge orifice(s) are permanently open. This means that the discharge orifice(s) do not offer any mechanical resistance to the flow of fluid into or out of the reactor vessel, except for a possible existing narrowing of the flow cross section. Thus, the opening(s) are not closed.

[0029] In contrast, in a group of embodiments hereinafter referred to as the "second group," one or more discharge orifices are configured to open above a predetermined pressure level. The one or more discharge orifices are configured to close below the set pressure level or to open temporarily or permanently when the set pressure level is reached. In this respect, the term "permanently" open specifically refers to an irreversible opening, which in this embodiment does not reclose due to the release of gas after a subsequent undershoot of the set pressure level. In contrast, the term "temporarily" open refers to an opening that is reclosed.

[0030] To open at a set pressure level, the discharge orifice or orifices may have, for example, one or more spring-loaded or weight-loaded flaps with an opening resistance defined by a spring or load characteristic value and thus only open at the corresponding pressure. In one embodiment of the second group of embodiments, one or more burst disks or pressure relief valves may also be used in a manner known per se. It is also possible to detect the pressure value, for example, by a sensor, and trigger any type of opening mechanism, such as a firing mechanism or an electrically actuated drive, if a set threshold is exceeded. This makes it possible to release a sufficiently large cross-section that is kept closed in the described manner during normal operation, if necessary, within a short response time.

[0031] In particular, in the first group of embodiments, and possibly also in the second group of embodiments, the reactor can be configured to be constantly purged with inert gas. In other words, the described gas supply means is configured to continuously supply inert gas into the reaction vessel. In the first group of embodiments, the inert gas can flow out, in particular primarily through one or more permanently open discharge orifices, possibly through additional discharge orifices, in particular through unavoidable or intentionally created gas leaks or bypasses, for example, to an existing chimney. In the second group of embodiments, in which the one or more permanently open discharge orifices are normally closed, additional openings for the outflow of inert gas are provided, for example, by a bypass line to a chimney, or are necessarily present, for example, due to a leak in the reaction vessel.

[0032] However, instead of constant purging, provision can be made for one-time or periodic supply of inert gas to the reactor according to one or more predetermined criteria. The gas supply means is then configured for such operation. The one or more predetermined criteria can include, for example, reaching a set pressure value and / or a set concentration, such as a minimum or allowable oxygen content. However, one criterion can also be the first time the reactor is operated. In particular, continuous measurements can be performed, and the supply of inert gas can be initiated whenever the corresponding measured value indicates that the set criteria are no longer met. The one-time or periodic supply of inert gas can be provided below the pressure value at the opening of one or more discharge orifices, particularly in the second group of embodiments, because this prevents the inert gas from freely escaping and allows the inert gas to be retained in the reactor for a long period of time.

[0033] In a particularly preferred embodiment of the first group of embodiments, the reactor is configured for operation at a reduced pressure. In this case, a means for forming a gas flow exiting the reactor is provided. In this regard, in this group of embodiments, one or more permanently open discharge orifices can be connected to a chimney with a sufficient chimney opening, also in a permanently open state. This increases the temperature inside the reactor, creating a static negative pressure within the reactor, which in turn reduces the density of the contained gas volume. In this regard, it is also possible to provide, for example, the use of a blower until a corresponding static negative pressure is formed.

[0034] In contrast, in particularly preferred embodiments of the second group of embodiments, the reactor is configured for operation of the reaction vessel at an overpressure level, which can be achieved in particular by supplying inert gas to an overpressure level that is below the opening pressure of the discharge orifice.

[0035] Systems according to the first group of embodiments that are to some extent inerted and "open" to the environment (in particular with a slight negative pressure in the reactor vessel as a result of the chimney effect) or "openable" systems according to the second group of embodiments of the invention (in particular capable of operating at a certain overpressure in the reactor vessel) can limit the rate of pressure rise and damage to the reactor tubes in the event of hydrocarbon leakage to an acceptable amount that meets the design limits of the reactor vessel.

[0036] As a result of the concept of supplying the reactor with an inert gas, the oxygen content present in the reactor can be reduced. The reaction rate of the escaping hydrocarbons in case of damage and the significant additional volume increase (as a result of the reaction heat input) scales to a first approximation with the oxygen partial pressure or molar oxygen content inside the box.

[0037] In both groups of embodiments of the present invention, as a result of the supply of inert gas, advantageously the walls of the reaction vessel do not have to be designed to be completely gas-tight, as high temperatures in certain places where movement is required would result in very high material costs, for example, using heat-resistant bellows structures. In the case of operation at reduced pressure level in conjunction with a chimney, air could be drawn into the reaction vessel by a corresponding leak, but this air is exhausted and diluted by the continuous flow provided by the chimney. In this way, safety issues in the use of inert gas or its components that may be harmful to breathing can be avoided. In contrast, in the case of operation at overpressure level, the pressure propagation is uniform, so that the inflow of air into the reaction vessel can be reliably avoided. Inert gas that escapes due to a leak can be exhausted or diluted, for example, by providing sufficient ventilation outside the reaction vessel.

[0038] As a result of the proposed concept of supplying the reactor with an inert gas, the oxygen content in the reactor can be reduced. As can be utilized according to the present invention, the reaction rate of the escaping hydrocarbons, and therefore the rate of significant additional volume increase (as a result of the reaction heat input), correlates, to a first approximation, with the oxygen partial pressure or oxygen mole fraction. This correlation is summarized in Table 1 below, where xO2 represents the molar oxygen content and V reak represents the reaction-related volume increase rate.

[0039] Therefore, the gas supply means is advantageously set to adjust the maximum oxygen content in the reaction vessel based on the sizing of the chimney or chimneys.

[0040] [Table 1]

[0041] Maximum allowable pressure p max depends on the mechanical stability of the respective chamber or surrounding confinement. This pressure is the pressure in the relevant chamber volume V in the case of a coil shredder or other corresponding safety-related event. Box , chimney diameter DChimney and pressure p, which depends on the molar oxygen content box It must be at least as large as p max ≧p box =f(V BOX ,D Chimney ,xO2)

[0042] This requirement becomes the design criterion for the dimensioning of the chimney, i.e., its communication to the permanently or temporarily existing environment via one or more discharge orifices, and vice versa. This relationship will now be explained again with reference to Figure 9. For example, if a maximum allowable pressure rise of 20 mbar is used here as a criterion, as illustrated by dashed lines 601, 602, then the reaction-related volume increase rate must be at most about 10 mbar, in order to be able to use a chimney (dashed line 601) with a diameter of 500 mm. 3 / s, which results in a maximum oxygen content of approximately 1%, which is adjusted by inerting.

[0043] Conversely, if inerting to a maximum oxygen content of 1% is performed, a chimney diameter of at least 500 mm must be used. To be able to use a chimney with a diameter of 900 mm (dashed line 602), the volume increase is approximately 42 m 3 / s, resulting in a maximum oxygen content of approximately 4%, which is regulated by inerting. Conversely, and similarly to the explanation above, if inerting to a maximum oxygen content of 4% is used, a chimney diameter of at least 900 mm must be used here.

[0044] The lower the oxygen content in the reactor, the smaller the volume increase. As a result, the diameter of the emergency chimney, which requires the evacuation of additional volume, can be reduced. For efficient oxygen content restriction, it is important to always have a sufficiently good seal against the environment, in order to prevent as much as possible or sufficiently the intrusion of oxygen-containing false air. However, as explained, a perfect seal is not required.

[0045] In other words, within the framework of the present invention, the maximum oxygen content in the reaction vessel is adjusted by the inert gas, which is selected in the first group of embodiments in which one or more chimneys are present based on the dimensioning of the chimney or chimneys, or the gas supply means is set to supply the inert gas or adjust the oxygen content based on this. The gas supply means can also be set in particular to supply the gas so as not to exceed the target pressure. In the second group of embodiments, the supply can similarly be based on the oxygen concentration or the target pressure and the dimensioning of the chimney.

[0046] The amount of inert gas supplied can be regulated by corresponding regulation means, in particular based on oxygen measurements in the reaction vessel or, if present, in the chimney, so that the oxygen content can be kept constant during operation. A corresponding safety concept includes, in accordance with the invention, preventing or continuing the operation of the reactor if the measured oxygen content exceeds the target oxygen content. For example, the supply of hydrocarbons to the reaction tubes and / or their heating can be released only if the required oxygen content is lowered. If a fault is detected, the reaction operation can generally be prevented by adding hydrocarbons to the reaction tubes.

[0047] Unacceptable leakage of gas from the reactor tubes can be detected, for example, via a pressure measurement sensor, and if a gas leakage is detected, the supply of hydrocarbons to the reactor tubes can be prevented in order to minimize the total leakage of hydrocarbons.

[0048] The hydrocarbon content (e.g. in the form of carbon monoxide equivalents) in the reactor vessel or, if present, the chimney, can also be measured continuously in order to detect very small damages (leakage without a sudden pressure rise). Likewise, unacceptable values ​​can result in the avoidance of hydrocarbon feed.

[0049] Thus, the invention more generally encompasses determining a value characterizing gas leakage from one or more reactor tubes based on pressure and / or hydrocarbon measurements, and initiating one or more safety measures if this value exceeds a set threshold.

[0050] To carry out a chemical reaction, the method proposed by the invention uses a reactor having a reaction vessel, one or more reaction tubes and means for electrical heating of the reaction tube or tubes. According to the invention, the reaction vessel used is a reaction vessel having one or more discharge orifices, which are permanently open or set to open above a set pressure level, and an inert gas is supplied to the interior of the reaction vessel by means of a gas supply means according to the invention.

[0051] For further features and advantages of the corresponding method, in which a reactor according to one of the developments of the invention already described is advantageously used, reference is made to the above description.

[0052] The invention will be further elucidated below with reference to the accompanying drawings illustrating the development of the invention with reference to and comparison with the prior art. [Brief explanation of the drawings]

[0053] [Figure 1] FIG. 1 is a schematic diagram showing a reactor for carrying out chemical reactions according to a non-inventive development. [Figure 2] FIG. 2 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 3] FIG. 3 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 4] FIG. 4 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 5] FIG. 5 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 6] FIG. 6 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 7] FIG. 7 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 8] FIG. 8 is a schematic diagram illustrating a reactor for carrying out chemical reactions, according to an embodiment of the present invention. [Figure 9] FIG. 9 is a schematic diagram illustrating the principle of chimney sizing according to an embodiment of the present invention. DETAILED DESCRIPTION OF THE INVENTION

[0054] In the following figures, elements that correspond to one another functionally or structurally are designated by the same reference numerals and will not be described again for the sake of clarity. Where components of a device are described below, the corresponding description also relates in each case to the method carried out thereby, and vice versa. The description of the figures repeatedly refers to AC heating. However, as mentioned above, the invention is also equally suitable for the use of DC for heating. Reference is made here to the above description.

[0055] FIG. 1 shows diagrammatically a reactor for carrying out chemical reactions according to a non-inventive development.

[0056] Here, a reactor designated 300 is set up to carry out a chemical reaction. For this purpose, the reactor comprises, in particular, an insulated reaction vessel 10 and a reaction tube 20, of which multiple tube sections, designated 21 in only two cases here, extend between a first zone 11' and a second zone 12' in the reaction vessel 10, respectively. The reaction tube 20, which will be explained in more detail below with reference to FIG. 2, is attached to the sealing or support structure of the reaction vessel by means of a suitable suspension 13. In the lower region, the reaction vessel may comprise, in particular, a furnace (not shown). Needless to say, in each case, multiple reaction tubes may be provided here and subsequently.

[0057] FIG. 2 shows a schematic diagram of a reactor, generally designated 100, for carrying out chemical reactions, according to an embodiment of the present invention.

[0058] The zones previously designated by 11' and 12' now take the form of regions 11 and 12, and the tube sections 21 for heating in the first region 11 can in each case be electrically connected to phase connections U, V, W of a polyphase AC power supply 41 via connection elements 42, resulting in the formation of means, generally designated 40, for electrically heating the reactor tubes 20. Specific types of connections, such as switches, are not illustrated. In the embodiment of the invention illustrated here, the tube sections 21 are integrally connected to one or more reactor tubes 20 and are conductively connected to one another in the second region 12 by connection elements 30 arranged within the reactor vessel 10. A neutral conductor may also be connected to the connection elements 30.

[0059] In the example illustrated here, a star circuit of multiple alternating current phases is thus realized, but as mentioned several times, the invention can also be provided using single-phase AC heating, DC heating or other heating means, for example induction heating or indirect heating in the sense explained above.

[0060] Thus, in the reactor 100 illustrated here, multiple tube sections 21 of one reactor tube 20 (although multiple such reactor tubes 20 may be provided) are arranged side by side within the reactor vessel 10. The tube sections 21 meet each other via U-shaped bends 23 (only partially designated) and are connected to a feed section 24 and an extraction section 25.

[0061] A first group (lower in the drawing) of U-shaped bends 23 are arranged side by side in the first region 11, and a second group (upper in the drawing) of U-shaped bends 23 are arranged side by side in the second region 12. The U-shaped bends 23 of the second group are formed in the connecting element 30, and the pipe portion 21 extends from the connecting element 30 in the second region 12 to the first region 11. The power input element 52 can be designed as desired, for example to be rigid, have a rod-shaped portion and be able to pass through the wall of the reaction vessel 10.

[0062] Means for supplying inert gas to the reaction vessel are generally indicated at 50. As illustrated by arrow 53 (and accordingly only partially shown), the inert gas is supplied to the reaction vessel 10, in particular via wall openings, nozzles, etc. in one or more walls of the reaction vessel 10. For providing and supplying the inert gas, suitable gas supply means are provided, also shown here in a highly simplified manner, and comprise, for example, one or more gas tanks 51 and corresponding lines 52.

[0063] FIG. 3 shows diagrammatically a reactor for carrying out chemical reactions, generally designated 200, according to an embodiment of the present invention.

[0064] In reactor 200, the tube sections, here by contrast designated 22, in each case comprise a tube section 22 consisting of a plurality of reaction tubes 20, which are arranged side by side in a fluidly disconnected manner in the reaction vessel 10 and which are connected in each case to a feed section 24 and an extraction section 25. For the remaining elements, explicit reference is made to the above explanations relating to the previous figures.

[0065] The use of the connection element 30 within the framework of the present invention is then optional, but is advantageous, especially when using multiphase AC heaters. Again, the power input element 42 is illustrated in a very simplified manner. The inert gas supply is provided by arrow 53, substantially as described above. The power input element 42 can have a sleeve-like region 43, which is arranged in the first region 11 around the reactor tube 20 or tube section.

[0066] 4 to 8 show further simplified partial views of a reactor according to an embodiment of the invention, in each case illustrating a chimney 60. The gas supply means 50 for supplying inert gas are not shown, nor are the means for electrical heating 40. The reactor tube 20 is shown with a U-shaped bend according to FIG. 2, but can also be designed in any other form, for example according to FIG. 3. The inert gas supply is indicated only at one point by an arrow 53.

[0067] False air can enter the reactor vessel 10 through one or more false air inlets, as shown by arrows 54 in FIG. 4. In the illustrated embodiment, the reactor vessel 10 has a permanently open discharge orifice 61 connected to a chimney 60. The supply of inert gas and the high temperature within the reactor vessel 10 associated with the end 63 of the chimney 60 result in a flow indicated by arrows 64. Within the reactor, if the supply of inert gas is carried out in an appropriate manner, the high temperature will create a static pressure p Box This static pressure is greater than the atmospheric pressure in the surrounding environment, p Atm In other words, the amount of purge gas is not selected too large here. With a very large amount of purge gas, the pressure loss in the chimney 60 can cause the internal pressure in the reaction vessel 10 to approach or even exceed the external pressure.

[0068] In this embodiment, where there is a negative pressure in the reactor, this amount avoids the occurrence of a backflow of ambient air into the reactor 10 and also compensates for low levels of false air ingress due to insufficient sealing. The supply of inert gas to the reactor 10 is regulated in particular by the oxygen measurement value 65 in the chimney 60, so that the oxygen content can be kept constant during operation.

[0069] In contrast to the embodiment according to Figure 4, the reaction vessel 10 according to Figure 5 is operated at an overpressure level, where an inert gas is continuously fed into the reaction vessel 10. The reaction vessel 10 has an outlet orifice 62, for example in the form of a rupture disc, which is set to open above a set pressure level.

[0070] In this alternative embodiment with pressurized operation, the supply of inert gas compensates for low gas leakage to the atmosphere, here indicated by arrow 55. In this case, the purge volume can be adjusted by the pressure measurement in the reaction vessel 10. For continuous purging of the inert gas, a correspondingly dimensioned outlet opening can be provided in a safe place (in the region of the chimney 60 or another not easily accessible, hazard-free place) so that a flow 66 from the reaction vessel 10 occurs.

[0071] 5, the reactor vessel 10 according to FIG. 6 is operated at an overpressure level. Here too, the reactor vessel 10 has a discharge orifice 62, for example in the form of a rupture disk, which is set to open above a set pressure level. However, since a continuous flow of inert gas is not provided, no flow 66 is formed in this embodiment.

[0072] In this alternative embodiment involving pressurized operation, the initial inerting purge is performed, for example, only during preparation for operation. During subsequent operation, only an amount of inert gas equivalent to the leakage flow from the reaction vessel to the atmosphere is added, either continuously or at intervals. Thus, in this embodiment, there is no permanently open outlet for releasing inert gas to the atmosphere during normal operation.

[0073] In the embodiment according to FIGS. 4 to 6, operation of the reactor with hydrocarbons is advantageously released only when the required oxygen content falls below.

[0074] In the embodiments according to FIGS. 4 and 5 with continuous purging, the oxygen content is preferably measured at the purge gas discharge downstream of the reaction vessel 10 (e.g., in the chimney 60 or another discharge line). Additionally or alternatively, the oxygen content can be measured at one or more locations in the region of the reaction vessel 10 by a suitable measurement method (e.g., a tunable diode laser, a zirconium oxide probe, a GC paramagnet). In the embodiment according to FIG. 6, the oxygen content can similarly be measured in the purge gas discharge line optionally used for initial inerting and / or in the reaction vessel 10 itself. Additionally, according to the embodiments according to FIGS. 5 and 6, the pressure in the reaction vessel can be continuously measured and monitored for early detection of unacceptable inert gas losses.

[0075] As shown in the more detailed drawings below, the chimney 60 of all embodiments shown so far can have structural elements (so-called velocity seals / confusers), particularly in the region of the chimney wall, to avoid a return flow of air back into the reaction vessel 20 (e.g., due to free convection).

[0076] 7 shows a schematic diagram of a reactor for carrying out chemical reactions according to an embodiment of the present invention in an extension of the previous figure description, with the above-described elements not being shown again in part. For further explanation, see in particular FIG. 4 above.

[0077] As shown here, an ignition device or pilot burner 68 can further be installed in the region of the chimney outlet 63 to at least partially prevent unburned hydrocarbons from escaping into the atmosphere in the event of a disaster. As further illustrated, inert gas is supplied to the reaction vessel 10 on different sides. The walls of the reaction vessel 10 and the wall passages of the fasteners or power input devices, respectively, can advantageously be designed to be gas-tight and are indicated by 15. I and O represent the supply and removal of process gas from the reaction tube 20.

[0078] Figure 8 illustrates a schematic diagram of a reactor for carrying out chemical reactions according to an embodiment of the invention, extending the representation according to Figure 7 or a variant thereof. Components already described with reference to Figure 7 are not here provided again, in part, with reference numerals.

[0079] As exemplified here, the chimney 60 may have suitable insulation 69 in the area adjacent to the reaction vessel 10. The chimney 70 may have a height h of, for example, 20 to 50 meters above ground level. The chimney 60 may be provided with a so-called velocity seal 66.

[0080] FIG. 9 shows, in diagram form, a schematic representation of the principle of chimney sizing according to an embodiment of the present invention, in which the oxygen content in percent is plotted on the horizontal axis and the rate of volume increase associated with the reaction is plotted on the m 3 / s are plotted on the vertical axis. Graph 601 illustrates the relationship already explained with reference to the table. Dashed line 602 shows the value required for a maximum pressure rise of 20 mbar for a chimney diameter of 500 mm, and dashed line 603 shows the corresponding value for a chimney diameter of 900 mm.

Claims

1. A reactor (100, 200) for carrying out a chemical reaction, comprising a reaction vessel (10), one or more reaction tubes (20), and means (40) for electrical heating of said one or more reaction tubes (20), said reaction tubes (20) being guided through said reaction vessel (10) with at least one U-shaped bend or extending through said reactor (100, 200) without a U-shaped bend, said reaction vessel (10) being provided with one or more discharge orifices that are permanently open or that are set to open above a set pressure level.

1. A reactor (100, 200) comprising a gas supply means (50) having a vent (61, 62) and configured to supply an inert gas to the reaction vessel (10), and means configured to prevent reaction operation by blocking the supply of hydrocarbons to the one or more reaction tubes (20) if the oxygen content and / or pressure and / or hydrocarbon content measured in the reaction vessel (10) and / or in a discharge line downstream of the reaction vessel exceed respective set values.

2. 2. The reactor (100, 200) according to claim 1, configured to carry out the chemical reaction at a temperature level above 500°C, in particular between 700°C and 1000°C.

3. 3. The reactor (100, 200) of claim 1 or claim 2, wherein the one or more discharge orifices (61) are permanently open.

4. 3. The reactor (100, 200) of claim 1 or claim 2, wherein the one or more discharge orifices (62) are configured to close below a set pressure level and to open temporarily or permanently when the set pressure level is reached.

5. 5. The reactor (100, 200) of any one of claims 1 to 4, wherein the gas supply means (50) is configured to continuously supply the inert gas into the reaction vessel (10).

6. 6. The reactor (100, 200) according to any one of claims 1 to 5, wherein the gas supply means (50) is configured to supply the inert gas to the reaction vessel (10) either once or periodically.

7. 7. The reactor (100, 200) according to any one of claims 1 to 6, wherein the gas supply means (50) is configured to provide as the inert gas a gas or gas mixture having a superatmospheric pressure content of nitrogen, carbon dioxide and / or argon, respectively.

8. The reactor (100, 200) according to any one of claims 1 to 7, wherein the one or more discharge orifices (61, 62) are connected to one or more chimneys (60).

9. 9. The reactor (100, 200) of claim 8, wherein the gas supply means (50) is configured to adjust the maximum oxygen content in the reaction vessel (10) based on the sizing of the chimney (60).

10. 10. The reactor (100, 200) of any one of claims 1 to 9, wherein the gas supply means (50) is configured to regulate the amount of inert gas based on an oxygen measurement.

11. A method for carrying out a chemical reaction, in which a reactor vessel (10) is used, which has one or more reaction tubes (20) and means (40) for electrical heating of said one or more reaction tubes (20), said reaction tubes (20) being guided through said reactor (100, 200) with at least one U-shaped bend or extending through said reactor (100, 200) without a U-shaped bend, said method being carried out in such a way that said reactor vessel (10) used is permanently open or is set to open above a set pressure level.

1. A method for producing a reactor vessel (10) having a plurality of discharge orifices (61, 62), characterized in that an inert gas is fed to the reactor vessel (10) using a gas supply means (50), and that means are provided which are configured to prevent reaction operation by blocking the feed of hydrocarbons to the one or more reaction tubes (20) if the oxygen content and / or pressure and / or hydrocarbon content measured in the reactor vessel (10) and / or in a discharge line downstream of the reactor vessel exceed respective set values.

Citation Information

Patent Citations

  • Reactor tubes that can often be heated electrically and by means of fuel for steam reforming of a hydrocarbon feedstock

    DE102015004121A1

  • Furnace with electrically heatable and fuel heatable reactor tubes for hydrocarbon steam reforming

    EP3075704A1

  • JP1002143560A

  • JP1972-050984B

  • JP1975100006A