Electrochemical upgrading of reduced carbon products

Abstract

A method for producing a reduced carbon product, comprising contacting a gas stream with an electrolyte solution, wherein the gas stream contains carbon dioxide (CO2), thereby capturing 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 a subset of the first reduced carbon product to produce a second reduced carbon product, wherein the second reduced carbon product (e.g., upgraded RCP) contains a greater number of carbon atoms than the first reduced carbon product. A method is provided herein that includes producing a second reduced carbon product.

Description

Technical Field

[0001] Cross-reference This application claims the benefit of U.S. Provisional Application No. 63 / 343,018, filed May 17, 2022, which is hereby incorporated by reference in its entirety.

Background Art

[0002] A variety of types of reduced carbon products, including but not limited to alcohols, aldehydes, ketones, and linear, branched, and cyclic alkanes and alkenes, can be produced from the electrochemical reduction of carbon dioxide (“CO2”). In some cases, the reduced carbon products can be further reduced, such that additional carbon, hydrogen, and in some cases oxygen atoms are added to the reduced carbon products along with electrons, increasing their size and energy and changing their combustion characteristics.

Summary of the Invention

[0003] The present disclosure provides systems and methods for the electrochemical reduction of carbon dioxide (“CO2”) to reduced carbon products such as fuels, and for the upgrading or further reduction of the reduced carbon products to larger products. In some cases, the upgrading of the reduced carbon products is achieved without high temperature and / or high pressure catalysis. It is recognized herein that there is a growing need for an efficient method of upgrading reduced carbon products to larger reduced carbon products that can be used as diesel or jet fuels. The methods and systems described herein can enable 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.

[0004] In one aspect, a method for producing a reduced carbon product, comprising: (a) contacting a gas stream with an electrolyte, wherein the gas stream contains carbon dioxide (CO2), thereby capturing CO2 from the gas stream into the electrolyte; (b) reducing the CO2 in the electrolyte to produce a first reduced carbon product; and (c) reducing a subset of the first reduced carbon product to produce a second reduced carbon product, wherein the second reduced carbon product contains a greater number of carbon atoms than the first reduced carbon product. A method is provided herein that includes these steps.

[0005] Optionally, the method includes reducing CO2 using an electrochemical laminate to produce a first reduced carbon product. Optionally, the method includes reducing a subset of the first reduced carbon product using an electrochemical laminate to produce a second reduced carbon product. Optionally, the electrochemical laminate further includes a carbon nanotube (CNT) membrane. Optionally, the CNT membrane separates the first reduced carbon product from the second reduced carbon product.

[0006] Optionally, the method further includes removing an additional subset of the first reduced carbon product from the electrochemical laminate. Optionally, the method further includes recycling at least a portion of the additional subset of the first reduced carbon product to the electrochemical laminate. Optionally, the method further includes controlling one or more parameters of the electrochemical laminate to promote or increase the production of the second reduced carbon product in (c).

[0007] Optionally, the one or more parameters include the pH of the electrochemical laminate. Optionally, the pH of the electrochemical laminate is greater than 10. Optionally, the pH of the electrochemical laminate is greater than 12. Optionally, the pH of the electrochemical laminate is greater than 14.

[0008] In some cases, one or more parameters include the concentration of total inorganic carbon (TIC) in the electrochemical laminate. In some cases, the concentration of TIC in the electrochemical laminate exceeds 0.5 mol / L (M). In some cases, the concentration of TIC in the electrochemical laminate is about 0.5 M to 2.5 (M).

[0009] In some cases, one or more parameters include the flow profile or flow rate of the electrolytic solution through the electrochemical laminate. In some cases, the flow profile of the electrolytic solution includes laminar flow. In some cases, the laminar flow has a Reynolds number of less than 2000.

[0010] In some cases, the electrochemical laminate contains a catalyst, and one or more parameters include a catalyst with a certain particle size. 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 25 nanometers (nm) to 100 nm.

[0011] In some cases, one or more parameters include the residence time of the electrolytic solution in the electrochemical laminate. In some cases, the electrochemical laminate contains a catalyst.

[0012] In some cases, one or more parameters include at least two of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolyte through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte in the electrochemical laminate. In some cases, one or more parameters include at least three of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolyte through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte in the electrochemical laminate. In some cases, one or more parameters include at least four of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolyte through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte in the electrochemical laminate. In some cases, one or more parameters include (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolyte through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolyte in the electrochemical laminate.

[0013] In some cases, (c) includes using an additional electrochemical laminate separate from the electrochemical laminate to reduce a first reduced carbon product to produce a second reduced carbon product. In some cases, this further includes (a) controlling a first parameter set of the electrochemical laminate to promote or increase the production of the first reduced carbon product in the electrochemical laminate and (b) controlling a second parameter set of the additional electrochemical laminate to promote or increase the production of the second reduced carbon product in the additional electrochemical laminate.

[0014] In some cases, the electrochemical laminate includes a first catalyst, and the additional electrochemical laminate includes a second catalyst. In some cases, the first parameter set or the second parameter set includes at least two of (a) the pH of the electrochemical laminate or the additional electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate or the additional electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate or the additional electrochemical laminate, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate or the additional electrochemical laminate. In some cases, the first parameter set or the second parameter set includes at least three of (a) the pH of the electrochemical laminate or the additional electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate or the additional electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate or the additional electrochemical laminate, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate or the additional electrochemical laminate. In some cases, the first parameter set or the second parameter set includes at least four of (a) the pH of the electrochemical laminate or the additional electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate or the additional electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate or the additional electrochemical laminate, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate or the additional electrochemical laminate. In some cases, the first parameter set or the second parameter set includes (a) the pH of the electrochemical laminate or the additional electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate or the additional electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate or the additional electrochemical laminate, (d) the particle size of the first catalyst or the second catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate or the additional electrochemical laminate.

[0015] In some cases, the electrochemical laminate is operated at a lower pH than an additional electrochemical laminate. In some cases, the electrochemical laminate has a lower total inorganic carbon (TIC) concentration than an additional electrochemical laminate. In some cases, the electrolyte within the electrochemical laminate has a lower Reynolds number than the electrolyte within an additional electrochemical laminate. In some cases, an additional electrochemical laminate is taller than the electrochemical laminate. In some cases, an additional electrochemical laminate is wider than the electrochemical laminate. In some cases, the electrochemical laminate includes a first catalyst and the additional electrochemical laminate includes a second catalyst. In some cases, the particle size of the second catalyst is larger than that of the first catalyst. In some cases, the residence time of the electrolyte within the electrochemical laminate is shorter than the residence time of the electrolyte within an additional electrochemical laminate.

[0016] In another aspect, a method for producing a reduced carbon product from carbon dioxide (CO2) includes: (a) contacting a gas stream with an electrolyte, wherein the gas stream contains CO2, thereby capturing CO2 from the gas stream into the electrolyte; and (b) using an electrochemical laminate to reduce the CO2 in the electrolyte to produce a reduced carbon product, wherein one or more parameters of the electrochemical laminate are selected such that the reduced carbon product has a predetermined number of carbon atoms.

[0017] In some cases, the one or more parameters include the pH of the electrochemical laminate. In some cases, the pH of the electrochemical laminate exceeds 10. In some cases, the pH of the electrochemical laminate exceeds 12. In some cases, the pH of the electrochemical laminate exceeds 14.

[0018] In some cases, the one or more parameters include the concentration of total inorganic carbon (TIC) within the electrochemical laminate. In some cases, the concentration of TIC within the electrochemical laminate exceeds 0.5 mol / L (M). In some cases, the concentration of TIC within the electrochemical laminate is about 0.5 M to 2.5 (M).

[0019] In some cases, one or more parameters include the flow profile or flow rate of the electrolytic solution through the electrochemical laminate. In some cases, the flow profile of the electrolytic solution includes laminar flow. In some cases, the laminar flow has a Reynolds number of less than 2000.

[0020] In some cases, the electrochemical laminate includes a catalyst, and one or more parameters include a catalyst having a certain particle size. 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 25 nanometers (nm) to 100 nm.

[0021] In some cases, one or more parameters include the residence time of the electrolytic solution in the electrochemical laminate. In some cases, the electrochemical laminate includes a catalyst.

[0022] In some cases, one or more parameters include at least two of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate. In some cases, one or more parameters include at least three of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate. In some cases, one or more parameters include at least four of (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate. In some cases, one or more parameters include (a) the pH of the electrochemical laminate, (b) the concentration of total inorganic carbon (TIC) in the electrochemical laminate, (c) the flow profile or flow rate of the electrolytic solution through the electrochemical laminate, (d) the particle size of the catalyst, and (e) the residence time of the electrolytic solution in the electrochemical laminate.

[0023] In another aspect, there is provided a system for producing reduced carbon products from carbon dioxide (CO2), the system comprising: (a) a CO2 capture unit configured to contact a gas stream containing CO2 with an electrolyte to thereby capture CO2 from the gas stream into the electrolyte; (b) a first electrochemical laminate in fluid communication with the CO2 capture unit and configured to reduce CO2 in the electrolyte to produce a first reduced carbon product; and (c) a second electrochemical laminate in fluid communication with the first electrochemical laminate, the second electrochemical laminate being configured to reduce at least a portion of the first reduced carbon product to produce a second reduced carbon product, the second reduced carbon product containing a greater number of carbon atoms than the first reduced carbon product.

[0024] In some cases, the second electrochemical laminate is taller than the first electrochemical laminate. In some cases, the second electrochemical laminate is wider than the first electrochemical laminate. In some cases, the first electrochemical laminate or the second electrochemical laminate includes a carbon nanotube (CNT) membrane. In some cases, the CNT membrane is configured to separate one or more reduced carbon products based on size. In some cases, the system further comprises a separation unit disposed between the first electrochemical laminate and the second electrochemical laminate. In some cases, the separation unit is configured to separate the first reduced carbon product from the electrolyte. In some cases, the separation unit is configured to direct the separated electrolyte to the CO2 capture unit. In some cases, the separation unit includes a carbon nanotube (CNT) membrane. In some cases, the system further comprises a splitting unit disposed downstream of the second electrochemical laminate. In some cases, the 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. In some cases, the splitting unit is further configured to direct the smaller reduced carbon product stream to the second electrochemical laminate for further upgrading. In some cases, the splitting unit includes a carbon nanotube (CNT) membrane.

[0025] Incorporation by reference All publications, patents, and patent applications mentioned in this specification are hereby incorporated by reference into this specification to the same extent as if each individual publication, patent, or patent application was specifically and individually indicated to be incorporated by reference. To the extent that the incorporated publications and patents or patent applications conflict with the disclosure contained herein, this specification is intended to supersede and / or prevail over such conflicting material.

[0026] The novel features of the invention are set forth in detail in the appended claims. A better understanding of the features and advantages of the invention will be obtained from the following detailed description, which illustrates exemplary embodiments in which the principles of the invention are utilized, and from the accompanying drawings (also referred to herein as "Figure" and "FIG.").

Brief Description of the Drawings

[0027]

Figure 1

Figure 2

Figure 3

Modes for Carrying Out the Invention

[0028] Although various embodiments of the invention have been shown and described herein, it will be apparent to those skilled in the art that such embodiments are provided by way of example only. A person skilled in the art can make numerous variations, changes, and substitutions without departing from the invention. It should be understood that various alternative forms to the embodiments of the invention described herein may be used.

[0029] When the terms "at least", "greater than", or "above" are in front of the first numerical value of a series of two or more numerical values, the terms "at least", "greater than", or "above" always apply to each numerical value of that series of numerical values. For example, 1 or more, 2, or 3 is equal to 1 or more, 2 or more, or 3 or more.

[0030] When the terms "no more than", "less than", or "less than or equal to" are in front of the first numerical value of a series of two or more numerical values, the terms "no more than", "less than", or "less than or equal to" always apply to each numerical value of that series of numerical values. For example, 3 or less, 2, or 1 is equivalent to 3 or less, 2 or less, or 1 or less.

[0031] As used herein, the term "about" generally refers to within ±1% of 10% of the value, within 5%. For example, when described as "a temperature of about 100 degrees Celsius", it can be implied that the temperature can be 90°C to 110°C.

[0032] As used in this specification and the appended claims, the singular forms "a", "an", and "the" include plural referents unless the context clearly indicates otherwise. Also, note that the term "or" is generally used in the sense of "and / or" unless the context clearly indicates otherwise.

[0033] As used herein, the terms "C1+" and "C1+ compound" generally refer to compounds containing one or more carbon atoms, such as 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, propene, butane, butylene, etc. C1+ compounds, when used herein, may also be referred to as reduced carbon products (RCPs) or reduced carbon materials.

[0034] As used herein, the term "unit" generally refers to a unit operation, which is a basic operation in a process. Unit operations can include physical or chemical transformations such as, for example, separation, crystallization, evaporation, filtration, polymerization, isomerization, conversion, and other reactions. A given process may require one or more unit operations to obtain the desired one or more products from one or more starting materials or one or more feedstocks.

[0035] As used herein, the term "carbon-containing material" generally refers to any material that contains at least one carbon atom. In some examples, the carbon-containing material is carbon monoxide (CO), carbon dioxide (CO2), or a mixture of CO and CO2. The carbon-containing material may be a material derived from CO and / or CO2 such as bicarbonate or bicarbonate ions. Systems, devices, and methods are provided herein for the electrochemical reduction of CO2 to reduced carbon products and the upgrading of the reduced carbon products to larger products. Many carbon species can be produced from the electrochemical reduction of CO2 (i.e., the addition of electrical energy in the form of chemical bonds), including carbon monoxide, hydrocarbon gas, alcohol, aldehyde, and organic acid. Further, these reduced carbon products can be upgraded to longer-chain hydrocarbons, many of which have a high potential to be converted into useful products such as transportation fuels and polymers. The RCP can be upgraded to longer-chain hydrocarbons by chemical reactions, electrochemical reduction, or combinations thereof.

[0036] Electrochemical reduction systems for converting CO2 to other chemical substances can include various components that may be necessary for the reduction of CO2. In some examples, the electrochemical reduction system may be referred to herein as a chemical conversion system. The components can include a cathode, an anode, a contactor, an extractor, a pump, a gas-liquid separator (e.g., a micro- or nanostructured membrane), and an ion exchange membrane. In some embodiments, the electrochemical reduction system includes a cathode and an anode. In some embodiments, the electrochemical reduction system includes a cathode, an anode, and an ion exchange membrane. In some embodiments, the electrochemical reduction system is referred to as a laminate. In some embodiments, the cathode includes a catalyst. In some examples, some components may be included in or excluded from the chemical reduction system depending on the preferred embodiment of the device. In some examples, the chemical reduction system can be a single, stand-alone, or fully integrated system that performs all processes in the electrochemical reduction of CO2. In other examples, the electrochemical reduction system may include at least two or more operably connected unit operations that collectively perform the processes necessary in the electrochemical reduction of CO2.

[0037] An electrochemical reduction system can include a cathode, an anode, and an electrolyte that collectively provide the components necessary to reduce carbon dioxide to other chemical species. The electrolyte can include an aqueous salt solution configured at an optimal ionic strength and pH for the electrochemical reduction of CO or CO2. The electrolyte can include an aqueous salt solution containing bicarbonate ions. In some examples, the electrolyte can include an aqueous solution of sodium bicarbonate or potassium bicarbonate. In some examples, the bicarbonate ions can dissociate in the presence of one or more catalysts to produce CO or CO2 molecules for the reduction reaction. The optimal concentration of bicarbonate ions can be regenerated or maintained by the dissolution of CO or CO2 in the electrolyte.

[0038] 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 laminate or in series configuration to adjust the system voltage to an optimal value. The electrochemical reduction system can have an operating voltage of about 0.1 volts (V), 0.2 V, 0.3 V, 0.4 V, 0.5 V, 0.75 V, 1.0 V, 2.0 V, 3.0 V, 4.0 V, 5.0 V, 10 V, 15 V, or about 20 V. The electrochemical reduction system can have an operating voltage of at least about 0.1 volts (V), 0.2 V, 0.3 V, 0.4 V, 0.5 V, 0.75 V, 1.0 V, 2.0 V, 3.0 V, 4.0 V, 5.0 V, 10 V, 15 V, or about 20 V, or more. The electrochemical reduction system can have an operating voltage of 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 less, or about 0.1 V, or less.

[0039] The anode may include an elemental metal such as nickel, tin, or gold. The anode can include a wire mesh, metal foam, or other permeable structure of the selected anode material. The anode material may be operably in contact with an anion exchange membrane material or another physical separator that prevents contact with the cathode.

[0040] The cathode may include any suitable material. In some embodiments, the cathode may include a catalyst. In some embodiments, the cathode includes a film including a catalyst. In some embodiments, the catalyst is used to reduce a carbon-containing material in an electrolyte. In some examples, the cathode may include copper nanoparticles and / or N-doped carbon nanomaterials. In some examples, the cathode can include a micro- or nanostructured membrane material. In some examples, the cathode may include one or more catalysts for the electrochemical reduction of CO or CO2 or other chemical reactions. The cathode material may be operably in contact with an anion exchange membrane material or another physical separator that prevents contact with the cathode. In some examples, the distance between the cathode and the anode may be minimized to reduce resistance. In some examples, forced convection of the electrolyte between the electrodes can further reduce the electrical resistance and / or allow for a greater distance between the electrodes. In some cases, the electrodes may be in different housings. In some examples, the anode and the cathode may have a minimum distance with an ion-selective membrane therebetween. In some examples, an ion-selective membrane may not be used.

[0041] 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 species from a feed stream. In some examples, the extractor can include a membrane separator. In some examples, the extractor may include a micro- or nanostructured membrane. In some cases, the extractor can extract one or more chemical species resulting from the reduction of carbon dioxide. In some examples, the extractor can extract one or more chemical species resulting from the reduction of CO or CO2 from an electrolyte. In other examples, the extractor can separate one or more chemical species resulting from subsequent reactions of the electrochemical reduction products of carbon dioxide.

[0042] Using a micro- or nano-structured membrane, selective separation of one or more chemical species from a mixture containing two or more chemical species can be performed. The micro- or nano-structured membrane can include one or more micro-scale or nano-scale material features (including, for example, positive features such as micro-scale or nano-scale structures, and / or negative features such as micro-scale and nano-scale pores or micro-scale and nano-scale depressions). In some examples, the membrane can include carbon nanotubes, carbon nanospheres, carbon nano-onions, graphene-like materials, or pyrolyzed porous carbon materials. Micro- or nano-structured materials embedded in a substrate or material can create pores within the structured membrane. The pores can enable selective passage of specific chemical species. Other substrates or materials in the membrane can be selected with respect to material properties such as rigidity, strength, and conductivity. The membrane can include materials having a characterized porous structure. The materials can include nano-pores, meso-pores, and micro-pores. In some examples, nano-pores can be characterized as having an average pore diameter of about 2 nm or less. In some cases, meso-pores can be characterized as having an average pore diameter of about 2 nm to about 20 nm. In some examples, micro-pores can be characterized as having an average pore diameter of about 20 nm or more. The membrane can include structures having pore diameters within a range of pore diameters (e.g., nano-pores and meso-pores). The membrane can include structures having pore diameters from within a specific classification of pore diameters (e.g., meso-pores only). The pores can have a circular, elliptical, non-circular or irregular pore shape or pore cross-sectional profile. The pore diameter can be characterized as an average characteristic cross-sectional dimension (e.g., pore diameter or cross-sectional area). The membrane can include pores (e.g., micro-pores or nano-pores) having an average cross-sectional dimension of at least about 0.5 nm, 1 nm, 5 nm, 10 nm, 15 nm, 20 nm, 30 nm, 40 nm, 50 nm, 100 nm, 250 nm, 500 nm, 1 micron (μm), or at least about 5 μm, or more. The membrane can include pores having an average cross-sectional dimension of 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.

[0043] A film containing a microstructured material or a nanostructured material can enable the transport of one or more chemical species in the film. The film containing a microstructured material or a nanostructured material can be selective for a particular species. In some examples, the film containing a microstructured material or a nanostructured material can selectively transfer CO or CO2 from a gas stream. In some examples, the film containing a microstructured material or a nanostructured material can selectively transfer gaseous ethylene or ethanol from a gas mixture. In some examples, the film containing a microstructured material or a nanostructured material can selectively transfer hydrocarbons from an aqueous liquid mixture. The film containing a microstructured material or a nanostructured material can transfer a particular chemical species by diffusive mass transport or convective mass transport. In some examples, the mass transfer can be enhanced by the application of an external force or an external field. In certain examples, the mass transfer can be driven or enhanced by the application of a magnetic field or an electric field. In other examples, the mass transfer can be driven by a pressure gradient (e.g., pulling a vacuum on one side of the film). In some examples, the selectivity of the film can be reversed by reversing the applied field or force. In other examples, the film can have a unidirectional or invariant mass transfer selectivity.

[0044] The electrochemical reduction system may comprise one or more contactor units. The contactor unit may include any unit operation or separation unit that selectively separates one or more chemical species from a feed stream. In some examples, the contactor may comprise a gas adsorption column. In other examples, the contactor may comprise packing for increasing the liquid solution surface area 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 examples, the extractor may include a membrane separator. In some examples, the extractor may include a micro- or nanostructured membrane. In some examples, the contactor may extract one or more chemical species from the feed stream. In some examples, the contactor may extract carbon dioxide from the feed stream. In some examples, the contactor may separate CO or CO2 from the feed stream and dissolve the CO or CO2 in an electrolyte. Optionally, the feed stream may be air. Optionally, the feed stream may be filtered prior to use. Such filtering can, optionally, remove particulate matter and / or volatile organic materials and / or various types of unwanted materials. The uptake of CO or CO2 in the gas contactor can be enhanced by the presence of hydroxide ions generated within the electrochemical reduction system.

[0045] In some embodiments, the electrochemical reduction system comprises a voltage source configured to supply a voltage to the electrochemical reduction system. In some embodiments, while a voltage is applied, a carbon-containing material (e.g., bicarbonate) is reduced to a C1+ product in the electrochemical reduction system.

[0046] Various chemical products and reaction mixtures produced via the electrochemical reduction of CO₂ captured from an input air stream are described herein. Electrochemical reduction involves the addition of electrical energy (e.g., voltage) in the form of chemical bonds. Electrochemical reduction can produce carbon species including one or more members selected from the group consisting of carbon monoxide, hydrocarbon gas, alkanes, alkenes, alcohols, aldehydes, organic acids, and other organic molecules of different chain lengths. In some embodiments, electrochemical reduction can produce carbon species having a chain length of 1 to 40 carbons. The products of the described electrochemical reduction system may be further processed into useful products such as transportation fuels and polymers.

[0047] Various chemical products and reaction mixtures produced via the 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 CO₂-bearing gas stream. Chemical products can include any process stream exiting a chemical processing system or any process stream that does not undergo a further reactive process. Reaction mixtures can include any process mixture, reagent, or compound within a chemical reactor, within the scope of a reactor system, or in a process stream between chemical reactors or reactor systems. The chemical products and reaction mixtures of the systems and methods described herein can include organic molecules in which one or more of the constituent carbon atoms are derived from CO₂. In some examples, the chemical product or reaction mixture can include only carbon atoms derived from CO₂. In other examples, the chemical product can include carbon atoms derived from CO₂ and carbon atoms from other sources (e.g., biofuels). In some examples, the chemical products of the systems and methods described herein can have a distinct carbon isotope signature that matches the carbon isotope signature of CO₂ derived from the atmosphere. In some examples, the chemical products and reaction mixtures of the systems and methods described herein can have a distinct carbon isotope signature that matches the carbon isotope signature of CO₂ derived from non-atmospheric sources such as the combustion of fossil fuels. The carbon isotope signature of the chemical product or reaction mixture is 14 C: 12 C or 13 C: 12It can be measured by the isotope ratio of C. In some examples, the isotope signature of a chemical product or reaction mixture can be measured as the difference per mill between the natural isotope ratio of carbon and the measured isotope ratio. The natural isotope ratio of carbon and 14 The measured isotope ratio Δ of 14 C and the difference per mill can be calculated as follows.

Number

Number

Number

[0048] The chemical product or reaction mixture may contain gaseous substances, liquid substances, or solid substances. The chemical product and reaction mixture may contain 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 nonpolar. The chemical product and reaction mixture may be acidic, basic, or neutral. Examples of organic compounds include alkanes, alkenes, alkynes, cycloalkanes, cycloalkenes, cycloalkynes, substituted alkanes, substituted alkenes, substituted alkynes, alcohols, esters, carboxylic acids, ethers, amines, amides, aromatics, heteroaromatics, sulfides, sulfones, sulfates, thiols, aldehydes, ketones, amides, and halogenated compounds. The chemical product and reaction mixture may contain branched or straight-chain compounds. The chemical product and reaction mixture may contain oxygen, methane, ethane, ethylene, propane, butane, hexane, octane, decane, carbon monoxide, methanol, ethanol, propanol, butanol, hexanol, octanol, and formates. The chemical product and reaction mixture may contain organometallic compounds. The chemical products and reaction mixtures of the present disclosure may include compounds intended for consumer or industrial use such as fuels, solvents, additives, polymers, food additives, food supplements, pharmaceuticals, fertilizers, pesticides, coatings, lubricants, and building materials. The chemical products and reaction mixtures of the present disclosure may further include precursors, components, substituents, or substrates for products produced by further processing.

[0049] The organic compounds of the present disclosure (e.g., C1+ products) may contain one or more carbon atoms. In some examples, 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 examples, 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. In some examples, the organic compound may contain 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 examples, 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 examples, 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 examples, the organic compound may contain 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.

[0050] In some embodiments, the C1+ product can contain from about 1 carbon atom to about 40 carbon atoms. In some embodiments, the C1+ product can contain from about 1 carbon atom to about 30 carbon atoms. In some embodiments, the C1+ product can contain from about 1 carbon atom to about 20 carbon atoms. In some embodiments, the C1+ product can contain from about 10 carbon atoms to about 20 carbon atoms. In some embodiments, the C1+ product can contain from about 12 carbon atoms to about 20 carbon atoms.

[0051] The chemical products or reaction mixtures of the present disclosure can contain two or more chemical species. 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, 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 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, 12, 11, 10, 9, 8, 7, 6, 5, 4 or less, or about 3 or less detectable chemical compounds.

[0052] The chemical product or reaction mixture of the present disclosure may contain a specific compound at a specific weight percent or mole percent of the entire chemical product or reaction mixture. For example, a specific chemical product may contain at least about 50 wt% ethanol. In another example, a specific chemical product may contain about 1 wt% or less water. In some examples, 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 the chemical product or reaction mixture may be a specific chemical compound on a weight or mole basis. In some examples, about 99%, 98%, 97%, 96%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15% or less, or about 10% or less of the chemical product or reaction mixture may be a specific chemical compound on a weight or mole basis.

[0053] The chemical product or reaction mixture of the present disclosure may include compounds within a specific range of molecular weight or carbon number. In some examples, 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 the chemical product or reaction mixture may include compounds within a specific molecular weight range or carbon number range. In some examples, about 99%, 98%, 97%, 96%, 95%, 90%, 85%, 80%, 75%, 70%, 65%, 60%, 55%, 50%, 45%, 40%, 35%, 30%, 25%, 20%, 15% or less, or about 10% or less of the chemical product or reaction mixture may include compounds within a specific molecular weight range or carbon number range.The chemical product or reaction mixture may contain a compound within 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 100 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, 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 compounds within the range of carbon numbers 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 about C30, about C2 to about 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 C4 to about C5, about C4 to about C6, about C4 to about C8, about C4 to about C10, about C4 to about C20, about C4 to about C30, about C4 to about C40, about C5 to about C6, about C5 to about C8, about C5 to about C10, about C5 to about C20, about C5 to about C30, about C5 to about C40, about C6 to about C8, about C6 to about C10, about C6 to about C20, about C6 to about C30, about C6 to about C40, about C8 to about C10, about C8 to about C20, about C8 to about C30, about C8 to about C40, about C10 to about C20, about C10 to about C30, about C10 to about C40, about C20 to about C30, about C20 to about C40, or about C30 to about C40.

[0054] The chemical products or reaction mixtures of the present disclosure may contain one or more impurities. The impurities may be derived from reaction streams, reactor contaminants, destruction or decomposition products of the produced organic compounds, catalyst compounds, or side reactions in an electrochemical reduction system or other chemical conversion systems described herein. The chemical product or reaction mixture may contain one or more organic impurities such as formates or high 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 derived from sources such as catalyst degradation or leaching and corrosion of processing equipment. The 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. The inorganic impurities may be present in an oxidized or reduced oxidation state. The inorganic impurities may be present in the form of organometallic complexes. The impurities in the chemical product or reaction mixture may be detectable by any common analytical technique such as gas or liquid chromatography, mass spectrometry, IR or UV-Vis spectroscopy, Raman spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, or other methods. One or more impurities may be detectable in an amount of at least about 1 ppb, 5 ppb, 10 ppb, 50 ppb, 100 ppb, 250 ppb, 500 ppb, 750 ppb, 1 ppm, 5 ppm, 10 ppm, 50 ppm, 100 ppm or more. One or more impurities may be detectable in an amount of about 100 ppm, 50 ppm, 10 ppm, 5 ppm, 1 ppm, 750 ppb, 500 ppb, 250 ppb, 100 ppb, 50 ppb, 10 ppb, 5 ppb or less, or about 1 ppb or less.

[0055] The chemical product can have a specific level of purity. In some examples, the chemical product can have a purity sufficient to achieve a particular grade or standard. The chemical product can be of ACS grade, reagent grade, USP grade, NF grade, laboratory grade, purified grade, or industrial grade. The chemical product can have a purity exceeding the azeotropic composition, e.g., >95% ethanol. The gaseous chemical products described herein can have a purity level of about N1.0, N2.0, N3.0, N4.0, N5.0, N6.0, or higher. The chemical product can achieve a purity level according to defined international standards. For example, the ASTM D-1152 / 97 standard for methanol purity.

[0056] In some examples, the chemical product or reaction mixture from an electrochemical reduction system may not have a detectable amount of a particular impurity. In some examples, the chemical product or reaction mixture may not have a detectable amount of a biological molecule or its derivative. The chemical product or reaction mixture may not contain a detectable amount of lipids, saccharides, proteins, nucleic acids, amino acids, spores, bacteria, viruses, protozoa, fungi, animal or plant cells, or any components thereof.

[0057] The electrochemical reduction system may capture CO2 and convert the CO2 into reduced carbon products. In one example, the system may be introduced into an air stream containing CO2. In some examples, the incoming air stream containing CO2 may interact with the electrolyte. In some embodiments, the electrolyte contains water. In some embodiments, the interaction between the incoming air stream containing CO2 and the electrolyte occurs within a contactor. In some cases, the interaction between the incoming air stream containing CO2 and the electrolyte may result in the capture of CO2 in the electrolyte. In some examples, the capture of CO2 may occur as adsorption of CO2 to the electrolyte or absorption of CO2 into the electrolyte. In some examples, the capture of CO2 may occur as a physical interaction between CO2 and the electrolyte (e.g., electrostatic interaction, adsorption, absorption). In some examples, the capture of CO2 may occur as a chemical interaction between CO2 and the electrolyte. In some examples, the captured CO2 molecules may be in the form of bicarbonate ions. For example, an air stream containing CO2 may interact with water to produce carbonic acid as shown in the following reaction scheme, which further dissociates in water to form bicarbonate ions and hydronium ions (e.g., H + , H3O + , or protons).

[0058] CO2 + H2O -> H2CO3 -> HCO3 - + H + In such examples, the generation of bicarbonate ions and hydronium ions can lower the pH of the electrolyte (e.g., increase the acidity). In some embodiments, CO2 can be transported to a separate chamber or compartment while being captured in the electrolyte. In some embodiments, CO2 is reduced within this separate chamber. In some examples, the captured CO2 molecules (e.g., bicarbonate ions) can be directly reduced in the presence of a voltage to obtain reduced carbon products. In some examples, 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 bicarbonate ions, and the bicarbonate ions can be directly reduced to the reduced carbon product without an additional step that requires desorption of CO2 from the bicarbonate ions. In one example, CO2 captured in the form of bicarbonate can be reduced to ethanol in the presence of a voltage according to the following reaction scheme.

[0059] 2HCO3 - +9H + +9e - ->CH3CH2OH+5OH - The reduced carbon product may include an alcohol, an aldehyde, an alkene, an alkane, an acid, a ketone, or a combination thereof. The alcohol may include methanol, ethanol, propanol, isopropanol, butanol, isobutanol, tert-butanol, pentanol, isopentanol, hexanol, isohexanol, or any other straight-chain or branched-chain alcohol. The aldehyde may include methanal, ethanal, propanal, isopropanal, butanal, isobutanal, or any other straight-chain or branched-chain aldehyde. The alkene may be a straight-chain or branched-chain alkene or alkane. In some embodiments, the alkene or alkane includes an alkyl chain having at least 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 30, 40, or more carbon atoms in length. In some embodiments, the reduced carbon product (e.g., RCP) can be further reduced in the presence of a voltage and / or electrolyte to form additional reduced carbon products (e.g., upgraded RCP). In some embodiments, an RCP containing an amine, hydride, alkyne, alkene, or cyclic functional group can be further converted to an upgraded RCP that no longer contains one or more of the original functional groups.

[0060] In some embodiments, the electrochemical system is configured to produce an alkane, an alkene, or a combination thereof. In some embodiments, the electrochemical system produces an alkane, an alkene, an alcohol (e.g., a compound containing one or more hydroxyl groups), a ketone, an aldehyde, or a combination thereof. In some examples, the aldehyde, ketone, and alcohol may undergo a secondary reaction (e.g., a further reaction) to produce an upgraded RCP.

[0061] In some embodiments, the conversion of CO2 to ethanol and hydroxide ions is by the following chemical reaction, where CO2 and HCO3 - are in equilibrium in the solution.

[0062] 2CO2 + 9H2O + 12e --> C2H5OH + 12OH - In some examples, the production of hydroxide ions raises the pH of the solution (e.g., decreases the acidity or increases the basicity). In some embodiments, by applying a voltage to the captured CO2 solution, at least about 40%, 50%, 60%, 70%, 80%, 90%, 95%, 98%, 99%, or 100% of the captured CO2 can be converted to reduced carbon products.

[0063] An electrochemical conversion system may include one or more unit operations for separation. Separation unit operations may include distillation columns, reactive distillation columns, gas absorption columns, stripping columns, additional catalytic operations, such as by catalytic packed columns, flash tanks, humidifiers, leaching units, liquid-liquid extraction units, dryers, adsorption systems, ion exchange columns, membrane separation units, filtration units, sedimentation units, and crystallization units. 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 can include one or more unit operations for heat transfer. Operations of heat transfer units can include mantle heaters, cartridge heaters, tape heaters, pad heaters, resistance heaters, radiant heaters, fan heaters, shell and tube heat exchangers, plate heat exchangers, extended surface heat exchangers, scraped surface heat exchangers, condensers, vaporizers, and evaporators. The chemical conversion system can include one or more unit operations for fluid transfer. Fluid transfer devices can include pipes, tubing, joints, valves, pumps, fans, blowers, compressors, agitators, agitators, and blenders. The pump device 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 separate from the electrochemical reduction reactor. Chemical reaction units can include plug flow reactors, continuous stirred tank reactors, packed bed columns, fluidized bed reactors, and batch reactors. Chemical reactors can be used for various upgrades and conversions, such as dehydrogenation, hydrogenation, cracking, dehydration, decarboxylation, carboxylation, amination, deamination, alkylation, dealkylation, oxidation, reduction, polymerization, and depolymerization.

[0064] The chemical conversion system may include one or more electrochemical reduction units (e.g., laminates). In some embodiments, the chemical conversion system includes one laminate. In some embodiments, the chemical conversion system includes two or more laminates. In some embodiments, the laminate is used to produce and / or upgrade RCP. For example, in a system comprising one laminate, RCP can be produced within the laminate while a voltage is applied, and at least a portion of the RCP can be recycled back to the laminate for upgrading (e.g., to make a larger RCP). In another example, in a system including two laminates, the RCP may be produced in the first laminate, and at least a portion of the RCP may be directed to the second laminate for upgrading (e.g., to make a larger RCP).

[0065] In the electrochemical reduction of CO2, various reduced carbon products (“RCPs”), including but not limited to C1-C40 alcohols, aldehydes, ketones, and linear, branched, and cyclic alkanes and alkenes, can be produced. In some cases, by retaining these reduced carbon products within the electrochemical reactor, their growth can be enabled, such that additional carbon, hydrogen, and in some cases oxygen atoms are added to them along with electrons, increasing their size and energy and changing their combustion characteristics. For example, ethanol can be produced as an initial RCP of the CO2 reduction reaction. By remaining within the electrochemical stack (e.g., a taller stack or a wider stack) for an extended period, ethanol can act as a reactant for further reduction reactions (such as from ethanol to butanol, etc.), thereby producing an upgraded, larger RCP. In some embodiments, the upgraded RCP is a carbon product that includes at least one additional carbon atom, hydrogen atom, or oxygen atom, or a combination thereof, from the corresponding original RCP (e.g., the parent 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 can be a C12 ketone, while the original RCP is a C10 alkene.

[0066] In some cases, upgrading the RCP includes introducing additional oxygen (e.g., a hydroxyl group) into the RCP. In some embodiments, an increase in the number of oxygen atoms in the RCP correlates with greater insolubility of the RCP in the aqueous phase.

[0067] In some embodiments, upgrading involves oligomerization of two or more RCPs. For example, two C2RCPs can react during an upgrading process to produce a C4RCP. In some embodiments, upgrading involves reacting with additional electrolyte (e.g., bicarbonate). For example, C3RCP can react with bicarbonate in an electrochemical laminate during an upgrading process to produce C4RCP.

[0068] In some cases, the reduced carbon products may be separated from the electrolyte stream and introduced into a separate electrochemical reactor where they can undergo further reduction such that additional carbon, hydrogen, and optionally oxygen atoms are added to them along with electrons, thereby allowing their growth to increase their size and energy and change their combustion characteristics. For example, ethanol can be produced as an initial RCP of a CO2 reduction reaction, directed to a second separate electrochemical reactor that may contain an electrochemical laminate, and further reduced to butanol, thereby producing a larger RCP. For example, a mixture of C1-C15 RCPs can be produced in a first laminate, RCPs containing six or more carbon atoms can be separated from the mixture through a micro- or nanostructured membrane (e.g., a membrane containing carbon nanotubes), and RCPs containing five or fewer carbon atoms can be directed to a second laminate (or recycled back to the first laminate) for further reaction and upgrading.

[0069] In some embodiments, the RCP may include a heat of combustion per mole at a constant pressure of 298K and 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, -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 a heat of combustion per mole at a constant pressure of 298K and 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, -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.

[0070] In some embodiments, the RCP may include a heat of combustion per mole that is greater (e.g., more negative) than the heat of combustion per mole of the upgraded RCP. For example, if the heat of combustion per mole is about -1,000 kJ / mol for the RCP, the heat of combustion of the corresponding upgraded RCP will be less than -1,000 kJ / mol (e.g., < -1,000 kJ / mol).

[0071] The residence time of RCP in an electrochemical reduction system can affect the size (e.g., molar weight) of RCP. In some embodiments, the residence time of RCP in the laminate is determined as a factor of the dimensions of the laminate. In some embodiments, a taller (vertically) electrochemical reduction laminate results in a longer residence time compared to a relatively shorter laminate. In some embodiments, a shorter (vertically) electrochemical reduction laminate results in a shorter residence time compared to a relatively taller laminate. In some embodiments, a wider (horizontally) electrochemical reduction laminate results in a longer residence time compared to a relatively narrower laminate. In some embodiments, a narrower (horizontally) electrochemical reduction laminate results in a shorter residence time compared to a relatively wider laminate.

[0072] Depending on the purpose of operating the electrochemical reduction system, it may be desirable to have RCP present in the electrochemical reduction system for a short or long period of time. For example, the goal may be to separate RCP in the vapor phase, so a shorter residence time is sufficient to obtain small RCP that can easily vaporize (e.g., less than 6 carbons). On the other hand, for example, the goal may be to produce RCP with a higher energy density (e.g., to enhance compatibility with an engine designed to operate on diesel fuel or jet fuel), so a longer residence time in the electrochemical reduction system is required to produce RCP with a longer carbon chain (e.g., higher molecular weight). In some embodiments, a longer residence time can be achieved within a single electrochemical reduction unit. In some embodiments, a longer residence time can be achieved within two or more electrochemical reduction units. For example, RCP may be produced in a first electrochemical reduction unit (e.g., a laminate) within a certain time period and directed to a second electrochemical reduction unit to further shorten an additional certain time period. The second electrochemical reduction unit may be referred to herein as a second electrochemical laminate, an upgrade laminate, an oligomerization laminate, or a cyclization laminate. The certain time periods may be the same or different.

[0073] With respect to the size and residence time of RCPs, the operation of a CO2 electrochemical reduction system can have conflicting objectives. On the one hand, it may be desirable to separate the reduced carbon products in the vapor phase, which operates best with smaller carbon products, e.g., RCPs having less than 6 carbon atoms. However, it may be desirable to produce longer carbon chain products (“upgraded” RCPs), e.g., to increase their energy density and increase compatibility with engines designed to operate with diesel or jet fuel.

[0074] It can be particularly useful to continuously remove or separate RCPs while operating an integrated direct air capture (DAC) and electrochemical stack system. By continuously separating and removing RCPs during operation, it may be possible for a minimum number of RCPs to remain in the stream directed back to the DAC unit, a minimum number of RCPs to vaporize and be lost to the air while further CO2 is being captured, and for larger (e.g., higher molecular weight) RCPs to be produced by further electrochemical reduction. Systems and methods for continuously removing (or separating) RCPs are disclosed herein to minimize the number of RCPs lost to the air while producing larger RCPs.

[0075] In some embodiments, one or more parameters of the electrochemical stack system can be adjusted to upgrade the RCPs. In some embodiments, the pH, total inorganic carbon (TIC), flow rate of the electrolyte (including dissolved CO2), stack dimensions, catalyst design, or combinations thereof are adjusted to obtain RCPs of a desired size.

[0076] In some embodiments, the pH of the laminate, the TIC within the laminate, the flow of electrolyte within the laminate, the laminate dimensions, or the catalyst design are adjusted to obtain an RCP of a desired size. In some embodiments, at least two of the pH of the laminate, the TIC within the laminate, the flow of electrolyte within the laminate, the laminate dimensions, and the parameters of the catalyst design are adjusted to produce an RCP of a desired size. In some embodiments, at least three of the pH of the laminate, the TIC within the laminate, the flow of electrolyte within the laminate, the laminate dimensions, and the parameters of the catalyst design are adjusted to produce an RCP of a desired size. In some embodiments, all of the pH of the laminate, the TIC within the laminate, the flow of electrolyte within the laminate, the laminate dimensions, and the parameters of the catalyst design are adjusted to obtain an RCP of a desired size. In some embodiments, not adjusting any of the parameters of the laminate may result in no further upgrade of the RCP. For example, by circulating ethanol (e.g., C2 alcohol) produced as an RCP to the same laminate or a different laminate under the same conditions, only ethanol can be obtained.

[0077] The pH of the electrochemical laminate can be adjusted or selected to regulate the identity or molecular weight of the RCP. The pH of the laminate can be adjusted by adding an acidic or basic solution to the laminate. The pH of the laminate can be adjusted by adding or subtracting an electrolyte solution from the laminate. In some embodiments, the electrochemical laminate is operated at a pH of from about 10 to about 15. In some embodiments, the electrochemical laminate is operated at a pH of about 10, about 11, about 12, about 13, about 14, or about 15. In some embodiments, the electrochemical laminate is operated at a pH of at least 10. A particular pH can be selected to regulate the identity or molecular weight of the RCP. For example, a laminate operated at a higher pH can produce an RCP having a greater amount of carbon compared to a laminate at a relatively lower pH. Individually or in combination with adjusting at least one other parameter of the laminate, operating the laminate at an elevated pH can result in an upgraded RCP (or, for example, an RCP having more than 12 carbon atoms).

[0078] In some embodiments, the total inorganic carbon in the electrochemical laminate can be selected to adjust the identity or molecular weight of the RCP. Optionally, the TIC in the electrochemical laminate is from about 0.5 mol / L (M) to about 2.5 M. Optionally, the TIC in the electrochemical laminate is about 0.5 M to about 1 M, about 0.5 M to about 1.25 M, about 0.5 M to about 1.5 M, about 0.5 M to about 1.75 M, about 0.5 M to about 2 M, about 0.5 M to about 2.5 M, about 1 M to about 1.25 M, about 1 M to about 1.5 M, about 1 M to about 1.75 M, about 1 M to about 2 M, about 1 M to about 2.5 M, about 1.25 M to about 1.5 M, about 1.25 M to about 1.75 M, about 1.25 M to about 2 M, about 1.25 M to about 2.5 M, about 1.5 M to about 1.75 M, about 1.5 M to about 2 M, about 1.5 M to about 2.5 M, about 1.75 M to about 2 M, about 1.75 M to about 2.5 M, or about 2 M to about 2.5 M. Optionally, the TIC in the electrochemical laminate is about 0.5 M, about 1 M, about 1.25 M, about 1.5 M, about 1.75 M, about 2 M, or about 2.5 M. A particular pH can be selected to adjust the identity or molecular weight of the RCP. Optionally, a laminate operating at a higher TIC can produce an RCP having a greater amount of carbon compared to a laminate having a relatively lower TIC. Individually or in combination with adjusting at least one other parameter of the laminate, operating the laminate at an increased TIC concentration with an increased pH can result in an upgraded RCP (or, for example, an RCP having more than 12 carbon atoms). In some embodiments, the flow rate or flow profile of the electrolyte or other fluid throughout the electrochemical laminate is decreased to eliminate turbulent flow. Optionally, the electrolyte has a laminar flow profile within the electrochemical laminate. Optionally, the flow of the electrolyte throughout the electrochemical laminate is characterized by a Reynolds number of about 500 to about 3,000.In some cases, the flow of the electrolyte throughout the electrochemical laminate 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 throughout the electrochemical laminate 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 throughout the electrochemical laminate is characterized by a Reynolds number of up to about 1,000, about 1,500, about 2,000, about 2,500, or about 3,000. The flow rate or flow profile of the electrolyte or other fluid throughout the electrochemical laminate can be selected to regulate the identity or molecular weight of the RCP. In some cases, a laminate operating at a lower flow rate or Reynolds number can result in an RCP having a greater amount of carbon compared to a laminate having a relatively low flow rate or Reynolds number. In some cases, a laminar flow profile can increase the contact time between the RCP and the catalyst within the electrochemical laminate, and thus an upgraded RCP can result. By operating the laminate with a laminar flow profile, either individually or in combination with adjusting at least one other parameter of the laminate, an upgraded RCP (or, for example, an RCP having more than 12 carbon atoms) can be obtained.

[0079] In some embodiments, a catalyst is used within an electrochemical laminate to facilitate the reduction of CO2 or the upgrading of RCP. The identity or composition can be adjusted or selected to modulate the identity or molecular weight of the RCP. For example, the size of the catalyst nanoparticles can be adjusted to increase the size of the RCP. In some cases, the catalyst comprises nanoparticles having a diameter of from about 25 nm to about 100 nm. In some cases, the catalyst comprises nanoparticles having a diameter of from about 25 nm to about 50 nm, from about 25 nm to about 75 nm, from about 25 nm to about 100 nm, from about 50 nm to about 75 nm, from about 50 nm to about 100 nm, or from about 75 nm to about 100 nm. In some cases, the catalyst comprises nanoparticles having a diameter of about 25 nm, about 50 nm, about 75 nm or about 100 nm. In some cases, the catalyst comprises nanoparticles having a diameter of at least about 25 nm, about 50 nm or about 75 nm. In some cases, the catalyst comprises nanoparticles having a diameter of up to about 50 nm, about 75 nm, or about 100 nm. In some instances, a laminate comprising a catalyst with larger nanoparticles can produce a greater amount of carbon-containing RCP compared to a laminate comprising a catalyst with relatively smaller nanoparticles. By either individually tuning the catalyst size or in combination with adjusting at least one other parameter of the laminate, upgraded RCP (or, for example, RCP having more than 12 carbon atoms) can be obtained.

[0080] Various embodiments of a CO2 reduction system are described herein that can continuously remove RCP while enabling the production of larger-sized carbon products. For example, referring to FIG. 1, RCP can be generated within an electrochemical laminate and removed from the electrolyte. The RCP can exit the laminate by heat, gas stripping, adsorption, or combinations thereof, before the depleted electrolyte is sent back to the DAC system to further capture CO2. The removed RCP can be present with some water (also removed from the electrolyte by the removal process) and can be directed to a second electrochemical laminate for further reduction to larger RCP. For example, the first electrochemical laminate can be C5 - C within the second electrochemical laminate 16It is possible to mainly produce a mixture of C1 - C4 RCPs that can be further reduced to RCP.

[0081] In some cases, as shown in FIG. 1, an electrolyte stream 107 containing an electrolytic solution (e.g., water) for use in an electrochemical CO2 reduction process can be brought into contact with a CO2 - containing gas within a direct air capture (DAC) unit 108 to produce a CO2 - enriched electrolyte. In some cases, the CO2 - enriched electrolyte contains bicarbonate. The CO2 - containing gas may be air from the atmosphere and may be introduced into the DAC unit 108 through an inlet (not shown). In some examples, the pH, temperature, or other properties of the electrolyte stream 107 can be controlled to optimize the capture of CO2 from the CO2 - containing gas into the electrolytic solution. In some examples, the CO2 - containing gas also contains water that can be absorbed by the electrolyte stream.

[0082] The CO2 - enriched electrolyte stream 101 can enter a first electrochemical stack 102. The electrochemical stack 102 can include a cathode, an anode, and an ion - exchange membrane. Within the electrochemical stack, carbon in the electrolytic solution 101 can be reduced to one or more RCPs by electrical energy (e.g., an applied voltage). The first electrochemical stack 102 may include a first catalyst. In some embodiments, the first catalyst includes copper, a defect - containing or doped carbon material, 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. The specific parameters of the first stack 102 can be adjusted to produce a smaller - sized RCP compared to the second electrochemical stack. Such parameters can include pH, total inorganic carbon, stack height, stack width, catalyst size, residence time, flow rate, or flow profile, or any combination thereof.

[0083] The RCP-enriched electrolyte stream 103 may be directed towards the extraction or separation means 104. The extractor 104 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 (e.g., depleted electrolyte) in which the RCP may be depleted can exit the extractor 104 as the electrolyte stream 107 and return to the DAC unit 108 to further capture CO2, whereby it can be reused within the electrochemical reduction system described herein. The electrolyte stream 107 can enter the DAC 108 for use in capturing additional CO2. It may be particularly useful to continuously remove the RCP so that little or no RCP remains in the electrolyte stream 107 directed towards the DAC 108. This can prevent the RCP from being lost to the air during direct air capture of CO2. In some embodiments, the electrolyte stream exiting the extractor 104 may not be reused within the electrochemical reduction system.

[0084] The reduced carbon product can exit the extractor 104 as the RCP stream 105 and enter the second electrochemical laminate (upgraded laminate) 106. Optionally, the RCP stream 105 may contain RCP present in water that may have been removed from the electrolyte within the extractor 104. The second electrochemical laminate 106 can be used to further reduce or upgrade the RCP to larger reduced carbon products having a higher molecular weight. The second electrochemical laminate 106 may include a second cathode, a second anode, and a second membrane. The second electrochemical laminate 106 may include a second catalyst. In some embodiments, the second catalyst includes copper, a defect-containing or doped carbon material, silver palladium or nickel, or any combination thereof. Optionally, the second catalyst includes the same material as the first catalyst. Optionally, the second catalyst includes the same material as the first catalyst in different ratios or amounts. In some embodiments, the second catalyst acts to produce an upgraded set of larger (e.g., higher molecular weight) and / or cyclic RCPs. The second catalyst may include a catalyst material specifically designed to produce desired carbon products such as branched or cyclic carbon molecules. The specific parameters of the second laminate 106 can be adjusted to produce larger sized RCPs as compared to the first electrochemical laminate. Such parameters can include pH, total inorganic carbon, laminate height, laminate width, catalyst size, residence time, flow rate, or flow profile, or any combination thereof.

[0085] The electrochemical reduction of RCP in the second electrochemical laminate 106 can occur in the liquid phase, gas phase, or mixed phase. In some cases, the reduction reaction in the second electrochemical laminate 106 occurs in the gas phase using humidified air containing RCP. In some cases, the reduction reaction in the second electrochemical laminate 106 may be in the aqueous phase using an electrolyte. Hydrogen may be introduced into the second electrochemical laminate 106. In some cases, the introduced hydrogen is produced in the first electrochemical laminate 102 and introduced into the second electrochemical laminate 106. In some cases, the second electrochemical laminate may be in the gas phase and may contain humidified air containing RCP and / or hydrogen gas. To promote the production of RCP of a desired size, the temperature of the second laminate 106 may be higher or lower than that of the first laminate 102.

[0086] The upgraded RCP can exit the second electrochemical laminate 106 as the RCP stream 109 and enter the second separation unit 110. The second separation unit 110 may also be referred to as a splitting unit. In the second separation unit 110, the upgraded RCP can be separated based on their size. Larger RCP (e.g., having about C 12 , or a higher carbon number range, e.g.) can be separated from smaller RCP (e.g., having a carbon number range of about C1 to about C 12 , e.g.) by various means such as a carbon nanotube ("CNT") membrane, hydrocyclone, or a vapor or pervaporation (PV) separation method using adsorption separation. The larger RCP may be poorly soluble or insoluble in water, may have a low vapor pressure, and require a separation method different from those ideally used for the separation of RCP produced in the first electrochemical laminate. After separation, the smaller (e.g., lower molecular weight) RCP exits the splitting unit 110 as the stream 112, re-enters the second electrochemical laminate 106, and can be further reduced. The RCP having an increased carbon number exits the splitting unit 110 as the stream 111 and may be used or sold as a final product or may undergo further processing. In some cases, the stream 111 can be sold or used as a finished fuel product such as diesel fuel or jet fuel.

[0087] In some cases, as shown in FIG. 2, an electrolyte stream 209 containing an electrolyte solution (e.g., water) for use in an electrochemical CO2 reduction process can be contacted with a CO2-containing gas within a direct air capture (DAC) unit 210 to produce a CO2-enriched electrolyte. In some cases, the CO2-enriched electrolyte contains bicarbonate. The CO2-containing gas may be air from the atmosphere and may be introduced into the DAC unit 210 through an inlet (not shown). In some examples, the temperature or other characteristics of the electrolyte stream 209 can be controlled to optimize the capture of CO2 from the CO2-containing gas into the electrolyte solution. In some examples, the CO2-containing gas also contains water that can be absorbed by the electrolyte stream 209.

[0088] The CO2-enriched electrolyte stream 201 can enter the electrochemical stack 202. The electrochemical stack 202 can include a cathode, an anode, and a membrane, and within the electrochemical stack, carbon in the electrolyte solution 201 can be reduced to one or more RCPs by electrical energy (e.g., an applied voltage). To produce larger RCPs, the residence time of the CO2-enriched electrolyte stream within the electrochemical stack 202 can be increased. For example, increasing the residence time within the electrochemical stack can, for example, increase the production of RCPs with a carbon number greater than C 12 There may be an increase in the production of larger RCPs. In some embodiments, one or more parameters of the electrochemical stack 202 can be adjusted to upgrade the RCP. In some embodiments, the pH, total inorganic carbon (TIC), flow rate of the electrolyte solution (including dissolved CO2), stack dimensions, catalyst design, or a combination thereof can be adjusted to obtain an RCP of a desired size.

[0089] In some cases, by enabling the RCP to be retained within the electrochemical laminate 202, the RCP can expand by adding carbon atoms, hydrogen atoms, and oxygen atoms. The expanded RCP can have different combustion characteristics compared to their smaller counterparts. The electrochemical laminate 202 may include a catalyst. In some embodiments, the first catalyst includes copper, a defect-containing or doped carbon material, silver palladium or nickel, or any combination thereof.

[0090] The RCP-enriched electrolyte stream 203 may be directed towards the extraction or separation means 204. The extractor 204 can separate the RCP from the electrolyte. The RCP can be removed from the electrolyte by thermal stripping, gas stripping, or adsorption, or any combination thereof. The electrolyte that may be depleted of RCP (e.g., the depleted electrolyte) exits the extractor 204 and returns to the DAC unit 210 as the electrolyte stream 209, where it can further capture CO2 and thus be reused within the electrochemical reduction system described herein. In some embodiments, the electrolyte stream exiting the extractor 204 may not be reused within the electrochemical reduction system.

[0091] The RCP can exit the extractor 204 as the RCP stream 205 and enter the separation unit 206. The second separation unit 206 may also be referred to as a splitter. Within the separation unit 206, the RCP can be separated based on their size. The larger RCP can be separated from the smaller RCP by various means such as, for example, a carbon nanotube (''CNT'') membrane, a hydrocyclone, or a vapor or pervaporation separation method that utilizes adsorption separation. After separation, the smaller (e.g., lower molecular weight) RCP exits the splitter 206 as the stream 208 and re-enters the electrochemical laminate 102 where it can be further reduced. The RCP having an increased carbon number range exits the splitter 206 as the stream 207 and may be used or sold as a final product or may undergo further processing. In some cases, the stream 207 can be sold or used as a finished fuel product such as diesel fuel and jet fuel.

[0092] Computer system The present disclosure provides a computer system programmed to implement the methods of the present disclosure. FIG. 3 shows a computer control system 1201 programmed or configured to control a chemical reduction system or a process within a chemical reduction system (e.g., controlling the pH within an electrochemical laminate, controlling the flow rate of an electrolyte). The computer control system 1201 can adjust various aspects of the methods of the present disclosure, such as, for example, a method of producing a reduced carbon product or a method of monitoring potentially hazardous operating conditions. The computer control system 1201 can be implemented on a user's electronic device or on a computer system located remotely from the electronic device. The electronic device may be a mobile electronic device.

[0093] The computer system 1201 includes a central processing unit (CPU, referred to herein as "processor" and "computer processor") 1205, which can 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., hard disk), a communication interface 1220 (e.g., network adapter) for communicating with one or more other systems, and peripheral devices 1225 such as cache, 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 can be a data storage unit (or data repository) for storing data. The computer system 1201 can be operably coupled to a computer network ("network") 1230 with the assistance of the communication interface 1220. The network 1230 can be the Internet, the Internet and / or an extranet, or an intranet and / or an extranet that communicates with the Internet. The network 1230 can be, in some cases, a telecommunications and / or data network. The network 1230 can include one or more computer servers that enable distributed computing, such as cloud computing. The network 1230 can, in some cases, implement a peer-to-peer network in which devices coupled to the computer system 1201 can operate as clients or servers with the assistance of the computer system 1201.

[0094] The CPU 1205 can execute a series of machine-readable instructions that can be embodied by a program or software. The instructions can be stored in a memory location such as the memory 1210. The instructions can be directed to the CPU 1205, and the CPU 1205 can then program or configure the CPU 1205 to implement the methods of the present disclosure. Examples of operations performed by the CPU 1205 can include fetch, decode, execute, and write-back.

[0095] The CPU 1205 can be part of a circuit such as an integrated circuit. One or more other components of the system 1201 can be included in the circuit. In some cases, the circuit is an application-specific integrated circuit (ASIC).

[0096] The storage unit 1215 can store files such as drivers, libraries, and stored programs. The storage unit 1215 can store user data, such as user preferences and user programs. The computer system 1201 can include one or more additional data storage units external to the computer system 1201, such as being located on a remote server that communicates with the computer system 1201 via an intranet or the Internet in some cases.

[0097] The computer system 1201 can communicate with one or more remote computer systems via the network 1230. For example, the computer system 1201 can communicate with a remote computer system of a user (e.g., a user who monitors the pH and temperature of an electrolyte flow). Examples of remote computer systems include personal computers (e.g., portable PCs), slates or tablet PCs (e.g., Apple® iPad, Samsung® Galaxy Tab), telephones, smartphones (e.g., Apple® iPhone, Android-compatible devices, Blackberry®), or personal digital assistants. A user can access the computer system 1201 via the network 1230.

[0098] The methods described herein can be implemented by machine (e.g., computer processor) executable code stored in an electronic storage location of the computer system 1201, such as, for example, the memory 1210 or the electronic storage unit 1215. The machine executable code or machine readable code can be provided in the form of software. In use, the code can be executed by the processor 1205. In some cases, the code can be retrieved from the storage unit 1215 and stored in the memory 1210 so as to be readily accessible by the processor 1205. In some situations, the electronic storage unit 1215 can be excluded and the machine executable instructions can be stored in the memory 1210.

[0099] The code can be pre-compiled and configured for use on a machine having a processor adapted to execute the code, or can be compiled during runtime. The code can be supplied in a programming language that can be selected to enable the code to be executed in a pre-compiled or compiled manner.

[0100] Aspects of the systems and methods provided herein, such as computer system 1201, can be embodied in programming. Various aspects of the technology can typically be considered a "product" or "manufactured article" in the form of machine (or processor) executable code and / or associated data carried on or embodied in some form of machine-readable medium. The machine executable code can be stored in an electronic storage device such as a memory (e.g., read-only memory, random access memory, flash memory, cloud) or a hard disk. A "storage" type medium can include any or all of tangible memories such as computers, processors, or associated modules such as various semiconductor memories, tape drives, disk drives, etc., and can serve as non-transitory storage at any time for software programming. All or part of the software can sometimes be communicated via the Internet or various other electrical communication networks. Such communication can, for example, enable the loading of software from one computer or processor to another, such as from a management server or host computer to an application server's computer platform. Thus, another type of medium on which software elements can be carried includes light waves, electrical waves, and electromagnetic waves such as those used over wired and optical terrestrial networks and via various air links at the physical interface between local devices. Physical elements that carry such waves, such as wired or wireless links, optical links, etc., can also be considered a medium for carrying software. As used herein, unless limited to non-transitory and tangible "storage" media, terms such as "readable medium" of a computer or machine refer to any medium involved in providing instructions to a processor for execution.

[0101] Thus, machine-readable media such as computer-executable code can take many forms including, but not limited to, tangible storage media, carrier wave media, or physical transmission media. Non-volatile storage media can include, for example, any one or more of the storage devices within a computer such as optical disks or magnetic disks that can be used to implement a database shown in the drawings. Volatile storage media can include dynamic memory such as the main memory of such a computer platform. Tangible transmission media can include coaxial cables, copper wire and fiber optics, wires having a bus within a computer system, and the like. Carrier wave transmission media can take the form of electrical signals 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 can include, for example, floppy disks, flexible disks, hard disks, magnetic tape, any other magnetic media, CD-ROM, DVD or DVD-ROM, any other optical media, punch cards, paper tapes, any other physical storage media with patterns of holes, RAM, ROM, PROM and EPROM, FLASH-EPROM, any other memory chip or cartridge, carrier waves that carry data or instructions, cables or links that carry such carrier waves, or any other media that a computer can read programming code and / or data from. Many of these forms of computer-readable media can be involved in carrying one or more sequences of one or more instructions to a processor for execution.

[0102] Computer system 1201 can include, or be communicable with, an electronic display 1235 that includes, for example, a user interface (UI) 1240 for providing the pH, flow rate, or temperature of an electrolyte stream. Examples of UIs can include, but are not limited to, graphical user interfaces (GUIs) and web-based user interfaces.

[0103] The methods and systems of the present disclosure can be implemented by one or more algorithms. The algorithms can be implemented by software when executed by a central processing unit 1205. The algorithms can, for example, adjust the flow rate of a gas stream containing CO2 through a direct air capture unit to optimize the capture of CO2 by an electrolytic solution. As another example, the algorithms can regulate the electric field applied to a microstructured or nanostructured membrane to control the selectivity of the membrane for a particular chemical species.

[0104] The methods and systems of the present disclosure may be combined with, or modified by, other methods and systems such as those disclosed in U.S. Patent No. 10,590,548 and International Publication No. 2020 / 131837, each of which is hereby incorporated by reference in its entirety.

[0105] Although the preferred embodiments of the present invention have been shown and described herein, it will be apparent to those skilled in the art that such embodiments are provided by way of example only. The present invention is not intended to be limited by the specific examples provided herein. Although the present invention has been described with reference to the foregoing specification, the description and illustration of the embodiments herein are not to be construed in a limiting sense. The section headings used herein are for purposes of organization only and are not to be construed as limiting the subject matter described. Those skilled in the art will be able to make numerous variations, modifications, and substitutions herein without departing from the present invention. Further, it should be understood that all aspects of the present invention are not limited to the specific depictions, configurations, or relative proportions described herein, which depend on various conditions and variables. It should be understood that various alternative forms of the embodiments of the present invention described herein may be used in the practice of the present invention. Accordingly, the present invention is intended to embrace any such alternative, modified, variant, or equivalent. The following claims define the scope of the present invention, and it is intended that methods and structures within the scope of these claims and their equivalents be covered thereby.

Claims

1. A method for producing reduced carbon products, (a) Bringing a gas stream into contact with an electrolyte, wherein the gas stream is carbon dioxide (CO2). ２ ) includes, thereby the CO ２ To capture the gas from the gas flow into the electrolyte, (b) The CO in the electrolyte ２ The first reduced carbon product is produced by reducing it, (c) Reducing a subset of the first reduced carbon product to produce a second reduced carbon product, wherein the second reduced carbon product contains a greater number of carbon atoms than the first reduced carbon product. A method that includes this.

2. (b) Using an electrochemical laminate, the CO ２ The method according to claim 1, comprising reducing to produce the first reduced carbon product.

3. The method according to claim 2, wherein (c) the electrochemical laminate is used to reduce the subset of the first reduced carbon product to produce the second reduced carbon product.

4. The method according to claim 3, wherein the electrochemical laminate further comprises a carbon nanotube (CNT) film.

5. The method according to claim 3, further comprising removing an additional subset of the first reduced carbon product from the electrochemical laminate.

6. The method according to claim 5, further comprising recycling at least a portion of the additional subset of the first reduced carbon product into the electrochemical laminate.

7. The method according to claim 3, further comprising controlling one or more parameters of the electrochemical laminate to promote or increase the generation of the second reduced carbon product in (c).

8. The method according to claim 7, wherein one or more of the parameters include the pH of the electrochemical laminate.

9. The method according to claim 8, wherein the pH of the electrochemical laminate is greater than 10.

10. The method according to claim 7, wherein one or more of the parameters include the concentration of total inorganic carbon (TIC) in the electrochemical laminate.

11. The method according to claim 10, wherein the concentration of the TIC in the electrochemical laminate exceeds 0.5 mol / L (M).

12. The method according to claim 7, wherein one or more of the parameters include the flow profile or flow rate of the electrolyte through the electrochemical laminate.

13. The method according to claim 12, wherein the flow profile of the electrolyte includes laminar flow, and the laminar flow has a Reynolds number of less than 2000.

14. The method according to claim 7, wherein the electrochemical laminate includes a catalyst, and one or more parameters include the catalyst of a certain particle size.

15. The method according to claim 14, wherein the particle size of the catalyst is greater than 25 nanometers (nm).

16. The method according to claim 7, wherein one or more of the parameters include the residence time of the electrolyte in the electrochemical laminate.

17. The method of claim 2, wherein (c) is to reduce the first reduced carbon product to produce the second reduced carbon product using an additional electrochemical laminate separate from the electrochemical laminate.

18. The method according to claim 17, further comprising (a) controlling a first set of parameters of the electrochemical laminate to promote or increase the generation of the first reduced carbon product in the electrochemical laminate, and (b) controlling a second set of parameters of the additional electrochemical laminate to promote or increase the generation of the second reduced carbon product in the additional electrochemical laminate.

19. The method according to claim 17, wherein the electrochemical laminate is operated at a pH lower than that of the additional electrochemical laminate.

20. The method according to claim 17, wherein the electrochemical laminate has a lower total inorganic carbon (TIC) concentration than the additional electrochemical laminate.

21. The method according to claim 17, wherein the electrolyte in the electrochemical laminate has a lower Reynolds number than the electrolyte in the additional electrochemical laminate.

22. The method according to claim 17, wherein the additional electrochemical laminate is taller than the electrochemical laminate.

23. The method according to claim 17, wherein the additional electrochemical laminate is wider than the electrochemical laminate.

24. The method according to claim 17, wherein the electrochemical laminate comprises a first catalyst, and the additional electrochemical laminate comprises a second catalyst, wherein the particle size of the second catalyst is larger than that of the first catalyst.

25. The method according to claim 17, wherein the residence time of the electrolyte in the electrochemical laminate is shorter than the residence time of the electrolyte in the additional electrochemical laminate.

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