Systems and methods for producing hydrogen and carbon

Abstract

A method for producing hydrogen and carbon from a hydrocarbon in a reaction chamber is provided. The method includes introducing a hydrocarbon into the chamber such that the hydrocarbon rotates in a first direction. The method includes generating a direct current (DC) based plasma from a portion of the hydrocarbon, where the hydrocarbon is heated, at least in part, by the DC based plasma to a temperature greater than 1,000° C. The method includes rotating the DC based plasma in a second direction different from the first direction. The method includes converting the hydrocarbon into elemental components of the hydrocarbon, including carbon solids and hydrogen gas. The method includes separating the carbon solids from the hydrogen gas to provide a solid portion and a gas portion.

Description

[Technical field]

[0001] Related Patent Cross-References This application claims priority to U.S. Provisional Patent Application No. 63 / 235,025, filed August 19, 2021, entitled "Systems and Methods for the Production of Hydrogen and / or Carbon," and U.S. Provisional Patent Application No. 63 / 242,273, filed September 9, 2021, entitled "Systems and Methods for the Production of Hydrogen from Liquids, Oils, Semi-Solid Hydrocarbons," the disclosures of each of which are incorporated by reference in their entireties herein.

[0002] Embodiments are disclosed relating to systems and methods for the production of hydrogen and / or carbon black that involve the use of plasma-induced decomposition of hydrocarbon feedstocks. The embodiments disclosed herein relate to hydrogen production systems and methods that utilize any type of liquid, oil, or semi-solid hydrocarbon as a primary feedstock and utilize gaseous hydrocarbons for plasma-based pyrolysis. [Background technology]

[0003] Various devices and methods have been utilized over the years to crack hydrocarbons into their constituent molecules, namely hydrogen and carbon. The uses of these by-products are diverse. For example, hydrogen is used in numerous applications in various sectors, including but not limited to the industrial and transportation sectors. When the hydrocarbons are cracked into their constituent molecules, the result may include a synthesis gas that contains hydrogen. In some embodiments, the synthesis gas is further processed to separate the hydrogen.

[0004] Moreover, carbon by-products have many uses, including when the carbon by-products are processed into carbon black, a form of paracrystalline carbon with a high surface area to volume ratio, which can be used in many applications, including tires, hoses, belts, pipes, inks, batteries, plastics, and other products where a black color is desired.

[0005] Conventional prior art devices and methods utilized to crack hydrocarbons into hydrogen and carbon include steam methane reforming (SMR) and polymer electrolyte membrane (PEM) cells. SMR is a method of producing synthesis gas (hydrogen and carbon monoxide) by reacting hydrocarbons with water (as steam), which releases significant amounts of carbon dioxide (CO2), e.g., about 3-10 kg CO2 per kg of hydrogen produced. PEM cells can also be used to crack hydrocarbons from methanol, which also releases significant amounts of CO2, e.g., about 1-3 kg CO2 per kg of hydrogen produced. Furthermore, conventional prior art devices and methods dissociate only about 70% of the input hydrocarbon gas, in other words, conventional prior art devices and methods have a maximum efficiency of 70% in generating hydrogen and carbon from a hydrocarbon gas input.

[0006] Such processes are highly polluting, releasing many tonnes of greenhouse gases each year, and are inefficient in that each requires a significant amount of energy to produce one kilogram (kg) of hydrogen.

[0007] Light and heavy refinery residual oils, semi-solids, and natural gas have long been sources for producing hydrogen and carbon. Examples include partial gasification in the presence of water for hydrogen and water quenching for carbon black, through processes that dissociate the hydrocarbon molecules into carbon and hydrogen. When processing these hydrocarbon-containing materials (refinery oils, semi-solids, natural gas, etc.), the hydrocarbon-containing materials have typically been used as an energy source to produce hydrogen and carbon. Summary of the Invention [Means for solving the problem]

[0008] Due to the high temperatures involved in the process of producing hydrogen and carbon from hydrocarbon-containing materials, the high flow rates used for both energy and feedstock, and the difficulties in trying to control the properties of the products resulting from such complex processes, there is a need for methods and apparatus for producing such products in a more efficient and effective manner that requires less energy and improves the properties of the products produced. Furthermore, there is a need for methods and apparatus for producing such products without significant CO2 emissions or other pollution. Furthermore, methods for producing hydrogen and carbon from oils, lubricants, waste oils, and semi-solids are unique to the industry and are needed to prevent these waste products from being sold and burned for heat, releasing large amounts of CO2. It should be noted that approximately 80% of the recycled oil is not recycled, but simply filtered and burned. The embodiments shown and described herein represent an advancement over the prior art through the use of plasma and other system elements to directly utilize plasma energy into these feedstocks to produce hydrogen and high grade carbon black from a variety of feedstocks in an energy-efficient and environmentally friendly manner. Embodiments can produce hydrogen and / or carbon with significantly less CO2 emissions or other pollution than prior methods, and in embodiments can do so without any of the CO2 emissions or other pollution that would result from treating a hydrocarbon-containing gas without oxygen as a plasma source and transferring its high energy directly to liquids and semi-solids as heat. Embodiments can dissociate both gaseous and liquid hydrocarbons substantially greater than 70% (although prior art devices cannot achieve this in liquids), and in embodiments reach dissociation rates of greater than 98%, up to substantially 100% (e.g., 99.99%).

[0009] Embodiments herein describe, among other things, methods and apparatus for generating hydrogen and carbon (e.g., carbon powder) by dissociating methane and other hydrocarbons through the use of a system that utilizes a plasma discharge and a reaction chamber. In embodiments, a hydrocarbon gas is introduced into the reaction chamber at an angle such that the hydrocarbon gas rotates within the chamber and is in rotational contact with the plasma created within the chamber. In some embodiments, the plasma is also regulated by a current-controlled magnet to rotate at high rotational speeds within the chamber and in a different (e.g., opposite) direction compared to the rotation of the hydrocarbon gas.

[0010] In some embodiments, the plasma and the hydrocarbon gas are rotated in counter-rotating directions. The relative angular rotation of the gas and plasma results in increased generation of plasma that contacts the gas and dissociates the hydrocarbons into elemental components of hydrogen and carbon, providing processing for separation and purification of the resulting product, such as quenching to produce carbon black. Various plasma techniques may also be used, including, for example, DC plasma, or a combination of DC plasma and RF plasma.

[0011] Embodiments can be realized as small modular units. These small modular units can then be loaded onto a mobile vehicle (e.g., a ship) and processed on the move or at the point of unloading, with the advantages described herein. Because the conversion vessel (including the hydrocarbon dissociation system described herein) is offshore, it does not need to expend energy to produce the additional cooling water / liquids required for the conversion process, but simply pumps in and out all the cooling liquids required. This is a huge energy savings and a huge reduction in emissions emitted.

[0012] Advantages include: Hydrogen is very light, making it costly to transport even as a liquid. Countries that want to move beyond the emissions from using hydrocarbon fuels to drive a hydrogen economy, but do not have the resources to produce this clean-burning fuel at affordable and practical economic levels, would still have the option of purchasing Liquid Natural Gas ("LNG"), given their existing resources and transportation infrastructure, and converting the LNG to H2 at a point when the most efficient transportation is completed and bulk storage is most advantageous.

[0013] The carbon produced by fuel conversion needs to be removed, and since it is completely inert, it can also be collected and sold if the receiving customer wishes for further processing on land, or it can be dumped overboard. Recovery is desirable since there may be future discoveries and uses for this material.

[0014] In some embodiments, by producing electricity on board for the conversion process, power generation on ships at sea is subject to different regulations versus power generation on land. The proposed method would use regasified LNG as natural gas in the generator sets of the conversion ship, a much cleaner option than diesel or bunker fuels.

[0015] Further advantages of the embodiments are operational and raw material costs, which are improved by using plasma to induce dissociation in the manner described herein. Additionally, the embodiments are efficient, allowing the maximum utilization of every kilowatt used to process the conversion of feedstock to products. The embodiments improve the productivity and efficiency of the dissociation process over known methods.

[0016] According to a first aspect, there is provided a method of producing hydrogen and carbon from a hydrocarbon in a reaction chamber. The method includes introducing a hydrocarbon into the chamber such that the hydrocarbon rotates in a first direction. The method includes generating a direct current (DC) based plasma from a portion of the hydrocarbon, the hydrocarbon being heated at least in part by the DC based plasma to a temperature greater than 1,000° C. The method includes rotating the DC based plasma in a second direction different from the first direction. The method includes converting the hydrocarbon into elemental components of the hydrocarbon including carbon solids and hydrogen gas. The method includes separating the carbon solids from the hydrogen gas to provide a solid portion and a gas portion.

[0017] According to a second aspect, an apparatus for producing hydrogen and carbon solids from gaseous hydrocarbons is provided. The apparatus comprises a process chamber having a gas inlet, a gas outlet and a solids outlet. The apparatus comprises a direct current (DC) plasma generator configured to generate a plasma in a plasma processing zone of the process chamber, the DC plasma generator comprising a cathode and an anode in the process chamber, the DC plasma generator configured to heat gas passing through the plasma processing zone to a temperature above 1000°C and dissociate hydrocarbons in the gas. The apparatus comprises a magnet external to the process chamber configured to rotate the plasma generated by the DC plasma generator. The apparatus includes a cooling system in a separation zone of the process chamber, and the gas inlet is configured to rotate the gas passing through the gas inlet.

[0018] According to a third aspect, an apparatus for producing hydrogen and carbon solids from gaseous hydrocarbons is provided. The apparatus includes a process chamber having a gas inlet, a gas outlet, and a solids outlet. The apparatus includes a plasma generator configured to generate a plasma in a plasma processing zone of the process chamber, the DC plasma generator configured such that the plasma heats gas passing through the plasma processing zone to a temperature of more than 1,400° C. to dissociate the hydrocarbons in the gas. The apparatus includes a magnet external to the process chamber configured to rotate the plasma generated by the DC plasma generator. The apparatus includes a cooling system in a separation zone of the process chamber, the cooling system capable of reducing the gas temperature to about 500° C. (or 1,000° C.) or less to stop the formation of carbon black particles, aggregates, and agglomerates.

[0019] According to a fourth aspect, there is provided a method of producing hydrogen and carbon solids from liquid hydrocarbons. The method includes introducing liquid hydrocarbons into a process vessel. The method includes introducing a plasma-forming gas. The method includes forming or maintaining a DC plasma discharge between a cathode and an anode based at least in part on the plasma-forming gas, the anode being rotatable and at least partially immersed in the liquid hydrocarbon. The method includes rotating the anode to form a liquid film over the anode, whereby the hydrocarbons in the liquid film are heated by the DC plasma discharge to a temperature in the range of 1500K to 6000K, whereby at least a portion of the hydrocarbons in the liquid film are converted to elemental components. The method includes cooling the components to form a product mixture of gas and solids comprising hydrogen gas and carbon solids. The method includes extracting the product mixture of hydrogen gas and carbon solids.

[0020] According to a fifth aspect, there is provided a system for producing hydrogen and carbon solids from liquid hydrocarbons. The system comprises a process vessel having a first region for receiving a gas and a second region for receiving a liquid hydrocarbon. The system comprises a cathode and an anode for forming or maintaining a DC plasma discharge between the cathode and the anode, the anode being rotatable. The system comprises a gas output in the first region. The system comprises a carbon output in the second region. The system comprises a liquid inlet in the second region for introducing the liquid hydrocarbon into the process vessel. The system comprises a power source coupled to the anode and the cathode.

[0021] According to a sixth aspect, there is provided a system for producing hydrogen and carbon solids from liquid hydrocarbons. The system comprises an array of process vessels, each process vessel having a first region for containing a gas and a second region for containing a liquid hydrocarbon. The system comprises each process vessel having a cathode and an anode for forming or maintaining a DC plasma discharge between the cathode and the anode, the anode being rotatable. Each process vessel has a gas output in the first region, a carbon output in the second region, a liquid inlet in the second region for introducing the liquid hydrocarbon into the process vessel, and a power source coupled to the anode and the cathode.

[0022] According to a seventh aspect, there is provided a method of producing hydrogen and carbon solids from liquid hydrocarbons. The method includes introducing the liquid hydrocarbon into a process vessel. The method includes introducing a plasma-forming gas. The method includes forming or maintaining a plasma between a cathode and an anode based at least in part on the plasma-forming gas. The method includes directing a plasma jet formed from the plasma at the liquid hydrocarbon, whereby the hydrocarbon proximate the plasma jet is heated by the plasma jet to a temperature in the range of 1500K to 6000K, whereby at least a portion of the hydrocarbon proximate the plasma jet is converted to elemental components. The method includes cooling the components to form a product mixture of gas and solids comprising hydrogen gas and carbon solids. The method includes extracting the product mixture of gas and solids.

[0023] According to an eighth aspect, there is provided a system for producing hydrogen and carbon solids from liquid hydrocarbons. The system comprises a process vessel having a first region for receiving a gas and a second region for receiving a liquid hydrocarbon. The system comprises a plasma formation reactor having a cathode and an anode for forming or maintaining a plasma between the cathode and the anode, and further comprising a nozzle for directing a plasma jet formed from the plasma to the second region. The system comprises a gas output in the first region. The system comprises a carbon output in the second region. The system comprises a liquid inlet in the second region for introducing the liquid hydrocarbon into the process vessel. The system comprises a power source coupled to the anode and the cathode.

[0024] According to a ninth aspect, there is provided a system for producing hydrogen and carbon solids from liquid hydrocarbons, the system comprising an array of process vessels, each process vessel having a first region for containing a gas and a second region for containing liquid hydrocarbons, each process vessel having a plasma forming reactor having a cathode and an anode for forming or maintaining a plasma between the cathode and the anode, the plasma forming reactor further having a nozzle for directing a plasma jet formed from the plasma to the second region, a gas output in the first region, a carbon output in the second region, a liquid inlet in the second region for introducing the liquid hydrocarbon into the process vessel, and a power source coupled to the anode and the cathode.

[0025] The accompanying drawings, which are incorporated in and form a part of this specification, illustrate various embodiments. [Brief description of the drawings]

[0026] [Figure 1] FIG. 1 illustrates a hydrocarbon dissociation system according to one embodiment.

[0027] [Diagram 2] FIG. 1 illustrates a hydrocarbon dissociation system according to one embodiment.

[0028] [Diagram 3] FIG. 1 illustrates a reactor according to one embodiment.

[0029] [Figure 4] FIG. 1 illustrates a reactor according to one embodiment.

[0030] [Diagram 5] 1A and 1B show a gas injection system according to one embodiment.

[0031] [Figure 6] 1A-1D show SEM micrographs of clusters of carbon particles at different temperatures, according to one embodiment.

[0032] [Figure 7] 1A and 1B show a dynamic cathode positioner according to one embodiment.

[0033] [Figure 8] 1A, 1B, and 1C are diagrams illustrating nozzle openings for flowing source gases into the system chamber, according to one embodiment.

[0034] [Figure 9A] FIG. 2 illustrates a cathode according to one embodiment. [Figure 9B] FIG. 2 illustrates a cathode according to one embodiment. [Figure 9C] FIG. 2 illustrates a cathode according to one embodiment.

[0035] [Figure 9D] FIG. 2 illustrates a cathode insertion device according to one embodiment.

[0036] [Figure 10] FIG. 1 illustrates a liquid hydrocarbon dissociation system that utilizes a rotating drum to create a liquid film, according to one embodiment.

[0037] [Figure 11]FIG. 1 illustrates a liquid hydrocarbon dissociation system utilizing an inserted sub-fluid cone intimate contact device according to one embodiment.

[0038] [Figure 12] FIG. 1 illustrates a multiple liquid hydrocarbon dissociation system utilizing a rotating drum generated liquid film device as a method for combining fluid holding vessels, fluid filtration requirements, cooling requirements, and gas filtration and purification requirements, according to one embodiment.

[0039] [Figure 13] FIG. 1 illustrates a hydrogen dissociation system according to one embodiment.

[0040] [Figure 14] FIG. 2 illustrates a process vessel with a top cathode according to one embodiment.

[0041] [Figure 15] FIG. 1 illustrates a process vessel with a plasma torch or reactor on top, according to one embodiment.

[0042] [Figure 16] FIG. 2 illustrates an illustration of a block process flow for a hydrocarbon dissociation system, according to one embodiment. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0043] The following description is generally applicable to the embodiments of the hydrocarbon dissociation systems disclosed herein, including the hydrocarbon dissociation systems illustrated in the figures of this disclosure. As described below, some embodiments are applicable to the dissociation of various forms of hydrocarbons, including gas, liquid, semi-liquid, etc.

[0044] In some embodiments, regardless of the type of plasma reactor used, control software is employed to enhance the use of the plasma reactor based on measurable parameters, e.g., to improve energy usage, conversion efficiency, etc. In these embodiments, key performance measurements may be monitored to enhance control of the reactor. One measurement may include the amount of energy used to generate each kilogram of hydrogen, and in embodiments, the control system attempts to ensure that this value is consistent and as small as possible. In embodiments, for pyrolysis and thermolysis (high temperature pyrolysis without oxygen) processes, the following equations may be utilized to assist in process control and govern one or more of gas flow rates and pressures, power levels between the cathode and anode, and magnet power to rotation speed, among other process parameters applicable to a given plasma reactor.

[0045] In an embodiment, one or more process parameters may be adjusted by a process control index to maintain the mass and quality of the product output. One process control index may be the kilograms (mass) of hydrogen produced per hour divided by the kilograms of methane used. This percentage is continuously compared to a threshold, such as a laboratory documented ratio of 98%. If the percentage changes, directly controlled variables such as flow rate (e.g., controlled by one or more control valves) and electrical input (e.g., controlled by a power supply control) may be adjusted by a control software algorithm. The mass and purity of methane used may be measured directly and compared to Equation 1 below to ensure consistency. The mass and purity of hydrogen produced may be measured directly and calculated from flow rate, temperature, and gas chromatograph measurements. The electrical variables total energy, applied voltage consistency, and phase voltage may be determined by Equations 2, 3, and 4 below. Because these are the result of controlled equipment variables and have a direct impact on the conversion of methane to hydrogen, the impact on methane may be adjusted to maintain a consistent output volume and quality of hydrogen.

[0046] Equation 1: Mass flow rate In total =Out solids +Out Gas +By-pass Gas / Hydrocarbon vapor In = current hydrocarbon mass flow rate (m per hour) 3 direct measurement) Out solids = Carbon black collection / discharge separation and cyclone mass Out gas = Calculated syngas mass flow minus monitored CO2 (treatment control of O2 contamination / leakage of input hydrocarbons in the system) By-pass gas / hydrocarbon = the volume of stream from a filtration process that does not pass through the filter or is adsorbed by an adsorbent. The unwanted part of a purification process.

[0047] Equation 2: Energy Used for DC / RF Total Heating Energy = DC Watts + RF Watts (if used) - Watts generated in ORC (ORC = Organic Rankine Cycle Cooling)

[0048] Equation 3: Voltage Consistency Cathode / anode differential voltage = direct measurement - pre-set parameter The preset parameters are experimentally determined and input as reference variables; experimental determinations; made in advance for desired product properties; H2 percent conversion, the desired product value for carbon black. In embodiments using a positionable cathode that maintains a consistent cathode to anode distance, the magnitude of the difference may be used by a control software program to adjust the position of the cathode, and the position of the cathode is adjusted to keep this difference to a minimum. The cathode voltage can be adjusted as a secondary method after the positioning software, and this voltage change may or may not be limited to one percent of the range or a statistical fraction of the differential voltage as an initial small adjustment (followed by a position change).

[0049] Equation 4: Anode voltage / phase as a way to rotate the DC discharge around the inner diameter of the anode and create a high intensity plasma volume that allows dissociation Actual anode voltage change (from experimentally established median value) = Inlet gas flow rate change (real-time measured parameter) (corrected for gas law for temperature vs. volume) x Experimentally determined and preset raw material to product conversion percentage x Anode operating voltage (real-time measurement parameter) (rate of change per V voltage unit from 100 to 700 VDC) = Anode voltage change adjusted in real time.

[0050] The goal of the process control software is to maintain the primary conversion rate from hydrocarbons at the highest achievable value (e.g., 100%) to hydrogen or the lowest consistent energy value to another product quality attribute. Measurements of process parameters such as pressure, flow, voltage, current, etc., augmented by chemical analytical instruments downstream of the hydrogen and carbon separation process sections that more directly determine the percent hydrogen content of the total gas stream, are utilized within the software coding with the above equations (which are equations discussed above as Equations 1-4) while being compared to experimentally determined process parameter relationships.

[0051] The anode is configured and operated in such a manner as to maximize the amount of discharge moving around the reactor / torch plasma gas flow space. Both the voltage and "spin speed" of the discharge affect the operational results such as feed to product hydrogen and carbon black structure results. Control software is utilized to keep the desired results constant.

[0052] Some embodiments (such as those described herein with respect to Figures 1-9) are directed to reactors designed to dissociate hydrocarbon gases. These embodiments are generally described below.

[0053] In some embodiments, a plasma reactor is provided that includes a reaction chamber that may be formed by ceramic-coated water-cooled walls. A DC discharge and / or arc plasma reactor may be part of the plasma reactor and may include a DC plasma cathode. An electric arc or arc discharge is an electrical breakdown of gas that causes a long-lasting electrical discharge. Therefore, for the purposes of this disclosure, the terms plasma discharge or plasma arc may be used interchangeably. The DC plasma cathode and the supply gas system may be located at the top of the reactor. A DC plasma cylindrical anode (electrically insulated from the cathode) is part of the reactor and is located downstream of and coaxial with the nozzle. The anode is surrounded by a magnetic coil or other device that carries an electric current and provides a magnetic field. The magnetic field created by the current passing through the coil rotates the plasma, and the speed at which the plasma rotates depends on the DC current (e.g., typical values ​​are 1,500 to 5,000 amps for a 1 megawatt system operating at 700 to 200 volts, respectively, based on drive voltage and total wattage) and the magnetic field (typically 800 to 1,000 gauss (B)). Large anode area and high rotation speeds significantly increase plasma volume, process efficiency, and electrode life.

[0054] In some embodiments, RF power may also be applied, for example, between the cathode and the anode and / or between the anode and the feedstock injection plate. The frequency of the RF power may be adjusted to the ion cyclotron resonance frequency (e.g., the ion cyclotron frequency of atomic hydrogen is 1.4 MHz at B=900 Gauss). Adjusting the RF power to the ion cyclotron resonance frequency may accelerate the hydrogen ions and / or increase their kinetic energy, improving dissociation. Exemplary operating parameters are listed below.

[0055] In some embodiments, the target temperature for dissociating the hydrocarbon-containing gas is about 1,500° C., and may be about 1,000° C.-2,000° C. At or within this temperature range, a high percentage of the hydrocarbons may dissociate (e.g., greater than 98% of the hydrocarbons dissociate) with efficient energy usage, e.g., 5 kWh / kg H2-25 kWh / kg H2. Dissociation may still be successful at higher temperatures (e.g., greater than 2,000° C.), but the additional energy to reach those temperatures is effectively "wasted" in that dissociation is not substantially improved relative to the additional energy used.

[0056] In some embodiments, to reach the target temperature, the rotation speed of the plasma can be between about 5,000 revolutions per minute (RPM) and 6,000 RPM, and can be in a broader range of between about 1,000 RPM and 6,000 RPM. The rotation of the plasma creates a more uniform temperature profile (e.g., plasma cloud) of the hydrocarbon-containing gas, allowing the hydrocarbon-containing gas to be heated to the desired temperature and dissociated. This is because the rotation of the plasma discharge allows the DC plasma discharge to affect a larger volume of gas, not just the gas close to the standing discharge, but the entire or substantially the entire volume of gas in the plasma processing zone.

[0057] In an embodiment, one or more sensors (e.g., optical spectroscopy, laser interferometry, stack gas chromatograph, flow meter) may be used to monitor the process. For example, in the context of FIG. 1 (discussed below), one or more sensors may be used to measure the amount of hydrocarbon-containing gas exiting the reactor 102 through either the hydrogen outlet 114 and the carbon outlet 116, and / or the amount of hydrocarbon-containing gas passing through the plasma processing zone or in the quench zone and / or separation zone. Sensors may also be used to measure the amount of hydrocarbon-containing gas entering the reactor 102 through the input 110. From these measurements, the amount of hydrocarbon-containing gas dissociated may be determined. If this amount is too low (e.g., less than 98%), a control circuit coupled to the anode power supply may change the current flow to spin the plasma faster or control other process parameters. Examples of such process parameters include gas flow rate, gas temperature, RF power, or other parameters that maximize the decomposition efficiency.

[0058] FIG. 1 illustrates a hydrocarbon dissociation system 100 according to one embodiment. As illustrated, the hydrocarbon dissociation system 100 includes a reactor 102, a plasma source 104, an input 110, a magnet 112, a hydrogen outlet 114, and a carbon outlet 116. The reactor 102 may be, for example, a cylindrical vessel made of a dielectric material that contains the plasma and provides one or more regions or zones for dissociation of the hydrocarbons and purification of the resulting hydrogen and carbon products, and provides an outlet for collecting the resulting hydrogen and carbon products (such as a plasma treatment zone 310, a quench zone 312, a separation zone 314, etc.). In an embodiment, the reactor 102 may be elongated, with a diameter to length ratio of about 1:5 to 1:10, and may be positioned and operated in a vertical, horizontal, and / or angled configuration.

[0059] The plasma source 104 may comprise a direct current (DC) discharge plasma source, as shown in FIG. 1. The DC discharge plasma source 104 comprises a cathode 106 and an anode 108. The cathode 106 and the anode 108 may take on a variety of shapes, including cylindrical, conical, ring, and other geometric configurations. Exemplary materials for the cathode 106 and the anode 108 include graphite, lithium cobalt oxide (LCO), lithium nickel manganese cobalt oxide (NMC), lithium nickel cobalt oxide doped with alumina (NCA), lithium manganese oxide (LMO), and lithium iron phosphate (LFP). Other materials are also within the scope of the embodiments disclosed herein.

[0060] The DC discharge plasma source 104 also includes a power source, such as a DC power source. When DC power is applied to the cathode 106 and the anode 108 in the presence of a hydrocarbon-containing gas, a plasma discharge is created, which occurs between the cathode 106 and the anode 108. In some embodiments, the plasma source 104 may further include a radio frequency (RF) power source capable of creating an RF-based plasma between the cathode 106 and the anode 108. While the DC-based plasma is a single-point rotating discharge, the RF-based plasma expands to fill the volume of the reactor 102 within the plasma processing zone.

[0061] The reactor 102 may include an inlet 110 that may be used to provide a hydrocarbon feedstock gas to the reactor 102. The inlet 110 may have a nozzle that rotates the hydrocarbon gas as it is fed into the reactor 102, such as the gas outlet 806 (shown in FIG. 8C). As shown, the inlet 110 (or gas inlet) is positioned in the cathode 106 at the top of the reactor 102. The nozzle may be angled or shaped in a manner to facilitate rotation of the hydrocarbon gas as it is fed through the inlet 110 and downstream of the nozzle further into the reactor 102. An embodiment of the inlet 110 is further described with respect to FIGS. 8A, 8B, and 8C. The magnet 112 may be a permanent magnet or may be a coil(s) wrapped around the reactor 102 that may induce a magnetic field when a current is applied to the coil and may be thermally cooled. The magnet 112 is provided to help control or otherwise regulate the speed of the rotational direction of the plasma.

[0062] A hydrogen outlet 114 is provided to allow gaseous hydrogen to be collected. For example, the hydrogen outlet 114 may include valves and piping to allow hydrogen to be exhausted from the hydrocarbon dissociation system 100. The exhausted hydrogen may contain some amount of hydrocarbon gases and / or other impurities and may undergo further purification processing. In some embodiments, the remaining hydrocarbon gases may be recycled to the reactor 102, for example, by pumping it to the gas injection system 302 (shown in FIG. 3).

[0063] A carbon outlet 116 is provided to allow solid carbon to be collected. For example, the carbon outlet 116 may comprise a rotating airlock and an auger or conveyor that allows carbon to be discharged from the hydrocarbon dissociation system 100 in a manner that excludes air ingress. The auger or conveyor may be cooled (e.g., by a fluid such as water).

[0064] In some embodiments, a set of injectors (e.g., ceramic injectors such as nozzles or tubes 304 first shown in FIG. 3) may be provided in the quench zone 312 (e.g., via gas injection system 302) to inject gas into the region and allow the carbon temperature to be reduced from about 2,000 K to about 1,000 K or about 500 K. Hydrogen, which has the highest thermal conductivity of all gases and is one of the gases produced by the embodiments disclosed herein, allows for quenching of the carbon without the use of water, which is an advantage over prior systems. This is described in more detail in connection with FIGS. 3-4, 5A and 5B.

[0065] For example, in embodiments where carbon dioxide release is permitted, the reactor 102 may be cooled, for example, by a water cooling system 105 coupled to the reactor 102 .

[0066] As shown, the reactor 102 is oriented vertically and may be referred to as a vertical reactor. In embodiments, positioning the reactor 102 in this orientation may improve the efficiency of hydrogen and carbon separation and purification, for example, by allowing gravity to assist in separating the (heavier) solid carbon from the (lighter) gaseous hydrogen. Other orientations of the reactor 102 are also possible (e.g., sideways (e.g., horizontal) or at an angle).

[0067] In operation, DC power is supplied to the cathode 106 and the anode 108 to create a plasma. A hydrocarbon-containing gas is introduced into the gas inlet 110 and enters the process zone in the reactor 102 at an angle through an opening (such as the gas outlet 806 shown in FIG. 8C). In some embodiments, RF power may also be supplied to the cathode 106 and the anode 108 to generate a plasma simultaneously with the generation of the DC-based plasma, for example.

[0068] Ideally, the hydrocarbon-containing gas is a pure or substantially pure hydrocarbon. In reality, there will be impurities that need to be filtered out. Furthermore, there may be a single hydrocarbon-containing gas or a mixture of different hydrocarbon-containing gases (e.g., methane and natural gas).

[0069] In an embodiment, the cathode 106 has a port (such as port 902 shown in FIGS. 9A, 9B, and 9C) on its side that imparts a physical spin rotation of the hydrocarbon-containing gas as it exits the nozzle of the gas inlet 110 and enters the plasma processing zone. As described below in connection with FIGS. 9A, 9B, and 9C, the port 902 may be angled (as shown in FIG. 9A) by an angle α, for example, in some embodiments, α may range from 10° to 30°. In some embodiments, this rotation of the gas imparted by the port in the cathode 106 is in addition to the rotation imparted by the gas inlet 110. In the plasma processing zone, a small amount of the hydrocarbon-containing gas (e.g., about 2% to 3%) is transformed into a plasma (e.g., a high-energy plasma) and the remaining gas is heated as it passes through the plasma processing zone. In this zone, the spin of the gas imparts angular momentum that drives all the gas into a DC plasma discharge, increasing mixing and improving efficiency. When the magnets 112 induce the spin of a DC plasma discharge, the discharge can heat a larger volume of gas within the plasma processing zone. In an embodiment, the magnets 112 may rotate the plasma at speeds between 1,000 RPM and 6,000 RPM.

[0070] The gas flow of the hydrocarbon-containing gas pushes it into the plasma treatment zone. The high energy plasma discharge and rotation of the plasma causes the hydrocarbon-containing gas passing through this zone to collide with high energy, dissociating with great efficiency and breaking the carbon-hydrogen bonds in the hydrocarbons into single hydrogen and carbon atoms, i.e., the elemental components of the hydrocarbons. In this zone, the hydrocarbon-containing gas is heated to a temperature in the range of 1,000°C to 2,000°C, in embodiments about 1,500°C, and most or substantially most of the hydrocarbons are converted to their elemental components.

[0071] For example, in some embodiments, more than 90% of the hydrocarbon-containing gas is dissociated, in other embodiments, more than 95% dissociation is achieved, in other embodiments, more than 98%, and in other embodiments, substantially 100% (e.g., 99.99%) is achieved. Process control parameters, such as, but not limited to, gas flow rate, can adjust this resulting dissociation efficiency. There is a nominal flow rate that achieves 99.99% dissociation and is monitored by spectral analysis of the output gas for organic source gas (e.g., methane) below a threshold amount (e.g., below the detection limit of the equipment). If the flow rate of the process gas is increased beyond this point (i.e., the nominal flow rate), the energy from the plasma is not sufficient to reach the dissociation temperature of about 1500° C., and some undissociated hydrocarbons (e.g., methane) pass through unchanged and are detected by the aforementioned sensor. An increase of the nominal flow rate from 0% to 3% results in a conversion result of 98%. An increase from 3% to 5% results in a result of 95%, and so on (based on process simulations and the inventor's experience).

[0072] These single elements exit the plasma treatment zone and enter the quench zone (312) based on, for example, a pressure difference caused by the gas being heated in the plasma treatment zone. After the quench zone, the single elements move to a separation zone (314), where hydrogen recombines as it cools back to its natural state of H2 and leaves the zone as a gas. In the separation zone 314, the dissociated carbon tends to move towards the wall of the reactor 102 (in the separation zone 314) based on centrifugal force effects, since the gas was rotating when it entered the reactor 102, and the gas and subsequent constituent molecules tend to continue to rotate downstream. The quench process to control the carbon product is further described with respect to the gas injection system 302 and the length of the quench zone 312 as the critical "contact time" or quench rate. The carbon recombines and naturalizes as solid particles, aggregates or agglomerates that are heavier than hydrogen. These particles fall under the force of gravity to the bottom of the separation zone and can be removed, for example, by an auger, conveyor, or other mechanical device to a carbon outlet.

[0073] As the carbon falls into the reactor 102, some of the carbon particles (or aggregates or agglomerates) will coat the inside of the walls of the reactor 102. At this point, the solid carbon is very dry, the thickness of carbon on the walls of the reactor 102 will thin, and the remaining carbon will fall to the bottom of the separation zone. In embodiments, the walls of the reactor 102 may be coated in a manner that prevents carbon buildup. Also, in embodiments, the geometry of the walls of the reactor 102 and / or the surface material of the walls and / or the coating applied to the walls may affect the amount of carbon buildup. In other embodiments, the limited carbon buildup that occurs may help improve the insulation of the reactor 102.

[0074] FIG. 2 illustrates a hydrocarbon dissociation system 200 according to an embodiment. Some of the components of the system 200 are similar to those described with respect to the system 100, and the same reference numbers are used to indicate the similar components. The system 200 differs from the system 100 in that a hybrid plasma reactor is provided by means of a DC discharge plasma source 104 and a separate RF plasma source 202. The system 100 in some embodiments may include an RF-based plasma between the cathode 106 and the anode 108. In the system 200, the RF-based plasma is generated by a coil 203 around the reactor 102, which is a separate plasma source from that used in the system 100. In some embodiments, the RF-based plasma is advantageous. For example, the RF-based plasma can be stabilized more easily than a DC-based plasma, can provide a more uniform temperature throughout the reactor 102, and can provide additional energy to increase molecular collisions from the angular momentum already provided by the gas injection spin, as described above, to create more plasma volume in the reactor 102. In some cases, it may be difficult to efficiently treat hydrocarbons using only an RF-based plasma, so in embodiments, an RF-based plasma is combined with a DC-based plasma to improve system efficiency.

[0075] The RF plasma source 202 uses RF energy to create a plasma, e.g., an inductively coupled plasma (ICP). The RF plasma source 202 may include a coil 203 that provides the electromagnetic induction necessary to generate an RF-based plasma (e.g., ICP). The RF plasma source 202 introduces the RF-based plasma to a plasma processing zone within the reactor 102. In the plasma processing zone, a physically rotating hydrocarbon-containing gas is energized by RF power and may be controlled to have certain parameters (e.g., frequency, amplitude, bias) such that the generated plasma has a large amount of energy, causing the hydrocarbon-containing gas to heat up and expand, filling the entire plasma processing zone.

[0076] In an embodiment, the typical frequency of the RF power source is between 1.76 MHz and 13.56 MHz, and the amplitude is about 5 kV to about 10 kV. By expanding the hydrocarbon-containing gas to fill the entire plasma processing zone, the processing volume is maximized and the resulting dissociation is more efficient. In an embodiment using both DC-based plasma and RF-based plasma, doubly energizing the hydrocarbon-containing gas (i.e., by both DC-based plasma and RF-based plasma) potentially results in higher conversion efficiency at lower DC power. As described above, once dissociation of the hydrocarbon-containing gas occurs, the constituent molecules are sent to a separation zone. The filter 204 may be coupled to the hydrogen outlet 114 and the carbon outlet 116. For example, as hydrogen passes through the hydrogen outlet 114, hydrogen may interact with the filter 204 such that carbon particles passing through can be captured by the filter 204 and possibly allowed to enter the carbon outlet 116. Additionally, as the carbon passes through the carbon outlet 116, the openings in the carbon outlet 116 may allow any gas in the carbon outlet 116 to interact with the filter 204 such that any gas passing through the carbon outlet 116 may enter the hydrogen outlet 114. Because the gas is still hot as it passes through the carbon outlet 114, the gas will tend to rise and pass through the openings, allowing the gas to further pass through the filter 204 and into the hydrogen outlet 114. The filter 204 may comprise a ceramic high temperature filter.

[0077] 3 and 4 further illustrate a hydrocarbon dissociation system. The reactor 102 is similar to the reactor 102 shown in FIGS. 1 and 2, and generally the same reference numbers are used to indicate the same or similar components. The reactor 102 includes a gas injection system 302. The gas injection system 302 may include a number of nozzles or tubes 304 for allowing gas to enter the reactor 102 at the quench zone 312. The nozzles or tubes 304 may be radially spaced apart. In an embodiment, hydrogen that passes through the hydrogen outlet 114 is reintroduced into the reactor 102 through the tubes 304 for cooling, which causes quenching and helps process the carbon product into carbon black. Generally, the process performed by the reactor 102 can be divided into zones 310, 312, and 314. Plasma treatment occurs in zone 310, coalescence and quenching occurs in zone 312, and separation occurs in zone 314, where the products may be further processed, filtered, and / or removed from the reactor 102.

[0078] An advantage of the systems disclosed herein is that they are much more efficient since generally less energy is required to crack the hydrocarbons and almost all of the energy put into the plasma is spent on the dissociation process. In some embodiments, the systems can achieve efficiencies of about 24 kWh / Kg, and in some embodiments, efficiencies can be about 15 kWh / Kg to about 30 kWh / Kg. Prior art systems have significantly lower efficiencies.

[0079] The following generally applies to any of the hydrocarbon dissociation systems disclosed herein, including the hydrocarbon dissociation systems 100 and 200. The cathode 106 may be optionally movable. With use, the material of the cathode 106 degrades and is etched away, thereby becoming smaller over time. By controlling the position of the cathode 106, for example, a constant distance between the cathode 106 and the anode 108 is maintained. This improves the operation of the system over time and can increase the continuous operation time before the cathode 106 must be replaced. The dynamic cathode positioner is further described with respect to Figures 7A and 7B. The positioning is controlled by an electrically driven correction, and the magnitude of the change in position is continuously determined by feedback from the cathode to the anode and monitoring of the operating current.

[0080] Exemplary hydrocarbon-containing gases for use in the embodiments disclosed herein include methane, natural gas, compressed natural gas (CNG), petroleum gas, synthetic gas, biodiesel, and other types of hydrocarbons, including any combination thereof.

[0081] In an embodiment, hydrogen and carbon from the hydrocarbon-containing gas are separated by the centrifugal effect of the rotating plasma. In particular, the rotation of the plasma creates a more uniformly heated space in the reactor 102, and a larger volume of the hydrocarbon-containing gas is dissociated than would otherwise be the case due to the angular momentum collision rate. The different (e.g., opposite) rotations of the hydrocarbon-containing gas on the one hand and the plasma on the other hand enhance the angular contact between the plasma and at least a portion of the hydrocarbon-containing gas, resulting in a greater dissociation effect and efficiency. Each of the hydrocarbon-containing gas and the plasma may rotate in one or more of three dimensions (e.g., x, y, z dimensions), and the respective rotations may differ in one or more of these dimensions. The different rotations of the hydrocarbon-containing gas and the plasma, as well as their respective angular momentum, improve the heating of the hydrocarbon-containing gas by making it more uniform. The centrifugal effect causes the heavy carbon particles to move towards the cooled wall, where part of the quenching process occurs. The hydrogen is transported to a heat exchanger (not shown) and a cyclone dust separator (not shown) for cooling and heat recovery. The carbon powder collects on the walls and bottom of the water-cooled reactor, creating a plug of material at the exhaust port that isolates the air from the reactor chamber, and is transported by a water-cooled conveyor / auger to a packaging system. A hydrogen purification unit (e.g., hydrogen purification system 107) based on highly selective membranes or pressure swing absorbents for extracting high purity hydrogen from the gas stream generated in the plasma reactor may be located in close proximity such that the gas exhausted from hydrogen exhaust 114 passes through the hydrogen purification unit.

[0082] Carbon black has various properties that make it useful depending on the application of the carbon black in various industries. For example, physical properties such as particle size, and / or surface activity (tested by nitrogen uptake), and / or iodine adsorption among others can affect the value of carbon black in industries such as tire manufacturing, rubber for belts and hoses, plastics, food service, carbon fiber, and other black materials. These properties can be controlled during processing in a hydrocarbon dissociation system by manipulating process parameters such as power, gas velocity, gas mixing, flight / cooling time, etc. Adjustment of particle size and other properties is important to provide the desired grade of product for, for example, tire manufacturing, plastic compounding, additives to paints and inks, and many other industries. The process of generating hydrogen achieves this without additional energy costs, creating beneficial economies of scale in providing a second product to an already growing market worldwide.

[0083] In an embodiment, a method is proposed to change the cooling time (i.e., quenching rate). The method includes providing an adjustable cooling gas curtain by using generated hydrogen gas, such as using the gas injection system 302 shown in FIG. 3. As soon as the dissociated constituent molecules pass through the anode of the plasma reactor, where decomposition occurs, they begin to cool. The constituent molecules, including elemental carbon, form a hot jet stream and are agglomerated by the collision dynamics of the turbulent flow into small clusters that resemble grapes on a stem. The cooling may also be controlled by adjusting the distance between the anode and the quenching gas ring, known as the flight time. That is, a long distance (or long flight time) results in more cooling, and a short distance (or short flight time) results in less cooling.

[0084] Figure 6 shows SEM micrographs of clusters of carbon particles at different temperatures. The hot jet stream carries these very fine carbon particles, and the longer the carbon particles remain in the hot state (e.g., above 1,000°C, usually in the range of 1,000°C to 2,000°C), the larger and more complex they become, as shown in Figure 6. This is because the finest particles occur at 2,000°F (or about 1,100°C) and are cooled by convection and collision until they are cool enough to stop the process. Artificially stopping this process is called quenching, and is done by cleaning and cooling the evolved hydrogen gas and injecting it into the appropriate part of the tail of the hot jet stream. Injecting the evolved hydrogen gas dramatically reduces the temperature of the hot jet stream, so that the properties of the carbon, for example, the size of the clusters that the carbon particles form, can be controlled. For example, the time range required for quenching is known to be from about 30 milliseconds to about 90 milliseconds. Depending on the desired characteristics, the quench location may be calculated based on, for example, the gas velocity exiting the anode location, placing the gas injection about 40 milliseconds to about 60 milliseconds downstream from the anode 108.

[0085] In embodiments, a gas temperature quench after dissociation may be used to stop the reassociation of carbon into particles, aggregates or agglomerates. The size of the resulting carbon product may be determined by the process parameters of the dissociation plasma and the location in the reactor 102 where the quench occurs. The specific median and range of carbon particle size may be experimentally predetermined and may be adjustable, for example, in the quench zone by moving the location of the quench. In embodiments, the quench may be accomplished by pre-cooled inert gas, or preferably pre-cooled hydrogen product gas, rather than by water that turns to steam as is conventional. This is accomplished in some embodiments by a predetermined nozzle arrangement, such as the gas injection system 302. The nozzle or tube 304 may be made of high temperature ceramic and may be oriented in the center of the flow, or may be arranged as a ring around the internal dimension of the bonding chamber immediately after the plasma jet connection and oriented in the center of the flow, but may also be adjustable for axial positioning up to 50% of the length of the separation zone downstream from the plasma processing zone. The arrangement may be made of materials such as, but not limited to, stainless steel with ceramic nozzles and may be fluid-cooled to withstand the operating temperatures of the post-plasma chamber environment. 5A and 5B, with the specific injection through the inlet 110 creating an angular (spin) gas velocity and increasing turbulent contact with the energetic plasma, a hot jet of particles travels downstream from the anode location and the gas continues to spin. The spin gas passes through a cooling injection nozzle 304 for hydrogen injection, and in some embodiments, the gas continues to spin. 6 A quench rate of K / sec may be achieved to reduce the temperature significantly below 1,000°C, whereby aggregate formation is stopped and the carbon black formation may be adjusted to small size, high value grades (such as N300 and below). N300 refers to a grade of carbon black having a particle size of 30 mm to 35 mm. The quench rate of this process, K / sec, is related to the rate of change of temperature in Kelvin per second and is determined by molecular collision dynamics.

[0086] The processes disclosed herein may be run continuously with little or no interruption. This minimizes the impact of downtime due to maintenance. Allowing the process to stabilize and operate at preferred nominal process parameters leads to more consistent product quality. One of the few maintenance interruptions in the disclosed processes is the replacement of the high temperature cathode 106 in the reactor 102. The cathode 106 may be made, for example, of graphite or a graphite composite, and may be made with desirable dimensions, particularly for extended service life, but due to the etching effect of high currents on the cathode 106, it will corrode over time and must be replaced. In some embodiments, the cathode is positioned relative to the anode to adjust the size and potential of the plasma energy, and in embodiments, this dimensional feature is within about + / - 10% of a predetermined value. This corrosion occurs over time, so this dimension will change with continued use. In some embodiments, to extend operational life, a cathode section may be used that is significantly longer than would otherwise be used, for example, 2-10 times the nominal design length. Additionally, in some embodiments, there may be a mechanism to slowly insert excess cathode 106 length at a predetermined corrosion rate (e.g., on the order of millimeters per day) so that the required cathode to anode position is held relatively constant, e.g., within + / - 10%. This mechanism is an active process control device, also known as a dynamic cathode positioner. Additionally, in some embodiments, a cathode rod can be attached (e.g., screwed) onto an existing rod to extend its life without shutting down the system.

[0087] 7A and 7B show a dynamic cathode positioner 700 according to one embodiment. The cathode 703 may be rod-shaped and fixed in a holder 702 that is sufficiently rigid to support the cathode (e.g., made of graphite) without breaking, but is also designed to interface with an injection screw 701 device that injects the cathode into the reactor 102 and the plasma treatment zone 310. A speed-adjustable insertion device 705 coupled to the holder 702 can guide the cathode, for example by a motor, establish an insertion speed (e.g., on the order of a few millimeters per day), and seal the cathode so that no air leaks into the plasma treatment zone 310. A power supply 704 is also provided, which may include timing and control circuits with an operating software interface screen. The insertion device 705 may comprise a long support channel with a screw 701 equipped with bearings. The screw has fine threads running its length, and a fine positioning stepper motor 706 at the base end for rotating the screw, thereby creating linear motion up and down for the holder 702. A lubricated mount with a clamping device coupled to the holder 702 for holding the cathode 703 at one end is on this threaded screw, and is mounted within the channel in such a manner that it is free to move from one end of the channel to the other. A fitting that bolts this device to the top of the reactor 102, i.e. to the rod guide, screws into the base at the other end, sealing off the reactor 102 and the screw motor 706 from air.

[0088] The software for the dynamic cathode positioner may manipulate the cathode insertion through the air seal and into the plasma processing zone 310 to the anode narrowed diameter of the reactor 102. For example, the software may be based on process modeling and / or experimental proof and in some embodiments may be run at a predetermined speed or adjusted to account for the operating conditions. For example, a particular power supply operating parameter range, such as voltage consistency, may be used as a backup to the pre-determined insertion speed. The plasma main power may be held at a constant current or the voltage may be varied to hold the high temperature dissociation process constant. If the voltage operating range begins to change excessively, this may be a signal that the cathode is out of the nominal position. A software algorithm may be used to change the insertion speed to adjust for this process change.

[0089] 8A, 8B, and 8C show a top view, a cutaway perspective view, and a side view, respectively, of a gas input head 800 according to one embodiment. The gas input head 800 may be used, for example, as the gas input 110 shown in FIGS. 1 and 2, and may be located at the top or substantially at the top of the reactor 102. As shown, the gas input head 800 has chambers 810 and 820, and may have cooling water flowing in the upper level chamber 810 and gas dispersion in the lower level chamber 820. The lower level chamber 820 has directional vanes 804 that help control the flow of gas in the otherwise hollow chamber. The vanes 804 may be, for example, but not limited to, machined into the hollow cavity of the chamber 820. In an embodiment, the vanes 804 occupy less than 50% of the available volume, and in some embodiments, less than 25%.

[0090] The vanes are shaped and positioned in such a manner that they spin the gas in the lower level chamber 810 as it travels to the outlet 806, which is the gap between the chamber 820 and the plate 821 through which the gas can escape. The end of the vaned chamber 820 has a diameter smaller than that of the reactor 102, so that the gas being pushed out of the chamber 820 easily travels to the plasma processing zone of the reactor 102 as it passes through the outlet 806. The gas is injected into the top input hole 802 (off-center) of the gas injection head 800. The gas fills the central region where the angled vanes 804 are located. As a result, it is squeezed between the vanes, giving it a tangential direction. This direction creates a spin in the gas as it exits the gas injection head 800 and enters the plasma processing zone of the reactor 102.

[0091] 9A, 9B, and 9C show a top view, a partial side view, and a side view, respectively, of a cathode 900 according to one embodiment. The cathode 900 may be configured to replace the cathode 106 shown in FIGS. 1 and 2, for example. The ports 902 may be located on the sides of the cathode 900 to provide a physical spin rotation of the hydrocarbon-containing gas as it exits the nozzle of the gas inlet 110 and enters the plasma processing zone. In some embodiments, the ports 902 are angled such that the angle offset α shown in FIG. 9A may range from 10° to 30°. This angle represents the angle from the longitudinal axis of the ports 902 with respect to a line from the outer edge of the cathode 900 to the center of the cathode. Different ports 902 may have the same angle in some embodiments, and may have different angles in the range of 10° to 30° in other embodiments. The angular offset α causes the ports 902 to impart a physical spin rotation to the hydrocarbon containing gas as it exits the nozzle of the gas inlet 110 and enters the plasma processing zone.

[0092] FIG. 9D shows a cathode insertion device 900D according to one embodiment. The cathode 901D to be inserted has a threading feature (or other end-to-end matable connection method) machined on each end, as shown, shown as 902D, which allows the cathode to be extended by threading the male feature of the new cathode length into the female feature of the cathode currently in use, thus allowing continuous operation. This cathode 901D is within a motorized metering device 905D that can move the cathode 901D. The motor of this device can be a digital servo motor as known in the industry, with precise movement controlled by a digital control board and computer electronics. As shown in one embodiment, the cathode 901D is sandwiched between gears 906D that are part of the motorized metering device 905D, specifically, sandwiched between the gears 906D with enough resistance to push the cathode 901D into the reactor 102 (not shown in FIG. 9D). The gear is a mechanism that transmits the rotation of a motor controlled, for example, by a digital servo type motor as part of, but not limited to, 905D, which has a gear to the motor on one side and a friction device that grips the cathode on the other. This gripping method may be done by a material such as rubber, or a groove in a metal wheel with sufficient depth and material strength to move the cathode but not damage it. The cathode insertion device 900D may be used to insert a cathode of appropriate size (such as the cathode 106 shown in FIG. 1) for use in the disclosed embodiments. In an embodiment, the cathode insertion device 900D may include a specially designed water-cooled seal 907D with a seal 908D of a specific material that allows the cathode to move into the reactor 102 but does not allow air to enter the reactor 102. In one embodiment, the seal may be a double seal consisting of two parts that surround the entire diameter of the cathode and is a heat resistant material such as, but not limited to, rubber, synthetic nylon, Teflon, etc.Here, the material is at each end of the integrated tube in such a manner as to create an airlock along a length of the cathode (e.g., 1-6 inch length) to prevent air from entering the reactor. Also, the seal 907D and drive 905D are electrically isolated from the charge placed on the cathode 901D via the connections in 907D. Additionally, the plasma generation methods described herein may corrode the cathode 901D over time, so it is necessary to be able to replace the cathode 901D in the reactor 102. As shown, an additional cathode 903D having a screw thread 904D that matches the screw thread 904D of 902D can be attached to the threaded end 902D of the cathode 901D. That is, the screw thread ends 904D and 902D fit together. This allows for continuous and uniform system operation.

[0093] The reactor system may comprise a single reactor or multiple parallel reactors of the same or different types, in other words, the hydrocarbon dissociation system disclosed herein is modular.

[0094] Some embodiments (such as those described herein with respect to Figures 10-16) are directed to reactors designed to dissociate hydrocarbon liquids, semi-liquids, oils, etc. These embodiments are generally described below.

[0095] The embodiments also describe a method and control system for maintaining an appropriate and adjustable liquid level of a feed liquid contained within a vessel, the temperature of which is controlled and maintained. Removal of carbon-rich fluid from this vessel during continuous operation requires returning the filtered fluid to the vessel to continue processing, monitoring the opacity of the fluid to control filtration quality, and replenishing the appropriate fluid level with new feed, in order to deplete the original volume of fluid and convert a consistent volume.

[0096] The embodiments herein describe a method and apparatus for generating hydrogen and carbon (e.g., carbon black) by dissociating methane and other gaseous hydrocarbons using a plasma generation system. The plasma generation system utilizes, among other things, a DC plasma discharge reactor and / or a DC plasma discharge chamber with an RF ICP plasma reaction to create gaseous hydrogen and solid carbon for all (or a portion) of the gaseous hydrocarbon gas by transferring heat from the plasma stream exiting the plasma torch / zone to the remaining gaseous hydrocarbon gas and imparting its high energy to a liquid contained in a vessel. The two products immediately separate as the carbon remains in the liquid. And because the gas is hot, it rises to a gas vent. In an embodiment, the hydrocarbon gas is introduced at an angle into the reactor or torch chamber so that it rotates in the chamber and is in rolling contact with the plasma created in the chamber. In some embodiments, the DC plasma is also regulated by the plasma controlled magnets, voltage and sequence control software, and integrated portions of the anode portion of the cathode / anode pair that make up the plasma reactor, rotating in a different (e.g., opposite) direction at a high rotational speed within the chamber compared to the rotation of the hydrocarbon gas.

[0097] In some embodiments, the plasma and the hydrocarbon gas are rotated in opposite directions. The relative angular rotation of the gas and plasma results in increased generation of plasma that contacts the gas and dissociates the hydrocarbons into elemental components of hydrogen and carbon, providing a process for separating and purifying the resulting products, such as quenching into the liquid of the vessel to produce carbon black. Since the dissociated gas has angular momentum imparted by the spin imparted by the injection cap of the plasma zone and the magnetically controlled counter DC discharge rotation, the carbon-containing gas spins outwards by centripetal force into the liquid and is cooled by cold water in the vessel wall. This stops / quenches the carbon-carbon bonding process at nano- and micro-sized scales, thus establishing the carbon black aggregate structure (the result of elemental carbon bonding with elemental carbon). This then forms the carbon black properties, which are collected in the fluid, filtered out of the fluid, and the fluid reduced to dry quality, which can then be sorted by various processing methods and equipment.

[0098] Various plasma techniques, including, for example, DC plasma or a combination of DC plasma and RF plasma, may also be used with controllable process parameters, such as, but not limited to, plasma gas flow rate and velocity (given by the controllable pressure of the raw gas), raw gas flow rate in the post-plasma zone, cathode and anode voltages, rotation speed of the DC discharge plasma, etc. The controllable process parameters may be used, for example, to expand the plasma heating volume through which the raw gas flows and is decomposed.

[0099] In some embodiments, the liquid conversion process may include filtering the liquid, drying the filtered carbon black, a plasma torch or reactor and heat generation method, attachment of the heat generation method to the liquid container, methods and equipment for venting, cooling, collecting, filtering, and desteaming / fluidizing the hydrogen product gas, purification of the product hydrogen, a plasma energy control system and fluid exchange controls, filtering, de-oiling, and processing the filtered, de-oiled, semi-dried carbon solids, all in a pyrolysis kiln.

[0100] In some embodiments, pre-treatment of the feed fluid may be applied prior to entry into the vessel, post-generation treatment of the gaseous hydrogen product, and post-generation treatment of generated solids (e.g., carbon black) may be applied. Pre-treatment of the feed fluid may include blending of the bulk delivery to create a more uniform fluid composition that is placed into the vessel, chemical analysis to allow adjustment of processing parameters in an effort to maximize the quality and characteristics of the products driven by the business, removal and / or filtration of solids, degassing, and dehydration.

[0101] An embodiment includes a method for post-treatment of a gaseous hydrogen product, which exits a treatment vessel through a sealed vent at the top, passes to a treatment vapor mist condenser, passes to a hydrogen compressor at a pressure of up to, but not limited to, 30 bar, and then passes through a membrane hydrogen purification unit to obtain hydrogen purity of about 99.9%. The bypass gas from this purification step is generally high in hydrocarbon content and is circulated back to the plasma generator.

[0102] In some embodiments, hot plasma gas steam is emitted from the chamber at high temperature (2,000°C-6,000°C) and the plasma is created vertically in a vessel containing a second hydrocarbon feedstock. This hot plasma gas steam intimately contacts the liquid feedstock, imparting thermal energy and decomposing the feedstock into hydrogen and carbon. Consistent carbon black composition and surface quality may be obtained in a controlled manner, for example in less than a second, by quenching the carbon aggregate formation. The method includes the evolution of hydrogen from this interaction as the newly created molecular hydrogen (H2) bubbles up, which is a gas and therefore separates from the liquid. The method includes the separation of carbon (solid) from hydrogen (gas) as the carbon remains in the liquid and collects, providing a solid portion and a gas portion in the liquid. The gas portion rises above the liquid and is collected in a vent pipeline where it is cooled and cooled for further filtering and purification of droplets, fumes, particles, etc. The carbon-containing liquid is filtered to remove the carbon and may be further processed to dry solids, with excess liquid being returned to the vessel for processing.

[0103] In some embodiments, the method includes quenching the carbon (solids), the carbon (solids) comprising carbon black, and the formation of carbon black is stopped by the temperature of the liquid surrounding the area impinged by the DC discharge. In some embodiments, the hydrocarbon gas used to generate the plasma stream is contained in a gas that is substantially free of oxygen, nitrogen, and sulfur. In some embodiments, the amount of oxygen, nitrogen, and sulfur in the gas is less than 1 mole percent. In some embodiments, the liquid feed is prepared to reduce the presence of water. In some embodiments, separating the carbon (solids) from the liquid feed hydrocarbon includes removing a portion of the liquid by fluid pumping to a solid-liquid separation device, which may include, but is not limited to, a filter press, a centrifuge device, a caking device, an auger press, or other device designed to remove all or a portion of the carbon. In one embodiment, the carbon "cake" is removed via a fluid-cooled auger in a manner that limits the reintroduction of air into the carbon cake (solids).

[0104] In some embodiments, the carbon cake is further processed in an oxygen-free pyrolysis rotary machine where the remaining wet / liquid oil along with the carbon is volatilized into high calorific value syngas. In this embodiment, this syngas may be combusted as a heat source for the rotary machine. In another embodiment, this syngas is returned to the plasma generation chamber where it is utilized to generate heated plasma water vapor. In this embodiment, the now dried and deoiled carbon is collected, cooled, and sorted into a saleable carbon black product.

[0105] In some embodiments, the liquid hydrocarbon feedstock is heated to a temperature between 1,400° C. and 2,000° C. by the gaseous hydrocarbon plasma stream.

[0106] FIG. 10 illustrates a hydrocarbon dissociation system 1000 according to one embodiment. As shown in FIG. 10, the system 1000 has a liquid reactor 1002 including a vessel 1004, and in some embodiments, the entire vessel 1004 encompasses all or most of the components of the reactor 1002. The liquid hydrocarbon feedstock 1006 to be treated is held at a constant level within the vessel 1004, for example at or near the top (apex) of the anode rotating element 1008. In one embodiment, the cathode 1010 is positioned above the anode 1008 at an appropriate distance to facilitate the generation of a DC discharge plasma 1012 from the cathode 1010 to the anode 1008. In an embodiment, the rotating anode 1008 may be in the form of a drum, which may pull the interior of the liquid 1006 up above its surface and into the path of the discharge plasma 1012. The interior of the liquid 1006 on the surface of the rotating anode 1008 may form a fluid layer 1014, which will depend on the viscosity and surface tension properties of the liquid as it relates to the surface of the rotating anode 1008. In an embodiment, the thickness of the fluid layer 1014 may be from about 0.1 mm to about 6 mm.

[0107] Decomposition of the fluid 1006 occurs during this process, and hydrogen gas is discharged into the space 1016 above the fluid 1006, rises from the liquid region, and exits the vessel 1004 as syngas, for example, through a syngas output 1018. The carbon-laden fluid is removed from the bottom of the vessel, which may have a funnel bottom to facilitate collection of the carbon (such as those shown in Figures 14 and 15). The removed fluid is then filtered, decanted, centrifuged, and / or subjected to other methods to remove carbon solids from the liquid, such as by a carbon / liquid separator 1020. Excess hydrocarbon fluid is returned to the vessel 1004, for example, through a pump 1026, which pumps the liquid from the carbon / liquid separator 1020 to a liquid return inlet 1022. The liquid returned through the return inlet 1022 includes the recycled and filtered liquid hydrocarbons from the carbon / liquid separator (filtration) device 1020.

[0108] The cathode 1010 is one side of a high voltage / high current supply that creates the discharge plasma discharge 1012, where the decomposition occurs. The syngas output 1018 facilitates the exhaust of the gases produced in the reactor 1002, including the hydrogen gas in the space 1016. The anode 1008 is on the other side of the high voltage / high current supply for the discharge plasma 1012 and can be configured as a rotating drum. This drum can be immersed in the liquid hydrocarbon 1006, and as previously described, surface friction and viscosity pull the liquid up into a layer 1014 on the drum. During the processing and operation of the reactor 1002, carbon solids 1028 are formed and captured by the liquid 1006. A pump 1026 removes the liquid from the reactor 1002, for example, at a constant rate (predetermined experimentally by the decomposition rate), during which the liquid passes through a separator or filter 1020. The separated carbon can be discharged from the separator / filter in a concentrated form and sent for further processing. A pump 1026 may then return the filtered liquid to the reactor 1002 via liquid return 1022 for reprocessing. Fresh fluid also enters the vessel 1004 through a fresh fluid inlet 1024 that is configured to maintain a reasonably constant level of fluid in the vessel 1004.

[0109] As used, referenced, described, or otherwise disclosed in this application, liquid hydrocarbons may include, but are not limited to, oil, waste oil, glycerin, vegetable oil, refinery by-products, asphalt, and other hydrocarbons.

[0110] Figure 11 illustrates a hydrocarbon dissociation system 1100 according to one embodiment. As shown in Figure 11, the system 1100 has a liquid reactor 1102 that includes a vessel 1103, and in some embodiments, the entire vessel 1103 encompasses all or most of the components of the reactor 1102. Input liquid to be treated may enter the vessel 1103 at a liquid return 1104. This liquid return 1104 may contain filtered liquid hydrocarbons that are recycled from a carbon / liquid separator (filtration) device 1106.

[0111] The reactor 1102 may be configured to generate a high enthalpy plasma jet flow 1108 through the use of an input gas such as a natural gas feedstock 1110. The gas used to form this plasma jet 1108 may also include a portion of the syngas generated by the reactor apparatus (e.g., returned through gas return 1116 via syngas output 1114). The gas used to form this plasma jet 1108 may be, for example, all syngas or a mixture of fresh input feedstock gases, but is not limited to methane and syngas. Ranges for each gas component may include, for example, from 50% methane, 25% hydrogen, and 25% carbon dioxide to 98% methane, 1% hydrogen, and 1% carbon dioxide. The resulting cracking of such a gas mixture results in all of the carbon dioxide and hydrogen passing through the cracker as an input fraction, with 99+% of the methane (or any other hydrocarbon) cracked into hydrogen and solid carbon. In an embodiment, a portion of the syngas may be output via syngas outlet 1114 and a portion of the syngas may be returned to the reactor via syngas return inlet 1116 .

[0112] Gas is injected around and through the cathode 1118 (in the diagram shown in FIG. 11 , shaped like a downward facing triangle) which is configured so that the gas exits the cathode in a spiral fashion. The spinning or rotating gas 1120 encounters a counter-spinning or rotating DC discharge 1122 to maximize the rate and efficiency of decomposition, generating a high enthalpy plasma jet. In one embodiment, the anode 1124 is provided as a magnet, which may be a permanent magnet, or a coil(s) that can be wrapped around the reactor 1102 and induce a magnetic field when a current is applied to it, to help control or otherwise regulate the rotation of the plasma.

[0113] The plasma forming gas expands and is forced out of the bottom nozzle 1128 as plasma 1108 into the fluid 1136 where it transfers all of the plasma heat and breaks down the local fluid around the nozzle 1128, thereby generating hydrogen, syngas, and carbon solids. That is, the heat of the plasma 1108 exiting the nozzle 1128 heats the fluid or liquid 1136 in the area of ​​the nozzle 1128 and breaks it down into its component molecules, resulting in hydrogen, syngas, and carbon solids. As shown, the level of the fluid 1136 is above the nozzle 1128, so that as the plasma 1108 exits the nozzle 1128, it immediately comes into contact with the fluid or liquid 1136 in the area of ​​the nozzle 1128. The heated gas bubbles around the nozzle 1128 and is discharged from the vessel via the syngas output 1114 for purification.

[0114] In one embodiment, the reactor 1102 includes a discharge plasma reactor 1130 in which a hot gas stream (or plasma jet) 1108 is generated that is directed through a nozzle 1128 toward and directed into a liquid 1136. As explained above, the plasma jet stream 1008 is directed into the liquid 1136, providing thermal energy that results in the decomposition of hydrocarbons in the liquid 1136. There is a natural gas feedstock 1110 that provides gas to the discharge plasma reactor 1130 to create the hot plasma jet 1108.

[0115] The cathode 1118 side of the high voltage / high current reactor apparatus is shown in FIG. 11 in a triangular shape, although this shape is not limiting and may be any suitable shape. The cathode 1118 is one side of the high voltage / high current supply that creates a plasma discharge where the decomposition occurs. The syngas output 1114 is the outlet for all gases produced by the reactor shown in FIG. 11, including hydrogen. In one embodiment, there is an additional amount of syngas return (e.g., a given percentage of the exhaust gas), which may provide a means to recycle filtered bypass gas from the syngas output 1114, where the desired hydrogen is filtered from the decomposition.

[0116] The anode 1124 is the other side of the high voltage / high current supply for the discharge plasma 1122, driving its movement for the decomposition of the raw gas that is fed into the hot plasma jet. The discharge plasma 1122 may move as shown diagrammatically by the curved line showing the plasma 1122 in FIG. 11. As the plasma exits the nozzle 1128, it flows into the liquid 1136 as shown diagrammatically by the curved arrow below the nozzle 1128. The nozzle 1128 focuses the plasma jet into the liquid due to the heat of decomposition. During the process, carbon solids 1134 are formed and are shown as black particles captured by the liquid 1136. The pump 1138 removes the liquid from the reactor at a constant rate (predetermined experimentally by the decomposition rate), for example. During this time, the liquid passes through the filter 1106. After the filter 1106, the carbon is concentrated and may be sent for further processing. A pump 1138 may return the filtered liquid to the reactor via liquid return 1104 for reprocessing.

[0117] FIG. 12 shows an additional embodiment, where the process vessel 1202 shown and described herein, including in conjunction with FIGS. 10-11, is of modular design and can be clustered together to increase the total hydrogen / syngas output per unit area. The number of units in a cluster is not limited, but in practice may be practically limited by the output requirements of such a facility. This arrangement also allows for economies of scale to be leveraged from a larger single syngas purification unit and a single fluid / solid carbon removal (filter / decanter / centrifuge) unit. As shown, the individual syngas outputs of each module connect to a common syngas output 1204. Similarly, the modules share a common carbon output 1206. In some embodiments, the vessel may have a sloped or funnel-shaped bottom of each modular unit, for example, to facilitate collection of carbon solids. Such modules may also be clustered together in multiple dimensions (e.g., in a matrix-like arrangement) to create an even larger liquid pool unit. Again, this allows for economies of scale using other shared equipment to reduce processing costs and facility size.

[0118] Figure 13 shows a cross-sectional view of an embodiment similar to that shown and described with respect to Figure 11, where the plasma reactor is in intimate contact with the fluid in the vessel. As shown in Figure 13, a hydrocarbon dissociation system 1300 includes a reactor 1302 having a vessel 1304, and further includes (i) a plasma source 1306 (e.g., a DC plasma reactor), (ii) an input of natural gas (or other hydrocarbon-based) feedstock 1308, which is a selected hydrocarbon that is dissociated in a high temperature, high energy plasma jet generated by the reactor 1302 and directed into a liquid pool 1310 of hydrocarbons to be cracked, (iii) an anode 1314 of the DC plasma reactor 1306, and (iv) a plasma source 1306 connected to the reactor 1302, which is connected to the vessel 1304. 12 and magnets that intensify the DC discharge rotation around the interior of the discharge plasma in such a manner as to dissociate all of the natural gas; (iv) a hydrogen (H2) outlet 1314 where the gas produced by the cracking is directed for cooling and purification; and (v) a carbon outlet 1316, e.g., at the bottom left, where carbon-laden liquids are pumped through an oil filter separator 1318 and the freshly filtered oil is returned to the liquid pool 1310 via an oil return port 1320 for continued processing.

[0119] The reactor 1302 may include a cylindrical vessel 1304, made, for example, of a dielectric material or steel, that contains the plasma and provides a liquid pool, multi-port injection of natural gas, oil filtration, and an H2 outlet to a gas cooling station 1322. The gas cooling station 1322 may include a carbon collection zone (e.g., a cyclone-type particle separator for dust and particulates) at the bottom of the station that leads to a separation and purification module 1324. In an embodiment, the reactor may be elongated and may have a diameter to length ratio of about 2:1 to 10:1.

[0120] Figure 14 shows an approximate isometric cross-sectional view of an embodiment similar to the configuration of Figure 10, where the cathode is positioned over the anode in the form of a rotating drum half wetted by the fluid in the vessel, and the DC discharge goes directly from the cathode to the anode drum partially embedded in the fluid. As shown in Figure 14, a carbon graphite rod 1401 as the plasma source cathode electrode is installed vertically at the top of the vessel; 1402-hydrogen exhaust is a pipe extending at an angle of about 45 degrees from the top right; 1403-the rotating drum anode across the width of the vessel is wetted with the hydrocarbon liquid, where the plasma discharge dissociates the hydrocarbon into hydrogen and solid carbon; 1404-the anode drum rotating gear motor is controllable from 0 to 100 revolutions per minute; 1405-the wet liquid level of the rotating drum (and also the top part of the vessel 1406, which is removable for maintenance) is controlled by the drum. is held constant so that the top of extends above the liquid level; 1406 - carbon and hydrocarbon container and bottom funnel; 1407 - carbon enrichment pump at the bottom center of the schematic is where the carbon laden liquid is moved to filtration; 1408 and 1409 - solid carbon removal is shown in this feature but could be a filter, centrifuge, decantation tank, or other solids in liquid separation method; 1408 - bottom left shows outlet for separated carbon to further processing; 1410 - filtered hydrocarbon liquid returns to center left as this oil stream for recirculation.

[0121] Figure 15 is a schematic diagram utilizing a CAD revision of an approximate cross-sectional view of an "as built" implementation of an embodiment similar to that shown in Figures 11 and 13, in which a processing vessel includes a plasma reactor that is at the top but positioned flush with the fluid level in the vessel in such a manner as to inject a high temperature plasma jet into the fluid. The processing vessel includes a plasma reactor that is at the top but positioned flush with the fluid level in the vessel in such a manner as to inject a high temperature plasma jet into the fluid. 1501 - plasma source reactor (also DC plasma reactor in FIG. 13 and discharge plasma reactor in FIG. 11); 1502 - hydrogen exhaust (also H2 in FIG. 13 and syngas output in FIG. 11); 1503 - thermal plasma gas injection level into the liquid (this is also the oil-filled liquid leveller in FIG. 13); 1504 - hydrocarbon container (the container in FIG. 11 and the reactor containment in FIG. 13); 1505 - liquid level held at this point (not shown in FIG. 11 but shown as oil-filled liquid leveller in FIG. 13); 1506 - carbon and hydrocarbon liquid funnel at the bottom where oil is removed for filtration; 1507 - carbon concentrate pump which is the oil filter in FIG. 13 and the carbon / liquid separator in FIG. 11; 1508 - solid carbon removal at the bottom left is the carbon outlet where carbon is further processed; 1509 - represents the filter; 1510 - filtered hydrocarbon liquid return.

[0122] In some embodiments, the carbon formation is stopped by direct contact with the liquid feedstock. This quenching of the carbon formation process determines the properties of the carbon black formed, and therefore its marketability.

[0123] The reactor is cooled, for example, by a water cooling system coupled to the reactor, not shown in these figures. In operation, DC power is supplied to the cathode and anode to create a plasma. Hydrocarbon-containing gas is introduced into the top gas inlet and enters the process zone in the reactor at an angle through an angled opening (such as gas outlet 806 shown in FIG. 8C).

[0124] Also, in some embodiments, RF power may be provided to the cathode and anode to create the plasma, for example, simultaneously with the generation of the DC-based plasma. Ideally, the hydrocarbon-containing gas is a pure or substantially pure hydrocarbon. In practice, there are impurities that must be filtered out. Furthermore, there may be a single hydrocarbon-containing gas or a mixture of different hydrocarbon-containing gases (e.g., methane and natural gas).

[0125] The gas flow of the hydrocarbon-containing gas pushes it into a plasma treatment zone where the high energy plasma discharges collide with the hydrocarbon-containing gas passing through this zone with high energy, dissociating with great efficiency and breaking the carbon-hydrogen bonds in the hydrocarbons into single hydrogen and carbon atoms, i.e., the elemental components of the hydrocarbons. In this zone, the hydrocarbon-containing gas is heated to a temperature in the range of 1,000°C to 2,000°C, in embodiments about 1,500°C, where most or substantially most of the hydrocarbons are converted to their elemental components.

[0126] For example, in some embodiments, more than 90% of the hydrocarbon-containing gas is dissociated, in other embodiments, more than 95% dissociation is achieved, in other embodiments, more than 98%, and in other embodiments, substantially 100% (e.g., 99.99%) is achieved. Operational parameters such as, but not limited to, a plasma gas feed flow rate slower than the experimental nominal values, in combination with higher voltage and current values ​​applied to the cathode and anode, result in higher / highest conversion rate of hydrocarbons to hydrogen (dissociation rate) as well as the highest productivity. Higher flow rates and lower voltages reduce the conversion rate but produce hydrogen at a higher rate. The actual parameters are based on the magnitude and range of the plasma generator power and the desired product characteristics, hydrogen specifications or carbon specifications to be maximized.

[0127] The discharge plasma is generated through the thin film from the cathode to the rotating anode drum, instantly vaporizing the thin film at the highest possible temperature, as shown in Figure 10. The discharge is oscillated / scanned across the top of the rotating drum to maximize the volume of exposed liquid, where hydrogen is generated.

[0128] In Figure 11, a plasma flame is generated just above the liquid level in the reactor, and this high temperature / high velocity gas blows through the liquid, imparting dissociation energy to produce hydrogen as a gas and carbon as a solid wetted by the liquid, which is then filtered from the liquid by recirculating filtration.

[0129] An advantage of the systems disclosed herein is that they are much more efficient since generally less energy is required to crack the hydrocarbons and almost all of the energy put into the plasma is spent on the dissociation process. In some embodiments, the systems can achieve efficiencies of about 24 kWh / Kg, and in some embodiments, efficiencies can be about 15 kWh / Kg to about 30 kWh / Kg. Prior art systems have significantly lower efficiencies.

[0130] The following generally applies to any of the hydrocarbon dissociation systems disclosed herein, including the hydrocarbon dissociation system: The cathode may be optionally movable. The cathode material degrades and etches with use, becoming smaller over time. For example, the position of the cathode may be controlled to maintain a constant distance between the cathode and the anode. This improves operation of the system over time and can increase the continuous operation time before the cathode must be replaced. Dynamic cathode positioners are described further herein. In another embodiment, the inserted cathode can be configured with an additional cathode that screws into the rear end of the first cathode, increasing the overall usable life.

[0131] Exemplary hydrocarbon-containing gases for use in the embodiments disclosed herein include methane, natural gas, compressed natural gas (CNG), petroleum gas, synthetic gas, biodiesel, and other types of hydrocarbons, including any combination thereof.

[0132] In some embodiments, the target temperature for dissociating the hydrocarbon-containing gas is about 1,500° C., and may be about 1,000° C.-2,000° C. At or within this temperature range, a high percentage of the hydrocarbons may be dissociated (e.g., greater than 98% of the hydrocarbons are dissociated) with efficient energy usage. Dissociation may still be successful at higher temperatures (e.g., greater than 2,000° C.), but the additional energy to reach those temperatures is effectively "wasted" in that dissociation is not substantially improved relative to the additional energy used.

[0133] The reactor system may comprise a single reactor or multiple parallel reactors of the same or different types, in other words, the hydrocarbon dissociation system disclosed herein is modular.

[0134] The hydrocarbon dissociation system disclosed herein may be used in a variety of applications, examples of which may include, but are not limited to, light oils such as vegetable cooking oils, fuels such as alcohol, acetone, kerosene, methanol, diesel and gasoline, heavy liquids such as crude oil, waste crankcase oil, transmission fluids, and semi-solids such as asphalt where the feedstock needs to be preheated in order to flow into the vessel.

[0135] The plasma source / reactor may comprise a direct current (DC) discharge plasma source, as shown in Figures 10, 11, 12 and 13. The DC discharge plasma source comprises a cathode and an anode. The cathode and anode may take a variety of shapes, including cylindrical, conical, ring-shaped, and other geometric configurations. Exemplary materials for the cathode and anode include lithium cobalt oxide (LCO), lithium nickel manganese cobalt oxide (NMC), lithium nickel cobalt oxide doped with alumina (NCA), lithium manganese oxide (LMO) and lithium iron phosphate (LFP).

[0136] The DC discharge plasma source also includes a power source, such as a DC power source. When DC power is applied to the cathode and anode in the presence of a hydrocarbon-containing gas, a plasma discharge is created, which occurs between the cathode and the anode. In some embodiments, the plasma source may further include a radio frequency (RF) power source that can create an RF-based plasma between the cathode and the anode. Although the DC-based plasma is a discharge, if an RF-based plasma is used, it expands to fill the volume of the reactor in the plasma processing zone.

[0137] A hydrogen / syngas output is provided to allow gaseous hydrogen to be collected. For example, a hydrogen outlet may include valves and piping to allow hydrogen to be exhausted from the hydrocarbon dissociation system. The exhausted hydrogen may contain some amount of hydrocarbon gas and / or other impurities and may undergo further purification processing. In some embodiments, the remaining hydrocarbon gas may be recycled to the reactor, for example, by pressure already provided by a purification compressor or by venture into the plasma gas feedstock supply.

[0138] As shown in the bottom left of each figure, a carbon outlet (shown as a carbon / liquid separator) is provided to allow for filtering and collection of solid carbon from the feed liquid. From this filtered collection, the carbon along with some of the fluid is transferred to a rotating oxygen-free pyrolysis kiln operating at about 800°C where the fluid is vaporized as synthesis gas and returned to the plasma reactor for conversion, and the dried carbon, now carbon black, is packaged for sale or further processing.

[0139] FIG. 12 illustrates a multiple liquid hydrocarbon dissociation system utilizing a rotating drum generated liquid film device as a method of combining fluid holding vessels, fluid filtration requirements, cooling requirements, and gas filtration and purification requirements, according to one embodiment.

[0140] The processes disclosed herein can be run continuously with little or no interruption. This minimizes the impact of downtime due to maintenance. Allowing the process to stabilize and operate at preferred nominal process parameters leads to more consistent product quality. One of the few maintenance interruptions in the disclosed processes is the replacement of a high temperature cathode in the reactor. The cathode can be made, for example, of graphite or graphite composite, and can be made with desirable dimensions, particularly for extended service life, but due to the etching effect of high current on the cathode, it will corrode over time and must be replaced. In some embodiments, the cathode is positioned relative to the anode to adjust the size and potential of the plasma energy, and in embodiments, this dimensional feature is within about + / - 10% of a predetermined value.

[0141] In an embodiment, as shown in Figures 11, 12, 15 and 16, a sensor (e.g., a Honeywell Co. methane gas detector) may be used to measure the amount of hydrocarbon-containing gas exiting the reactor through either the hydrogen and carbon outlets and / or passing through the gas / solids separation zone or the syngas output / hydrogen exhaust (702). Sensors may also be used to measure the amount of hydrocarbon-containing gas entering the reactor through the inputs. From these measurements, the amount of hydrocarbon-containing gas that dissociates may be determined. If this amount is too low (e.g., less than 98%), a control circuit coupled to the DC power supply may change the current flow, rotation speed, and other process control parameters to have the effect of spinning the plasma faster to keep the conversion rate constant and high.

[0142] FIG. 16 illustrates the process flow of liquid cracking in a block diagram according to one embodiment. In this embodiment, a tanker or other transport vehicle delivers oil, lubricants, and other types of liquids (including but not limited to waste liquids and waste liquids) which are temporarily stored. Liquid pretreatment is performed during storage and before use. This includes chemical analysis, blending for homogeneity, degassing, and dehydration. Since the liquids are obtained from various supplies and stored in different tanks for pretreatment, it is assumed that the chemicals and concentrations of said chemicals are different, so analysis may be required to determine the blending portions of different liquids together as components to form an acceptable and processable feedstock. A pre-determined blending chart may assist the process in obtaining relative cracking rates, uniform flow of hydrogen, heating consistency, and carbon / hydrogen ratio. This ratio establishes the process parameters that are pre-determined by experimental results for best hydrogen conversion and purity. While the fluids are waiting, pretreatment of degassing and dehydration (indirect heating to >100°C and <150°C) is performed. The fluids are then mixed during transport to the processor, but because they are warm from the pretreatment, entry into the reactor can be achieved by low energy liquid pumping. When the natural gas (or syngas) as an ionized plasma gas releases all the plasma energy to the liquid, the process is instantaneous, generating hydrogen in gaseous form, carbon particles in the liquid, and numerous other hydrocarbon gas vapors. Optionally, a direct discharge into the liquid is also described herein as a decomposition method. The gas then passes to a cooling and condensation unit without contact with or dilution from the outside air. This facility reduces the hydrogen temperature below the condensation temperature of the hydrocarbon vapors. The condensed vapor is returned to the vessel liquid pool for reprocessing, and the hydrogen passes to membrane or PSA decontamination. This results in hydrogen of 99-99.99% (if woven or PSA treated, respectively) quality suitable for industrial or fuel cell use, respectively. The clean hydrogen is pumped to a storage tank at a pressure above 10 bar. Further pressurization and / or pressure transfer to a delivery truck or rail car may be required, which is accomplished with additional pump / compression pressures of 170 to 350 bar, or in some embodiments 500 bar.The oil collects the carbon that is generated. This carbon accumulates and settles to the bottom of the vessel. The dense carbon sinks to the bottom of the vessel and is slowly pumped to a filtration mechanism where the excess oil extracted here is reprocessed by pouring it back into the vessel's constant level liquid. The collected carbon moves to a final processor, which may be a top-loading plasma reactor, similar to a gas processing unit, where the carbon chunks undergo "drop-in" cracking to create hydrogen and carbon black. In some embodiments, the collected carbon may be processed through a pyrolytic plasma / syngas pyrolysis kiln to convert the oil-soaked carbon into hydrogen and carbon black.

[0143] The hydrocarbon dissociation system disclosed herein may be used in a variety of applications. For example, dissociation of hydrocarbons may be useful when dealing with natural gas, such as liquefied natural gas (LNG). A supply facility liquefies the natural gas into LNG, which can then be transported in ships specially designed to carry LNG from the supply facility to the receiving facility. Typically, LNG is transported from oil and gas fields where it is drilled and liquefied. It is then transported in ships to the customer's location, since the energy density of this liquid is higher than that of hydrogen. From there, it is regasified (the physical phase simply changes from liquid to gas) and then pumped to storage tanks on land, or pumped on land in the same liquid state as it was transported. This is simply a change in physical state, not a conversion to a different compound (as this application calls it).

[0144] The vessel may have three main processing components on board. First, there may be a regasification processor, such as those known in the industry, sized to accommodate the expected volume of natural gas processed per day and the natural gas generator power required for processing and associated equipment. Second, the vessel may have a smaller and more limited amount of LNG storage, but sufficient to accommodate a number of days of power generation and feed gas from the on-board natural gas generators. Third, the vessel may have a conversion reactor (i.e., a hydrocarbon dissociation system as described herein) to produce and store hydrogen from the hydrocarbon feedstock.

[0145] In an embodiment, the vessels may be equipped with a hydrocarbon dissociation system such as system 100 or system 200. For example, the vessel may have reactors of various sizes, e.g., 5-10 megawatt reactors, capable of generating high quality hydrogen. The vessel may travel to a receiving location to receive LNG. A portion of the LNG may be transferred to a regasification processor for regasification. Regasification of LNG is performed as needed, with some margin for surge capacity. If dehumidification is required, it is performed here to ensure a high quality feedstock source for processing, and the gaseous NG is immediately used to generate electricity. As a result of this regasification, electricity may be generated, and exhaust gases may be used for heating (e.g., as required by the regasification), or cooled exhaust gases may be released. Additionally or alternatively, natural gas (or other feed gas) may be converted to hydrogen by the on-board hydrocarbon dissociation system, and this hydrogen may be stored and pumped to a receiving facility. Additionally, the conversion of natural gas to hydrogen may produce carbon, which may be packaged and transported to the same or a different receiving facility, or dumped as an inert solid without negative environmental impact.

[0146] Aspects of the present disclosure are further illustrated by the following non-limiting list of clauses: Clause 1. A method for producing hydrogen and carbon from hydrocarbons in a reaction chamber, comprising: introducing a hydrocarbon into a chamber to rotate the hydrocarbon in a first direction; generating a direct current (DC) based plasma from a portion of the hydrocarbon and at least partially heating the hydrocarbon with the DC based plasma to a temperature greater than 1,000°C; rotating the DC-based plasma in a second direction different from the first direction; converting the hydrocarbons into their elemental components, including carbon solids and hydrogen gas; and separating the carbon solids from the hydrogen gas to provide a solid portion and a gas portion. Clause 2. The method of clause 1, wherein the second direction is opposite to the first direction. Clause 3. The method of any one of clauses 1-2, further comprising quenching the carbon solids, the carbon solids comprising carbon black. Clause 4. The method of any one of clauses 1-3, wherein the portion of the plasma and the portion of the hydrocarbon contact each other at an angle based on their respective rotations that differ in one or more dimensions. Clause 5. The method according to any one of clauses 1 to 4, wherein the hydrocarbon is contained in a gas that is substantially free of oxygen, nitrogen and sulfur. Clause 6. The method of any one of clauses 1 to 4, wherein the amount of oxygen, nitrogen and sulfur in the gas is less than 1 mole percent. Clause 7. The method of any one of clauses 1-6, further comprising generating a radio frequency (RF)-based plasma. Clause 8. The method of any one of clauses 1-7, wherein separating the carbon solids from the hydrogen gas includes removing the carbon solids via a fluid-cooled auger in a manner that limits reintroduction of air to the carbon solids in the separation chamber. Clause 9. The method of any one of clauses 1 to 8, wherein the hydrocarbon is heated to a temperature of 1,400°C to 2,000°C. Clause 10. Separating said carbon solids from said hydrogen gas comprises: placing the carbon solids and the hydrogen gas in a volumetrically larger section of the reaction chamber to reduce gas velocity and allow the carbon solids to sink due to gravity; reducing the temperature by allowing the carbon solids and / or the hydrogen gas to contact the walls of the reaction chamber, thereby reducing the volume and velocity of gas; 10. The method of any one of clauses 1-9, further comprising one or more of: physically retarding the carbon solids by contacting the carbon solids and / or the hydrogen gas with the walls, so that the carbon solids can gather and fall to the bottom of the reaction chamber. Article 11. An apparatus for producing hydrogen and carbon solids from gaseous hydrocarbons, comprising: a process chamber having a gas inlet, a gas outlet, and a solids outlet; a direct current (DC) plasma generator configured to generate a plasma in a plasma processing zone of the processing chamber, the direct current (DC) plasma generator comprising a cathode and an anode in the processing chamber, the plasma configured to heat gas passing through the plasma processing zone to a temperature in excess of 1,000° C. to dissociate hydrocarbons in the gas; a magnet external to the process chamber and configured to rotate the plasma generated by the DC plasma generator; a cooling system in a separation zone of the processing chamber, the gas inlet configured to rotate gas passing through the gas inlet. Clause 12. The apparatus of clause 11, wherein the cathode is movable, the apparatus further comprising a control system configured to move the cathode to maintain a predetermined distance between the anode and the cathode. Clause 13. The apparatus of any one of clauses 11-12, further comprising a fluid-cooled auger configured to remove solid carbon from the treatment chamber. Clause 14. An apparatus as described in any one of clauses 11 to 13, wherein the magnet external to the processing chamber is configured to rotate the plasma generated by the DC plasma generator at a speed of between 1,000 RPM and 6,000 RPM. Clause 15. The apparatus of any one of clauses 11-14, further comprising a radio frequency (RF) plasma generator configured to generate a plasma within the plasma processing zone of the processing chamber. Clause 16. The apparatus of any one of clauses 11 to 15, wherein the magnet, external to the processing chamber and configured to rotate the plasma generated by the DC plasma generator, is further configured to rotate the plasma generated by the DC plasma generator in a direction opposite to a direction of rotation of the gas passing through the gas inlet. Article 17. An apparatus for producing hydrogen and carbon solids from gaseous hydrocarbons, comprising: a process chamber having a gas inlet, a gas outlet, and a solids outlet; a plasma generator configured to generate a plasma in a plasma processing zone of the processing chamber, the DC plasma generator configured such that the plasma heats gas passing through the plasma processing zone to a temperature in excess of 1,400° and dissociates hydrocarbons in the gas; a magnet external to the process chamber and configured to rotate the plasma generated by the DC plasma generator; a cooling system in a separation zone of the treatment chamber, the cooling system capable of reducing a gas temperature to below about 500° C. to stop the formation of carbon black particles, aggregates, and agglomerates. Article 18. An apparatus for producing hydrogen and carbon solids from gaseous hydrocarbons, comprising: a process chamber having a gas inlet, a gas outlet, and a solids outlet; a plasma generator configured to generate a plasma in a plasma processing zone of the processing chamber, the DC plasma generator configured such that the plasma heats gas passing through the plasma processing zone to a temperature in excess of 1,400° and dissociates hydrocarbons in the gas; a magnet external to the process chamber and configured to rotate the plasma generated by the DC plasma generator; a cooling system in a separation zone of the treatment chamber, the cooling system capable of reducing a gas temperature to below about 1000° C. to stop the formation of carbon black particles, aggregates, and agglomerates. Clause 19. The apparatus of any one of clauses 17-18, wherein the cooling system comprises a plurality of gas injection nozzles arranged circumferentially around a portion of the reaction chamber downstream from the anode, the gas injection nozzles being coupled to a source of hydrogen gas capable of passing through the gas injection nozzles to create a cooling gas curtain through which the gas exiting the plasma processing zone must pass. Clause 20. The apparatus of clause 19, wherein the source of hydrogen gas is a small portion of pressurized hydrogen gas from a purification system coupled to the gas outlet. Clause 21. A method for producing hydrogen and carbon solids from liquid hydrocarbons, comprising: Introducing liquid hydrocarbons into a treatment vessel; introducing a plasma forming gas; forming or maintaining a DC plasma discharge between a cathode and an anode based at least in part on the plasma-forming gas, the anode being rotatable and at least partially immersed in the liquid hydrocarbon; rotating the anode to form a liquid film covering the anode, such that hydrocarbons within the liquid film are heated by the DC plasma discharge to a temperature in the range of 1500K to 6000K, thereby converting at least a portion of the hydrocarbons in the liquid film to elemental components; cooling the ingredients to form a product mixture of gas and solids comprising hydrogen gas and carbon solids; and extracting the product mixture of hydrogen gas and carbon solids. Clause 22. The method of clause 21, wherein the hydrogen gas in the product mixture of hydrogen gas and carbon solids is in a syngas, and extracting the product mixture of hydrogen gas and carbon solids includes separating hydrogen from other components of the syngas. Clause 23. Extracting the product mixture of hydrogen gas and solids comprises: allowing the hydrogen gas in the hydrogen gas and solid product mixture to be discharged from a gas output; allowing the carbon solids in the hydrogen gas and solids product mixture to be discharged from a carbon output; and separating carbon solids from liquid in the carbon output. Clause 24. The method of clause 23, wherein the gas output is positioned above a predetermined level of liquid in the process vessel and the carbon output is positioned below the predetermined level of liquid in the process vessel. Clause 25. The method of any one of clauses 21-24, wherein separating carbon solids from liquid in the carbon output includes using a filter. Clause 26. The method of any one of clauses 21-25, wherein liquid separated from carbon solids in the carbon output is returned to the processing vessel. Clause 27. The method of any one of clauses 21-26, further comprising separating vapor laden H2 gas having a vapor content above a threshold from the H2 gas in the gas output, and returning condensed liquid from the vapor laden H2 gas to the process vessel. Clause 28. A method according to any one of clauses 21 to 27, wherein the treatment vessel is sealed such that atmospheric gases cannot enter above the level of liquid in the treatment vessel. Clause 29. The method of any one of clauses 21-28, wherein introducing a plasma-forming gas includes converting a portion of the liquid hydrocarbon into a gas and a solid. Clause 30. The method of any one of clauses 21 to 29, further comprising controlling a level of liquid in the processing vessel to maintain the level of liquid at a predetermined level. Clause 31. The method of any one of clauses 21 to 30, wherein the anode comprises a drum. Clause 32. The method of any one of clauses 21-31, further comprising pre-treating the liquid hydrocarbons to remove one or more of entrapped gas, water and light hydrocarbons prior to introducing the liquid hydrocarbons into the treatment vessel. Clause 33. A system for producing hydrogen and carbon solids from liquid hydrocarbons, comprising: a process vessel having a first region for containing a gas and a second region for containing a liquid hydrocarbon; a cathode and an anode, the cathode and the anode forming or maintaining a DC plasma discharge between the cathode and the anode, the anode being rotatable; a gas output in the first region; a carbon output in the second region; a liquid inlet in the second region for introducing liquid hydrocarbons into the treatment vessel; a power source coupled to the anode and the cathode. Clause 34. The system of clause 33, wherein the carbon output includes a filter. Clause 35. The system of clause 34, further comprising a liquid return port; and a pump coupled to said filter and said liquid return port and configured to reintroduce liquid from said carbon output into said treatment vessel. Clause 36. The system of any one of clauses 33-35, further comprising a gas inlet and a gas separation device coupled to the gas output and to the gas inlet, the gas separation device configured to separate pure hydrogen from other gases and further configured to reintroduce the separated other gases back to the process vessel. Clause 37. A system as described in any one of clauses 33 to 36, wherein the treatment vessel is sealed such that atmospheric gases cannot enter above the level of liquid in the treatment vessel. Clause 38. The system of any one of clauses 33-37, further comprising a controller coupled to one or more of the liquid inlets and the carbon outputs and configured to control the level of liquid in the treatment vessel to maintain the level of liquid at a predetermined level. Clause 39. The system of any one of clauses 33-38, wherein the anode comprises a drum. Clause 40. A system for producing hydrogen and carbon solids from liquid hydrocarbons, comprising an array of processing vessels; Each treatment vessel has a first region for containing a gas and a second region for containing a liquid hydrocarbon; Each process vessel has a cathode and an anode, where a DC plasma discharge is formed or maintained between the cathode and the anode, the anode being rotatable; Each process vessel has a gas output in the first region; Each treatment vessel has a carbon output in the second region; each treatment vessel having a liquid inlet in the second region for introducing liquid hydrocarbons into the treatment vessel; Each process vessel includes a power supply coupled to the anode and the cathode. Clause 41. The system of clause 40, wherein the array of processing vessels includes a row of n processing vessels, the number n>1. Clause 42. The system of clause 40, wherein the array of processing vessels includes m rows of n processing vessels, the first number being n>1 and the second number being m>1. Clause 43. The system of any one of clauses 40-42, wherein the carbon output of one of the processing vessels is shared between two or more of the processing vessels. Clause 44. The system of any one of clauses 40-42, wherein the carbon output of each of the processing vessels is shared between each of the processing vessels. Clause 45. A method for producing hydrogen and carbon solids from liquid hydrocarbons, comprising: Introducing liquid hydrocarbons into a treatment vessel; introducing a plasma forming gas; forming or maintaining a plasma between a cathode and an anode based at least in part on the plasma-forming gas; directing a plasma jet formed from the plasma into the liquid hydrocarbon, such that the hydrocarbons proximate to the plasma jet are heated by the plasma jet to a temperature in the range of 1500K to 6000K, thereby converting at least a portion of the hydrocarbons proximate to the plasma jet into elemental components; cooling the ingredients to form a product mixture of gas and solids comprising hydrogen gas and carbon solids; and extracting said gas and solid product mixture. Article 46. Extracting the product mixture of gas and solids comprises: allowing the hydrogen gas in the gas and solid product mixture to be discharged from a gas output; allowing said carbon solids in said product mixture of gas and solids to be discharged from a carbon output; and separating carbon solids from liquid in the carbon output. Clause 47. The method of clause 46, wherein the gas output is positioned above a predetermined level of liquid in the process vessel and the carbon output is positioned below the predetermined level of liquid in the process vessel. Clause 48. The method of any one of clauses 46-47, wherein separating carbon solids from liquid in the carbon output includes using a filter. Clause 49. The method of any one of clauses 46-48, wherein liquid separated from carbon solids in the carbon output is returned to the processing vessel. Clause 50. The method of any one of clauses 46-49, further comprising separating vapor laden H2 gas having a vapor content above a threshold from the H2 gas in the gas output, and returning condensed liquid from the vapor laden H2 gas to the process vessel. Clause 51. A method according to any one of clauses 46 to 50, wherein the treatment vessel is sealed such that atmospheric gases cannot enter above the level of liquid in the treatment vessel. Clause 52. The method of any one of clauses 46 to 51, wherein introducing the plasma-forming gas includes one or more of: (i) supplying a plasma-forming gas into the processing vessel from outside the processing vessel; and (ii) returning a portion of the extracted gas. Clause 53. The method of any one of clauses 46-52, further comprising controlling a level of liquid in the processing vessel to maintain the level of liquid at a predetermined level. Clause 54. A system for producing hydrogen and carbon solids from liquid hydrocarbons, comprising: a process vessel having a first region for containing a gas and a second region for containing a liquid hydrocarbon; a plasma generating reactor having a cathode and an anode for forming or maintaining a plasma between the cathode and the anode, and further having a nozzle for directing a plasma jet formed from the plasma to the second region; a gas output in the first region; a carbon output in the second region; a liquid inlet in the second region for introducing liquid hydrocarbons into the treatment vessel; a power source coupled to the anode and the cathode. Clause 55. The system of clause 54, wherein the carbon output includes a filter. Clause 56. The system of clause 55, further comprising a liquid return port; and a pump coupled to said filter and said liquid return port and configured to reintroduce liquid from said carbon output into said treatment vessel. Clause 57. The system of any one of clauses 54-56, further comprising a gas inlet and a gas separation device coupled to the gas output and to the gas inlet, the gas separation device configured to separate pure hydrogen from other gases and further configured to reintroduce the separated other gases back into the process vessel. Clause 58. A system as described in any one of clauses 54 to 57, wherein the treatment vessel is sealed such that atmospheric gases cannot enter above the level of liquid in the treatment vessel. Clause 59. The system of any one of clauses 54 to 58, further comprising a controller coupled to one or more of the liquid inlets and carbon outputs and configured to control the level of liquid in the treatment vessel to maintain the level of liquid at a predetermined level. Clause 60. A system for producing hydrogen and carbon solids from liquid hydrocarbons, comprising an array of processing vessels; Each treatment vessel has a first region for containing a gas and a second region for containing a liquid hydrocarbon; Each processing vessel includes a plasma generating reactor having a cathode and an anode for forming or maintaining a plasma between the cathode and the anode, and further including a nozzle for directing a plasma jet formed from the plasma to the second region; Each process vessel has a gas output in the first region; Each treatment vessel has a carbon output in the second region; each treatment vessel having a liquid inlet in the second region for introducing liquid hydrocarbons into the treatment vessel; Each process vessel includes a power supply coupled to the anode and the cathode. Clause 61. The system of clause 60, wherein the array of processing vessels includes a row of n processing vessels, the number n>1. Clause 62. The system of clause 60, wherein the array of processing vessels includes m rows of n processing vessels, the first number being n>1 and the second number being m>1. Clause 63. The system of any one of clauses 60-62, wherein the carbon output of one of the processing vessels is shared between two or more of the processing vessels. Clause 64. The system of any one of clauses 60-62, wherein the carbon output of each of the processing vessels is shared between each of the processing vessels.

[0147] While various embodiments have been described herein, it should be understood that they have been presented by way of example only, and not limitation. Thus, the breadth and scope of the present disclosure should not be limited by any of the exemplary embodiments described above. Moreover, the present disclosure encompasses any combination of the above-described embodiments in all possible variations thereof, unless otherwise indicated herein or clearly contradicted by context.

[0148] In addition, while the methods described above and illustrated in the drawings are shown as a series of steps, this is done for purposes of illustration only, and it is therefore contemplated that steps may be added, steps may be omitted, the order of steps may be rearranged, or some steps may be performed in parallel.

Claims

[Claim 1] The invention described in this specification.

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