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

Abstract

The present invention relates, in various embodiments, to systems and methods configured to enable improved / optimized control of hydrocarbon pyrolysis processes. Embodiments have been developed for implementation in the context of hydrocarbon gas pyrolysis systems in which there is a reactor subsystem having a reactor chamber in which hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material.

Description

[0001] Related applications

[0002] This application claims priority from Australian Provisional Patent Application No. 2022903775, filed on 9 December 2022. The contents of AU'775 are incorporated herein by reference in their entirety. Field of the Invention

[0003] The present invention relates to systems and methods configured, in various embodiments, to achieve improved / optimized control of a hydrocarbon pyrolysis process. Embodiments have been developed for implementation in the context of a hydrocarbon gas pyrolysis system including a reactor subsystem having a reactor chamber in which the hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material. Background of the Invention

[0005] Any discussion of the background art throughout the specification should in no way be considered as an admission that this art is widely known or forms part of the common general knowledge in the field.

[0006] Methane pyrolysis (also known as natural gas pyrolysis or methane decomposition) is a process that converts methane into solid carbon and hydrogen. This generates multiple benefits, for example related to the inherent value of the solid carbon and hydrogen, and also in the context of initiatives to reduce atmospheric carbon dioxide.

[0007] Hydrogen has numerous commercial applications, including as a clean, environmentally friendly alternative fuel for vehicles. Carbon, and more specifically graphite, is considered a key material in the emerging green technology market. It has demonstrated applications in energy storage / batteries, electrical conductive devices, catalyst supports, lubricant additives, and modern electronic devices. All references to carbon in this patent refer to carbon in its graphite form, and the terms are used interchangeably throughout.

[0008] However, conventional methods of producing hydrogen from fossil fuels, such as steam methane reforming (SMR), produce carbon dioxide (natural gas steam reforming and coal gasification), which is harmful to the environment.

[0009] Solid carbon, and more specifically graphite, is considered a key material for the emerging green technology market. It has proven applications in energy storage, electric vehicles, photovoltaics, and modern electronic devices.

[0010] According to reaction formula (1), natural gas can be catalytically cracked into hydrogen and solid carbon.

[0011] CH4 → C + 2H2 (1)

[0012] During this process, carbon is deposited on the catalyst surface and hydrogen is produced. Currently, a wide variety of catalysts are known to be used in this process, including precious metal catalysts and carbon-based catalysts.

[0013] While the above-mentioned processes are known, they have not yet been commercialized for a variety of economic reasons. This is primarily related to the underlying catalyst costs, including initial supply costs and catalyst recovery and regeneration costs. Most researchers in this field have utilized expensive and complex supported catalysts, which, despite their high catalytic activity and product yields, result in extremely high catalyst turnover costs. These costs are a significant barrier to the commercial use of such catalysts. There is a significant need for new and improved methods and catalysts for the catalytic conversion of hydrocarbons into stable and commercially valuable hydrogen and solid carbon.

[0014] The present applicant is named in numerous patent publications, such as WO 2016 / 154666, WO 2017 / 031529, and WO 2018 / 170543, each of which is incorporated herein by cross-reference. Among other things, these publications describe techniques for pyrolyzing methane using fluidized bed reactors and iron-containing catalysts (synthetic and naturally occurring). The present inventors have recognized improvements to such techniques.

[0015] 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. Summary of the Invention

[0016] Example embodiments provide a method for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber in which hydrocarbon gas decomposes in the presence of an electrically conductive particulate material, the method comprising:

[0017] receiving time-series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, wherein the reactor output sensor system is configured to monitor a composition of a reactor output released from the reactor subsystem;

[0018] processing the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output;

[0019] operating a control optimization module to process data including the one or more parameters representing real-time reactor subsystem outputs based on the computer executable code to generate one or more control instructions; and

[0020] The operating control module thereby sends the one or more control instructions to achieve control of at least one of the following: (i) a heating control system (optionally wherein the heating control system controls the current and / or voltage level applied to one or more electrodes, wherein the one or more electrodes are configured to deliver current into the reactor chamber so that the current propagates through the conductive particulate material); and (ii) a particulate material transport control system, wherein the particulate material transport control system is configured to control the metered delivery of primary particulate material into the reactor chamber.

[0021] In an exemplary embodiment, the one or more parameters are related to each of: (i) a measurement of hydrogen in the reactor output; and / or (ii) a measurement of one or more particulate materials in the reactor output. In another exemplary embodiment, the one or more parameters are related to only one of: (i) a measurement of hydrogen in the reactor output; and (ii) a measurement of one or more particulate materials in the reactor output.

[0022] In an exemplary embodiment, the one or more control instructions implement control of each of the heating control system and the particulate matter transport control system. In another exemplary embodiment, the one or more control instructions implement control of only one of the heating control system and the particulate matter transport control system.

[0023] In an exemplary embodiment, the one or more parameters representing real-time reactor subsystem output are derived from: a measurement of the relative proportion of hydrogen in the gas mixture; a measurement of the purity of the mixture based on hydrogen; the amount of hydrogen passing through a region over time; a measurement of particle fluidity; a measurement of the ratio of primary particulate material to conductive particulate material; and the temperature of the hydrogen-containing output stream.

[0024] In an exemplary embodiment, the one or more parameters representing real-time reactor subsystem output are derived from: a metric related to the amount of one or more particulate materials released from the reactor subsystem over 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.

[0025] In an example embodiment, the one or more control instructions include control instructions representing one or more of the following: (i) instructions to adjust the rate at which the primary particulate material is released into the reactor chamber; (ii) instructions to release a defined amount of the primary particulate material into the reactor chamber at a defined rate; (iii) instructions to perform batch delivery of a defined amount of the primary particulate material into the reactor chamber at a defined time; (iv) and instructions to adjust the rate of pneumatic transport fluid for the primary particulate material; instructions to adjust the batch size for the primary particulate material; or (vi) instructions to adjust the batch frequency for the primary particulate material.

[0026] In an example embodiment, the one or more control instructions include instructions that result in an increase or decrease in the amount of current and / or voltage delivered through the one or more electrodes of the heating control system (as measured by current intensity and / or total current per predefined time block, for example where pulsed current is used).

[0027] In example embodiments, the instructions that result in increasing or decreasing the amount of current and / or voltage delivered through the one or more electrodes of the heating control system represent a defined target temperature change within the reactor chamber.

[0028] In an example embodiment, the instructions that result in increasing or decreasing the amount of current and / or voltage delivered through the one or more electrodes of the heating control system are provided to a reactor control module of the reactor subsystem.

[0029] In an example embodiment, the reactor subsystem includes a reactor controller module, and wherein operating the reactor control module to issue the one or more control instructions includes providing a signal to the reactor controller module to cause the reactor control module to operate in a defined manner.

[0030] In an example embodiment, causing the reactor control module to operate in a defined manner includes causing the reactor control module to: (i) increase or decrease heat in the reactor chamber; (ii) change one or more fluidization parameters within the reactor chamber; or (iii) change the pressure within the reactor chamber.

[0031] In an exemplary embodiment, the reactor subsystem comprises a fluidized bed reactor.

[0032] In an example embodiment, the particulate matter delivery control system includes a quantity determination device configured to measure the amount of the primary particulate material prior to delivery to the fluidized bed reactor.

[0033] In an example embodiment, the particulate matter transport control system includes a particulate matter storage assembly coupled to a particulate matter transport assembly, wherein the particulate matter transport assembly includes at least one transport antechamber configured to be selectively pressurized during transport of the primary particulate material prior to transport to the reactor.

[0034] In an exemplary embodiment, the control optimization module for processing data is additionally configured to process data from one or more other sources, the other 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 of particulate matter detected in the output of the reactor subsystem; (iv) an input representing one or more input gas delivery parameters; (v) an input representing desired future operating conditions for the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the output of the reactor subsystem.

[0035] In an exemplary embodiment, the conductive particulate material comprises one or more particulate materials selected from the group consisting of: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or low-grade iron oxides; preferably, the conductive material is selected from the group consisting of: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or low-grade iron oxides.

[0036] In an exemplary embodiment, the primary particulate material comprises a catalytic particulate material for pyrolysis of hydrocarbons within the reactor subsystem.

[0037] In example embodiments, the primary particulate material comprises a material selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low grade iron oxides.

[0038] In an exemplary embodiment, the primary particulate material comprises a graphite material.

[0039] In example embodiments, the graphite material is selected from naturally occurring or synthetic graphite; flake graphite; and conductive carbon forms.

[0040] In an example embodiment, the control optimization module is responsive to the one or more parameters representing reactor subsystem outputs and an additional input representing desired future operation to generate the one or more control instructions.

[0041] In example embodiments, the inputs representing desired future operations include any one or more of: (i) desired hydrogen output parameters; (ii) desired carbon output parameters; and (iii) desired carbon output form.

[0042] In a further exemplary embodiment, the present 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 in which hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material, the method comprising:

[0043] receiving time-series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, wherein the reactor output sensor system is configured to monitor a composition of a reactor output released from the reactor subsystem;

[0044] processing the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output;

[0045] operating a control optimization module to process data based on the computer executable code, the data including one or more parameters representing real-time reactor subsystem outputs to generate one or more control instructions; and

[0046] The operation control module thereby sends the one or more control instructions to achieve control of at least one of the following: a heating control system, wherein the heating control system controls the temperature within the reactor chamber; and a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control the metered delivery of primary particulate material into the reactor chamber.

[0047] In a further exemplary embodiment, the present invention comprises a system for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system comprises a reactor subsystem having a reactor chamber, wherein hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material, the method comprising:

[0048] a data input module configured to receive time-series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, wherein the reactor output sensor system is configured to monitor the composition of a reactor output released from the reactor subsystem;

[0049] a processing module configured to process the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measurement of hydrogen in the reactor output; and (ii) a measurement of particulate material in the reactor output;

[0050] a control optimization module operable to process data including the one or more parameters representing real-time reactor subsystem outputs based on computer executable code to generate one or more control instructions; and

[0051] a control module operable to send the one or more control instructions to effectuate control of at least one of: a heating control system, wherein the heating control system controls the temperature within the reactor chamber; and a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control metered delivery of primary particulate material into the reactor chamber.

[0052] In a further exemplary embodiment, the present invention includes a method for pyrolysis of hydrocarbon gas, the method comprising:

[0053] receiving input data from a sensor configured to monitor an output of a fluidized bed reactor fed by a hydrocarbon gas input;

[0054] processing the input to determine one or more parameters representative of an output of the fluidized bed reactor;

[0055] an operational control optimization module, the control optimization module being responsive to one or more parameters representing an output of the fluidized bed reactor for generating one or more control instructions;

[0056] At least one of the control instructions is applied to a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control metered delivery of particulate matter into the fluidized bed reactor.

[0057] In an embodiment, the one or more parameters include a parameter representing the amount of hydrogen or the ratio of hydrogen to hydrocarbon gas. This may include a measurement of the hydrogen flux through the monitored area, or a percentage increase in hydrogen represented by the ratio of hydrogen to hydrocarbon gas.

[0058] In an embodiment, the control instructions represent one or more of the following: (i) instructions to adjust the rate at which the particulate material is released into the fluidized bed reactor; (ii) instructions to release a defined amount of the primary particulate material into the reactor chamber at a defined rate; (iii) instructions to perform batch delivery of a defined amount of the primary particulate material into the reactor chamber at a defined time; (iv) and instructions to adjust the rate of the pneumatic conveying fluid used for the primary particulate material; instructions to adjust the batch size used for the primary particulate material; or (vi) instructions to adjust the batch frequency used for the primary particulate material.

[0059] In an embodiment, the particulate matter delivery control system includes a quantity determination device configured to measure the amount of the particulate material prior to delivery to the fluidized bed reactor. In an embodiment, the particulate matter delivery control system includes a particulate matter storage assembly coupled to a particulate matter delivery assembly, wherein the particulate matter delivery assembly includes a delivery antechamber configured to be selectively pressurized during delivery of the particulate material prior to delivery to the fluidized bed reactor.

[0060] In an embodiment, the control optimization module is further responsive to data derived from one or more further inputs for generating one or more control instructions. For example, the one or more further sensors may include any one or more of the following: (i) a sensor configured to monitor 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 in the output of the fluidized bed reactor; (iv) an input representing one or more input gas transport 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 in the output of the fluidized bed reactor.

[0061] In embodiments, the one or more sensors are spaced apart within the fluidized bed reactor. In embodiments, the one or more sensors are located at a distal end of the fluidized bed reactor.

[0062] In an embodiment, the particulate material is selected from the group comprising: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides; preferably, the conductive material is selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0063] In embodiments, the particulate material is a catalytic particulate material for pyrolysis of methane in the fluidized bed reactor.In embodiments, the catalytic particulate material is selected from the group comprising: carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low grade iron oxides.

[0064] In embodiments, the particulate material is a non-catalytic particulate material selected to promote methane pyrolysis within the fluidized bed reactor. Preferably, it is a graphite material, for example selected from natural or synthetic graphite, preferably flake graphite. Other forms of carbon may be used, although preferably conductive carbon forms may be used (e.g., where the fluidized bed reactor is heated via an electric current flowing through a conductive material in the fluidized bed reactor (applied and / or induced)). In some embodiments, if the carbon is non-conductive, a conductive second material is present, such as a silica or alumina-based material.

[0065] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coalbed methane, landfill gas, and biogas. The composition of the hydrocarbon gas can vary significantly, but will typically contain one or more light hydrocarbons from the group consisting of methane, ethane, ethylene, propane, and butane. In a preferred embodiment, the hydrocarbon gas is selected from the group consisting of methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In a preferred embodiment, the hydrocarbon gas consists primarily of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0066] In an embodiment, the control instructions include control instructions for controlling one or more other components in the pyrolysis of hydrocarbons. Preferably, the one or more other components include thermal control components for a fluidized bed reactor.

[0067] In an embodiment, the control optimization module generates the one or more control instructions in response to the one or more parameters representing the output of the fluidized bed reactor and an additional input representing the desired future operation. Preferably, the input representing the desired future operation includes any one or more of the following: (i) a desired hydrogen output parameter; (ii) a desired carbon output parameter; and (iii) a desired carbon output form.

[0068] A second aspect of the present invention provides a system for controlling components used in a hydrocarbon gas pyrolysis plant, the system comprising:

[0069] a module configured to receive input data from a sensor configured to monitor an output of a fluidized bed reactor fed by a hydrocarbon gas input;

[0070] a processing module configured to process the input to determine one or more parameters representative of an output of the fluidized bed reactor;

[0071] a control optimization module responsive to one or more parameters representing an output of the fluidized bed reactor for generating one or more control commands; and

[0072] An output module is configured to apply at least one of the control instructions to a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control metered delivery of particulate matter into the fluidized bed reactor.

[0073] In an embodiment, the one or more parameters include a parameter representing the amount of hydrogen gas. This may include the flux of hydrogen gas through the monitored area.

[0074] In an embodiment, the control instructions represent one or more of the following: (i) instructions to adjust the rate at which the particulate material is released into the fluidized bed reactor; (ii) instructions to release a defined amount of the primary particulate material into the reactor chamber at a defined rate; (iii) instructions to perform batch delivery of a defined amount of the primary particulate material into the reactor chamber at a defined time; (iv) and instructions to adjust the rate of the pneumatic conveying fluid used for the primary particulate material; instructions to adjust the batch size used for the primary particulate material; or (vi) instructions to adjust the batch frequency used for the primary particulate material.

[0075] In an embodiment, the particulate matter delivery control system includes a quantity determination device configured to measure the amount of the particulate material prior to delivery to the fluidized bed reactor. In an embodiment, the particulate matter delivery control system includes a particulate matter storage assembly coupled to a particulate matter delivery assembly, wherein the particulate matter delivery assembly includes a delivery antechamber configured to be selectively pressurized during delivery of the particulate material prior to delivery to the fluidized bed reactor.

[0076] In an embodiment, the control optimization module is further responsive to data derived from one or more further inputs for generating one or more control instructions. For example, the one or more further sensors may include any one or more of the following: (i) a sensor configured to monitor 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 of particulate matter detected in the output of the fluidized bed reactor; (iv) an input representing one or more input gas transport 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 in the output of the fluidized bed reactor.

[0077] In an embodiment, the particulate material is selected from the group comprising: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides; preferably, the conductive material is selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0078] In embodiments, the particulate material is a catalytic particulate material for pyrolysis of methane in the fluidized bed reactor.In embodiments, the catalytic particulate material is selected from the group comprising: carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low grade iron oxides.

[0079] In embodiments, the particulate material is a non-catalytic particulate material selected to promote methane pyrolysis within the fluidized bed reactor. Preferably, it is a graphite material, for example selected from natural or synthetic graphite, preferably flake graphite. Other forms of carbon may be used, although preferably conductive carbon forms may be used (e.g., where the fluidized bed reactor is heated via an electrical current (applied and / or induced) through a conductive material in the fluidized bed reactor).

[0080] In an embodiment, the control instructions include control instructions for controlling one or more other components in the pyrolysis of hydrocarbons. Preferably, the one or more other components include thermal control components for a fluidized bed reactor.

[0081] In an embodiment, the control optimization module generates the one or more control instructions in response to the one or more parameters representing the output of the fluidized bed reactor and an additional input representing the desired future operation. Preferably, the input representing the desired future operation includes any one or more of the following: (i) a desired hydrogen output parameter; (ii) a desired carbon output parameter; and (iii) a desired carbon output form.

[0082] In a further exemplary embodiment, the present invention includes a method for pyrolysis of hydrocarbon gas, the method comprising:

[0083] providing an initial raw material of conductive carbon material to a fluidized bed reactor;

[0084] commencing operation of the fluidized bed reactor, wherein the fluidized bed reactor is fed by an input of hydrocarbon gas;

[0085] operating a high frequency power supply to deliver alternating current to a conductive coil at least partially surrounding the fluidized bed reactor, thereby inducing an induction effect within the fluidized bed reactor, such that the induction effect causes current to flow through the conductive carbon material, thereby heating the conductive carbon material to a predetermined temperature for initiating and maintaining pyrolysis of the hydrocarbon gas; and

[0086] The outlet component is operated to release process materials from the fluidized bed reactor, wherein the released process materials include carbon material, unreacted hydrocarbon gas and / or hydrogen gas.

[0087] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0088] In an embodiment, the conductive carbon material is selected from the group comprising: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0089] In embodiments, the method includes feeding a supply of conductive carbon material into a fluidized bed reactor.

[0090] In an embodiment, the conductive carbon material is selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0091] In an embodiment, the predetermined temperature is between 600 and 1500 degrees Celsius, preferably between 800 and 1200 degrees Celsius.

[0092] In embodiments, the graphite starting material is selected from natural or synthetic graphite, preferably flake graphite.

[0093] In embodiments, the method further comprises the steps of capturing at least a portion of the carbon material extracted via the outlet and processing the carbon material to produce a regenerated graphite material.

[0094] In an embodiment, the conductive coils are centrally cooled.

[0095] In an embodiment, multiple conductive coils are used.

[0096] In an embodiment, each conductive coil may be operated independently of the others to reach a predetermined temperature.

[0097] In an embodiment, the predetermined temperature is between 600 and 1500 degrees Celsius, preferably between 800 and 1200 degrees Celsius.

[0098] In a further exemplary embodiment, the present invention includes a system for pyrolysis of hydrocarbon gas, the system comprising:

[0099] a fluidized bed reactor configured to contain an initial feed of conductive carbon material upon startup;

[0100] a gas input system for the fluidized bed reactor, configured to deliver a hydrocarbon gas input supply to the fluidized bed reactor;

[0101] at least one electrically conductive coil at least partially surrounding the fluidized bed reactor;

[0102] a high-frequency power supply configured to deliver alternating current to the conductive coil, thereby causing an induction effect within the fluidized bed reactor, such that the induction effect causes current to flow through the conductive carbon material, thereby heating the conductive carbon material to a predetermined temperature that initiates and maintains pyrolysis of the hydrocarbon gas; and

[0103] An outlet system is configured to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon gas, and / or hydrogen gas.

[0104] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0105] In an embodiment, the conductive carbon material is selected from the group comprising: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0106] In embodiments, the system includes feeding a supply of conductive carbon material into a fluidized bed reactor.

[0107] In an embodiment, the conductive carbon material is selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

[0108] In an embodiment, the predetermined temperature is between 600 and 1500 degrees Celsius, preferably between 800 and 1200 degrees Celsius.

[0109] In embodiments, the graphite starting material is selected from natural or synthetic graphite, preferably flake graphite.

[0110] In embodiments, the system further comprises the steps of capturing at least a portion of the carbon material extracted via the outlet and processing the carbon material to produce a regenerated graphite material.

[0111] In an embodiment, the conductive coils are centrally cooled.

[0112] In an embodiment, multiple conductive coils are used.

[0113] In an embodiment, each conductive coil may be operated independently of the others to reach a predetermined temperature.

[0114] In an embodiment, the predetermined temperature is between 600 and 1500 degrees Celsius, preferably between 800 and 1200 degrees Celsius.

[0115] In a further example embodiment, the present invention includes a system for pyrolysis of hydrocarbon gas, the system comprising:

[0116] a fluidized bed reactor (FBR) configured to contain an initial feedstock of conductive carbon material upon startup;

[0117] a gas input system for the fluidized bed reactor, configured to deliver a hydrocarbon gas input supply to the fluidized bed reactor;

[0118] at least one pair of conductive electrodes configured to, in use, cause an electric current to flow through the conductive carbon material contained in the fluidized bed reactor, the fluidized bed reactor comprising a feedstock of the conductive carbon material upon start-up;

[0119] a high-frequency power supply configured to deliver an electric current between the at least one pair of electrodes, thereby causing the electric current to flow through the conductive carbon material contained in the fluidized bed reactor, thereby heating the conductive carbon material to a predetermined temperature to obtain an average temperature for initiating and maintaining pyrolysis of the hydrocarbon gas; and

[0120] An outlet system is configured to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon material, and / or hydrogen.

[0121] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0122] In embodiments, the conductive material comprises a conductive carbon material. In embodiments, the conductive material further comprises an inert / non-reactive conductive auxiliary material (eg, silica beads) that transfers heat to the surrounding process material.

[0123] In an embodiment, there are multiple pairs of electrodes. In such an embodiment, optionally, a single electrode is a member of two or more of the multiple pairs of electrodes.

[0124] In a further exemplary embodiment, the present invention includes a system for pyrolysis of hydrocarbon gas, the system comprising:

[0125] Fluidized bed reactor (FBR);

[0126] a gas input system for the fluidized bed reactor, configured to deliver a hydrocarbon gas input supply to the fluidized bed reactor;

[0127] at least one heating element disposed within the fluidized bed reactor;

[0128] a high frequency power supply configured to deliver high frequency power to at least one heating element to heat the fluidized bed reactor to a predetermined temperature that initiates and maintains pyrolysis of the hydrocarbon gas; and

[0129] An outlet system is configured to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon material, and / or hydrogen.

[0130] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0131] In embodiments, the system includes a plurality of heating elements. In embodiments, each of the plurality of heating elements can be individually controlled to maintain an average temperature. In some embodiments, the plurality of heating elements are each configured to apply heat to different regions within the fluidized bed reactor. Preferably, in some embodiments, such heating elements are individually controllable to apply variable amounts of heat to different regions within the fluidized bed reactor. In some embodiments, the different regions can be defined based on vertical / horizontal and / or radial coordinates.

[0132] In a further exemplary embodiment, the present invention includes a system for pyrolysis of hydrocarbon gas, the system comprising:

[0133] Fluidized bed reactor (FBR);

[0134] a gas input system for the fluidized bed reactor, configured to deliver a hydrocarbon gas input supply to the fluidized bed reactor;

[0135] at least one heating element disposed on a side wall of the fluidized bed reactor;

[0136] a high frequency power supply configured to deliver high frequency power to at least one heating element to heat the fluidized bed reactor to a predetermined temperature that initiates and maintains pyrolysis of the hydrocarbon gas; and

[0137] An outlet system is configured to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon material, and / or hydrogen.

[0138] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0139] In 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 region within the fluidized bed reactor. Preferably, such heating elements are individually controllable so that variable amounts of heat are applied to different regions within the fluidized bed reactor to maintain an average temperature. In some embodiments, the different regions can be defined based on vertical / horizontal and / or radial coordinates.

[0140] In a further exemplary embodiment, the present invention includes a system for pyrolysis of hydrocarbon gas, the system comprising:

[0141] Fluidized bed reactor (FBR);

[0142] a gas input system for the fluidized bed reactor, configured to deliver a hydrocarbon gas input supply to the fluidized bed reactor;

[0143] a plurality of heating devices (located inside or outside the reactor, i.e., hot-wall reactor or cold-wall reactor) configured to apply heat to the fluidized bed reactor;

[0144] a high frequency power supply system configured to deliver high frequency power to the or each of the heating devices to heat within the fluidized bed reactor to a predetermined temperature that initiates and maintains pyrolysis of the hydrocarbon gas; and

[0145] An outlet system is configured to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon material, and / or hydrogen.

[0146] In embodiments, the hydrocarbon gas is, comprises, or consists essentially of methane gas.

[0147] Preferably, the heating device or each of the multiple heating devices includes at least two different types of heating devices, and the types of heating devices are selected from the group consisting of: at least one heating element, which is arranged on the side wall of the fluidized bed reactor; at least one heating element, which is arranged inside the fluidized bed reactor; at least one pair of conductive electrodes, which are configured to pass current through the conductive material contained in the fluidized bed reactor in use, thereby causing heating of the conductive material; and at least one conductive coil wrapped around the fluidized bed reactor, which is configured to pass current through the conductive material contained in the fluidized bed reactor in use, thereby causing heating of the conductive material.

[0148] definition

[0149] In describing and claiming the present invention, the following terminology will be used in accordance with the definitions listed below. It should also be understood that the terminology used herein is for the purpose of describing specific embodiments of the present invention only and is not intended to be limiting. Unless otherwise indicated, all scientific and technical terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.

[0150] In this specification, unless the context requires otherwise, the term "low grade" should be understood to imply that the material is non-synthetic. It will be understood by those skilled in the art that synthetic materials are produced by chemical reaction of precursor materials. Standard synthesis techniques for catalysts, such as impregnation of nanoscale catalytic elements onto inert supports, are not encompassed by the present invention. While the term "low grade" does include naturally occurring materials, it should not be understood to exclude materials that have been physically enriched (e.g., extruded and sieved or classified).

[0151] As used herein, the term "dusting" is an industry term used to describe the reaction of breaking down a metal material (usually an iron material) into fragments and graphite within a carburizing environment. This effect begins with the adsorption and dissociation of methane molecules (or other carbon-containing gases) on the surface of a metal-containing catalyst, and the resulting carbon diffuses to the bulk metal surface. Once the outer layer is saturated with carbon, it forms metal carbides, which then precipitate out from the metal grain boundaries in the form of graphitic carbon. Over time, this results in intergranular pressures that separate the metal carbide particles from the parent bulk metal and cause the metal structure to decompose through "dusting". In this process, the catalyst separates and breaks into nano-fragments and is encapsulated in carbon / graphite. The resulting graphitic carbon material encapsulating Fe particles is hereinafter referred to as "carbon material with encapsulated iron" or "Hazer graphite".

[0152] The term "hydrocarbon gas" is intended to encompass a pure single gas, such as methane, or a gas mixture comprising one or more hydrocarbon gases, such as natural gas. Although preferred embodiments of the present invention relate to the pyrolysis of methane (or the pyrolysis of a methane-containing gas stream), it should be understood that other hydrocarbon gases (e.g., ethane, propane, etc.) are also suitable for use with the technology described herein.

[0153] Unless the context clearly requires otherwise, throughout the specification and claims, the words "comprises," "comprising," and the like should be construed in an inclusive sense rather than an exclusive or exhaustive sense; that is, to mean "including but not limited to."

[0154] 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 within the body of a claim, rather than immediately following a preamble, it limits only the elements recited in that clause; other elements are not excluded from the claim as a whole. As used herein, the phrase "consisting essentially of" limits the scope of a claim to the specified elements or method steps, plus those that do not materially affect one or more basic and novel characteristics of the claimed subject matter.

[0155] As used herein, the term "power source" may refer to alternating current or direct current.

[0156] With respect to the terms "comprising," "consisting of," and "consisting essentially of," when any of these three terms is used herein, the presently 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 by "consisting of," or alternatively, by "consisting essentially of."

[0157] Except in the operating examples or otherwise noted, all numbers used herein expressing the amounts of ingredients or reaction conditions should be understood to be modified by the term "about" in all cases, taking into account the normal tolerances in the art. These examples are not intended to limit the scope of the invention. Hereinafter, or where otherwise indicated, "%" will mean "weight %", "ratio" will mean "weight ratio" and "parts" will mean "parts by weight".

[0158] Unless stated otherwise, the term "substantially" as used herein shall mean comprising more than 50% by weight, if relevant.

[0159] The term "about" should be interpreted by those skilled in the art taking into account normal tolerance in the relevant art.

[0160] The recitation of numerical ranges using endpoints includes all numbers subsumed within that range (eg, 1 to 5 includes 1, 1.5, 2, 2.75, 3, 3.80, 4, 5, etc.).

[0161] The terms "preferred" and "preferably" refer to embodiments of the invention that may provide certain benefits under certain 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 and is not intended to exclude other embodiments from the scope of the invention.

[0162] It must also be noted that, as used in the specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the context clearly dictates otherwise.

[0163] Unless expressly stated otherwise, the prior art mentioned herein is fully incorporated by reference.

[0164] Although example embodiments of the disclosed technology are described in detail herein, it should be understood that other embodiments are contemplated. Accordingly, the scope of the disclosed technology is not limited to the details of construction and the arrangement of components set forth in the following description or illustrated in the accompanying drawings. The disclosed technology is capable of other embodiments and can be practiced or carried out in various ways.

[0165] This specification has been prepared in accordance with principles of general applicability. Therefore, where this specification discloses generally applicable principles, the claims may be drafted using corresponding general terms (Biogen v Medeva

[1997] RPC 1, 48). "Generally applicable principles" are general principles that are practically applicable in the manufacture of a class of products or in the performance of a process, including situations where the claims define a product or one or more processes in terms of the results to be achieved.

[0166] Features stated in a claim in generic terms will represent generally applicable principles where it is reasonable to expect (reasonably predict) that the claimed invention will function with anything falling within the scope of the generic term. Such a feature defined in generic terms may be the main part of the claim or it may be a simple descriptive word. In either case, a feature expressed in generic terms in a claim will be sufficiently implementable if the disclosure enables at least one form or application of the general principle of the feature and a person skilled in the art could reasonably expect that the invention will function with anything falling within the scope of the generic term. (Kirin-Amgen Inc. v Hoechst Marion Roussel Ltd

[2005] RPC 9,

[112] ).

[0167] Where claims are drafted more broadly, they may be considered enabled if it appears on the face of it that: a) the disclosure teaches the principles that a person skilled in the art would need to follow in order to implement each and every embodiment within the scope of the claims; and b) the specification discloses at least one application of those principles and provides those skilled in the art with sufficient information to carry out alternative applications of those principles in a manner that, although not explicitly disclosed, would be obvious to them (T 484 / 92).

[0168] Example embodiments are described below in the section entitled "Claims."

[0169] Reference throughout this specification to "one embodiment," "some embodiments," or "an embodiment" means that a particular feature, structure, or characteristic described in connection with the embodiment is included in at least one embodiment of the present invention. Thus, appearances of the phrases "in one embodiment," "in some embodiments," or "in an embodiment" in various places throughout this specification are not necessarily all referring 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.

[0170] As used herein, unless otherwise indicated, ordinal adjectives such as "first," "second," and "third," when used to describe common objects, indicate only different instances of the similar objects being referred to and are not intended to imply that the objects being described must be in a given order, whether temporally, spatially, in ranking, or in any other manner.

[0171] In the following claims and the description herein, any of the terms "comprising", "comprised of" or "which includes" is an open term, meaning that at least the elements / features listed thereafter are included, but other elements / features are not excluded. Therefore, when the term "comprising" is used in a claim, it should not be interpreted as limiting the devices or elements or steps listed thereafter. For example, the scope of an apparatus that expresses the inclusion of A and B should not be limited to an apparatus consisting only of elements A and B. As used herein, any of the terms "including" or "which includes / that includes" is also an open term, which also means including at least the elements / features listed thereafter, but not excluding others. Therefore, "comprising" is synonymous with "comprising".

[0172] As used herein, the term "exemplary" is used to provide an example, rather than to indicate a quality. That is, an "exemplary embodiment" is an embodiment provided as an example, but does not necessarily refer to an embodiment having exemplary qualities.

[0173] The present invention is not limited in scope by any specific embodiments described herein. These embodiments are provided for illustrative purposes only. Functionally equivalent products, formulations, and methods are clearly within the scope of the invention described herein.

[0174] The invention described herein may include one or more numerical ranges (e.g., size, concentration, etc.). A range of values ​​should be understood to include all values ​​within the range, including the values ​​defining the range, as well as values ​​adjacent to the range that result in the same or substantially the same results as the values ​​immediately adjacent to the values ​​defining the boundaries of the range.

[0175] Other definitions of selected terms used herein can be found in the detailed description of the invention and are used throughout. Unless otherwise defined, all other scientific and technical terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.

[0176] In this specification, unless the context requires otherwise, the term "selective synthesis" is to be understood as the preferential synthesis of one morphology over other morphologies. Although the process of the present invention will typically produce a mixture of morphologies, the applicant has determined that the choice of temperature and pressure of the process has an impact on the morphology of the graphite so produced.

[0177] Throughout this specification, unless the context requires otherwise, it should be understood that the process of the present invention can be carried out at temperatures and / or pressures within more than one specific 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 initially carried out at 600° C., wherein the temperature is increased to 800° C. during the contacting of the metal-containing catalyst with 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 initially carried out at 0 bar(g), wherein the pressure is increased to 8 bar(g) during the contacting of the metal-containing catalyst with the hydrocarbon gas.

[0178] In this specification, unless the context requires otherwise, the term "selectivity" refers to the percentage of graphite material produced having a desired morphology.

[0179] In 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 the pressure (in bars) above ambient pressure.

[0180] As used herein, the term "predetermined range of values" refers to a specific range of pressure and temperature that can be selected by one skilled in the art to selectively synthesize a graphite material having a desired morphology. One skilled in the art will be able to select the appropriate temperature(s) and pressure(s) within these ranges to selectively synthesize the desired graphite material.

[0181] Features of the present invention will now be discussed with reference to the following non-limiting description and examples. BRIEF DESCRIPTION OF THE DRAWINGS

[0182] Embodiments of the present invention will now be described, by way of example only, with reference to the accompanying drawings, in which:

[0183] Figure 1 A schematic diagram of an example hydrocarbon pyrolysis system is shown as a context for embodiments of the control techniques described herein.

[0184] Figure 2 A system configured to enable improved / optimized control of a hydrocarbon pyrolysis process is shown, along with selected components of a broader hydrocarbon pyrolysis system.

[0185] Figure 3A A first heating device for a hydrocarbon pyrolysis system is shown according to one embodiment.

[0186] Figure 3B A second heating device for a hydrocarbon pyrolysis system is shown according to one embodiment.

[0187] Figure 4 A table is provided that lists representative relationships between control variables and manipulated variables according to one embodiment.

[0188] Detailed Description of the Preferred Embodiments

[0189] The present invention, in various embodiments, relates to systems and methods configured to enable improved / optimized control of a hydrocarbon pyrolysis process. The embodiments have been developed for implementation in the context of a hydrocarbon gas pyrolysis system, wherein a reactor subsystem having a reactor chamber is present in which the hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material.

[0190] Overview of Control Optimization Technology

[0191] In general, the various embodiments disclosed herein relate to techniques that enable control of a particular form of hydrocarbon gas pyrolysis system, enabling control for the purpose of process improvement and / or optimization based on specific objectives, and / or for other purposes (e.g., achieving desired outputs and / or operating parameters). The present disclosure relates to the configuration of various hardware components and the pyrolysis system as a whole, rather than to the specific detailed logic associated with operating control or optimization techniques. However, it should be understood that the techniques disclosed herein can be configured / operated in a manner that achieves optimization or other intended control, such as through facility-specific testing and knowledge building, and / or implementation of known techniques (e.g., machine learning).

[0192] The technology disclosed herein relates to a hydrocarbon gas pyrolysis system comprising a reactor subsystem having a reactor chamber in which the hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material. This electrically conductive particulate material serves a dual purpose: it both aids in the decomposition process and additionally promotes heating of the fluidized mixture of particulates and gas within the reactor chamber.

[0193] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coalbed methane, landfill gas, and biogas. The composition of the hydrocarbon gas can vary significantly, but will typically contain one or more light hydrocarbons from the group consisting of methane, ethane, ethylene, propane, and butane. In preferred embodiments, the hydrocarbon gas is selected from the group consisting of methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In preferred embodiments, the hydrocarbon gas consists primarily of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0194] Embodiments particularly contemplate heating devices in which electrodes are disposed within the reactor chamber and current is applied to at least one of these electrodes, causing the current to flow through the conductive particulate material, whereby resistive effects result in heating. For example, the reactor subsystem may take the form of a fluidized bed reactor (FBR). Control of the current intensity applied via one or more electrodes, optionally in addition to other FBR controls (e.g., fluidization control), also has an effect on increasing / decreasing the temperature within the reactor chamber.

[0195] It should be understood that FBR technology is known, and the concept of heating an FBR via electrodes in this manner is also known. However, applying these known concepts and techniques to the current specific environment leads to additional complexities that cannot be addressed solely through FBR control. In particular, for the system discussed herein, the amount of particulate material within the reactor chamber is not fixed. Instead, there is insertion and extraction of particulate material, as well as changes in the composition / morphology of the particulate material. For example:

[0196] Within the reactor chamber, there is always a conductive particulate material, which in this case comprises graphitic carbon or iron substantially encapsulated by graphitic carbon. This is necessary to achieve electrode-induced heating within the reactor chamber.

[0197] A particulate matter delivery control system is configured to control the metered delivery of a precursor particulate material into the reactor chamber.

[0198] The primary particulate material may comprise iron oxides (synthetic or naturally occurring) and may be introduced as a low conductivity particulate material and later converted to a higher conductivity particulate material (e.g., carbon encapsulated iron) as carbon produced by the hydrocarbon decomposition process is deposited on the iron oxides.

[0199] Carbon deposition is not limited to iron oxides but also occurs on carbon particles, including carbon-encapsulated iron.

[0200] The conductive particulate material is preferably selected from the group consisting of: carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides. The primary particulate material preferably comprises carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides. In the case where the primary particulate material is a catalytic particulate material for pyrolysis of methane in a fluidized bed reactor, the catalytic particulate material is selected from the group consisting of: carbon materials with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides. In some cases, the primary particulate material is a non-catalytic particulate material selected to promote pyrolysis of methane in the fluidized bed reactor. Preferably, it is a graphite material, for example, selected from natural or synthetic graphite, preferably flake graphite. Other forms of carbon may be used, although it is preferred to use a conductive carbon form (for example, where the fluidized bed reactor is heated by an electric current (applied and / or induced) flowing through a conductive material in the fluidized bed reactor).

[0201] The amount of particulate material within the reactor chamber, along with the overall composition and morphology of the particulate material, has a direct impact on multiple parameters associated with the pyrolysis process. For example, this will affect: (i) the rate and efficiency at which pyrolysis occurs at a given temperature (and / or fluidization rate); (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 the desired fluidization rate; and (iv) the morphological characteristics of the reacting and extracting particulate material.

[0202] Thus, the present disclosure sets forth hardware configurations and processes that can be applied to enable improved / optimized control of hydrocarbon pyrolysis processes in such scenarios. This achieves a range of advantages (discussed below), including (but not limited to) mitigation of issues associated with unwanted carbon surface deposition, the ability to adjust catalytic input, control of residence time, and control of product purity (e.g., carbon, particularly graphitic carbon in various forms, and hydrogen). Other advantages may include greater scalability, better temperature control, simpler construction, and increased energy efficiency.

[0203] Example Pyrolysis Control Process

[0204] In an exemplary 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 released from the reactor subsystem. For example, this may 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 respective sampling rates and delay / time-lag properties).

[0205] The method then includes processing the time series input data to determine one or more parameters representing the real-time reactor subsystem output. The one or more parameters representing the real-time reactor subsystem output are related to either or both of: (i) a measurement of hydrogen gas in the reactor output; and (ii) a measurement of particulate material in the reactor output. That is, in some embodiments, parameters are calculated that are related to both, while in other embodiments, the calculated parameters are related to only one of these measurements.

[0206] The outlet member that enables the release of 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 (the solids flow from the reactor is the result of particle elutriation). Therefore, the elutriation rate will depend on the geometry, flow rate and overall design. Other means of operating the outlet member are also contemplated.

[0207] For example, where the parameters representing real-time reactor subsystem output are related to measurements of hydrogen in the reactor output, these parameters may be derived from any one or more of the following:

[0208] Measurement of the relative proportion of hydrogen in a gaseous mixture;

[0209] Purity measurement of hydrogen-based mixtures;

[0210] the amount of hydrogen passing through the region as a function of time;

[0211] Gas flow rate; and

[0212] The temperature of the hydrogen-containing output stream.

[0213] Likewise, where the parameter representing the real-time reactor subsystem output is related to a measurement of the conductive particulate material, the measurement may be derived from any one or more of the following:

[0214] an indicator related to the amount of one or more particulate materials released from the reactor subsystem over time;

[0215] an indicator related to the particle size of one or more particulate materials released from the reactor subsystem; and

[0216] An indicator related to the morphology of one or more particulate materials released from a reactor subsystem.

[0217] For clarity, the term "real time" as used in this specification indicates that these parameters can be functionally and reasonably correlated with the current conditions within the reactor chamber. This may include a process of extrapolating forward or otherwise accepting / accounting for delays caused by, for example, the time between when the material leaves the reactor and when it is observed by the sensor. In this context, delays on the order of seconds or minutes are considered "real time."

[0218] As a further aspect, in embodiments where the primary particulate material is a catalyst (e.g., iron oxide, which reacts to form iron which is then encapsulated in graphite by the decomposed hydrogen), data representing the catalyst / gas ratio in the reaction chamber is of particular interest compared to hydrocarbon (e.g., methane) conversion. Another factor of interest is the hydrogen purity (and / or hydrogen production) in the output relative to the rate at which hydrocarbon feed gas is provided to the reactor chamber. Other relevant factors include reactor temperature, bed level, gas residence time (in a dense bed), and operating pressure. It should be understood that the gas feed rate, reactor heat input, reactor pressure, and particle release rate / dosing rate are the primary manipulated or independent variables. The dependent variables are hydrogen purity, hydrogen production, graphite purity (note the manner in which iron oxide reacts in the chamber to form iron encapsulated in graphite), the ratio of primary particulate material to conductive particulate material (optionally calculated via monitoring a conductivity-related measure (or more specifically, iron / iron oxide graphite encapsulating iron) in the output stream), and hydrocarbon / methane conversion. Optionally, any one or more of the dependent variables (or a measure directly / indirectly representing the dependent variable) are quantified, thereby enabling the system to control one or more of the primary manipulated or independent variables, such as particle insertion release rate / metering, feed rate and / or various parameters, such as reactor chamber temperature, pressure and fluidization parameters, which can be controlled by a processor associated with the FBR.

[0219] The method then includes executing computer executable code via a control optimization module to process data, including one or more parameters representing real-time reactor subsystem outputs (and optionally other real-time data combinations). This generates one or more control instructions. The control module is then operated to issue one or more control instructions to control components within the pyrolysis system. This may include controlling one or both of the following:

[0220] (i) Heating control system. For example, in some embodiments, the heating control system controls the current and / or voltage level applied to one or more electrodes, which in turn are configured to deliver current to the reactor chamber so that the current propagates through the conductive particulate material (thereby achieving heating of the reactor chamber). In some embodiments, control of the heating system is indirect and is performed via communication with a separate reactor control module that controls the operation of a reactor subsystem (in some embodiments, a FBR). For example, the FBR may operate its heating control (e.g., the current delivered to the electrodes) based on a defined temperature target, and the control instructions sent by the control optimization module represent instructions for adjusting the target temperature.

[0221] (ii) A particulate material delivery control system. The particulate material delivery control system is configured to control the metered delivery of a primary particulate material into the reactor chamber. For example, the particulate material delivery control system includes a quantity determination device configured to measure the amount of the primary particulate material prior to direct or indirect delivery to the reactor chamber. In some embodiments, the particulate material delivery control system includes a particulate material storage assembly coupled to a particulate material delivery assembly, wherein the particulate material delivery assembly includes a delivery antechamber configured to be selectively pressurized during delivery of the primary particulate material prior to delivery to the reactor chamber.

[0222] Preferably, the control optimization module and the control module are configured so that control signals can be delivered to both systems. However, it should be understood that the latter is particularly important. It should be noted that the control optimization module need not be strictly used for "optimization" purposes, and that control can be implemented for a variety of purposes (e.g., improvement, testing, startup / shutdown, ramp-up / down, and intentional deoptimization, etc.). The "Optimization" label in the "Control Optimization Module" is merely representative.

[0223] There are various references to controlling current and / or voltage. It should be recognized that controlling one of these and leaving the other floating may offer advantages. For example, this may affect the heating rate of the reactor chamber (i.e., the fluidized bed); the superficial velocity of the particulate material affects the resistance and, therefore, the heating rate.

[0224] The heating control concepts discussed herein are not limited to control (direct or indirect) of the FBR heating system (e.g., current / voltage delivered via electrodes). Heating control can also be achieved via other factors, such as reactor pressure (which will have an impact on flow resistance), primary particle delivery rate, and particle extraction (e.g., relative purity of graphite in the chamber will have a direct impact on flow resistance).

[0225] The one or more control instructions include instructions to the reactor control system (ie, the processor that controls the operating parameters of the fluidized bed reactor) to cause adjustments related to any one or more of heating, fluidization rate, and / or pressure.

[0226] In some embodiments, the control optimization module is further configured to process data from one or more further sources. These may include one or more of the following: (i) a sensor configured to monitor the temperature in 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 of 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 for the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the reactor subsystem output.

[0227] In some embodiments, when multiple real-time parameters are observed, a subset of one or more of these parameters is defined as target parameters and a target value / range is specified. Control instructions are then defined according to an optimization method that is designed to manipulate and maintain the target parameters within the specified target value / range. For example, the target parameters may include: (i) a desired hydrogen output parameter; (ii) a desired carbon output parameter; and (iii) a desired carbon output morphology.

[0228] Example Pyrolysis Framework

[0229] Figure 1 A system 110 for converting a hydrocarbon feedstock 112 into hydrogen 114 and graphitic carbon 116 is shown. This description is provided to provide a general example of a system to which the control optimization techniques described herein are optionally applied. However, it should be understood that system 110 should not be considered an unnecessarily limiting example. Further disclosure regarding how the control optimization techniques may be implemented is provided further below, with reference to the example of system 110.

[0230] The hydrocarbon feedstock 112 is introduced into an optional pre-reactor conditioner 118, which is adapted to condition the hydrocarbon feedstock 112 to produce a conditioned hydrocarbon feedstock 120. In preferred embodiments, the hydrocarbon feedstock is selected from the group consisting of methane, ethane, ethylene, propane, and / or butane, or mixtures thereof. In preferred embodiments, the hydrocarbon feedstock consists essentially of one of methane, ethane, ethylene, propane, or butane, preferably methane.

[0231] 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 .

[0232] The pre-reactor conditioner is in communication with one or more reactors 26. The one or more reactors 26 are adapted to contact a conditioned iron oxide catalyst 29 with a conditioned hydrocarbon feedstock 20 at a temperature of 600° C. to 1000° C. (or higher) to produce a mixed phase stream 30 comprising hydrogen, 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 typically increases the temperature and pressure of the hydrocarbon feedstock prior to injection into the one or more reactors 26.

[0233] In communication with the catalyst inlet 132 is a catalyst conditioner 137. The catalyst conditioner 137 is adapted to condition the iron oxide catalyst 128 prior to entering the one or more reactors 126 to produce a conditioned iron oxide catalyst 129. Contemplated conditioning may include one or more of beneficiation, washing, drying, crushing, grinding, screening, purification, and heating of the catalyst.

[0234] The mixed phase outlet 136 is in communication with a post-reactor conditioner 142. The post-reactor conditioner 142 is adapted to condition the mixed phase stream 130 to produce a conditioned mixed phase stream 144. The post-reactor conditioner 142 may perform any one or more of dehydration, cooling, and / or volatile extraction of the mixed phase stream 130. Preferably, the post-reactor conditioner 142 cools and / or dehydrates the mixed phase stream 130.

[0235] 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 54, a second gas outlet 163, and a solid outlet 156. The one or more solid / gas separators 46 are adapted to separate at least a portion of the conditioned mixed phase stream 144 into a gas stream 148 comprising hydrogen and a solid stream 150 comprising graphitic carbon. The contemplated second gas outlet 163 may optionally be in communication with one or more of the pre-reactor conditioner 118, the reactor heater 165, and / or the generator 169 so that at least a portion of the gas stream 148 can be recycled. The generator 169 may optionally be used to provide power 180 to the reactor heater 165 or other portions of the system as desired.

[0236] Solids outlet 156 is in communication with solids conditioner 158. Solids conditioner 158 is adapted to condition solids stream 150 to produce graphitic carbon stream 16. Solids conditioner 158 may perform one or more conditioning functions of packaging (pelletizing, compressing), functionalizing, and / or purifying solids stream 150.

[0237] The gas outlet 154 is in communication with a pre-gas separation conditioner 160, which includes a conditioned gas outlet 161, so that at least a portion of the gas stream 148 is conditioned to produce a conditioned gas stream 162. The pre-gas separation conditioner 160 may perform one or more of pressurization, cooling, and purification / purification to remove impurities from the gas outlet product 148. Preferably, the pre-gas separation conditioner 160 pressurizes and / or purifies the gas stream 148.

[0238] Gas pre-separation conditioner 160 is fluidly connected to a gas separator 164 adapted to separate and purify at least a portion of the components of 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.

[0239] Gas separator 164 is in communication with post-gas separation conditioner 168, which is adapted to condition purified gaseous product stream 166 to provide hydrogen 114 in purified form and one or more conditioned gaseous streams 170, which may comprise one or more of CH, CO, CO, or a mixed gaseous stream. Purified hydrogen stream 114 may be connected to one or more storage tanks for pipeline transport to an end user, or optionally used as an energy source for one, or 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 heat reactor 126 directly or indirectly, as discussed in further detail below.

[0240] When the conditioned gaseous product stream 170 comprises a mixed gaseous stream of one or more of CO, CH4, and CO2, the mixed gaseous stream may optionally be connected to the pre-reactor conditioner 18 for supplying one or more reactors as a hydrocarbon feedstock, or may optionally be input into a generator 169 for power generation. The generator 169 may optionally provide power 180 to the reactor heater 165 or other parts of the system as needed.

[0241] Sensors configured to collect data for control optimization purposes may be located at a variety of locations 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 delay / time lag representative of current reactor conditions.

[0242] Regarding heating, Figure 1 The system in Figure 1 shows a reactor 126 and an associated reactor heater 165. It is assumed that the reactor is a fluidized bed reactor (FBR). In such a configuration, the contents of the reactor (e.g., including catalyst, carbon, methane, and hydrogen, collectively referred to as "process materials") are maintained in a stirred and fluidized state so that the process materials are substantially uniform throughout the reactor (i.e., preferably without significant vertical or horizontal stratification). The configuration and control of the reactor heater have an impact on the manner in which the reaction occurs in the reactor. The following heating techniques are optionally used in various embodiments (alone or in combination).

[0243] Electric bed heating

[0244] In such a configuration, one or more electrodes (e.g., including one or more pairs of electrodes) are positioned within the FBR such that current flows from the first electrode of a pair to the second electrode of the pair (optionally, wherein a given electrode forms part of a plurality of pairs of electrodes). In such a configuration, there is a resulting current flowing through the conductive carbon within the process material, which, due to its resistive properties, increases the temperature of the process material. Thus, the conductive carbon essentially acts as a resistive heating element (when in a homogenized fluidized state within the FBR), resulting in overall heating of the process material. It should be noted that in some embodiments, there is an odd number of electrodes (e.g., three, optionally using alternating current), thereby generating one or more pairs of electrodes, plus a single additional electrode.

[0245] In some embodiments, the electrodes are positioned to enable differential heating of different zones / pathways within a fluidized bed reactor (FBR). This is optionally combined with internal sensors (e.g., zone-specific temperature sensors) and a control system configured to apply differential currents within zones (and / or along different paths) to promote altered fluid motion behavior within the process material. This can be used to achieve functions including optimizing temperature uniformity and / or addressing identified stratification trends in the process material (e.g., by promoting convective motion).

[0246] External resistance heating (hot wall)

[0247] In this example, heat is applied directly through the sidewalls of the FBR, such as via external resistive elements. In this case, heating of the process material relies on proximity or contact between the process material and the FBR sidewalls. This approach has advantages in overall simplicity, however, there are potential scale limitations as the internal FBR radius increases (e.g., increased heat needs to be applied through the sidewalls to achieve a desired consistent temperature throughout the process material). At larger radii, higher energy transfer through the walls is required and is ultimately limited by the strength of the material at high temperatures.

[0248] Internal resistance heating (cold wall)

[0249] In this example, heat is applied by the element arranged in the central cavity of FBR. The shape, position and configuration of these elements can be adjusted according to reactor size, for example, to promote efficient, consistent heating. As a general principle for all heating examples described herein, it is advantageous to optimize / limit the temperature difference between the following: the outer surface of (i) heating element; and (ii) the target temperature of process material (selected based on the reaction conditions adjusted for optimal reaction conditions and / or desired output results). The shape, position and configuration of these elements also can be adjusted based on other factors, for example, in order to promote stirring and / or uniformity of process material. For example, a preferred embodiment utilizes multiple heating elements, which are shaped and / or positioned to promote the movement of process material in FBR, thereby optimizing heating efficiency and consistency of whole process material.

[0250] Another preferred embodiment utilizes a single heating element with a complex three-dimensional shape (e.g., spiral or coil), which promotes the movement of the process material in the FBR, thereby optimizing the heating efficiency and consistency of the whole process material. In an embodiment, such heating elements can be included in the FBR as one or more heating elements to optimize the heating of the process material. In an embodiment, one or more heating elements are arranged into a double helix structure or a coil of different diameters. In an embodiment, the coil is tightly spiral (similar to a spring).

[0251] In embodiments, one or more heating elements are positioned at larger heating element inside. In some embodiments, one or more heating elements can be operated separately. In some embodiments, there are multiple independently controllable heating elements, each occupying the corresponding region (optionally vertical, radial or based on the region defined by other coordinate systems) in the FBR, these heating elements are independently controllable, thereby can realize region-specific heating or ensure the uniform heating of process material. This is optionally combined with internal sensor (such as region-specific temperature sensor) and control system, and described control system is configured to apply temperature difference between regions, thereby promotes the fluid motion behavior of change in process material. This can be used for realizing and comprises optimizing temperature consistency and / or solving the function of determined process material stratification trend (such as, by promoting convection motion).

[0252] In some embodiments, process material (eg, methane) may be inserted at one or more insertion points in the FBR.

[0253] Induction heating

[0254] In this example, a magnetic field is generated via components outside the FBR chamber (e.g., using a conductive coil through which an alternating current is passed), which causes current to flow within the process material, thereby heating the process material based on the conductive / resistive properties of the carbon. More details about the potential induction heating device will be provided further below. This provides a form of "internal heating" - that is, applying heat to the process material inside the reactor sidewall - using infrastructure outside the reactor sidewall. In this regard, the conductive carbon in the process material essentially acts as an internal heating element.

[0255] It is understood that eddy currents are induced in conductive materials.

[0256] In further embodiments, various FBR heating technologies and / or systems may be combined to achieve objectives including: (i) heating consistency within the process material; (ii) limiting the surface temperature of internal components within the FBR chamber, thereby reducing the risk of surface carbon deposition; and (iii) zoning control to promote desired heating / convection / agitation effects.

[0257] Example Control System Device

[0258] Now refer to Figure 2 Describe an example control system.

[0259] Figure 2 Illustrated are selected components of an example pyrolysis system for converting hydrocarbon feedstock into hydrogen and graphitic carbon, which components may be incorporated into and / or form Figure 1 part of the system.

[0260] Figure 1 The pyrolysis system includes a fluidized bed reactor (FBR) 201. The detailed configuration and control issues of the FBR for the purposes of the present invention are beyond the scope of this disclosure. Nevertheless, the key components will be described.

[0261] FBR 201 has a body 202 that encloses a reactor chamber 203 in which a fluidized bed is held. In particular, an input gas fluidization infrastructure 204 is configured to deliver a hydrocarbon feed 205 to an FBR inlet 206. The FBR inlet 206 is coupled to an FBR gas delivery component 207 that is configured to control the delivery of the hydrocarbon feed 205 into the reactor chamber 203 and maintain uniform fluidization of the process material contained therein.

[0262] 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 type of heating infrastructure is preferably electrified bed heating, wherein one or more electrodes (e.g., comprising one or more pairs of electrodes) are positioned within the FBR such that an electric current flows from a first electrode of a pair of electrodes to a second electrode of the pair of electrodes (optionally, wherein a given electrode forms part of a plurality of pairs of electrodes). In a preferred embodiment, there are three electrodes, and alternating current is used. In such a configuration, there is an electric current generated by the conductive carbon within the process material, which increases the temperature due to its resistive properties. Thus, the conductive carbon essentially acts as a resistive heating element (when in a homogenized fluidized state within the FBR), resulting in overall heating of the process material.

[0263] Other forms of heating may also be used, options include (but are not limited to) one or more of the following:

[0264] External resistive heating (hot wall), where heat is applied directly through the side walls of the FBR, such as by external resistive elements.

[0265] Internal resistance heating (cold wall), where heat is applied by elements placed in the central reactor chamber of the FBR.

[0266] Induction heating, in which a magnetic field is generated via components outside the FBR reactor chamber (e.g., using a conductive coil through which alternating current is passed), which causes current to flow within the process material, thereby heating the process material based on the conductive / resistive properties of the carbon. Further details on potential induction heating devices will be provided further below. This provides a form of "internal heating"—i.e., heat is applied to the process material from within the reactor sidewall—using infrastructure external to the reactor sidewall. In this regard, the conductive carbon within the process material essentially acts as an internal heating element.

[0267] In the illustrated example, the FBR 201 is coupled to a FBR control system 230 that controls various operating parameters, such as the operation of the heating infrastructure and control of the gas release / fluidization assembly.

[0268] FBR 201 further includes an output assembly 208 configured to release output process material 209 to output processing infrastructure 210. For example, output processing infrastructure 210 may include various components for gas and solids separation, separation of hydrogen from other gases, solids filtration and separation, and support for other downstream operations.

[0269] The system includes a primary particulate matter delivery control system 212. The primary particulate matter delivery control system is configured to control the metered delivery of primary particulate matter to the FBR 201. The precise nature of the system 212 (e.g., components and configuration) varies between different embodiments, and Figure 1 The devices described are examples intended only to demonstrate certain functionality.

[0270] As a core function, system 212 is configured to deliver primary particulate material (the inventory of which is optionally contained in feed hopper 213) to the process material of FBR 201. This delivery is achieved through various components, preferably components that can control the metered delivery of particulate material (e.g., based on volume and / or weight). The manner in which this is achieved varies among various embodiments, but as a common feature, it is preferably to have electronically controllable components that enable computerized control of the material delivery.

[0271] The primary particulate material may comprise catalytic particulate material, non-catalytic particulate material, or a combination of both. For example:

[0272] In embodiments, the particulate material is a catalytic particulate material for pyrolysis of methane in the fluidized bed reactor.In embodiments, the catalytic particulate material is selected from the group comprising: carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low grade iron oxides.

[0273] In embodiments, the particulate material is a non-catalytic particulate material selected to promote methane pyrolysis within the fluidized bed reactor. Preferably, it is a graphite material, for example selected from natural or synthetic graphite, preferably flake graphite. Other forms of carbon may be used, although conductive carbon forms are preferred (e.g., where the fluidized bed reactor is heated by an electric current (applied and / or induced) through a conductive material in the fluidized bed reactor).

[0274] It should be understood that the choice of particulate material is a matter of design choice for a particular pyrolysis operation, and the delivery techniques described herein are agnostic in this regard. In some cases, there are multiple hoppers containing different materials that can be selectively used in a single FBR. To operate this embodiment, the reactor chamber requires a conductive particulate material for heating purposes; the primary particulate material delivered via system 212 can have the required conductive properties, or it can acquire such conductive properties upon introduction into the reactor chamber (as in the case of iron oxides, which are reduced to iron and then encapsulated in carbon, thereby increasing the particle conductivity).

[0275] In the illustrated example, hopper 213 is coupled to a first material delivery control component 214, which controls the delivery of the primary particulate material from the hopper via a gravity feed mechanism to a metering chamber 216. Metering chamber 216 includes a conveyor belt 215 that delivers the material in a controlled manner to a delivery antechamber 218. Delivery antechamber 218 preferably includes one or more sensors configured to measure the amount of particulate material in (or passing through) chamber 218 (e.g., by reference weight or volume). Chamber 218 (optionally in conjunction with chamber 216) can be pressurized to prevent leakage of process material from the FBR reactor chamber 203 into chamber 218. For example, when chamber 218 is filled with a predetermined amount of particulate material, first seal 219 is maintained in a sealed configuration, chamber 218 is pressurized, and then seal 219 is opened while seal 218 is closed. In another embodiment, pressurization is provided between seal 219 and element 214, allowing for continuous metered delivery of particulate material via conveyor belt 215. These are just two possible physical infrastructure arrangements that can enable controlled / metered delivery of particulate material into a FBR via one or more pressurized delivery antechambers.

[0276] Figure 2 A system configured to achieve pyrolysis process optimization is shown in the form of a pyrolysis monitoring and control system (PMCS) 220. The PMCS 220 is preferably defined by one or more networked computing terminals that execute computer executable code (software instructions) to achieve Figure 2 The key function of PMCS 220 is to control the delivery of particulate material to the reactor chamber of FBR 201. Other functions may also be optionally performed, such as those described further below.

[0277] The software executed on PMCS220 is 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 embodiment refer not only to modules in the computer program, but also to modules in the hardware configuration. The discussion of the embodiment is also a discussion of computer programs for making the modules function (including programs that make the computer perform each step, programs that make the computer function as a device, and programs that make the computer perform each function), as well as a discussion of systems and methods. For ease of explanation, the phrases "store information", "cause information to be stored" and other equivalent phrases are used. If the embodiment is a computer program, these phrases are intended to express "causing a storage device to store information" or "controlling a storage device so that the storage device stores information". Modules can correspond one to one with functions. In software implementation, one module can form a program, or multiple modules can form a program. One module can form multiple programs. Multiple modules can be executed by one computer. A single module can be executed by multiple computers in a distributed environment or a parallel environment. A module can contain another module. In the following discussion, the term "connection" refers not only to physical connections, but also to logical connections (such as the exchange of data, instructions, and data references). The term "predetermined" refers to matters that have been determined before the process of interest. Therefore, "predetermined" refers to matters that have been determined before the process of interest in the implementation scheme. Even after the process in the implementation scheme has begun, the term "predetermined" refers to matters that have been determined before the target process based on the conditions or state of the implementation scheme at the current point in time, or based on the conditions or state that have persisted until the current point in time. If "predetermined values" are plural, the predetermined values ​​may be different from each other, or two or more of the predetermined values ​​(including all values) may be equal to each other. The statement "if A, then B will be performed" is intended to mean "determine whether something is A, and if something is determined to be A, then action B will be performed." If it is not determined whether something is A, this statement becomes meaningless.

[0278] In each process executed by a module, or in one of the processes executed by a module, information as a processing target is read from a storage device, the information is processed, and the processing result is written to the storage device. The description related to reading information from a storage device before processing and writing the processed information to the storage device after processing can be appropriately omitted. The storage device may include a hard disk, a random access memory (RAM), an external storage medium, a storage device connected via a communication network, and a register in a CPU (central processing unit).

[0279] The PMCS 220 includes one or more modules configured to receive input data from one or more sensors configured to monitor the output of the FBR 201. In the illustrated example, this includes a sensor input module 221 configured to receive data from a hydrogen sensor 211a that monitors hydrogen in the output material from the FBR 201, and a particle sensor 211b that monitors an indicator of particle output from the FBR 201 (e.g., as discussed further above). The sensor input module 221 is configured to process the input to determine one or more parameters representative of hydrogen and / or particle output from the fluidized bed reactor (e.g., any one or more of: hydrogen flux and output gas / material ratio over time, as defined by hydrogen, particle size / morphology, particle flux, and other parameters).

[0280] The PMCS includes a component that operates as a control optimization module that responds to one or more parameters representing the output of the fluidized bed reactor to generate one or more control instructions. In the illustrated example, this is provided as a function of the control optimization module 223. In this regard, the processing module 223 is configured to apply one or more algorithms (or other computerized processes) to receive inputs including data representing one or more parameters representing hydrogen output and output data representing instructions for controlling the system 212 (and optionally, other controllable components in the broader pyrolysis system) from these algorithms. For example, based on inputs including detected hydrogen levels, the module 212 outputs data representing instructions to perform one or more of the following:

[0281] Increase the rate at which particulate material is delivered to the FBR.

[0282] Increase the rate at which particulate material is delivered to the FBR.

[0283] A predetermined sized batch of particulate material is delivered to the FBR at a specified time (the specified time may be predetermined, or may be "immediate" in nature).

[0284] When there are multiple hoppers 213 containing different particulate materials, switching between the particulate materials and / or adjusting the ratio of the different particulate materials.

[0285] Module 212 may also provide control instructions for other components, such as FBR control system 230 (e.g., providing instructions related to heating, such as temperature set points, instructions related to fluidization parameters, etc.). In some embodiments, module 212 is configured to directly control the heating and / or fluidization infrastructure.

[0286] The control instruction delivery module 224 is configured to apply the control instructions defined by the processing module 224, which in the illustrated example involves delivering the control instructions to the conveying system 212. The module 224 preferably executes based on a plurality of predefined rules that enable algorithmic decisions regarding whether (and optionally when) to implement the control instructions, for example, based on safety and other factors. For example, the module 224 may access data including the availability of material in the hopper 212, the scheduling of shutdowns and other operations, and inputs from other sensors in the broader system.

[0287] In the illustrated example, control instruction execution module 224 interacts with primary material delivery module 225 and secondary material delivery module 226 to give the control instructions physical, real-world effects. The former accesses controllable components associated with chamber 218 (e.g., valves, sensors, and pressurization components), while the latter accesses controllable components associated with chamber 216 (e.g., component 214 and other valves, sensors, and pressurization components). This is merely an example; the manner in which modules within control system 220 provide control instructions to components within system 212 may vary from one implementation to another, depending on the specific nature of system 212 and its operation. This can vary widely in complexity (e.g., from a simple implementation in which system 212 is capable of receiving instructions regarding the rate of release of particulate material, to a complex implementation in which the component controllers within system 212 require individual control / actuation).

[0288] In further embodiments, the control instructions generated by the control optimization module 224 and executed via the execution module 224 may relate to components other than those belonging to the system 12. For example, the system 220 includes an other input module 222 for receiving data from other sensors associated with the FBR or other pyrolysis system components, as well as data inputs from other sources (e.g., desired operating characteristics, planned operating factors (e.g., shutdowns), etc.). That is, the PMCS 220 additionally (as an optional feature) includes an other input module 222 configured to monitor other outputs and / or operating parameters of the FBR 201. This may include one or more of the following:

[0289] Input from a sensor configured to monitor the temperature within the fluidized bed reactor.

[0290] An input representing the predicted future temperature within the fluidized bed reactor.

[0291] An input representing one or more parameters derived from monitoring particulate matter detected in the fluidized bed reactor output (eg, carbon purity, carbon form, particle size, etc.).

[0292] An input representing one or more desired parameters related to the particulate matter detected in the fluidized bed reactor output (eg, carbon purity, carbon morphology, particle size, etc.).

[0293] An input representing one or more desired parameters related to hydrogen output.

[0294] An input representing one or more input gas delivery parameters.

[0295] Input representing desired future operating conditions for the fluidized bed reactor (e.g., planned outage).

[0296] An input representing one or more parameters related to gases other than hydrogen detected in the fluidized bed reactor output.

[0297] Furthermore, as previously described, modules 223 and 224 may be configured to additionally / alternately generate and execute control instructions for components other than components of system 12 (optionally including FBR components, such as heating infrastructure and / or other components in the broader pyrolysis system).

[0298] The manner in which the processing module 223 operates varies between embodiments based on a number of factors (e.g., FBR size / shape, facility usage, input gas parameters, and catalyst / non-catalytic material properties, etc.). Broadly, the following methods may optionally be used:

[0299] A rule-based algorithmic approach, in which logic rules are generated to match predefined inputs (such as hydrogen flux rate, desired output carbon form, and other desired operating parameters) with control instructions.

[0300] An AI / machine learning driven approach, in which a software module is trained based on training data to receive inputs (e.g., hydrogen flux rate, desired output carbon form, and other desired operating parameters) and perform AI / machine learning-based processing to deliver outputs representing control instructions. For example, a neural network can be trained based on input data collected from historical operations of one or more similar methane pyrolysis systems, the training data including past / future time series data representing components of particulate matter delivery (e.g., catalyst delivery) into the FBR, as well as operating parameters (e.g., hydrogen flux). Again as a representative example, this can be used to train a neural network to receive current data representing FBR operations as input (including hydrogen flux) and provide an output representing the amount of particulate material (e.g., a known catalytic material) delivered to the FBR to maximize hydrogen flux. Such a neural network can also be trained to enable control of the carbon form generated in the FBR (although in this case, control of the FBR temperature would also be meaningful in addition to control of the particulate delivery rate).

[0301] In the latter case, it is preferred to continuously generate training data to facilitate continuous learning and optimized control of a particular pyrolysis system during its operation.

[0302] Example Control Rules

[0303] Listed below are a few example control rules that can be used by Figure 2 The systems shown and / or processes / methods described herein may be implemented in combination.

[0304] If the hydrogen output is below a threshold, instructions are generated to insert a prescribed amount of primary particulate material at one time.

[0305] If the hydrogen output is below a threshold, instructions are generated to increase the rate of insertion of the precursor particulate material.

[0306] If the hydrogen output is below a threshold, instructions are generated to increase the temperature target for the reactor chamber.

[0307] If the hydrogen output is below a threshold, instructions are generated to increase the current to the reactor chamber electrodes.

[0308] If the hydrogen output is below a threshold, instructions are generated to adjust the degree of agitation / fluidization in the reactor.

[0309] If the particulate material output is below a threshold, instructions are generated to insert a prescribed amount of primary particulate material at one time.

[0310] If the particulate material output is below a threshold, instructions are generated to increase the rate of insertion of the primary particulate material.

[0311] If the particulate material output is below a threshold, instructions are generated to increase the temperature target for the reactor chamber.

[0312] If the particulate material output is below a threshold, instructions are generated to increase the current to the reactor chamber electrodes.

[0313] If the particulate material output is below a threshold, instructions are generated to adjust the degree of agitation / fluidization in the reactor.

[0314] If the average size of the outputted granular material is above a threshold value, an instruction is generated to insert a prescribed amount of primary granular material at one time.

[0315] If the outputted average size of the particulate material is above a threshold, instructions are generated to increase / decrease the insertion rate of the primary particulate material.

[0316] If the outputted average size of the particulate material is above a threshold, instructions are generated to increase / decrease the temperature target of the reactor chamber.

[0317] If the outputted average size of the particulate material is above a threshold, instructions are generated to increase / decrease the current flowing to the reactor chamber electrodes.

[0318] If the output average size of the particulate material is above a threshold, instructions are generated to adjust the degree of agitation / fluidization in the reactor.

[0319] If the morphology of the granular material in the output is outside the defined target range, instructions are generated to insert a defined amount of primary granular material at once.

[0320] If the morphology of the particulate material in the output is outside a defined target range, instructions are generated to increase / decrease the insertion rate of the primary particulate material.

[0321] If the particulate material morphology in the output is outside of a set target range, instructions are generated to increase / decrease the temperature target for the reactor chamber.

[0322] If the particulate material morphology in the output is outside of a set target range, instructions are generated to increase / decrease the current to the reactor chamber electrodes.

[0323] If the particulate material morphology in the output falls outside a set target range, instructions are generated to adjust the degree of agitation / fluidization in the reactor.

[0324] It should be understood that these are merely examples 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.

[0325] Figure 4 Provides additional details about the relationship between the example controlled and manipulated variables in the event that the controlled variable is above or below a defined threshold. In this example, the controlled variables are as follows:

[0326] The ratio of catalyst to gas in the reactor chamber.

[0327] The purity of hydrogen in the output.

[0328] Methane (or other hydrocarbon) conversion rate.

[0329] Hydrogen production.

[0330] Reactor chamber temperature.

[0331] Reactor superficial velocity (for particulate matter).

[0332] FBR bed level.

[0333] Gas residence time in the reactor chamber.

[0334] Graphite purity in the reactor output.

[0335] Graphite morphology in the reactor output.

[0336] Heat input to the reactor chamber.

[0337] Bed resistivity in the reactor chamber.

[0338] Example manipulated variables are as follows:

[0339] Feed rate: The rate at which the gaseous hydrocarbon feed is supplied to the reactor.

[0340] Catalyst Addition Rate: The rate at which catalyst (ie, primary particulate material) is provided to the reactor chamber.

[0341] The pressure in the reactor chamber.

[0342] The voltage and / or current applied to the heating electrode.

[0343] Figure 4 The table in provides an example relationship between controlled variables and manipulated variables. The control technology described herein is configured to control some or all (directly and / or indirectly) of the manipulated variables based on some or all of the measured values ​​and / or target values ​​in the controlled variables. For example, this can be achieved by applying known technologies such as dynamic matrix control (DMC) and / or real-time optimization (RTO). DMC is a multivariable optimization software program located above regulatory control and pushes variables in one direction based on a predefined set of relationships between variables and priority inputs. RTO is a model based on basic chemical engineering that adjusts the limits and priorities in DMC based on economic optimization signals and an understanding of process optimum conditions (DMC does not consider optimum conditions; it is based on constraints). Alternatively, other proprietary software methods can also be implemented.

[0344] from Figure 4 From the table, we can derive the following example control instructions:

[0345] If the catalyst-gas ratio is above a threshold, a command is generated to increase the feed rate

[0346] If the hydrogen purity is above a threshold, a command is generated to increase the feed rate

[0347] If the methane conversion is above a threshold, a command is generated to increase the feed rate

[0348] If hydrogen production is above a threshold, a command is generated to increase the feed rate

[0349] If the reactor temperature is above a threshold, a command is generated to increase the feed rate

[0350] If the reactor superficial velocity is above a threshold, generate instructions to reduce the feed rate

[0351] If the bed level is above a threshold, generate instructions to increase or decrease the feed rate

[0352] If the gas residence time is above a threshold, a command is generated to increase the feed rate

[0353] If the graphite purity is above a threshold, generate instructions to increase the feed rate

[0354] If the heat input is above a threshold, a command is generated to increase the feed rate

[0355] If the bed resistivity is above a threshold, a command is generated to reduce the feed rate

[0356] If the catalyst-gas ratio is above a threshold, a command is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0357] If the hydrogen purity is above a threshold, instructions are generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0358] If the methane conversion rate is above a threshold, a command is generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0359] If the hydrogen production is above a threshold, a command is generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0360] If the reactor temperature is above a threshold, an instruction is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0361] If the reactor superficial velocity is above the threshold, an instruction is generated to - the catalyst addition rate (i.e., the primary particulate material addition rate)

[0362] If the bed level is above a threshold, a command is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0363] If the gas residence time is above a threshold, a command is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0364] If the graphite purity is above a threshold, an instruction is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0365] If the heat input is above a threshold, a command is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0366] If the bed resistivity is above a threshold, a command is generated to - the catalyst addition rate (i.e., the primary particulate material addition rate)

[0367] If the catalyst-gas ratio is above a threshold, a command is generated to reduce the pressure

[0368] If the hydrogen purity is above a threshold, a command is generated to increase or decrease the pressure

[0369] If the methane conversion rate is above a threshold, a command is generated to increase or decrease the pressure

[0370] If hydrogen production is above a threshold, a command is generated to increase or decrease pressure

[0371] If the reactor temperature is above a threshold, a command is generated to increase or decrease the pressure

[0372] If the reactor superficial velocity is above a threshold, a command is generated to increase the pressure

[0373] If the bed level is above a threshold, a command is generated to increase or decrease the pressure

[0374] If the gas residence time is above a threshold, generate a command to increase or decrease the pressure

[0375] If the graphite purity is above a threshold, generate instructions to increase or decrease the pressure

[0376] If the heat input is above a threshold, a command is generated to increase or decrease the pressure

[0377] If the bed resistivity is above a threshold, a command is generated to increase or decrease the pressure

[0378] If the catalyst-gas ratio is above a threshold, a command is generated to reduce the voltage or current

[0379] If the hydrogen purity is above the threshold, a command is generated to reduce the voltage or current

[0380] If the methane conversion rate is above a threshold, a command is generated to reduce the voltage or current

[0381] If hydrogen production is above a threshold, a command is generated to reduce voltage or current

[0382] If the reactor temperature is above a threshold, a command is generated to reduce the voltage or current

[0383] If the reactor superficial velocity is above a threshold, a command is generated to - voltage or current

[0384] If the bed level is above a threshold, a command is generated to reduce the voltage or current

[0385] If the gas residence time is above a threshold, a command is generated to reduce the voltage or current. If the graphite purity is above a threshold, a command is generated to reduce the voltage or current.

[0386] If the heat input is above a threshold, a command is generated to reduce the voltage or current

[0387] If the bed resistivity is above a threshold, a command is generated to reduce the voltage or current

[0388] If the catalyst-gas ratio is above a threshold, a command is generated to reduce the feed rate. If the hydrogen purity is above a threshold, a command is generated to reduce the feed rate.

[0389] If the methane conversion is above a threshold, a command is generated to reduce the feed rate

[0390] If hydrogen production is above a threshold, a command is generated to reduce the feed rate

[0391] If the reactor temperature is above a threshold, a command is generated to reduce the feed rate

[0392] Generates a command to increase the feed rate if the reactor superficial velocity is above a threshold. Generates a command to increase or decrease the feed rate if the bed level is above a threshold. Generates a command to decrease the feed rate if the gas residence time is above a threshold.

[0393] If the graphite purity is above a threshold, generate instructions to reduce the feed rate

[0394] If the heat input is above a threshold, a command is generated to reduce the feed rate

[0395] If the bed resistivity is above a threshold, a command is generated to increase the feed rate

[0396] If the catalyst-gas ratio is above a threshold, a command is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0397] If the hydrogen purity is above a threshold, a command is generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0398] If the methane conversion rate is above a threshold, a command is generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0399] If the hydrogen production is above a threshold, a command is generated to increase or decrease the catalyst addition rate (i.e., the primary particulate material addition rate)

[0400] If the reactor temperature is above a threshold, an instruction is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0401] If the reactor superficial velocity is above the threshold, an instruction is generated to - the catalyst addition rate (i.e., the primary particulate material addition rate)

[0402] If the bed level is above a threshold, a command is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0403] If the gas residence time is above a threshold, a command is generated to increase the catalyst addition rate (i.e., the primary particulate material addition rate)

[0404] If the graphite purity is above a threshold, an instruction is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0405] If the heat input is above a threshold, a command is generated to reduce the catalyst addition rate (i.e., the primary particulate material addition rate)

[0406] If the bed resistivity is above a threshold, a command is generated to - the catalyst addition rate (i.e., the primary particulate material addition rate)

[0407] If the catalyst-gas ratio is above a threshold, a command is generated to increase the pressure

[0408] If the hydrogen purity is above a threshold, a command is generated to increase or decrease the pressure

[0409] If the methane conversion rate is above a threshold, a command is generated to increase or decrease the pressure

[0410] If hydrogen production is above a threshold, a command is generated to increase or decrease pressure

[0411] If the reactor temperature is above a threshold, a command is generated to increase or decrease the pressure

[0412] If the reactor superficial velocity is above a threshold, a command is generated to reduce the pressure

[0413] If the bed level is above a threshold, a command is generated to increase or decrease the pressure

[0414] If the gas residence time is above a threshold, generate a command to increase or decrease the pressure

[0415] If the graphite purity is above a threshold, generate instructions to increase or decrease the pressure

[0416] If the heat input is above a threshold, a command is generated to increase or decrease the pressure

[0417] If the bed resistivity is above a threshold, a command is generated to increase or decrease the pressure

[0418] If the catalyst-gas ratio is above a threshold, a command is generated to increase the voltage or current

[0419] If the hydrogen purity is above a threshold, a command is generated to increase the voltage or current

[0420] If the methane conversion rate is above a threshold, a command is generated to increase the voltage or current

[0421] If hydrogen production is above a threshold, a command is generated to increase voltage or current

[0422] If the reactor temperature is above a threshold, a command is generated to increase the voltage or current

[0423] If the reactor superficial velocity is above a threshold, a command is generated to - voltage or current

[0424] If the bed level is above a threshold, a command is generated to increase the voltage or current

[0425] If the gas residence time is above a threshold, a command is generated to increase the voltage or current

[0426] If the graphite purity is above a threshold, a command is generated to increase the voltage or current

[0427] If the heat input is above a threshold, a command is generated to increase the voltage or current

[0428] If the bed resistivity is above a threshold, a command is generated to increase the voltage or current

[0429] Again, it should be understood that these are merely examples.

[0430] Example Electric Bed Heating Configuration

[0431] Figure 3A A diagram illustrating a system 300 including a FBR with induction heating configured to Figure 1 The examples disclosed herein are combined operations of methane pyrolysis.

[0432] In this example, a refractory-lined FBR 301 has three electrodes (302A-C) extending into the reactor chamber such that the electrodes are exposed to a fluidized bed of hydrocarbon gas and particulate material (including conductive particles). Current flowing between the electrodes is conducted through the conductive particles in this manner, causing them to heat up, thereby heating the entire contents of the reactor chamber due to conductivity and fluidization.

[0433] Although three electrodes are shown, there may be other numbers, and the positions may vary between embodiments.In some embodiments, the FBR housing serves as another electrode.

[0434] In operation, a high-voltage power supply 310 works in conjunction with a transformer 311 and a thyristor controller 312 (for controlling current, voltage, and power). The thyristor controller operates on a single-phase or three-phase AC voltage. This AC voltage is passed through a low-voltage cable to carry current across the electrodes, which can be either AC or DC (depending on the implementation).

[0435] In use, the feed gas supply 314 delivers hydrocarbons to the FBR 301. Specific material supply systems (not shown), such as Figure 2 The system delivers a controlled / metered supply of particulate material that acts as a catalyst for the pyrolysis of hydrocarbons in the FBR. The FBR releases an output 315 of product gas (including hydrogen) and particulate material (including graphite).

[0436] Example Induction Heating Configuration

[0437] Figure 3B A simplified cross-sectional view of a system 350 is shown, comprising a FBR with induction heating configured as shown in FIG. Figure 1 The examples disclosed herein are combined operations of methane pyrolysis.

[0438] System 350 includes a sidewall 351, which is preferably cylindrical and formed of a strong material selected from a group consisting of metals (e.g., steel). The height of the sidewall can vary between embodiments. Inside the sidewall is a sidewall cavity 352 and a refractory reactor shell 353 (e.g., a silica refractory material suitable for insulating the sidewall from excess heat and also suitable for encapsulating / supporting the conductive coils), which defines a central cavity 354 in which the fluidized bed (fluidizing components not illustrated) is maintained.

[0439] The chamber 354 has a plurality of connection ports (not shown) including: (i) at least one first inlet for delivering a feed gas (not shown) containing a hydrocarbon gas (e.g., methane), preferably located at or near the lower end; (ii) a second inlet for delivering a starting material feed, such as a graphite material, Hazer graphite, or an iron-containing catalyst (e.g., iron ore or synthetic iron oxide), preferably located at or near the upper end; and (iii) an outlet for releasing a process material comprising particles (including carbon) and a gas (including hydrogen). The coil may also be embedded in the refractory material.

[0440] A conductive coil 355 is housed within the sidewall cavity 352 such that the coil is positioned adjacent to the refractory reactor housing 353. The coil is configured to carry alternating current delivered via a high-frequency power supply 358 and input / output connections 356 and 357. The coil includes a central cavity through which a coolant (e.g., water) is configured to flow, thereby preventing the coil from reaching undesirable temperatures during use. The coil is spaced a threshold distance from the steel sidewall 351 to prevent inductive heating of the sidewall (this distance will vary between embodiments and is selected based on factors including the overall size of the system and current flux parameters). In some embodiments, the system includes multiple conductive coils. In some embodiments, each of the multiple conductive coils can be independently operated.

[0441] The alternating current transmitted through coil 355 induces induction within the process material, causing current to propagate throughout the conductive carbon particles in the process material. The electrical resistance in the carbon particles causes these particles to heat, thereby heating the entire process material. This enables the process material to reach and maintain a desired temperature range of approximately 600 to 1500 degrees Celsius.

[0442] Preferably, one or more temperature sensors are configured to monitor the temperature within the process material fluidized within the central chamber 354 and transmit the temperature data to the controller 359. The controller 359 executes software instructions configured to control the high frequency power supply 358 based on the temperature sensor data to maintain the process material within a desired temperature range.

[0443] 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 discussed above, it avoids components / areas where localized surface temperatures reach levels where carbon deposition occurs.

[0444] In some cases, controlled heating of process materials in reactors (particularly fluidized bed reactors) can be used to improve processes. This provides a range of advantages (discussed below), including (but not limited to) mitigation of problems associated with unwanted carbon surface deposition, the ability to adjust catalytic input, control of residence time, and control of product purity (e.g., carbon, particularly graphitic carbon in various forms, and hydrogen). Other advantages can include greater scalability, better temperature control, simpler construction, and increased energy efficiency.

[0445] Generally, the bottom layer pyrolysis method includes a method for pyrolysis of hydrocarbon gas, the method comprising: providing an initial feedstock of conductive carbon material to a fluidized bed reactor; commencing operation of the fluidized bed reactor, wherein the fluidized bed reactor is fed by an input of hydrocarbon gas; operating a power supply to deliver current (via controlled current and / or voltage) to one or more electrodes and / or conductive coils to heat the conductive carbon material to a predetermined temperature, wherein the predetermined temperature initiates and maintains pyrolysis of the hydrocarbon gas; and operating an outlet component to release process material from the fluidized bed reactor, wherein the released process material includes carbon material, unreacted hydrocarbon gas and / or hydrogen.

[0446] The hydrocarbon gas can be any gas stream containing light hydrocarbons. Illustrative examples of hydrocarbon gases include, but are not limited to, natural gas, coalbed methane, landfill gas, and biogas. The composition of the hydrocarbon gas can vary significantly, but will typically contain one or more light hydrocarbons from the group consisting of methane, ethane, ethylene, propane, and butane. In preferred embodiments, the hydrocarbon gas is selected from the group consisting of 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.

[0447] In a preferred embodiment, the hydrocarbon gas is natural gas.

[0448] In a preferred embodiment, the hydrocarbon gas is biogas.

[0449] In a preferred embodiment, the hydrocarbon gas consists essentially of methane.

[0450] The outlet member can be operated in a controlled or uncontrolled manner. In one embodiment, it is uncontrolled (the solids flow from the reactor is the result of particle elutriation). Therefore, the elutriation rate will depend on the geometry and overall design. Other means of operating the outlet member are also contemplated.

[0451] In one form of the invention, the FBR is operated at a pressure above atmospheric pressure. In one form of the invention, the FBR is operated at a pressure of about 0 bar to 100 bar. Preferably, the pressure is between about 0 bar and 50 bar. More preferably, the pressure is between about 0 bar and 20 bar. Even more preferably, the pressure is between about 2 bar and 10 bar.

[0452] In one form of the invention, the predetermined temperature is between about 600°C and 1500°C. Preferably, the predetermined temperature is between about 600°C and 1200°C. More preferably, the predetermined temperature is between about 800°C and 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.

[0453] In one form of the invention, the average temperature is between about 600°C and 1500°C. Preferably, the average temperature is between about 600°C and 1200°C. More preferably, the average temperature is between about 800°C and 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.

[0454] In embodiments, the graphite starting material has a purity greater than about 95% w / w. Preferably, the graphite starting material has a purity greater than about 99% w / w. More preferably, the graphite starting material has a purity greater than about 99.5% w / w. Most preferably, the graphite starting material has a purity greater than about 99.9% w / w.

[0455] In embodiments, the graphite starting material has a purity of about 50% w / w. Preferably, the graphite starting material has a purity of greater than about 60% w / w. More preferably, the graphite starting material has a purity of greater than about 70.5% w / w. Most preferably, the graphite starting material has a purity of greater than about 80% w / w.

[0456] In embodiments, the reclaimed graphite material has a purity greater than about 95% w / w. Preferably, the reclaimed graphite material has a purity greater than about 99% w / w. More preferably, the reclaimed graphite material has a purity greater than about 99.5% w / w. Most preferably, the reclaimed graphite material has a purity greater than about 99.9% w / w.

[0457] In one form of the invention, the iron-containing catalyst is a synthetic metal-containing catalyst. Throughout this specification, unless the context requires otherwise, the term "synthetic" will be understood to imply that the material has been synthesized by chemical techniques. Synthetic metal-containing catalysts are generally of higher purity.

[0458] In one form of the invention, the synthetic iron-containing catalyst is a synthetic iron oxide-containing material. In one form of the invention, the synthetic metal-containing catalyst iron oxide is Fe2O3 or Fe3O4.

[0459] In another form of the invention, the iron-containing catalyst is non-synthetic. Throughout this specification, unless the context requires otherwise, the term "non-synthetic" will be understood to imply that the material is not synthesized by chemical techniques. While the term "non-synthetic" does include naturally occurring materials, it should not be understood to exclude materials that have been physically enriched (e.g., squeezed and sieved or classified).

[0460] In one form of the invention, the iron-containing catalyst is a non-synthetic iron-containing oxide material. In one form of the invention, the iron-containing catalyst is a non-synthetic iron-containing oxide ore. In one form of the invention, the non-synthetic iron-containing oxide ore is iron ore. The iron ore can be hematite iron ore or goethite iron ore. The iron ore can be low-grade iron ore.

[0461] In one form of the invention, the iron-containing catalyst may undergo a pretreatment step to increase its catalytic effect. The pretreatment step may include high-temperature pre-reduction. Advantageously, the inventors have found that the present invention can omit such a pretreatment step.

[0462] As will be appreciated by those skilled in the art, graphite materials can exist in a variety of forms, for example:

[0463] Graphite fibers (which are fibrous carbon structures typically ranging in length from 100 nm to 100 microns), carbon nanotubes (CNTs) (which are cylindrical nanostructures containing single or multiple graphene sheets arranged concentrically or perpendicular to a central axis) are also within the scope of graphite fibers;

[0464] Carbon nanoonions (CNOs), which are structures composed of multiple spherical graphene sheets concentrically layered from a central core, typically a catalyst particle or void. These carbon structures typically have diameters in the range of 50-500 nm;

[0465] Carbon microspheres (CMS), which are hollow spherical graphite structures typically larger than 500 nm in size. They are spherical in shape but can also be chain-like. This synthetic form of graphite is novel and only occurs naturally in the following substances: meteorites; and

[0466] Graphene, which is a single-layer or single-digit-layer graphene sheet.

[0467] In an embodiment, the carbon material is selectively synthesized to substantially have one or more desired morphologies. In a preferred form of the present invention, the desired morphology is selected from the group comprising: graphite fiber, carbon nano-onion (CNO), carbon micro-shell (CMS) and graphene. More preferably, the graphite fiber comprises a mixture of carbon nanotubes (CNT) and other graphite fibers. In a preferred form of the present invention, the desired morphology is selected from the group comprising one or more: graphite fiber, carbon nano-onion (CNO), carbon micro-shell (CMS) and graphene. In an embodiment, the desired morphology mainly includes graphite fiber. In an embodiment, the desired morphology mainly includes carbon nano-onion (CNO). In an embodiment, the desired morphology mainly includes carbon micro-shell (CMS). In an embodiment, the desired morphology mainly includes graphene.

[0468] The use of current-based FBR heating allows for multiple reaction pathways beyond those described for Figure 1 The application scope of the iron ore catalyst is as follows:

[0469] (1) Using an iron-embedded carbon feedstock in conjunction with an iron ore catalyst. The iron ore catalyst enables the pyrolysis reaction to occur at a relatively low temperature (e.g., around 900 degrees Celsius), where carbon grows on the iron ore particles. The iron ore catalyst requires continuous or periodic replenishment because, although the catalyst is not consumed in the reaction, it is incorporated into the carbon and removed from the reactor within the extracted carbon particles.

[0470] (2) Using an iron-embedded carbon feedstock in conjunction with an iron ore catalyst. The iron ore catalyst enables the pyrolysis reaction to occur at relatively low temperatures (e.g., around 900°C), where carbon grows on the iron ore particles. The iron ore catalyst requires continuous or periodic replenishment because, although the catalyst is not consumed in the reaction, it is incorporated into the carbon and removed from the reactor within the extracted carbon particles.

[0471] (3) A graphite feedstock is used at the start of the reaction and the reaction is carried out in a high temperature, non-catalytic state. For example, induction heating can be used to raise the temperature of the process material to over 1000 degrees Celsius, preferably over 1100 degrees Celsius. In this state, the hydrocarbon feedstock gas decomposes into hydrogen and carbon, and the carbon grows on the flake graphite feedstock. The large particle carbon produced is extracted together with the output process material, and preferably; at least a portion of it is processed and recovered as graphite feedstock material for reintroduction into the reactor. The control system is configured to input additional graphite feedstock material into the reactor on a continuous or periodic basis, thereby providing a matrix on which carbon can be deposited in the pyrolysis reaction.

[0472] The latter option has the benefit that the reaction itself can produce a continuous supply of graphite feedstock material and the purity level of the carbon extracted from the FBR can be maintained at an extremely high level.

[0473] In some embodiments, the system or method of the present invention comprises a plurality of reactors. In some embodiments, the plurality of reactors are arranged in series or in parallel.

[0474] Conclusion and Interpretation

[0475] It will be appreciated that the foregoing disclosure provides useful improvements in the context of methane pyrolysis technology.

[0476] Although specific embodiments of the present invention have been described, it will be appreciated by those skilled in the art that there are other embodiments that are equivalent to the described embodiments. Therefore, it will be understood that the present invention is not limited by the specific embodiments described, but is limited only by the scope of the appended claims.

[0477] It should be understood that in the description of exemplary embodiments of the invention, various features of the invention are sometimes grouped together in a single example, figure, or description thereof for the purpose of simplifying the disclosure and aiding understanding of one or more of the various inventive aspects. However, this method of disclosure should not be interpreted as reflecting an intention that the claimed invention requires more features than are expressly recited in each claim. On the contrary, as reflected in the following claims, inventive aspects lie in less than all features of a single aforementioned disclosed embodiment. Therefore, 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 the invention.

[0478] Furthermore, while some embodiments described herein include some features included in other embodiments, they do not include other features included in other embodiments, and combinations of features from different embodiments are intended to be within the scope of the present invention and to form different embodiments, as will be understood by those skilled in the art. For example, in the following claims, any of the claimed embodiments may be used in any combination.

[0479] In addition, some of the embodiments described herein as methods or combinations of method elements can be implemented by a processor of a computer system or other device that performs functions. Therefore, a processor with the necessary instructions for performing such methods or method elements forms a device for performing the methods or method elements. In addition, the elements of the device embodiments described herein are examples of devices for performing the functions performed by the elements, for carrying out the purposes of the present invention.

[0480] Many specific details are set forth in the description provided herein. However, it should be understood that embodiments of the present invention can be practiced without these specific details. In other cases, well-known methods, structures, and techniques are not presented in detail to avoid obscuring an understanding of this specification.

[0481] Likewise, it is important to note that when the term “coupled” is used in the claims, it should not be construed as limited to direct connections. The terms “coupled” and “connected,” along with their derivatives, may be used. It should be understood that these terms are not synonymous with each other. Thus, the expression “device A is coupled to device B” should not be limited to devices or systems where the output of device A is directly connected to the input of device B. This means that there is a path between the output of A and the input of B, which may be a path involving other devices or equipment. “Coupled” can mean that two or more elements are in direct physical or electrical contact, or it can mean that two or more elements are not in direct contact with each other but still cooperate or interact with each other.

[0482] Thus, while what is considered to be the preferred embodiment of the present invention has been described, it will be appreciated by those skilled in the art that other and further modifications may be made thereto without departing from the spirit of the invention, and it is intended that all such changes and modifications be within the scope of the invention. For example, any formulas given above are merely representative of possible procedures. Functions may be added or deleted from the block diagrams, and operations may be interchanged between functional blocks. Steps may be added to or deleted from the described methods within the scope of the invention.

Claims

1. A method for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber in which hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material, the method comprising: receiving time-series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, wherein the reactor output sensor system is configured to monitor a composition of a reactor output released from the reactor subsystem; processing the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output; operating a control optimization module to process data including the one or more parameters representing real-time reactor subsystem outputs based on the computer executable code to generate one or more control instructions; as well as The operation control module thus sends the one or more control instructions to achieve control of at least one of the following: (i) a heating control system, wherein the heating control system controls the current and / or voltage level applied to one or more electrodes configured to deliver current into the reactor chamber such that the current propagates through the electrically conductive particulate material; and (ii) a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control the metered delivery of a primary particulate material into the reactor chamber.

2. The method of claim 1 , wherein the one or more parameters are related to each of: (i) a measurement of hydrogen in the reactor output; and (ii) a measurement of one or more particulate materials in the reactor output.

3. The method of claim 1, wherein the one or more parameters are related to a measurement of hydrogen in the reactor output.

4. The method of claim 1, wherein the one or more parameters are related to measurements of one or more particulate materials in the reactor output.

5. The method of any one of claims 1-4, wherein the one or more control instructions implement control of each of the heating control system and the particulate matter transport control system.

6. The method according to any one of claims 1 to 4, wherein the one or more control instructions implement control of a heating control system.

7. The method of any one of claims 1-4, wherein the one or more control instructions implement control of the particulate matter transport control system.

8. A method as described in any of the preceding claims, wherein the one or more parameters representing real-time reactor subsystem output are derived from the following selections: a measurement of the relative proportion of hydrogen in the gas mixture; a measurement of the purity of the mixture based on hydrogen; the amount of hydrogen passing through a region over time; a measurement of particle fluidity; a measurement of particle conductivity; a measurement of graphite particle purity; a measurement of the ratio of the primary particulate material to the conductive particulate material; and the temperature of the hydrogen-containing output stream; an indicator related to the amount of one or more particulate materials released from the reactor subsystem over time; an indicator related to the particle size of one or more particulate materials released from the reactor subsystem; an indicator related to the morphology of one or more particulate materials released from the reactor subsystem.

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

10. A method as described in any of the preceding claims, wherein the one or more control instructions include control instructions representing one or more of the following: (i) instructions to adjust the rate at which the primary particulate material is released into the reactor chamber; (ii) instructions to release a defined amount of the primary particulate material into the reactor chamber at a defined rate; (iii) instructions to perform batch delivery of a defined amount of the primary particulate material into the reactor chamber at a defined time; (iv) and instructions to adjust the rate of pneumatic conveying fluid for the primary particulate material; instructions to adjust the batch size for the primary particulate material; or (vi) instructions to adjust the batch frequency for the primary particulate material.

11. The method of any preceding claim, wherein the one or more control instructions include instructions that result in an increase or decrease in the amount of current and / or voltage delivered through the one or more electrodes of the heating control system.

12. The method of claim 11, wherein the instructions that result in increasing or decreasing the amount of current and / or voltage delivered through the one or more electrodes of the heating control system represent a defined target temperature change within the reactor chamber.

13. The method of any one of the preceding claims, wherein the one or more control instructions comprise instructions to a processor that controls an operating parameter of the fluidized bed reactor, resulting in adjustments relating to any one or more of heating, fluidization rate, and / or pressure.

14. The method of any preceding claim, wherein the reactor subsystem includes a reactor controller module, and wherein the operations control module thereby sending the one or more control instructions includes providing a signal to the reactor controller module to cause the reactor control module to operate in a defined manner.

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

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

17. A method as claimed in any preceding claim, wherein the particulate matter delivery control system comprises a quantity determination device configured to measure the amount of the precursor particulate material prior to delivery to the reactor chamber.

18. The method of claim 17, wherein the particulate matter transport control system comprises a particulate matter storage assembly coupled to a particulate matter transport assembly, wherein the particulate matter transport assembly includes a transport antechamber configured to be selectively pressurized during transport of the precursor particulate material prior to transport to the reactor chamber.

19. The method of any preceding claim, wherein the control optimization module for processing data is additionally configured to process data from one or more other sources, the other sources comprising: (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) inputs representing one or more parameters derived from monitoring of particulate matter detected in the output of said reactor subsystem; (iv) inputs representing one or more input gas delivery parameters; (v) input representing desired future operating conditions for the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the output of the reactor subsystem.

20. A method as claimed in any one of the preceding claims, wherein the electrically conductive particulate material comprises one or more particulate materials selected from the group comprising: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides; preferably, the electrically conductive material is selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low-grade iron oxides.

21. The method of any one of the preceding claims, wherein the primary particulate material comprises a catalytic particulate material for pyrolysis of hydrocarbons within the reactor subsystem.

22. A method as claimed in any one of the preceding claims, wherein the primary particulate material comprises a material selected from the group comprising: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides or low grade iron oxides.

23. A method as claimed in any preceding claim, wherein the primary particulate material comprises a graphite material.

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

25. The method of any preceding claim, wherein the control optimization module is responsive to the one or more parameters representing reactor subsystem outputs and an additional input representing desired future operation to generate the one or more control commands.

26. The method of claim 25, wherein the input representative of desired future operation comprises any one or more of: (i) a desired hydrogen output parameter; (ii) a desired carbon output parameter; and (iii) a desired carbon output form.

27. A system for controlling a hydrocarbon gas pyrolysis process, wherein the hydrocarbon gas pyrolysis process comprises operating a reactor subsystem having a reactor chamber in which hydrocarbon gas decomposes in the presence of an electrically 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, wherein the reactor output sensor system is configured to monitor the composition of a reactor output released from the reactor subsystem; a processing module configured to process the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output; a control optimization module operable to process data including the one or more parameters representing real-time reactor subsystem outputs based on the computer executable code to generate one or more control instructions; as well as a control module operable to send the one or more control instructions to effectuate control of at least one of: a heating control system, wherein the heating control system controls current and / or voltage levels applied to one or more electrodes, the one or more electrodes being configured to deliver current into the reactor chamber such that the current propagates through the conductive particulate material; and a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control metered delivery of primary particulate material into the reactor chamber.

28. The system of claim 27, wherein the one or more parameters are related to each of: (i) a measurement of hydrogen in the reactor output; and (ii) a measurement of one or more particulate materials in the reactor output.

29. The system of claim 27, wherein the one or more parameters are related to a measurement of hydrogen in the reactor output.

30. The system of claim 27, wherein the one or more parameters are related to measurements of one or more particulate materials in the reactor output.

31. The system of any one of claims 27-30, wherein the one or more control instructions implement control of each of the heating control system and the particulate matter transport control system.

32. The system of any one of claims 27-30, wherein the one or more control instructions implement control of a heating control system.

33. The system of any one of claims 27-30, wherein the one or more control instructions implement control of the particulate matter transport control system.

34. A system as described in any of claims 27-33, wherein the one or more parameters representing real-time reactor subsystem output are derived from the following: a measurement of the relative proportion of hydrogen in the gas mixture; a measurement of the purity of the mixture based on hydrogen; the amount of hydrogen passing through a region as a function of time; a measurement of particle fluidity; a measurement of particle conductivity; a measurement of graphite particle purity; a measurement of the ratio of the primary particulate material to the conductive particulate material; and the temperature of the hydrogen-containing output stream; an indicator related to the amount of one or more particulate materials released from the reactor subsystem as a function of time; an indicator related to the particle size of one or more particulate materials released from the reactor subsystem; an indicator related to the morphology of one or more particulate materials released from the reactor subsystem.

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

36. A system as described in any one of claims 27-35, wherein the one or more control instructions include control instructions representing one or more of the following: (i) instructions to adjust the rate at which the primary particulate material is released into the reactor chamber; (ii) instructions to release a defined amount of the primary particulate material into the reactor chamber at a defined rate; (iii) instructions to perform batch delivery of a defined amount of the primary particulate material into the reactor chamber at a defined time; (iv) and instructions to adjust the rate of pneumatic conveying fluid used for the primary particulate material; instructions to adjust the batch size used for the primary particulate material; or (vi) instructions to adjust the batch frequency used for the primary particulate material.

37. The system of any one of claims 27-36, wherein the one or more control instructions include instructions that result in an increase or decrease in the amount of current and / or voltage delivered through the one or more electrodes of the heating control system.

38. The system of claim 37, wherein the instructions that result in increasing or decreasing the amount of current and / or voltage delivered through the one or more electrodes of the heating control system represent a target temperature change defined within the reactor chamber.

39. The system of any one of claims 27-38, wherein the one or more control instructions comprise instructions to a processor that controls an operating parameter of the fluidized bed reactor, resulting in adjustments related to any one or more of heating, fluidization rate, and / or pressure.

40. The system of any one of claims 27-39, wherein the reactor subsystem includes a reactor controller module, and wherein operating the control module to send the one or more control instructions includes providing a signal to the reactor controller module to cause the reactor control module to operate in a defined manner.

41. The system of any one of claims 27-40, wherein causing the reactor control module to operate in a defined manner comprises causing the reactor control module to: (i) increase or decrease heat in the reactor chamber; (ii) change one or more fluidization parameters within the reactor chamber; or (iii) change the pressure within the reactor chamber.

42. The system of any one of claims 27-41, wherein the reactor subsystem comprises a fluidized bed reactor.

43. The system of any one of claims 27-42, wherein the particulate matter delivery control system includes a quantity determination device configured to measure the amount of the precursor particulate material prior to delivery to the reactor chamber.

44. The system of any one of claims 27-43, wherein the particulate matter transport control system comprises a particulate matter storage assembly coupled to a particulate matter transport assembly, wherein the particulate matter transport assembly comprises a transport antechamber configured to be selectively pressurized during transport of the primary particulate material prior to transport to the reactor chamber.

45. The system of any one of claims 27-44, wherein the control optimization module for processing data is further configured to process data from one or more other sources, the other sources comprising: (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 of particulate matter detected in the output of said reactor subsystem; (iv) an input representing one or more input gas delivery parameters; (v) input representing desired future operating conditions for the reactor subsystem; and (vi) an input representing one or more parameters related to gases other than hydrogen detected in the output of the reactor subsystem.

46. ​​The system of any one of claims 27-45, wherein the electrically conductive particulate material comprises one or more particulate materials selected from the group consisting of: a graphite starting material, a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or low-grade iron oxides; preferably, the electrically conductive material is selected from the group consisting of: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or low-grade iron oxides.

47. The system of any one of claims 27-46, wherein the primary particulate material comprises a catalytic particulate material for pyrolysis of hydrocarbons within the reactor subsystem.

48. The system of any one of claims 27-47, wherein the primary particulate material comprises a material selected from the group consisting of: a carbon material with encapsulated iron, iron ore, synthetic or naturally occurring iron oxides, or low-grade iron oxides.

49. The system of any one of claims 27-48, wherein the primary particulate material comprises a graphite material.

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

51. The system of any one of claims 27-50, the control optimization module generating the one or more control commands in response to the one or more parameters representing reactor subsystem outputs and an additional input representing desired future operation.

52. The system of claim 51, wherein the inputs representing desired future operation include any one or more of: (i) desired hydrogen output parameters; (ii) desired carbon output parameters; and (iii) desired carbon output form.

53. A method for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber in which hydrocarbon gas is decomposed in the presence of an electrically conductive particulate material, the method comprising: receiving time-series input data from a reactor output sensor system provided by the hydrocarbon gas pyrolysis system, wherein the reactor output sensor system is configured to monitor a composition of a reactor output released from the reactor subsystem; processing the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output; operating a control optimization module to process data including the one or more parameters representing real-time reactor subsystem outputs based on the computer executable code to generate one or more control instructions; as well as The operation control module thereby sends the one or more control instructions to achieve control of at least one of the following: a heating control system, wherein the heating control system controls the temperature within the reactor chamber; and a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control the metered delivery of primary particulate material into the reactor chamber.

54. A system for controlling a hydrocarbon gas pyrolysis system, wherein the hydrocarbon gas pyrolysis system includes a reactor subsystem having a reactor chamber in which hydrocarbon gas is decomposed in the presence of an electrically 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, wherein the reactor output sensor system is configured to monitor the composition of a reactor output released from the reactor subsystem; a processing module configured to process the time series input data to determine one or more parameters representative of a real-time reactor subsystem output, wherein the one or more parameters representative of a real-time reactor subsystem output are related to either or both of: (i) a measure of hydrogen in the reactor output; and (ii) a measure of particulate material in the reactor output; a control optimization module operable to process data including the one or more parameters representing real-time reactor subsystem outputs based on the computer executable code to generate one or more control instructions; as well as a control module operable to send the one or more control instructions to effectuate control of at least one of: a heating control system, wherein the heating control system controls the temperature within the reactor chamber; and a particulate matter delivery control system, wherein the particulate matter delivery control system is configured to control metered delivery of primary particulate material into the reactor chamber.

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