Method and reactor for producing one or more products

The dynamic gas compression and mixing process addresses carbon deposition and energy inefficiencies in natural gas decomposition, optimizing hydrogen yield and reducing emissions by integrating with a direct carbon fuel cell for efficient, low-cost hydrogen production.

JP7701962B2Active Publication Date: 2025-07-02EKONA POWER INC
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Patent Information

Application Number
JP2023199763
Authority / Receiving Office
JP · JP
Patent Type
Patents
Current Assignee / Owner
Priority Date
2018-12-10
Filing Date
2023-11-27
Publication Date
2025-07-02
Estimated Expiration
2039-12-09

AI Technical Summary

Technical Problem

Conventional methods for natural gas decomposition, such as steam methane reforming and pyrolysis, face challenges including high CO2 emissions, costly cleanup processes, carbon deposition on reactor surfaces, and high production costs due to energy inefficiencies and carbon accumulation, which complicate the process and increase environmental impact.

Method used

A dynamic gas compression and mixing process is used to pyrolyze natural gas, combining a mixing chamber with a combustion chamber to transfer energy efficiently, minimize carbon fouling through pressure waves, and recover solid carbon for secondary use, integrating with a direct carbon fuel cell to produce low-cost 'clean' hydrogen.

Benefits of technology

The process optimizes hydrogen yield, minimizes carbon emissions, and recovers solid carbon for electricity generation, achieving low-cost, efficient hydrogen production with reduced environmental impact.

✦ Generated by Eureka AI based on patent content.

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Abstract

To provide a method and a system for producing one or more products by way of decomposing feedstock gas such as natural gas.SOLUTION: Feedstock gas, such as natural gas, is introduced into a mixing chamber. Combustible gas is introduced into a combustion chamber, for example simultaneously with the introduction of the feedstock gas. Thereafter, the combustible gas is ignited so as to cause the combustible gas to flow into the mixing chamber via one or more fluid flow paths between the combustion chamber and the mixing chamber, and to mix with the feedstock gas. One or more products are produced by the mixing of the combustible gas with the feedstock gas.SELECTED DRAWING: Figure 5
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Description

Technical Field

[0001] The present invention relates to a method for producing one or more products through the decomposition of a feed gas such as natural gas, for example, and a related reactor.

Background Art

[0002] The chemical decomposition of natural gas (CH4) refers to the separation of the natural gas into its components, carbon (C) and hydrogen (H2). Conventional hydrogen production methods such as steam methane reforming (SMR) result in significant dilute CO2 emissions. This may require costly post-reform cleanup (purification) for separation. As a result, SMR produces approximately 8 to 10 tons of CO2 per ton of H2 produced. Adding CO2 cleanup to the SMR flue gas stream is generally costly unless the penalty for carbon dioxide emissions increases up to the break-even point.

[0003] There are other methods of pyrolysis for producing hydrogen and solid carbon, such as thermal pyrolysis, liquid metal pyrolysis, plasma pyrolysis, etc. These processes are generally tuned to maximize the production of solid carbon for the related carbon market and are widely used in these industries.

[0004] The pyrolysis of natural gas is typically a steady-flow process at constant pressure, according to which the natural gas is heated until it reaches the temperature required to initiate the formation of hydrogen and carbon. At this point, the temperature is maintained for a predetermined time to complete the equilibrium reaction. As the temperature increases, assuming a constant pressure of 1 ATM, the time required for methane conversion decreases (shown in Figure 1 - a figure obtained from the reaction rate model of the homogeneous pyrolysis of methane and ethane, Maryam Younessi-Sinaki, Edgar A. Matida, Feridun Hamdullahpur, Carleton University, Department of Mechanical and Aerospace Engineering, 1125 Colonel By Drive, Ottawa, ON K1S 5B6, Canada, the entire document of which is incorporated herein by reference).

[0005] In such a steady-flow reactor, the carbon formed tends to deposit on the surface of the reactor and eventually becomes very thick, impairing the performance of the reactor. Mechanical scraping processes or burning the carbon from the surface by introducing air into the reactor are two common means of cleaning the reactor. Mechanical scraping is difficult to implement and may not be able to remove hard carbon deposits. Burning the carbon with air produces significant CO2 emissions, which is undesirable. Therefore, first and foremost, it is highly desirable not to form carbon on the surface, and it is highly desirable to send the generated carbon to a downstream process.

[0006] Furthermore, to reduce the size of the reactor, a shorter reaction time is required, which requires high temperatures and special materials that are very expensive. To overcome this, a catalyst that has the effect of lowering the reaction temperature is added to the reactor. However, carbon deposition also occurs on the surface of the catalyst, which deactivates the catalyst over time and requires a catalyst reactivation process or replacement. All of these options are costly and complicate the process.

[0007] Liquid media reactors such as liquid metal reactors involve heat treatment where natural gas is bubbled through a column of a high-temperature liquid such as liquid metal or liquid salt. Since this is a constant-pressure steady-flow process, the same temperature vs. time reaction rate as described above applies. The advantage of this process is that the hydrogen produced bubbles out outside the upper part of the reactor column, carbon floats on the surface of the liquid medium, and theoretically can be scooped out, thus simplifying the separation of hydrogen and carbon. In some examples, liquid metal alloys that provide a catalytic effect to lower the reaction temperature have been identified. However, in all cases, carbon accumulation at the upper part of the reactor remains a problem, and the use of molten media adds complexity, material issues, and cost to the reactor.

[0008] In most heat treatments, the energy required to heat the reactor to maintain the process is usually supplied by burning excess natural gas with air. This flue gas releases CO2 into the atmosphere and contributes to global warming. In some cases, excess carbon deposition and / or hydrogen can be used to provide the heat of reaction.

[0009] Plasma reactors pass natural gas at a constant pressure through a high-temperature plasma generated electrically. The plasma can be generated, for example, by using electrodes or microwaves. In these reactors, carbon accumulation can still be a problem, but since the high-temperature plasma is confined to a very small area, it is not as much of a problem as in thermal reactors. Unlike thermal reactors, plasma reactors rely only on electricity as the energy input. Compared to thermal systems, the cost of electricity for the input energy is much higher than that of natural gas, resulting in much higher production costs for hydrogen and methane.

[0010] Therefore, in the art, there is a need for a type of natural gas decomposition process that uses thermal energy with lower capital costs and is less affected by the carbon accumulation problem. Summary of the Invention

[0011] Overall, the present invention relates to (but is not limited to) the decomposition of natural gas into its components, carbon (C) and hydrogen (H2), and uses dynamic gas compression and mixing to generate the pressures and temperatures required to pyrolyze natural gas. The goal of the process is to optimize the process for hydrogen yield, minimize carbon greenhouse gas emissions, and recover solid carbon as a secondary value stream. When combined with a direct carbon fuel cell (DCFC), the carbon product can be used to generate electricity and can also be used to produce a pure product stream of CO2 suitable for sequestration (see Figure 2). As a result, low-cost "clean" hydrogen production is achieved.

[0012] According to a first aspect of the present invention, there is provided a method of producing one or more products, comprising the steps of introducing a feed gas containing one or more gases into a mixing chamber, introducing a combustible gas containing one or more gases into a combustion chamber, and then igniting the combustible gas and causing the combustible gas to flow into the mixing chamber through one or more fluid flow paths between the combustion chamber and the mixing chamber to mix with the feed gas, wherein energy is transferred from the combustible gas to the feed gas, thereby producing one or more products.

[0013] The introduction of the feed gas and the combustible gas can be done such that the feed gas does not substantially mix with the combustible gas, or hardly mixes with the combustible gas, or only mixes to an ignorable extent, before the ignition step.

[0014] The method may further comprise the step of stopping further production of the one or more products.

[0015] The method may further comprise the step of preheating the feed gas before the step of introducing the feed gas into the mixing chamber.

[0016] The method may further comprise a step of preheating the combustible gas before the step of introducing the combustible gas into the combustion chamber.

[0017] The ratio of the volume of the mixing chamber to the volume of the combustion chamber may be less than about 10:1, or may be equal to about 10:1.

[0018] The ratio of the length of the mixing chamber to the diameter of the mixing chamber may be less than about 30:1, or may be equal to about 30:1.

[0019] The source gas may include natural gas. The source gas may include a mixture of natural gas and recycled gas. The recycled gas may include one or more of natural gas, hydrogen, carbon monoxide, and carbon dioxide.

[0020] The combustible gas may include an oxidizing agent. The oxidizing agent may include one or more of oxygen and air. The combustible gas may include a mixture of CH4 and O2. The combustible gas may include a mixture of recycled gas and the oxidizing agent. The recycled gas may include one or more of natural gas, hydrogen, carbon monoxide, and carbon dioxide.

[0021] The combustible gas may be introduced into the combustion chamber simultaneously with the introduction of the source gas into the mixing chamber.

[0022] The combustible gas may be introduced into the combustion chamber at a pressure equal to the pressure at which the source gas is introduced into the mixing chamber.

[0023] The one or more products may include one or more of hydrogen and carbon.

[0024] The one or more products may include one or more of hydrogen and carbon monoxide.

[0025] The one or more products may include one or more of hydrogen, nitrogen, and carbon. Hydrogen and nitrogen may be used for ammonia production.

[0026] The step of stopping further production of the one or more products may include the step of reducing the pressure in the mixing chamber. The pressure in the mixing chamber can be reduced sufficiently rapidly, for example by at least 50% in less than 1 second, to suppress carbon fouling of the mixing chamber.

[0027] The pressure wave generated by the combustion of the combustible gas may suppress carbon fouling of the mixing chamber.

[0028] The energy can be transferred from the combustible gas to the feed gas using dynamic compression and mixing of the gases.

[0029] The temperature in the combustion chamber after ignition and before mixing with the feed gas of the combustible gas can be, for example, ~90 ATM and ~3700 K when using pure O2 as oxidation and recycled gas as the combustible gas.

[0030] After mixing the combustible gas with the feed gas and before the one or more products are produced, at least a portion of the mixture of the feed gas and the combustible gas can be transferred to a third chamber. Thus, the combustion chamber and the mixing chamber can be replenished with fresh combustible gas and feed gas while the user waits for the one or more products to be produced in the third chamber.

[0031] According to a further aspect of the present invention, there is provided a raw material gas reactor comprising a mixing chamber, a combustion chamber, a valve for controlling the flow of gas into and out of the mixing chamber and the combustion chamber, an igniter, and one or more controllers configured to perform the following method. The method includes controlling the valve to introduce a raw material gas containing one or more gases into the mixing chamber, controlling the valve to introduce a combustible gas containing one or more gases into the combustion chamber, and then controlling the igniter to ignite the combustible gas so that the combustible gas flows into the mixing chamber through one or more fluid flow paths between the combustion chamber and the mixing chamber and is mixed with the raw material gas. Energy is transferred from the combustible gas to the raw material gas, thereby producing one or more products. The raw material gas reactor is characterized by this.

[0032] The introduction of the raw material gas and the combustible gas may be performed so that the raw material gas does not substantially mix with the combustible gas.

[0033] The method may further include controlling the valve to stop further production of the one or more products.

[0034] The combustion chamber may be disposed within the mixing chamber. The combustion chamber may be offset from the longitudinal axis of the mixing chamber.

[0035] The combustion chamber may be disposed outside the mixing chamber.

[0036] The combustion chamber may have one or more openings formed therein.

[0037] The raw material gas reactor may include any of the features described in connection with the first aspect of the present invention.

[0038] According to a further aspect of the present invention, there is provided a raw material gas reactor comprising a mixing chamber, a combustion chamber having one or more openings formed therein, a valve for controlling the flow of gas into and out of the mixing chamber and the combustion chamber, and an igniter, wherein the one or more openings provide one or more fluid flow paths from the combustion chamber to the mixing chamber.

[0039] The raw material gas reactor may include any of the features described in relation to the first aspect of the present invention.

[0040] The step of controlling the valve may include the step of controlling the opening and / or closing of individual valves. Alternatively or additionally, the step of controlling the valve may include the step of rotating the valve with respect to the reactor (for example, using a motor).

[0041] According to a further aspect of the present invention, there is provided a system comprising a plurality of raw material reactors, each reactor having a mixing chamber, a combustion chamber, and an igniter, a valve for controlling the flow of gas into and out of the plurality of mixing chambers and the plurality of combustion chambers, and one or more controllers configured to perform the following method in each reactor, the method including controlling the valve to introduce a raw material gas containing one or more gases into the mixing chamber, controlling the valve to introduce a combustible gas containing one or more gases into the combustion chamber, and then controlling the igniter to ignite the combustible gas so that the combustible gas flows into the mixing chamber through one or more fluid flow paths between the combustion chamber and the mixing chamber and is mixed with the raw material gas, wherein energy is transferred from the combustible gas to the raw material gas, thereby producing one or more products, and in a given reactor, the method is performed out of phase with at least one other reactor of the plurality of reactors.

[0042] In each reactor, the introduction of the raw material gas and the combustible gas can be made such that the raw material gas is not substantially mixed with the combustible gas.

[0043] In each reactor, the method may further include the step of controlling the valve to stop further production of the one or more products.

[0044] The plurality of reactors may be arranged radially around a central axis, and the system may further include a rotor configured to rotate the plurality of reactors around the central axis with respect to a valve assembly including the valve, or to rotate the valve assembly including the valve around the central axis with respect to the plurality of reactors. Thereby, the valve assembly can be rotated while the plurality of reactors are stationary, or the valve assembly can be stationary while the plurality of reactors are rotating. In some embodiments, the valve assembly and the plurality of reactors may be rotated simultaneously.

[0045] The step of controlling the valve may include the step of controlling the opening and / or closing of individual valves. Alternatively or additionally, the step of controlling the valve may include the step of rotating the valve with respect to the plurality of reactors (e.g., using a motor).

[0046] The system may include any of the features described in connection with the first aspect of the present invention.

[0047] In a further aspect of the present invention, there is provided a system comprising one or more of the aforementioned reactors and one or more fuel cells coupled to the one or more reactors and configured to receive carbon produced from the mixing of a raw material gas of a combustible gas.

[0048] The system may include any of the features described in connection with the first aspect of the present invention.

[0049] Embodiments of the present invention will be described in detail with reference to the accompanying drawings.

Brief Description of the Drawings

[0050]

Figure 1

[0051]

Figure 2

[0052]

Figure 3

[0053]

Figure 4A

Figure 4B

[0054]

Figure 5

[0055]

Figure 6

[0056]

Figure 7

[0057]

Figure 8

[0058]

Figure 9

[0059]

Figure 10

[0060]

Figure 11

[0061]

Figure 12

[0062]

Figure 13

[0063]

Figure 14

DETAILED DESCRIPTION OF THE INVENTION

[0064] The present invention aims to provide an improved method and reactor for producing one or more products. Although various embodiments of the present invention are described below, the present invention is not limited to these embodiments, and variations of these embodiments can fully fall within the scope of the present invention, which should only be limited by the appended claims.

[0065] As used in the claims and / or the specification, the term "a" or "an" when used with the terms "comprising" or "including" may mean "one", but unless the context clearly states otherwise, it is also consistent with the meanings of "one or more", "at least one", and "one or more than one". Similarly, the term "another" may mean at least a second or more, unless the context clearly states otherwise.

[0066] As used herein, the terms "coupled", "coupling", or "connected" may have several different meanings depending on the context in which the term is used. For example, the terms "coupled", "coupling", or "connected" may have a mechanical or electrical meaning. For example, as used herein, the terms "coupled", "coupling", or "connected" may indicate that two elements or devices are directly connected to each other, or are connected to each other through one or more intermediate elements or devices via electrical elements, electrical signals, mechanical elements, etc., depending on the specific context. The term "and / or" as used herein, when used in relation to a list of items, means any one or more of the items constituting the list.

[0067] As used herein, references to "about ## (a numerical value)" or "substantially ## (a numerical value)" mean within + / - 10% of that numerical value.

[0068] Overall, embodiments of the present invention describe an ultra-rich pulse pyrolysis process for producing hydrogen-rich gas and / or carbon products from natural gas feedstocks. For large-scale hydrogen production, the process can compete with SMR.

[0069] According to embodiments of the present invention, the use of an unsteady-state constant-volume pulse reaction process for producing hydrogen and carbon products from natural gas-based feedstocks is described. A separate chamber for the combustible gas and the oxidizer provides the energy for the reaction, and this energy is directly transferred to the feedstock mixing chamber by the dynamic compression of the gas and rapid mixed thermal energy exchange through direct contact. In the following description, air is used as the oxidizer. However, other oxidizers such as pure oxygen can also be used in the process. Further, the feedstock gas and the combustible gas can include the same gas or gas mixture, or can include different gases or gas mixtures. In some embodiments, the combustible gas can include a recycle gas mixture.

[0070] The reactor includes a mixing chamber and a combustion chamber. These chambers are connected via several passages that are always open. In some embodiments, the reactor includes a perforated tube (combustion chamber) within a larger solid tube (mixing chamber) (see FIGS. 3 and 4A). In other embodiments, the combustion chamber can be external to the mixing chamber (as shown in FIG. 4B). External valves provide the feedstock gas, oxidizer, and combustible gas (shown as CH4), as well as the exhaust hydrogen, carbon, and other gases produced during the reaction.

[0071] Referring to FIG. 5, at the start of the cycle, the mixing chamber is filled with the products of the previous reaction cycle. The mixing chamber is filled with a mixture of the products of the feed reaction and a portion of the products of the combustion reaction. The combustion chamber is mainly filled with the products of the combustion reaction. In step 500, fresh feed gas and possibly some recycled product gas are introduced into the mixing chamber, moving the products of the previous cycle from the ends of the mixing chamber. At the same time, a combustible gas / air mixture is introduced into the combustion chamber, moving the products of combustion from the ends of the combustion chamber. In step 502, all inlet and outlet valves are closed, creating a closed volume. Next, in step 504, the gas in the combustion chamber is ignited, resulting in an increase in pressure and temperature in the combustion chamber. In step 506, the passage between the combustion chamber and the mixing chamber is allowed to let combustible gas products enter the mixing chamber, thereby compressing the feed gas and raising their pressure and temperature. Also, the hot combustion chamber gas products mix with the feed gas, thereby transferring their thermal energy to the feed gas and further raising their temperature. The resulting temperature and pressure of the feed gas cause a reaction to occur. In step 508, the reaction is allowed to proceed for a certain period, the desired reaction is completed, and the desired product is generated. In step 510, the pressure in the mixing chamber is rapidly reduced by discharging the product into an external volume (not shown). The combustion product gas remaining in the combustion chamber can be discharged together with the mixing chamber gas or separately through a dedicated port. The pressure drop in the mixing chamber reduces the temperature and stops or terminates (quenches) the reaction. This rapid depressurization and expansion also has the desirable effect of removing solid reaction products such as carbon from the walls of the reactor. Further, the pressure wave generated from the combustion can strip carbon deposits from the walls of the reactor.

[0072] When the raw material gas and the combustible gas are premixed, the mixture may be too rich (too concentrated) and thus may not ignite. Therefore, the mixing chamber and the combustion chamber are separated from each other before ignition, so that no mixing occurs between the raw material gas and the combustible gas, or preferably only very little mixing occurs.

[0073] A plurality of reactor systems can be bundled and operated in a slightly phase-shifted state with respect to each other to generate a continuous flow into and out of the reactor system. As shown in FIG. 6, the valve may be of a stationary type or a rotary type. In some embodiments, the reactor can be rotated and the valve can maintain a stationary state (see FIG. 7 modified from FIG. 2 of "A Wave Rotor Design Method with Three Steps Including Experimental Verification", Chan Shining et al., Journal of Engineering for Gas Turbines and Power, December 2017. The entire document is incorporated herein by reference).

[0074] To enable the reactor to operate effectively, various parameters can be adjusted. The raw material gas can be preheated to just below the temperature at which the reaction starts before being introduced into the mixing chamber. Typical temperatures are in the range of 600K to 1000K, depending on the components of the raw material gas and the operating pressure.

[0075] Furthermore, the mixture of combustible gas / oxidant to be introduced can also be preheated before entering the combustion chamber. Typical temperatures are in the range of 400K to 700K, depending on the combustible gas used. Preheating the combustible gas / oxidant mixture can improve the efficiency of the process, and more combustion energy is transferred to the reactants rather than being used to heat the combustion products.

[0076] The volume ratio between the mixing chamber and the combustion chamber should be set such that an exact amount of energy contained within the combustion chamber is provided to the mixing chamber to produce the desired products. Also, there should be sufficient combustible gas products entering the mixing chamber to provide effective mixing. Generally, a volume ratio of less than 10:1 is desired. When using air as the oxidizer, nitrogen can be beneficial as a non-reactive gas that promotes a lower volume ratio and increases mixing. When using pure oxygen as the oxidizer, another gas such as CO2 can provide the same advantages as nitrogen when using air as the oxidizer. Introducing additional CO2 into the mixture of combustible gases can result in an increase in the amount of solid carbon produced.

[0077] The length-to-diameter ratio is important for obtaining efficient energy transfer from the combustion chamber to the mixing chamber. Short and large-diameter reactors tend to have insufficient mixing, while long and narrow reactors encounter difficulties in introducing the feed gas and combustible gas into the reactor along its length. Generally, a length-to-diameter ratio of less than 30:1 is desirable.

[0078] According to some embodiments, the reactor uses methane (or natural gas) as the feed gas in addition to some recycled product gas, and a mixture of recycled gas / oxidizer as the combustible gas. The reactor can be designed and operated to maximize the production of hydrogen and solid carbon in the flow of reaction products. The reactor can include a combustion chamber, which is a perforated tube, inside the mixing chamber. The perforated combustion chamber can be offset from the center of the mixing chamber, can be coupled to the wall of the mixing chamber, and can provide structural integrity and support as seen in FIG. 13. The volume ratio of the mixing chamber / combustion chamber can be 10:1 or less, and the length-to-diameter ratio can be 10:1. In some embodiments, the volume ratio of the mixing chamber / combustion chamber can be about 6:1, and in some embodiments, the volume ratio of the mixing chamber / combustion chamber can be about 3.5:1.

[0079] As shown in FIG. 14, a plurality of reaction tubes can be arranged with an external rotating valve that provides all the flows and sequencing of the feed gas, combustible gas, and reaction products. Separate ports may discharge the combustion products of the combustion chamber.

[0080] The reactor can be operated at a sufficiently high pressure such that the hydrogen obtained can be purified using standard pressure swing absorption techniques. According to some embodiments, product gases such as unreacted methane (CH4), carbon monoxide (CO), and some hydrogen are recycled and mixed with more methane to produce a feed gas mixture to the reactor. The combustible gas mixture includes the recycled gas mixture and pure oxygen, in addition to the CO2 removed from the CO2 removal system (in the case of an air blown reactor). In some embodiments, the recycled gas mixture flowing into both the combustion chamber and the mixing chamber contains CO2 in addition to CH4, CO, and H2. The feed gas mixture and the combustible gas mixture are each preheated to ~900K and ~600K from the thermal energy recovered from the reactor product stream via a multi-stream heat exchanger. In an alternative embodiment, the volume ratio of the mixing chamber / combustion chamber is 3.5:1 and a methane (or natural gas) / air mixture is used for the combustible gas.

[0081] Next, a detailed description of embodiments of the present invention is provided.

[0082] Referring to FIG. 8, the combustible gas 10 and the oxidant gas 20 enter a combustion mixture adjustment control system 30, which adjusts the combustible gas mixture 31 to the correct temperature and pressure required by the chamber 60. The feed gas 40 and the recycled gas mixture 91 enter a feed mixture adjustment control system 50, which adjusts the feed mixture 51 to the correct temperature and pressure required by the chamber 60. In some embodiments, the recycled gas mixture is not available and only the feed gas 40 enters the feed mixture adjustment control system 50.

[0083] The chamber 60 is a constant volume (constant volume) device that uses the combustion energy from the adjusted combustible gas mixture 31 to raise the pressure and temperature of the adjusted raw material mixture 51 to the reaction preparation level. A combustion product gas mixture 67 mainly composed of the combustion products of the adjusted combustible gas mixture 31 that has been combusted can be discharged from the chamber 60. The gas mixture 61 ready for reaction enters the reactor 70 and remains there until the gas mixture is converted into a reaction product mixture 71 by a constant volume endothermic reaction. The constant volume reaction is an unsteady process, operates in batch mode, and requires control of the flow timing. This is achieved by flow control in the adjustment systems 30, 50, and the separation control system 80.

[0084] The reaction product mixture 71 enters the product separation control system 80, and the product separation control system 80 stops the reaction in the reactor 70 by reducing the pressure and temperature of the desired reaction product mixture 71, and separates and / or purifies the individual product components 81, 82, the unwanted product 83, and the recycle gas mixture 84. The recycle gas mixture 84 enters the pre-adjusted recycle gas system 90, and in the pre-adjusted recycle gas system 90, the recycle gas mixture 84 is pre-adjusted to the desired temperature and pressure and flows to the raw material mixture adjustment control system 50.

[0085] In some embodiments, the combustible gas 10 and the raw material gas 40 are natural gas, and the oxidant gas 20 is air. The desired reaction in the reactor 70 is generally methane pyrolysis given by the following equation.

[0086] CH4 (methane) + energy → C (carbon) + 2H2 (hydrogen)

[0087] The individual product 81 is hydrogen gas, the individual product 82 is carbon, and the unwanted product 83 is mainly carbon dioxide, nitrogen, and water. The recycle gas mixture 84 mainly consists of unreacted natural gas, hydrogen, nitrogen, and carbon monoxide.

[0088] The system of FIG. 9 is similar to that of FIG. 8, except that the chamber 60 and the reactor 70 are coupled within the constant volume reactor 62.

[0089] FIG. 10 is similar to FIG. 9, except that a portion of the recycle mixture 84 conditioned by the pre-conditioning recycle gas system 90 is sent to the combustible gas conditioning control system 30 to offset the required amount of the combustible gas 10.

[0090] FIG. 11 shows a cross-sectional view of the chamber 60 or the constant volume reactor 62. In this description, it shows the constant volume reactor 62.

[0091] The constant volume reactor 62 includes a combustion volume 65 contained within a combustion chamber 63. The combustion chamber 63 is surrounded by a reactor volume 64 contained within a reactor chamber 68. A plurality of passages 66 connect the combustion volume 65 to the reactor volume 64. Although the combustion chamber 63 is shown at the center of the reactor chamber 68, the combustion chamber 63 can be disposed anywhere within the reactor chamber 68, including positions in contact with the outer wall 69 of the reaction chamber 68.

[0092] The conditioned combustible gas mixture 31 enters the combustion chamber 63 through the combustible gas mixture valve 32 and the passage 33, and moves the combustion product gas mixture 67 present within the combustion volume 65 out of the reactor 62 via the passage 74 and the combustion product valve 75. The conditioned feed gas mixture 51 enters the mixing chamber 68 through the feed gas mixture valve 52 and the passage 53, and moves the desired reaction product mixture 71 present within the reactor volume 64 out of the reactor 62 via the passage 73 and the product valve 72. Both the conditioned combustible gas mixture 31 and the conditioned feed gas mixture 51 can enter the constant volume reactor 62 simultaneously at the same pressure, such that there is little mixing through the passage 66.

[0093] Once substantially all of the combustible gas mixture 67 and the desired product mixture 71 have been transferred from the reactor 62, the combustion product valve 75 and the product valve 72 are closed. When the desired reactor pressure is reached, the combustible gas mixture valve 32 and the feed gas mixture valve 52 are closed, creating a closed volume within the reactor 62. The igniter 100 generates an ignition energy 101 that permits the combustible gas mixture 31 within the combustion chamber 63 to combust in an exothermic reaction, producing a combustion product gas mixture 67 at high temperature and pressure. Due to the resulting pressure differential between the combustion chamber 63 and the mixing chamber 68, a portion of the combustible gas mixture 67 enters the reactor volume 64, compressing the feed gas mixture 51 to a higher pressure. At the same time, this portion of the hot combustible gas mixture 67 mixes and heats the feed gas mixture 51 by conduction, convection, and radiation. The feed gas mixture 51 is now in a high temperature and high pressure state, creating the conditions for an endothermic reaction to occur. The constant volume reactor 62 is maintained as a closed volume until the endothermic reaction has proceeded long enough to produce the desired product mixture 71. When this state is reached, the product valve 72 and the combustion product valve 75 are opened, which reduces the pressure and temperature and stops the endothermic reaction. Thereafter, the above process is repeated.

[0094] Figure 12 shows an embodiment of the chamber 60 or the constant volume reactor 62 with the combustion chamber 63 external to the mixing chamber 68. The combustion volume 65 is connected to the reactor volume 64 via a plurality of passages 68. A plurality of igniters may be positioned along the combustion chamber 63 and may generate specific combustion conditions as required. If the combustion chamber 63 is positioned adjacent to the reactor chamber wall 69, the plurality of igniters may be disposed within the constant volume reactor 62 of FIG. 11.

[0095] Figure 13 shows an isometric view of an embodiment of the chamber 60 or the constant volume reactor 62 in which the combustion chamber 63 is directly coupled to the reactor chamber wall 69 of the reactor chamber 68. Directly coupling the combustion chamber 63 to the reactor chamber wall 69 provides structural support and alignment to the combustion chamber 63 and creates an essentially one-piece chamber 60 or constant volume reactor 62.

[0096] To create a quasi- or semi-continuous flow system, a plurality of chambers 60 or constant volume reactors 62 can be arranged together and each chamber or reactor can be operated with a phase shift so as to go through different parts of the process described in FIG. 11.

[0097] FIG. 14 shows an embodiment of a multi-tube reactor 110. The numerous individual constant volume reactors 62 shown in FIG. 14 are arranged in a circle. The adjusted combustible gas mixture 31 enters the multi-tube reactor 110 into the plenum 35 through the passage 34. The adjusted feed gas mixture 51 enters the multi-tube reactor 110 into the plenum 55 through the passage 54. The timing of the adjusted combustion gas mixture and the adjusted feed gas mixture entering the multi-tube reactor 110 is controlled by an inlet rotary valve 120 which is part of a rotary valve assembly 121. The inlet rotary valve 120 performs the same functions as the combustible gas mixture valve 32, passage 33, feed gas mixture valve 52, and passage 53 described in FIG. 11. The timing of the combustion product gas mixture 67 and the desired product mixture 71 exiting the multi-tube reactor 110 is controlled by an outlet rotary valve 122 which is part of a rotary valve assembly 121. The outlet rotary valve 122 performs the same functions as the combustion product valve 72, passage 73, feed product valve 75, and passage 74 described in FIG. 11.

[0098] The combustion product gas mixture 67 from each constant volume reactor 62 is collected in a combustion product plenum 123 and distributed out of the multi-tube reactor 110 through the passage 125. The product mixture 71 from each constant volume reactor 62 is collected in a product plenum 124 and distributed out of the multi-tube reactor 110 through the passage 126.

[0099] The present invention has mainly been presented in the context of the decomposition of a feed gas, but the present invention extends to other methods of producing one or more products from a feed gas. For example, syngas (H2 and CO) can be produced by adjusting one or more parameters of a process in which a combustible gas reacts with (in addition to being mixed with) the feed gas. For example, the ratio of oxidant to recycle gas in the combustible gas can be increased, and the pressure and temperature of the combustible gas immediately after ignition can be increased, thereby inducing an appropriate reaction between the combustible gas and the feed gas.

[0100] The present invention has been described in connection with specific embodiments, but it is to be understood that the present invention is not limited to these embodiments and that changes, modifications, and variations of these embodiments can be made by those skilled in the art without departing from the scope of the present disclosure. Further, it is contemplated that any aspect or any part of any embodiment discussed herein can be implemented or combined with any other aspect or any part of any other embodiment discussed herein.

Claims

1. A method for decomposing a raw material gas in a raw material gas reactor, comprising: introducing the raw material gas into a mixing chamber of the raw material gas reactor; introducing a combustible gas into a combustion chamber of the raw material gas reactor; burning the combustible gas in the combustion chamber to form one or more combustion product gases, wherein the one or more combustion product gases flow into the mixing chamber and mix with the raw material gas, and as a result of the mixing of the one or more combustion product gases with the raw material gas, energy is transferred from the one or more combustion product gases to the raw material gas, thereby causing a chemical reaction for decomposing the raw material gas to produce one or more reaction products; extracting a stream of the mixed product having the one or more reaction products and unreacted raw material gas from the mixing chamber; recycling at least a portion of the stream of the mixed product containing at least a portion of the unreacted raw material gas back to the raw material gas reactor; and the combustion chamber is connected to the mixing chamber. A method characterized by the above.

2. The stream of the mixed product contains carbon, and the method further comprises separating at least some of the carbon from the stream of the mixed product. The method according to claim 1, characterized by the above.

3. The stream of the mixed product contains hydrogen, and the method further comprises separating at least some of the hydrogen from the stream of the mixed product. The method according to claim 1 or 2, characterized by the above.

4. The step of separating at least some of the hydrogen comprises using pressure swing absorption. The method according to claim 3, characterized by the above.

5. The stream of the mixed product contains carbon and hydrogen, and the step of recycling at least a portion of the stream of the mixed product comprises separating at least some of the carbon and at least some of the hydrogen from the stream of the mixed product to form a recycle gas mixture; and recycling the recycle gas mixture back to the raw material gas reactor. The method according to any one of claims 1 to 4, characterized by the above.

6. The step of recycling the recycle gas mixture comprises a step of adjusting the recycled gas mixture to a desired temperature and pressure; a step of recycling the adjusted recycled gas mixture to the raw material gas reactor; The method according to claim 5, characterized by comprising the above.

7. The step of recycling the recycled gas mixture comprises: a step of mixing a first part, which is a part of the recycled gas mixture, with an oxidizing agent; a step of mixing a second part, which is another part of the recycled gas mixture, with the source of the raw material gas; The method according to claim 5 or 6, characterized by comprising the above.

8. The sum of the first part and the second part is 1 The method according to claim 7, characterized by this.

9. The step of recycling the mixture comprises: a step of introducing the mixture of the oxidizing agent and the first part of the recycled gas mixture into the combustion chamber; a step of introducing the mixture of the raw material gas and the second part of the recycled gas mixture into the mixing chamber; The method according to claim 7 or 8, characterized by comprising the above.

10. The step of introducing the mixture of the oxidizing agent and the first part of the recycled gas mixture into the combustion chamber comprises: a step of adjusting the mixture of the oxidizing agent and the first part of the recycled gas mixture to a desired temperature and pressure; a step of introducing the adjusted mixture into the combustion chamber; The method according to claim 9, characterized by comprising the above.

11. The step of introducing the mixture of the raw material gas and the second part of the recycled gas mixture into the mixing chamber comprises: a step of adjusting the mixture of the raw material gas and the second part of the recycled gas mixture to a desired temperature and pressure; a step of introducing the adjusted mixture into the mixing chamber; The method according to claim 9 or 10, characterized by comprising the above.

12. The step of burning the combustible gas includes a step of igniting the combustible gas The method according to any one of claims 1 to 11, characterized by this.

13. The raw material gas is decomposed in a reaction process with a constant volume The method according to any one of claims 1 to 12, characterized by this.

14. Before burning the combustible gas in the combustion chamber, in order to generate a closed volume, a step of closing all of the inlet valve and the outlet valve of the raw material gas reactor The method according to any one of claims 1 to 13, further comprising the above.

15. A raw material gas reactor having a mixing chamber, a combustion chamber connected to the mixing chamber, and at least one igniter; A valve for controlling the flow of gas into and out of the mixing chamber and the combustion chamber; A controller; Comprising; The controller; Controls the valve to introduce raw material gas into the mixing chamber; Controls the valve to introduce combustible gas into the combustion chamber; Controls the at least one igniter to burn the combustible gas in the combustion chamber to form one or more combustion product gases, the one or more combustion product gases flow into the mixing chamber and mix with the raw material gas, and as a result of the mixing of the one or more combustion product gases with the raw material gas, energy is transferred from the one or more combustion product gases to the raw material gas, thereby causing a chemical reaction to decompose the raw material gas to produce one or more reaction products; Controls the valve to extract a stream of the mixed product having the one or more reaction products and unreacted raw material gas from the mixing chamber; Controls the valve to recycle at least a portion of the stream of the mixed product containing at least a portion of the unreacted raw material gas back to the raw material gas reactor Is operable to A system characterized by this.

16. The stream of the mixed product contains carbon and hydrogen, The system further includes a carbon separator and a hydrogen separator for separating at least some of the carbon and at least some of the hydrogen from the stream of the mixed product to form a recycle gas mixture, The controller is further operable to control the valve to recycle the recycle gas mixture back to the raw material gas reactor A system according to claim 15, characterized by this.

17. The controller further; Mixes a first portion, which is part of the recycle gas mixture, with an oxidant; Mixes a second portion, which is another part of the recycle gas mixture, with the source of the raw material gas; Recycles the mixture of the oxidant and the first portion of the recycle gas mixture, and the mixture of the raw material gas and the second portion of the recycle gas mixture, back to the raw material gas reactor; Is operable to control the valve to The system according to claim 16, characterized in that...

18. The sum of the first part and the second part is 1 The system according to claim 17, characterized in that...

19. The controller further introduces a mixture of the oxidant and the first part of the recycle gas mixture into the combustion chamber, introduces a mixture of the raw material gas and the second part of the recycle gas mixture into the mixing chamber and is operable to control the valve so as to... The system according to claim 17 or 18, characterized in that...

20. The system further comprises a combustion mixture adjustment control system for adjusting a mixture of the oxidant and the first part of the recycle gas mixture to a desired temperature and pressure, and the controller further introduces the adjusted mixture into the combustion chamber and is operable to control the valve so as to... The system according to claim 19, characterized in that...

21. The system further comprises a raw material mixture adjustment control system for adjusting a mixture of the raw material gas and the second part of the recycle gas mixture to a desired temperature and pressure, and the controller further introduces the adjusted mixture into the mixing chamber and is operable to control the valve so as to... The system according to claim 19 or 20, characterized in that...

22. The raw material gas reactor has at least one inlet valve and at least one outlet valve, and the controller is further operable to control all of the inlet valve and the outlet valve of the raw material gas reactor to generate a closed volume before controlling the at least one igniter to burn the combustible gas in the combustion chamber. The system according to any one of claims 15 to 21, further comprising...

Citation Information

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