EA041025B1 - RESISTANCE HEATED STEAM REFORMING - Google Patents

Description

Field of invention

Embodiments of the invention relate to a reactor system and process for steam reforming of a feed gas containing hydrocarbons in which heat for the endothermic reaction is provided by resistance heating.

State of the art

In steam reforming reactions, there is often a problem with the efficiency of heat transfer to the reaction zone of the catalyst bed within the reactor unit. Conventional heat transfer by convective or conductive heat transfer and/or radiative heating may not be fast enough, and often in many configurations, the application of such heat transfer methods will be associated with significant difficulties. This problem can be illustrated by the example of a tubular reformer in a steam reformer, which can practically be considered as a large heat exchanger, with heat transfer limiting the speed of the reformer. The temperature in the most central part of the tubular reformer tubes is somewhat lower than the temperature outside the tubes due to the rate of heat transfer through the tube walls and the catalyst inside the tubes, and also due to the endothermic nature of the steam reforming reaction.

One way to supply heat inside the catalyst, rather than outside the tubes containing the catalyst, is resistance heating. DE 102013226126 describes an allothermic methane reforming process with physical energy recovery, in which methane is reformed using carbon dioxide to produce a synthesis gas consisting of carbon monoxide and hydrogen. The feed gases CH ₄ and CO ₂ are fed into a fixed bed reactor consisting of electrically conductive and catalytic particles, which is electrically heated to a temperature of about 1000 K. In the fixed bed reactor, the reaction gases are converted and heat is released from the generated synthesis gas.

The aim of the invention is to provide an alternative configuration of the electrically heated steam reforming reactor system.

It is also an object of the invention to provide a reactor system with a built-in heat source and catalysts.

Another object of the invention is to provide a reactor system and process for producing synthesis gas by steam reforming, in which the overall energy consumption is reduced compared to an externally heated reactor system, such as a side or top fired methane steam reformer (SMR), which is standard for industrial steam reforming. By means of electrical heating, the generation of high temperature combustion gases as in the case of externally heated SMRs can be avoided, so that the electrically heated reforming section of the reactor consumes less power.

Yet another object of the invention is to provide a reactor system and a process for the production of synthesis gas by steam reforming, in which the amount of catalyst and the size of the reactor system are reduced compared to SMR. In addition, the invention makes it possible to optimize the reactor according to requirements and thus reduce the amount of catalytically active material while controlling the front of the reforming reaction.

Furthermore, it is an object of the invention to provide a reactor system and process for the production of synthesis gas by steam reforming, in which the amount of synthesis gas produced in a reactor with a single pressure vessel is significantly increased compared to known tubular steam reformers.

Furthermore, it is an object of the invention to provide a method for producing synthesis gas using a steam reforming system, in which the synthesis gas leaving the steam reforming system has a relatively high temperature and a relatively high pressure. In particular, it is desirable that the temperature of the synthesis gas leaving the steam reforming system is about 900-1100°C, or even reaches 1300°C, and the pressure of the synthesis gas leaving the steam reforming system is in the range of about 30-100 bar. The invention will provide the possibility of precise control of the temperature of the synthesis gas at the outlet of the steam reforming system.

The advantage of the invention is that the overall emission of carbon dioxide and other climate-damaging substances can be significantly reduced, in particular if the energy used in the reactor system comes from renewable energy sources.

Brief summary of the invention

Embodiments of the invention generally relate to a reactor system for steam reforming of a feed gas containing hydrocarbons, wherein the reactor system comprises a structured catalyst designed to catalyze the steam reforming of said feed gas containing hydrocarbons, wherein said structured catalyst comprises a macroscopic structure of an electrically conductive material, at the same time, a ceramic coating is located on said macroscopic structure, while said ceramic coating acts as a substrate of a catalytically active material, and the high-pressure housing contains an inlet for supplying the source gas and an outlet for removing the gaseous product, while the inlet located so that the source gas is fed into the front of the structured catalyst, and the gaseous product exits from the back of the structured catalyst;

a pressure vessel containing the structured catalyst;

a heat-insulating layer between the structured catalyst and the pressure vessel;

at least two conductors electrically connected to the structured catalyst and to a power source that is located outside the pressure vessel, and the power source is designed to heat at least a portion of the structured catalyst to a temperature of at least 500°C by passing an electric current through structured catalyst, wherein at least two conductors are connected to the structured catalyst at a point on the structured catalyst located closer to the front of the structured catalyst than to the back of the structured catalyst, wherein the structured catalyst is configured to direct electric current from one conductor to substantially back of the structured catalyst and back to the second conductor of at least two conductors.

In accordance with the topology of the reactor system, the compressed source gas is fed into it through the inlet and directed to the pressure vessel of the reactor system. The pressure vessel has an internal configuration of thermal insulation layers and inert material such that the source gas is directed through the channels of the structured catalyst where it will contact the ceramic coating and the catalytically active material which is located on the ceramic coating substrate, while the catalytically active material will catalyze the reaction steam reforming. In addition, heating the structured catalyst provides the necessary heat for the endothermic reaction. The gaseous product from the structured catalyst is directed to the outlet from the reactor system.

The term structured catalyst front means that part of the structured catalyst where feed gas is supplied to the structured catalyst, and the term structured catalyst back means that part of the structured catalyst where gas exits from the structured catalyst. In addition, it should be understood that the expression at least two conductors connected to the structured catalyst at a point on the structured catalyst located closer to the front of the structured catalyst than to the back of the structured catalyst means that both conductors / all conductors are connected closer to to the front of the structured catalyst than to the back. At least two conductors are preferably connected to the front of the structured catalyst or within a quarter of the length of the macroscopic structure closest to the front.

Due to the close proximity between the catalytically active material and the macroscopic structures, efficient heating of the catalytically active material is possible by thermal conduction of the solid material away from the resistance-heated macroscopic structure. An important feature of the resistance heating process is that the heat is generated within the object itself, rather than being heated by an external heat source through convective or conductive heat transfer and/or radiative heating. In addition, the hottest part of the reactor system will be inside the reactor pressure vessel. Preferably, the power supply and the structured catalyst are sized such that at least a portion of the structured catalyst reaches a temperature of 850°C, preferably 900°C, more preferably 1000°C, or even more preferably 1100°C. The amount and composition of the catalytically active material can be adapted to the steam reforming reaction under given operating conditions. The surface area of the macroscopic structure, the portion of the macroscopic structure coated with the ceramic coating, the type and structure of the ceramic coating, and the amount and composition of the catalytic material can be adapted to the steam reforming reaction under given operating conditions. However, it should be noted that advantageously substantially the entire surface of the macroscopic structure has a ceramic coating, and preferably all or most of the ceramic coating acts as a substrate for the catalytically active material. Preferably, only those portions of the macroscopic coating that are connected to the conductors are free of the ceramic coating. The ceramic coating acting as a substrate for the catalytically active material reduces or prevents carbon deposits according to the reaction

Due to the ceramic coating of the metal structure serving as the substrate of the catalytically active material, the metal phase of the macroscopic structure is coated with a coherent oxide layer, which has less potential for carbon formation reactions. In addition, the catalytically active material of the oxide phase will catalyze the steam reforming reactions and

- 2 041025 bring the reacting gas to thermodynamic equilibrium. This increases the hydrogen partial pressure and lowers the methane partial pressure, thereby reducing or in many cases eliminating the thermodynamic potential for carbon formation according to reaction (A) above.

When the pressure vessel comprises an inlet for supplying a source gas and an outlet for withdrawing a gaseous product, the inlet is positioned such that the source gas is supplied to the front of the structured catalyst and the gaseous product exits from the back of the structured catalyst, and when at least two conductors are connected to the structured catalyst at a point on the structured catalyst located closer to the front of the structured catalyst than to the back of the structured catalyst, at least two conductors can be placed in a relatively colder part of the reactor system. The front of the structured catalyst has a lower temperature than the back of the structured catalyst due to the following factors:

the feed gas supplied through the inlet may cool at least two conductors before being heated by the structured catalyst downstream of the gas through the structured catalyst;

the feed gas at the front of the structured catalyst will have a lower temperature than the product gas leaving the back of the structured catalyst due to the heat provided by the electrical heating of the structured catalyst;

the steam reforming reaction is endothermic, therefore, during such a reaction, heat is absorbed;

the structured catalyst is configured to direct electrical current from one conductor substantially to the back of the structured catalyst and back to a second conductor of at least two conductors.

Therefore, the temperature profile in the structured catalyst will correspond to a substantially continuously increasing temperature along the feed gas path through the structured catalyst. This corresponds to a significant increase in the degree of conversion of methane in the source gas into hydrogen and carbon monoxide.

Thus, current is directed into and out of the macroscopic structure through conductors located in its relatively cold front. It is advantageous that the temperature of all electrically conductive elements except the macroscopic structure is kept low in order to protect the connections between the conductors and the structured catalyst. If the conductors and other electrically conductive members other than the macroscopic structure are kept at a relatively low temperature, this allows a wider range of materials to be used for the conductors and other electrically conductive members other than the macroscopic structure. As the temperature of the electrically conductive elements increases, their resistivity also increases, hence it is desirable to avoid unnecessary heating of all other parts except the macroscopic structure within the reactor system.

In addition, the combination of thermal insulation and connection of conductors to the front, colder part of the macroscopic structure allows the pressure in the pressure vessel to be increased to more than 5 bar.

It should be noted that the term electrically conductive elements, except for the macroscopic structure, contains the corresponding electrically conductive elements that are intended to connect a power source to a structured catalyst and for potential connections between macroscopic structures or structured catalysts.

A combination of a profile of substantially continuously increasing temperatures in the structured catalyst along the feed gas path through the structured catalyst, controlled heat flow from the structured catalyst, and control of the chemical reaction front can be provided.

As used throughout this document, the term macroscopic structure means that the structure is large enough to be visible to the naked eye without magnifying devices. As a rule, the macroscopic structure has dimensions ranging from tens of centimeters or up to several meters. The macroscopic structure is preferably sized to match, at least in part, the internal dimensions of the pressure vessel housing the structured catalyst, thereby saving space for the thermal insulation layer and conductors. Two or more macroscopic structures can be connected, resulting in a set of macroscopic structures, at least one of the external dimensions of which is in the meter range, for example, at least one size of such a set of macroscopic structures can be 0.5, 1, 2 or 5 m. Such two or more macroscopic structures may be referred to as a set of macroscopic structures. In this case, the dimensions of the set of macroscopic structures are preferably made to correspond, at least in part, to the internal dimension of the pressure vessel in which the structured catalyst is placed (saving space for the heat-insulating layer). It is assumed that such

- 3 041025 a set of macroscopic structures can occupy a volume from 0.1 to 10 m ³ or even more volume. The structured catalyst may include one macroscopic structure or a set of macroscopic structures, wherein a ceramic coating is located on the macroscopic structures, while the specified ceramic coating acts as a substrate of the catalytically active material. If the structured catalyst contains a set of macroscopic structures, such macroscopic structures can be electrically connected to each other. However, as an alternative, the macroscopic structures may not be electrically connected to each other. Thus, a structured catalyst may include two or more macroscopic structures located next to each other. Macroscopic structures can be made by extrusion and sintering. Alternatively, macroscopic structures can be produced by 3D printing and sintering.

The macroscopic structures may have any suitable physical dimensions, thus the height may be less than the width of the macroscopic structure, or vice versa.

A ceramic coating is disposed on said macroscopic structure, said ceramic coating acting as a support for the catalytically active material. The term macroscopic structure having a ceramic coating means that at least part of the surface of the macroscopic structure is coated with a ceramic material. Thus, this term does not mean that the entire surface of the macroscopic structure is covered with a ceramic material; in particular, at least those parts of the macroscopic structure that are electrically connected to the conductors do not have a ceramic coating. The coating is a ceramic material with pores in the structure, which allows the application of the catalytically active material on and within the coating. Advantageously, the catalytically active material contains catalytically active particles having a size in the range of approximately 5-250 nm.

The macroscopic structure is preferably made by extruding a mixture of powdered metal particles and a binder into an extruded structure and then sintering the extruded structure, resulting in a material with a high geometric surface area to volume ratio. Alternatively, the macroscopic structure is made using 3D printing technology. Preferably, an extruded or 3D printed structure is sintered in a reducing atmosphere to obtain a macroscopic structure. A ceramic coating, which may contain a catalytically active material, is applied to the macroscopic structure prior to the second sintering in an oxidizing atmosphere to form chemical bonds between the ceramic coating and the macroscopic structure. Alternatively, the catalytically active material may be impregnated onto the ceramic coating after the second sintering. When chemical bonds are formed between the ceramic coating and the macroscopic structure, a particularly high thermal conductivity is possible between the electrically heated macroscopic structure and the catalytically active material which is located on the ceramic coating, which ensures close and almost direct contact between the heat source and the catalytically active material of the structured catalyst. Due to the close proximity between the heat source and the catalytically active material, heat transfer is efficient, so that heating of the structured catalyst can be carried out with high efficiency. Thus, an optimum gas treatment per unit volume of the reactor system can be achieved, so the reactor system containing the structured catalyst can be compact.

When used in the text of this document, the terms 3D printing technology and 3D printing mean production technology using a metal additive. Such metal-additive manufacturing techniques include 3D printing processes, in which, under automated control, a material is combined into a specific structure to obtain a three-dimensional object, in which the structure is cured, for example, by sintering, to obtain a macroscopic structure. In addition, such metal additive manufacturing technologies include 3D printing processes that do not require subsequent sintering, such as preformed layer melting technology or layer-by-layer electron beam melting technology. Examples of such preformed layer melting or layered electron beam melting technologies are 3D printing processes using a laser beam, electron beam, or plasma printing.

The reactor system according to the invention does not require an oven and this greatly reduces the overall size of the reactor. In addition, it is an advantage that the amount of synthesis gas produced in the single pressure vessel reactor is significantly increased compared to prior art tubular steam reformers. In a standard tubular steam reforming reactor, the amount of synthesis gas produced in one reactor tube is as high as 500 Nm ³ /h. For comparison, with the reactor system according to the invention, productivity up to 2000 Nm ³ /h or more can be achieved, for example up to 10000 Nm ³ /h or more, in a single pressure vessel. In this case, O ² may not be present in the source gas, and less than 10% in the resulting synthesis gas

- 4 041025 methane. When a single pressure vessel accommodates a catalyst capable of producing up to 10,000 Nm ³ /h of synthesis gas, there is no longer a need for multiple pressure vessels or arrangements for distributing feed gas into several such separate pressure vessels.

Another advantage of this reactor system is that within the reactor system, the flow through the structured catalyst can be directed upwards due to the fact that the structured catalyst has a macroscopic structure. Alternatively, the flow through the structured catalyst may be directed horizontally or in any other suitable direction. This is more problematic if the reactor contains granules due to the risk of fluidized bed formation, crushing and blowing of the granules. Thus, it is possible not to use a large number of pipes, which reduces installation costs. In addition, in the case of upward or horizontal flow, the flexibility of the installation configuration is increased.

Preferably the macroscopic structure contains Fe, Cr, Al or an alloy thereof. Such an alloy may contain additional elements such as Si, Mn, Y, Zr, C, Co, or combinations thereof. The catalytically active material may contain, for example, nickel, ruthenium, rhodium, iridium, platinum, cobalt, or a combination thereof. Thus, it is possible that the catalytically active material is a combination of nickel and rhodium and another combination of nickel and iridium. The ceramic coating may be, for example, an oxide containing Al, Zr, Mg, Ce and/or Ca. The coating may be, for example, calcium aluminate or magnesium aluminum spinel. Such a ceramic coating may contain additional elements such as La, Y, Ti, K, or combinations thereof. Preferably, the conductors and macroscopic structure are made of different materials. The conductors may be made of, for example, iron, nickel, aluminium, copper, silver or an alloy thereof. The ceramic coating is an electrically insulating material and typically has a thickness in the range of about 100 microns, such as about 10-500 microns.

The macroscopic structure is preferably a cohesive or intrinsically solid material in order to provide electrical conductivity throughout the macroscopic structure and therefore to provide thermal conductivity throughout the structured catalyst, in particular to heat the catalytically active material located on the macroscopic structure. With the help of a cohesive or internally solid material, it is possible to ensure a uniform distribution of current in the macroscopic structure and thus a uniform distribution of heat within the structured catalyst. For the purposes of this document, the term connected is synonymous with connected; thus, cohesive refers to a material that is internally solid or cohesive. Because the structured catalyst is a cohesive or intrinsically solid material, control is provided over the electrical connectivity within the structured catalyst material and thus conduction of the macroscopic structure is ensured. It should be noted that even if further modifications to the macroscopic structure are made, such as slits within portions of the macroscopic structure or incorporation of an insulating material into the macroscopic structure, the macroscopic structure is still a coherent or internally integral material.

As shown in the figures, the gas flow through the structured catalyst is in the same direction as the length or z-axis of the structured catalyst, or the gas flow is coaxial with the length or z-axis of the structured catalyst. While the z-axis of the structured catalyst is vertical in the figures, it should be noted that the reactor may be positioned in any appropriate manner such that the structured catalyst and the gas flow through it may be in a horizontal or opposite direction to that shown in the figures, or may be directed at an angle, for example 45°, to the horizontal.

In the context of the invention, the term hydrocarbon gas means a gas containing one or more hydrocarbons and possibly other components. Thus, as a rule, hydrocarbon gas contains CH4 and in some cases also higher hydrocarbons in relatively small amounts in addition to small amounts of other gases. Higher hydrocarbons are components with two or more carbon atoms, such as ethane and propane. Examples of hydrocarbon gas can be natural gas, domestic gas, gasoline fraction or a mixture of methane and higher hydrocarbons. Hydrocarbons can also be components with atoms other than carbon and hydrogen, such as oxygenates. The term hydrocarbon containing feed gas means a feed gas containing a hydrocarbon gas with one or more hydrocarbons mixed with steam, hydrogen and possibly other components such as carbon monoxide, carbon dioxide, and possibly also some nitrogen and argon. As a rule, the source gas supplied to the reactor system has a certain ratio of hydrocarbon gas, steam and hydrogen, and possibly also carbon dioxide.

- 5 041025

In addition, the term steam reforming means a reforming reaction according to one or more of the following equations:

CH ₄ + H ₂ O θ CO + ZN ₂ (i)

CH ₄ + 2H ₂ O θ CO ₂ + 4H ₂ (th)

CH ₄ + CO ₂ θ 2CO + 2H ₂ (iii)

Reactions (i) and (ii) are steam methane reforming reactions, while reaction (iii) is a dry methane reforming reaction.

For higher hydrocarbons, i.e. for CnH _m , where n>2, m>4, equation (i) has the following general form:

СцНшch + η Н ₂ О θ nCO + (n + m/2)H ₂ (iv), where n>2 and m>4.

Steam reforming is usually accompanied by the following water gas shift reaction (v): CO + H ₂ O θ CO ₂ + H ₂ (v)

The term methane steam reforming includes reactions (i) and (ii), the term steam reforming includes reactions (i), (ii) and (iv), while the term methanation includes the reverse reaction of reaction (i). In most cases, at the outlet of the reactor system, all these reactions (i)-(v) have reached equilibrium or are close to it.

The term pre-reforming is often used to refer to the catalytic conversion of higher hydrocarbons according to reaction (iv). Pre-reforming is typically accompanied by steam reforming and/or methanation (depending on gas composition and operating conditions) and a water gas shift reaction. Pre-reforming is often carried out in adiabatic reactors, but may also take place in heated reactors.

The steam reforming reaction proceeds with the absorption of a large amount of heat. To achieve a satisfactory degree of methane conversion in the feed gas, high temperatures are required, typically temperatures in excess of 800-850°C. The SMR consists of several tubes filled with catalyst grains inside a furnace. The length of the pipes, as a rule, is 10-13 m, the inner diameter is 80-160 mm. The burners placed in the furnace provide the necessary heat for the reactions by burning the fuel gas. The maximum average heat flow is often 80000-90000 kcal/h/m ² of the inner surface of the pipe. The overall limitation of the heat flow is due to mechanical factors, so the power is increased by increasing the number of pipes and the size of the furnace. Detailed information about the reactor system type SMR known from the literature, for example from the work Production of synthesis gas for Fischer-Tropsch synthesis (Synthesis gas production for FT synthesis); section 4, p. 258-352, 2004. As used throughout this document, the abbreviation SMR refers to the above-described tubular methane steam reforming reactor with external heating.

Typically, the feed gas is desulfurized before entering the reactor system to prevent deactivation of the catalysts in the process.

If necessary, as an initial stage of the process, which is usually carried out after the desulfurization stage, the hydrocarbon gas, together with steam and possibly also with hydrogen and/or other components such as carbon dioxide, will also be pre-reformed in accordance with the reaction (iv) in a temperature range of approximately 350-550°C for the conversion of higher hydrocarbons. This eliminates the risk of carbon formation from higher hydrocarbons on the catalyst in subsequent process steps. Optionally, carbon dioxide or other components may also be mixed with the gas leaving the pre-reformer to form a feed gas.

Typically, the feed gas entering the reactor system is preheated. However, due to the heat flux from the structured catalyst, the feed gas entering the reactor system may be relatively cold. Thus, it may be sufficient to preheat the source gas to a temperature of from about 200°C to about 450°C.

The term electrically conductive means materials with electrical resistivity in the range of 10 ^-5 to 10 ^-8 Ω-m at 20°C. Thus, electrically conductive materials are, for example, metals such as copper, silver, aluminium, chromium, iron, nickel or metal alloys. In addition, the term electrically insulating means materials with electrical resistivity above 10 Ω-m at 20°C, for example, in the range of 109-10 ²⁵ Ω-m at 20°C.

If the reactor system comprises a thermal insulation layer between the structured catalyst and the pressure vessel, the necessary thermal or electrical insulation is provided between the structured catalyst and the pressure vessel. The presence of a heat-insulating layer between the structured catalyst and the pressure vessel helps to avoid excessive heating of the pressure vessel and helps to reduce thermal loss to the environment. Temperatures in the structured catalyst, at least in some of its parts, can reach approximately 1300 ° C, however, with the help of a heat-insulating layer between the structured

- 6 041025 catalyst and pressure vessel can maintain a lower temperature of the pressure vessel, for example 500 or even 200°C, which is an advantage because typical structural steel materials usually cannot be used under load at temperatures above 1000°C. In addition, the heat insulating layer between the pressure vessel and the structured catalyst helps control the electrical current in the reactor system, since the heat insulating layer is also electrically insulating. The thermal barrier layer may be one or more layers of hard material such as ceramic, inert material, refractory material, gas barrier, or a combination thereof. Thus, it is also possible for a part of the heat-insulating layer to constitute or form a purge gas or a gas inside the catalyst.

In addition, it should be noted that the term thermal insulation material means materials with a thermal conductivity of approximately 10 W(m'-K'1) or lower. Examples of thermal insulation materials are ceramics, refractory materials, alumina materials, zirconia materials, and the like.

Any appropriate gaps between the structured catalyst, thermal insulation layer, pressure vessel and/or any other components within the reactor system are preferably filled with inert material, for example in the form of grains of inert material. Such gaps can be, for example, the gap between the underside of the structured catalyst and the bottom of the pressure vessel and the gap between the sides of the structured catalyst and the insulating layer covering the inner sides of the pressure vessel. The inert material may be, for example, a ceramic material in the form of grains or tiles. The inert material helps control the distribution of gas in the reactor system and control the flow of gas through the structured catalyst. In addition, the inert material generally has a heat-insulating effect.

In one of the embodiments of the invention, the design pressure of the pressure vessel is in the range of 5-30 bar. For a small scale configuration, the design pressure of the pressure vessel can be in the range of 5-15 bar. Since the hottest part of the reactor system is the structured catalyst, around which there will be an insulating layer inside the pressure vessel of the reactor system, the temperature of the pressure vessel will be maintained at a level significantly lower than the maximum operating temperature. This makes it possible to have a relatively low pressure vessel design temperature, for example 700 or 500° C., preferably 300 or 200° C., at a maximum structured catalyst operating temperature of 900 or even 1100° C. or even up to 1300° C. The strength of the material is higher at the lower of these temperatures (corresponding to the pressure vessel design temperature as above); this means that, unlike an externally heated steam methane reformer such as a top or side heated SMR, the reactor system of the present invention can be designed to operate at (higher) pressure. In SMR, the maximum pipe wall temperature can be up to 1000°C. Another advantage is that, due to the lower design temperature compared to SMR, the thickness of the pressure vessel can be reduced in some cases, reducing costs.

In one embodiment of the invention, the design pressure of the pressure vessel is in the range of 30-200 bar, preferably in the range of 80-180 bar.

The reactor system of the invention may be part of a plant, such as a hydrogen plant. Such a plant may advantageously include one or more compressors and/or pumps downstream of the reactor system of the invention. The compressors/pumps are designed to compress the feed gas to a pressure of 30-200 bar before being fed into the reactor system. Feed gas components, in particular steam, hydrogen and hydrocarbon feed gas, can be individually compressed and fed separately to the reactor system of the invention. If the source gas is compressed before being fed into the reactor system according to the invention and the reactor system comprises a pressure vessel having a design pressure of 30-200 bar, the compression step after the reactor system according to the invention can be simplified or eliminated entirely. In a hydrogen plant that is part of a refinery where hydrogen product is used for hydrotreatment, the hydrotreater compressor can be omitted if the product gas pressure is approximately 150-200 bar at the outlet of the reactor system.

In one embodiment, the resistivity of the macroscopic structure is in the range of 10-5-10 ^-7 Ω-m. A material with a resistivity in this range provides efficient heating of the structured catalyst when energy is supplied from a power source. The resistivity of graphite is approximately 10 ^-5 Ω-m at 20°C, the resistivity of kanthal is approximately 10 ^-6 Ω-m at 20°C, the resistivity of stainless steel is approximately 10 ^-7 Ω-m at 20°C. Kanthal is a brand name for the iron-chromium aluminum (FeCrAl) family of alloys. The macroscopic structure may, for example, be made of FeCrAlloy having a resistivity of approximately 1.5-10 ^-6 Ω-m at 20°C.

It should be noted that the system of the invention may include any suitable number of power supplies and any suitable number of conductors connecting the power supplies and macroscopic structures of the structured catalyst.

According to one embodiment of the reactor system, each of the at least two conductors passes through the pressure vessel in a fitting such that the at least two conductors are electrically isolated from the pressure vessel. The fitting may be partly made of plastic and/or ceramic material. The term fitting means a device that allows the mechanical connection of two pieces of equipment that are in such a configuration under load. With its use, the pressure inside the pressure vessel can be maintained, even if at least two conductors pass through it. Non-limiting examples of fittings include electrical insulating fittings, dielectric fittings, power compression seals, compression fittings, or flanges. The pressure vessel typically includes side walls, end walls, flanges, and possibly other elements. The term pressure vessel can refer to any of these components.

The fittings are connected to the front of the macroscopic structure. For example, the fittings are located downstream of the front of the macroscopic structure (relative to the direction of the feed gas). Thus, the temperature of the fittings themselves will be relatively low. With the combination of a thermal insulation layer and fittings in the relatively cold part of the pressure vessel, a pressure in the pressure vessel of more than 5 bar can be achieved, despite the fact that the fittings pass through the wall of the pressure vessel and that the maximum temperature of the structured catalyst can reach about 950°C. If the fittings are heated to high temperatures, there is a risk of mechanical defects, such as deformation, and gas leakage from the pressure housing is likely. In addition, an electrical connection between at least two conductors and the pressure vessel must be avoided. To do this, it is important to avoid excessive heating of the fittings. For example, the fitting may contain a polymer as well as a compression fitting.

In one embodiment, the pressure housing also has one or more inlets adjacent to or in combination with at least one fitting to allow refrigerant gas to pass through, around, adjacent to, or within at least one conductor within said housing. high pressure. In this way, cooling of the conductors is ensured and the heating temperature of the fitting is kept low. If no cooling gas is used, the conductors may be heated by the feed gas supplied to the reactor system, resistive heating of the conductor due to current injection and/or heat transfer from the structured catalyst. The cooling gas may, for example, be hydrogen, nitrogen, steam, carbon dioxide or mixtures thereof. The temperature of the cooling gas at the supply to the pressure vessel may be, for example, approximately 100, or 200, or 250°C. In one embodiment, the conductors are hollow to allow cooling gas to pass through the conductors and cool them from the inside. By maintaining a low fitting temperature, for example, around 100-200°C, it is easier to achieve a tight configuration. In one embodiment, a portion of the feed gas, such as carbon dioxide and/or steam, is fed into the pressure vessel as cooling gas. In yet another embodiment, a portion of the feed gas or a gas of the same composition as the feed gas is used as the cooling gas.

In one of the embodiments, the reactor system further comprises an inner tube, wherein heat exchange takes place between it and the structured catalyst, wherein the inner tube is adapted to remove the gaseous product from the structured catalyst in such a way that between the gaseous product entering through the inner pipe or pipes, heat exchange with the gas entering through the structured catalyst, however, the inner tube is electrically isolated from the structured catalyst. This configuration is referred to herein as a bayonet reactor system. In this configuration, the product gas in the inner tube contributes to the heating of the process gas entering through the structured catalyst. Electrical isolation between the inner tube and the structured catalyst may be provided by gas in the gap between the inner tube and the structured catalyst, or by an inert material located around the inner tube and the structured catalyst. The gas may flow through the structured catalyst in an upward or downward direction. While the electrical insulation between the inner tube and the structured catalyst also provides thermal insulation, this thermal insulation effect is never complete and some heat transfer will occur through the electrical insulation layer.

In one of the embodiments of the invention, the connection between the structured catalyst and these at least two conductors is a mechanical connection, a welded joint, a solder joint, or a combination thereof. The structured catalyst may include terminals physically and electrically connected to the structured catalyst to provide a more efficient electrical connection between the macroscopic structure of the structured catalyst and the at least two conductors. The term mechanical connection means a connection in which two components are held together mechanically, such as by a threaded connection or clamp, so that current can flow between the components.

In one of the embodiments of the invention, the macroscopic structures in the set of macroscopic structures can be electrically connected to each other. The connection between two or more macroscopic structures can be achieved by mechanical connection, clamping, soldering, welding, or any combination of these connection methods. Each macroscopic structure may include contact leads to provide a more efficient electrical connection. Two or more macroscopic structures can be connected to the power supply in series or in parallel. The electrical connection between two or more macroscopic structures is preferably coherent and uniform along the interface between the two or more macroscopic structures, such that the two or more macroscopic structures act as a single cohesive or intrinsically solid material, thereby ensuring uniform electrical conductivity of the two or more macroscopic structures. Alternatively, or additionally, the structured catalyst may include a set of macroscopic structures that are not electrically connected to each other. Instead, two or more macroscopic structures are placed together inside the pressure vessel, but are not electrically connected to each other. Thus, in this case, the structured catalyst contains macroscopic structures connected in parallel to the power source.

A ceramic coating with or without a catalytically active material can be applied directly to a metal surface by a pickle primer. The mordant primer is a known technology and is described in e.g. Cybulski, A., Moulijn, J.A., Structured Catalysts and Reactors, Marcel Dekker, Inc., New York, 1998, chapter 3, ref. materials in this document. A ceramic coating may be applied to the surface of the macroscopic structure and then the catalytically active material may be added. Alternatively, a ceramic coating containing a catalytically active material is applied to the macroscopic structure.

As a result of extrusion and sintering or 3D printing and sintering, a homogeneous macroscopic structure of a cohesive shape is obtained, which can subsequently be applied with a ceramic coating.

The sintering of the macroscopic structure and the ceramic coating may be carried out in an oxidizing atmosphere to form chemical bonds between the ceramic coating and the macroscopic structure. This provides a particularly high thermal conductivity between the macroscopic structure and the catalytically active material, which is located on the ceramic coating substrate. Thus, the structured catalyst is optimized in terms of heat transfer to the active catalytic site, and also the reactor system in which the structured catalyst is located can be optimized and limited mainly by the chemical reaction rate. Heat transfer from outside the pressure vessel to the structured catalyst is not carried out, as in the case of known SMRs, where heat transfer occurs through the walls of the pipes to the catalyst inside the pipes.

In one of the embodiments of the invention, the structured catalyst has at least one electrically insulating part, with which the length of the current path between the conductors increases and becomes greater than the length of the structured catalyst in the longest dimension. A current path between the conductors greater than the largest dimension of the structured catalyst can be provided by placing an electrically insulating part(s) between the conductors when no current passes through some part of the structured catalyst. Such electrically insulating parts are intended to increase the current path and thus increase the resistance in the structured catalyst. Thus, the current path through the structured catalyst can be, for example, more than 50%, 100%, 200%, 1000% or 10000% longer than the largest dimension of the structured catalyst.

In addition, such electrically insulating parts are designed to direct current from one conductor, which is located closer to the front of the structured catalyst than to the back of the structured catalyst, to the back of the structured catalyst, and back to the second conductor, located closer to the front of the structured catalyst than towards the back. Preferably, the current flows from the front of the end of the structured catalyst to the back and back to the front. As shown in the figures, the front of the structured catalyst is its top. The arrow marked z in FIG. 5-7 indicates the z-axis along the length of the structured catalyst. The main current path through the structured catalyst will have a positive or negative z-coordinate value of the corresponding current density vector over most of the current path. The main current path means the path of electrons through the macroscopic structure of the structured catalyst with the highest current density. The main current path can also be understood as the path having the minimum length through the macroscopic

- 9 041025 the structure of the structured catalyst. From a geometric point of view, the main current path can be quantified as the largest current density vector in a plane perpendicular to the direction of gas flow in a connected section of a macroscopic structure. At the bottom of the structured catalyst, as shown in the figures, the current will change direction, and here the z-coordinate of the corresponding current density vector will be zero.

As used throughout this document, the term bonded section means a cross section of a macroscopic structure where all walls of the bonded section are geometrically connected to one or more other walls of the bonded section in the same plane.

In one embodiment of the invention, the structured catalyst has at least one electrically insulating portion configured to direct current through said structured catalyst to provide a non-zero value of the current density vector component of the main current path for at least 70% of the length of said structured catalyst parallel to the length of said structured catalyst. catalyst. Thus, for at least 70% of the length of said structured catalyst, the current density vector will have a positive or negative component value parallel to the length of said structured catalyst. Thus, for at least 70%, for example 90% or 95% of the length of the structured catalyst, i.e. along the z-axis of the structured catalyst shown in FIG. 5-10, the current density vector of the main current path will have a positive or negative value of the z component of the structured catalyst. This means that the current is directed from the front of the structured catalyst to the back of it and then back to the front. Heat from the structured catalyst is absorbed during heating of the gas entering the front of the structured catalyst and during the endothermic steam reforming reaction over the structured catalyst. Therefore, the front of the structured catalyst remains cooler than the back, and provided that the current density vector of the main current path has a non-zero component value, parallel to the length of said structured catalyst, this provides a profile of substantially constantly increasing temperatures, which in turn provides controlled reaction front. In one embodiment, the current density vector has a non-zero component value parallel to the length of said structured catalyst for 70% of the length of said structured catalyst, preferably 80%, more preferably 90%, even more preferably 95% of the length of said structured catalyst. It should be noted that the term structured catalyst length refers to the dimension of the structured catalyst in the direction of the gas flow. For the structured catalysts shown in the figures, the length corresponds to the longitudinal direction, i. length is the largest measurement of a catalyst. In some figures, this direction is indicated by an arrow labeled z.

As non-limiting examples of insulating parts, slots, slots or openings in the structure can be cited. If necessary, a solid insulating material such as ceramic can be used in the slots in the structure. In the case where the solid insulating material is a porous ceramic material, the catalytically active material may advantageously be introduced into the pores, for example by impregnation. A solid insulating material within the slot helps isolate the portions of the structured catalyst on the sides of the slot from each other. When used in the text of the present invention, the term the largest dimension of the structured catalyst means the largest internal dimension of the geometric shape occupied by the structured catalyst. If the structured catalyst is box-shaped, the largest dimension will be the diagonal from one corner to the farthest corner, also referred to as the space diagonal.

It should be noted that even though due to the electrically insulating parts provided to increase the current path, the current can pass through the structured catalyst with a change of direction, the gas passing through the reactor system enters one part of the reactor system and passes through the structured catalyst once before how to get out of the reactor system. In appropriate gaps between the structured catalyst and the rest of the reactor system, an inert material is preferably present so that, within the reactor system, the gas passes through the structured catalyst and the catalytically active material.

In one embodiment, the length of the gas passage through the structured catalyst is less than the length of the current path from one conductor through the structured catalyst to the next conductor. The ratio of the length of the gas channel to the length of the current path can be less than 0.6 or 0.3, 0.1 or even 0.002.

In one embodiment, the structured catalyst has at least one electrically insulating portion by which current is directed through the structured catalyst in a zigzag path. In this document, the term zigzag path means a path from one conductor to another, the direction of which changes at different angles. A zigzag path is, for example, a path that goes up, turns, and then goes down. zigzag path

- 10 041025 can have many turns, it can go up and then down many times while passing through the structured catalyst, even if one turn is enough to make the path zigzag.

It should be noted that insulating parts designed to increase the current path are not necessarily associated with a ceramic coating on the macroscopic structure, although this ceramic coating is also considered electrically insulating, it does not change the length of the current path between conductors connected to the macroscopic structure.

In one embodiment of the invention, the macroscopic structure has a plurality of parallel or nearly parallel channels, a plurality of non-parallel channels, and/or a plurality of reversing channels, wherein the channels are limited by walls. Thus, several different forms of macroscopic structure can be used as long as the surface area of the structured catalyst exposed to the gas is maximized. In a preferred embodiment, the macroscopic structure has parallel channels, since such parallel channels provide a very small pressure drop in the structured catalyst. In a preferred embodiment, the parallel longitudinal channels are arranged at an angle with respect to the longitudinal axis of the macroscopic structure. Thus, gas molecules entering through the macroscopic structure will hit the walls inside the channels rather than simply flowing straight through the channel without making contact with the wall. The size of the channels must be such as to provide sufficient resistance to the macroscopic structure. For example, the channels may be square (in a cross section perpendicular to the channels) with a side length of 1-3 mm, however, channels with a maximum cross-sectional extent of up to about 4 cm are also possible. large electrical resistance, and large enough to provide sufficient mechanical strength. The wall thickness may, for example, be 0.2-2 mm, eg approximately 0.5 mm, and the thickness of the ceramic coating located on the walls, 10-500 µm, eg 50-200 µm, eg 100 µm. In another embodiment, the macroscopic structure of the structured catalyst has transverse corrugation.

In general, when the macroscopic structure has parallel channels, the pressure drop from the inlet to the outlet of the reactor system can be significantly reduced compared to a reactor in which the catalyst material is in the form of grains, such as a standard SMR.

In one of the embodiments of the invention, the reactor system further comprises a layer of the second catalytic material in the course of the process before the structured catalyst inside the pressure vessel. In this document, the term upstream means upstream in the direction of flow of the source gas. Thus, as used herein, the term downstream means that the feed gas is passed through the bed of the second catalyst material prior to being fed into the structured catalyst. This provides a situation where such a second catalyst material can be used to pre-reform the feed gas (according to reaction (iv) above) so that the reactor system is pre-reformed and steam reformed within the same pressure vessel. This may also provide a situation where the hydrocarbons in the feed gas react with steam and/or CO ₂ over the second catalyst material (for example, in accordance with reactions (i)-(v) above) and when the process gas supplied to the structured catalyst , has a lower hydrocarbon content than the feed gas for the second catalyst material. The second catalyst may alternatively alternatively or additionally be a catalyst adapted to also capture sulfur compounds in the feed gas. The layer of the second catalytic material does not require special heating, however, indirect heating of the layer of the second catalytic material can be carried out if it is in close proximity to the structured catalyst. Alternatively, indirect heating of the second catalytic material can be carried out.

In one of the embodiments of the invention, the reactor system further comprises a third catalyst material in the form of grains, extrudates or granules of the catalyst, which are loaded into the channels of the structured catalyst. Thus, in this embodiment, the reactor system will have the catalytically active material in the coating of the macroscopic structure and the third catalyst material in the form of grains, extrudates or granules within the channels of the structured catalyst. This makes it possible to increase the catalytic reactivity in the channels or channel segments of the structured catalyst. To clarify the terminology used herein, it should be noted that the term structured catalyst may also refer to the first catalyst material to distinguish it from the second and/or third and/or fourth catalyst material.

The grains, for example, may be of a size that approximates the size of the channels so as to form a single chain of grains stacked on top of each other within the channel of the macroscopic structure. Alternatively, the grains, extrudates or granules may be substantially smaller than the size of the channel to form a compacted layer within each channel. At

- 11 041025 used in the text of the present invention, the term grain means any specific structure having a maximum external size in the range of millimeters or centimeters, while the terms extrudate and granulate define a catalyst material with a maximum external size in a certain range.

In one of the embodiments of the invention inside the pressure vessel after the specified structured catalyst is placed a layer of the fourth catalytic material. Such fourth catalyst material may be in the form of grains, extrudates, or catalyst pellets. This provides a situation where the fourth catalyst material can be used to reduce the near-equilibrium temperature for the gas leaving the structured catalyst by creating a pseudo-adiabatic equilibrium of the steam reforming reaction.

In one embodiment, the second, third, and fourth catalyst materials are catalyst materials suitable for a steam reforming reaction, a pre-reforming reaction, or a water gas shift reaction. Examples of suitable catalysts are Ni/MgAl ₂ O ₄ , Ni/CaAl ₄ O ₄ , Ni/Al ₂ O ₄ and Cu/Zn/Al ₂ O ₃ . In a configuration where the reactor system contains a combination of second, third and fourth catalyst material, the catalyst of each catalyst material may be different.

In one of the embodiments of the invention, the material of the macroscopic structure is selected in such a way that by heating the material with a resistance, a heat flux of 500-50000 kW/m/m ² is created. Preferably, the resistance heating of the material provides a heat flux in the range of 5-12 kW/m ² , for example in the range of 8-10 kW/m ² . Heat flux is defined as the amount of heat per geometric surface area exposed to the gas.

In one of the embodiments of the invention, the geometric surface area of the macroscopic structure is in the range of 100-3000 m ² /m ³ for example 500-1100 m ² /m ³ . The heat flux from the material is preferably chosen according to the reactivity of the catalytically active material.

In one of the embodiments of the invention, the structured catalyst contains a first part configured to create a first heat flux, and a second part configured to create a second heat flux, the first heat flux being less than the second heat flux, the first part being in the process ahead of the second part. In this document, the term first part is downstream before the second part means that the gas supplied to the reactor system reaches the first part before the gas reaches the second part. The first part and the second part of the structured catalyst can be two different macroscopic structures with a ceramic coating on which the catalytically active material is located, while such two different macroscopic structures can be located so as to generate different heat fluxes for given values of electric current and voltage. For example, the front of the structured catalyst may have a larger surface area than the back of the structured catalyst. This can be achieved in that the structured catalyst in the second part may have a smaller cross-sectional area than the cross-sectional area of the catalyst in the first part. Alternatively, the current path through the first part of the structured catalyst may be less curved than the current path through the second part of the structured catalyst, so that the current path through the second part will change direction more times than in the first part of the structured catalyst, resulting in the current generates more heat in the second part of the structured catalyst than in the first part. As mentioned earlier, due to the slits in the macroscopic structure, the current path through the macroscopic structure can be zigzag. It should be noted that the first and second parts of the structured catalyst can be supplied with different current and voltage values in order to be able to provide heat fluxes with different values. However, different heat fluxes in the first and second parts can also be achieved by supplying the same current and voltage through the first and second parts due to the different physical properties of the materials in the first and second parts, as mentioned above.

In one of the embodiments of the invention, the reactor system further comprises a control system configured to control the supply of electricity so that the temperature of the gas leaving the pressure vessel is within a certain range and/or so that the degree of conversion of hydrocarbons in the feed gas is within a certain range. range, and/or to ensure that the molar concentration of methane in the dry state was in a certain range, and/or to approach the equilibrium conditions of the steam reforming reaction in a certain range.

Typically, the maximum gas temperature is 500-1000°C, eg 850-1000°C, eg approximately 950°C, but higher temperatures are possible, eg up to 1300°C. However, the maximum temperature of the gas leaving the reactor system may be as low as 500° C., for example in the case where the reactor system is bayonet. The maximum gas temperature will be reached closer to the lowest part of the structured catalyst with respect to the direction

- 12 041025 source gas flow. However, when using a bayonet-type figure, the maximum temperature of the gas leaving the reactor system may be somewhat lower due to heat exchange with the feed gas; the maximum temperature of the gas leaving the bayonet reactor system according to the invention may be 500-900°C. Power supply control means control of electrical power from a power source. The control of the power supply may, for example, be carried out as a control of the voltage and/or current supplied from the power supply, as a control by switching on/off the power supply, or by a combination of these methods. The structured catalyst may be supplied with alternating or direct current.

The voltage between the at least two conductors may be any value suitable to provide the required heat flow. If the voltage is too low, the heat flow may be insufficient, and if the voltage is too high, the risk of arcing increases. Example voltage values: 50-4000 V, eg 100-1000 V. Such values enable a compact macroscopic structure and thus a reactor system. Through the macroscopic structure between the conductors, a current of any value suitable for the required heat flow with a selected voltage can be supplied. The current value may, for example, be in the range of 100-2000 A, for example in the range of 200-1500 A.

The predetermined temperature range of the gas leaving the pressure vessel/reactor system is preferably 500-1300°C, preferably 800-1150°C, eg 900-1000°C. Preferably, the temperature range for approaching the equilibrium conditions of the methane steam reforming reaction is 1-60°C, more preferably 5-30°C, most preferably 5-20°C.

In order to control the reaction temperature, it is necessary to balance the heat supplied to the reactor system or removed from the reactor system with the heat consumed/produced during the chemical reaction. Heat input/removal must be balanced by the reaction rate and, in particular, by the temperature approaching equilibrium conditions, defined by β, where β is the ratio between the reaction coefficient and the equilibrium constant of the reaction. If the value of β approaches 1, this means that the reaction mixture is close to equilibrium, and values approaching 0 mean that the reaction mixture is far from equilibrium. In general, it is desirable to have as high a reaction rate as possible, which is achieved at low β, provided that the temperature can be controlled in parallel sufficiently to balance the added energy.

In the case of an endothermic methane steam reforming reaction, it is necessary to supply additional heat to continue the reaction, because otherwise the reaction will be balanced, the value of β will approach 1, and the reaction will slow down. However, on the other hand, it is desirable that the temperature increase be consistent with the rate of reaction, since exposing unreacted hydrocarbons to high temperatures can lead to carbon formation. One can effectively monitor this by approaching equilibrium conditions. The temperature approaching the equilibrium conditions of the steam reforming reaction is determined first by calculating the reaction coefficient (Q) for a specific gas:

_with .Uso-Y^ _{2 p2}

Usn ₄ 'un ₂ o

Here y is the mole fraction j of the compound and P is the total pressure in bar. This equation is used to determine the equilibrium temperature (T _eq ) at which a given reaction coefficient is equal to the equilibrium constant:

Q = ^SMR(Teq) where K _SMR is the thermodynamic equilibrium constant of the methane steam reforming reaction. The temperature approaching equilibrium conditions (AT _{equals SMR} ) of the methane steam reforming reaction is determined as follows:

△Trav., SMR ⁼ t - T _e q where T is the mass average temperature of the gas surrounding the catalytic material used, such as a structured catalyst.

To ensure good performance of the steam reforming catalyst, it is desirable that the catalyst is continuously operated in the direction of decreasing ΔT _equal ., _SMR . Historically, large-scale industrial SMRs have had near-equilibrium temperatures of 5-20° C. at the outlet.

The use of the present invention allows the heat flow to be controlled and matched directly to the kinetic characteristics of the structured catalyst, since they are to some extent independent.

In one of the embodiments of the invention in the reactor system, the ratio between the equivalent diameter of the horizontal cross-sectional area of the structured catalyst and the height of the structured is in the range of 0.1-2.0. The equivalent cross-sectional area diameter of a reactor system is defined as the diameter of a circle with an area equivalent to the cross-sectional area. When the ratio between the equivalent area diameter and the height

- 13 041025 structured catalyst is 0.1-2.0, the high pressure vessel in which the structured catalyst is located can be relatively small compared to existing SMRs. Each reactor system can handle more feed gas than is possible in a single pipe in the SMR. In this way, the number of external pipelines leading to the reactor system can be reduced compared to known SMRs, and thus the cost of such pipelines is reduced. Typically, the gas flows through the reactor system in an upward or downward direction, so that the gas flows through channels in the structured catalyst in the height direction of the structured catalyst. When the structured catalyst contains several macroscopic structures or a set of macroscopic structures, individual macroscopic structures within the array may be placed side by side, on top of each other, or there may be a combined arrangement of macroscopic structures. It is emphasized that when a structured catalyst contains more than one macroscopic structure, the dimensions of the structured catalyst are determined by the dimensions of several macroscopic structures. Thus, for example, if a structured catalyst consists of two stacked macroscopic structures, each having a height h, the height of the structured catalyst is 2h.

The volume of the structured catalyst is selected taking into account the desired temperature, including the temperature approaching equilibrium conditions, and/or the desired degree of conversion of hydrocarbons, and/or the dry mole concentration of hydrocarbons in the gaseous product, and/or the temperature outside the reactor system, correlated with the heat release of the macroscopic structure , and/or to ensure the molar concentration of dry hydrocarbons in the gaseous product in a given range and/or to provide a temperature approaching the equilibrium conditions of the methane steam reforming reaction (reaction (i)) in a given range.

In one embodiment of the invention, the height of the reactor system is 0.5-7 m, more preferably 0.5-3 m. The height of the reactor system may be, for example, less than 5 m, preferably less than 2 m, or even 1 m. Dimensions of the reactor system and the structured catalyst within the reactor system are interconnected. Obviously, due to the pressure vessel and thermal insulation layer, the reactor system is somewhat larger than the structured catalyst itself. In comparison, commercial scale SMRs are typically constructed with catalyst tubes of 10 m or more in order to maximize the outer surface area of the tubes. The present invention has the advantage that the design of the reactor system does not have such limitations.

In the context of the present invention, the meaning of the term reactor system including a structured catalyst is not limited to a reactor system with only one macroscopic structure. On the contrary, this term means both a structured catalyst with a macroscopic structure, a ceramic coating and a catalytically active material, and a set of such macroscopic structures.

Another aspect of the invention relates to a process for steam reforming of a hydrocarbon containing feed gas in a reactor system comprising a pressure vessel containing a structured catalyst for catalyzing the steam reforming of a hydrocarbon containing feed gas. A ceramic coating is located on the structured catalyst, which includes a macroscopic structure of an electrically conductive material, and on the macroscopic structure itself. The ceramic coating acts as a substrate for the catalytically active material, and a thermal insulation layer is provided between the structured catalyst and the pressure vessel in the reactor system. In the reactor system, a heat-insulating layer is provided between the structured catalyst and the pressure vessel.

The method includes the following steps:

compressing the source gas containing hydrocarbons to a pressure of at least 5 bar;

supply of compressed source gas to the reactor system;

steam reforming reaction of the source gas over the structured catalyst and removal of the gaseous product from the reactor system; and supplying current through the conductors connecting the power source, which is located outside the pressure vessel, and the structured catalyst, while the current is passed through the macroscopic structure, resulting in heating at least a portion of the structured catalyst to a temperature of at least 500°C. .

The method provides the same advantages as described for the reactor system. The gaseous product is synthesis gas. Synthesis gas is a gas containing carbon monoxide and hydrogen, as well as other components such as steam, carbon dioxide and methane. However, the process may include additional steps in which the gaseous product will be processed, such as purification, pressurization, heating, cooling, water gas shift reaction, etc., to obtain the final gaseous product that will be used in the process after the reactor systems according to the invention.

It should be noted that the feed gas may contain individual feed gases such as steam, hydrocarbon gas, carbon dioxide and hydrogen, and that the step of compressing the feed gas may include compressing the individual feed gases. In addition, it should be noted that the steps of the process do not have to be performed in the specified order, for example, two steps or multiple steps may be performed simultaneously, or the order may be different from the above order.

In one embodiment, the process includes the step of compressing the feed gas upstream of the pressure vessel to a pressure of at least 5 bar. For a small scale configuration, the design pressure of the pressure vessel can be in the range of 5-15 bar. For large scale configurations, the design pressure of the pressure vessel can be, for example, 15, 30 bar or up to 50 bar. It is even possible to use a pressure vessel with design pressures up to 150 or 200 bar.

In one of the embodiments of the method according to the invention, the temperature of the source gas entering the reactor system is 200-700°C. For SMR with external heating, the temperature of the source gas, as a rule, is increased to a temperature of 450-650°C; however, since the reactor system used in the process is an internally heated reactor system, the temperature of the feed gas can be as low as 200°C. However, in all embodiments, the feed gas temperature and pressure are controlled to ensure that the feed gas temperature is above the dew point.

In one of the embodiments of the process according to the present invention, the structured catalyst is heated so that the maximum temperature of the structured catalyst is in the range of 500-1300°C. Preferably, the maximum temperature of the structured catalyst is 700-1100°C, for example 900-1000°C. The maximum temperature of the structured catalyst depends on the material of the macroscopic structure. Thus, if the macroscopic structure is made from a Fecralloy® whose melting point is 1380-1490°C (depending on the actual properties of the alloy), the maximum temperature should be somewhat below the melting point, for example approximately 1300°C if the melting point of the macroscopic structure is approximately 1400 ° C, since when approaching the melting point, the material will become soft and ductile. The maximum temperature may be further limited by the wear resistance of the coating and the catalytically active material.

In one embodiment, the method of the present invention includes the step of supplying refrigerant gas through an inlet in the pressure housing so that refrigerant gas can pass through at least one conductor and/or fitting. The cooling gas may preferably be hydrogen, nitrogen, steam, carbon dioxide, or any other gas suitable for cooling the region or zone around the at least one conductor. A portion of the source gas, such as carbon dioxide and/or steam, can be fed into the pressure vessel as cooling gas.

In one embodiment of the process, the gas space velocity, measured as the gas flow rate relative to the geometric surface area of the structured catalyst, is in the range of 0.6-60 Nm ³ /m ² /h, for example in the range of 3-17 Nm ³ /m ² /h or, for example, 9-14 nm ³ /m ² /h. With respect to the occupied volume of the structured catalyst, the space velocity is in the range of 700-70000 Nm ³ /m ³ /h, for example in the range of 3500-20000 Nm ³ /m ³ /h or in the range of 11000-16000 Nm ³ /m ³ /h. If the space velocity is given relative to the active catalyst volume, i.e. volume of the ceramic coating, the volumetric velocity is in the range of 6000-1200000 nm ³ /m ³ /h. Working in these ranges of space velocity allows you to provide the required degree of conversion. It should be noted that the term gas space velocity refers to the space velocity of the gas entering the reactor system, namely both the feed gas velocity and the cooling gas velocity.

In one embodiment of the invention, the process further includes the step of supplying refrigerant gas through an inlet in the pressure housing so that refrigerant gas can pass through at least one conductor and/or fitting. Any suitable gas can be used as the cooling gas, for example, the cooling gas can be hydrogen, nitrogen, steam, carbon dioxide, or mixtures thereof. Coolant gas can flow through the conductors and cool them from the inside, in which case the conductors must be hollow to accommodate the cooling gas. A portion of the feed gas or a gas of the same composition as the feed gas can be used as the cooling gas.

The following is a detailed description of the embodiments of the present invention with reference to the accompanying drawings. Exemplary embodiments are described in sufficient detail to illustrate the invention. However, such a detailed description does not limit possible modifications of the embodiments; on the contrary, the aim is to cover all possible modifications, equivalents and alternatives that fall within the spirit and scope of the present invention, as defined in the appended claims.

Brief description of the figures

In FIG. 1a is a cross-sectional view of a reactor system of the invention with a structured catalyst comprising a set of macroscopic structures, in accordance with one embodiment of the invention.

In FIG. 1b shows a reactor system which is also shown in FIG. 1a, while in Fig. 1b part of the pressure vessel and thermal insulation layer has been removed.

In FIG. 2 is an enlarged view of part of the reactor system.

In FIG. 3a and 3b are cross-sectional views of a reactor system including a structured catalyst, in accordance with one embodiment of the invention.

In FIG. 4 and 5 show an embodiment of a structured catalyst with a set of macroscopic structures, top view and side view, respectively.

In FIG. 6 shows an embodiment of a structured catalyst that can be used in the reactor system of the invention.

In FIG. 7 and 8 show embodiments of a structured catalyst with connectors.

In FIG. 9a shows an embodiment of a structured catalyst that can be used in the reactor system of the invention.

In FIG. 9b shows the current density of the structured catalyst according to FIG. 9a as a function of the electrical effect transferred to the structured catalyst.

In FIG. 10 is a schematic cross-sectional view of a structured catalyst with electrically insulating parts.

In FIG. 11a and 11b show temperature and conversion profiles as a function of the electrical effect transferred to the structured catalyst.

In FIG. 12a and 12b show the results of modeling temperature and gas composition along the length of the structured catalyst.

In FIG. 13 shows the required maximum temperature in the reactor system according to the invention as a function of pressure.

In FIG. 14 is a graph of the approach to equilibrium conditions (AT _equals SMR) of the methane steam reforming reaction for various rates of gas flow through the structured catalyst.

Detailed description of the figures

Throughout the figures, reference numbers refer to the respective elements.

In FIG. 1 is a cross-sectional view of a reactor system 100 in accordance with one embodiment of the invention. The reactor system 100 contains a structured catalyst 10 arranged in a set of macroscopic structures 5. Each macroscopic structure 5 in the set has a ceramic coating impregnated with a catalytically active material. In addition, the reactor system 100 includes conductors 40, 40' connected to a power source (not shown in the figures) and to a structured catalyst 10, namely a set of macroscopic structures. The conductors 40, 40' pass through the wall of the pressure vessel 20 containing the structured catalyst and through the insulating material 30 on the inside of the pressure vessel through fittings 50. The conductors 40' are connected to the set of macroscopic structures 5 via conductor busbars 41.

In one of the embodiments of the invention, a power supply with a voltage of 70 V and a current of 800 A is used. In another embodiment of the invention, a power supply with a voltage of 170 V and a current of 2000 A is used. and the current passes through the structured catalyst 10 from one conductor bar 41, for example from a conductor bar, which in FIG. 1a is shown on the left, up to another conductor bar 41, for example a conductor bar, which in FIG. 1a is shown on the right. The current may be variable and, for example, flow alternately in both directions, or it may be constant and flow in one of the two directions.

The macroscopic structures 5 are made of an electrically conductive material. Particularly preferred is a kanthal alloy consisting of aluminium, iron and chromium. The ceramic coating, such as an oxide, deposited on the structured catalyst 5 is impregnated with a catalytically active material. The conductors 40, 40' are made of materials such as iron, aluminium, nickel, copper or their alloys.

During operation, the source gas is fed into the reactor system 100 from above, as indicated by arrow 11, and exits the reactor system from below, as indicated by arrow 12.

In FIG. 1b shows a reactor system 100, which is also shown in FIG. 1a, while in Fig. 1b, part of the pressure vessel 20 and the thermal insulation layer 30 have been removed, and in FIG. 2 is an enlarged view of a portion of reactor system 100. FIG. 1b and 2 the connections between the conductors 40' and the contact bars 41 of the conductor are shown more clearly than in FIG. 1a. In addition, it can be seen that the conductors 40 pass through the walls of the pressure vessel by means of fittings 50 and that inside the pressure vessel one conductor 40 is divided into three conductors 40'. It should be noted that any suitable number of conductors 40' may be used, for example less than three or more than three conductors may be used.

In the reactor system shown in FIG. 1a, 1b and 2, conductors 40, 40' pass through the wall of the pressure vessel 20 containing the structured catalyst and through the insulating material 30 on the inside of the pressure vessel through fittings 50. The steam reforming feed gas is fed into the reactor system 100 through the inlet at the top of the reactor system 100, indicated by arrow 11, and the reformed gas leaves the reactor system 100 through the outlet at the bottom of the reactor system 100, indicated by arrow 12. Moreover, adjacent to the fittings 50 or in combination with fittings, one or more additional inlets (not shown in Figs. 1a-2) can advantageously be located. Such additional inlets allow refrigerant gas to pass through, around, adjacent to, or within at least one conductor within said pressure vessel to reduce heating of the fitting. The cooling gas may, for example, be hydrogen, nitrogen, steam, carbon dioxide or mixtures thereof. The temperature of the cooling gas at the supply to the pressure vessel may be, for example, approximately 100°C.

In the reactor system 100 shown in FIG. 1a-2, between the bottom of the structured catalyst 10 and the bottom of the pressure vessel there is predominantly an inert material (not shown in FIGS. 1a-2). Moreover, an inert material is preferably present between the outer sides of the structured catalyst 10 of the macroscopic structures 5 and the insulating material 30. Thus, one side of the insulating material 30 faces the inside of the pressure vessel 20 and the other side of the insulating material 30 faces the inert material. The inert material is, for example, a ceramic material. The inert material may be in the form of granules. The inert material assists in controlling the pressure drop across the reactor system 100 and controlling the flow of gas through the reactor system 100 so that the gas flow flows over the surfaces of the structured catalyst 10.

In FIG. 3a and 3b are cross-sectional views of a reactor system 100', 100'' including a structured catalyst 10a, in accordance with one embodiment of the invention. The structured catalyst 10a may consist of a single ceramic-coated macroscopic structure that acts as a support for the catalytically active material, or the structured catalyst may include two or more macroscopic structures. Each of the reactor systems 100', 100''c includes a pressure vessel 20 and a thermal insulation layer 80 between the structured catalyst 10a and the pressure vessel 20; in fig. 3a and 3b, the inert material 90 is indicated by hatching. An inert material 90 may be used to fill the gap between the structured catalyst 10a and the thermal barrier layer or pressure vessel 20. FIG. 3a and 3b, inert material 90 is indicated by hatching; the inert material 90 may be in any suitable form, such as inert granules, and may be, for example, a ceramic material. The inert material 90 assists in controlling the pressure drop in the reactor system and controlling the flow of gas through the reactor system. In addition, the inert material generally has a heat-insulating effect.

From FIG. 3a and 3b, it can be seen that the reactor systems 100', 100'' additionally comprise an inner tube 15, heat exchange between it and the structured catalyst 10a. The inner tube 15 is configured to withdraw product gas from the structured catalyst 10a such that the product gas entering through the inner tube or tubes is heat exchanged with the gas entering through the structured catalyst; however, the inner tube 15 is electrically isolated from the structured catalyst 10a by a heat insulating layer 80 or an inert material 90 or a gap or a combination thereof. This configuration is referred to as a bayonet reactor system. In this configuration, the product gas in the inner tube contributes to the heating of the process gas entering through the macroscopic structure. In the configurations shown in FIG. 3a and 3b, the feed gas is fed into the reactor system 100', 100 through the inlet indicated by the arrow 11 and enters the structured catalyst 10a at the front portion 101a as shown by the arrows 13. While the feed gas passes through the structured catalyst 10a, the reaction steam reforming of the source gas. The gas exiting the back portion 102a of the structured catalyst 10a is at least partially reacted in the reforming reaction. The streams of at least partially reformed gas exiting the back portion 102a of the structured catalyst 10a enter the inner tube 15 as indicated by arrows 14 and exit the inner tube through the pressure vessel outlet as indicated by arrows 12. Even though With inert material 80 present between inner tube 15 and structured catalyst 10a, there will be some heat transfer from the gas inside the inner tube 15 and the gas inside the structured catalyst 10a or upstream of the structured catalyst 10a. In the embodiments shown in FIG. 3a and 3b, the feed gas flows downward through the structured catalyst 10a, from the structured catalyst front 101a to the back 102a, and then upwards through the inner tube 15; however, the reverse configuration is also possible, so that the feed gas will flow upwards through the structured catalyst 10a and downwards through the inner tube 15. In this case, the lower part of the structured catalyst will act as a front part, and the upper part

- 17 041025 structured catalyst will act as the rear part.

In FIG. 4 and 5 show an embodiment of a structured catalyst including a set of macroscopic structures, top and side views, respectively. In FIG. 4 shows a structured catalyst 10 including a set of macroscopic structures 5, viewed from above, namely the view along the direction of the arrow 11 in FIG. 1a and 1b. This set has 6 rows, namely 1a, 1b, 1c, 1d, 1e and 1f of five macroscopic structures 5. Macroscopic structures 5 in each row are connected to an adjacent macroscopic structure in the same row, and the two extreme macroscopic structures in each row are connected to contact bus 41 conductor. Neighboring macroscopic structures 5 in a row of macroscopic structures are connected to each other by means of a connecting element 3.

In FIG. 5 shows a structured catalyst 10 having the set of macroscopic structures 5 shown in FIG. 4, side view. In FIG. 5 it can be seen that each macroscopic structure 5 extends in the longitudinal direction perpendicular to the cross section shown in FIG. 4. Each macroscopic structure 5 has a slot 60 cut in the longitudinal direction relative to the macroscopic structure (see Fig. 5). Therefore, the current from the power supply is fed into the set of macroscopic structures 5 through the contact strip 41 of the conductor, it passes through the first macroscopic structure 5 down to the lower border of the slot 60 and then it is fed upwards to the connecting element 3. The current follows a corresponding zigzag path down and up through each macroscopic structure 5 in each row 1a-1f of macroscopic structures 5 in the set 10. The advantage of this configuration is that in this case the resistance is increased compared to the structured catalyst 10.

In FIG. 6 shows a perspective view of the structured catalyst 10' of the present invention. Structured catalyst 10' contains a macroscopic structure that has a ceramic coating impregnated with a catalytically active material. Within the structured catalyst there are channels 70 extending in the longitudinal direction (shown by an arrow labeled h in FIG. 6) of the macroscopic structure 5, these channels are delimited by walls 75. In the embodiment shown in FIG. 6, walls 75 form a series of parallel square channels 70 as viewed from the direction of flow indicated by arrow 12. Structured catalyst 10' has a substantially square (when viewed from above) perimeter defined by edges e1 and e2. However, the perimeter can also be circular or have a different shape.

The walls 75 of the structured catalyst 10' are made of a ceramic-coated extruded material, such as an oxide, deposited on a macroscopic structure in the form of a coating. the ceramic coating is not shown in the figures. The ceramic coating is impregnated with a catalytically active material. A ceramic coating, and hence catalytically active material, is present on each wall of the structured catalyst 10', which carries a gas stream during operation of the reactor and interacts with the heated surface of the structured catalyst and catalytically active material.

Thus, in a steam reforming reactor system, the hydrocarbon feed gas passes through channels 70 and interacts with the heated surface of the structured catalyst and with the catalytically active material located on the ceramic coating substrate.

In the structured catalyst 10' shown in FIG. 6, there is a slot 60. Due to this slot 60, the current flows inside the macroscopic structure in a zigzag way (in this case down and then up), as a result of which the current path increases, and therefore the resistance increases, and therefore the amount of heat increases, which is given to the macroscopic structure. An insulating material may be embedded in slot 60 within the macroscopic structure to ensure that current does not flow in a direction transverse to slot 60.

The channels 70 in the structured catalyst 5 are open at both ends. When using a structured catalyst in a reactor system, the hydrocarbon feed gas flows through the plant in the direction shown by arrows 11 and 12 in FIG. 1a and 1b and is heated by contact with the walls 75 of the channels 70 and by radiation heating. Due to the heat, the necessary steam reforming process is initiated. The thickness of the walls 75 of the channels 70 may be, for example, 0.5 mm, and the thickness of the ceramic coating applied to the walls 75 may be, for example, 0.1 mm. Although arrows 11 and 12 (see FIGS. 1a and 1b) indicate that the flow of the hydrocarbon feed gas is directed downward, the opposite direction of flow is also possible, namely, the flow may be directed upward.

In FIG. 7 is a view of the structured catalyst 5 according to FIG. 1a and 1b are perspective views with connectors 7 attached. Each connector 7 connects a portion of the structured catalyst 10' to a conductor 40. Both conductors 40 are connected to a power source (not shown). Each of the connectors 7 is connected to the top of the structured catalyst. When the conductors 40 are connected to a power supply, the current is supplied to the corresponding connector 7 through the conductor and passes through the structured catalyst 10'. The slot 60 prevents the passage of current in the transverse direction (horizontal direction in Fig. 7) along its entire length along the height h of the structured catalyst 10'. Therefore, the current flows in downwards, as shown in Fig. 7 in structure part

- 18 041025 of the structured catalyst along the slot 60, then it passes perpendicular to the longitudinal axis of the structured catalyst under the slot 60, as shown in FIG. 7, and finally the current flows upward, parallel to the longitudinal axis of the structured catalyst, to another connector 7. The connectors 7 in FIG. 7 are mechanically attached to the structured catalyst, in particular by means of mechanical fasteners such as screws and bolts. However, additional or alternative fasteners are possible. In one of the embodiments of the invention, a power supply with a voltage of 3 V and a current of 400 A is used.

The conductors 7 are made, for example, of materials such as iron, aluminium, nickel, copper or their alloys.

As already mentioned, the structured catalyst 10' has a ceramic coating, for example of an oxide, which acts as a support for the catalytically active material. However, the portions of the structured catalyst 10' that are connected to the connectors 7 must not be coated with oxide. Instead, the macroscopic structure of the structured catalyst must be in direct contact with or connected to the connectors 7 in order to provide the necessary electrical contact between the macroscopic structure and the connector.

When the connectors 7 and hence the conductors 40 are connected to one part of the structured catalyst 5, i. e. towards the top, as shown in Fig. 7, the gas supplied to the reactor system containing the structured catalyst 10' will be able to cool the connectors 7 and conductors 40. For example, the hydrocarbon gas supplied to such a reactor system will have a temperature of 400 or 500°C, thus will prevent connectors 7 and conductors 40 from reaching temperatures much higher than this temperature.

In FIG. 8 shows another embodiment of a structured catalyst 10' with connectors 7'''. The structured catalyst 10' is, for example, the structured catalyst shown in FIG. 6. Each of the connectors 7''' has three holes at its top for connection to conductors (not shown). Inside the slot 60 of the structured catalyst 10' is a piece of electrically insulating material 61 (see FIG. 6).

In FIG. 9a shows an embodiment of a structured catalyst 10'' that can be used in the reactor system of the invention. In FIG. 9a shows the structured catalyst 10 in perspective. It can be seen that the structured catalyst 10'' has a single vertical slot 60 along the longitudinal axis of the catalyst 10' as shown in FIG. 9a. A single vertical slot 60 extends from the top of the structured catalyst 10'' to its bottom, occupying approximately 90% of the length of the structured catalyst. A single vertical slot 60 may be considered to separate the structured catalyst 10'' into two halves. Each of these two halves has five horizontal slots 65. The vertical slot 60 and horizontal slots 65 serve to direct current through the structured catalyst in a zigzag path.

In FIG. 9b shows the current density of the structured catalyst 10 according to FIG. 9a as a function of the electrical effect transmitted to the structured catalyst 10''. Also in FIG. 9b shows data obtained from a multiphysics simulation of the current distribution in the structure shown in FIG. 9a using CFD methods using Comsol software. In FIG. 9b is a side view of the structured catalyst 10''. Two conductors (not shown in Fig. 9b) are connected to the top of the structured catalyst 10'' on the left side. As demonstrated by the current density intensity as shown on the scale on the right side of FIG. 9b, when a power supply is connected to the structured catalyst 10″, due to the horizontal slots, current flows from its top in a zigzag pattern to the bottom of the structured catalyst 10 towards its rear, i.e. into paper, as shown in Fig. 9b and then zigzag up to the second conductor. The temperature of the structured catalyst 10'' depends on the current density in the structured catalyst 10''. Also in FIG. 9b, it can be seen that the current density is highest at the end points of the horizontal slots 65 in the structured catalyst 10''. At these points, the current path changes direction, i.e. at these points there is a change in the direction of the current passing through the structured catalyst 10''. In addition, it can be concluded that the current density vector of the main current path has a non-zero component value, parallel to the length of the specified structured catalyst for more than 80% of the structure. Finally, from FIG. 9b shows that the main current path can be controlled in the structured catalyst. This makes it possible to control the temperature profile within the structured catalyst.

In FIG. 10 is a schematic cross-sectional view of a structured catalyst with electrically insulating parts. In FIG. 10 shows a schematic cross-sectional view of a structured catalyst 10''' according to the invention with electrically insulating parts 61'. In FIG. 10 the electrically insulating parts are shown in hatching. In the embodiment shown in FIG. 10, three electrically insulating portions 61' traverse the major portion of the structured catalyst 10''' in the longitudinal direction. The conductors 7 are connected to the upper side of the structured catalyst 10' as shown in FIG. 10. During the use of a structured cathal

- 19 041025 plug 10''', the conductors 7 are connected to a power source, and the original hydrocarbon gas is in contact with the structured catalyst 10'''. Thus, the current flows from the first conductor through the structured catalyst 10''' in a zigzag direction, namely downwards from the first conductor, along the underside of the first electrically insulating portion 61', then upwards, along the upper side of the middle electrically insulating portion 61', then down again. and along the underside of the third electrically insulating portion 61' and finally upwards to the second conductor 7. It should be noted that any suitable number of electrically insulating portions 61' may be used. The electrical insulating parts 61' are made of a solid electrical insulating material, such as glass, and are in slots in the macroscopic structure. Due to the electrically insulating parts 61', the macroscopic structure parts are separated by the sides of the electrically insulating parts 61'. It should be noted that in this embodiment, as in other embodiments, the gas flow may flow in the same direction as the direction of the current through the structured catalyst, or in a different direction. In the embodiment shown in FIG. 10, the gas flow is directed, for example, from the top of the structured catalyst 10''' to the bottom of the structured catalyst 10'''; thus, the direction of the current coincides with the direction of the gas flow only in some parts of the structured catalyst 10''', while in other parts the direction of the current is perpendicular to the direction of the gas flow and opposite to the direction of the gas flow (when the current goes up).

In FIG. 11a and 11b show temperature and conversion profiles as a function of the electrical effect transferred to the structured catalyst. In FIG. 11a shows the results of laboratory testing of a structured catalyst bench reactor system 12 cm long and 108 cm ³ in volume, which is defined by its outer walls/sides, and with the configuration shown in FIG. 6, where copper conductors are welded to the first 2 cm of the monolith on opposite sides in the front. The pressure in the pressure vessel was 3.5 bar, the temperature at the source gas supply to the reactor system was approximately 200°C. The feed gas used was 31.8% CH ₄ , 2.4% H ₂ , 65.8% H ₂ O and the total gas flow was 102.2 NL/h. It should be noted that the energy balance is much better in a larger scale reactor than under the conditions of a small scale experiment, the results of which are plotted in FIG. 11a due to the high energy loss at such a relatively small scale. However, from FIG. 11a shows that with increasing power, both the degree of methane conversion and the temperature increase. The temperature exceeds 900°C, and the degree of methane conversion reaches more than 98%.

In FIG. 11b shows an experiment similar to that described above, but with a pressure of 21 bar. Again from FIG. 11a it can be seen that with increasing power, the degree of methane conversion and temperature increase. The temperature exceeds 1060°C, and the degree of methane conversion reaches more than 95%.

In FIG. 12a and 12b show the results of modeling temperature and gas composition along the length of the structured catalyst. A single channel of the structured catalyst is modeled. The length of the structured catalyst in this model, and therefore the length of one channel, is 10 cm. The following conditions are provided inside the pressure vessel/structured catalyst/channel:

pressure: 29 bar i.d.;

Tin: 466°C;

total flow: 30 Nl/h

the composition of the source gas at the feed to the reactor/channel: 31.8% methane, 8.8% hydrogen, 2.3% carbon dioxide and 57.1% steam.

In FIG. 12a, the temperature of the channel wall is indicated by Tw, and the temperature at the center of the channel is indicated by Tc. The values of Tw and Tc are indicated on the scale to the right of the graphs. The degree of methane conversion is denoted by Cs, the corresponding values are indicated on the scale to the left of the graphs.

From FIG. 12a shows that the temperature of the channel wall in the structured catalyst increases continuously along almost the entire length of the structured catalyst. At the front (z=0 cm) of the structured catalyst, the temperature is approximately 480°C and at the back of the structured catalyst (z=10 cm) is approximately 1020°C. The temperature increases most rapidly in the first 10% of the length of the structured catalyst, with little change in temperature over the last few percent of the length of the structured catalyst. Thus, as the current changes direction at the rear of the structured catalyst, from downward to upward in FIG. 1-9a, the temperature of the channel walls of the structured catalyst does not change significantly with increasing z values. However, in FIG. 12a also shows that the temperature at the center of the channel continues to increase along the entire length of the structured catalyst. However, it should be noted that the temperature in the center of the channel remains almost constant for the first 5–7% of the length of the structured catalyst. This is due to the fact that the gas supply to the structured catalyst provides cooling of the structured catalyst near its front due to the delay in the transfer of thermal energy from the wall to the center of the channel.

In FIG. 12a also shows data on the conversion of methane in the center of the structured ca

- 20 041025 tote. It can be seen that for the first 10-12% of the channel length, the degree of conversion is close to zero, and then the conversion gradually increases and reaches a value of about 85%. As noted above, simulations for small scale reactors provide sub-optimal values, and a much higher conversion rate is achievable in a real scale reactor system. However, the simulation provides information on the trends in the conversion rate and temperature in the structured catalyst.

In FIG. 12b shows the partial pressures of the main active gases in the channel of the structured catalyst in FIG. 12a. From FIG. 12b shows that the partial pressures of steam and methane decrease significantly along the length of the channel of the structured catalyst, while the partial pressures of hydrogen and carbon monoxide increase significantly. In addition, the partial pressure of carbon dioxide increases slightly along the length of the structured catalyst, but decreases at the highest temperatures, when the water gas shift reverse reaction is thermodynamically preferable.

In FIG. 13 shows the required maximum temperature within the reactor system of the invention as a function of pressure for pressures in the range of approximately 30-170 bar during steam reforming of a feed gas of 30.08% CH ₄ , 69.18% H ₂ O, 0, 09% H ₂ , 0.45% CO ₂ , 0.03% Ar, 0.02% CO, 0.15% N 2 to achieve a methane conversion of 88% at 10° C. under near-equilibrium methane steam reforming conditions. The required maximum temperature increases with increasing pressure due to Le Chatelier's principle. This shows that due to the high temperatures that can be used in the present invention, significantly higher pressures can be used than those used in traditional SMR where, due to external heating of the tubes, temperatures above 950°C cannot be used. A temperature of 950°C corresponds to 27 barg. in fig. 13. The reactor system according to the invention can use, for example, a maximum temperature of 1150°C, which provides a pressure of up to 146 barg. while maintaining the above degree of methane conversion.

In FIG. 14 is a graph of the approach to equilibrium conditions (AT _{equals SMR} ) of the methane steam reforming reaction for various rates of gas flow through the structured catalyst. in fig. 14 shows that at a certain gas flow rate through the structured catalyst, conditions close to equilibrium at the inlet to the reactor system with the structured catalyst inside are created at a temperature in the range of 160-175°C, since the feed gas is far from equilibrium. As the hydrocarbon gas passes through the structured catalyst, the temperature approaching equilibrium conditions decreases due to catalytic reactions.

In FIG. 14 shows near-equilibrium conditions (AT _{equals SMR} ) for gas flow rates from 10,000 Nm ³ /h to 200,000 Nm ³ /h. For the lowest gas flow rate, 10,000 Nm ³ /h, the temperature approaching equilibrium conditions becomes less than 10° C. for about 13% of the length of the reactor system. Here, the length of the reactor system is considered as the outer height of the structured catalyst in the flow direction, so that the length of the reactor system of the structured catalyst 10 is about 1h according to the embodiment shown in FIG. 6. For higher gas flow rates, the temperature approaching equilibrium conditions is higher, the higher the gas flow rate, therefore, at a gas flow rate of 200,000 Nm ³ /h, the temperature approaching equilibrium conditions reaches a minimum value of just under 80°C.

The general trend for all curves in Fig. 14 is that the temperature for near-equilibrium conditions decreases continuously from entering the structured catalyst until pseudo-equilibrium is reached, where heat input and heat consumption are approximately equal to each other. From this point on, the temperature of approach to equilibrium conditions remains practically constant or slightly increases due to the general increase in the temperature of the reactor system. For example, at a flow rate of 150,000 Nm ³ /h, the temperature approaching equilibrium conditions falls below 60°C for about 80% of the length of the reactor system, but subsequently increases to about 60°C.

It should be noted that even though the figures show structured catalysts with square cross-sectional channels (when viewed perpendicular to the z-axis), any suitable channel cross-sectional shape is possible. Thus, as an alternative, the channels of the structured catalyst may be, for example, triangular, hexagonal, octagonal, or circular in shape. Triangular, square or hexagonal channels are preferred.

Examples

The invention is illustrated by the description of various embodiments and examples, and although these embodiments and examples are described in some detail, the Applicant does not intend to limit the scope of the appended claims to such a detailed description. Additional advantages and possible modifications will be apparent to those skilled in the art. Therefore, the invention in general aspects is not limited to the given specific details, typical methods and illustrative examples. Accordingly, deviations from such details are permissible without distorting the essence or scope of the Applicant's general inventive concept.

- 21 041025

All the examples described below refer to compact reactor systems. This is possible due to the fact that the reactor systems contain compact structured catalysts in the form of compact macroscopic substrates with a high heat flux during electric heating. In addition, it should be noted that the dimensions of the structured catalysts can be chosen relatively freely, so that the structured catalyst may have an almost cubic external shape, or its width may be greater than its height.

All examples describe high pressure operating conditions in the range of 28-182 bar. Such high pressures are possible due to the configuration of the reactor system because the structured catalyst within the reactor system has a high heat flux when electrically heated, it is thermally insulated from the pressure vessel to some extent, and a very low pressure drop across the structured catalyst compared to SMR is achieved. In the reactor system, the structured catalyst will have the highest temperature, while the pressure vessel will have a significantly lower temperature due to the thermal insulation layer between the structured catalyst and the pressure vessel. Ideally, the temperature of the pressure vessel should not exceed 500°C. When a high pressure product gas, such as 30 bar or higher, is required, the product gas leaving the reactor system can often be used directly without the use of compressors. This is possible due to the stage of compression of the source gas during the process before the reactor system according to the invention. Compressing the feed gas requires less energy than compressing the gaseous product because the volume of the feed gas is smaller than the volume of the gaseous product, since the steam reforming reaction has a net formation of molecules. In addition, one of the feed gas components can be pumped, which requires significantly less energy compared to compressing the gas.

In all of the examples below, the feed gas enters the reactor system and passes through the structured catalyst within it. When the reactor system has a heat insulating material, the heat insulating material typically occupies most of the space between the structured catalyst and the pressure vessel along the walls of the pressure vessel, so that when passing through the pressure vessel, the feed gas is forced to flow along the walls of the macroscopic structure.

All of the examples below (with the exception of the comparative example) refer to the structured catalyst reactor system. The structured catalysts described in these examples include one or more macroscopic structures. In the examples below, one or more macroscopic structures are provided with a ceramic coating, said ceramic coating acting as a support for the catalytically active material. Preferably, almost the entire surface of the macroscopic structure has a ceramic coating acting as a substrate for the catalytically active material; however, at connection points, such as at the junction of two adjacent macroscopic structures or at the junction of the macroscopic structure and the conductor, the macroscopic structure may not have a ceramic coating in order to facilitate the connection between the conductor and the macroscopic structure.

Example 1

In table. 1 below shows an example of calculating the parameters of the method according to the invention. The reactor system according to the invention is fed with a feed gas. The feed gas entering the reactor system is at a pressure of 28 kg/cm-g and has a temperature of 500°C. A structured catalyst is placed inside the reactor system with a set of nine macroscopic structures with a square cross section, and each macroscopic structure has a size of 0.53x0.53x2.3 m. Each macroscopic structure additionally has 17778 channels with a square cross section and with a side or edge length of 0, 32 cm. Each macroscopic structure has slots parallel to its longitudinal direction, so that 5 groups of 5 channels are formed. Each group of channels is isolated from the next, except for the end portions, so that the current flows through the macroscopic structure in a zigzag path. Each macroscopic structure in the reactor system of the invention is subjected to a current of 200 A and a voltage of approximately 5.5 kW to heat the structured catalyst and hence the gas passing through the structured catalyst, corresponding to an input power of 9899 kW.

The overall internal diameter of the reactor system in this configuration can be 3.2 m and the overall internal height 5.5 m if the reactor system is cylindrical with spherical heads. In this particular configuration, the macroscopic structures are arranged in a square with a diagonal length of 2.3 m. In all examples described herein, except for the comparative example, an inert material is located around the structured catalyst, closing the gap between the insulating material adjacent to the pressure vessel. The insulating material in example 1 has a cylindrical shape with an inner diameter of 2.5 m and a thickness of 0.35 m.

During the passage of the feed gas through the reactor system, the feed gas is heated by the heat of the structured catalyst and a steam reforming reaction is carried out to obtain a gaseous

- 22 041025 different product with an outlet temperature of 963°C.

Table 1

Macroscopic structure size: Edge length [m] 0.53 Height (m) 2.3 Number of macroscopic structures 9 Total volume of structured catalyst [l] 5888 Height/diagonal length structured catalyst [-] 1.02 source gas gaseous product T[°C] 500 963 P [kg/cm ² g] 27.97 27.47 CO2 [nm ³ /h] 168 727 N2 [nm ³ /h] 26 26 CH4 [nm ³ /h] 2630 164 H2 [nm ³ /h] 590 8545 CO [nm ³ /h] 1 1907 H2O [nm ³ /h] 8046 5022 Total flow [nm ³ /h] 11461 16391 AT _paBH ,SMR [°C] 10 Power, kWt] 9899 Heat flux [kW/m ² ] 2.2 Volume velocity [nm ³ /m ³ /h] 1950

Example 2

In table. 2 below shows an example of calculating the parameters of the method according to the invention. The reactor system according to the invention is fed with a feed gas. The feed gas entering the reactor system is at a pressure of 28 kg/cm-g and has a temperature of 500°C. Inside the reactor system, a structured catalyst is placed in the form of one macroscopic structure with a square cross section with a size of 0.4x0.4x0.35 m. The macroscopic structure additionally has 10,000 channels with a square cross section and with a side or edge length of 0.32 cm. parallel to its longitudinal direction, so that 5 groups of 5 channels are formed. Each group of channels is isolated from the next, except for the end portions, so that the current flows through the macroscopic structure in a zigzag path. The macroscopic structure in the reactor system of the invention is subjected to a current of 200 A and a voltage of approximately 500 V to heat the structured catalyst, and hence the gas passing through the structured catalyst, corresponding to an input power of 99 kW.

The total internal diameter of the reactor system in this configuration may be 1.2 m and the total internal height 1.5 m if the reactor system is cylindrical with spherical heads. In this particular configuration, the diagonal of the structured catalyst has a length of 0.6 m. Surrounding the structured catalysts is an inert material covering the gap between an insulating material with an internal diameter of 0.6 m and a thickness of 0.3 m.

During the passage of the feed gas through the reactor system, the feed gas is heated by the heat of the structured catalyst and a steam reforming reaction is carried out to obtain a gaseous product with an outlet temperature of 963°C.

- 23 041025

table 2

Macroscopic structure size: Edge length [m] 0.4 Height (m) 0.35 Number of macroscopic structures 1 Total volume of structured catalyst [l] 55.4 Height/length of the diagonal structured catalyst [-] 0.61 source gas gaseous product T[°C] 500 963 P [kg/cm ² g] 27.97 27.47 CO2 [nm ³ /h] 1.7 7.3 N2 [nm ³ /h] 0.3 0.3 CH4 [nm ³ /h] 26.3 1.6 H2 [nm ³ /h] 5.9 85.4 CO [nm ³ /h] 0 19.1 H2O [nm ³ /h] 80.5 50.2 Total flow [nm ³ /h] 114.7 163.9 AT _paBH ,SMR [°C] 10 Power, kWt] 99 Heat flux [kW/m ² ] 2.2 Volume velocity [nm ³ /m ³ /h] 2071

Example 3

In table. 3 below shows an example of calculating the parameters of the method according to the invention. The reactor system according to the invention is fed with a feed gas. The feed gas entering the reactor system is at a pressure of 97 bar, i.e. 97 kg/cm ² -g and has a temperature of 500°C.

A structured catalyst is placed inside the reactor system with a set of nine macroscopic structures with a square cross section, and each macroscopic structure has a size of 0.53x0.53x2.3 m. Each macroscopic structure additionally has 17778 channels with a square cross section and with a side or edge length of 0, 32 cm. Each macroscopic structure has slots parallel to its longitudinal direction, so that 5 groups of 5 channels are formed. Each group of channels is isolated from the next, except for the end portions, so that the current flows through the macroscopic structure in a zigzag path. Each macroscopic structure in the reactor system of the invention is subjected to a current of 200 A and a voltage of approximately 5.5 kW to heat the structured catalyst and hence the gas passing through the structured catalyst, corresponding to an input power of 9899 kW.

The overall internal diameter of the reactor system in this configuration can be 3.2 m and the overall internal height 5.5 m if the reactor system is cylindrical with spherical heads. In this particular configuration, the macroscopic structures are arranged in a square with a diagonal length of 2.3 m. An inert material is located around the structured catalyst, closing the gap between the insulating material with an internal diameter of 2.5 m and a thickness of 0.35 m.

During the passage of the feed gas through the reactor system, the feed gas is heated by the heat of the structured catalyst and a steam reforming reaction is carried out to obtain a gaseous product with an outlet temperature of 1115°C. From Table. 3 it can be seen that the total flow rates of the source gas and the gaseous product in example 3 are lower compared to example 1.

Since the product gas leaving the reactor system has a pressure of 97 bar, it is not necessary to use compressors downstream of the reactor system during the process if a high pressure product gas is required. This greatly reduces the overall cost of the installation with the reactor system according to the invention.

- 24 041025

Table 3

Macroscopic structure size: Edge length [m] 0.53 Height (m) 2.3 Number of macroscopic structures 9 Total volume of structured catalyst [l] 5888 Height/diagonal length structured catalyst [-] 1.01 source gas gaseous product T[°C] 500 1115 P [kg/cm ² g] 96.97 96.47 CO2 [nm ³ /h] 111 510 N2 [nm ³ /h] 23 23 CH4 [nm ³ /h] 2337 143 H2 [nm ³ /h] 372 7354 CO [nm ³ /h] 1 1796 H2O [nm ³ /h] 7111 4518 Total flow [nm ³ /h] 9955 14344 4Tp _aBH ,SMR [°C] 10 Power, kWt] 9899 Heat flux [kW/m ² ] 2.2 Volume velocity [nm ³ /m ³ /h] 1691

Example 4

In table. 3 below shows an example of calculating the parameters of the method according to the invention. The reactor system according to the invention is fed with a feed gas. The feed gas entering the reactor system is at a pressure of 28 bar, i.e. 28 kg/cm-g and has a temperature of 500°C.

A structured catalyst is placed inside the reactor system with a set of 25 macroscopic structures with a square cross section, and each macroscopic structure has a size of 0.24x0.24x0.9 m. Each macroscopic structure additionally has 3600 square channels and with a side or edge length of 0, 33 cm. Each macroscopic structure has slots parallel to its longitudinal direction, so that 10 groups of 10 channels are formed. Each group of channels is isolated from the next, except for the end portions, so that the current flows through the macroscopic structure in a zigzag path. Each macroscopic structure in the reactor system of the invention is subjected to a current of 1500 A and a voltage of approximately 260 kW to heat the structured catalyst and hence the gas passing through the structured catalyst, corresponding to an input power of 9899 kW.

The total internal diameter of the reactor system in this configuration may be 2.3 m and the total internal height 3.2 m if the reactor system is cylindrical with spherical heads. In this particular configuration, the macroscopic structures are arranged in a square with a diagonal length of 1.7 m. An inert material is located around the structured catalyst, closing the gap between the insulating material with an internal diameter of 1.8 m and a thickness of 0.25 m.

During the passage of the feed gas through the reactor system, the feed gas is heated by the heat of the structured catalyst, and a steam reforming reaction is carried out to obtain a gaseous product with an outlet temperature of 963°C. From Table. 4 shows that the structured catalyst according to example 4 is slightly smaller than the structured catalyst according to examples 1 and 3 due to the higher current strength. The total flow rates of feed gas and product gas correspond to those of Example 1.

- 25 041025

Table 4

Macroscopic structure size: Edge length [m] 0.24 Height (m) 0.9 Number of macroscopic structures 25 Total volume of structured catalyst [l] 1324 Height/length of the diagonal structured catalyst [-] 0.54 source gas gaseous product T[°C] 500 963 P [kg/cm ² g] 27.97 27.47 CO2 [nm ³ /h] 168 727 N2 [nm ³ /h] 26 26 CH4 [nm ³ /h] 2630 164 H2 [nm ³ /h] 590 8545 CO [nm ³ /h] 1 1907 H2O [nm ³ /h] 8046 5022 Total flow [nm ³ /h] 11461 16391 AT _paBH ,sMR [°C] 10 Power, kWt] 9899 Heat flux [kW/m ² ] 9.0 Volume velocity [nm ³ /m ³ /h] 8653

Example 5

In table. 4 below shows an example of calculating the parameters of the method according to the invention. The reactor system according to the invention is fed with a feed gas. The feed gas entering the reactor system is at a pressure of 182 bar and has a temperature of 500°C.

A structured catalyst is placed inside the reactor system with a set of nine macroscopic structures with a square cross section, and each macroscopic structure has a size of 0.53x0.53x2.3 m. Each macroscopic structure additionally has 17778 channels with a square cross section and with a side or edge length of 0, 32 cm. Each macroscopic structure has slots parallel to its longitudinal direction, so that 5 groups of 5 channels are formed. Each group of channels is isolated from the next, except for the end portions, so that the current flows through the macroscopic structure in a zigzag path. Each macroscopic structure in the reactor system of the invention is subjected to a current of 200 A and a voltage of approximately 5.5 kW to heat the structured catalyst and hence the gas passing through the structured catalyst, corresponding to an input power of 9899 kW.

The total internal diameter of the reactor system in this configuration may be 3.2 m and the total internal height 5.5 m if the reactor system is cylindrical with spherical heads. In this particular configuration, the macroscopic structures are arranged in a square with a diagonal length of 2.3 m. An inert material is located around the structured catalyst, closing the gap between the insulating material with an internal diameter of 2.5 m and a thickness of 0.35 m.

During the passage of the feed gas through the reactor system, the feed gas is heated by the heat of the structured catalyst, and a steam reforming reaction is carried out to obtain a gaseous product with an outlet temperature of 1236°C. The overall flow rates of the source gas and the gaseous product are lower compared to examples 1 and 4.

Since the gaseous product leaving the reactor system is already at a pressure of 181 bar, it can be fed to, for example, a refinery hydrotreater without further compression. Thus, compressors are not required between the reactor system and the refinery hydrotreater. This greatly reduces the overall cost of the installation with the reactor system according to the invention.

- 26 041025

Table 5

Macroscopic structure size: Edge length [m] 0.53 Height (m) 2.3 Number of macroscopic structures 9 Total volume of structured catalyst [l] 5888 Height/length of the diagonal structured catalyst [-] 1.01 source gas gaseous product T[°C] 500 1236 P [kg/cm ² g] 181.97 181.47 CO2 [nm ³ /h] 86 395 N2 [nm ³ /h] 21 21 CH4 [nm ³ /h] 2116 96 H2 [nm ³ /h] 278 6648 CO [nm ³ /h] 0 1711 H2O [nm ³ /h] 6425 4096 Total flow [nm ³ /h] 8926 12967 AT _paB H,SMR [°C] 10 Power, kWt] 9899 Heat flux [kW/m ² ] 2.2 Volume velocity [nm ³ /m ³ /h] 1516

Example 6

Example 6 refers to a reactor system consisting of a structured catalyst with 78540 channels with a total wall length of each channel in cross section of 0.00628 m and a wall length of 2 m, so the total surface area of the catalyst is 987 m ² . For a reactor system with such a structured catalyst, simulations were performed with varying gas flow through the structured catalyst, while all calculations used gas with the following composition: 8.8% H ₂ , 56.8% H2O, 0.2% N2, 0.1% CO, 2.3% CO2 and 31.8% CH ₄ . In each simulation, a kinetic model was used for steam reforming and water gas shift, and changing the surface energy flux (Q) from the electrically heated structured catalyst to 920°C was performed to control the temperature of the product gas leaving the reactor system containing the structured catalyst. . A kinetic model was used similar to that used by Xu and Froment (J. Xu, GF Froment, Methane steam reforming, methanation and water-gas shift: I. intrinsic kinetics. American Institution of Chemical Engineers Journal, 35:88-96, 1989 ). In FIG. 14 shows the temperature approaching equilibrium conditions along the length of the reactor system at various total flow rates. the figure shows that at low feed gas flow rates (10,000 Nm ³ /h), the temperature approaching equilibrium conditions at the outlet of the reactor system is less than 5°C, because of this, the degree of hydrocarbon conversion is 77%, while at high flow rate (150,000 nm ³ /h), the temperature approaching equilibrium conditions is more than 60°C, which corresponds to a degree of hydrocarbon conversion of only 64%, so the use of hydrocarbons is less efficient. Thus, due to the precise control of the heat flow, the present invention provides control of the temperature approaching equilibrium conditions along the entire length of the reactor system. The general trend for all curves in Fig. 14 is that the temperature for conditions close to equilibrium decreases continuously until pseudo-equilibrium is reached, when heat supply and heat consumption are approximately equal to each other. From this point on, the temperature of approach to equilibrium conditions remains practically constant or slightly increases due to the general increase in the temperature of the reactor system.

Example 7 (comparative example).

Used by SMR with a number of identical pipes. The inner diameter of each pipe is 10 cm and the length is 13 m. The total heat flow to the SMR pipes is adjusted according to an average heat flow value (based on the inner surface area of the pipes) of 90,000 kcal/h/ ^m2 , which corresponds to approximately 105 kW / m ² . Catalyst grains are loaded into each tube. The catalyst grain sizes are adjusted so that the void fraction is 60%. This configuration allows approximately 410 Nm ³ /h of process gas per tube to be processed in the SMR if the feed gas has the following composition: 8.8% hydrogen, 56.8% water, 0.2% nitrogen, 0.1% carbon monoxide, 2.3% carbon dioxide and 31.8% methane.

-

Claims (28)

This allows you to get the following values. Total internal volume of the pipe (volume limited by the inner surface of the pipe and the height of the pipe): 0.1021 m ³ ; the internal volume of the pipe occupied by the catalyst material: 0.0408 m ³ ; total internal volume of the pipe occupied by the catalyst material per unit volume of the internal reactor system: 0.4 m ³ /m ³ ; total amount of energy supplied to the inside of the pipe: 427.4 kW; the amount of energy supplied to the internal space of the pipe per unit internal volume of the pipe: 4186 kW/m ³ ; amount of processed gas per volume of reactor catalyst: 4015 Nm ³ /m ³ /h. Example 8 The reactor system of the present invention is provided. A structured catalyst with a geometric surface area of 800 m ² /m ³ is provided. 95% of the area is ceramic coated with catalytically active material. The thickness of the ceramic coating is 0.1 mm. A power of 9 kW/m ² is applied to the surface of the structured catalyst. This reactor configuration allows the processing of approximately 7700 Nm ³ /m ³ /h of gas relative to the volume of the structured catalyst, if the feed gas has the following composition: 8.8% hydrogen, 56.8% water, 0.2% nitrogen, 0.1% carbon monoxide, 2.3% carbon dioxide and 31.8% methane. This allows you to get the following values. The amount of energy supplied to the structured catalyst per unit volume of the structured catalyst: 7200 kW/m ³ ; total internal volume of the reactor system occupied by the catalyst material per unit volume of the internal reactor system: 0.076 m ³ /m ³ ; amount of processed gas per volume of reactor catalyst: 101315 Nm ³ /m ³ /h. From a comparison with example 7, it can be seen that the internal volume of the reactor system can be significantly more compact. In addition, the reactor system of the present invention does not require the use of a furnace, which greatly reduces the size of the reactor. In addition, compared with the prior art, the amount of the catalytically active material is significantly reduced. CLAIM 1. A reactor system for carrying out steam reforming of a source gas containing hydrocarbons, while the reactor system contains a structured catalyst designed to catalyze the steam reforming of the specified source gas containing hydrocarbons, while the specified structured catalyst includes a macroscopic structure of an electrically conductive material, while on the specified a macroscopic structure is a ceramic coating, while the specified ceramic coating acts as a substrate of the catalytically active material; high-pressure housing, in which the specified structured catalyst is located, while the specified high-pressure housing contains an inlet for supplying the source gas and an outlet for removing the gaseous product, while the inlet is located so that the source gas enters the front of the specified structured catalyst, and the specified gaseous product exits the back of the specified structured catalyst; a heat-insulating layer between said structured catalyst and said pressure vessel; and at least two conductors electrically connected to said structured catalyst and to a power source that is located outside of said pressure vessel, wherein the power source is designed to heat at least a portion of said structured catalyst to a temperature of at least 500° C. by passing an electric current through said macroscopic structure, wherein said at least two conductors are connected to the structured catalyst at a point on the structured catalyst located closer to the front of said structured catalyst than to the back of said structured catalyst, wherein the structured catalyst is configured to directing electric current from one conductor substantially to the back of the structured catalyst and back to the second conductor of said at least two conductors. 2. Reactor system according to claim 1, characterized in that the design pressure of the pressure vessel is in the range of 5-30 bar. 3. Reactor system according to claim 1, characterized in that the design pressure of the pressure vessel is in the range of 30-200 bar, preferably in the range of 80-180 bar. 4. The reactor system according to any one of claims 1 to 3, characterized in that the resistivity of macro- - 28 041025 of the scopic structure is in the range of ^10-5-10-7 Ω-m. 5. Reactor system according to any one of claims 1 to 4, characterized in that each of the at least two conductors passes through the pressure vessel in the fitting in such a way that at least two conductors are electrically isolated from the pressure vessel. 6. The reactor system of claim 5, wherein said pressure vessel has one or more inlets adjacent to or in combination with at least one fitting to allow refrigerant gas to pass through, around, adjacent to, or within the at least one conductor inside said pressure vessel. 7. Reactor system according to any one of claims 1 to 6, characterized in that it further comprises an inner tube between which heat exchange takes place and the structured catalyst, but which is electrically isolated from the structured catalyst, said inner tube being configured to remove gaseous product from the structured catalyst. catalyst in such a way that between the gaseous product entering through the inner tube, heat exchange is carried out with the gas entering through the structured catalyst. 8. Reactor system according to any one of claims 1 to 7, characterized in that the connection between the structured catalyst and said at least two conductors is a mechanical connection, a welded connection, a soldered connection, or a combination thereof. 9. Reactor system according to any one of claims 1 to 8, characterized in that the macroscopic structure is a structure that is made by extrusion and sintering or made by 3D printing and sintering technology. 10. Reactor system according to any one of claims 1 to 9, characterized in that the structured catalyst includes a set of macroscopic structures electrically connected to each other. 11. Reactor system according to any one of claims 1 to 10, characterized in that said structured catalyst has electrically insulating parts configured to increase the length of the main current path between said at least two conductors to a length greater than the longest dimension of the structured catalyst. 12. Reactor system according to any one of claims 1 to 11, characterized in that said structured catalyst has at least one electrically insulating part configured to direct current through said structured catalyst to provide a non-zero value of the current density vector component of the main current path of at least measure for 70% of the length of said structured catalyst, parallel to the length of said structured catalyst. 13. Reactor system according to any one of claims 1 to 12, characterized in that said macroscopic structure has a plurality of parallel channels, a plurality of non-parallel channels and/or a plurality of channels with changing direction. 14. Reactor system according to any one of claims 1 to 13, characterized in that it further comprises a layer of a second catalytic material downstream of said structured catalyst inside said pressure vessel. 15. The reactor system according to any one of claims 12 to 14, characterized in that it further comprises a third catalyst material in the form of catalyst grains, extrudates or pellets, which are loaded into the channels of said structured catalyst. 16. The reactor system according to any one of claims 1 to 15, further comprising a layer of a fourth catalytic material placed inside the pressure vessel and downstream of said structured catalyst. 17. Reactor system according to any one of claims 1 to 16, characterized in that the macroscopic structure material is selected as a material capable of generating a heat flux of 500-50,000 W/m ² by heating the material with resistance. 18. The reactor system according to any one of claims 1 to 17, characterized in that the structured catalyst comprises a first part configured to create a first heat flux and a second part configured to create a second heat flux, the first heat flux being less than the second heat flux. flow, while the first part is in the course of the process before the second part. 19. The reactor system according to any one of claims 1 to 18, characterized in that said reactor system further comprises a control system configured to control the supply of electricity to ensure that the temperature of the gas exiting the pressure vessel is within a predetermined range, and /or to ensure that the degree of conversion of hydrocarbons in the feed gas is in a predetermined range, and/or to ensure that the molar concentration of methane in the dry state is in a predetermined range, and/or to ensure that the equilibrium conditions of the steam reforming reaction are approximated in a predetermined range . 20. Reactor system according to any one of claims 1 to 19, characterized in that in said reactor system the ratio between the equivalent diameter of the horizontal cross-sectional area - 29 041025 structured catalyst and the height of the structured catalyst is in the range 0.1-2.0. 21. Reactor system according to any one of claims 1 to 20, characterized in that the height of the reactor system is 0.5-7 m, more preferably 0.5-3 m. 22. A method for steam reforming a feed gas containing hydrocarbons in a reactor system according to any one of claims 1 to 21, said method comprising the following steps: compressing the source gas containing hydrocarbons to a pressure of at least 5 bar; supplying said compressed feed gas to said pressure vessel through an inlet that is positioned such that said feed gas enters the front of said structured catalyst; providing a steam reforming reaction of the source gas over the structured catalyst and the removal of the gaseous product from the specified pressure vessel, while the specified gaseous product exits the rear of the specified structured catalyst; supplying current through the conductors connecting the power source located outside the specified pressure vessel, and the specified structured catalyst, which allows the transmission of current through the specified macroscopic structure, while heating at least part of the specified structured catalyst to a temperature of at least 500 °C, wherein said at least two conductors are connected to the structured catalyst at a point on the structured catalyst located closer to the front of said structured catalyst than to the back of said structured catalyst, wherein the structured catalyst is configured to direct electric current from one conductor practically to the back of the structured catalyst and back to the second conductor of at least two of these conductors. 23. The method of claim 22, further comprising the step of compressing the feed gas upstream of the pressure vessel to a pressure in the range of 5-30 bar. 24. The method of claim 22 or 23, further comprising the step of compressing said feed gas upstream of said pressure vessel to a pressure in the range of 30-200 bar, preferably in the range of 80-180 bar. 25. The method according to any one of claims 22-24, characterized in that the temperature of the source gas at the feed to the reactor system is in the range of 200-700°C. 26. The method according to any one of claims 22-25, characterized in that the macroscopic structure is heated in such a way that the maximum temperature of the macroscopic structure is in the range of 500-1300°C. 27. The method according to any one of claims 22-26, further comprising the step of supplying refrigerant gas through an inlet in the pressure housing located adjacent to or in combination with at least one fitting, to allow refrigerant gas to pass through, around, adjacent to or inside at least one conductor inside said pressure vessel. 28. The method according to any one of claims 22-27, characterized in that the space velocity, estimated as the gas flow rate relative to the geometric surface area of the structured catalyst, is in the range of 0.6-60 or 700-70000 nm ³ /m ³ /h at estimated as the ratio of gas consumption to the occupied volume of the structured catalyst. -