Electrochemical upgrade of reduced carbon products

Abstract

Described herein is a method for reducing carbon product generation, the method comprising: contacting a gas stream with an electrolyte solution wherein the gas stream comprises carbon dioxide (CO2), thereby trapping the CO2 from the gas stream into the electrolyte solution; reducing the CO2 in the electrolyte solution to produce a first reduced carbon product; and reducing the first reduced carbon product to produce a second reduced carbon product, where the second reduced carbon product (e.g., an upgraded RCP) includes a greater number of carbon atoms than the first reduced carbon product.

Description

[0001] Cross-references

[0002] This application claims the benefit of U.S. Provisional Application No. 63 / 343,018, filed May 17, 2022, which is incorporated herein by reference in its entirety. Background Art

[0003] The electrochemical reduction of carbon dioxide ("CO2") can generate various types of reduced carbon products, including but not limited to alcohols, aldehydes, ketones, and linear, branched, and cyclic alkanes and alkenes. In some cases, the reduced carbon products can be further reduced so that additional carbon, hydrogen, and oxygen atoms (in some cases) are added to the reduced carbon products along with electrons, thereby increasing their size and energy and changing their combustion characteristics. Summary of the invention

[0004] The present disclosure provides systems and methods for electrochemically reducing carbon dioxide ("CO2") to reduced carbon products (such as fuels) and upgrading or further reducing the reduced carbon products to larger products. In some cases, the upgrading of the reduced carbon products is achieved without the need for high temperature and / or high pressure catalysis. It is recognized herein that there is an increasing demand for efficient methods of upgrading reduced carbon products to larger reduced carbon products that can be used as diesel or jet fuel. The methods and systems described herein can allow the production of larger reduced carbon products without the need for high temperature or high pressure catalysis. This can significantly reduce the cost of producing larger reduced carbon products or fuels from CO2.

[0005] In one aspect, the present invention provides a method for generating reduced carbon products, the method comprising: (a) contacting a gas stream with an electrolyte solution, wherein the gas stream comprises carbon dioxide (CO2), thereby capturing CO2 from the gas stream into the electrolyte solution; (b) reducing the CO2 in the electrolyte solution to generate a first reduced carbon product; and (c) reducing a subset of the first reduced carbon products to generate a second reduced carbon product, wherein the second reduced carbon product comprises a greater number of carbon atoms than the first reduced carbon product.

[0006] In some cases, the method includes reducing CO2 using an electrochemical stack to generate a first reduced carbon product. In some cases, the method includes reducing a subset of the first reduced carbon product using an electrochemical stack to generate a second reduced carbon product. In some cases, the electrochemical stack also includes a carbon nanotube (CNT) film. In some cases, the CNT film separates the first reduced carbon product from the second reduced carbon product.

[0007] In some cases, the method further includes removing an additional subset of the first reduced carbon products from the electrochemical stack. In some cases, the method further includes recycling at least a portion of the additional subset of the first reduced carbon products to the electrochemical stack. In some cases, the method further includes controlling one or more parameters of the electrochemical stack to promote or increase the generation of the second reduced carbon product in (c).

[0008] In some cases, the one or more parameters include the pH of the electrochemical stack. In some cases, the pH of the electrochemical stack is greater than 10. In some cases, the pH of the electrochemical stack is greater than 12. In some cases, the pH of the electrochemical stack is greater than 14.

[0009] In some cases, the one or more parameters include a concentration of total inorganic carbon (TIC) in the electrochemical stack. In some cases, the concentration of TIC in the electrochemical stack is greater than 0.5 mol / L (M). In some cases, the concentration of TIC in the electrochemical stack is between about 0.5 M and 2.5 (M).

[0010] In some cases, the one or more parameters include a flow curve or flow rate of the electrolyte solution through the electrochemical stack. In some cases, the flow curve of the electrolyte solution includes laminar flow. In some cases, the Reynolds number of the laminar flow is less than 2000.

[0011] In some cases, the electrochemical stack includes a catalyst, and the one or more parameters include a particle size of the catalyst. In some cases, the particle size of the catalyst is greater than 25 nanometers (nm). In some cases, the particle size of the catalyst is between 25 nanometers (nm) and 100 nm.

[0012] In some cases, the one or more parameters include a residence time of the electrolyte solution in the electrochemical stack. In some cases, the electrochemical stack includes a catalyst.

[0013] In some cases, the one or more parameters include at least two of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include at least three of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include at least four of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow profile or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack.

[0014] In some cases, (c) includes reducing the first reduced carbon product to generate a second reduced carbon product using an additional electrochemical stack separate from the electrochemical stack. In some cases, the method further includes: (a) controlling a first set of parameters of the electrochemical stack to promote or increase generation of the first reduced carbon product in the electrochemical stack, and (b) controlling a second set of parameters of the additional electrochemical stack to promote or increase generation of the second reduced carbon product in the additional electrochemical stack.

[0015] In some cases, the electrochemical stack includes a first catalyst, and wherein the additional electrochemical stack includes a second catalyst. In some cases, the first set of parameters or the second set of parameters include at least two of the following: (a) pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack. In some cases, the first set of parameters or the second set of parameters include at least three of the following: (a) pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack. In some cases, the first set of parameters or the second set of parameters includes at least four of the following: (a) pH of the electrochemical stack or the additional electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) flow profile or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) particle size of the first catalyst or the second catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack. In some cases, the first set of parameters or the second set of parameters includes the following: (a) pH of the electrochemical stack or the additional electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) flow profile or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) particle size of the first catalyst or the second catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack.

[0016] In some cases, the electrochemical stack operates at a lower pH than the additional electrochemical stack. In some cases, the electrochemical stack has a lower total inorganic carbon (TIC) concentration than the additional electrochemical stack. In some cases, the electrolyte solution in the electrochemical stack has a lower Reynolds number than the electrolyte solution in the additional electrochemical stack. In some cases, the additional electrochemical stack is higher than the electrochemical stack. In some cases, the additional electrochemical stack is wider than the electrochemical stack. In some cases, the electrochemical stack includes a first catalyst, and wherein the additional electrochemical stack includes a second catalyst. In some cases, the particle size of the second catalyst is greater than the first catalyst. In some cases, the residence time of the electrolyte solution in the electrochemical stack is less than the residence time of the electrolyte solution in the additional electrochemical stack.

[0017] On the other hand, provided herein is a method for producing a reduced carbon product from carbon dioxide (CO2), the method comprising: (a) contacting a gas stream with an electrolyte solution, wherein the gas stream comprises CO2, thereby capturing CO2 from the gas stream into the electrolyte solution; and (b) using an electrochemical stack to reduce the CO2 in the electrolyte solution to generate a reduced carbon product, wherein one or more parameters of the electrochemical stack are selected so that the reduced carbon product has a predetermined number of carbon atoms.

[0018] In some cases, the one or more parameters include the pH of the electrochemical stack. In some cases, the pH of the electrochemical stack is greater than 10. In some cases, the pH of the electrochemical stack is greater than 12. In some cases, the pH of the electrochemical stack is greater than 14.

[0019] In some cases, the one or more parameters include a concentration of total inorganic carbon (TIC) in the electrochemical stack. In some cases, the concentration of TIC in the electrochemical stack is greater than 0.5 mol / L (M). In some cases, the concentration of TIC in the electrochemical stack is between about 0.5 M and 2.5 (M).

[0020] In some cases, the one or more parameters include a flow curve or flow rate of the electrolyte solution through the electrochemical stack. In some cases, the flow curve of the electrolyte solution includes laminar flow. In some cases, the Reynolds number of the laminar flow is less than 2000.

[0021] In some cases, the electrochemical stack includes a catalyst, and the one or more parameters include a particle size of the catalyst. In some cases, the particle size of the catalyst is greater than 25 nanometers (nm). In some cases, the particle size of the catalyst is between 25 nanometers (nm) and 100 nm.

[0022] In some cases, the one or more parameters include a residence time of the electrolyte solution in the electrochemical stack. In some cases, the electrochemical stack includes a catalyst.

[0023] In some cases, the one or more parameters include at least two of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include at least three of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include at least four of the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack. In some cases, the one or more parameters include the following: (a) pH of the electrochemical stack, (b) concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) flow profile or flow rate of the electrolyte solution through the electrochemical stack, (d) particle size of the catalyst, and (e) residence time of the electrolyte solution in the electrochemical stack.

[0024] On the other hand, the present invention provides a system for producing a reduced carbon product from carbon dioxide (CO2), the system comprising: (a) a CO2 capture unit, the CO2 capture unit being configured to contact a gas stream including CO2 with an electrolyte solution, thereby capturing CO2 from the gas stream into the electrolyte solution; (b) a first electrochemical stack fluidly connected to the CO2 capture unit, wherein the first electrochemical stack is configured to reduce the CO2 in the electrolyte solution to generate a first reduced carbon product; and (c) a second electrochemical stack fluidly connected to the first electrochemical stack, wherein the second electrochemical stack is configured to reduce at least a portion of the first reduced carbon product to generate a second reduced carbon product, and wherein the second reduced carbon product comprises a greater number of carbon atoms than the first reduced carbon product.

[0025] In some cases, the second electrochemical stack is higher than the first electrochemical stack. In some cases, the second electrochemical stack is wider than the first electrochemical stack. In some cases, the first electrochemical stack or the second electrochemical stack includes a carbon nanotube (CNT) film. In some cases, the CNT film is configured to separate one or more reduced carbon products based on size. In some cases, the system also includes a separation unit located between the first electrochemical stack and the second electrochemical stack. In some cases, the separation unit is configured to separate the first reduced carbon product from the electrolyte solution. In some cases, the separation unit is configured to guide the separated electrolyte solution to the CO2 capture unit. In some cases, the separation unit includes a carbon nanotube (CNT) film. In some cases, the system also includes a shunt unit located downstream of the second electrochemical stack. In some cases, the shunt unit is configured to separate one or more reduced carbon products based on size, thereby obtaining a smaller reduced carbon product stream and a larger reduced carbon product stream. In some cases, the shunt unit is configured to guide a smaller reduced carbon product stream to the second electrochemical stack for further upgrading. In some cases, the flow dividing unit includes a carbon nanotube (CNT) membrane.

[0026] Incorporation by reference

[0027] All publications, patents, and patent applications mentioned in this specification are incorporated herein by reference to the same extent as if each individual publication, patent, or patent application was specifically and individually indicated to be incorporated by reference. In the event that a publication and patent or patent application incorporated by reference contradicts the disclosure contained in the specification, the specification is intended to supersede and / or take precedence over any such contradictory material. BRIEF DESCRIPTION OF THE DRAWINGS

[0028] The novel features of the present invention are particularly set forth in the appended claims. A better understanding of the features and advantages of the present invention will be obtained by referring to the following detailed description which sets forth illustrative embodiments in which the principles of the present invention are utilized and the accompanying drawings (also referred to herein as "Figures"), in which:

[0029] Figure 1 A schematic diagram of a method for upgrading a reduced carbon product using an upgrading stack is illustrated, according to some embodiments.

[0030] Figure 2 Additional schematic diagrams are illustrated of methods for upgrading reduced carbon products without an upgrading stack, according to some embodiments.

[0031] Figure 3 A schematic diagram of a computer system for use with the systems and methods described herein is illustrated, according to an embodiment. DETAILED DESCRIPTION

[0032] Although various embodiments of the present invention have been shown and described herein, it will be readily understood by those skilled in the art that these embodiments are provided by way of example only. A variety of changes, modifications and substitutions may be envisioned by those skilled in the art without departing from the present invention. It should be understood that various alternatives to the embodiments of the present invention described herein may be employed.

[0033] Whenever the term "at least", "greater than", or "greater than or equal to" precedes the first value in a series of two or more values, the term "at least", "greater than", or "greater than or equal to" applies to each value in the series. For example, greater than or equal to 1, 2, or 3 is equivalent to greater than or equal to 1, greater than or equal to 2, or greater than or equal to 3.

[0034] Whenever the term "not more than," "less than," or "less than or equal to" precedes the first value in a series of two or more values, the term "not more than," "less than," or "less than or equal to" applies to every value in the series. For example, less than or equal to 3, 2, or 1 is equivalent to less than or equal to 3, less than or equal to 2, or less than or equal to 1.

[0035] As used herein, the term "about" generally means within ±1%, 5%, or 10% of a value. For example, if it is stated as "a temperature of about 100 degrees Celsius," it may imply that the temperature may be 90°C to 110°C.

[0036] As used in this specification and the appended claims, the singular forms "a," "an," and "the" include plural referents unless the content clearly dictates otherwise. It should also be noted that the term "or" is generally employed in its sense including "and / or" unless the content clearly dictates otherwise.

[0037] As used herein, the terms "C1+" and "C1+ compounds" generally refer to compounds containing one or more carbon atoms, for example, one carbon atom (C1), two carbon atoms (C2), etc. C1+ compounds include, but are not limited to, alkanes (e.g., methane, CH4), alkenes (e.g., ethylene, C2H2), alkynes, and aromatic compounds containing two or more carbon atoms. In some cases, C1+ compounds include aldehydes, ketones, esters, and carboxylic acids. Examples of C1+ compounds include, but are not limited to, methane, ethane, ethylene, acetylene, propane, propylene, butane, butene, etc. As used herein, C1+ compounds may also be referred to as reduced carbon products (RCPs) or reduced carbon materials.

[0038] As used herein, the term "unit" generally refers to a unit operation, which is a basic operation in a process. A unit operation may involve a physical change or chemical transformation, for example, separation, crystallization, evaporation, filtration, polymerization, isomerization, conversion, and other reactions. A given process may require one or more unit operations to obtain a desired product from a starting material or feedstock.

[0039] As used herein, the term "carbonaceous material" generally refers to any material comprising at least one carbon atom. In some embodiments, the carbonaceous material is carbon monoxide (CO), carbon dioxide (CO2), or a mixture of CO and CO2. The carbonaceous material can be a material derived from CO and / or CO2, such as bicarbonate or bicarbonate ion. Provided herein are systems, devices and methods for electrochemically reducing CO2 to reduced carbon products and upgrading reduced carbon products to larger products. The electrochemical reduction of CO2 (i.e., adding electrical energy in the form of chemical bonds) can produce a lot of carbon substances, including carbon monoxide, hydrocarbon gases, alcohols, aldehydes and organic acids. In addition, these reduced carbon products can be upgraded to longer chain hydrocarbons, many of which have a high potential for conversion into useful products (including transportation fuels and polymers). RCP can be upgraded to longer chain hydrocarbons by chemical reaction, electrochemical reduction or a combination thereof.

[0040] The electrochemical reduction system for converting CO2 into other chemicals may include various components required for reducing CO2. In some cases, the electrochemical reduction system may be referred to as a chemical conversion system in this article. Components may include cathodes, anodes, contactors, extractors, pumps, gas-liquid separators (e.g., microstructures or nanostructured membranes) and ion exchange membranes. In some embodiments, the electrochemical reduction system includes cathodes and anodes. In some embodiments, the electrochemical reduction system includes cathodes, anodes and ion exchange membranes. In some embodiments, the electrochemical reduction system is referred to as a stack. In some embodiments, the cathode includes a catalyst. In some cases, according to a preferred embodiment of the device, some components may be included in or excluded from the chemical reduction system. In some cases, the chemical reduction system may be a single, independent or fully integrated system that performs all processes in the electrochemical reduction of CO2. In other cases, the electrochemical reduction system may include at least two or more operably linked unit operations that jointly perform the necessary processes in the electrochemical reduction of CO2.

[0041] The electrochemical reduction system may include a cathode, an anode, and an electrolyte solution that together provide the components required to reduce carbon dioxide to other chemicals. The electrolyte may include a saline solution having an optimal ionic strength and pH for electrochemical reduction of CO or CO2. The electrolyte may include a saline solution containing bicarbonate ions. In some cases, the electrolyte may include an aqueous solution of sodium bicarbonate or potassium bicarbonate. In some cases, the bicarbonate ions may be dissociated in the presence of one or more catalysts to produce CO or CO2 molecules for the reduction reaction. Dissolution of CO or CO2 into the electrolyte solution may regenerate or maintain an optimal concentration of bicarbonate ions.

[0042] The electrochemical reduction system can be configured to operate at an optimal voltage for reducing CO or CO2 to a reduction product. The electrochemical reduction system can be arranged in a stack or series configuration to adjust the system voltage to an optimal value. The electrochemical reduction system can have an operating voltage of about 0.1 volt (V), 0.2V, 0.3V, 0.4V, 0.5V, 0.75V, 1.0V, 2.0V, 3.0V, 4.0V, 5.0V, 10V, 15V or about 20V. The electrochemical reduction system can have an operating voltage of at least about 0.1 volt (V), 0.2V, 0.3V, 0.4V, 0.5V, 0.75V, 1.0V, 2.0V, 3.0V, 4.0V, 5.0V, 10V, 15V or about 20V or higher. The electrochemical reduction system may have an operating voltage of no more than about 20 V, 15 V, 10 V, 5.0 V, 4.0 V, 3.0 V, 2.0 V, 1.0 V, 0.75 V, 0.5 V, 0.4 V, 0.3 V, 0.2 V, or about 0.1 V or less.

[0043] The anode may comprise an elemental metal such as nickel, tin or gold. The anode may comprise a screen, metal foam or other permeable structure of the selected anode material. The anode material may be in operative contact with an anion exchange membrane material or another physical separator that prevents contact with the cathode.

[0044] The cathode may include any suitable material. In some embodiments, the cathode may include a catalyst. In some embodiments, the cathode includes a film containing a catalyst. In some embodiments, the catalyst is used to reduce the carbonaceous material in the electrolyte. In some cases, the cathode may include copper nanoparticles and / or N-doped carbon nanomaterials. In some cases, the cathode may include a microstructure or nanostructure membrane material. In some cases, the cathode may include one or more catalysts for electrochemical reduction or other chemical reactions of CO or CO2. The cathode material may be in operative contact with an anion exchange membrane material or another physical separator that prevents contact with the cathode. In some cases, the distance between the cathode and the anode may be minimized to reduce resistance. In some cases, forced convection of the electrolyte between the electrodes may also reduce resistance and / or may allow a greater distance between the electrodes. In some cases, the electrodes may be in different housings. In some cases, the anode and cathode may have a minimum distance, with an ion selective membrane between them. In some cases, an ion selective membrane may not be used.

[0045] The electrochemical reduction system may include one or more extractor units. The extractor unit may include any unit operation or separation unit that selectively separates one or more chemical substances from a feed stream. In some cases, the extractor may include a membrane separator. In some cases, the extractor may include a microstructured or nanostructured membrane. In some cases, the extractor may extract one or more chemical substances derived from carbon dioxide reduction. In some cases, the extractor may extract one or more chemical substances derived from CO or CO2 reduction from an electrolyte solution. In other cases, the extractor may separate one or more chemical substances derived from subsequent reactions of the products of the electrochemical reduction of carbon dioxide.

[0046] Microstructure or nanostructure membrane can be used to selectively separate one or more chemicals from a mixture containing more than one chemical substance. Microstructure or nanostructure membrane can include one or more micron-scale or nanometer-scale material features (for example, including positive features (such as micron-scale or nanometer-scale structures) and / or negative features (such as micron-scale and nanometer-scale holes or micron-scale and nanometer-scale depressions)). In some cases, the membrane can include carbon nanotubes, carbon nanospheres, carbon nano onions, graphene-like materials or pyrolytic porous carbon materials. Microstructure or nanostructure materials embedded in substrates or materials can produce holes in structured membranes. Holes can allow certain chemicals to pass selectively. Other substrates or materials in the membrane can be selected according to material properties including rigidity, strength and conductivity. The membrane can include materials with characterized porous structures. Materials can include nanopores, mesopores and micropores. In some cases, nanopores can be characterized as having an average pore size of about 2nm or less. In some cases, mesopores can be characterized as having an average pore size between about 2nm and about 20nm. In some cases, micropores can be characterized as having an average pore size of about 20nm or more. The membrane can include a structure with an pore size within the entire pore size range (e.g., nanopores and mesopores). The membrane can include a structure with an pore size within a specific pore size classification (e.g., only mesopores). The hole can have a circular, elliptical, non-circular or irregular pore shape or pore cross-sectional profile. The pore size can be characterized as an average characteristic cross-sectional size (e.g., pore diameter or cross-sectional area). The membrane can include an average cross-sectional size of at least about 0.5nm, 1nm, 5nm, 10nm, 15nm, 20nm, 30nm, 40nm, 50nm, 100nm, 250nm, 500nm, 1 micron (μm) or at least about 5μm or larger pores (e.g., micropores or nanopores). The membrane may include pores having an average cross-sectional size of no more than about 5 μm, 1 μm, 500 nm, 250 nm, 100 nm, 50 nm, 40 nm, 30 nm, 20 nm, 15 nm, 10 nm, 5 nm, 1 nm, 0.5 nm, or less.

[0047] The membrane comprising microstructure or nanostructure material can allow one or more chemical substances to transfer across the membrane. The membrane comprising microstructure or nanostructure material can be selective to a particular species. In some cases, the membrane comprising microstructure or nanostructure material can selectively transfer CO or CO2 from a gas stream. In some cases, the membrane comprising microstructure or nanostructure material can selectively transfer gaseous ethylene or ethanol from a gas mixture. In some cases, the membrane comprising microstructure or nanostructure material can selectively transfer hydrocarbons from an aqueous liquid mixture. The membrane comprising microstructure or nanostructure material can transfer specific chemical substances by diffusion or convection mass transfer. In some cases, mass transfer can be enhanced by applying an external force or field. In certain cases, mass transfer can be driven or enhanced by applying a magnetic field or electric field. In other cases, mass transfer can be driven by a pressure gradient (e.g., vacuuming on one side of the membrane). In some cases, the selectivity of the membrane can be reversed by reversing the field or force applied. In other cases, the membrane can have a unidirectional or constant mass transfer selectivity.

[0048] The electrochemical reduction system may include one or more contactor units. The contactor unit may include any unit operation or separation unit that selectively separates one or more chemical substances from a feed stream. In some cases, the contactor may include a gas adsorption tower. In other cases, the contactor may include a filler for increasing the surface area of ​​the liquid solution and a fan for increasing the gas passage at the liquid interface. Such a contactor may share design features with a cooling tower. In other cases, the extractor may include a membrane separator. In some cases, the extractor may include a microstructure or nanostructure membrane. In some cases, the contactor may extract one or more chemical substances from the feed stream. In some cases, the contactor may extract carbon dioxide from the feed stream. In some cases, the contactor may separate CO or CO2 from the feed stream and dissolve CO or CO2 in an electrolyte solution. In some cases, the feed stream may be air. In some cases, the feed stream may be filtered before use. In some cases, such filtration may remove particulate matter and / or volatile organic materials and / or various undesirable materials. The absorption of CO or CO2 in the gas contactor may be enhanced by the presence of hydroxide ions generated in the electrochemical reduction system.

[0049] In some embodiments, the electrochemical reduction system includes a voltage source configured to supply voltage to the electrochemical reduction system. In some embodiments, while applying voltage, the carbonaceous material (e.g., bicarbonate) is reduced to a C1+ product in the electrochemical reduction system.

[0050] Various chemical products and reaction mixtures generated by electrochemical reduction of CO2 captured from an input air stream are described herein. Electrochemical reduction includes adding electrical energy (e.g., voltage) in the form of chemical bonds. Electrochemical reduction can produce carbonaceous materials comprising one or more members selected from the following: carbon monoxide, hydrocarbon gases, alkanes, olefins, alcohols, aldehydes, organic acids, and other organic molecules with different chain lengths. In some embodiments, electrochemical reduction can produce carbonaceous materials including chain lengths of 1 to 40 carbons. The products of the electrochemical reduction system can also be processed into useful products, including transportation fuels and polymers.

[0051] Various chemical products and reaction mixtures generated by electrochemical reduction of CO2 derived from a gas source are described herein. The gas source may be the atmosphere. The gas source may be any gas stream containing CO2. The chemical product may include any process stream output from a chemical treatment system, or any process stream that does not pass through other reactive processes. The reaction mixture may include any process mixture, reagent, or compound in a process stream within a chemical reactor, a reactor system, or between chemical reactors or reactor systems. The chemical products and reaction mixtures of the systems and methods described herein may include organic molecules, wherein one or more constituent carbon atoms are derived from CO2. In some cases, the chemical product or reaction mixture may only contain carbon atoms derived from CO2. In other cases, the chemical product may contain carbon atoms derived from CO2 and carbon atoms derived from other sources (e.g., biofuels). In some cases, the chemical products of the systems and methods described herein may have a unique carbon isotope signature consistent with the carbon isotope signature of CO2 derived from the atmosphere. In some cases, the chemical products and reaction mixtures of the systems and methods described herein may have a unique carbon isotope signature consistent with the carbon isotope signature of CO2 derived from a non-atmospheric source (such as the combustion of fossil fuels). The carbon isotopic signature of a chemical product or reaction mixture can be determined by 14 C: 12 C or 13 C: 12 In some cases, the isotopic signature of a chemical product or reaction mixture can be measured as the parts per thousand difference between the natural isotope ratio of carbon and the measured isotope ratio. 14 The difference between the isotope ratios of C in parts per thousand Δ 14 C can be calculated as:

[0052]

[0053] The natural isotope ratio of carbon and 13 The difference between the measured isotope ratios of C in parts per thousand Δ 13 C can be calculated as:

[0054]

[0055] The chemical product or reaction mixture may have a Δ 14 C. The chemical product or reaction mixture may have a ΔC of at least about -100‰, -10‰, 0‰, 5‰, 10‰, 20‰, 30‰, 40‰, 45‰, 50‰, or at least about 100‰ or more. 14 C. The chemical product or reaction mixture may have a ΔC of at most about -100‰, -10‰, 0‰, 5‰, 10‰, 20‰, 30‰, 40‰, 45‰, 50‰, or at most about 100‰ or less. 14 C. The chemical product or reaction mixture may have a ΔC of about -40‰, -35‰, -30‰, -28‰, -26‰, -24‰, -22‰, -20‰, -15‰, -10‰, -8‰, or about -5‰. 13 C. The chemical product or reaction mixture may have a ΔC of at least about -40‰, -35‰, -30‰, -28‰, -26‰, -24‰, -22‰, -20‰, -15‰, -10‰, -8‰, or at least about -5‰ or more. 13 C. The chemical product or reaction mixture may have a ΔC of at most about -40‰, -35‰, -30‰, -28‰, -26‰, -24‰, -22‰, -20‰, -15‰, -10‰, -8‰, or at most about -5‰ or less. 13 C. The present invention provides a 13 C is greater than -25‰ of the composition or reaction mixture. In one embodiment, Δ 13 C may correspond to the Δ of the ambient temperature from which the CO2 is captured 13 C (e.g., -8‰). 13 C may differ from the isotopic signature of products derived from, for example, fossil-based fuels or biogenic (e.g., plant-based) fuels. In plant-based fuels, 13 C levels are lower than those in the atmosphere 13 C level, Δ 13 C can be -25‰. In another embodiment, in fossil fuels (e.g., from oil, coal, etc.), Δ 13C may be even less than plant-based fuels, i.e., less than -25‰. Alternatively or in addition, the products or reaction mixtures described herein may include compositions that have no detectable sulfur, metals, and / or aromatic compounds. In one embodiment, the detectable level may refer to a composition that is at most 1%, 0.1%, 0.01%, 0.001%, 0.0001%, 0.00001%, or less by weight. The products or reaction mixtures of the present disclosure may include a hydrocarbon mixture that includes a C1+ product.

[0056] The chemical product or reaction mixture may include gaseous, liquid or solid substances. The chemical product and reaction mixture may include one or more organic compounds. The chemical product and reaction mixture may be miscible or immiscible in water. The chemical product and reaction mixture may be polar or non-polar. The chemical product and reaction mixture may be acidic, alkaline or neutral. The organic compound may include alkanes, olefins, alkynes, cycloalkanes, cycloolefins, cycloalkynes, substituted alkanes, substituted alkenes, substituted alkynes, alcohols, esters, carboxylic acids, ethers, amines, amides, aromatic compounds, heteroaromatic compounds, sulfides, sulfones, sulfates, mercaptans, aldehydes, ketones, amides and halogenated compounds. The chemical product and reaction mixture may include branched or straight chain compounds. The chemical product and reaction mixture may include oxygen, methane, ethane, ethylene, propane, butane, hexane, octane, decane, carbon monoxide, methanol, ethanol, propanol, butanol, hexanol, octanol and formate. The chemical product and reaction mixture may include organometallic compounds. The chemical products and reaction mixtures of the present disclosure may include compounds intended for consumer use or industrial use, such as fuels, solvents, additives, polymers, food additives, food supplements, pharmaceuticals, fertilizers, agricultural chemicals, coatings, lubricants, and building materials. The chemical products and reaction mixtures of the present disclosure may include precursors, components, substitutes, or substrates for products produced by further processing.

[0057] The organic compounds (e.g., C1+ products) of the present disclosure may contain one or more carbon atoms. In some cases, the organic compound may contain about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65 or about 70 carbon atoms. In some cases, the organic compound can include at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65, or about 70 or more carbon atoms. In some cases, the organic compound can include no more than about 70, 65, 60, 55, 50, 45, 40, 35, 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2 or fewer carbon atoms. The organic compounds of the present disclosure may contain one or more carbon atoms derived from CO or CO2. In some cases, the organic compound may contain about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65, or about 70 carbon atoms derived from CO or CO2. In some cases, the organic compound may contain at least about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65, or about 70 or more carbon atoms derived from CO or CO2. In some cases, the organic compound may contain no more than about 70, 65, 60, 55, 50, 45, 40, 35, 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 12, 11, 10, 9, 8, 7, 6, 5, 4, 3, 2, or fewer carbon atoms derived from CO or CO2.

[0058] In some embodiments, the C1+ product may contain from about 1 carbon atom to about 40 carbon atoms. In some embodiments, the C1+ product may contain from about 1 carbon atom to about 30 carbon atoms. In some embodiments, the C1+ product may contain from about 1 carbon atom to about 20 carbon atoms. In some embodiments, the C1+ product may contain from about 1 carbon atom to about 20 carbon atoms. In some embodiments, the C1+ product may contain from about 10 carbon atoms to about 20 carbon atoms. In some embodiments, the C1+ product may contain from about 12 carbon atoms to about 20 carbon atoms.

[0059] The chemical product or reaction mixture of the present disclosure can contain more than one chemical substance. The chemical product or reaction mixture can be a mixture of about 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95 or about 100 detectable chemical compounds. The chemical product or reaction mixture can be a mixture of at least about 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, 25, 26, 27, 28, 29, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95 or about 100 or more detectable chemical compounds. The chemical product or reaction mixture can be a mixture of no more than about 100, 95, 90, 85, 80, 75, 70, 65, 60, 55, 50, 45, 40, 35, 30, 29, 28, 27, 26, 25, 24, 23, 22, 21, 20, 19, 18, 17, 16, 15, 14, 13, 11, 10, 9, 8, 7, 6, 5, 4 or no more than about 3 or fewer detectable chemical compounds.

[0060] Chemical product of the present disclosure or reaction mixture may include specific compounds accounting for specific weight percentage or molar percentage of total chemical product or reaction mixture.For example, specific chemical product may include at least about 50wt% ethanol.In another embodiment, specific chemical product may include water that is no more than about 1wt%.In some cases, at least about 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 95%, 96%, 97%, 98%, 99% or more chemical product or reaction mixture may be specific chemical compounds based on weight or mole. In some cases, no more than about 99%, 98%, 97%, 96%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15%, or no more than about 10% or less of the chemical product or reaction mixture is a particular chemical compound based on weight or moles.

[0061] Chemical products or reaction mixtures of the present disclosure may include compounds within a specific range of molecular weight or carbon number. In some cases, at least about 10%, 15%, 20%, 25%, 30%, 35%, 40%, 45%, 50%, 55%, 60%, 65%, 70%, 75%, 80%, 85%, 90%, 95%, 96%, 97%, 98%, 99% or more of chemical products or reaction mixtures may include compounds within a specific molecular weight range or carbon number range. In some cases, no more than about 99%, 98%, 97%, 96%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15% or no more than about 10% or less of chemical products or reaction mixtures may include compounds within a specific molecular weight range or carbon number range. The chemical product or reaction mixture may include a molecular weight range of about 15 g / mol to about 30 g / mol, about 15 g / mol to about 60 g / mol, about 15 g / mol to about 100 g / mol, about 15 g / mol to about 200 g / mol, about 15 g / mol to about 400 g / mol, about 15 g / mol to about 600 g / mol, about 15 g / mol to about 1000 g / mol, about 30 g / mol to about 60 g / mol, about 30 g / mol to about 100 g / mol, about 30 g / mol to about 200 g / mol, about 30 g / mol to about 400 g / mol, about 30 g / mol to about 600 g / mol, about 30 g / mol to about 1000 g / mol, about 60 g / mol to about 200 g / mol, about 60 g / mol to about 400 g / mol, about 60 g / mol to about 600 g / mol, about 60 g / mol to about 1000 g / mol, about 100 g / mol to about 200 g / mol, about 100 g / mol to about 400 g / mol, about 100 g / mol to about 600 g / mol, about 100 g / mol to about 1000 g / mol, about 200 g / mol to about 400 g / mol, about 200 g / mol to about 600 g / mol, about 200 g / mol to about 1000 g / mol / mol, about 400 g / mol to about 600 g / mol, about 30 g / mol to about 1000 g / mol, about 30 g / mol to about 100 g / mol, about 30 g / mol to about 200 g / mol, about 30 g / mol to about 400 g / mol, about 30 g / mol to about 600 g / mol, about 400 g / mol to about 1000 g / mol, or about 600 g / mol to about 1000 g / mol.The chemical product or reaction mixture may include carbon numbers ranging from about C1 to about C2, about C1 to about C3, about C1 to about C4, about C1 to about C5, about C1 to about C6, about C1 to about C8, about C1 to about C10, about C1 to about C20, about C1 to about C30, about C1 to about C40, about C2 to about C3, about C2 to about C4, about C2 to about C5, about C2 to about C6, about C2 to about C8, about C2 to about C10, about C2 to about C20, about C2 to C30, about C2 to C40, about C3 to about C4, about C3 to about C5, about C3 to about C6, about C3 to about C8, about C3 to about C10, about C3 to about C20, about C3 to about C30, about C3 to about C40, about C3 to about C4 From about C5, from about C4 to about C6, from about C4 to about C8, from about C4 to about C10, from about C4 to about C20, from about C4 to about C30, from about C4 to about C40, from about C5 to about C6, from about C5 to about C8, from about C5 to about C10, from about C5 to about C20, from about C5 to about C30, from about C5 to about C40, from about C6 to about C8, from about C6 to about C10, from about C6 to about C20, from about C6 to C30, from about C6 to about C40, from about C8 to about C10, from about C8 to about C20, from about C8 to C30, from about C8 to C40, from about C10 to about C20, from about C10 to about C30, from about C10 to about C40, from about C20 to about C30, from about C20 to about C40, or from about C30 to about C40.

[0062] The chemical product or reaction mixture of the present disclosure may contain one or more impurities. Impurities may originate from reactant streams, reactor pollutants, decomposition or cracking products of organic compounds produced, catalyst compounds, or side reactions in electrochemical reduction systems or other chemical conversion systems described herein. The chemical product or reaction mixture may contain one or more organic impurities, such as formate or higher molecular weight alcohols. The chemical product or reaction mixture may contain carbon or non-carbon nanomaterial impurities. The chemical product or reaction mixture may contain one or more inorganic impurities from sources such as leaching and corrosion of catalyst degradation or process equipment. Inorganic impurities may include sodium, magnesium, potassium, calcium, titanium, vanadium, chromium, manganese, iron, cobalt, nickel, copper, zinc, aluminum, silicon, yttrium, zirconium, niobium, molybdenum, ruthenium, rhodium, palladium, silver, cadmium, indium, tin, antimony, tantalum, tungsten, osmium, platinum, gold, mercury and lead. Inorganic impurities may exist in an oxidized or reduced oxidation state. Inorganic impurities may exist in the form of organometallic complexes. Impurities in chemical products or reaction mixtures can be detected by any common analytical techniques, such as gas or liquid chromatography, mass spectrometry, infrared or ultraviolet-visible spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction or other methods. The detectable amount of one or more impurities can be at least about 1 part per billion (ppb), 5ppb, 10ppb, 50ppb, 100ppb, 250ppb, 500ppb, 750ppb, 1 part per million (ppm), 5ppm, 10ppm, 50ppm, 100ppm or more. The detectable amount of one or more impurities can be no more than about 100ppm, 50ppm, 10ppm, 5ppm, 1ppm, 750ppb, 500ppb, 250ppb, 100ppb, 50ppb, 10ppb, 5ppb or no more than about 1ppb or less.

[0063] Chemical product can have specific purity level.In some cases, chemical product can have enough purity to reach specific grade or standard.Chemical product can be ACS grade, reagent grade, USP grade, NF grade, laboratory grade, refined grade or technical grade.The purity of chemical product can exceed azeotropic composition, for example, ethanol>95%.Gaseous chemical product as described herein can have about N1.0, N2.0, N3.0, N4.0, N5.0, N6.0 or higher purity level.Chemical product can reach the purity level of determined international standard.For example, ASTM D-1152 / 97 standard of methanol purity.

[0064] In some cases, the chemical product or reaction mixture from the electrochemical reduction system may not contain detectable amounts of certain impurities. In some cases, the chemical product or reaction mixture may not contain detectable amounts of biomolecules or derivatives thereof. The chemical product or reaction mixture may not include detectable amounts of lipids, carbohydrates, proteins, nucleic acids, amino acids, spores, bacteria, viruses, protozoa, fungi, animal or plant cells, or any components thereof.

[0065] The electrochemical reduction system can capture CO2 and convert CO2 into reduced carbon products. In one embodiment, the system can be introduced into an air stream containing CO2. In some embodiments, the input air stream containing CO2 can interact with an electrolyte solution. In some embodiments, the electrolyte solution contains water. In some embodiments, the interaction between the input air stream containing CO2 and the electrolyte solution occurs in a contactor. In some cases, the interaction between the input air stream containing CO2 and the electrolyte solution may result in the capture of CO2 in the electrolyte. In some embodiments, the capture of CO2 can occur as adsorption of CO2 on the electrolyte or absorption of CO2 in the electrolyte. In some embodiments, the capture of CO2 can occur as a physical interaction (e.g., electrostatic interaction, adsorption, absorption) between CO2 and the electrolyte. In some embodiments, the capture of CO2 can occur as a chemical interaction between CO2 and the electrolyte. In some embodiments, the captured CO2 molecules can be in the form of bicarbonate ions. For example, an air stream containing CO2 can interact with water to produce carbonic acid, which can be further dissociated into bicarbonate ions and hydronium ions (e.g., H + 、H3O + or protons), as shown in the following reaction scheme: CO2+H2O→H2CO3→HCO3 - +H + .

[0066] In such embodiments, the generation of bicarbonate ions and hydronium ions can reduce the pH of the electrolyte solution (e.g., increase the acidity). In some embodiments, CO2 can be transported to a separate chamber or compartment while being captured in the electrolyte solution. In some embodiments, CO2 is reduced in the separate chamber. In some embodiments, captured CO2 molecules (e.g., bicarbonate ions) can be directly reduced in the presence of a voltage to produce a reduced carbon product. In some cases, the captured CO2 may not need to be released (e.g., desorbed) from the captured CO2 material before being reduced to the reduced carbon product. For example, the captured CO2 can be a bicarbonate ion, and the bicarbonate ion can be directly reduced to the reduced carbon product without the need for an additional step to desorb CO2 from the bicarbonate ion. In one embodiment, CO2 captured in the form of bicarbonate can be reduced to ethanol in the presence of a voltage according to the following reaction scheme: 2HCO3 - +9H + +9e - →CH3CH2OH+5OH - .

[0067] The reduced carbon product can include alcohol, aldehyde, alkene, alkane, acid, ketone or its combination.Alcohol can include methanol, ethanol, propanol, isopropanol, butanol, isobutanol, tert-butyl alcohol, amyl alcohol, isoamyl alcohol, hexanol, isohexanol or any other straight or branched alcohol.Aldehyde can include formaldehyde, acetaldehyde, propionaldehyde, isopropanal, butyraldehyde, isobutyraldehyde or any other straight or branched aldehyde.Alkene or alkane can be straight or branched alkene or alkane.In some embodiments, alkene or alkane include length for at least 1 carbon, 2 carbons, 3 carbons, 4 carbons, 5 carbons, 6 carbons, 7 carbons, 8 carbons, 9 carbons, 10 carbons, 11 carbons, 12 carbons, 13 carbons, 14 carbons, 15 carbons, 16 carbons, 17 carbons, 18 carbons, 19 carbons, 20 carbons, 30 carbons, 40 carbons or more alkyl chains. In some embodiments, the reduced carbon product (e.g., RCP) can also be reduced in the presence of voltage and / or electrolyte to form additional reduced carbon products (e.g., upgraded RCP). In some embodiments, the RCP comprising amine, hydride, alkyne, olefin, or cyclic functional groups can be further converted to an upgraded RCP that no longer comprises one or more original functional groups.

[0068] In some embodiments, the electrochemical system is configured to produce alkanes, olefins, or combinations thereof. In some embodiments, the electrochemical system produces alkanes, olefins, alcohols (e.g., compounds comprising one or more hydroxyl groups), ketones, aldehydes, or combinations thereof. In some cases, aldehydes, ketones, and alcohols may undergo secondary reactions (e.g., further reactions) to produce upgraded RCPs.

[0069] In some embodiments, the conversion of CO2 to ethanol and hydroxide ions is according to the following chemical reaction, wherein CO2 and HCO 3- In equilibrium in the solution: 2CO2+9H2O+12e-→C2H5OH+12OH-.

[0070] In some embodiments, the generation of hydroxide ions increases the pH of the solution (e.g., decreases acidity or increases alkalinity). In some embodiments, applying a voltage to the captured CO2 solution can convert at least about 40%, 50%, 60%, 70%, 80%, 90%, 95%, 98%, 99%, or 100% of the captured CO2 into reduced carbon products.

[0071] The electrochemical conversion system may include one or more unit operations for separation. The separation unit operation may include a distillation column, a reactive distillation column, a gas absorption column, a stripping column, an additional catalytic operation such as a catalyst-filled column, a flash tank, a humidifier, a leaching unit, a liquid-liquid extraction unit, a dryer, an adsorption system, an ion exchange column, a membrane separation unit, a filtration unit, a precipitation unit, and a crystallization unit. In some embodiments, the separation unit includes a gas adsorption column. In some embodiments, the separation unit includes an adsorption system. In some embodiments, the separation unit includes a membrane. The chemical conversion system may include one or more unit operations for heat transfer. The heat transfer unit operation may include a hooded heater, a cartridge heater, a belt heater, a pad heater, a resistive heater, a radiant heater, a fan heater, a shell and tube heat exchanger, a plate heat exchanger, an extended surface heat exchanger, a scraped surface heat exchanger, a condenser, a vaporizer, and an evaporator. The chemical conversion system may include one or more unit operations for fluid transport. The fluid transport device may include pipes, tubes, fittings, valves, pumps, fans, blowers, compressors, agitators, mixers, and mixers. The pumping equipment may be operated at a pressure above atmospheric pressure or used to draw a vacuum. The chemical conversion system may include one or more chemical reaction units in addition to the electrochemical reduction reactor. The chemical reaction unit may include a plug flow reactor, a continuous stirred tank reactor, a packed bed column, a fluidized bed reactor, and a batch reactor. Chemical reactors may be used for a variety of upgrades and conversions, including dehydrogenation, hydrogenation, cracking, dehydration, decarboxylation, carboxylation, amination, deamination, alkylation, dealkylation, oxidation, reduction, polymerization, and depolymerization.

[0072] The chemical conversion system may include one or more electrochemical reduction units (e.g., a stack). In some embodiments, the chemical conversion system includes one stack. In some embodiments, the chemical conversion system includes two or more stacks. In some embodiments, the stack is used to generate RCP and / or upgrade RCP. For example, in a system including one stack, RCP can be generated in the stack while applying a voltage, and at least a portion of the RCP can be recycled back to the stack for upgrading (e.g., to a larger RCP). In another embodiment, in a system including two stacks, RCP can be generated in a first stack, and at least a portion of the RCP can be directed to a second stack for upgrading (e.g., to a larger RCP).

[0073] In the electrochemical reduction of CO2, various reduced carbon products ("RCPs") can be generated, including but not limited to C1-C40 alcohols, aldehydes, ketones, and straight-chain, branched and cyclic alkanes and olefins. In some cases, allowing these reduced carbon products to remain in the electrochemical reactor can allow the reduced carbon products to expand, so that more carbon, hydrogen and oxygen atoms (in some cases) are added to the reduced carbon products together with electrons, thereby increasing their size and energy and changing their combustion characteristics. For example, ethanol can be produced as the initial RCP of the CO2 reduction reaction. By staying in the electrochemical stack for a longer period of time (e.g., in a higher stack or in a wider stack), ethanol can serve as a reactant for further reduction reactions (such as ethanol conversion to butanol), thereby producing larger, upgraded RCPs. In some embodiments, the upgraded RCP is a carbon product including at least one additional carbon atom, hydrogen atom or oxygen atom or a combination thereof from the corresponding original RCP (e.g., mother RCP). In some embodiments, the upgraded RCP includes at least one additional carbon atom from the corresponding original RCP. For example, the upgraded RCP can be dodecane, while the original RCP is butane. In some embodiments, the upgraded RCP includes at least one additional oxygen atom from the corresponding original RCP.For example, the upgraded RCP may be a C12 ketone, while the original RCP is a C10 olefin.

[0074] In some cases, upgrading the RCP includes introducing additional oxygen to the RCP (eg, hydroxyl groups). In some embodiments, an increase in the number of oxygen atoms in the RCP is associated with greater insolubility of the RCP in an aqueous phase.

[0075] In some embodiments, upgrading includes oligomerization of two or more RCPs. For example, two C2 RCPs can react during the upgrading process to produce a C4 RCP. In some embodiments, upgrading includes reacting with an additional electrolyte (e.g., bicarbonate). For example, a C3 RCP can react with bicarbonate in an electrochemical stack during the upgrading process to produce a C4 RCP.

[0076] In some cases, the reduced carbon products can be separated from the electrolyte stream and introduced into a separate electrochemical reactor where they can undergo further reduction, which can allow the reduced carbon products to expand so that more carbon, hydrogen, and oxygen atoms (in some cases) are added to the reduced carbon products along with electrons, thereby increasing their size and energy and changing their combustion characteristics. For example, ethanol can be produced as an initial RCP for a CO2 reduction reaction and directed to a second separate electrochemical reactor that can include an electrochemical stack and further reduced to butanol, thereby producing a larger RCP. For example, a mixture of C1-C15 RCPs can be produced in a first stack, where RCPs comprising 6 or more carbon atoms can be separated from the mixture by a microstructured or nanostructured membrane (e.g., a membrane comprising carbon nanotubes), and RCPs comprising 5 or fewer carbon atoms can be directed to a second stack (or recycled back to the first stack) for further reaction and upgrading.

[0077] In some embodiments, the RCP may include at least about -15,000 kilojoules per mole (kJ / mol), -14,000 kJ / mol, -13,000 kJ / mol, -12,000 kJ / mol, -11,000 kJ / mol, -10,000 kJ / mol, -9,000 kJ / mol, -8,000 kJ / mol, -7,000 kJ / mol, -6,000 kJ / mol at 298 K and constant pressure. The molar heat of combustion of: l, -5,000 kJ / mol, -4,000 kJ / mol, -3,000 kJ / mol, -2,000 kJ / mol, -1000 kJ / mol, -900 kJ / mol, -800 kJ / mol, -700 kJ / mol, -600 kJ / mol, -500 kJ / mol, -400 kJ / mol, -300 kJ / mol, -200 kJ / mol, -100 kJ / mol or less. In some embodiments, the upgraded RCP may include at least about -15,000 kilojoules per mole (kJ / mol), -14,000 kJ / mol, -13,000 kJ / mol, -12,000 kJ / mol, -11,000 kJ / mol, -10,000 kJ / mol, -9,000 kJ / mol, -8,000 kJ / mol, -7,000 kJ / mol, -6,000 kJ / mol at 298 K and constant pressure. The molar heat of combustion may be -100 kJ / mol, -500 kJ / mol, -400 kJ / mol, -300 kJ / mol, -200 kJ / mol, -100 kJ / mol or less.

[0078] In some embodiments, the RCP may include a molar heat of combustion that is greater than (e.g., not less than) the molar heat of combustion of the upgraded RCP. For example, if the molar heat of combustion of the RCP is about -1,000 kJ / mol, the heat of combustion of the corresponding upgraded RCP will be less than -1,000 kJ / mol (e.g., <-1,000 kJ / mol).

[0079] The residence time of the RCP in the electrochemical reduction system can affect the size (e.g., molar mass) of the RCP. In some embodiments, the residence time of the RCP in the stack is determined as a factor of the stack size. In some embodiments, a taller (vertical height) electrochemical reduction stack results in a longer residence time compared to a relatively shorter stack. In some embodiments, a shorter (vertical height) electrochemical reduction stack results in a shorter residence time compared to a relatively taller stack. In some embodiments, a wider (horizontal) electrochemical reduction stack results in a longer residence time compared to a relatively narrower stack. In some embodiments, a narrower (horizontal) electrochemical reduction stack results in a shorter residence time compared to a relatively wider stack.

[0080] Depending on the purpose of operating the electrochemical reduction system, it can be expected that the RCP stays in the electrochemical reduction system for a short or long period of time. For example, the goal can be to separate the RCP in the gas phase, so a shorter residence time is sufficient to produce smaller RCPs (e.g., less than 6 carbons), which can be easily evaporated. On the other hand, for example, the goal can be to produce RCPs with higher energy density (e.g., in order to increase compatibility with engines designed to run with diesel or jet fuel), so it is necessary to stay in the electrochemical reduction system for a longer time to produce longer carbon chains (e.g., higher molecular weight) RCPs. In some embodiments, a longer residence time can be completed in a single electrochemical reduction unit. In some embodiments, a longer residence time can be completed in two or more electrochemical reduction units. For example, RCP can be produced in a first electrochemical reduction unit (e.g., stacking) within a fixed amount of time and is directed to a second electrochemical reduction unit for further reduction within an additional fixed amount of time. The second electrochemical reduction unit may be referred to herein as a second electrochemical stack, an upgraded stack, an oligomerization stack, or a cyclization stack. The fixed amount of time may be the same or different.

[0081] With respect to the size and residence time of the RCP, there can be opposing objectives in operating a CO2 electrochemical reduction system. On the one hand, it can be desirable to separate the reduced carbon products in the gas phase, which works best for smaller carbon products (e.g., RCPs with fewer than 6 carbon atoms). However, it can be desirable to produce longer carbon chain products ("upgraded" RCPs) due to their increased energy density and increased compatibility with engines designed to run on diesel or jet fuels.

[0082] Continuously removing or separating out RCP can be particularly useful while operating an integrated direct air capture (DAC) and electrochemical stack system. Continuously separating and removing RCP during operation can allow a minimal amount of RCP to remain in the stream directed back to the DAC unit, a minimal amount of RCP to evaporate and be lost to the air during additional capture of CO2, and can allow for the production of larger (e.g., higher molecular weight) RCPs by additional electrochemical reduction. Disclosed herein are systems and methods for continuously removing (or separating) RCPs so as to minimize the amount of RCP lost to the air while also producing larger RCPs.

[0083] In some embodiments, one or more parameters of the electrochemical stack system can be adjusted to upgrade the RCP. In some embodiments, pH, total inorganic carbon (TIC), flow rate of the electrolyte solution (with dissolved CO2), stack size, catalyst design, or a combination thereof are adjusted to produce an RCP of a desired size.

[0084] In some embodiments, the pH of the stack, the TIC in the stack, the flow of the electrolyte in the stack, the stack size, or the catalyst design are adjusted to produce an RCP of the desired size. In some embodiments, at least two of the following parameters are adjusted to produce an RCP of the desired size: the pH of the stack, the TIC in the stack, the flow of the electrolyte in the stack, the stack size, and the catalyst design. In some embodiments, at least three of the following parameters are adjusted to produce an RCP of the desired size: the pH of the stack, the TIC in the stack, the flow of the electrolyte in the stack, the stack size, and the catalyst design. In some embodiments, all of the following parameters are adjusted to produce an RCP of the desired size: the pH of the stack, the TIC in the stack, the flow of the electrolyte in the stack, the stack size, and the catalyst design. In some embodiments, not adjusting any parameter of the stack may not result in further upgrading of the RCP. For example, recycling ethanol (e.g., C2 alcohol) produced as RCP back to the same stack or a different stack with the same conditions may produce only ethanol.

[0085] The pH of the electrochemical stack can be adjusted or selected to adjust the characteristics or molecular weight of the RCP. The pH of the stack can be adjusted by adding an acidic solution or an alkaline solution to the stack. The pH of the stack can be adjusted by adding an electrolyte solution to the stack or reducing the electrolyte solution from the stack. In some embodiments, the electrochemical stack is operated at a pH of about 10 to about 15. In some embodiments, the electrochemical stack is operated at a pH of about 10, about 11, about 12, about 13, about 14 or about 15. In some embodiments, the electrochemical stack is operated at a pH of at least 10. A specific pH can be selected to adjust the characteristics or molecular weight of the RCP. For example, a stack operated at a higher pH can produce an RCP with a larger amount of carbon compared to a stack with a relatively lower pH. Operating the pH of the stack at an increased pH, alone or in combination with adjusting at least one other parameter of the stack, can result in an upgraded RCP (or an RCP with more than, for example, 12 carbon atoms).

[0086] In some embodiments, the total inorganic carbon within the electrochemical stack can be selected to adjust the characteristics or molecular weight of the RCP. In some cases, the TIC in the electrochemical stack is from about 0.5 mol / L (M) to about 2.5M. In some cases, the TIC in the electrochemical stack is about 0.5M to about 1M, about 0.5M to about 1.25M, about 0.5M to about 1.5M, about 0.5M to about 1.75M, about 0.5M to about 2M, about 0.5M to about 2.5M, about 1M to about 1.25M, about 1M to about 1.5M, about 1M to about 1.75M, about 1M to about 2M, about 1M to about 2.5M, about 1.25M to about 1.5M, about 1.25M to about 1.75M, about 1.25M to about 2M, about 1.25M to about 2.5M, about 1.5M to about 1.75M, about 1.5M to about 2M, about 1.5M to about 2.5M, about 1.75M to about 2M, about 1.75M to about 2M, or about 2M to about 2.5M. In some cases, the TIC in the electrochemical stack is about 0.5M, about 1M, about 1.25M, about 1.5M, about 1.75M, about 2M or about 2.5M. A specific pH can be selected to adjust the characteristics or molecular weight of the RCP. In some cases, a stack operated at a higher TIC can produce an RCP with a larger amount of carbon compared to a stack with a relatively lower TIC. Alone or in combination with adjusting at least one other parameter of the stack, operating the pH of the stack at an increased TIC concentration can result in an upgraded RCP (or an RCP with more than, for example, 12 carbon atoms). In some embodiments, the flow rate or flow curve of the electrolyte solution or other fluid in the entire electrochemical stack is reduced to eliminate turbulence. In some cases, the electrolyte solution has a laminar flow curve within the electrochemical stack. In some cases, the flow of the electrolyte solution in the entire electrochemical stack is characterized by a Reynolds number of about 500 to about 3,000. In some cases, the flow of the electrolyte solution throughout the electrochemical stack is characterized by a Reynolds number of about 500 to about 1,000, about 500 to about 1,500, about 500 to about 2,000, about 500 to about 2,500, about 500 to about 3,000, about 1,000 to about 1,500, about 1,000 to about 2,000, about 1,000 to about 2,500, about 1,000 to about 3,000, about 1,500 to about 2,000, about 1,500 to about 2,500, about 1,500 to about 3,000, about 2,000 to about 2,500, about 2,000 to about 3,000, or about 2,500 to about 3,000. In some cases, the flow of the electrolyte solution throughout the electrochemical stack is characterized by a Reynolds number of about 500, about 1,000, about 1,500, about 2,000, about 2,500, or about 3,000.In some cases, the flow of the electrolyte solution in the entire electrochemical stack is characterized by a Reynolds number of at most about 1,000, about 1,500, about 2,000, about 2,500, or about 3,000. The flow rate or flow curve of the electrolyte solution or other fluid in the entire electrochemical stack can be selected to adjust the characteristics or molecular weight of the RCP. In some cases, a stack operated at a lower flow rate or Reynolds number can produce an RCP with a larger amount of carbon compared to a stack with a relatively lower flow rate or Reynolds number. In some cases, a laminar flow curve can increase the contact time of the RCP with the catalyst within the electrochemical stack, thereby producing an upgraded RCP. Operating the stack under a laminar flow curve, alone or in combination with adjusting at least one other parameter of the stack, can result in an upgraded RCP (or an RCP with more than, for example, 12 carbon atoms).

[0087] In some embodiments, a catalyst is used in an electrochemical stack to promote the reduction of CO2 or to upgrade RCP. Characteristics or ingredients can be adjusted or selected to regulate the characteristics or molecular weight of RCP. For example, the size of the catalyst nanoparticles can be adjusted to increase the size of RCP. In some cases, the catalyst includes nanoparticles with a diameter of about 25nm to about 100nm. In some cases, the catalyst includes nanoparticles with a diameter of about 25nm to about 50nm, about 25nm to about 75nm, about 25nm to about 100nm, about 50nm to about 75nm, about 50nm to about 100nm, or about 75nm to about 100nm. In some cases, the catalyst includes nanoparticles with a diameter of about 25nm, about 50nm, about 75nm, or about 100nm. In some cases, the catalyst includes nanoparticles with a diameter of at least about 25nm, about 50nm, or about 75nm. In some cases, the catalyst includes nanoparticles with a diameter of at most about 50nm, about 75nm, or about 100nm. In some cases, a stack including catalysts with larger nanoparticles can produce an RCP with a greater amount of carbon than a stack including catalysts with relatively smaller nanoparticles. Adjusting the catalyst size, alone or in combination with adjusting at least one other parameter of the stack, can result in an upgraded RCP (or an RCP with more than, for example, 12 carbon atoms).

[0088] Various embodiments of a CO2 reduction system capable of continuous RCP removal while allowing for the production of larger sized carbon products are described herein. Figure 1, RCPs can be generated in an electrochemical stack and removed from the electrolyte. The RCPs can leave the stack by heating, gas stripping, adsorption, or a combination thereof before the removed electrolyte is sent back to the DAC system for further CO2 capture. The removed RCPs can be present along with some water (which is also removed from the electrolyte by the removal process) and can be directed to a second electrochemical stack for further reduction to larger RCPs. For example, a first electrochemical stack can produce a mixture of primarily C1 to C4 RCPs, which can be further reduced to C5 to C6 in a second electrochemical stack. 16 RCP.

[0089] In some cases, such as Figure 1 As depicted, an electrolyte stream 107 containing an electrolyte solution (e.g., water) for an electrochemical CO2 reduction process can be contacted with a gas containing CO2 in a direct air capture (DAC) unit 108 to produce a CO2-rich electrolyte. In some cases, the CO2-rich electrolyte contains bicarbonate. The gas containing CO2 can be air from the atmosphere and is directed to the DAC unit 108 through an inlet (not shown). In some cases, the pH, temperature, or other characteristics of the electrolyte stream 107 can be controlled to optimize the capture of CO2 from the gas containing CO2 into the electrolyte solution. In some cases, the gas containing CO2 also contains water, which can also be absorbed by the electrolyte stream.

[0090] The electrolyte stream 101 rich in CO2 can enter the first electrochemical stack 102. The electrochemical stack 102 can include a cathode, an anode, and an ion exchange membrane. Within the electrochemical stack, electrical energy (e.g., an applied voltage) can reduce the carbon in the electrolyte solution 101 to one or more types of RCP. The first electrochemical stack 102 may include a first catalyst. In some embodiments, the first catalyst includes copper, a carbon material containing defects or doping, silver palladium or nickel, or any combination thereof. The RCP produced in the first stack 102 may have fewer carbon atoms than the RCP produced in the second stack 106. Compared with the second electrochemical stack, certain parameters of the first stack 102 can be adjusted to produce a smaller RCP. Such parameters may include pH, total inorganic carbon, stack height, stack width, catalyst size, residence time, flow rate or flow curve, or any combination thereof.

[0091] The RCP-rich electrolyte stream 103 can be directed to an extraction or separation device 104. The extractor 104 can separate RCP from the electrolyte solution. RCP can be removed from the electrolyte solution by thermal stripping, gas stripping or adsorption or any combination thereof. The electrolyte solution from which RCP may have been excluded (e.g., the electrolyte after exclusion) can leave the extractor 104 as an electrolyte stream 107 and return to the DAC unit 108 to additionally capture CO2, so it can be reused in the electrochemical reduction system described herein. The electrolyte stream 107 can enter the DAC 108, where it can be used to additionally capture CO2. Continuous removal of RCP can be particularly useful so that there is no residual RCP or very little RCP in the electrolyte stream 107 directed to the DAC 108. This can prevent RCP from being lost to the air during direct air capture of CO2. In some embodiments, the electrolyte stream leaving the extractor 104 may not be reused in the electrochemical reduction system.

[0092] The reduced carbon product can leave the extractor 104 as an RCP stream 105 and enter the second electrochemical stack (upgrade stack) 106. In some cases, the RCP stream 105 includes RCPs present in water, which may have been removed from the electrolyte solution in the extractor 104. The second electrochemical stack 106 can be used to further reduce or upgrade the RCP to a larger, higher molecular weight reduced carbon product. The second electrochemical stack 106 may include a second cathode, a second anode, and a second membrane. The second electrochemical stack 106 may include a second catalyst. In some embodiments, the second catalyst includes copper, a carbon material containing defects or doping, silver palladium or nickel, or any combination thereof. In some cases, the second catalyst includes the same material as the first catalyst. In some cases, the second catalyst includes the same material as the first catalyst but in a different proportion or amount. In some embodiments, the second catalyst is used to produce a set of upgraded RCPs, which are larger (e.g., higher molecular weight) and / or cyclic. The second catalyst may include a catalyst material specifically designed to produce a desired carbon product (such as a branched or cyclic carbon molecule). Certain parameters of the second stack 106 may be adjusted to produce RCPs of larger size compared to the first electrochemical stack. Such parameters may include pH, total inorganic carbon, stack height, stack width, catalyst size, residence time, flow rate or flow profile, or any combination thereof.

[0093] The electrochemical reduction of the RCP in the second electrochemical stack 106 can be carried out in a liquid phase, a gas phase, or a mixed phase. In some cases, the reduction reaction in the second electrochemical stack 106 is carried out in a gas phase using humidified air including the RCP. In some cases, the reduction reaction in the second electrochemical stack 106 can be carried out in an aqueous phase using an electrolyte. Hydrogen can be introduced into the second electrochemical stack 106. In some cases, the introduced hydrogen is produced in the first electrochemical stack 102 and is directed to the second electrochemical stack 106. In some cases, the second electrochemical stack can be a gas phase and can include humidified air containing RCP and / or hydrogen. The temperature of the second stack 106 can be higher or lower than the first stack 102 to promote the generation of RCP of a desired size.

[0094] The upgraded RCP can leave the second electrochemical stack 106 as RCP stream 109 and enter the second separation unit 110. The second separation unit 110 can also be referred to as a splitter. Within the second separation unit 110, the upgraded RCP can be separated according to their size. Larger RCPs (e.g., carbon numbers ranging from about C to about C) can be separated by a variety of means, including, for example, steam or pervaporation (PV) separation methods using carbon nanotube ("CNT") membranes, hydrocyclones, or adsorption separations. 12 or more) with a smaller RCP (e.g., a carbon number ranging from about C1 to about C 12 ) separation. Larger RCPs may be slightly soluble or insoluble in water and may have a low vapor pressure, and therefore require a separation method different from the separation method ideally used in the separation of the RCPs produced in the first electrochemical stack. After separation, smaller (e.g., lower molecular weight) RCPs may leave the splitter 110 as stream 112 and re-enter the second electrochemical stack 106 to be further reduced. The RCPs with increased carbon number may leave the splitter 110 as stream 111 and be used or sold as a finished product, or undergo further processing. In some cases, stream 111 may be sold or used as a finished fuel product (including diesel or jet fuel).

[0095] In some cases, such as Figure 2As depicted, an electrolyte stream 209 containing an electrolyte solution (e.g., water) for an electrochemical CO2 reduction process can be contacted with a gas containing CO2 in a direct air capture (DAC) unit 210 to produce a CO2-rich electrolyte. In some cases, the CO2-rich electrolyte contains bicarbonate. The gas containing CO2 can be air from the atmosphere and is directed to the DAC unit 210 through an inlet (not shown). In some cases, the temperature or other characteristics of the electrolyte stream 209 can be controlled to optimize the capture of CO2 from the gas containing CO2 into the electrolyte solution. In some cases, the gas containing CO2 also contains water, which can also be absorbed by the electrolyte stream 209.

[0096] The CO2-rich electrolyte stream 201 can enter an electrochemical stack 202. The electrochemical stack 202 can include a cathode, an anode, and a membrane, and within the electrochemical stack, electrical energy (e.g., an applied voltage) can reduce the carbon in the electrolyte solution 201 to one or more types of RCP. The residence time of the CO2-rich electrolyte stream within the electrochemical stack 202 can be increased to produce a greater RCP. For example, increasing the residence time within the electrochemical stack can result in, for example, a carbon number greater than C 12 In some embodiments, one or more parameters of the electrochemical stack 202 may be adjusted to upgrade the RCP. In some embodiments, pH, total inorganic carbon (TIC), flow rate of the electrolyte solution (with dissolved CO2), stack size, catalyst design, or a combination thereof are adjusted to produce an RCP of a desired size.

[0097] In some cases, allowing the RCP to remain within the electrochemical stack 202 can allow it to expand by adding carbon, hydrogen, and oxygen atoms. The expanded RCP can have different combustion characteristics compared to a relatively smaller RCP. The electrochemical stack 202 may include a catalyst. In some embodiments, the first catalyst includes copper, a carbon material containing defects or doping, silver palladium, or nickel, or any combination thereof.

[0098] The RCP-rich electrolyte stream 203 can be directed to an extractor or separation device 204. The extractor 204 can separate the RCP from the electrolyte solution. The RCP can be removed from the electrolyte solution by thermal stripping, gas stripping, or adsorption, or any combination thereof. The electrolyte solution from which the RCP may have been removed (e.g., the removed electrolyte) can leave the extractor 204 as an electrolyte stream 209 and return to the DAC unit 210 to additionally capture CO2, so that it can be reused in the electrochemical reduction system described herein. In some embodiments, the electrolyte stream leaving the extractor 204 may not be reused in the electrochemical reduction system.

[0099] The RCP can leave the extractor 204 as an RCP stream 205 and enter the separation unit 206. The second separation unit 206 can also be referred to as a splitter. Within the separation unit 206, the RCP can be separated according to its size. Larger RCPs can be separated from smaller RCPs in a variety of ways, including, for example, steam or pervaporation separation methods using carbon nanotube ("CNT") membranes, hydrocyclones, or adsorption separations. After separation, smaller (e.g., lower molecular weight) RCPs can leave the splitter 206 as a stream 208 and re-enter the electrochemical stack 102 to be further reduced. RCPs with an increased carbon number range can leave the splitter 206 as a stream 207 and be used or sold as a finished product, or undergo further processing. In some cases, stream 207 can be sold or used as a finished fuel product, including diesel and jet fuel.

[0100] Computer Systems

[0101] The present disclosure provides a computer system programmed to implement the method of the present disclosure. Figure 3 A computer control system 1201 is shown that is programmed or otherwise configured to control a chemical reduction system or a process within a chemical reduction system (e.g., controlling pH within an electrochemical stack, controlling the flow rate of an electrolyte). The computer control system 1201 can adjust various aspects of the method of the present disclosure, for example, methods of producing reduced carbon products or monitoring potentially hazardous operating conditions. The computer system 1201 can be implemented on a user's electronic device or a computer system remotely located relative to the electronic device. The electronic device can be a mobile electronic device.

[0102] The computer system 1201 includes a central processing unit (CPU, also referred to herein as a "processor" and "computer processor") 1205, which may be a single-core or multi-core processor, or multiple processors for parallel processing. The computer system 1201 also includes a memory or memory location 1210 (e.g., random access memory, read-only memory, flash memory), an electronic storage unit 1215 (e.g., a hard disk), a communication interface 1220 (e.g., a network adapter) for communicating with one or more other systems, and peripheral devices 1225, such as cache memory, other memory, data storage, and / or an electronic display adapter. The memory 1210, storage unit 1215, interface 1220, and peripheral devices 1225 communicate with the CPU 1205 via a communication bus (solid lines) such as a motherboard. The storage unit 1215 may be a data storage unit (or data repository) for storing data. The computer system 1201 may be operably coupled to a computer network ("network") 1230 by means of the communication interface 1220. The network 1230 may be the Internet, the Internet and / or an extranet and / or an intranet and / or an extranet in communication with the Internet. In some cases, the network 1230 is a telecommunication and / or data network. The network 1230 may include one or more computer servers that may implement distributed computing, such as cloud computing. In some cases, with the aid of the computer system 1201, the network 1230 may implement a peer-to-peer network, which may enable a device coupled to the computer system 1501 to act as a client or server.

[0103] The CPU 1205 may execute a series of machine-readable instructions, which may be embodied in a program or software. The instructions may be stored in a memory location, such as the memory 1210. The instructions may be directed to the CPU 1205, which may then program or otherwise configure the CPU 1205 to implement the methods of the present disclosure. Examples of operations performed by the CPU 1205 may include fetching, decoding, executing, and writing back.

[0104] CPU 1205 may be part of a circuit such as an integrated circuit. One or more other components of system 1201 may be included in the circuit. In some cases, the circuit is an application specific integrated circuit (ASIC).

[0105] Storage unit 1215 can store files, such as drivers, libraries, and saved programs. Storage unit 1215 can store user data, such as user preferences and user programs. In some cases, computer system 1201 can include one or more additional data storage units that are external to computer system 1201, such as located on a remote server that communicates with computer system 1201 via an intranet or the Internet.

[0106] Computer system 1201 can communicate with one or more remote computer systems via network 1230. For example, computer system 1201 can communicate with a remote computer system of a user (e.g., a user monitoring pH and temperature of an electrolyte flow). Examples of remote computer systems include personal computers (e.g., portable PCs), tablet or slate PCs (e.g., iPad, Galaxy Tab), phones, smartphones (e.g. iPhone, Android-supported devices, ) or a personal digital assistant. A user can access the computer system 1201 via the network 1230.

[0107] The methods described herein may be implemented by machine (e.g., computer processor) executable code stored in an electronic storage location of the computer system 1201 (e.g., in the memory 1210 or electronic storage unit 1215). The machine executable code or machine readable code may be provided in the form of software. During use, the code may be executed by the processor 1205. In some cases, the code may be retrieved from the storage unit 1215 and stored on the memory 1210 for access by the processor 1205. In some cases, the electronic storage unit 1215 may be excluded and the machine executable instructions may be stored on the memory 1210.

[0108] The code may be precompiled and configured for use with a machine having a processor suitable for executing the code, or may be compiled during runtime. The code may be provided in a programming language, which may be selected to enable the code to be executed in a precompiled or as-compiled manner.

[0109] Aspects of the systems and methods provided herein, such as computer system 1201, may be embodied in programming. Aspects of the present technology may be considered as "products" or "articles of manufacture", which are generally in the form of machine (or processor) executable code and / or related data carried or embodied on some type of machine-readable medium. Machine executable code may be stored in an electronic storage unit such as a memory (e.g., read-only memory, random access memory, flash memory, cloud) or a hard disk. "Storage" type media may include any or all tangible memory, processor, etc. of a computer, or its related modules, such as various semiconductor memories, tape drives, disk drives, etc., which may provide non-temporary storage for software programming at any time. All or part of the software may sometimes communicate via the Internet or various other telecommunications networks. Such communication, for example, may enable software to be loaded from one computer or processor to another, for example, from a management server or host to a computer platform of an application server. Thus, another type of medium that can carry software elements includes optical, radio, and electromagnetic waves, such as those used across physical interfaces between local devices, through wired and optical landline networks, and through various air links. Physical elements that carry such waves, such as wired or wireless links, optical links, etc., can also be considered as media that carry software. As used herein, unless restricted to non-transitory tangible "storage" media, terms such as computer or machine "readable media" refer to any medium that participates in providing instructions to a processor for execution.

[0110] Thus, machine-readable media such as computer executable code may take many forms, including but not limited to tangible storage media, carrier media, or physical transmission media. Non-volatile storage media include, for example, optical or magnetic disks, such as any storage device in any computer, such as may be used to implement a database such as shown in the accompanying drawings. Volatile storage media include dynamic memory, such as the main memory of such a computer platform. Tangible transmission media include coaxial cables; copper wire and optical fiber, including the wires that make up a bus within a computer system. Carrier transmission media may take the form of electrical or electromagnetic signals, or acoustic or light waves, such as those generated during radio frequency (RF) and infrared (IR) data communications. Thus, common forms of computer readable media include, for example, a floppy disk, a flexible disk, a hard disk, a magnetic tape, any other magnetic medium, a CD-ROM, a DVD or DVD-ROM, any other optical medium, a punched card stock tape, any other physical storage medium having a pattern of holes, a RAM, a ROM, a PROM and an EPROM, a FLASH-EPROM, any other memory chip or cartridge, a carrier wave that transmits data or instructions, a cable or link that transmits such a carrier wave, or any other medium from which a computer can read programming code and / or data. Many of these forms of computer readable media may be involved in carrying one or more sequences of one or more instructions to a processor for execution.

[0111] The computer system 1201 may include or communicate with an electronic display 1235, which includes a user interface (UI) 1240 for providing, for example, pH, flow rate, or temperature of electrolyte flow. Examples of UIs include, but are not limited to, graphical user interfaces (GUIs) and web-based user interfaces.

[0112] The methods and systems of the present disclosure may be implemented by one or more algorithms. The algorithms may be implemented by software when executed by the central processing unit 1205. The algorithm may, for example, adjust the flow rate of a gas stream including CO2 through a direct air capture unit to optimize the capture of CO2 by an electrolyte solution. As another example, the algorithm may adjust the electric field applied to the microstructured or nanostructured membrane to control the selectivity of the membrane for a particular chemical.

[0113] The methods and systems of the present disclosure may be combined with or modified by other methods and systems, such as, for example, those disclosed in U.S. Patent No. 10,590,548 and WO / 2020 / 131837 (each of which is incorporated herein by reference in its entirety).

[0114] Although preferred embodiments of the present invention have been shown and described herein, it will be apparent to those skilled in the art that these embodiments are provided by way of example only. This does not mean that the present invention is limited by the specific embodiments provided in this specification. Although the present invention has been described with reference to the foregoing description, the description and explanation of the embodiments herein are not intended to be interpreted as limiting. The section titles used herein are only for organizational purposes and should not be interpreted as limiting the subject matter. Those skilled in the art will now think of various changes, modifications and substitutions without departing from the present invention. In addition, it should be understood that all aspects of the present invention are not limited to the specific description, configuration or relative proportions proposed herein according to various conditions and variables. It should be understood that various alternatives to the embodiments of the present invention described herein can be adopted in the process of practicing the present invention. Therefore, it is expected that the present invention should also cover any such alternatives, modifications, changes or equivalents. The attached claims are intended to define the scope of the present invention, and thus cover the methods and structures and their equivalents within the scope of these claims.

Claims

1. A method for reducing carbon products, the method comprising: (a) contacting a gas stream with an electrolyte solution, wherein the gas stream comprises carbon dioxide (CO 2 ), thereby capturing the CO 2 from the gas stream into the electrolyte solution; (b) reducing the CO2 in the electrolyte solution to generate a first reduced carbon product; as well as (c) reducing a subset of the first reduced carbon products to produce second reduced carbon products, wherein the second reduced carbon products include a greater number of carbon atoms than the first reduced carbon products.

2. The method of claim 1, wherein (b) comprises reducing the CO 2 using an electrochemical stack to generate the first reduced carbon product.

3. The method of claim 2, wherein (c) comprises reducing the subset of the first reduced carbon products using the electrochemical stack to generate the second reduced carbon products. The method of claim 3 , wherein the electrochemical stack further comprises a carbon nanotube (CNT) film.

5. The method of claim 4, wherein the CNT membrane separates the first reduced carbon product from the second reduced carbon product.

6. The method of claim 3, further comprising removing an additional subset of the first reduced carbon products from the electrochemical stack.

7. The method of claim 6, further comprising recycling at least a portion of the additional subset of the first reduced carbon products to the electrochemical stack.

8. The method of claim 3, further comprising controlling one or more parameters of the electrochemical stack to promote or increase the production of the second reduced carbon product in (c).

9. The method of claim 8, wherein the one or more parameters include the pH of the electrochemical stack.

10. The method of claim 9, wherein the pH of the electrochemical stack is greater than 10. The method of claim 10 , wherein the pH of the electrochemical stack is greater than 12.

12. The method of claim 11, wherein the pH of the electrochemical stack is greater than 14.

13. The method of claim 8, wherein the one or more parameters include a concentration of total inorganic carbon (TIC) in the electrochemical stack.

14. The method of claim 13, wherein the concentration of the TIC in the electrochemical stack is greater than 0.5 mol / L (M).

15. The method of claim 14, wherein the concentration of the TIC in the electrochemical stack is between about 0.5 M and 2.5 (M).

16. The method of claim 8, wherein the one or more parameters include a flow profile or flow rate of the electrolyte solution through the electrochemical stack. The method of claim 16 , wherein the flow profile of the electrolyte solution comprises laminar flow.

18. The method of claim 17, wherein the laminar flow has a Reynolds number of less than 2000.

19. The method of claim 8, wherein the electrochemical stack comprises a catalyst, and wherein the one or more parameters comprises a particle size of the catalyst.

20. The method of claim 19, wherein the particle size of the catalyst is greater than 25 nanometers (nm).

21. The method of claim 20, wherein the particle size of the catalyst is between 25 nanometers (nm) and 100 nm.

22. The method of claim 8, wherein the one or more parameters include a residence time of the electrolyte solution in the electrochemical stack.

23. The method of claim 8, wherein the electrochemical stack comprises a catalyst.

24. A method according to claim 23, wherein the one or more parameters include at least two of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

25. A method according to claim 23, wherein the one or more parameters include at least three of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

26. A method according to claim 23, wherein the one or more parameters include at least four of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

27. A method according to claim 23, wherein the one or more parameters include: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

28. The method of claim 2, wherein (c) comprises reducing the first reduced carbon product to generate the second reduced carbon product using an additional electrochemical stack separate from the electrochemical stack.

29. The method according to claim 28, further comprising: (a) controlling a first set of parameters of the electrochemical stack to promote or increase the generation of the first reduced carbon product in the electrochemical stack, and (b) controlling a second set of parameters of the additional electrochemical stack to promote or increase the generation of the second reduced carbon product in the additional electrochemical stack.

30. The method of claim 29, wherein the electrochemical stack comprises a first catalyst, and wherein the additional electrochemical stack comprises a second catalyst.

31. A method according to claim 30, wherein the first set of parameters or the second set of parameters includes at least two of the following: (a) the pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack.

32. A method according to claim 30, wherein the first set of parameters or the second set of parameters includes at least three of the following: (a) the pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack.

33. A method according to claim 30, wherein the first set of parameters or the second set of parameters includes at least four of the following: (a) the pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack.

34. A method according to claim 30, wherein the first set of parameters or the second set of parameters includes the following: (a) the pH of the electrochemical stack or the additional electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack or the additional electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack or the additional electrochemical stack, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack or the additional electrochemical stack.

35. The method of claim 28, wherein the electrochemical stack operates at a lower pH than the additional electrochemical stack.

36. The method of claim 28, wherein the electrochemical stack has a lower total inorganic carbon (TIC) concentration than the additional electrochemical stack.

37. The method of claim 28, wherein the electrolyte solution in the electrochemical stack has a lower Reynolds number than the electrolyte solution in the additional electrochemical stack.

38. The method of claim 28, wherein the additional electrochemical stack is taller than the electrochemical stack.

39. The method of claim 28, wherein the additional electrochemical stack is wider than the electrochemical stack.

40. The method of claim 28, wherein the electrochemical stack comprises a first catalyst, and wherein the additional electrochemical stack comprises a second catalyst.

41. The method of claim 40, wherein the second catalyst has a larger particle size than the first catalyst.

42. The method of claim 28, wherein a residence time of the electrolyte solution in the electrochemical stack is less than a residence time of the electrolyte solution in the additional electrochemical stack.

43. A method for producing a reduced carbon product from carbon dioxide (CO2), the method comprising: (a) contacting a gas stream with an electrolyte solution, wherein the gas stream comprises CO2, thereby capturing the CO2 from the gas stream into the electrolyte solution; as well as (b) reducing the CO2 in the electrolyte solution using an electrochemical stack to generate a reduced carbon product, One or more parameters of the electrochemical stack are selected such that the reduced carbon product has a predetermined number of carbon atoms.

44. The method of claim 43, wherein the one or more parameters include the pH of the electrochemical stack.

45. The method of claim 44, wherein the pH of the electrochemical stack is greater than 10.

46. ​​The method of claim 45, wherein the pH of the electrochemical stack is greater than 12.

47. The method of claim 46, wherein the pH of the electrochemical stack is greater than 14.

48. The method of claim 43, wherein the one or more parameters include a concentration of total inorganic carbon (TIC) in the electrochemical stack.

49. The method of claim 48, wherein the concentration of the TIC in the electrochemical stack is greater than 0.5 mol / L (M).

50. The method of claim 39, wherein the concentration of the TIC in the electrochemical stack is between about 0.5 M and 2.5 (M).

51. The method of claim 43, wherein the one or more parameters include a flow profile or flow rate of the electrolyte solution through the electrochemical stack.

52. The method of claim 51, wherein the flow profile of the electrolyte solution comprises laminar flow.

53. The method of claim 52, wherein the laminar flow has a Reynolds number of less than 2000.

54. The method of claim 43, wherein the electrochemical stack comprises a catalyst, and wherein one or more parameters comprises a particle size of the catalyst.

55. The method of claim 54, wherein the particle size of the catalyst is greater than 25 nanometers (nm).

56. The method of claim 54, wherein the particle size of the catalyst is between 25 nanometers (nm) and 100 nm.

57. The method of claim 43, wherein the one or more parameters include a residence time of the electrolyte solution in the electrochemical stack.

58. The method of claim 57, wherein the electrochemical stack comprises a catalyst.

59. A method according to claim 43, wherein the one or more parameters include at least two of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

60. A method according to claim 43, wherein the one or more parameters include at least three of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

61. A method according to claim 43, wherein the one or more parameters include at least four of the following: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

62. A method according to claim 43, wherein the one or more parameters include: (a) the pH of the electrochemical stack, (b) the concentration of total inorganic carbon (TIC) in the electrochemical stack, (c) the flow curve or flow rate of the electrolyte solution through the electrochemical stack, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte solution in the electrochemical stack.

63. A system for producing a reduced carbon product from carbon dioxide (CO2), comprising: (a) a CO2 capture unit configured to contact a gas stream comprising the CO2 with an electrolyte solution, thereby capturing the CO2 from the gas stream into the electrolyte solution; (b) a first electrochemical stack in fluid communication with the CO2 capture unit, wherein the first electrochemical stack is configured to reduce the CO2 in the electrolyte solution to generate a first reduced carbon product; as well as (c) a second electrochemical stack in fluid communication with the first electrochemical stack, wherein the second electrochemical stack is configured to reduce at least a portion of the first reduced carbon product to generate a second reduced carbon product, and wherein the second reduced carbon product includes a greater number of carbon atoms than the first reduced carbon product.

64. The system of claim 63, wherein the second electrochemical stack is taller than the first electrochemical stack.

65. The system of claim 63, wherein the second electrochemical stack is wider than the first electrochemical stack.

66. The system of claim 63, wherein the first electrochemical stack or the second electrochemical stack comprises a carbon nanotube (CNT) film.

67. The system of claim 66, wherein the CNT membrane is configured to separate one or more reduced carbon products based on size.

68. The system of claim 63, further comprising a separation unit located between the first electrochemical stack and the second electrochemical stack.

69. The system of claim 68, wherein the separation unit is configured to separate the first reduced carbon product from the electrolyte solution.

70. The system of claim 69, wherein the separation unit is configured to direct the separated electrolyte solution to the CO2 capture unit.

71. The system of claim 68, wherein the separation unit comprises a carbon nanotube (CNT) membrane.

72. The system of claim 63, further comprising a flow splitter unit located downstream of the second electrochemical stack.

73. The system of claim 72, wherein the stream splitting unit is configured to separate one or more reduced carbon products based on size, thereby obtaining a smaller reduced carbon product stream and a larger reduced carbon product stream.

74. The system of claim 73, wherein the diversion unit is configured to direct the smaller reduced carbon product stream to the second electrochemical stack for further upgrading.

75. The system of claim 72, wherein the diversion unit comprises a carbon nanotube (CNT) membrane.

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