Conductive Liquid Hydrocarbon Gas Plasmas for Materials and Chemical Synthesis and Transformations

Abstract

A high-voltage discharge between two electrodes that generates a plasma is placed in the reactor chamber. Hydrocarbon gas and a conductive liquid are passed through one or more electrodes, so that the conductive liquid cools the electrodes and avoids contamination. Such a discharge can produce hydrogen gas and additional carbon-containing by-products that can be used, released, or sequestered.

Description

[Technical field]

[0001] CROSS REFERENCE TO RELATED PATENT APPLICATIONS This application claims priority to U.S. Provisional Application No. 63 / 330,953, filed April 14, 2022, the disclosure of which is incorporated by reference in its entirety herein. [Background technology]

[0002] background The present invention relates generally to the fields of energy production, gas to liquid fuel conversion, macro and nano materials synthesis, hydrogen generation and carbon sequestration. Summary of the Invention [Means for solving the problem]

[0003] Abstract Some embodiments relate to a multiphase non-equilibrium plasma hydrocarbon reactor. The reactor may include a first electrode configured to receive a first conductive liquid from a first inlet port and energize the first conductive liquid to a first voltage. The reactor may include a second electrode configured to receive a second conductive liquid from a second inlet port and energize the second conductive liquid to a second voltage. The second electrode may be located at a distance from the first electrode. The difference between the first and second voltages may exceed the dielectric breakdown of a gas disposed within the reactor over that distance.

[0004] In some embodiments, the reactor may include a gas injection port configured to supply gas to the hydrocarbon gas reactor. In some embodiments, the gas injection port is one of the first or second electrodes. In some embodiments, the gas disposed in the reactor is a non-oxidizing gas that includes a hydrocarbon. In some embodiments, the hydrocarbon includes natural gas. The natural gas may be raw gas from a wellhead, gas from a natural gas collection line, or natural gas from a distribution line. In some embodiments, the hydrocarbon gas may be obtained from another process, such as a gasifier, biosynthesis, or other hydrocarbon gas production process. The hydrocarbon gas may therefore include non-hydrocarbon impurities common to such sources. In some embodiments, the dielectric sheath is in conjunction with the first injection port to supply the first conductive liquid to the first electrode. In some embodiments, the reactor may include a first exhaust vent for the gas, and an ignition source configured to ignite the exhaust gas. In some embodiments, the reactor includes a bypass vent configured to vent the gas prior to its introduction into the reactor. In some embodiments, the reactor includes a hydrogen generator, such as a fuel cell or a turbine, configured to receive hydrogen generated in the reactor and generate electrical energy. In some embodiments, the hydrogen electric energy generator includes at least one of a pressure swing absorption (PSA) system, a temperature swing absorption (TSA) system, a membrane purifier, or a dryer purification system that can condition the gas to specifications corresponding to the energy generation system. In some embodiments, the reactor is configured to generate a radial plasma and liquid vortex along an inner surface of its sidewall. In some embodiments, the reactor includes a plurality of magnets disposed about an outer surface of its sidewall. In some embodiments, the reactor is configured to adjust the flow rate of the first conductive liquid or the second conductive liquid in response to the conductivity of the respective conductive liquid.

[0005] Some embodiments relate to a system. The method may include a multi-phase non-equilibrium plasma hydrocarbon reactor. The reactor may include a first electrode configured to receive a first conductive liquid from a first injection port and energize the first conductive liquid to a first voltage. The reactor may include a second electrode configured to receive a second conductive liquid from a second injection port and energize the second conductive liquid to a second voltage. The second electrode is at a minimum distance from the first electrode. The gas injection port may be configured to supply a hydrocarbon gas to the reactor. The difference between the first voltage and the second voltage may exceed the dielectric breakdown of the hydrocarbon gas disposed within the reactor over that distance.

[0006] In some embodiments, the first injection port and the second injection port are different ports. In some embodiments, the gas injection port is one of the first or second electrodes. In some embodiments, the system includes a plurality of magnets arranged around an exterior surface of the reactor sidewall, the plurality of magnets configured to generate radial plasma swirls in combination with an electric field between the first electrode and the second electrode.

[0007] Some embodiments relate to a method. The method may include receiving a first conductive liquid at a first injection port by a multiphase non-equilibrium plasma hydrocarbon reactor. The method may include energizing the first conductive liquid at a first voltage by a first electrode of the reactor. The method may include receiving a second conductive liquid at a second voltage by the reactor, the second conductive liquid being located remotely from the first conductive liquid. The method may include receiving a hydrocarbon gas by the reactor. A difference between the first voltage and the second voltage may exceed a dielectric breakdown of the hydrocarbon gas to ionize the hydrocarbon gas.

[0008] In some embodiments, the method includes receiving a conductive liquid from the reactor. In some embodiments, the method includes separating a first portion of the conductive particles from the conductive liquid, and then injecting the separated conductive liquid into the reactor. In some embodiments, the method includes receiving a second conductive liquid from the reactor. In some embodiments, the method includes cooling the second conductive liquid by a heat exchanger. In some embodiments, the method includes injecting the cooled second conductive liquid into the reactor. [Brief description of the drawings]

[0009] [Figure 1] FIG. 1 is a cross-sectional view of a hydrocarbon gas reactor according to various embodiments. [Diagram 2] FIG. 2 is another cross-sectional view of a hydrocarbon gas reactor according to various embodiments. [Diagram 3] FIG. 3 is yet another cross-sectional view of a hydrocarbon gas reactor according to various embodiments. [Figure 4] FIG. 4 is a block diagram of a system for processing hydrocarbon gases provided in accordance with some embodiments. [Diagram 5] FIG. 5 is another block diagram of a system for processing hydrocarbon gases provided in accordance with some embodiments. [Figure 6] FIG. 6 is yet another block diagram of a system for processing hydrocarbon gases provided in accordance with some embodiments. [Figure 7] FIG. 7 is an isolated portion of a system 700 for processing hydrocarbon gases according to some embodiments. [Figure 8] FIG. 8 is another cross-sectional view of a hydrocarbon gas reactor according to various embodiments. [Figure 9] Figure 9A is a cross-sectional view of a hydrocarbon reactor according to some embodiments, and Figure 9B is an isometric view of the hydrocarbon reactor of Figure 9A according to some embodiments. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0010] Detailed Description Although hydrocarbons such as methane (e.g., biomethane) and other hydrocarbon gases contain hydrogen atoms, the formation of H2 or other substances or energy from these hydrocarbons represents a challenge. Some of these challenges include carbon released into the atmosphere, which can have adverse environmental and regulatory consequences. For example, carbon monoxide can be released from a methane-steam reforming reaction according to the reaction CH4+H2O<=>CO+3H2. In some reactors, carbon dioxide can be released from a combustion process used to drive the above-mentioned reaction. Passing methane through a plasma discharge can cause various chemical reactions that result in the formation of H2. For example, a reactor chamber can be filled with a substantially non-oxidizing gas, such as methane, and at least one electrode pair can be energized to a voltage high enough to cause breakdown of the gap between the two electrodes. The gap can be about 10-20 mm, and the electrodes can be energized (e.g., by an alternating or direct current source) to about a 10-20 kV potential. One skilled in the art will appreciate that the voltage and gap may be adjusted depending on the dielectric breakdown of the gas between the electrodes (eg, pressure, composition, etc.).

[0011] The plasma discharge may be operated such that non-equilibrium chemical reactions occur. Non-equilibrium conditions may be maintained in the presence of an electric field high enough that electrons have enough energy to initiate non-thermal ionization, dissociation, and chemical excitation. The reduced electric field in these non-equilibrium embodiments may range from tens to hundreds of Townsend (Td) in some embodiments. In non-equilibrium conditions, the reaction chemistry may differ from the reaction chemistry in an equilibrium system. For example, some steam-methane-reforming (SMR) processes may produce a hydrogen to carbon monoxide ratio of about 3 to 1 (H2:CO=3:1). Various embodiments of non-equilibrium multi-phase plasma reactors (e.g., reformers) may range, for example, from about 3 to 1 to about 10 to 1 for some operating conditions.

[0012] In some embodiments, higher water temperatures (e.g., above 30° C.) or more turbulent water flow can incorporate more steam into the plasma discharge zone and produce a relatively low H2:CO ratio. In some embodiments, lower water temperatures (e.g., below 30° C.) or less turbulent water flow can incorporate less steam into the plasma discharge zone and produce a relatively high H2:CO ratio. In addition, reactors that produce a relatively high H2:CO ratio use lower water temperatures (e.g., based on water content or heat exchangers), higher system pressures (e.g., controlled by headspace valves), salt water solutions (e.g., controlled by the addition of salt or other particles), larger dynamic plasma discharges, and larger amounts of non-thermal plasma. Reactors that use conductive liquids, such as conductive oils, that contain less oxygen than water can be used to generate gaseous products with a relatively high H2:CO ratio, which can reduce the impact of carbon dioxide emissions throughout the process.

[0013] The subsequent dielectric breakdown can create a plasma discharge between the electrodes, so that when a hydrocarbon, such as methane gas, enters the discharge, it can undergo various chemical reactions to produce products of H2, various oxygenates, or carbon particles, which can then be separated, sequestered, or otherwise used.

[0014] The operating voltage of the plasma can be lower than the original energization voltage, for example, 500V to 3kV. In the gas phase, hydrogen can be produced along with other species such as gaseous hydrocarbons (e.g., alkanes or alkenes). In some embodiments, such as when water is used as a liquid electrode, hydroxyl radicals and oxidized and partially oxidized compounds can be formed. In the liquid and solid phases, by-products such as, for example, carbon solids, polymers, alcohols, etc. can be sequestered and / or used. Hydrocarbons (e.g., natural gas) can enter the reactor through a gas injection port. In some embodiments, one or more electrodes can be hollow / cannulated, allowing gas to pass through the electrodes toward the plasma discharge.

[0015] The products of the system may occur in gas, liquid, and solid phases. For example, short chain alcohols, such as methanol, ethanol, propanol, propenol, and ketones, may be produced therein. In the production of hydrogen from hydrocarbons, gaseous carbon oxides or carbon solids may be produced. Coke (a grey, hard, high carbon content solid) is a possible product of hydrocarbon processing in the absence of oxygen. This coke, when formed, may present a challenge to transport out of the reactor to prevent contamination (such as the accumulation of unwanted material on surfaces such as electrodes). Maintenance cycles may be performed on the equipment to remove the coke and other buildup. Non-thermal multiphase plasma reactors with liquid electrodes may transport the generated solids out of the reactor to eliminate or reduce such maintenance. Non-equilibrium plasmas may produce solid particles on the scale of about 10 nm to about 1000 nm in some embodiments due to the high intensity of the processing reactions and the short residence time of the particles in the reaction zone. Such solids may cover large surface areas, such as electrode surfaces, if not transported. A non-limiting composition table of some example hydrophobic nanographene solids obtained by SEM-EDS is given below; other solid compositions and structures can be formed by varying the process temperature, pressure, current, solution salinity, flow rate, etc.

[0016] [Table 1]

[0017] In some embodiments, by-products may contaminate the reactor by forming particles on the electrodes, as in various pyrolysis and discharge pyrolysis systems. Contamination may occur when particles collect and accumulate on surfaces, preventing them from having the intended shape or surface properties (e.g., electrical conduction). For example, contamination with conductive carbon may cause the dielectric surface to become conductive and alter the discharge. In some embodiments, contamination is prevented by convecting the solids away from the surface using a (conductive) liquid as the discharge electrode. The conductive liquid may include water, molten metal, or oil. The conductive liquid may include various dissolved components to adjust its conductivity. Furthermore, the amount of such dissolved components may be adjusted or maintained. Similar to a metal electrode, a conductive liquid electrode may function as an electrical circuit electrode at the boundary of the plasma. Part of the liquid may volatilize and become a component of the plasma discharge. The volatilization may be controlled depending on the boiling point of the liquid electrode, the specific heat of the liquid electrode, etc.

[0018] In some embodiments, the liquid electrode contains water, and evaporation of a portion of the water electrode can add steam or methane reforming to the chemistry of the system, and can add aqueous shift reactions. In some embodiments, the liquid electrode contains water with salt, where this evaporation injects alkali, alkaline earth, or metal elements (e.g., Na, Ca, Mg, K) into the plasma discharge. These elements can significantly lower the electric field required to sustain the plasma and improve the efficiency of plasma generation (e.g., by lowering the electric field to sustain the plasma at the same current by 10% to 50%, according to some embodiments) compared to other elements (e.g., carbon) that can use additional energy to ionize.

[0019] The conductive liquid may be passed over one or more electrodes, thereby removing any contamination of the electrodes (e.g., carbon solid contamination), cooling the electrodes, etc. In some embodiments, the conductive liquid may be passed over one or more electrodes during operation, such that the conductive liquid functions as an electrode. For example, the conductive liquid may contain salts or other substances (e.g., NaCl, carbon solids, etc.) that may increase the conductivity of the conductive liquid and allow the conductive liquid to act as an effective extension of the electrodes. Advantageously, such embodiments may provide for cooling the chamber containing the electrodes during operation, removing and / or avoiding carbon buildup along solid electrodes, and further providing additional availability of steam, which may increase hydrogen production (e.g., in the case of water-containing electrodes, via the methane-water reaction). Additionally, such embodiments may use the turbulent and / or vortex motion of the conductive liquid to remove carbon contaminants, polymers, and / or other solids from the chamber (e.g., by precipitating various solids from solution via a collection area, by passing the conductive liquid through a filtration element, etc.). The various conductive liquid streams in these examples may be held at significantly different potentials and electrically separated upstream to ensure a high voltage discharge between the conductive liquid electrodes.

[0020] In some embodiments, various mechanical features of the dielectric sheath, electrodes, and various additional components (e.g., fans, magnets, heaters, etc.) can be used to direct the flow of conductive liquids, hydrocarbon gases, impart forces to the plasma, and accelerate or retard various chemical reactions. In some embodiments, the electrodes, dielectrics, and cannulas (e.g., various injection ports) can be positioned relative to one another to increase plasma raw gas interaction. For example, a dielectric sleeve can be extended beyond the end of the hollow electrode to press the plasma attachment point against the inner surface of the electrode. A mixture of axial and vortex flows can be used to convect the gas through the discharge to achieve the desired residence time of the gas in the active discharge zone. Similarly, a magnetic field can be applied to the plasma to convect the plasma discharge through the gas. A permanent magnet or electromagnet can generate a magnetic field (e.g., axial). The combination of a radial electric field E between the outer wall electrode and the centerline electrode and a radial current J can generate a JxB azimuthal Lorentz force. This can cause the plasma to rotate azimuthal (e.g., swirl). This movement may increase the rate of non-equilibrium plasma reactions and further disperse the formation of carbon particle synthesis, which may prevent contaminant particles from accumulating.

[0021] Many embodiments, as shown in the various figures herein, orient the top and bottom electrodes vertically, although some embodiments, including various embodiments that include fluid electrodes (i.e., the terminal portions of the electrodes are fluid, such as water), may orient the electrodes vertically or otherwise. Additionally, the positions of the top and bottom electrodes may be reversed, either mechanically or electrically. Thus, the nomenclature of the top and bottom electrodes is intended only to refer to the figures herein and is not intended to limit the present disclosure, which contemplates the top and bottom electrodes in various positions and with various relative polarizations. Additionally, electrodes may be referred to as first and second (and third and fourth, and inner and outer, etc.) as well. These nomenclatures are not intended to limit the position, polarization, fabrication, or energization order of the various electrodes, and are merely for clarity of reference. For example, in another embodiment, the discharge may occur between a centrally / axially disposed electrode and the inner wall of a cylindrical annulus, with the discharge being primarily radial. The conductive liquid may be in the outer annulus by tangential injection or swirling motion. The conductive liquid may also flow radially from the central electrode. Swirl may refer to a circular or helical rotation within the reactor body. For example, any fluid (e.g., vapor or liquid fluid) along with any plasma swirls in response to magnetic forces, electrical forces, gas input velocity, conductive liquid input velocity, mechanical rotation, etc.

[0022] The temperature of the conductive liquid can be controlled by adjusting the volume of water injected into or removed from the reactor. For example, for a water electrode, a temperature below 30°C can be maintained by increasing the flow rate of water through the reactor, or increased by decreasing the flow rate of water through the reactor to control its partial pressure in the hydrocarbon gas / steam mixture. This can reduce oxidation products, including CO and CO2, which are products of plasma steam reforming of hydrocarbons. Similarly, the pressure inside the reactor can be increased to reduce the evaporation of the liquid electrode material. Again, in the water electrode example, this increase in pressure reduces the production of CO and CO2 relative to the production of H2. All or only a portion of the liquid will evaporate when it encounters the heat and plasma in the reactor, and therefore the flow rate can be determined in combination with the rate of steam entering or leaving the reactor.

[0023] Similarly, the flow rate of the conductive fluid may be adjusted to control its conductivity. For example, a settling tank, filter, skimmer, or other separator for particles such as salts, carbon solids, etc. may remove particles from the water such that the flow rate of the conductive liquid between the reactor and the separator may control the conductivity of the conductive liquid. The reactor may adjust the flow rate to control the flow rate such that the liquid flow is effective to remove contamination to the electrodes, control the temperature of the reactor, etc. The flow rate may be controlled such that the conductivity loss through the liquid is maintained below a threshold value. For example, the reactor may include or interface with a controller configured to execute instructions of the non-transient medium. The controller may network with the various valves disclosed herein, along with sensors, to determine the temperature, pressure, conductivity, and other properties of the reactor, such as the conductive liquid, and may actuate the various valves in response to comparing the detected values ​​to threshold values.

[0024] In some embodiments, the material of the container containing the conductive liquid is formed from a conductive or dielectric component. Similarly, the hollow tube through which the conductive liquid is convected can be conductive or dielectric. The configuration of the circuit in which all materials in contact with the conductive liquid are either dielectric or plasma can be configured such that no metal or solid conductors are in contact with the conductive liquid. Such a configuration can advantageously facilitate the manufacture of embodiments having electrochemical reactions at the electrodes (e.g., both anodic and cathodic reactions) that can be suppressed to avoid chemical reactions of metal ions. Alternatively or additionally, the container containing the conductive liquid flow can be made of a specific conductor to specifically introduce a particular metal ion that is favorable to the product being produced. For example, those skilled in the art are familiar with the field of nanotube growth and will understand that Ni metal particles can serve as seeds for the synthesis of carbon nanoparticles of various shapes. In some embodiments, Ni ions in solution at the conductive liquid-plasma interface can serve as seeds for nanotube growth through one or more chemical pathways.

[0025] Referring to FIG. 1, a cross-sectional view of a hydrocarbon gas reactor 100 is provided according to various embodiments. The reactor 100 includes a hollow upper electrode 110, a conductive liquid injection port 120, and a dielectric sheath 130. The upper electrode 110 is connected to a first voltage, for example, via a bus bar, wire, or the like. In some embodiments, the various electrodes can be energized by applying an electric charge to the conductive liquid 120 and then dropping a droplet of the conductive liquid 125 onto the lower electrode 160, which can advantageously allow electrical isolation of the electrodes. The hollow center of the upper electrode 110 can be configured to pass the hydrocarbon gas from a storage facility, utility, or downwell location along a flow path 140 into the reactor chamber.

[0026] The upper electrode 110 may include one or more conductive elements. For example, a first metallic element may be connected to a first voltage source, and a second fluid element may be a conductive liquid 125, such as an aqueous solution including water and additives to adjust viscosity, conductivity, etc. Such an aqueous solution is referred to as water for ease of reference herein. For example, a salt (e.g., NaCl) may be added to the water to increase the conductivity of the water, and the water in contact with the first electrode (i.e., the first water) may be energized to approximately a first voltage.

[0027] In some embodiments, the conductive liquid may include a molten metal (e.g., cerium, gallium, combinations thereof, etc.). The metal may be liquid at about room temperature (e.g., below 100° C., such as below 30° C.), which may reduce the energy usage of the reactor. In some embodiments, the conductive liquid includes a hydrocarbon liquid (which may be nominally low conductivity) that includes carbon or metal conductive particles in solution. These may include microparticles or nanoparticles in solution. The particles may be added to the liquid or synthesized in the system and recycled in the liquid stream. The conductive liquid may include mixtures of various liquids as described herein, etc.

[0028] The bottom electrode 160 is shown as a conductive liquid electrode and may cover a conductive element (not shown) (e.g., a ground plane, bus bar, ground strap, etc.) for grounding the conductive liquid. A second conductive liquid injection port may supply conductive liquid to the bottom electrode. For example, in FIG. 1, the second conductive liquid port is the top conductor (i.e., the first conductive liquid may fall into the second conductive liquid either directly as droplets or after evaporation and recondensation). The second electrode 160 may be energized to a second voltage that exceeds the breakdown voltage of the gap (i.e., minimum distance) between the top electrode 110 and the bottom electrode 160 (including the conductive liquid 125 contained in the electrodes 110, 160) compared to the first electrode to form the plasma 150. A central opening in the hollow top electrode 110 may be used to pass a hydrocarbon gas (e.g., methane) through the gap between the top and bottom electrodes, which allows the gas to enter the plasma 150 at a controlled rate and induce various chemical reactions, including the formation of H2. The reactor may be a multi-phase reactor in which materials such as hydrocarbons may react in multiple phases (eg, solid, liquid, gas, and plasma phases).

[0029] The dielectric sheath 130 provides mechanical support to the upper electrode 110, such as by adhering the upper electrode 110 to the top or side of the reactor, and provides fluid retention to the electrode (e.g., to maintain the conductive liquid along the electrode). The flow rate of the conductive liquid may be set to maintain the conductive liquid along the electrode, to maintain a desired level of vapor of the conductive liquid, etc. Additionally, the conductive liquid may include various thickeners, detergents, etc. to adhere the conductive liquid to the electrodes, to avoid electrical connections (e.g., shorts) between the first and second electrodes, in addition to or instead of controlling the conductive liquid flow, surface smoothness, position of the upper or lower electrodes, etc.

[0030] In some embodiments, the amount of salt, particles, or other additives added to the conductive liquid can control its conductivity to control the formation of various substances. For example, the addition of NaCl at a concentration of about 3% can result in a relatively large percentage of carbon solids being formed, while NaCl at a concentration of about 0.1% can result in a relatively large percentage of polymers being formed. In conductive liquids that contain oxygen, such as water, some of the conductive liquid can form CO or CO2. Hydrocarbon containing conductive liquids can reduce oxidation and contribute to the production of solid particles or hydrocarbon gas. Those skilled in the art will understand that the production of various by-products can vary depending on the pressure, temperature, amount, flow rate, and composition of the hydrocarbon gas, and the conductive liquid. Various by-products can be produced in response to various inputs. The conductive liquid can be fed onto the first conductor by a conductive liquid injector that can inject the conductive liquid from outside the reactor through the first conductive liquid injection port 120 and / or recycle the conductive liquid from the reactor.

[0031] 2, another cross-sectional view of a hydrocarbon gas reactor 200 is provided, according to some embodiments. As shown, the conductive liquid 125 is received along the periphery of the dielectric sheath 130, which may advantageously simplify the design of the upper electrode 110. The dielectric sheath may be chamfered or otherwise shaped to allow the conductive liquid 125 to pass along the edge of the electrode (e.g., along a surface of the upper electrode, through a channel in the electrode configured to receive the conductive liquid 125, etc.). Advantageously, such an embodiment may avoid the multiple generally concentric openings found in the upper electrode of FIG. 1.

[0032] The upper electrode 110 may be a cannula (e.g., a stainless steel capillary electrode) configured to receive a hydrocarbon gas, including natural gas (e.g., ethane, methane, propane, etc.). The flow path 140 of the hydrocarbon gas indicates a net transfer of gas into the chamber, which may correspond to a pressure gradient between the gas source and the reactor.

[0033] Referring to FIG. 3, yet another cross-sectional view of the hydrocarbon gas reactor 100 is provided, according to some embodiments. As shown, the hydrocarbon gas 305 is introduced from the lower electrode 160, which may advantageously simplify the structure of the upper electrode. The hydrocarbon gas 305 is directed to the upper electrode via the hydrocarbon gas injector 310. In some embodiments, the hydrocarbon gas injector 310 may be the second electrode 160 or a conductive element that energizes a conductive liquid in contact with the second electrode 160 to a second voltage. In some embodiments, the conductive liquid 125 may be energized to the second voltage in other ways, and the hydrocarbon gas 305 may be guided in other ways (e.g., by a non-conductive port such as glass or plastic, by hydrodynamics such as vortexes in the conductive liquid, etc.). In some embodiments, multiple upper electrodes 110 or a large cross-sectional area of ​​the upper electrode 110 may eliminate the need to guide the methane other than by selecting an appropriate insertion point. Those skilled in the art will understand that the various elements of the illustrated embodiments may be adjusted, changed, and substituted amongst themselves, and that various mechanical pressures, etc., or other mechanisms may supply a conductive liquid to a pair of fluid electrodes at a first controlled rate, and introduce a controlled flow of a hydrocarbon gas at a second controlled rate, and maintain or adjust the distance between those electrodes, the first rate, the second rate, etc.

[0034] With reference to Figures 4-6, a carbon sequestration system is provided according to various embodiments. The system can be used for the combustion of natural gas or other gas sources. Natural gas can be treated as an incidental by-product (e.g., incidental to oil extraction) and released into the atmosphere, which may be undesirable (e.g., for environmental and / or regulatory reasons). Natural gas can include multiple components, including methane. To distinguish between the originally constituted natural gas and the later processed form, the originally constituted material can be referred to as associated gas or raw natural gas. Raw natural gas is often combusted, which can control the pressure of the natural gas (e.g., at the oil extraction site), but carbon dioxide and unburned methane can also be released. Some embodiments can process natural gas (e.g., including methane) by any of the methods disclosed herein. In some embodiments, the hydrocarbon gas is biologically derived (e.g., biogas from an anaerobic digester). Thus, at least a portion of the raw natural gas may be converted to H2, carbon solids, carbon-containing polymers, and additional carbon-containing chemicals in aqueous solution (alcohols, ketones, aldehydes, fatty acids, etc.). The new products as well as various gaseous products (e.g., acetylene, carbon monoxide, etc.) may also be separated (e.g., preferentially separated) and absorbed into a solid phase or an immiscible liquid phase (e.g., an oil phase containing condensable alkanes, alkenes, etc.). The various products may then be captured for reuse or further processing, or may be ignited (e.g., by an ignition source such as a pilot light or electric igniter) as a flare that may satisfy safety or regulatory concerns. Advantageously, because at least a portion of the methane is converted to H2, and because at least a portion of the carbon (e.g., carbon solids) becomes available for sequestration, the resulting flare may emit lower CO2 than raw natural gas. In some embodiments, there may be additional (e.g., fail-safe) carbon flare emission sites, which may allow for continued emission of raw natural gas, and in some embodiments, flaring.

[0035] With particular reference to FIG. 4, a block diagram of a system 400 for processing hydrocarbon gas is provided, according to some embodiments. A power supply unit 405 provides power to the hydrocarbon reactor 100. The power supply unit 405 may include a solar array, grid-based energy, or another energy source (e.g., natural gas or oil-based energy source). The hydrocarbon reactor 100 may receive hydrocarbon gas from a hydrocarbon gas input source 410, which may be a downwell source, an anaerobic digester, or other source. The hydrocarbon reactor 100 may be interposed with one or more gas input valves 475. As the hydrocarbon reactor 100 operates, the fluid electrode material may accumulate carbon or other materials therein. The hydrocarbon reactor 100 may be connected to a settling tank 420 or other process to control (e.g., remove or add) the accumulated materials. A reactor fluid outlet valve 415 may control the rate at which fluid is removed from the hydrocarbon reactor 100, thereby controlling the content of the reactor fluid. The settling tank 420 can separate the fluid, entrained gases, and particulate matter, and can include filters, separators, skimmers, and the like. A pump (e.g., a clarifier pump) can return the fluid to the reactor. A reactor fluid inlet valve 460 can control the rate or pressure of the fluid return. The settling tank 420 can receive water from a water source 465 via a water source valve 470. As above, various references to water can be substituted by various conductive liquids, such as metal or oil, having macro- or nanoparticles disposed therein. For example, the water source 465 can be a molten metal source 465.

[0036] The hydrocarbon reactor 100 can supply hydrocarbon gases to a condenser 430 via a reactor outlet valve 425. The condenser 430 can output the gases to a knock-out (KO) drum 440, where the vapor, gas, and entrained fluids can be separated. The entrained fluids and condensed vapors can be returned to a settling tank by a KO drum fluid valve 435. The gases can be output via a gas output valve 480 to a gas output 445, which can include flaring, gas storage, energy production, etc. Solids from the settling tank can be passed through a pump 442 (e.g., a carbon slurry pump) to sequester or otherwise dispose of the carbon-containing compounds in a storage location 450.

[0037] With particular reference to FIG. 5, another block diagram of a system 500 for processing hydrocarbon gases is provided, according to some embodiments. The system 500 includes a gas output 505 capable of receiving a purified hydrocarbon gas, such as hydrogen. The system 500 may include many of the various components of FIG. 4, along with a second stage KO drum 520. The second stage KO drum 520 may receive the output from the first stage KO drum 440 of FIG. 4, which may include a compressor 510 and a condenser 515 to further remove vapors, fluids, or other contents. Such fluids may be returned to the settling tank 420 via a second stage fluid valve 525. The gas may further pass through a dryer 530 and an H2-based purification section 535 (e.g., a membrane purifier). A purified gas (e.g., H2 gas) may be provided from the purification section 535, and another portion of the gas may be conveyed to the gas output 505 for flare or other disposal.

[0038] In some embodiments, a portion of the processed natural gas may be used to generate electrical energy, such as by use of an H2 fuel cell or a hydrogen turbine engine and generator. Advantageously, such a power source may supplement or eliminate the need for grid-supplied energy to operate the reactor. Excess electrical energy (greater than the energy to power the plasma discharge) may also be generated and sold or used in other processes. With particular reference to FIG. 6, such a fuel cell 605 may receive output from the purification portion 535 of the system and provide energy therefrom to the hydrocarbon reactor 100.

[0039] Figure 7 illustrates an isolation portion of a system 700 for processing hydrocarbon gases according to some embodiments. The isolation portion may be used with other systems, such as the systems illustrated in Figures 5, 6, and 7. Indeed, the various embodiments provided herein may be substituted, modified, and otherwise combined.

[0040] Reactor fluid inlet valve 705, outlet valve 710, and transfer valve 715 can maintain the flow rates into and out of the reactor. A filter, skimmer, or other separator can receive fluid from outlet valve 710 or transfer valve 715 and provide a first portion of the carbon (e.g., low density solids) for sequestration. Other material can pass to settling tank 420. The settling tank can receive other fluids, including conductive liquids, from the reactor or other sources. Settling tank 420 can provide material to a cooler 740 connected in series with a water pump 455 or a cyclone 745 (e.g., a hydrocyclone) to densify the carbon, which can then be sequestrated.

[0041] The illustrated systems 400, 500, 600, 700 are not intended to be limiting, and various elements may be added, omitted, substituted, or modified. For example, a steam washing drum may be interposed from the conductive liquid source through a solids settling tank 420 and may return a portion of the vapor or liquid to the KO drum 440. A condenser 430 may be interposed between the steam washing drum and the KO drum 440. A heat exchanger may reduce the temperature of the conductive liquid and return the cooled conductive liquid to the reactor 100. Some embodiments may omit the flare and include a collection line for all or all non-H2 gases.

[0042] Figure 8 shows yet another cross-sectional view of a hydrocarbon reactor 100, according to some embodiments. The lower electrode 160 can feed a hydrocarbon gas along the same flow path 140 as shown in Figure 4. The upper electrode 110 can contain a conductive liquid 125. For example, the reactor of Figure 8 can be the same as the reactor of Figure 4, where the surfaces of both electrodes 110, 160 contain a conductive liquid, such as molten metal.

[0043] 9A shows a cross-sectional view of a hydrocarbon reactor, according to some embodiments. A gas injection port 905 in the upper electrode 110 supplies hydrocarbon gas to the reactor body 940. The gas injection port 905, like other ports herein, can receive various amounts or pressures of gas depending on various reactor geometries. For example, in some embodiments, the gas injection port 905 receives between 0.5 and 20 standard liters per minute (SLPM) of hydrocarbon gas. A dielectric sheath 130 electrically isolates the upper electrode 110 from the reactor body 940.

[0044] The first conductive liquid inlet port 120A is configured to receive a conductive liquid (not shown) and pass the conductive liquid along the outer wall (e.g., sidewall 935) of the reactor. A liquid channel 910 inside the reactor can swirl the liquid tangentially along its sidewall 935. The first conductive liquid inlet port 120A can receive the conductive liquid at a rate of about 0.1-20 SLPM. The second conductive liquid inlet port 120B is configured to receive a conductive liquid for downward electrode flow and cooling, at least a portion of which can be evaporated or ionized in the reactor. The second conductive liquid inlet port 120B can receive the conductive liquid at a rate of about 0-100 standard cubic centimeters per minute (SCCM).

[0045] In some embodiments, the chamber may include various portions that are selectively coupled together, such as by retaining pins 920 as shown. Removal of the retaining pins may allow the reactor to be opened (e.g., for servicing, such as periodic decontamination). A plurality of permanent magnets 925 are disposed around the sidewall 935 of the reactor. The plurality of permanent magnets 925 may generate an inter-reactor magnetic field of about 100 Gauss to 5000 Gauss. In various embodiments, stronger magnets, weaker magnets, or variable magnets (e.g., electromagnets) may be used. The magnets 925 may combine with an electric field to swirl the plasma, thereby improving the efficiency of the reactor through increased reaction. The magnetic field may reduce blow-by and increase the amount of non-thermal plasma. A water outlet valve 915 may release water from the reactor. Now referring to FIG. 9B, an isometric view of the hydrocarbon reactor of FIG. 9A is provided, according to some embodiments. A gas outlet valve 930 may allow gas to be removed from the reactor to control its pressure or to harvest the gas. The gas may be purified (e.g., H2 enriched) relative to the hydrocarbon gas input to the reactor.

[0046] The following are representative of other examples that include potential embodiments of the disclosed approach and are not intended to be limiting in any way:

[0047] Embodiment A1: A multiphase non-equilibrium plasma hydrocarbon reactor comprising: a first electrode configured to receive a first conductive liquid from a first injection port and energize the first conductive liquid to a first voltage; and a second electrode positioned spaced apart from the first electrode, the second electrode configured to receive a second conductive liquid from a second injection port and energize the second conductive liquid to a second voltage such that the difference between the first voltage and the second voltage exceeds the dielectric breakdown of a gas disposed within the reactor over that distance.

[0048] Embodiment A2: The reactor of embodiment A1, further comprising a gas injection port configured to supply gas to the hydrocarbon gas reactor.

[0049] Embodiment A3: The reactor of embodiment A2, wherein the gas injection port is one of the first or second electrodes.

[0050] Embodiment A4: The reactor of any of embodiments A1 to A3, wherein the gas placed in the reactor is a non-oxidizing gas comprising a hydrocarbon.

[0051] Embodiment A5: The reactor of embodiment A4, wherein the hydrocarbon comprises natural gas.

[0052] Embodiment A6: The reactor of any of Embodiments A1-A5, wherein the dielectric sheath cooperates with the first injection port to supply the first conductive liquid to the first electrode.

[0053] Embodiment A7: The reactor of any of Embodiments A1-A6, further comprising a first exhaust vent for the gases, and an ignition source configured to ignite the exhaust gases.

[0054] Embodiment A8: The reactor of any of Embodiments A1-A7, further comprising a bypass vent configured to vent the gas prior to its introduction into the reactor.

[0055] Embodiment A9: The reactor of any of Embodiments A1-A8, further comprising a motive power generator configured to receive hydrogen generated in the reactor and generate electrical energy.

[0056] Embodiment A10: The reactor of embodiment A9, wherein the driving generator comprises at least one of a pressure swing absorption (PSA) system, a temperature swing absorption (TSA) system, a membrane purifier, or a dryer purification system.

[0057] Embodiment A11: The reactor of any of embodiments A1-A10, wherein the reactor is configured to generate radial plasma and liquid swirl along the interior surface of its sidewall.

[0058] Embodiment A12: The reactor of embodiment A11, wherein the reactor comprises a plurality of magnets disposed about the exterior surface of the side wall.

[0059] Embodiment A13: The reactor of any of Embodiments A1-A12, wherein the reactor is configured to adjust the flow rate of the first conductive liquid or the second conductive liquid based at least in part on the conductivity of the respective conductive liquid.

[0060] Embodiment B1: A plasma hydrocarbon reactor comprising: a first injection port configured to supply a first conductive liquid at a first electrode; a second injection port configured to supply a second conductive liquid at a second electrode spaced from the first electrode; and a gas injection port configured to supply a hydrocarbon gas to the plasma hydrocarbon reactor; and a system including a controller configured to generate an electric field between the first electrode and the second electrode by a power supply.

[0061] Embodiment B2: The system of embodiment B1, wherein the first injection port and the second injection port are different ports.

[0062] Embodiment B3: The system of either embodiment B1 or B2, wherein the gas injection port is one of the first electrode or the second electrode.

[0063] Embodiment B4: The system of any of Embodiments B1-B3, further comprising a plurality of magnets disposed about an exterior surface of the sidewall of the multi-phase non-equilibrium plasma hydrocarbon reactor.

[0064] Embodiment B5: The reactor of any of Embodiments B1-B4, wherein the controller is further configured to generate radial plasma swirls in combination with the electric field between the first electrode and the second electrode.

[0065] Embodiment C1: A method comprising: receiving a first conductive liquid by a hydrocarbon reactor at a first injection port; receiving a second conductive liquid by the hydrocarbon reactor at a second injection port, the second conductive liquid being separate from the first conductive liquid; receiving a hydrocarbon gas by the hydrocarbon reactor; and energizing the first conductive liquid to a first voltage and energizing the second conductive liquid to a second voltage such that a difference between the first voltage and the second voltage exceeds a dielectric breakdown of the hydrocarbon gas.

[0066] Embodiment C2: The method of embodiment C1, further comprising: receiving a conductive liquid from a reactor; separating a first portion of the conductive particles from the conductive liquid; and then injecting the separated conductive liquid into the reactor.

[0067] Embodiment C3: The method of any of Embodiments C1 or C2, further comprising: receiving a second conductive liquid from a reactor; cooling the second conductive liquid by a heat exchanger; and injecting the cooled second conductive liquid into the reactor.

[0068] For the purposes of this disclosure and unless otherwise specified, "a" or "an" means "one or more." As used herein, "about" will be understood by those of ordinary skill in the art and will vary to some extent depending on the context in which it is used. If the use of a term is not clear to those of ordinary skill in the art, "about" will mean up to plus or minus 10% of the particular term, given the context in which it is used.

[0069] References to "or" may be construed as inclusive, such that any term described using "or" may refer to either one, more than one, and all of the listed terms. Reference to at least one of a linked list of terms may be construed as an inclusive OR, referring to either one, more than one, and all of the listed terms. For example, a reference to "at least one of 'A' and 'B'" may include "A" only, "B" only, and both "A" and "B." Such references used in combination with "comprising" or other open terminology may include additional items.

[0070] All publications, patent applications, issued patents, and other documents referred to in this specification are incorporated herein by reference as if each individual publication, patent application, issued patent, or other document was specifically and individually indicated to be incorporated by reference in its entirety. Definitions contained in the texts incorporated by reference are excluded to the extent that they conflict with definitions in this disclosure.

[0071] The embodiments illustratively described herein may be suitably practiced even if any element or limitation is not specifically disclosed herein. Thus, for example, terms such as "comprising," "including," "containing," and the like, are to be interpreted expansively and without limitation. Furthermore, the terms and expressions used herein are used as terms of description and not as terms of limitation, and the use of such terms and expressions is not intended to exclude any equivalents of the features shown and described or portions thereof, but is recognized to be capable of various modifications within the scope of the claimed technology. Furthermore, the expression "consisting essentially of" is understood to include the elements specifically recited and additional elements that do not materially affect the basic and novel characteristics of the claimed technology. The expression "consisting of" excludes any elements not specified.

[0072] The present disclosure is not limited with respect to the specific embodiments described in this application, which are intended as illustrations of various aspects. As will be apparent to those skilled in the art, many modifications and variations can be made without departing from the spirit and scope thereof. Functionally equivalent compositions, devices, and processes within the scope of the present disclosure, in addition to those recited herein, will be apparent to those skilled in the art from the foregoing description. Such modifications and variations are intended to be included within the scope of the appended claims. The present disclosure is to be limited only by the terms of the appended claims, and the full scope of equivalents to which such claims are entitled. It is to be understood that the present disclosure is not limited to specific processes, reagents, compounds, compositions, or biological systems, which, of course, can vary. It is also to be understood that the terminology used herein is for the purpose of describing specific embodiments only, and is not intended to be limiting.

[0073] Furthermore, where features or aspects of the disclosure are described in terms of a Markush group, one of skill in the art will recognize that the disclosure is thereby also described in terms of any individual members or subgroups of members of the Markush group, with respect to reactor design, chemical species thereof, and the like.

[0074] As will be understood by those skilled in the art, for any and all purposes, particularly in terms of providing a written description, all ranges disclosed herein also encompass any and all possible subranges and combinations of subranges. Any recited range is fully described and can be easily recognized as being capable of dividing the same range into at least one half, one third, one quarter, one fifth, one tenth, etc. As a non-limiting example, each range discussed herein can be easily divided into a lower third, a middle third, and an upper third, etc. As will also be understood by those skilled in the art, all words such as "up to," "at least," "greater than," "less than," etc. refer to a range that includes the recited numbers and that can be subsequently divided into subranges as described above. Finally, as will be understood by those skilled in the art, a range includes individual members.

[0075] While particular embodiments have been illustrated and described, it is to be understood that changes and modifications may be made by those skilled in the art without departing from the technology in its broader aspects defined in the following claims.

Claims

1. 1. A multi-phase non-equilibrium plasma hydrocarbon reactor comprising: a first electrode configured to receive a first conductive liquid from a first inlet port and energize the first conductive liquid to a first voltage; and a second electrode positioned spaced from the first electrode, the second electrode configured to receive a second conductive liquid from a second inlet port and to energize the second conductive liquid to a second voltage such that the difference between the first voltage and the second voltage exceeds the dielectric breakdown of a gas disposed within the reactor over that distance; A reactor comprising:

2. 10. The reactor of claim 1 further comprising a gas injection port configured to deliver gas to the hydrocarbon gas reactor.

3. 3. The reactor of claim 2, wherein the gas injection port is in one of the first or second electrodes.

4. 2. The reactor of claim 1, wherein the gas disposed within the reactor is a non-oxidizing gas comprising a hydrocarbon.

5. 5. The reactor of claim 4, wherein the hydrocarbon comprises natural gas.

6. 2. The reactor of claim 1, wherein the dielectric sheath cooperates with the first injection port to supply the first conductive liquid to the first electrode.

7. 10. The reactor of claim 1 further comprising a first exhaust vent for the gases and an ignition source configured to ignite the exhaust gases.

8. 10. The reactor of claim 1, further comprising a bypass vent configured to vent the gas prior to its introduction into the reactor.

9. 10. The reactor of claim 1, further comprising a hydrogen-powered generator configured to receive hydrogen generated in the reactor and generate electrical energy.

10. 10. The reactor of claim 9, wherein the hydrogen-driven generator comprises at least one of a pressure swing adsorption (PSA) system, a temperature swing adsorption (TSA) system, a membrane purifier, or a dryer purification system.

11. 10. The reactor of claim 1, wherein the reactor is configured to generate radial plasma and liquid swirl along an interior surface of the sidewall.

12. 12. The reactor of claim 11, wherein the reactor comprises a plurality of magnets disposed about an exterior surface of the sidewall thereof.

13. 12. The reactor of claim 11, wherein the reactor is configured to adjust a flow rate of the first conductive liquid or the second conductive liquid based at least in part on the conductivity of the respective conductive liquid.

14. A plasma hydrocarbon reactor comprising: a first injection port configured to supply a first conductive liquid at the first electrode; a second injection port configured to supply a second conductive liquid at a second electrode remote from the first electrode; a gas injection port configured to deliver a hydrocarbon gas to the plasma hydrocarbon reactor; and a controller configured to generate an electric field between the first electrode and the second electrode via a power supply; A system including:

15. 15. The system of claim 14, wherein the first injection port and the second injection port are different ports.

16. The system of claim 14 , wherein the gas injection port is one of the first electrode or the second electrode.

17. 15. The system of claim 14, further comprising a plurality of magnets disposed about an exterior surface of the sidewall of the plasma hydrocarbon reactor, wherein the controller is further configured to generate radial plasma swirls in combination with the electric field between the first electrode and the second electrode.

18. receiving a first conductive liquid at a first injection port by a hydrocarbon reactor; receiving a second conductive liquid at a second injection port by the hydrocarbon reactor, the second conductive liquid being separate from the first conductive liquid; receiving a hydrocarbon gas by a hydrocarbon reactor; and energizing the first conductive liquid to a first voltage and energizing the second conductive liquid to a second voltage such that the difference between the first and second voltages exceeds the dielectric breakdown of the hydrocarbon gas. The method includes:

19. receiving a conductive liquid from the reactor; separating a first portion of the conductive particles from the conductive liquid; and thereafter injecting the separated conductive liquid into the reactor.

20. The method of claim 18, further comprising:

20. receiving a second conductive liquid from the reactor; cooling the second conductive liquid by a heat exchanger; and injecting a cooled second conductive liquid into said reactor; 20. The method of claim 18, further comprising:

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