Systems and methods configured to enable improved / optimized control of hydrocarbon pyrolysis processes

Abstract

The present invention, in various embodiments, relates to systems and methods configured to enable improved / optimized control of a hydrocarbon pyrolysis process. Embodiments are developed for implementation in the context of a hydrocarbon gas pyrolysis system having a reactor subsystem with a reactor chamber within which hydrocarbon gases are decomposed in the presence of conductive particulate material.

Description

[Technical Field]

[0001] CROSS-REFERENCE TO RELATED APPLICATIONS This application claims convention priority from Australian Provisional Patent Application No. 2022903775, filed December 9, 2022. The entire contents of AU'775 are incorporated herein by reference.

[0002] The present invention, in various embodiments, relates to systems and methods configured to enable improved / optimized control of a hydrocarbon pyrolysis process. Embodiments have been developed for implementation in the context of a hydrocarbon gas pyrolysis system having a reactor subsystem with a reactor chamber within which hydrocarbon gases are decomposed in the presence of conductive particulate material. [Background technology]

[0003] Any description of background art throughout this specification should not be taken as an admission that such art is widely known or forms part of common general knowledge in the field.

[0004] Methane pyrolysis (also known as natural gas pyrolysis or methane cracking) refers to the process by which methane is converted into solid carbon and hydrogen, which offers multiple benefits, for example, regarding the intrinsic value of both the solid carbon and the hydrogen, and also in the context of atmospheric carbon dioxide mitigation initiatives.

[0005] Hydrogen has many commercial uses, such as a clean, environmentally friendly alternative fuel for vehicles. Carbon, or more specifically graphite, is considered a key material in the emerging green technology market. It has been shown to be useful in energy storage / batteries, conductive devices, catalyst supports, lubricant additives, and modern electronics. All references to carbon within this patent relate to the graphitic form of carbon, and therefore these terms are used interchangeably throughout.

[0006] However, conventional methods of generating hydrogen from fossil fuels, such as Steam Methane Reforming (SMR), produce carbon dioxide (steam reforming of natural gas and coal gasification), which is harmful to the environment.

[0007] Solid carbon, or more specifically graphite, is considered a key material in the emerging green technology market, as it has been shown to be useful in energy storage, electric vehicles, photovoltaics, and modern electronic devices.

[0008] Natural gas is catalytically cracked into both hydrogen gas and solid carbon according to equation (1). CH4 → C + 2H2(1)

[0009] In such a process, carbon is deposited on the surface of the catalyst and hydrogen gas is evolved. There are many known catalysts for the process, including noble metal and carbon-based catalysts.

[0010] Although the above-mentioned processes are known, they have not been commercially utilized for a number of economic reasons. This is primarily related to the underlying catalyst cost, both in terms of the initial feed amount and the cost of recycling and regenerating the catalyst. Numerous researchers in this field have utilized expensive and complex supported catalysts that, despite high catalytic activity and product yields, result in extremely high catalyst turnover costs. These costs are a significant obstacle to commercializing the use of such catalysts. There is a great need for new and improved processes and catalysts for the catalytic conversion of hydrocarbons to stable, commercially valuable hydrogen and solid carbon.

[0011] This application cites numerous patent publications, such as WO 2016 / 154666, WO 2017 / 031529, and WO 2018 / 170543, each of which is incorporated herein by cross-reference. In particular, these patent publications describe technology for methane pyrolysis using fluidized bed reactors and ion-containing catalysts (synthetic and naturally occurring). The present inventors have recognized improvements in such technology. Summary of the Invention [Problem to be solved by the invention]

[0012] It is an object of the present invention to overcome or ameliorate at least one of the disadvantages of the prior art, or to provide a useful alternative. [Means for solving the problem]

[0013] One example embodiment is a method for controlling a hydrocarbon gas pyrolysis system, the hydrocarbon gas pyrolysis system including a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the method comprising: receiving time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; processing the time series input data, thereby determining one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of the real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; operating a control optimization module to process data including one or more parameters representative of real-time reactor subsystem outputs based on the computer executable code, thereby generating one or more control instructions; operating the control module, thereby sending one or more control commands to cause control of at least one of: (i) a heating control system (optionally, the heating control system controls a level of current and / or voltage applied to one or more electrodes configured to send current into the reactor chamber so that the current propagates through the conductive particulate material); and (ii) a particulate matter feed control system configured to control the metered feed of primary particulate material into the reactor chamber; The present invention provides a method comprising:

[0014] In one example embodiment, the one or more parameters relate to each of: (i) the level of hydrogen gas in the reactor output; and / or (ii) the level of one or more particulate materials in the reactor output. In another example embodiment, the one or more parameters relate to only one of: (i) the level of hydrogen gas in the reactor output; and (ii) the level of one or more particulate materials in the reactor output.

[0015] In one example embodiment, the one or more control instructions result in control of each of the heating control system and the particulate matter delivery control system. In another example embodiment, the one or more control instructions result in control of only one of the heating control system and the particulate matter delivery control system.

[0016] In one embodiment, one or more parameters representative of the real-time reactor subsystem output are derived from: the relative predominance of hydrogen gas in the gaseous mixture; the degree of purity of the hydrogen-based mixture; the amount of hydrogen passing through an area as a function of time; the degree of fluidity in the particles; the ratio of primary particulate material to conductive particulate material; and the temperature of the hydrogen-containing output stream.

[0017] In one embodiment, the one or more parameters representative of the real-time reactor subsystem output are derived from: a metric related to the quantum of one or more particulate materials released from the reactor subsystem as a function of time; a metric related to the particle size of one or more particulate materials released from the reactor subsystem; and a metric related to the morphology of one or more particulate materials released from the reactor subsystem.

[0018] In one embodiment, the one or more control instructions include control instructions representing one or more of: (i) instructions to adjust the discharge rate of the primary particulate material into the reactor chamber; (ii) instructions to discharge a predetermined amount of primary particulate material into the reactor chamber at a predetermined rate; (iii) instructions to perform batch delivery of a predetermined amount of primary particulate material into the reactor chamber at a predetermined time; (iv) and an air transport fluid velocity relative to the primary particulate material; a batch size of the primary particulate material; or (vi) instructions to adjust the batch frequency of the primary particulate material.

[0019] In one example embodiment, the one or more control commands include commands that result in an increase or decrease in the amount of current and / or voltage being sent through one or more electrodes of the heating control system (e.g., as measured by the magnitude of the current and / or the total current per predefined time block, if pulsing currents are used).

[0020] In one embodiment, commands that result in an increase or decrease in the amount of current and / or voltage being sent through one or more electrodes of the heating control system represent a specified target temperature change within the reactor chamber.

[0021] In one embodiment, an increase or decrease in the amount of current and / or voltage being sent through one or more electrodes of the heating control system is provided to the reactor control module for the reactor subsystem.

[0022] In one embodiment, the reactor subsystem includes a reactor controller module, and operating the reactor control module thereby sending one or more control commands includes providing a signal to the reactor controller module thereby causing the reactor control module to operate in a specified manner.

[0023] In one embodiment, operating the reactor control module in a prescribed manner includes causing the reactor control module to: (i) increase or decrease the heat in the reactor chamber; (ii) modify one or more fluidization parameters in the reactor chamber; or (iii) modify the pressure in the reactor chamber.

[0024] In one embodiment, the reactor subsystem includes a fluidized bed reactor.

[0025] In one embodiment, the particulate matter feed control system includes a quantity determining arrangement configured to measure the amount of primary particulate material prior to delivery to the fluidized bed reactor.

[0026] In one embodiment, the particulate matter feed control system includes a particulate matter storage assembly coupled to a particulate matter feed assembly, the particulate matter feed assembly including at least one pre-feed vestibule configured to be selectively pressurized during delivery of the primary particulate material prior to delivery to the reactor.

[0027] In one example embodiment, the control optimization module for processing data is further configured to process data from one or more additional sources, including: (i) a sensor configured to monitor the temperature within the reactor chamber; (ii) an input representing a predicted future temperature within the reactor subsystem; (iii) an input representing one or more parameters derived from monitoring particulate matter detected in the reactor subsystem output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing desired future operating conditions of the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the reactor subsystem output.

[0028] In one embodiment, the conductive particulate material comprises one or more particulate materials selected from the group comprising graphitic starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide; preferably, the conductive material is selected from the group comprising carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

[0029] In one embodiment, the primary particulate material comprises a catalytic particulate material for hydrocarbon pyrolysis in the reactor subsystem.

[0030] In one embodiment, the primary particulate material comprises a material selected from the group including carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

[0031] In one embodiment, the primary particulate material comprises a graphitic material.

[0032] In one embodiment, the graphitic material is selected from naturally occurring or synthetic graphite; flake graphite; and forms of conductive carbon.

[0033] In one example embodiment, the control optimization module is responsive to one or more parameters representing reactor subsystem outputs as well as inputs representing desired future operation to generate one or more control commands.

[0034] In one embodiment, the inputs representing desired future operation include any one or more of: (i) desired hydrogen output parameters; (ii) desired output carbon parameters; and (iii) desired carbon output form.

[0035] In a further example embodiment, the invention includes a method for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the method comprising: receiving time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; processing the time series input data, thereby determining one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of the real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; operating a control optimization module to process data including one or more parameters representative of real-time reactor subsystem outputs based on the computer executable code, thereby generating one or more control instructions; operating the control module, thereby sending one or more control commands to cause control of at least one of: a heating control system that controls the temperature within the reactor chamber; and a particulate matter feed control system that is configured to control the metered feed of primary particulate material into the reactor chamber; Includes:

[0036] In a further example embodiment, the invention includes a system for controlling a hydrocarbon gas pyrolysis system, where the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, and the method includes: a data input module configured to receive time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; a processing module configured to process the time series input data to thereby determine one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of the real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; a control optimization module operable to process data including one or more parameters representative of real-time reactor subsystem outputs based on the computer executable code, thereby generating one or more control instructions; a control module operable to send one or more control commands to cause control of at least one of: a heating control system for controlling temperature within the reactor chamber; and a particulate matter feed control system configured to control the metered feed of primary particulate material into the reactor chamber; Includes:

[0037] In a further example embodiment, the present invention includes a method for pyrolysis of a hydrocarbon gas, the method comprising: receiving input data from a sensor configured to monitor an output of a fluidized bed reactor fed by an input of hydrocarbon gas; processing the input to determine one or more parameters representative of the fluidized bed reactor output; operating a control optimization module responsive to one or more parameters representative of the fluidized bed reactor output to generate one or more control commands; applying at least one of the control commands to a particulate matter feed control system, the particulate matter feed control system configured to control metered feeding of the particulate matter into the fluidized bed reactor; Includes:

[0038] In certain embodiments, the one or more parameters include a parameter representative of the amount of hydrogen gas or the ratio of hydrogen to hydrocarbon gas, which may include the rate of hydrogen gas throughput through the monitored region or the degree of increase in the proportion of hydrogen as represented by the ratio of hydrogen to hydrocarbon gas.

[0039] In certain embodiments, the control instructions represent one or more of: (i) instructions to adjust the discharge rate of particulate material into the fluidized bed reactor; (ii) instructions to discharge a specified amount of primary particulate material into the reactor chamber at a specified rate; (iii) instructions to perform a batch feed of a specified amount of primary particulate material into the reactor chamber at a specified time; (iv) and an air transport fluid velocity relative to the primary particulate material; a batch size of the primary particulate material; or (vi) instructions to adjust the batch frequency of the primary particulate material.

[0040] In an embodiment, the particulate matter feed control system includes a quantity determining arrangement configured to measure the amount of particulate material prior to delivery to the fluidized bed reactor. In an embodiment, the particulate matter feed control system includes a particulate matter storage assembly coupled to a particulate matter feed assembly, the particulate matter feed assembly including a pre-feed vestibule configured to be selectively pressurized during delivery of the particulate material prior to delivery to the fluidized bed reactor.

[0041] In certain embodiments, the control optimization module is further responsive to data obtained from one or more additional inputs to generate the one or more control commands. For example, the one or more additional sensors may include any one or more of: (i) a sensor configured to monitor the temperature within the fluidized bed reactor; (ii) an input representing a predicted future temperature within the fluidized bed reactor; (iii) an input representing one or more parameters derived from monitoring particulate matter detected at the fluidized bed reactor output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing desired future operating conditions for the fluidized bed reactor; and (vi) an input representing one or more parameters related to gases other than hydrogen detected at the fluidized bed reactor output.

[0042] In some embodiments, the one or more sensors are spaced apart within the fluidized bed reactor, hi some embodiments, the one or more sensors are at the distal end of the fluidized bed reactor.

[0043] In certain embodiments, the particulate material is selected from the group comprising graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide, and preferably the conductive material is selected from the group comprising carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide.

[0044] In some embodiments, the particulate material is a catalytic particulate material for methane pyrolysis in a fluidized bed reactor, hi some embodiments, the catalytic particulate material is selected from the group including carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide.

[0045] In certain embodiments, the particulate material is a non-catalytic particulate material selected to facilitate methane pyrolysis in the fluidized bed reactor. Preferably, it is a graphitic material selected from, for example, naturally occurring or synthetic graphite, preferably flake graphite. While other forms of carbon may be used, preferably, a conductive form of carbon may be used (e.g., when the fluidized bed reactor is heated by the flow of electrical current (applied and / or induced) through a conductive material within the fluidized bed reactor). In some embodiments, when the carbon is non-conductive, a secondary material is present that is conductive, such as a silica- or alumina-based material.

[0046] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coal seam gas, landfill gas, and biogas. The composition of hydrocarbon gases can vary significantly, but generally includes one or more light hydrocarbons from the group including methane, ethane, ethylene, propane, and butane. In preferred embodiments, the hydrocarbon gas is selected from the group including methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In preferred embodiments, the hydrocarbon gas consists essentially of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0047] In certain embodiments, the control instructions include control instructions for one or more other components that control aspects of hydrocarbon pyrolysis. Preferably, the one or more other components include thermal control components for a fluidized bed reactor.

[0048] In certain embodiments, the control optimization module is responsive to one or more parameters representative of the fluidized bed reactor output and to inputs representative of desired future operation to generate one or more control commands. Preferably, the inputs representative of desired future operation include any one or more of: (i) a desired hydrogen output parameter; (ii) a desired output carbon parameter; and (iii) a desired carbon output configuration.

[0049] In a second aspect, the present invention provides a system for controlling components used in a facility performing hydrocarbon gas pyrolysis, the system comprising: a module configured to receive input data from a sensor configured to monitor an output of a fluidized bed reactor fed by an input of hydrocarbon gas; a processing module configured to process the input to determine one or more parameters representative of the fluidized bed reactor output; a control optimization module responsive to one or more parameters representative of the fluidized bed reactor output for generating one or more control commands; an output module configured to apply at least one of the control commands to a particulate matter feed control system, the particulate matter feed control system configured to control the metered feed of particulate matter into the fluidized bed reactor; Includes:

[0050] In certain embodiments, the one or more parameters include a parameter representative of hydrogen gas volume, which may include the rate of hydrogen gas throughput through the region being monitored.

[0051] In certain embodiments, the control instructions represent one or more of: (i) instructions to adjust the discharge rate of particulate material into the fluidized bed reactor; (ii) instructions to discharge a specified amount of primary particulate material into the reactor chamber at a specified rate; (iii) instructions to perform a batch feed of a specified amount of primary particulate material into the reactor chamber at a specified time; (iv) and an air transport fluid velocity relative to the primary particulate material; a batch size of the primary particulate material; or (vi) instructions to adjust the batch frequency of the primary particulate material.

[0052] In an embodiment, the particulate matter feed control system includes a quantity determining arrangement configured to measure the amount of particulate material prior to delivery to the fluidized bed reactor. In an embodiment, the particulate matter feed control system includes a particulate matter storage assembly coupled to a particulate matter feed assembly, the particulate matter feed assembly including a pre-feed vestibule configured to be selectively pressurized during delivery of the particulate material prior to delivery to the fluidized bed reactor.

[0053] In certain embodiments, the control optimization module is further responsive to data obtained from one or more additional inputs to generate the one or more control commands. For example, the one or more additional sensors may include any one or more of: (i) a sensor configured to monitor the temperature within the fluidized bed reactor; (ii) an input representing a predicted future temperature within the fluidized bed reactor; (iii) an input representing one or more parameters derived from monitoring particulate matter detected at the fluidized bed reactor output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing desired future operating conditions for the fluidized bed reactor; and (vi) an input representing one or more parameters related to gases other than hydrogen detected at the fluidized bed reactor output.

[0054] In certain embodiments, the particulate material is selected from the group comprising graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide, and preferably the conductive material is selected from the group comprising carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide.

[0055] In some embodiments, the particulate material is a catalytic particulate material for methane pyrolysis in a fluidized bed reactor, hi some embodiments, the catalytic particulate material is selected from the group including carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide.

[0056] In certain embodiments, the particulate material is a non-catalytic particulate material selected to facilitate methane pyrolysis in the fluidized bed reactor. Preferably, it is a graphitic material selected from, for example, naturally occurring or synthetic graphite, preferably flake graphite. Preferably, a conductive form of carbon is used (e.g., when the fluidized bed reactor is heated by the flow of electrical current (applied and / or induced) through a conductive material within the fluidized bed reactor), although other forms of carbon may be used.

[0057] In certain embodiments, the control instructions include control instructions for one or more other components that control aspects of hydrocarbon pyrolysis. Preferably, the one or more other components include thermal control components for a fluidized bed reactor.

[0058] In certain embodiments, the control optimization module is responsive to one or more parameters representative of the fluidized bed reactor output and to inputs representative of desired future operation to generate one or more control commands. Preferably, the inputs representative of desired future operation include any one or more of: (i) a desired hydrogen output parameter; (ii) a desired output carbon parameter; and (iii) a desired carbon output configuration.

[0059] In a further example embodiment, the present invention includes a method for pyrolysis of hydrocarbon gases, the method comprising: providing an initial feedstock of conductive carbon material in a fluidized bed reactor; starting up a fluidized bed reactor, the fluidized bed reactor being fed with an input of hydrocarbon gas; operating a high frequency power source to send an alternating current to an electrically conductive coil at least partially surrounding the fluidized bed reactor, thereby creating an inductive effect within the fluidized bed reactor, causing an electric current to flow through the electrically conductive carbon material by the inductive effect, thereby heating the electrically conductive carbon material to a predetermined temperature that initiates and sustains the pyrolysis of the hydrocarbon gas; operating an outlet component, thereby discharging a treatment material from the fluidized bed reactor, the discharged treatment material including carbonaceous material, unreacted hydrocarbon gas, and / or hydrogen gas; Includes:

[0060] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0061] In certain embodiments, the conductive carbon material is selected from the group including graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

[0062] In an embodiment, a method includes feeding a feed of conductive carbon material into a fluidized bed reactor.

[0063] In certain embodiments, the conductive carbon material is selected from the group including carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or lower iron oxides.

[0064] In one embodiment, the predetermined temperature is 600 to 1500 degrees Celsius, preferably 800 to 1200 degrees Celsius.

[0065] In certain embodiments, the graphite starting material is selected from naturally occurring or synthetic graphite, preferably flake graphite.

[0066] In certain embodiments, the method further includes capturing at least a portion of the carbon materials withdrawn from the outlet and processing the carbon materials to produce regenerated graphitic material.

[0067] In some embodiments, the conductive coil is center cooled.

[0068] In some embodiments, multiple conductive coils are used.

[0069] In some embodiments, each of the conductive coils is operable independently of one another to achieve a predetermined temperature.

[0070] In one embodiment, the predetermined temperature is 600 to 1500 degrees Celsius, preferably 800 to 1200 degrees Celsius.

[0071] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gases, the system comprising: a fluidized bed reactor configured to contain an initial feedstock of conductive carbon material at start-up; a gas input system for a fluidized bed reactor configured to provide an input feed of hydrocarbon gas to the fluidized bed reactor; at least one electrically conductive coil at least partially surrounding the fluidized bed reactor; a radio frequency power supply configured to send an alternating current to the conductive coil, thereby creating an inductive effect within the fluidized bed reactor, causing a current to flow through the conductive carbon material by the inductive effect, thereby heating the conductive carbon material to a predetermined temperature that initiates and sustains the pyrolysis of the hydrocarbon gas; an outlet system configured to discharge a treatment material from the fluidized bed reactor, the discharged treatment material comprising a carbonaceous material, unreacted hydrocarbon gas, and / or hydrogen gas; Includes:

[0072] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0073] In certain embodiments, the conductive carbon material is selected from the group including graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

[0074] In an embodiment, the system includes feeding a feed of conductive carbon material into a fluidized bed reactor.

[0075] In certain embodiments, the conductive carbon material is selected from the group including carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or lower iron oxides.

[0076] In one embodiment, the predetermined temperature is 600 to 1500 degrees Celsius, preferably 800 to 1200 degrees Celsius.

[0077] In certain embodiments, the graphite starting material is selected from naturally occurring or synthetic graphite, preferably flake graphite.

[0078] In certain embodiments, the system further includes capturing at least a portion of the carbon materials withdrawn through the outlet and processing the carbon materials to produce regenerated graphitic material.

[0079] In some embodiments, the conductive coil is center cooled.

[0080] In some embodiments, multiple conductive coils are used.

[0081] In some embodiments, each of the conductive coils is operable independently of one another to achieve a predetermined temperature.

[0082] In one embodiment, the predetermined temperature is 600 to 1500 degrees Celsius, preferably 800 to 1200 degrees Celsius.

[0083] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gases, the system comprising: a fluidized bed reactor (FBR) configured to contain an initial feedstock of conductive carbon material at start-up; a gas input system for a fluidized bed reactor configured to provide an input feed of hydrocarbon gas to the fluidized bed reactor; at least one pair of conductive electrodes configured to, in use, upon start-up, cause a flow of electrical current through a conductive carbon material contained in a fluidized bed reactor containing a feedstock of the conductive carbon material; a radio frequency power source configured to send an electric current between at least one pair of electrodes, thereby causing the electric current to flow through a conductive carbon material contained in a fluidized bed reactor, thereby heating the conductive carbon material to a predetermined temperature whose average temperature initiates and sustains the pyrolysis of the hydrocarbon gas; an outlet system configured to discharge a treatment material from the fluidized bed reactor, the discharged treatment material comprising a carbonaceous material, an unreacted hydrocarbon material, and / or hydrogen gas; Includes:

[0084] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0085] In some embodiments, the conductive material comprises a conductive carbon material, hi some embodiments, the conductive material further comprises an inert / non-reactive conductive co-material (e.g., silica beads) that transfers heat to the surrounding process material.

[0086] In some embodiments, there are multiple pairs of electrodes. In such embodiments, optionally, a single electrode is a member of more than one of the multiple pairs of electrodes.

[0087] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gases, the system comprising: Fluidized Bed Reactor (FBR) and; a gas input system for a fluidized bed reactor configured to provide an input feed of hydrocarbon gas to the fluidized bed reactor; at least one heating element disposed within the fluidized bed reactor; a radio frequency power source configured to deliver radio frequency power to at least one heating element to thereby heat the fluidized bed reactor to a predetermined temperature that initiates and sustains pyrolysis of the hydrocarbon gas; an outlet system configured to discharge a treatment material from the fluidized bed reactor, the discharged treatment material comprising a carbonaceous material, an unreacted hydrocarbon material, and / or hydrogen gas; Includes:

[0088] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0089] In certain embodiments, the system includes multiple heating elements. In certain embodiments, each of the multiple heating elements can be individually controlled to maintain an average temperature. In some embodiments, there are multiple heating elements, each configured to add heat to a different zone within the fluidized bed reactor. Preferably, in some embodiments, such heating elements are individually controllable, thereby adding variable heat to different zones within the fluidized bed reactor. In some embodiments, the different zones can be defined based on vertical / horizontal and / or radial coordinates.

[0090] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gases, the system comprising: Fluidized Bed Reactor (FBR) and; a gas input system for a fluidized bed reactor configured to provide an input feed of hydrocarbon gas to the fluidized bed reactor; at least one heating element disposed on a sidewall of the fluidized bed reactor; a radio frequency power source configured to deliver radio frequency power to at least one heating element to thereby heat the fluidized bed reactor to a predetermined temperature that initiates and sustains pyrolysis of the hydrocarbon gas; an outlet system configured to discharge a treatment material from the fluidized bed reactor, the discharged treatment material comprising a carbonaceous material, an unreacted hydrocarbon material, and / or hydrogen gas; Includes:

[0091] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0092] In certain embodiments, the system includes a plurality of heating elements. In embodiments, each of the plurality of heating elements is configured to apply heat to a different zone within the fluidized bed reactor. Preferably, such heating elements are individually controllable, thereby applying variable heat to different zones within the fluidized bed reactor to maintain an average temperature. In some embodiments, the different zones may be defined based on vertical / horizontal and / or radial coordinates.

[0093] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gases, the system comprising: Fluidized Bed Reactor (FBR) and; a gas input system for a fluidized bed reactor configured to provide an input feed of hydrocarbon gas to the fluidized bed reactor; a plurality of heating arrangements configured to apply heat to the fluidized bed reactor (inside or outside the reactor, i.e., hot or cold wall reactor); a radio frequency power supply system configured to deliver radio frequency power to the or each heating arrangement, thereby causing heating within the fluidized bed reactor to a predetermined temperature that initiates and sustains pyrolysis of the hydrocarbon gas; an outlet system configured to discharge a treatment material from the fluidized bed reactor, the discharged treatment material comprising a carbonaceous material, an unreacted hydrocarbon material, and / or hydrogen gas; Includes:

[0094] In certain embodiments, the hydrocarbon gas comprises or consists essentially of methane gas.

[0095] Preferably, the or each plurality of heating arrangements comprises at least two different heating arrangement types selected from the group comprising: at least one heating element disposed on a side wall of the fluidized bed reactor; at least one heating element disposed within the fluidized bed reactor; at least one pair of conductive electrodes configured to, in use, cause an electric current to flow through a conductive material contained in the fluidized bed reactor, thereby heating the conductive material; and at least one conductive coil wrapped around the fluidized bed reactor configured to, in use, cause an electric current to flow through a conductive material contained in the fluidized bed reactor, thereby heating the conductive material.

[0096] definition In describing and claiming the present invention, the following terminology will be used in accordance with the definitions set out below. It is also to be understood that the terminology used herein is for the purpose of describing particular embodiments of the invention only, and is not intended to be limiting. Unless otherwise defined, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention pertains.

[0097] Throughout this specification, unless the context requires otherwise, the term "inferior" is understood to include non-synthetic materials. As will be understood by those skilled in the art, synthetic materials are produced by chemical reaction of precursor materials. A standard synthesis technique for catalysts that is excluded from this invention is, for example, the impregnation of nano-sized catalytic elements onto an inert support. The term "inferior" includes naturally occurring materials, but should not be understood to exclude materials that have been subjected to physical beneficiation, such as crushing and sieving or classification.

[0098] As used herein, the term "dusting" is an industry term used to describe the reaction that causes a metallic material (often iron) to break down into debris and graphite in a carburizing environment. This effect begins with methane molecules (or other carbonaceous gases) adsorbing and dissociating on the surface of a metal-containing catalyst, and the resulting carbon diffuses to the surface of the bulk metal. Once this outer layer is saturated with carbon, metal carbides form, which then precipitate from the metal grain boundaries as graphitic carbon. Over time, this creates intergranular pressure that separates the metal carbide particles from the parent bulk metal, causing the metal structure to break down through "dusting." In doing so, the catalyst separates and breaks down into nano-fragments that become encapsulated within the carbon / graphite. The resulting graphitic carbon material encapsulating the Fe particles is hereinafter referred to as "carbon material with encapsulated iron" or "Hazer graphite."

[0099] The term "hydrocarbon gas" is intended to include a pure single gas, e.g., methane, or a gas mixture containing one or more hydrocarbon gases, e.g., natural gas. While preferred embodiments of the present invention relate to methane pyrolysis (or pyrolysis of methane-containing gas streams), it will be understood that other hydrocarbon gases, e.g., ethane, propane, etc., are also suitable for the techniques described herein.

[0100] Unless the context clearly dictates otherwise, throughout the description and claims, the words "comprise," "comprising," and the like are to be construed in an inclusive sense, i.e., "including, but not limited to," as opposed to an exclusive or exhaustive sense.

[0101] As used herein, the phrase "consisting of" excludes any element, step, or ingredient not specified in the claim. When the phrase "consisting of" (or variations thereof) appears in a clause in the body of a claim rather than immediately following the preamble, it limits only the elements described in that clause; other elements are not excluded from the claim as a whole. As used herein, the phrase "consisting essentially of" limits the claim to certain elements or method steps plus those that do not materially affect the underlying novel characteristics of the claimed subject matter.

[0102] As used herein, the term "power source" may refer to a source of alternating current or direct current.

[0103] With respect to the terms "comprising," "consisting of," and "consisting essentially of," when one of these three terms is used herein, the disclosed and claimed subject matter may include the use of either of the other two terms. Thus, in some embodiments not expressly recited otherwise, any instance of "comprising" may be replaced with "consisting of," or alternatively, "consisting essentially of."

[0104] Other than in the working examples, or where otherwise indicated, all numbers expressing amounts of materials or reaction conditions used herein are understood to be modified in all cases by the term "about," taking into account common tolerances in the art. The examples are not intended to limit the scope of the invention. Hereinafter, or where otherwise indicated, "%" means "% by weight," "ratio" means "weight ratio," and "parts" means "parts by weight."

[0105] As used herein, the term "substantially" means including more than 50% by weight, where relevant, unless otherwise indicated.

[0106] The term "about" should be interpreted by one of ordinary skill in the art taking into account common tolerances in the relevant art.

[0107] The recitation of numerical ranges using endpoints includes all numbers subsumed within that range (e.g., 1 to 5 includes 1, 1.5, 2, 2.75, 3, 3.80, 4, 5, etc.).

[0108] The terms "preferred" and "preferably" refer to embodiments of the invention that may offer certain benefits, under particular circumstances. However, other embodiments may also be preferred, under the same or other circumstances. Furthermore, the recitation of one or more preferred embodiments does not imply that other embodiments are not useful or is not intended to exclude other embodiments from the scope of the invention.

[0109] It should be noted that as used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise.

[0110] The prior art referenced herein is fully incorporated herein by reference unless specifically disclaimed.

[0111] Although example embodiments of the disclosed technology are described in detail herein, it should be understood that other embodiments are contemplated. Accordingly, it is not intended that the disclosed technology be limited in scope to the details of construction and the arrangement of components set forth in the following description or illustrated in the drawings. The disclosed technology enables other embodiments and can be practiced or carried out in various ways.

[0112] This specification has been prepared with a view to principles of general application in mind. As such, where the specification discloses principles of general application, the claims may be drafted in corresponding general terms (Biogen v Medeva

[1997] RPC 1 at 48). A "principle of general application" is a general principle that can be practically applied in making a certain product or operating a process, including where the claims define the product or process in terms of a result to be achieved.

[0113] Claim features stated in general terms represent principles of general application, where it is reasonable to expect (it is reasonable to predict) that the claimed invention will work with something that falls within the general term. Such features defined in general terms may be the body of a claim or may be simply descriptive language. In either case, a claim feature expressed in general terms is sufficiently enabled if the disclosure enables at least one form or one application of the general principle of the feature, and one skilled in the art would reasonably expect that the invention will work with something that falls within the general term. (Kirin-Amgen Inc. v Hoechst Marion Roussel Ltd

[2005] RPC 9 at

[0112] ).

[0114] If claims are drafted more broadly, they may be considered enabled if, at first sight: a) the present disclosure teaches a principle that one skilled in the art must follow in order to achieve each and every embodiment falling within the scope of the claims; and b) the description discloses at least one application of the principle and provides sufficient information for one skilled in the art to carry out alternative applications of the principle in ways that are not explicitly disclosed but are obvious to those skilled in the art (T 484 / 92).

[0115] Example embodiments are described below in the Claims section.

[0116] Throughout this specification, references to "one embodiment," "some embodiments," or "an embodiment" mean that a particular feature, structure, or characteristic described in connection with an embodiment is included in at least one embodiment of the invention. Thus, appearances of the phrases "in one embodiment," "some embodiments," or "an embodiment" in various places throughout this specification do not necessarily all refer to the same embodiment, but may. Furthermore, as will be apparent to one of ordinary skill in the art from this disclosure, the particular features, structures, or characteristics may be combined in any suitable manner in one or more embodiments.

[0117] As used herein, unless otherwise specified, the use of ordinal adjectives "first," "second," "third," etc. to describe a common object merely indicates that they refer to different instances of a similar object, and is not intended to imply that the objects so described should be in a given order, whether in time, space, rank, or in any other way.

[0118] In the claims below and in the description herein, any one of the terms comprising, comprised of, or which comprises is an open term meaning to include at least the element / feature before it, but not to exclude others. Therefore, when used in a claim, the term comprising should not be interpreted as being limited to the means, elements, or steps listed before it. For example, the scope of the expression "device comprising A and B" should not be limited to a device consisting only of A and B. When used herein, any one of the terms including, which includes, or that includes is also an open term meaning to include at least the element / feature before it, but not to exclude others. Therefore, including is synonymous with compris- ing.

[0119] As used herein, the term "exemplary" is used in the sense of providing an example, as opposed to indicating a quality; that is, an "exemplary embodiment" is an embodiment provided by way of example, as opposed to an embodiment that is necessarily of exemplary quality.

[0120] The present invention is not to be limited in scope by any of the specific embodiments described herein, which are intended for illustrative purposes only. Functionally equivalent products, formulations, and methods are clearly within the scope of the invention as described herein.

[0121] The invention described herein may include one or more ranges of values ​​(e.g., size, concentration, etc.) A range of values ​​is understood to include all values ​​within that range, including the values ​​defining the range and any adjacent values ​​within that range that achieve the same or substantially the same result as the values ​​immediately adjacent to the values ​​defining the boundaries of the range.

[0122] Other definitions of selected terms described herein may be found within the detailed description of the invention and may be applied throughout. Unless otherwise defined, all other scientific and technical terms described herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.

[0123] Throughout this specification, unless the context requires otherwise, the term "selectively synthesize" will be understood to refer to the preferential synthesis of one form over another. While the process of the present invention often produces a mixture of forms, Applicants have determined that the selection of process temperature and pressure will affect the morphology of the graphite so produced.

[0124] Throughout this specification, unless the context requires otherwise, it will be understood that the process of the present invention can be carried out at two or more temperatures and / or pressures within a specified range. For example, if a temperature range of 600°C to 800°C is provided, the step of contacting the metal-containing catalyst with the hydrocarbon gas can be carried out initially at 600°C, with the temperature being increased to 800°C during contact between the metal-containing catalyst and the hydrocarbon gas. Similarly, if a pressure range of 0 bar(g) to 8 bar(g) is provided, the step of contacting the metal-containing catalyst with the hydrocarbon gas can be carried out initially at 0 bar(g), with the pressure being increased to 8 bar(g) during contact between the metal-containing catalyst and the hydrocarbon gas.

[0125] Throughout this specification, unless the context requires otherwise, the term "selectivity" refers to the proportion of graphitic material produced that has the desired morphology.

[0126] Throughout this specification, unless the context requires otherwise, the term "bar (g)" refers to gauge pressure. As will be understood by those skilled in the art, gauge pressure refers to pressure in bars above ambient pressure.

[0127] The term "predetermined range of values" as used herein refers to a particular range of pressures and temperatures that can be selected by one skilled in the art to selectively synthesize a graphitic material having a desired morphology. One skilled in the art can select an appropriate temperature or temperatures and pressures, or pressures within these ranges, to selectively synthesize a desired graphitic material.

[0128] Features of the present invention will now be described with reference to the following non-limiting descriptions and examples.

[0129] Embodiments of the present invention will now be described, by way of example only, with reference to the accompanying drawings, in which: [Brief explanation of the drawings]

[0130] [Figure 1] A schematic overview of an example hydrocarbon pyrolysis system is provided as a context for embodiments of the control techniques described herein. [Figure 2] 1 illustrates a system configured to enable improved / optimized control of a hydrocarbon pyrolysis process, shown in conjunction with selected components of a broader hydrocarbon pyrolysis system. [Figure 3A] 1 illustrates a first heating arrangement for a hydrocarbon pyrolysis system according to one embodiment. [Figure 3B] 1 illustrates a second heating arrangement for a hydrocarbon pyrolysis system according to one embodiment. [Figure 4] A table is provided that lists exemplary relationships between controlled and manipulated variables according to one embodiment. DETAILED DESCRIPTION OF THE INVENTION

[0131] The present invention, in various embodiments, relates to systems and methods configured to enable improved / optimized control of a hydrocarbon pyrolysis process. Embodiments have been developed for implementation in the context of a hydrocarbon gas pyrolysis system having a reactor subsystem with a reactor chamber within which hydrocarbon gases are decomposed in the presence of conductive particulate material.

[0132] Overview of control optimization technology In summary, various disclosed embodiments relate to techniques that enable control of particular types of hydrocarbon gas pyrolysis systems for specific objective-based process improvement and / or optimization and / or for other purposes (e.g., to achieve desired output and / or operating parameters). The present disclosure relates to the configuration of the various hardware components and the overall pyrolysis system, as opposed to the specific detailed logic associated with operational control or optimization techniques. However, it will be understood that the techniques disclosed herein can be configured / operated to achieve optimization or other intentional control, for example, through facility-specific testing and knowledge building and / or implementation of known techniques such as machine learning.

[0133] The technology disclosed herein relates to a hydrocarbon gas pyrolysis system that includes a reactor subsystem having a reactor chamber within which hydrocarbon gases are decomposed in the presence of a conductive particulate material that serves two purposes: to assist in the decomposition process and to facilitate heating of a flowing mixture of particulates and gas within the reactor chamber.

[0134] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coal seam gas, landfill gas, and biogas. The composition of the hydrocarbon gas may vary widely, but generally comprises one or more light hydrocarbons from the group comprising methane, ethane, ethylene, propane, and butane. In a preferred embodiment, the hydrocarbon gas is selected from the group comprising methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In a preferred embodiment, the hydrocarbon gas consists essentially of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0135] Embodiments are particularly focused on heating arrangements whereby electrodes are disposed within the reactor chamber and an electric current is applied to at least one of the electrodes, causing the current to flow through a conductive particulate material, resulting in heating by the resistive effect. For example, the reactor subsystem may take the form of a fluidized bed reactor (FBR). Control of the magnitude of the electric current applied via one or more electrodes has an effect on increasing / decreasing the temperature within the reactor chamber, optionally in addition to other FBR controls, such as fluidization control.

[0136] It will be appreciated that FBR technology is known, and the concept of heating an FBR via electrodes is thus also known. However, the application of such known concepts and technology to the present specific environment introduces complexities that cannot be resolved by FBR control alone. In particular, with respect to the system described herein, the quantum of particulate material within the reactor chamber is not fixed. Rather, there is both insertion and removal of particulate material, as well as changes in the composition / morphology of the particulate material. For example: Within the reactor chamber there is always a conductive particulate material, in this case comprising graphitic carbon or iron substantially encapsulated by graphitic carbon, which is required to provide electrode-induced heating within the reactor chamber. A particulate matter feed control system is configured to control the metered feed of primary particulate material into the reactor chamber. The primary particulate material, which may include iron oxide (synthetic or naturally occurring), may be introduced as a low conductivity particulate material, followed by a transition to a higher conductivity particulate material (e.g., iron-encapsulated carbon) as carbon produced by the hydrocarbon cracking process is deposited on the iron oxide. Carbon deposition is not limited to iron oxides, but also occurs on carbon particles, including carbon encapsulated iron.

[0137] The conductive particulate material is preferably selected from the group comprising: carbonaceous material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide. The primary particulate material preferably comprises: carbonaceous material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide. When the primary particulate material is a catalytic particulate material for methane pyrolysis in a fluidized bed reactor, the catalytic particulate material is selected from the group comprising: carbonaceous material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide. Optionally, the primary particulate material is a non-catalytic particulate material selected to facilitate methane pyrolysis in the fluidized bed reactor. Preferably, this is a graphitic material selected from, for example, naturally occurring or synthetic graphite, preferably flake graphite. While other forms of carbon may be used, preferably, conductive forms of carbon may be used (e.g., when the fluidized bed reactor is heated by the flow (applied and / or induced) of electric current through a conductive material in the fluidized bed reactor).

[0138] The quantity of particulate material within the reactor chamber, along with the overall composition and morphology of those particulate materials, directly affects several parameters related to the pyrolysis process. For example, this affects: (i) the rate and efficiency (and / or fluidization rate) at which pyrolysis occurs at a given temperature; (ii) the relationship between current and heating effect (e.g., for a given fluidization rate); (iii) the operating settings of the fluidized bed reactor to achieve a desired fluidization rate; and (iv) the morphological properties of the reacted and extracted particulate materials.

[0139] Accordingly, the present disclosure presents hardware configurations and processes adapted to enable improved / optimized control of hydrocarbon pyrolysis processes in such scenarios. This allows for a range of benefits, as described below, including (but not limited to) mitigation of problems related to unwanted carbon surface deposition, the ability to adjust catalyst input, control of residence time, and control of product (e.g., carbon, particularly various forms of graphitic carbon, and hydrogen) purity. Other benefits may include greater scaling capabilities, better temperature control, simpler construction, and higher energy efficiency.

[0140] Example pyrolysis controlled process In one example embodiment, a computer-implemented method is performed that includes receiving time-series input data from a reactor output sensor system provided by a hydrocarbon gas pyrolysis system. The reactor output sensor system is configured to monitor the composition of the reactor output emitted from the reactor subsystem. For example, this can include the composition of gaseous and / or particulate matter (preferably both) output from the reactor subsystem. The time-series data preferably includes separate streams for each sensor (with their respective sampling rates and latency / delay characteristics).

[0141] The method then includes processing the time series input data to thereby determine one or more parameters representative of the real-time reactor subsystem output. The one or more parameters representative of the real-time reactor subsystem output relate to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output. That is, in some embodiments, parameters related to both are calculated, while in other embodiments, the calculated parameters relate to only one of these extents.

[0142] The outlet component, which can release gas and particulate material from the reactor subsystem / reactor chamber, can be operated in a controlled or uncontrolled manner. In one embodiment, it is uncontrolled (solids flow from the reactor is a result of particle elutriation). Therefore, the elutriation rate is a function of the geometry, flow rate, and overall design. Other means of operating the outlet component are contemplated.

[0143] As an example, in a situation where the parameters representing the real-time reactor subsystem output relate to the degree of hydrogen gas in the reactor output, those parameters are: The relative predominance of hydrogen gas in the gaseous mixture; · The degree of purity of the hydrogen-based mixture; The amount of hydrogen passing through an area as a function of time; gas flow rate; and Temperature of the hydrogen-containing output stream may be derived from any one or more of:

[0144] Similarly, in the situation where the parameter representing the real-time reactor subsystem output relates to the degree of conductive particulate material, the degree is: · A measure of the quantum of one or more particulate materials released from the reactor subsystem as a function of time; Indication of the particle size of one or more particulate materials emitted from the reactor subsystem; and Indicators of the morphology of one or more particulate materials emitted from the reactor subsystem may be derived from any one or more of:

[0145] For clarity, the term "real-time" as used herein indicates that a parameter can be reasonably functionally correlated to the current conditions within the reactor chamber. This may include a process of forward extrapolation or may otherwise accommodate / account for delays resulting from, for example, the time between material exiting the reactor and material being observed by a sensor. Delays on the order of seconds or minutes are considered "real-time" in this context.

[0146] As a further context, in embodiments where the primary particulate material is a catalyst (e.g., iron oxide, which reacts to iron and then encapsulates in graphite from hydrogen cracking), data representing the catalyst / gas ratio within the reaction chamber relative to hydrocarbon (e.g., methane) conversion are of particular interest. An additional factor of interest is the hydrogen purity (and / or hydrogen production) in the output relative to the rate at which the hydrocarbon feed gas is provided to the reactor chamber. Other relevant factors include reactor temperature, bed level, gas residence time (in the dense bed), and operating pressure. It will be understood that the gas feed rate, reactor heat input, reactor pressure, and particulate discharge rate / metering rate are primarily manipulated or independent variables. Dependent variables are hydrogen purity, hydrogen production, graphite purity (noting how iron oxide reacts within the chamber to form iron encapsulated in graphite), primary particulate material to conductive particulate material (optionally calculated by monitoring the degree of conductivity of the output stream), or more specifically, the iron / iron oxide graphite encapsulating iron ratio, and hydrocarbon / methane conversion rate. Any one or more of the dependent variables (or the extent to which they are directly / indirectly represented) are optionally quantified, thereby allowing the system to primarily control one or more of the manipulated or independent variables, such as particulate insertion / discharge rate / metering, feed rate, and / or various parameters, such as reactor chamber temperature, pressure, and fluidization parameters, which may be controlled by a processor associated with the FBR.

[0147] The method then includes executing computer-executable code by a control optimization module to process the data, including one or more parameters representing real-time reactor subsystem outputs (and optionally in combination with other real-time data), thereby generating one or more control instructions. The control module is operated to send one or more control instructions to effect control of components within the pyrolysis system. This may include controlling either or both of the following: (i) A heating control system. For example, in some embodiments, this is a heating control system that controls the level of current and / or voltage applied to one or more electrodes, which in turn are configured to send current into the reactor chamber so that the current propagates through the conductive particulate material (thus producing heating within the reactor chamber). In some embodiments, control of the heating system is indirect and is performed by interaction with a separate reactor control module that controls the operation of the reactor subsystem (which, in some embodiments, is an FBR). For example, the FBR manipulates its heating controls (e.g., current sent to the electrodes) based on a specified temperature target, and the control commands sent by the control optimization module represent commands to adjust the target temperature. (ii) A particulate matter feed control system. The particulate matter feed control system is configured to control the metered delivery of the primary particulate material into the reactor chamber. For example, the particulate matter feed control system includes a quantity determination arrangement configured to measure the amount of the primary particulate material prior to direct / indirect delivery into the reactor chamber. In some embodiments, the particulate matter feed control system includes a particulate matter storage assembly coupled to the particulate matter feed assembly, wherein the particulate matter feed assembly includes a pre-feed pre-chamber configured to be selectively pressurized prior to delivery to the reactor chamber during delivery of the primary particulate material.

[0148] Preferably, the control optimization module and the control module are configured to be able to send control signals to both of these systems. However, it will be appreciated that the latter is of particular importance. It should be noted that the control optimization module need not be used strictly for "optimization" purposes, and that control may be implemented for a range of purposes, e.g., improvement, testing, start-up / shutdown, ramp-up / ramp-down, intentional deoptimization, etc. The label "optimization" in the "control optimization module" is merely representative.

[0149] There are various references to controlling current and / or voltage. It should be recognized that it may be advantageous to control one of these while leaving the other floating. For example, this may affect the rate of heating through the reactor chamber (i.e., fluidized bed); the superficial velocity of the particulate material affects the resistance and therefore the heating rate.

[0150] The concept of heat control as described herein is not limited to the control (direct or indirect) of the FBR heating system (e.g., current / voltage delivered through the electrodes). Heat control can also be achieved through other factors, such as reactor pressure (which affects resistivity), primary particle feed and particle extraction rates (e.g., the relative graphite purity in the chamber has a direct effect on resistivity).

[0151] The one or more control instructions include instructions to a reactor control system (i.e., a processor that controls the operating parameters of the fluidized bed reactor), thereby causing adjustments to any one or more of the heating, fluidization rate, and / or pressure.

[0152] The control optimization module, in some embodiments, is further configured to process data from one or more additional sources, which may include any one or more of: (i) a sensor configured to monitor temperature within the reactor chamber; (ii) an input representing a predicted future temperature within the reactor subsystem; (iii) an input representing one or more parameters derived from monitoring particulate matter detected in the reactor subsystem output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing a desired future operating condition of the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the reactor subsystem output.

[0153] In some embodiments where multiple real-time parameters are observed, a subset of one or more of those parameters are defined as target parameters and assigned target values / ranges. Control instructions are then defined based on an optimization method that attempts to manipulate and maintain the target parameters within the assigned target values / ranges. For example, the target parameters may include: (i) a desired hydrogen output parameter; (ii) a desired output carbon parameter; and (iii) a desired carbon output form.

[0154] Example pyrolysis framework 1 illustrates a system 110 for the conversion of a hydrocarbon feedstock 112 to hydrogen gas 114 and graphitic carbon 116. This is illustrated to provide a general example of a system to which the control optimization techniques described herein may optionally be applied. However, it should be understood that system 110 should not be treated as an unnecessarily limiting example. Additional disclosure regarding how the control optimization techniques may be implemented is provided further below, which again refers to the example of system 110.

[0155] The hydrocarbon feedstock 112 is optionally introduced into a current pre-reactor conditioner 118 adapted to condition the hydrocarbon feedstock 112 to produce a conditioned hydrocarbon feedstock 120. In a preferred embodiment, the hydrocarbon feedstock is selected from the group comprising methane, ethane, ethylene, propane and / or butane or mixtures thereof. In a preferred embodiment, the hydrocarbon feedstock consists essentially of one of methane, ethane, ethylene, propane or butane, preferably methane.

[0156] The pre-reactor conditioner 18 is adapted to perform one or more of heating, pressurizing, plasma treating, cooling, desulfurizing, drying, purifying, and expanding the hydrocarbon feedstock 12 to produce a conditioned hydrocarbon feedstock 20.

[0157] The pre-reactor conditioner is in communication with one or more reactors 26. The one or more reactors 26 are adapted to contact a prepared hydrocarbon feedstock 20 with a prepared iron oxide catalyst 29 at a temperature between 600°C and 1000°C (or higher) to produce a mixed-phase stream 30 containing hydrogen gas, graphitic carbon, and unreacted hydrocarbons. Each reactor 26 includes a catalyst inlet 32, a gas inlet 34, and a mixed-phase outlet 36. The pre-reactor conditioner generally increases the temperature and pressure of the hydrocarbon feedstock prior to injection into the one or more reactors 26.

[0158] In communication with catalyst inlet 132 is catalyst conditioner 137. Catalyst conditioner 137 is adapted to condition iron oxide catalyst 128 prior to entering one or more reactors 126 to produce conditioned iron oxide catalyst 129. It is contemplated that conditioning may include one or more of beneficiating, washing, drying, crushing, milling, sieving, purifying, and heating the catalyst.

[0159] Mixed-phase outlet 136 is in communication with post-reactor conditioner 142. Post-reactor conditioner 142 is adapted to condition mixed-phase stream 130 to produce conditioned mixed-phase stream 144. Post-reactor conditioner 142 may perform any one or more of dehydrating, cooling, and / or stripping volatiles from mixed-phase stream 130; preferably, post-reactor conditioner 142 cools and / or dehydrates mixed-phase stream 130.

[0160] The post-reactor conditioner 142 is in communication with one or more solid / gas separators 146. The one or more solid / gas separators 146 include an inlet 152, a gas outlet 164, a second gas outlet 163, and a solids outlet 156. The one or more solid / gas separators 146 are adapted to separate at least a portion of the conditioned mixed-phase stream 144 into a gas stream 148 comprising hydrogen gas and a solids stream 150 comprising graphitic carbon. The second gas outlet 163 may optionally be in communication with one or more of the pre-reactor conditioner 118, a reactor heater 165, and / or a generator 169, and it is envisioned that at least a portion of the gas stream 148 may be recycled. The generator 169 may optionally be used to provide electricity 180 to the reactor heater 165 or to other portions of the system, as needed.

[0161] The solids outlet 156 is in communication with a solids conditioner 158. The solids conditioner 158 is adapted to condition the solids stream 150 to produce the graphitic carbon stream 16. The solids conditioner 158 may perform one or more of the following conditioning functions for the solids stream 150: packaging (pelletizing, pressing), functionalizing, and / or purifying.

[0162] Gas outlet 154 is in communication with gas pre-separation conditioner 160, which includes conditioned gas outlet 161 such that at least a portion of gas stream 148 is conditioned to produce conditioned gas stream 162. Gas pre-separation conditioner 160 may perform any one or more of pressurization, cooling, and scrubbing / purification to remove impurities from gas outlet product 148; preferably, gas pre-separation conditioner 160 pressurizes and / or scrubs gas stream 148.

[0163] The gas pre-separation conditioner 160 is in fluid communication with a gas separator 164, which is adapted to separate and purify at least a portion of the components of the gas stream 162 to produce one or more purified gaseous product streams 166. At least one of the purified gaseous product streams 166 comprises hydrogen gas.

[0164] Gas separator 164 is in communication with a post-gas separation conditioner 168, which is adapted to condition purified gaseous product stream 166 to produce a purified form of hydrogen gas 114 and one or more conditioned gaseous streams 170, which may include one or more of CH, CO, CO, or a mixed gaseous stream. Purified hydrogen stream 114 may be connected to one or more gas storage tanks, piped to an end user, or optionally used as an energy means for one or each of one or more or all of conditioners 118, 142, 158, 160, 168 or reactor heater 165, or optionally fed to generator 169 for power generation. Reactor heater 165 may directly or indirectly heat reactor 126; a more extensive discussion of reactor heater technology is provided further below.

[0165] When the conditioned gaseous product stream 170 comprises a mixed gaseous stream of one or more of CO, CH, and CO, the mixed gaseous stream may also optionally be connected to a pre-reactor conditioner 18 for supply to one or more reactors as a hydrocarbon feedstock, or may optionally be supplied to a generator 169 for power generation. The generator 169 may optionally be used to provide electricity 180 to the reactor heater 165 or to other parts of the system as needed.

[0166] Sensors configured to collect data for the purposes of enabling control optimization may be located at a range of points throughout the system 110. It will be appreciated that this will be a matter of design choice based on (for example) the nature of the sensor, the parameter to be observed / determined, and the tolerable latency / delay from representing current reactor conditions.

[0167] With respect to heating, the system of FIG. 1 shows a reactor 126 and associated reactor heater 165, where the reactor is a fluidized bed reactor (FBR). In such a configuration, the reactor contents (e.g., including catalyst, carbon, methane, and hydrogen, collectively referred to as "process materials") are maintained in an agitated, fluidized state, such that the process materials are substantially homogenous throughout the reactor (i.e., preferably without substantial vertical or horizontal stratification). The manner in which the reactor heater is configured and controlled is related to the manner in which the reaction occurs within the reactor. The following heating techniques are optionally used in various embodiments (either separately or in combination):

[0168] Electrified bed heating In such a configuration, one or more electrodes, including, for example, one or more pairs of electrodes, are positioned within the FBR, thereby causing a current flow from a first electrode of a pair to a second electrode of that pair (optionally, with a given electrode forming part of multiple pairs). In such a configuration, there is a resulting current flow through the conductive carbon within the process material, which increases the temperature due to its resistive qualities. As a result, the conductive carbon essentially behaves as a resistive heating element (while in a homogeneous flow state within the FBR), causing overall heating of the process material. It should be noted that in some embodiments, there are an odd number of electrodes (e.g., three, optionally using alternating current), resulting in more than one pair of electrodes, plus additional electrodes.

[0169] In some embodiments, the positioning of the electrodes is configured to allow differential heating of separate zones / pathways within the FBR. This is optionally combined with internal sensors (e.g., zone-specific temperature sensors) and a control system configured to apply differential current flow within the zones (and / or along different paths) to thereby encourage modified fluid movement behavior within the process material. This may be used to achieve functions including optimizing temperature consistency and / or resolving identified tendencies toward stratification of the process material (e.g., by encouraging convective movement).

[0170] External resistance heating (hot wall) In this example, heat is applied directly through the sidewalls of the FBR, e.g., by an external resistive element. Heating of the process material in this case relies on the proximity or contact of the process material with the FBR sidewalls. This approach has the advantage of overall simplicity, but may have limitations in scale as the inner FBR radius increases (e.g., assuming that the heat applied through the sidewalls will increase to achieve the desired consistent temperature throughout the process material). Larger radii will require higher energy transfer through the walls, ultimately limited by material strength at elevated temperatures.

[0171] Internal resistance heating (cold wall) In this example, heat is applied via elements located within the central cavity of the FBR. The shape, location, and configuration of these elements may be tailored based on reactor size, for example, to promote efficient and consistent heating. A general principle of all heating examples described herein is the benefit associated with optimizing / limiting the temperature difference between (i) the outer surface of the heating element; and (ii) the target temperature of the process material (selected based on optimal reaction conditions and / or reaction conditions tailored to desired output results). The shape, location, and configuration of these elements may also be tailored based on other factors, for example, to promote agitation and / or homogeneity of the process material. For example, one preferred embodiment utilizes multiple heating elements shaped and / or positioned to promote movement of the process material within the FBR, thereby optimizing efficient and consistent heating throughout the process material.

[0172] Another preferred embodiment utilizes a single heating element having a complex three-dimensional shape (e.g., a helix or coil) that facilitates movement of the process material within the FBR, thereby optimizing efficient and consistent heating throughout the process material. In some embodiments, such a heating element may be included as one or more heating elements within the FBR to optimize heating of the process material. In some embodiments, the one or more heating elements are arranged in a double helix configuration or coil of different diameters. In some embodiments, the coil is in the form of a tight spiral (like a spring).

[0173] In certain embodiments, one or more heating elements are present within a larger heating element. In some embodiments, one or more heating elements are individually operable. In some embodiments, there are multiple individually controllable heating elements, each occupying a respective zone (optionally a vertically, radially defined, or zone based on another coordinate system) within the FBR, and each individually controllable, thereby enabling zone-specific heating or ensuring uniform heating of the process material. This is optionally combined with internal sensors (e.g., zone-specific temperature sensors) and a control system configured to apply differential temperatures between zones, thereby encouraging modified fluid movement behavior within the process material. This may be used to achieve functions including optimizing temperature consistency and / or resolving identified tendencies toward stratification of the process material (e.g., by encouraging convective movement).

[0174] In some embodiments, the process material, for example methane, may be inserted into the FBR at one or more insertion points.

[0175] induction heating In this example, a magnetic field is generated through extremal components of the FBR cavity (e.g., using a conductive coil through which an alternating current is passed), thereby inducing current flow within the process material, thereby heating the process material based on the conductive / resistive properties of the carbon. Additional details regarding possible induction heating arrangements are provided further below. This provides a form of "internal heating"—in the sense that heat is applied to the process material within the reactor sidewalls—using infrastructure external to the reactor sidewalls. In that regard, the conductive carbon within the process material essentially functions as an internal heating element.

[0176] It will be appreciated that eddy currents are induced in conductive materials.

[0177] In further embodiments, multiple FBR heating techniques and / or systems may be combined to achieve objectives including: (i) consistent heating within the process material; (ii) limiting the surface temperatures of internal components within the FBR cavity, thereby reducing the risk of surface carbon deposition; and (iii) zonal control, thereby promoting desired heating / convection / agitation effects.

[0178] Example control system configuration An example control system will now be described with reference to FIG.

[0179] FIG. 2 illustrates selected components of an example pyrolysis system for converting a hydrocarbon feedstock into hydrogen gas and graphitic carbon, which may be incorporated into and / or form part of the system of FIG. 1.

[0180] The pyrolysis system of Figure 1 includes a fluidized bed reactor (FBR) 201, the detailed configuration and control of an FBR for this purpose being outside the scope of this disclosure, however the main components will be described.

[0181] FBR 201 includes a body 202 that encloses a reactor chamber 203 within which a fluidized bed is maintained. In particular, input gas fluidization infrastructure 204 is configured to deliver a hydrocarbon feed 205 to an FBR input 206. FBR input 206 is coupled to FBR gas delivery components 207, which are configured to control the delivery of hydrocarbon feed 205 into reactor chamber 203 to maintain homogeneous fluidization of the process material contained therein.

[0182] The FBR 201 includes a heating infrastructure configured to maintain the process material within the reactor chamber 203 at a predetermined temperature (which may be a predetermined average temperature). The nature of the heating infrastructure is preferably current-carrying layer heating, whereby one or more electrodes, including, for example, one or more pairs of electrodes, are positioned within the FBR, thereby causing current flow from a first electrode of a pair to a second electrode of that pair (optionally, with a given electrode forming part of multiple pairs). In a preferred embodiment, there are three electrodes, and alternating current is used. In such a configuration, there is a resulting current flow through the conductive carbon within the process material, thereby increasing its temperature due to its resistive properties. As a result, the conductive carbon essentially behaves as a resistive heating element (while in a homogeneous flow state within the FBR), resulting in overall heating of the process material.

[0183] Other forms of heating may also be used, and options include (but are not limited to) one or more of the following: · External resistance heating (hot wall) where heat is applied directly through the side wall of the FBR, for example via an external resistance element. · Internal resistance heating (cold wall) where heat is applied via elements located within the central reactor chamber of the FBR. Induction heating, where a magnetic field is generated through extremal components of the FBR reactor chamber (e.g., using a conductive coil through which an alternating current is passed), thereby causing current flow within the process material, thereby heating the process material based on the conductive / resistive properties of the carbon. Additional details regarding possible induction heating arrangements are provided further below. This provides a form of "internal heating"—in the sense that heat is applied to the process material within the reactor sidewalls—using infrastructure external to the reactor sidewalls. In that regard, the conductive carbon within the process material essentially functions as an internal heating element.

[0184] In the illustrated example, the FBR 201 is coupled to an FBR control system 230 that controls various operating parameters, such as the operation of the heating infrastructure and the control of gas release / fluidization components.

[0185] FBR 201 further includes an output assembly 208 configured to enable release of output treatment material 209 to output treatment infrastructure 210. For example, output treatment infrastructure 210 may include various components for gas and solid separation, separation of hydrogen gas from other gases, filtering and separation of solids, and support of other downstream operations.

[0186] The system includes a primary particulate matter feed control system 212 configured to control the metered feed of primary particulate matter into the FBR 201. The exact characteristics (e.g., components and configuration) of the system 212 will vary from embodiment to embodiment, and the arrangement shown in Figure 1 is merely an example intended to demonstrate certain features.

[0187] As a core function, system 212 is configured to feed primary particulate material, optionally stockpiled in feed hopper 213, into the process material of FBR 201. This feeding is facilitated by various components, preferably components that allow for controlled metered feeding of the particulate material (e.g., by volume and / or weight). While the manner in which this is accomplished varies between embodiments, a common feature is preferably electronically controllable components that allow for computerized control of material feeding.

[0188] The primary particulate material may include catalytic particulate material, non-catalytic particulate material, or a combination thereof. For example: In some embodiments, the particulate material is a catalytic particulate material for methane pyrolysis in a fluidized bed reactor. In some embodiments, the catalytic particulate material is selected from the group comprising carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide. In certain embodiments, the particulate material is a non-catalytic particulate material selected to facilitate the pyrolysis of methane in the fluidized bed reactor. Preferably, this is a graphitic material, preferably flake graphite, selected from naturally occurring or synthetic graphite, for example. Preferably, a conductive form of carbon is used (e.g., when the fluidized bed reactor is heated by the flow (applied and / or induced) of electrical current through a conductive material within the fluidized bed reactor), although other forms of carbon may be used.

[0189] It will be understood that the selection of particulate material is a matter of design choice for a particular pyrolysis operation, and that the delivery techniques described herein are agnostic in that regard. In some cases, there are multiple hoppers containing different materials that are selectively made available to a single FBR. For operation of this embodiment, the reactor chamber requires a conductive particulate material for heating purposes; the primary particulate material delivered by system 212 may have the required conductive properties, or alternatively may acquire such conductive properties when introduced into the reactor chamber (such as with iron oxide that is reduced to iron and then encapsulated in carbon, thereby increasing the conductivity of the particulate).

[0190] In the example shown, hopper 213 is coupled to a first material feed control component 214 that controls the feeding of the primary particulate material from the hopper via a gravity feed arrangement to a metering chamber 216. Metering chamber 216 includes a conveyor 215 that controllably conveys the primary material into a pre-feed pre-chamber 218. Pre-feed pre-chamber 218 preferably has one or more sensors configured to measure (e.g., by weight or volume) the amount of particulate material in (or passing through) chamber 218. Chamber 218 (optionally together with chamber 216) can be pressurized, thereby preventing process material from exiting FBR reactor chamber 203 into chamber 218. For example, first seal 219 is maintained in a sealing configuration while chamber 218 is filled with a predetermined amount of particulate material, chamber 218 is pressurized, and then seal 219 is opened with seal 218 closed. In another embodiment, pressurization occurs between seal 219 and component 214, allowing for continuous metered delivery of particulate material under the influence of conveyor 215. These are just two possible arrangements of the physical infrastructure that allow for the controlled / metered delivery of particulate material into the FBR via one or more pressurized feed vestibules.

[0191] Figure 2 illustrates a system configured to enable optimization of the pyrolysis process in the form of a Pyrolysis Monitoring and Control System (PMCS) 220. PMCS 220 is preferably defined by one or more networked computing terminals that execute computer-executable code (software instructions) to thereby convey the functionality of the modules shown in Figure 2 and described below. The primary function of PMCS 220 is to control the delivery of particulate material into the reactor chamber of FBR 201. Other functions may optionally be performed, for example, as further described below.

[0192] The software running on the PMCS 220 will be described by reference to multiple "modules." The term "module" refers to a logically separable software component (computer program) or hardware component. The modules of the embodiments refer not only to modules within a computer program but also to modules within a hardware configuration. The description of the embodiments also serves as a description of the computer program that causes the modules to function (including programs that cause a computer to execute each step, programs that cause a computer to function as a means, and programs that cause a computer to perform each function), as well as a description of the system and method. For convenience of description, the phrases "storing information," "storing information," and other equivalent phrases are used. When the embodiment is a computer program, these phrases are intended to mean "storing information in a memory device" or "controlling a memory device to store information in the memory device." Modules may correspond to one-to-one functions. In executing software, one module may form one program, or multiple modules may form one program. One module may form multiple programs. Multiple modules may be executed by a single computer. A single module can be executed by multiple computers in a distributed or parallel environment. One module can include other modules. In the following description, the term "connection" refers not only to a physical connection but also to a logical connection (e.g., data exchange, command, and data reference relationship). The term "predetermined" means that something is determined prior to the target processing. Therefore, the term "predetermined" is intended to refer to something that is determined prior to the target processing in an embodiment. Even after the start of processing in an embodiment, the term "predetermined" refers to something that is determined prior to the target processing, depending on the conditions or states of the current embodiment or on the conditions or states that continue from the previous time to the present. When there are multiple "predetermined values," the predetermined values ​​may be different from each other, or two or more predetermined values ​​(including all values) may be equal to each other.The statement "If A, then B is done" is intended to mean "It is determined whether something is A, and if it is determined that something is A, then action B is performed." The statement would be meaningless if the determination regarding whether something is A was not performed.

[0193] In each process performed by the module, or in one of the processes performed by the module, information to be processed is read from the memory device, then the information is processed, and the processing result is written to the memory device. Descriptions of reading information from the memory device before processing and writing the processed information to the memory device after processing may be omitted as appropriate. The memory device may include a hard disk, a random access memory (RAM), an external storage medium, a memory device connected by a communication network, and a ledger in a CPU (central processing unit).

[0194] PMCS 220 includes one or more modules configured to receive input data from one or more sensors configured to monitor the output of FBR 201. In the illustrated example, it includes a sensor input module 221, which is configured to receive data from hydrogen sensor 211 a that monitors hydrogen in the output feed from FBR 201 and particulate sensor 211 b that monitors an indication of particulate output from FBR 201 (e.g., as described further above). Sensor input module 221 is configured to process its inputs and thereby determine one or more parameters indicative of hydrogen and / or particulate output from the fluidized bed reactor output (e.g., any one or more of: percentage of output gas / material defined by hydrogen and hydrogen throughput as a function of time, particle size / particle morphology, particulate throughput quantities, and other parameters).

[0195] The PMCS includes a component that operates as a control optimization module that is responsive to one or more parameters representative of the fluidized bed reactor output to generate one or more control instructions. In the example shown, this is provided as functionality of control optimization module 223. In this regard, processing module 223 is configured to apply one or more algorithms (or other computerized processes) to thereby receive inputs including data representative of one or more parameters representative of the hydrogen output, and output data from those algorithms representing instructions for control system 212 (and optionally other controllable components in the broader pyrolysis system). For example, based on inputs including the detected hydrogen level, module 212 outputs data representing instructions to do one or more of the following: · Increased rate at which particulate material is delivered to the FBR. · Increased rate at which particulate material is delivered to the FBR. Delivery of pre-defined sized batches of particulate material to the FBR at defined times (defined times may be scheduled or essentially "immediate"). · Switching between particulate materials and / or adjusting the ratio of different particulate materials, if there are multiple hoppers 213 containing different particulate materials.

[0196] Module 212 may also provide control instructions for other components, such as FBR control system 230 (e.g., providing instructions regarding heating, e.g., temperature set points, instructions regarding fluidization parameters, etc.). In some embodiments, module 212 is configured to directly control the heating and / or fluidization infrastructure.

[0197] Control command delivery module 224 is configured to apply the control commands defined by processing module 224, which in the illustrated example includes transmitting the control commands to feed system 212. Module 224 preferably does so based on a number of predefined rules that enable an algorithmic decision as to whether (and optionally when) to execute the control commands, based, for example, on safety and other factors. For example, module 224 may have access to data including the availability of material in hopper 212, scheduled shutdowns and other operations, inputs from other sensors in the wider system, etc.

[0198] In the illustrated example, control instruction execution module 224 interacts with primary material delivery module 225 and secondary material delivery module 226, thereby providing physical, real-world effects to the control instructions. The former accesses controllable components (e.g., valves, sensors, pressurized components, etc.) associated with chamber 218, while the latter accesses controllable components (e.g., component 214 and other valves, sensors, pressurized components, etc.) associated with chamber 216. This is by way of example only; the manner in which modules within control system 220 provide control instructions to components within system 212 will vary from embodiment to embodiment depending on the specifics of system 212 and its operation. This can range in complexity significantly (e.g., from simple embodiments in which system 212 can receive instructions referencing particulate material emission rates, to complex embodiments in which the constituent controllers within system 212 require individual control / actuation).

[0199] The control instructions generated by control optimization module 224 and executed by execution module 224 may, in further embodiments, relate to components other than those belonging to system 12. For example, system 220 may include other input module 220 that receives data from other sensors associated with the FBR or other pyrolysis system components, and data input from other sources (e.g., desired operating characteristics, scheduled operating factors, such as shutdowns, etc.). That is, PMCS 220 may further (as an optional feature) include other input module 222 configured to monitor other outputs and / or operating parameters of FBR 201. This may include any one or more of the following: · Input obtained from a sensor configured to monitor the temperature within the fluidized bed reactor. · An input representing the predicted future temperature in the fluidized bed reactor. · Input representing one or more parameters derived from monitoring of particulate matter detected at the fluidized bed reactor output (e.g., carbon purity, carbon form, particle size, etc.). · Inputs representing one or more desired parameters regarding the particulate matter detected in the fluidized bed reactor output (e.g., carbon purity, carbon form, particle size, etc.). Inputs representing one or more desired parameters for hydrogen output. Inputs representing one or more input gas delivery parameters. Inputs representing desired future operating conditions for the fluidized bed reactor (e.g., planned outages). Inputs representing one or more parameters related to gases other than hydrogen detected at the fluidized bed reactor output.

[0200] Further, as noted, modules 223 and 224 may additionally / alternatively be configured to generate and execute control instructions for components other than those of system 12 (optionally including FBR components, e.g., heating infrastructure, and / or other components within the broader pyrolysis system).

[0201] The manner in which the processing module 223 operates varies from embodiment to embodiment based on a range of factors (e.g., FBR size / shape, facility objectives, input gas parameters, catalytic / non-catalytic material properties, etc.). Broadly, the following approaches may optionally be used: A rule-based algorithmic approach in which logical rules are generated that equate predefined inputs (e.g., hydrogen throughput rates, desired output carbon forms, and other desired operating parameters) with control commands. AI / machine learning-driven approaches, whereby a software module is trained based on training data to receive inputs (e.g., hydrogen throughput rate, desired output carbon morphology, and other desired operating parameters) and executes AI / machine learning-based processing to send outputs representing control commands. For example, a neural network can be trained based on input data collected from the historical operation of one or more similar methane pyrolysis systems, where the training data includes components representing particulate matter feed (e.g., catalyst feed) into the FBR, along with past / future time-series data representing operating parameters (e.g., hydrogen throughput). This, again by way of example, can be used to train a neural network to receive as input current data representing FBR operation, including hydrogen throughput, and provide outputs representing the amount of particulate material (e.g., known catalyst material) to feed to the FBR, thereby resulting in maximum hydrogen throughput. Such a neural network can also be trained to thereby enable control of the carbon morphology produced within the FBR (although in that situation control of FBR temperature is relevant in addition to control of the particulate feed rate).

[0202] In the latter case, there is preferably a continuous generation of training data, thereby facilitating continuous learning and optimization of the controls for a particular pyrolysis system over the course of its operation.

[0203] Example Control Rules Below are some example control rules, which may be implemented in combination, by the system of Figure 2 and / or by the processes / methods described herein: If the hydrogen output is below a threshold, generate an instruction to perform a one-time insertion of a specified amount of primary particulate material. If the hydrogen output is below a threshold, generate a command to increase the insertion rate of the primary particulate material. If the hydrogen output is below a threshold, generate a command to increase the reactor chamber temperature target. If the hydrogen output is below a threshold, generate a command to increase the current to the reactor chamber electrodes. If the hydrogen output is below a threshold, generate instructions to adjust the degree of agitation / fluidization in the reactor. If the particulate material output is below a threshold, generate an instruction to perform a one-time insertion of a specified amount of primary particulate material. If the particulate material output is below a threshold, generate a command to increase the insertion rate of the main particulate material. If the particulate material output is below a threshold, generate a command to increase the reactor chamber temperature target. If the particulate material output is below a threshold, generate a command to increase the current to the reactor chamber electrodes. If the particulate material output is below a threshold, generate instructions to adjust the degree of agitation / fluidization in the reactor. If the average size of the particulate material from the output is above a threshold, generating an instruction to perform a one-time insertion of a defined amount of primary particulate material. · If the average size of the particulate material from the output is above a threshold, generate a command to increase / decrease the insertion speed of the main particulate material. · Generates commands to increase / decrease reactor chamber temperature target if the average size of particulate material from the output is above a threshold. If the average size of particulate material from the output is above a threshold, generate a command to increase / decrease the current to the reactor chamber electrodes. If the average size of particulate material from the output is above a threshold, generate instructions to adjust the degree of agitation / fluidization in the reactor. If the particulate material morphology in the output is outside of a specified target range, generate an instruction to perform a one-time insertion of a specified amount of primary particulate material. Generates commands to increase / decrease the insertion rate of the main particulate material if the particulate material morphology during output is outside of the specified target range. Generates commands to increase / decrease reactor chamber temperature target if particulate material morphology in the output is outside of the specified target range. Generates commands to increase / decrease current to reactor chamber electrodes if particulate material morphology in the output is outside of a specified target range. Generates instructions to adjust the degree of agitation / fluidization in the reactor if the particulate material morphology in the output is outside of a specified target range.

[0204] It will be understood that these are examples only, and that in practice optimization and / or machine learning techniques are optionally used to configure processing logic to optimize pyrolysis performance based on one or more target parameter values.

[0205] Figure 4 provides additional details regarding the relationship between example controlled and manipulated variables in situations where the controlled variables are above or below specified thresholds. In this example, the controlled variables are: · Catalyst to gas ratio in the reactor chamber. Purity of hydrogen in the output. Methane (or other hydrocarbon) conversion. Hydrogen generation. Reactor chamber temperature. Reactor superficial velocity (with respect to particulates). · Layer level within the FBR. Gas residence time in the reactor chamber. · Graphite purity in the reactor output. · Graphite morphology in the reactor output. Heat input to the reactor chamber. Bed resistivity within the reactor chamber.

[0206] An example manipulated variable is: · Feed rate: The rate at which the gaseous hydrocarbon feedstock is fed into the reactor. · Catalyst addition rate: The rate at which catalytic activity (i.e., primary particulate material) is introduced into the reactor chamber. · Pressure in the reactor chamber. · The voltage and / or current applied to the heating electrode.

[0207] The table in Figure 4 provides a representation of example relationships between controlled and manipulated variables. The control techniques described herein are configured to control (directly and / or indirectly) some or all of the manipulated variables based on measured and / or target values ​​for some or all of the controlled variables. For example, this can be facilitated by applying known techniques such as Dynamic Matrix Control (DMC) and / or Real Time Optimization (RTO). DMC is a multivariable optimization software program that sits on top of regulatory control, pushing variables in certain directions based on a predefined set of relationships between variables and prioritization inputs. RTO is a basic chemical engineering-based model that adjusts limits and priorities within DMC based on economic optimization signals and an understanding of the process optimum (DMC does not assume optimum; it is constraint-based). Alternatively, other proprietary software approaches can be implemented.

[0208] From the table in FIG. 4, the following example control instructions can be obtained: Generates a command to increase the feed rate if the catalyst to gas ratio is above a threshold If the hydrogen purity is above a threshold, generate a command to increase the supply rate. If methane conversion is above a threshold, generate a command to increase the feed rate If hydrogen production exceeds a threshold, generate a command to increase the supply rate Generates a command to increase the feed rate if the reactor temperature exceeds a threshold Generates a command to reduce the feed rate if the reactor superficial velocity is above a threshold Generates instructions to increase or decrease the feed rate if the bed level is above a threshold Generates a command to increase the supply rate if the gas residence time exceeds a threshold Generates a command to increase the feed rate if the graphite purity is above a threshold If the heat input exceeds a threshold, generate a command to increase the feed rate Generates a command to reduce the feed rate if the layer resistivity is above a threshold Generates a command to reduce the catalyst addition rate (i.e., primary particulate material addition rate) if the catalyst to gas ratio is above a threshold value If the hydrogen purity is above a threshold, generate a command to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate). If methane conversion is above a threshold, generate commands to increase or decrease the catalyst addition rate (i.e., primary particulate material addition rate). If hydrogen production exceeds a threshold, generate a command to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate). Generate a command to increase the catalyst addition rate (i.e., primary particulate material addition rate) if the reactor temperature is above a threshold value Generates a command for the catalyst addition rate (i.e., primary particulate material addition rate) if the reactor superficial velocity is above a threshold value Generates a command to reduce the catalyst addition rate (i.e., primary particulate material addition rate) if the bed level is above a threshold Generate a command to reduce the catalyst addition rate (i.e., primary particulate material addition rate) if the gas residence time is above a threshold If the graphite purity is above a threshold, generate a command to increase the catalyst addition rate (i.e., the primary particulate material addition rate). Generates a command to increase the catalyst addition rate (i.e., primary particulate material addition rate) if the heat input exceeds a threshold. If the bed resistivity is above a threshold, generate a command for the catalyst addition rate (i.e., the primary particulate material addition rate). Generates a command to reduce pressure if the catalyst to gas ratio is above a threshold Generates commands to increase or decrease pressure if hydrogen purity is above a threshold Generates commands to increase or decrease pressure if methane conversion exceeds a threshold Generates commands to increase or decrease pressure if hydrogen production exceeds a threshold Generates commands to increase or decrease pressure if reactor temperature exceeds threshold Generates a command to increase pressure if the reactor superficial velocity exceeds a threshold Generates commands to increase or decrease pressure if the bed level is above a threshold Generates a command to increase or decrease pressure if the gas residence time exceeds a threshold Generates commands to increase or decrease pressure if graphite purity is above a threshold Generates commands to increase or decrease pressure if heat input exceeds a threshold Generates commands to increase or decrease pressure if the layer resistivity exceeds a threshold. Generates a command to reduce voltage or current if the catalyst to gas ratio exceeds a threshold. If the hydrogen purity is above a threshold, generate a command to reduce the voltage or current. Generates a command to reduce voltage or current if methane conversion exceeds a threshold Generates a command to reduce voltage or current if hydrogen production exceeds a threshold Generates a command to reduce voltage or current if the reactor temperature exceeds a threshold. Generates a command for voltage or current if the reactor superficial velocity exceeds a threshold Generates a command to reduce voltage or current if the layer level is above a threshold Generate a command to reduce voltage or current if the gas residence time exceeds a threshold. Generates a command to reduce voltage or current if graphite purity is above a threshold Generates a command to reduce voltage or current if the heat input exceeds a threshold Generate a command to reduce voltage or current if the layer resistivity exceeds a threshold Generates a command to reduce the feed rate if the catalyst to gas ratio is above a threshold Generates a command to reduce the supply rate if the hydrogen purity is above a threshold Generates a command to reduce the feed rate if methane conversion exceeds a threshold If hydrogen production exceeds a threshold, generate a command to reduce the supply rate Generates a command to reduce the feed rate if the reactor temperature exceeds a threshold Generates a command to increase the feed rate if the reactor superficial velocity is above a threshold Generates instructions to increase or decrease the feed rate if the bed level is above a threshold Generates a command to reduce the supply rate if the gas residence time exceeds a threshold Generates a command to reduce the feed rate if the graphite purity is above a threshold If the heat input exceeds a threshold, generate a command to reduce the supply rate If the layer resistivity is above a threshold, generate a command to increase the feed rate Generate a command to increase the catalyst addition rate (i.e., primary particulate material addition rate) if the catalyst to gas ratio is above a threshold. If the hydrogen purity is above a threshold, generate a command to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate). If methane conversion is above a threshold, generate commands to increase or decrease the catalyst addition rate (i.e., primary particulate material addition rate). If hydrogen production exceeds a threshold, generate a command to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate). Generates a command to slow down the catalyst addition rate (i.e., primary particulate material addition rate) if the reactor temperature is above a threshold value Generates a command for the catalyst addition rate (i.e., primary particulate material addition rate) if the reactor superficial velocity is above a threshold value If the bed level is above a threshold, generate a command to increase the catalyst addition rate (i.e., the primary particulate material addition rate). Generate a command to increase the catalyst addition rate (i.e., primary particulate material addition rate) if the gas residence time is above a threshold. Generates a command to slow down the catalyst addition rate (i.e., primary particulate material addition rate) if the graphite purity is above a threshold value Generates a command to slow down the catalyst addition rate (i.e., primary particulate material addition rate) if the heat input is above a threshold If the bed resistivity is above a threshold, generate a command for the catalyst addition rate (i.e., the primary particulate material addition rate). Generates a command to increase pressure if the catalyst to gas ratio is above a threshold Generates commands to increase or decrease pressure if hydrogen purity is above a threshold Generates commands to increase or decrease pressure if methane conversion exceeds a threshold Generates commands to increase or decrease pressure if hydrogen production exceeds a threshold Generates commands to increase or decrease pressure if reactor temperature exceeds threshold Generates a command to reduce pressure if the reactor superficial velocity exceeds a threshold Generates commands to increase or decrease pressure if the bed level is above a threshold Generates a command to increase or decrease pressure if the gas residence time exceeds a threshold Generates commands to increase or decrease pressure if graphite purity is above a threshold Generates commands to increase or decrease pressure if heat input exceeds a threshold Generates commands to increase or decrease pressure if the layer resistivity exceeds a threshold. Generates a command to increase voltage or current if the catalyst to gas ratio exceeds a threshold. Generates a command to increase voltage or current if hydrogen purity is above a threshold Generates a command to increase voltage or current if methane conversion exceeds a threshold If hydrogen production exceeds a threshold, generate a command to increase voltage or current Generates a command to increase voltage or current if the reactor temperature exceeds a threshold Generates a command for voltage or current if the reactor superficial velocity exceeds a threshold If the layer level is above a threshold, generate a command to increase the voltage or current Generate a command to increase voltage or current if the gas residence time exceeds a threshold If the graphite purity is above a threshold, generate a command to increase the voltage or current Generates a command to increase voltage or current if the heat input exceeds a threshold Generate a command to increase voltage or current if the layer resistivity exceeds a threshold

[0209] Again, it should be understood that these are examples only.

[0210] Example current-carrying layer heating configuration FIG. 3A shows a diagram of a system 300 including an inductively heated FBR configured to operate in conjunction with methane pyrolysis as disclosed in the example of FIG.

[0211] In this example, the refractory-lined FBR 301 has three electrodes (302A-C) that extend into the reactor chamber and are exposed within the fluidized bed of hydrocarbon gas and particulate material (including conductive particulates). In this manner, electrical current flowing between the electrodes is conducted through the conductive particulates, heating them and, thereby, heating the entire contents of the reactor chamber as a result of conductivity and fluidization.

[0212] Although three electrodes are shown, other numbers may be used and their locations may vary in different embodiments. In some embodiments, the FBR shell is used as an additional electrode.

[0213] In operation, a high voltage power supply 310 operates in conjunction with a transformer 311 and a thyristor controller 312 (for current, voltage and power). The thyristor controller is operated with an alternating voltage, either single phase or three phase, which passes through the low voltage cable and sends current across the electrodes, optionally as AC or DC (depending on implementation choice).

[0214] In use, a feed gas supply 314 delivers hydrocarbons to the FBR 301. A specific material delivery system (not shown), such as that shown in Figure 2, delivers a controlled / metered feed of particulate material that acts as a catalyst for hydrocarbon pyrolysis within the FBR. An output 315 of product gas (including hydrogen) and particulate material (including graphite) is released from the FBR.

[0215] Example induction heating configuration FIG. 3B shows a simplified cross-sectional view of a system 350 including an inductively heated FBR configured to operate in conjunction with methane pyrolysis as disclosed in the example of FIG.

[0216] System 350 includes a sidewall 351, which is preferably cylindrical and formed of a sturdy material selected from a group including metals such as steel. The height of the sidewall may vary depending on the embodiment. Within the sidewall is a sidewall cavity 352, a refractory reactor housing 353 (e.g., a silica refractory material suitable for insulating the sidewall from excessive heat and also enclosing / supporting a conductive coil), which defines a central cavity 354 within which a fluidized bed is maintained (fluidization components not shown).

[0217] The cavity 354 has a plurality of connection ports, not shown, including: (i) at least one first inlet, preferably at or adjacent the lower end, for delivering a feed gas containing a hydrocarbon gas, e.g., methane (not shown), (ii) a second inlet, preferably at or adjacent the upper end, for delivering a raw material of starting material, e.g., graphitic material, Hazer graphite, ion-containing catalyst (e.g., iron ore or synthetic iron oxide); and (iii) an outlet for discharging treatment material, including particulates (including carbon) and gases (including hydrogen). The coil may also be embedded in refractory.

[0218] An electrically conductive coil 355 is housed within sidewall cavity 352 such that the coil is positioned adjacent to refractory reactor housing 353. The coil is configured to carry alternating current delivered by radio frequency power supply 358 and input / output connections 356 and 357. The coil includes a central cavity through which a cooling fluid (e.g., water) is configured to flow, thereby preventing the coil from reaching undesirable temperatures during use. The coil is spaced from steel sidewall 351 by a threshold distance to prevent inductive heating of the sidewall (this distance varies depending on the embodiment and is selected depending on factors including the overall system dimensions and current handling parameters). In some embodiments, the system includes multiple electrically conductive coils. In some embodiments, each of the multiple electrically conductive coils is independently operable.

[0219] The alternating current conducted through the coil 355 creates induction within the treatment material, resulting in current flow throughout the conductive carbon particles of the treatment material. Electrical resistance within the carbon particles causes them to heat, and therefore the entire treatment material, thereby bringing the treatment material to and maintaining it within the desired temperature range of approximately 600-1500 degrees.

[0220] Preferably, one or more temperature sensors are configured to monitor the temperature within the treatment material fluidized within the central lumen 354 and pass the temperature data to the controller 359. The controller 359 executes software instructions configured to effect control of the radio frequency power supply 358 based on the temperature sensor data, thereby maintaining the treatment material within a desired temperature range.

[0221] The use of induction heating in the context of the present fluidized bed methane pyrolysis reaction is particularly advantageous because, unlike the other heating options mentioned above, induction heating avoids the presence of components / areas where localized surface temperatures reach levels where carbon deposition occurs.

[0222] In some cases, methods of controlled heating of process materials within reactors, particularly fluidized bed reactors, are used to enable process improvements. This allows for a range of benefits, as described below, including (but not limited to) mitigation of problems with unwanted carbon surface deposition, the ability to adjust catalyst input, control of residence time, and control of product (e.g., carbon, particularly various forms of graphitic carbon, and hydrogen) purity. Other benefits may include greater scaling capabilities, better temperature control, simpler construction, and greater energy efficiency.

[0223] Generally, the underlying pyrolysis method includes a method for hydrocarbon gas pyrolysis, the method including: providing an initial feedstock of conductive carbon material into a fluidized bed reactor; commencing operation of the fluidized bed reactor, the fluidized bed reactor being fed with an input of hydrocarbon gas; operating a power source, thereby sending electrical current (by controlling the current and / or voltage) to one or more electrodes and / or conductive coils, thereby heating the conductive carbon material to a predetermined temperature that initiates and maintains the pyrolysis of the hydrocarbon gas; and operating an outlet component, thereby discharging process material from the fluidized bed reactor, wherein the discharged process material includes the carbon material, unreacted hydrocarbon gas, and / or hydrogen gas.

[0224] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coal seam gas, landfill gas, and biogas. The composition of the hydrocarbon gas can vary widely, but generally comprises one or more light hydrocarbons from the group comprising methane, ethane, ethylene, propane, and butane. In a preferred embodiment, the hydrocarbon gas is selected from the group comprising methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In a preferred embodiment, the hydrocarbon gas consists essentially of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0225] In a preferred embodiment, the hydrocarbon gas is natural gas.

[0226] In a preferred embodiment, the hydrocarbon gas is biogas.

[0227] In a preferred embodiment, the hydrocarbon gas consists essentially of methane.

[0228] The outlet component can be operated in a controlled or uncontrolled manner. In one embodiment, it is uncontrolled (solids flow from the reactor is the result of particle elutriation). Therefore, the elutriation rate depends on the geometry and overall design. Other means of operating the outlet component are contemplated.

[0229] In one embodiment of the invention, the FBR is operated above atmospheric pressure. In one embodiment of the invention, the FBR is operated at a pressure between about 0 bar and 100 bar. Preferably, the pressure is between about 0 bar and 50 bar. More preferably, the pressure is between 0 bar and 20 bar. Even more preferably, the pressure is between about 2 bar and 10 bar.

[0230] In one embodiment of the present invention, the predetermined temperature is about 600°C to 1500°C. Preferably, the predetermined temperature is about 600°C to 1200°C. More preferably, the predetermined temperature is about 800°C to 1200°C. Even more preferably, the predetermined temperature is about 900°C. Even more preferably, the predetermined temperature is about 1000°C. Even more preferably, the predetermined temperature is about 1100°C. Even more preferably, the predetermined temperature is about 1200°C.

[0231] In one embodiment of the present invention, the average temperature is about 600°C to 1500°C. Preferably, the average temperature is about 600°C to 1200°C. More preferably, the average temperature is about 800°C to 1200°C. Even more preferably, the average temperature is about 900°C. Even more preferably, the average temperature is about 1000°C. Even more preferably, the average temperature is about 1100°C. Even more preferably, the average temperature is about 1200°C.

[0232] In certain embodiments, the purity of the graphite starting material is greater than about 95% w / w. Preferably, the purity of the graphite starting material is greater than about 99% w / w. More preferably, the purity of the graphite starting material is greater than about 99.5% w / w. Most preferably, the purity of the graphite starting material is greater than about 99.9% w / w.

[0233] In certain embodiments, the purity of the graphite starting material is about 50% w / w. Preferably, the purity of the graphite starting material is greater than about 60% w / w. More preferably, the purity of the graphite starting material is greater than about 70.5% w / w. Most preferably, the purity of the graphite starting material is greater than about 80% w / w.

[0234] In certain embodiments, the purity of the recycled graphite material is greater than about 95% w / w. Preferably, the purity of the recycled graphite material is greater than about 99% w / w. More preferably, the purity of the recycled graphite material is greater than about 99.5% w / w. Most preferably, the purity of the recycled graphite material is greater than about 99.9% w / w.

[0235] In one aspect of the present invention, the metal-containing catalyst is a synthetic metal-containing catalyst. Throughout this specification, unless the context requires otherwise, the term "synthetic" is understood to include the meaning that the material is synthesized by chemical techniques. Synthetic metal-containing catalysts are generally of high purity.

[0236] In one aspect of the invention, the synthetic iron-containing catalyst is a synthetic iron oxide-containing material. In one aspect of the invention, the iron oxide is a synthetic metal-containing catalyst and is Fe2O3 or Fe3O4.

[0237] In an alternative form of the invention, the ion-containing catalyst is non-synthetic. Throughout this specification, unless the context requires otherwise, the term "non-synthetic" is understood to include the meaning that the material has not been synthesized by chemical techniques. The term "non-synthetic" includes naturally occurring materials, but should not be understood to exclude materials that have been subjected to physical beneficiation, such as crushing and sieving or classification.

[0238] In one embodiment of the present invention, the ion-containing catalyst is a non-synthetic iron oxide-containing material. In one embodiment of the present invention, the ion-containing catalyst is a non-synthetic iron oxide-containing ore. In one embodiment of the present invention, the non-synthetic iron oxide-containing ore is iron ore. The iron ore may be hematite iron ore or goethite iron ore. The iron ore may be low-grade iron ore.

[0239] In one aspect of the present invention, the ion-containing catalyst may undergo a pretreatment step to enhance its catalytic effectiveness. The pretreatment step may include pre-reduction at elevated temperatures. Advantageously, the inventors have discovered that the present invention may obviate the need for such a pretreatment step.

[0240] As will be appreciated by those skilled in the art, graphitic materials come in many forms, such as: Graphite fibers, which are fibrous carbon structures generally ranging in length from 100 nm to 100 microns; carbon nanotubes (CNTs), which are cylindrical nanostructures containing single or multiple graphite sheets aligned concentrically or perpendicular to a central axis, also fall within the scope of graphite fibers; Carbon nano-onions (CNOs), which are structures consisting of multiple spherical graphite sheets layered concentrically from a central core, which is generally a catalyst particle or void. These carbon structures generally range in diameter from 50 to 500 nm; Carbon microspheres (CMS), which are hollow spherical graphitic structures generally greater than 500 nm in size. They can be spherical in shape and chain-like. This synthetic form of graphite is novel and has only been found naturally occurring in meteorites; and Graphene, a single layer or single-digit layer sheet of graphite It can exist in

[0241] In some embodiments, the carbon material is selectively synthesized to have substantially one or more desired morphologies. In preferred embodiments of the invention, the desired morphologies are selected from the group consisting of graphite fibers, carbon nano-onions (CNO), carbon microshells (CMS), and graphene. More preferably, the graphite fibers comprise a mixture of carbon nanotubes (CNT) and other graphite fibers. In preferred embodiments of the invention, the desired morphologies are selected from one or more of the group consisting of graphite fibers, carbon nano-onions (CNO), carbon microshells (CMS), and graphene. In some embodiments, the desired morphologies are substantially composed of graphite fibers. In some embodiments, the desired morphologies are substantially composed of carbon nano-onions (CNO). In some embodiments, the desired morphologies are substantially composed of carbon microshells (CMS). In some embodiments, the desired morphologies are substantially composed of graphene.

[0242] The use of current-based heating in FBRs allows multiple reaction pathways to be extended beyond the use of iron ore catalysts as described with respect to Figure 1. These are: (1) Utilizing an iron-embedded carbon feedstock in conjunction with iron ore catalyst. Iron ore catalysis allows the pyrolysis reaction to occur at relatively low temperatures (e.g., approximately 900°C), allowing carbon to grow on the iron ore particles. With iron ore catalysis, the catalyst is not consumed in the reaction but becomes incorporated into the carbon and is removed from the reactor in the extracted carbon particles, requiring continuous or periodic replenishment. (2) Utilizing an iron-embedded carbon feedstock in conjunction with iron ore catalyst. Iron ore catalysis allows the pyrolysis reaction to occur at relatively low temperatures (e.g., approximately 900°C), allowing carbon to grow on the iron ore particles. With iron ore catalysis, the catalyst is not consumed in the reaction but becomes incorporated into the carbon and is removed from the reactor in the extracted carbon particles, requiring continuous or periodic replenishment. (3) Utilizing a graphite feedstock at the beginning of the reaction, the reaction is operated at a high temperature in a non-catalytic state. For example, induction heating can be used to raise the process material temperature to above 1000°C, preferably above 1100°C. Under these conditions, the hydrocarbon feed gas decomposes into hydrogen and carbon, allowing the carbon to grow on the flake graphite feedstock. The resulting larger carbon particles are extracted along with the output process material, and preferably; at least a portion of this is processed back into the graphite feedstock for reintroduction into the reactor. The control system is configured to input additional graphite feedstock into the reactor either continuously or periodically, thereby providing a substrate on which carbon can deposit during the pyrolysis reaction.

[0243] The latter option has advantages in that the reaction itself can generate a continuous supply of graphite feedstock and the purity level of the carbon extracted from the FBR can be maintained at a very high level.

[0244] In some embodiments, the systems or methods of the present invention comprise multiple reactors, hi some embodiments, the multiple reactors are arranged in series or in parallel.

[0245] Conclusion and Interpretation It will be appreciated that the above disclosure provides useful improvements in the context of methane pyrolysis technology.

[0246] Although specific embodiments of the present invention have been described, those skilled in the art will recognize that there are other embodiments that are equivalent to the described embodiments. It is therefore to be understood that the present invention is not limited by the specifically illustrated embodiments, but only by the scope of the appended claims.

[0247] In the foregoing description of exemplary embodiments of the invention, it should be understood that various features of the invention are sometimes grouped together in a single embodiment, figure, or description thereof for the purpose of streamlining the disclosure and aiding in understanding one or more of the various inventive aspects. This method of disclosure, however, is not to be interpreted as reflecting an intention that the claimed invention requires more features than are expressly recited in each claim. Rather, as reflected in the following claims, inventive aspects lie in less than all features of a single foregoing disclosed embodiment. Thus, the claims following the Detailed Description are hereby expressly incorporated into this Detailed Description, with each claim standing on its own as a separate embodiment of this invention.

[0248] Furthermore, some embodiments described herein include some features included in other embodiments but not other features, and as will be understood by those skilled in the art, combinations of features from different embodiments are intended to be within the scope of the present invention and form different embodiments. For example, in the following claims, any of the claimed embodiments can be used in any combination.

[0249] Furthermore, some of the embodiments are described herein as methods or combinations of method elements that can be performed by a processor of a computer system or other means for performing functions. Thus, a processor with the necessary instructions for carrying out such a method or method element forms a means for carrying out the method or method element. Furthermore, the elements described herein of apparatus embodiments are examples of means for performing the functions performed by the elements for the purpose of implementing the invention.

[0250] In the description provided herein, numerous specific details are set forth. However, it will be understood that embodiments of the present invention may be practiced without these specific details. In other instances, well-known methods, structures and techniques have not been shown in detail in order not to obscure an understanding of this description.

[0251] Similarly, it should be noted that the term coupled, when used in the claims, should not be interpreted as being limited to only direct connections. The terms "coupled" and "connected," along with their derivatives, may be used. It should be understood that these terms are not intended to be synonyms for each other. Thus, the scope of the phrase device A coupled to device B should not be limited to devices or systems in which the output of device A is directly connected to the input of device B. It means that there is a path between the output of A and the input of B, which may be a path that includes other devices or means. "Coupled" can mean that two or more elements are in direct physical or electrical contact, or that two or more elements are not in direct contact with each other, but still cooperate or interact with each other.

[0252] Thus, while what are believed to be preferred embodiments of the present invention have been described, those skilled in the art will recognize that other and further modifications may be made without departing from the spirit of the present invention, and it is intended to claim all such changes and modifications as being within the scope of this invention. For example, any routines given above are merely representative procedures that may be used. Functions may be added or deleted from the block diagrams, and operations may be interchanged between functional blocks. Steps may be added or deleted to methods described within the scope of the present invention.

Claims

1. 1. A method for controlling a hydrocarbon gas pyrolysis system, the hydrocarbon gas pyrolysis system including a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the method comprising: receiving time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; processing the time series input data to thereby determine one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of a real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; operating a control optimization module based on the computer executable code to process data including the one or more parameters representative of real-time reactor subsystem outputs, thereby generating one or more control instructions; Operate a control module, thereby sending said one or more control instructions: (i) a heating control system that controls a level of current and / or voltage applied to one or more electrodes configured to transmit electrical current into the reactor chamber such that the electrical current propagates through the conductive particulate material; and (ii) a particulate matter feed control system configured to control the metered feed of primary particulate material into said reactor chamber; and causing control of at least one of Including, The method, wherein the control optimization module is responsive to the one or more parameters representing the reactor subsystem outputs and to inputs representing desired future operation to generate the one or more control commands.

2. 2. The method of claim 1, wherein the one or more parameters relate to any of: (i) the level of hydrogen gas in the reactor output; and (ii) the level of one or more particulate materials in the reactor output.

3. The method of claim 1 , wherein the one or more parameters relate to the degree of hydrogen gas in the reactor output.

4. 10. The method of claim 1, wherein the one or more parameters relate to the level of one or more particulate materials in the reactor output.

5. The method of any one of claims 1 to 4, wherein the one or more control commands result in control of each of the heating control system and the particulate matter delivery control system.

6. The method of any one of claims 1 to 4, wherein the one or more control commands result in control of a heating control system.

7. The method of any one of claims 1 to 4, wherein the one or more control commands result in control of the particulate matter delivery control system.

8. 2. The method of claim 1, wherein the one or more parameters representative of real-time reactor subsystem output are derived from a selection of the following: the relative predominance of hydrogen gas in the gaseous mixture; a degree of purity of the hydrogen-based mixture; the amount of hydrogen passing through an area as a function of time; a degree of fluidity in the particles; a degree of conductivity in the particles; a degree of purity of the graphite particles; a degree of the ratio of the primary particulate material to the conductive particulate material; and the temperature of the hydrogen-containing output stream; an indicator of the quantum of one or more particulate materials released from the reactor subsystem as a function of time; an indicator of the particle size of one or more particulate materials released from the reactor subsystem; or an indicator of the morphology of one or more particulate materials released from the reactor subsystem.

9. The method of claim 1 , wherein operating the control optimization module further comprises processing one or more parameters representing real-time reactor subsystem inputs, including a hydrocarbon feed rate.

10. 2. The method of claim 1, wherein the one or more control instructions comprise control instructions representing one or more of: (i) instructions to adjust the release rate of the primary particulate material into the reactor chamber; (ii) instructions to release a predetermined amount of the primary particulate material into the reactor chamber at a predetermined rate; (iii) instructions to perform batch feeding of a predetermined amount of the primary particulate material into the reactor chamber at a predetermined time; (iv) and instructions to adjust the air transport fluid velocity for the primary particulate material; the batch size of the primary particulate material; or (vi) the number of batches for the primary particulate material.

11. The method of claim 1 , wherein the one or more control commands include commands that result in an increase or decrease in the amount of current and / or voltage being sent through the one or more electrodes of the heating control system.

12. 12. The method of claim 11, wherein the commands that result in an increase or decrease in the amount of current and / or voltage being sent through the one or more electrodes of the heating control system represent a specified target temperature change within the reactor chamber.

13. 10. The method of claim 1, wherein the one or more control instructions comprise instructions to a processor to control operating parameters of a fluidized bed reactor, thereby causing adjustments to any one or more of heating, fluidization rate, and / or pressure.

14. 10. The method of claim 1, wherein the reactor subsystem includes a reactor controller module, and wherein said operating a control module thereby sending said one or more control commands comprises providing a signal to the reactor controller module thereby causing the reactor control module to operate in a prescribed manner.

15. 15. The method of claim 14, wherein operating the reactor control module in a prescribed manner comprises causing the reactor control module to: (i) increase or decrease the heat in the reactor chamber; (ii) modify one or more fluidization parameters in the reactor chamber; or (iii) modify the pressure in the reactor chamber.

16. The method of claim 1 , wherein the reactor subsystem comprises a fluidized bed reactor.

17. The method of claim 1 , wherein the particulate matter feed control system includes a quantity determining arrangement configured to measure the amount of the primary particulate material prior to delivery to the reactor chamber.

18. 18. The method of claim 17, wherein the particulate matter feed control system includes a particulate matter storage assembly coupled to a particulate matter feed assembly, the particulate matter feed assembly including a feed pre-chamber configured to be selectively pressurized during delivery of the primary particulate material prior to delivery to the reactor chamber.

19. 10. The method of claim 1, wherein the control optimization module for processing data is further configured to process data from one or more additional sources including: (i) a sensor configured to monitor temperature within the reactor chamber; (ii) an input representing a predicted future temperature within the reactor subsystem; (iii) an input representing one or more parameters derived from monitoring particulate matter detected in the reactor subsystem output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing desired future operating conditions of the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the reactor subsystem output.

20. 10. The method of claim 1, wherein the conductive particulate material comprises one or more particulate materials selected from the group comprising graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide, preferably the conductive material is selected from the group comprising carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

21. The method of claim 1 , wherein the primary particulate material comprises a catalytic particulate material for hydrocarbon pyrolysis in the reactor subsystem.

22. 10. The method of claim 1, wherein the primary particulate material comprises a material selected from the group including carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

23. The method of claim 1 , wherein the primary particulate material comprises a graphitic material.

24. 24. The method of claim 23, wherein the graphitic material is selected from naturally occurring or synthetic graphite; flake graphite; and certain forms of conductive carbon.

25. 10. The method of claim 1, wherein the inputs representing desired future operation include any one or more of: (i) a desired hydrogen output parameter; (ii) a desired output carbon parameter; and (iii) a desired carbon output form.

26. 1. A system for controlling a hydrocarbon gas pyrolysis process, the hydrocarbon gas pyrolysis process comprising operation of a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the system comprising: a data input module configured to receive time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; a processing module configured to process the time series input data to thereby determine one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of a real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; a control optimization module operable, based on computer executable code, to process data including the one or more parameters representative of real-time reactor subsystem outputs, thereby generating one or more control instructions; a control module operable to send the one or more control instructions to cause control of at least one of: a heating control system that controls a level of current and / or voltage applied to one or more electrodes configured to deliver current into the reactor chamber so that the current propagates through the conductive particulate material; and a particulate matter feed control system that is configured to control the metered feed of primary particulate material into the reactor chamber. Including, The control optimization module is responsive to the one or more parameters representing the reactor subsystem outputs and to inputs representing desired future operation to generate the one or more control commands.

27. 27. The system of claim 26, wherein the one or more parameters relate to any of: (i) the level of hydrogen gas in the reactor output; and (ii) the level of the one or more particulate materials in the reactor output.

28. 27. The system of claim 26, wherein the one or more parameters relate to the degree of hydrogen gas in the reactor output.

29. 27. The system of claim 26, wherein the one or more parameters relate to the level of one or more particulate materials in the reactor output.

30. The system of any one of claims 26 to 29, wherein the one or more control commands result in control of each of the heating control system and the particulate matter delivery control system.

31. A system according to any one of claims 26 to 29, wherein the one or more control commands result in control of a heating control system.

32. The system of any one of claims 26 to 29, wherein the one or more control commands result in control of the particulate matter delivery control system.

33. 27. The system of claim 26, wherein the one or more parameters representative of the real-time reactor subsystem output are derived from a selection of the following: the relative predominance of hydrogen gas in the gaseous mixture; the degree of purity of the hydrogen-based mixture; the amount of hydrogen passing through an area as a function of time; the degree of fluidity in the particles; the degree of conductivity in the particles; the degree of purity of the graphite particles; the degree of the ratio of the primary particulate material to the conductive particulate material; and the temperature of the hydrogen-containing output stream; an indicator of the quantum of one or more particulate materials released from the reactor subsystem as a function of time; an indicator of the particle size of one or more particulate materials released from the reactor subsystem; or an indicator of the morphology of one or more particulate materials released from the reactor subsystem.

34. 27. The system of claim 26, wherein the operation of the control optimization module further comprises processing one or more parameters representing real-time reactor subsystem inputs, including hydrocarbon feed rate.

35. 27. The system of claim 26, wherein the one or more control instructions include control instructions representing one or more of: (i) instructions to adjust the release rate of the primary particulate material into the reactor chamber; (ii) instructions to release a specified amount of the primary particulate material into the reactor chamber at a specified rate; (iii) instructions to perform batch delivery of a specified amount of the primary particulate material into the reactor chamber at a specified time; (iv) and instructions to adjust the air transport fluid velocity relative to the primary particulate material; the batch size of the primary particulate material; or (vi) the number of batches of the primary particulate material.

36. 27. The system of claim 26, wherein the one or more control commands include commands that cause an increase or decrease in the amount of current and / or voltage being sent through the one or more electrodes of the heating control system.

37. 37. The system of claim 36, wherein the commands that result in an increase or decrease in the amount of current and / or voltage being sent through the one or more electrodes of the heating control system represent a specified target temperature change within the reactor chamber.

38. 27. The system of claim 26, wherein the one or more control instructions include instructions to a processor to control operating parameters of a fluidized bed reactor, thereby causing adjustments to any one or more of heating, fluidization rate, and / or pressure.

39. 27. The system of claim 26, wherein the reactor subsystem includes a reactor controller module, and wherein operating a control module thereby sending the one or more control commands includes providing a signal to the reactor controller module thereby causing the reactor control module to operate in a prescribed manner.

40. 27. The system of claim 26, wherein operating the reactor control module in a prescribed manner includes causing the reactor control module to: (i) increase or decrease the heat in the reactor chamber; (ii) modify one or more fluidization parameters in the reactor chamber; or (iii) modify the pressure in the reactor chamber.

41. 27. The system of claim 26, wherein the reactor subsystem comprises a fluidized bed reactor.

42. 27. The system of claim 26, wherein the particulate matter feed control system includes a quantity determining arrangement configured to measure the amount of the primary particulate material prior to delivery to the reactor chamber.

43. 27. The system of claim 26, wherein the particulate matter feed control system includes a particulate matter storage assembly coupled to a particulate matter feed assembly, the particulate matter feed assembly including a feed pre-chamber configured to be selectively pressurized during delivery of the primary particulate material prior to delivery to the reactor chamber.

44. 27. The system of claim 26, wherein the control optimization module for processing data is further configured to process data from one or more additional sources including: (i) a sensor configured to monitor a temperature within the reactor chamber; (ii) an input representing a predicted future temperature within the reactor subsystem; (iii) an input representing one or more parameters derived from monitoring particulate matter detected in the reactor subsystem output; (iv) an input representing one or more input gas delivery parameters; (v) an input representing a desired future operating condition of the reactor subsystem; and (vi) an input representing one or more parameters related to a gas other than hydrogen detected in the reactor subsystem output.

45. 27. The system of claim 26, wherein the conductive particulate material comprises one or more particulate materials selected from the group comprising graphite starting material, carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide, preferably the conductive material is selected from the group comprising carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low grade iron oxide.

46. 27. The system of claim 26, wherein the primary particulate material comprises a catalytic particulate material for hydrocarbon pyrolysis in the reactor subsystem.

47. 27. The system of claim 26, wherein the primary particulate material comprises a material selected from the group including carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxide, or low-grade iron oxide.

48. 27. The system of claim 26, wherein the primary particulate material comprises a graphitic material.

49. 49. The system of claim 48, wherein the graphitic material is selected from naturally occurring or synthetic graphite; flake graphite; and certain forms of conductive carbon.

50. 27. The system of claim 26, wherein the inputs representing desired future operation include any one or more of: (i) a desired hydrogen output parameter; (ii) a desired output carbon parameter; and (iii) a desired carbon output form.

51. 1. A method for controlling a hydrocarbon gas pyrolysis system, the hydrocarbon gas pyrolysis system including a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the method comprising: receiving time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; processing the time series input data to thereby determine one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of a real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; operating a control optimization module based on the computer executable code to process data including the one or more parameters representative of real-time reactor subsystem outputs, thereby generating one or more control instructions; operating a control module, thereby sending the one or more control instructions to cause control of at least one of: a heating control system that controls a temperature within the reactor chamber; and a particulate matter feed control system that is configured to control the metered feed of primary particulate material into the reactor chamber; Including, The method, wherein the control optimization module is responsive to the one or more parameters representing the reactor subsystem outputs and to inputs representing desired future operation to generate the one or more control commands.

52. 1. A system for controlling a hydrocarbon gas pyrolysis system, the hydrocarbon gas pyrolysis system including a reactor subsystem having a reactor chamber within which hydrocarbon gas is decomposed in the presence of a conductive particulate material, the system comprising: a data input module configured to receive time series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, the reactor output sensor system configured to monitor a composition of a reactor output emitted from the reactor subsystem; a processing module configured to process the time series input data to thereby determine one or more parameters representative of a real-time reactor subsystem output, the one or more parameters representative of a real-time reactor subsystem output related to either or both of: (i) the extent of hydrogen gas in the reactor output; and (ii) the extent of particulate material in the reactor output; a control optimization module operable, based on computer executable code, to process data including the one or more parameters representative of real-time reactor subsystem outputs, thereby generating one or more control instructions; a control module operable to send the one or more control instructions to cause control of at least one of: a heating control system for controlling a temperature within the reactor chamber; and a particulate matter feed control system configured to control the metered feed of primary particulate material into the reactor chamber; Including, The control optimization module is responsive to the one or more parameters representing the reactor subsystem outputs and to inputs representing desired future operation to generate the one or more control commands.

Images