Systems, articles, and methods related to capture and / or conversion of gases including carbon dioxide

Abstract

Various embodiments of an integrated system for capturing carbon dioxide and converting it into at least one useful product is described herein. Carbon dioxide, in some embodiments, can be captured via liquid mist, separated from a gas stream electrostatically, and converted into at least one product using any of myriad of conversion apparatuses. In some embodiments, the integrated system can remove carbon dioxide from a combustion exhaust stream.

Description

[0001] SYSTEMS, ARTICLES, AND METHODS RELATED TO CAPTURE AND / OR CONVERSION OF GASES INCLUDING CARBON DIOXIDE

[0002] RELATED APPLICATIONS

[0003] This application claims priority under 35 U.S.C. § 119(e) to U.S. Provisional Patent Application No. 63 / 623,863, filed January 23, 2024, and entitled “CAPTURE AND / OR CONVERSION OF GASES INCLUDING CARBON DIOXIDE,” which is incorporated herein by reference in its entirety for all purposes.

[0004] TECHNICAL FIELD

[0005] Integrated systems for the capture and conversion of carbon dioxide are generally described.

[0006] BACKGROUND

[0007] Global CO2 emissions have continued to increase over the past several decades and have reached approximately 36 gigatonnes (Gt) in 2019. A significant portion of global CO2 emissions are released into the environment by points sources such as powerplants, which may combust fossil fuels to produce energy. CO2 emissions can be mitigated by capturing the produced carbon dioxide prior to its release into the atmosphere. Such carbon capture technologies aim to be implemented at the source of combustion and can classified into three main approaches: (i) chemical; (ii) physical; and (iii) biochemical. Chemical approaches include adsorption, direct or membrane-assisted absorption into a liquid, and chemical looping combustion. Physical approaches include membrane separation, physical absorption, and cryogenic distillation. A variety of biochemical methods utilizing enzymatic and algae-based approaches have also been proposed. Of these methods, chemical absorption into a liquid absorbent is widely considered to be the most promising technology due to the higher efficiencies, lower costs, and techno-economic maturity that it offers.

[0008] However, after the CO2 is removed and / or captured from exhaust gas, it often has relatively limited value. Coupled with the costs conventionally associated with carbon capture infrastructure, the limited intrinsic value of the captured carbon dioxide limits the widespread adoption of carbon capture technologies. To recoup a portion of these costs, it is possible to convert carbon dioxide into chemical compounds with greater value, such as ethanol, but to do so may require large capital and energy expenditures. Gaseous carbon dioxide may need to be compressed, stored, and / or transported to facilities configured to convert the CO2 into usable products. Additionally, the carbon dioxide and / or the captured form of the carbon dioxide may not be suitable for efficient conversion as its form, concentration, and / or other properties may influence the rate, efficiency, yield, and types of products produced by the conversion process. Therefore, there is a need more efficient carbon capture and conversion processes to reduce the capital and energy expenditures associated with mitigating carbon dioxide emissions.

[0009] SUMMARY

[0010] Systems and methods for the capture and conversion of carbon dioxide are generally described. The subject matter of the present disclosure involves, in some cases, interrelated products, alternative solutions to a particular problem, and / or a plurality of different uses of one or more systems and / or articles.

[0011] In one aspect, integrated systems for converting gaseous carbon dioxide into at least one product are described. In some embodiments, an integrated system for converting gaseous carbon dioxide into at least one product comprises a gas flow pathway having an inlet for receiving a gas stream comprising gaseous carbon dioxide and an outlet for releasing the gas stream containing less of the gaseous carbon dioxide than is contained in the gas stream at the inlet; a gaseous carbon dioxide absorption zone along the gas flow pathway; a source of a liquid mist configured to introduce the liquid mist into the gaseous carbon dioxide absorption zone, wherein the gaseous carbon dioxide absorption zone is configured to expose the liquid mist to the gas stream under conditions facilitating transfer of at least some of the gaseous carbon dioxide from the gas stream to the mist; an electrostatic separation zone along the gas flow pathway, fluidly connected to the gaseous carbon dioxide separation zone and configured to electrostatically separate at least some of the liquid mist from the gas stream to form a mist- captured feedstock; and a conversion apparatus configured to receive the mist-captured feedstock and expose at least some of the feedstock to conditions that facilitate the conversion of the feedstock into at least one product.

[0012] In some embodiments, an integrated system for converting gaseous carbon dioxide into at least one product, comprises a separation zone, fluidically connected to a gas flow pathway, configured to separate at least a portion of liquid mist from a gas stream flowing through the gas flow pathway; and a conversion apparatus configured to receive a mist-captured feedstock and expose at least some of the mist-captured feedstock to conditions that facilitate its conversion into at least one product, wherein the liquid mist is configured to at least partially react with the gaseous carbon dioxide in the gas stream to form the mist-captured feedstock. In one aspect, methods for converting gaseous carbon dioxide into at least one product are described. In some embodiments, a method for converting gaseous carbon dioxide into at least one product, comprises: exposing a gas stream, comprising gaseous carbon dioxide, in a gas flow pathway to a liquid mist, wherein a reactive component of the liquid mist is configured to at least partially react with the gaseous carbon dioxide; in a gaseous carbon dioxide absorption zone, reacting the reactive component and the gaseous carbon dioxide to produce a mist- captured feedstock; in a separation zone fluidly connected to the gaseous carbon dioxide absorption zone, separating at least some of the liquid mist and / or the mist-captured feedstock from the gas stream; and feeding the mist-captured feedstock into a conversion apparatus configured to expose at least some of the mist-captured feedstock to conditions that facilitate its conversion into at least one product.

[0013] Other advantages and novel features of the present disclosure will become apparent from the following detailed description of various non-limiting embodiments of the disclosure when considered in conjunction with the accompanying figures. In cases where the present specification and a document incorporated by reference include conflicting and / or inconsistent disclosure, the present specification shall control.

[0014] BRIEF DESCRIPTION OF THE DRAWINGS

[0015] Non-limiting embodiments of the present disclosure will be described by way of example with reference to the accompanying figures, which are schematic and are not intended to be drawn to scale unless otherwise indicated. In the figures, each identical or nearly identical component illustrated is typically represented by a single numeral. For purposes of clarity, not every component is labeled in every figure, nor is every component of each embodiment of the disclosure shown where illustration is not necessary to allow those of ordinary skill in the art to understand the disclosure. In the figures:

[0016] FIG. 1 depicts a schematic of an integrated system for converting gaseous carbon dioxide, according to some embodiments.

[0017] FIG. 2 depicts a schematic of an integrated system introducing liquid mist into a gas flow pathway and converting gaseous carbon dioxide into at least one product, according to some embodiments.

[0018] FIG. 3 depicts a schematic of a conversion apparatus configured to convert mist- captured feedstock into at least one product, according to some embodiments.

[0019] FIG. 4A depicts a diagram of a non-integrated capture and conversion system for gaseous carbon dioxide, according to some embodiments. FIG. 4B depicts a diagram of an integrated capture and conversion system for gaseous carbon dioxide, according to some embodiments.

[0020] FIG. 5 depicts the capital expenditure and process of a segmented carbon capture, utilization, and storage system (top) and an integrated capture and conversion system for gaseous carbon dioxide (below), according to some embodiments.

[0021] FIGS. 6A-6C depicts the relationship between carbonate loading and absorption rate of a capture apparatus configured to capture gaseous carbon dioxide, according to some embodiments.

[0022] FIGS. 7A-7B depicts the relationship between carbonate loading and efficiency of an electrochemical cell configured to convert a mist-captured feedstock back into carbon dioxide, according to some embodiments.

[0023] FIG. 8 is a diagram depicting an electrochemical cell configured to convert a mist- captured feedstock into one or more products (e.g., carbon monoxide, ethanol, ethylene), according to some embodiments.

[0024] FIGS. 9A-9C depicts the capture efficiency of a capture apparatus that relies on mist and electrostatic separation of mist from a gas stream, according to some embodiments.

[0025] DETAILED DESCRIPTION

[0026] Systems for converting gaseous carbon dioxide into at least one product are generally described. The inventors have recognized the need for carbon capture and conversion processes with greater efficiency and have developed an integrated system for both capturing gaseous carbon dioxide and converting it into at least one product (e.g. carbon monoxide, ethylene, and / or ethanol). In certain embodiments, only capture is implemented. In other embodiments, only conversion is implemented. In most embodiments described herein, both are involved, and are integrated, i.e., a single, connected system including a variety of apparatus is equipped to capture gas such as carbon dioxide, and then subject the gas to one or more chemical reactions resulting in one or more product(s).

[0027] The system can include an absorption zone along a gas flow pathway, wherein a gas stream comprising gaseous carbon dioxide is exposed to mist (e.g., of a liquid) under conditions facilitating transfer of at least some of the gaseous carbon dioxide to the mist. A separation zone, which can be an electrostatic separation zone, in some embodiments is configured to electrostatically separate at least some of the mist from the gas stream. A conversion apparatus, in certain embodiments, is configured to receive a mist-captured feedstock and expose at least some of the feedstock to conditions that facilitate its conversion into at least one product. The integrated system may advantageously result in relatively high conversion rates and / or conversion efficiencies compared to non-integrated carbon capture and conversion systems.

[0028] Non-integrated carbon capture and conversion systems that are known in the state of the art prior to this disclosure, may neglect the coupling between the capture system and the conversion system. That is, prior capture processes may produce a feedstock with incompatible and / or insufficient properties for conversion systems. Many known carbon conversion systems rely on the quality of feedstock to efficiently convert the feedstock into products. As an example, prior carbon capture systems that produce a feedstock of low concentration may impart an undue load on carbon conversion systems thus restricting the conversion efficiency and / or throughput. Moreover, known carbon conversion systems may operate with limited efficiency using feedstocks with suboptimal properties including but not limited to pH, temperature, and / or incompatible phases as additional processing steps may be required prior to conversion. Accordingly, to improve the efficiency of capture and / or conversion, the coupling between carbon capture system and the carbon conversion system may be strengthened with integrated capture and conversion systems disclosed herein.

[0029] Additionally, conventional, non-integrated, capture and conversion systems can be relatively expensive to design and construct due to the scale of the infrastructure needed to remove carbon dioxide or carbon-based byproducts from the waste streams of manufacturing processes and / or power plants. Typically, large absorption towers are required to remove carbon dioxide from flue gas. The capture carbon dioxide must then be separated from its captured medium into its gaseous form to be compress and transported to a processing facility to convert gaseous carbon dioxide into usable products. The large financial cost and energy expenditure associated with the infrastructure to capture, process, transport, and convert gaseous carbon dioxide increases the need for an integrated system for the capture and conversion of gaseous carbon dioxide.

[0030] This disclosure results in mist-captured feedstock and / or mist-captured feedstock product, in some embodiments, that is surprisingly more highly concentrated than feedstock produced via traditional carbon capture processes (e.g. membrane separation, physical absorption, cryogenic distillation, enzymatic and / or algae -based carbon capture approaches) under otherwise essentially identical conditions. Higher feedstock concentration can result in higher conversion efficiencies and higher conversion rates when provided to a suitable conversion apparatus, such as those described herein and / or available to those of ordinary skill in the art with the benefit of this disclosure, such as an electrochemical cell configured for carbon conversion. As described elsewhere in the present disclosure, feedstocks of low concentration may allow for relatively high capture rates, but when fed into conversion systems, conversion efficiencies and rates may be undesirably low. Feedstock of high concentration, on the other hand, generally have low absorption (e.g., capture) rates, but allow for higher conversion rates. The systems described herein produce feedstocks of relatively high concentration thereby allowing for increased throughput of conversion processes, and are able to maintain relatively high absorption (e.g., capture) rates by relying on mist to facilitate the transfer of carbon dioxide into the sorbent.

[0031] Moreover, the co-localization of capture processes and the conversion processes in integrated systems, further aided by the liquid state of the mist-captured feedstock, may reduce the cost and / or energy expenditure associated with non-integrated systems (FIGS. 4B and 5). For example, non-integrated capture and conversion systems may require the compression of the gaseous carbon dioxide for transport to facilities where conversion process can be implemented (FIG. 4A). Accordingly, the high capital and energy expenditures traditionally associated with non-integrated carbon capture and conversion approaches can be mitigated through integration of such systems (FIGS. 4B and 5).

[0032] In some embodiments, the integrated system converts carbon dioxide present in a gas stream. The gas stream may be any of a variety of suitable gas streams. In some embodiments, the gas stream may be associated with an exhaust stream and / or flue gas stream from a combustion plant (e.g. a facility that generates electricity via combustion of fuel). In some cases, the gas stream may be part of an exhaust stream from an industrial process (e.g. steel refinement and / or cement production). In some embodiments, the gas stream comprises carbon dioxide. In certain instances, the gas stream further comprises exhaust gases and / or particulate matter often associated with industrial processing and / or combustion processes. The gas stream, in some embodiments, flows through a gas flow pathway and can be directed into and / or out of zones (e.g. the absorption zone or separation zone) with or without the aid of additional fluidic control devices (e.g. fans, pumps, blowers, valves, etc.). In some embodiments, the gas stream comprises a gaseous species. In some embodiments, the gaseous species comprises carbon dioxide.

[0033] The gas stream may have any of a variety of suitable flow velocities (measured in m / s) or per-area gas fluxes (measured in (m3 / s) / (m2)). In certain embodiments, for example, the gas stream has a flow velocity greater than or equal to 0.1 m / s, greater than or equal to 0.5 m / s, greater than or equal to 1 m / s, greater than or equal to 2 m / s, greater than or equal to 3 m / s, greater than or equal to 4 m / s, greater than or equal to 5 m / s, greater than or equal to 6 m / s, greater than or equal to 7 m / s, greater than or equal to 8 m / s, or greater than or equal to 9 m / s. In some embodiments, the gas stream has a flow velocity less than or equal to 10 m / s, less than or equal to 9 m / s, less than or equal to 8 m / s, less than or equal to 7 m / s, less than or equal to 6 m / s, less than or equal to 5 m / s, less than or equal to 4 m / s, less than or equal to 4 m / s, less than or equal to 3 m / s, less than or equal to 2 m / s, less than or equal to 1 m / s, or less than or equal to 0.5 m / s. Combinations of the above recited ranges are possible (e.g., the gas stream has a flow velocity greater than or equal to 0.1 m / s and less than or equal to 10 m / s, the gas stream has a flow velocity greater than or equal to 4 m / s and less than or equal to 5 m / s). Other ranges are also possible.

[0034] In some embodiments, the gas stream flows through a gas flow pathway. The pathway can be defined by any combination of directing components that cause the gas stream to be treated as described herein. Auxiliary ducts, valves, impellers, and the like which may not be specifically described herein can be employed, so long as the outcomes of this disclosure are realized. Multiple individual paths, e.g. separate ducts, ports, openings, or the like through which the gas stream (or portions of the gas stream), flow sequentially or in parallel, may be part of and fall within what is meant by a gas flow pathway.

[0035] The gas stream may enter the gas flow pathway through an inlet of the gas flow pathway and exit through an outlet of the gas flow pathway. The overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be any of a variety of suitable values. In some embodiments, for example, the overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be greater than or equal to 1 x 10'5Pa, greater than or equal to 1 x IO"4Pa, greater than or equal to 1 x 10'3Pa, greater than or equal to 1 x 10'2Pa, greater than or equal to 1 x 10 Pa, greater than or equal to 1 Pa, greater than or equal to 10 Pa, greater than or equal to 100 Pa, or greater than or equal to 1000 Pa. In some embodiments, the overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be less than or equal to 10000 Pa, less than or equal to 1000 Pa, less than or equal to 100 Pa, less than or equal to 10 Pa, less than or equal to 1 Pa, less than or equal to 1 x 10'1Pa, less than or equal to 1 x 10'2Pa, less than or equal to 1 x 10'3Pa, or less than or equal to 1 x IO"4Pa. Combinations of the above recited ranges are possible (e.g., the overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be greater than or equal to 1 x IO"4Pa and less than or equal to 10000 Pa, the overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be greater than or equal to 1 x 10'1Pa and less than or equal to 1 Pa). Other ranges are also possible. In certain embodiments, the overall gas stream pressure drop between the inlet of the gas flow pathway and the outlet of the gas flow pathway may be determined by measuring the difference in the pressure of the gas stream between the inlet of the gas flow pathway and the outlet of the gas flow pathway (e.g., using a pressure sensor and / or pressure gauge).

[0036] In some embodiments, the gas stream contains greater than or equal to 10% less, greater than or equal to 20% less, greater than or equal to 30% less, greater than or equal to 40% less, greater than or equal to 50% less, greater than or equal to 60% less, greater than or equal to 70% less, greater than or equal to 80% less, or greater than or equal to 90% less of the gaseous carbon dioxide at the outlet of the gas flow pathway than is contained in the gas stream at the inlet of the gas flow pathway. In certain embodiments, the gas stream contains less than or equal to 100% less, less than or equal to 90% less, less than or equal to 80% less, less than or equal to 70% less, less than or equal to 60% less, less than or equal to 50% less, less than or equal to 40% less, less than or equal to 30% less, or less than or equal to 20% less of the gaseous carbon dioxide at the outlet of the gas flow pathway than is contained in the gas stream at the inlet of the gas flow pathway. Combinations of the above recited ranges are possible (e.g., the gas stream contains greater than or equal to 10% less and less than or equal to 100% less of the gaseous carbon dioxide at the outlet of the gas flow pathway than is contained in the gas stream at the inlet of the gas flow pathway, the gas stream contains greater than or equal to 60% less and less than or equal to 80% less of the gaseous carbon dioxide at the outlet of the gas flow pathway than is contained in the gas stream at the inlet of the gas flow pathway). Other ranges are also possible. In certain embodiments, the amount of the gaseous carbon dioxide in the gas stream (e.g., at the inlet, at the outlet) may be measured by gas chromatography and / or a gaseous carbon dioxide sensor (e.g., a CO2 sensor).

[0037] In some embodiments, the gas flow pathway comprises an inlet. In some embodiments, the gas flow pathway comprises an inlet for receiving the gas stream. The inlet may be configured to allow the gas stream to enter the gas flow pathway in a specified manner. Blowers, fans, filters, and / or other gas flow apparatuses designed to and / or configured to control, alter, and / or otherwise influence the flow of gas may be incorporated into the gas flow pathway at the inlet, if desired. The inlet of the gas flow pathway may be associated and / or fluidically connected to a facility that produces exhaust gases, flue gases, and / or other waste gases produced via combustion and / or industrial processes. In some embodiments, the gas flow pathway itself may be associated with a facility that produces exhaust gases, flue gases, and / or other waste gases produced via combustion and / or industrial processes.

[0038] The gas flow pathway may be a tube, column, pipe, and / or stack. Any of a variety of suitable arrangements for the gas flow pathway can be provided. Those of ordinary skill in the art will recognize, based on the totality of this disclosure, that the gas flow pathway can be constructed in any way so as to direct some or all of a gas stream introduced at the inlet toward and through the outlet. The gas flow pathway can be constructed from any of a variety of suitable materials, including, for example, in many cases standard materials that are used in similar gas treatment processes and / or materials chosen that are resistant to corrosion by a gas in the gas flow pathway, if desired.

[0039] In some embodiments, the gas flow pathway comprises an outlet. In some embodiments, the gas flow pathway comprises an outlet for releasing the gas stream. The gas stream released from the outlet of the gas flow pathway may contain less of the gaseous carbon dioxide than is contained in the gas stream at the inlet. As the gas stream flows through the gas flow pathway, carbon dioxide may be absorbed, separated, and converted into a mist-captured feedstock prior to the gas stream exiting via the outlet of the gas flow pathway. Accordingly, the gas stream exiting and / or released at the outlet of the gas flow pathway may comprise a lower amount and / or concentration of carbon dioxide than the gas stream at the inlet entering the gas flow pathway. In some embodiments, the flux of the gaseous carbon dioxide at the inlet may be less than or equal to the flux of the gaseous carbon dioxide at the outlet.

[0040] As an example, FIG. 1 depicts gas flow pathway 105 with inlet 105A and outlet 105B and several zones, including absorption zone 110 and separation zone 120, are positioned along gas flow pathway 105. Inlet 105A is configured to receive the gas stream such that the gas stream can flow along gas flow pathway 105 and exit gas flow pathway 105 via outlet 105B. The gas stream exiting outlet 105B may comprise less gaseous carbon dioxide than that at inlet 105A.

[0041] In some embodiments, the gaseous carbon dioxide is absorbed in a gaseous carbon dioxide absorption zone. The absorption zone, in some embodiments, can be along the gas flow pathway. That is, a segment and / or section of the gas flow pathway may comprise the absorption zone. The absorption zone may be fluidly connected to the gas flow pathway. According to some embodiments, the gaseous carbon dioxide absorption zone may be configured as a tube, column, and / or cylinder. Configuring the gaseous carbon dioxide absorption zone as a tube, column, and / or cylinder may advantageously facilitate the flow of the gas stream along the gas flow pathway through the gaseous carbon dioxide absorption zone. Other configurations for the gaseous carbon dioxide absorption zone are also possible, however, as the disclosure is not meant to be limiting in this regard, including, for example, a cube, prism, and / or cone configuration. The gaseous carbon dioxide absorption zone may have any of a variety of suitable dimensions. In some embodiments, for example, the gaseous carbon dioxide absorption zone has a length that is sufficiently long enough to provide an advantageously high interfacial area between the reactive component (e.g. an absorbent) in the liquid mist and the gas stream.

[0042] The gaseous carbon dioxide absorption zone may have any of a variety of suitable lengths. In some embodiments, for example, the length of the gaseous carbon dioxide absorption zone is greater than or equal to 10 centimeters, greater than or equal to 50 centimeters, greater than or equal to 1 meter, greater than or equal to 2 meters, greater than or equal to 3 meters, greater than or equal to 4 meters, greater than or equal to 5 meters, greater than or equal to 10 meters, or greater than or equal to 20 meters. In certain embodiments, the length of the gaseous carbon dioxide absorption zone is less than or equal to 30 meters, less than or equal to 20 meters, less than or equal to 10 meters, less than or equal to 5 meters, less than or equal to 4 meters, less than or equal to 3 meters, less than or equal to 2 meters, less than or equal to 1 meter, or less than or equal to 50 centimeters. Combinations of the above recited ranges are possible (e.g., the length of the gaseous carbon dioxide absorption zone is greater than or equal to 10 centimeters and less than or equal to 30 meters, the length of the gaseous carbon dioxide absorption zone is greater than or equal to 3 meters and less than or equal to 4 meters). Other ranges are also possible.

[0043] The gaseous carbon dioxide absorption zone may comprise any of a variety of suitable materials. According to some embodiments, for example, the gaseous carbon dioxide absorption zone may comprise a metal, a metal alloy, a clad material, a ceramic, a plastic, a carbon-based material, and / or combinations thereof. Other materials are also possible. In certain embodiments, the gaseous carbon dioxide absorption zone material may be at least partially coated. For example, in some embodiments, the gaseous carbon dioxide absorption zone material may be coated with a corrosion resistant material (e.g., a plastic coated with a corrosion resistant metal or alloy).

[0044] In certain embodiments, the gaseous carbon dioxide absorption zone is a non-packed bed reactor. According to some embodiments, for example, the gaseous carbon dioxide absorption zone does not comprise a packed bed reactor.

[0045] According to some embodiments, the gaseous carbon dioxide absorption zone may comprise any of a variety of suitable fluidic components to enhance the interaction between the gas stream and the absorbent. In certain embodiments, for example, the gaseous carbon dioxide absorption zone may comprise one or more secondary circulation flow promoters, flow obstruction promoters, and / or turbulence promoters configured to maximize the interaction between the gas stream and the absorbent. The gaseous carbon dioxide absorption zone may have any of a variety of suitable temperatures and / or pressures to facilitate absorption of the gaseous carbon dioxide from the gas stream by the absorbent. In some embodiments, for example, increased temperatures (e.g., relative to room temperature) may enhance reaction between the reactive component (e.g. an absorbent) and the gaseous carbon dioxide but may also contribute to faster rates of evaporation of the absorbent. In certain embodiments, an increased overall pressure of the gaseous carbon dioxide absorption zone may enhance dissolution of the gaseous carbon dioxide into the absorbent and / or reaction between the absorbent and the gaseous carbon dioxide but may also be unpractical from an economic standpoint. Accordingly, in certain embodiments, the temperature and / or overall pressure of the gaseous carbon dioxide absorption zone may be tuned and / or chosen by a user depending on the absorbent, target gaseous carbon dioxide, and / or the components of the gas stream to facilitate adsorption of the gaseous carbon dioxide from the gas stream while avoiding evaporation of the absorbent and / or increased costs.

[0046] Any of a variety of suitable arrangements for the gaseous carbon dioxide absorption zone can be provided. Those of ordinary skill in the art will recognize, based on the totality of this disclosure, that the gaseous carbon dioxide absorption zone can be constructed in any way so as to remove gaseous carbon dioxide from the gas stream by chemically and / or physically transforming it. Conditions, such as temperature, flow rate, interfacial area between the gas stream and the gaseous carbon dioxide absorption zone, pressure, and / or other conditions that may influence gaseous carbon dioxide absorption recognizable to those of ordinary skill in that art, may be controlled to allow for the absorption of gaseous carbon dioxide.

[0047] In some embodiments, the gas flow pathway is configured to expose the liquid mist to the gas stream. When the gas stream enters the absorption zone, the gaseous carbon dioxide may be at least partially absorbed and / or removed from the gas stream upon exposure to a liquid mist. The absorption zone, in some embodiments, can be configured to expose the liquid mist to the gas stream. That is, the absorption zone may comprise spray heads, jets, and / or other fluidic dispensing and / or atomizing devices to ensure that the liquid mist, when present, is introduced into the absorption zone with sufficient surface area for carbon dioxide absorption.

[0048] In some embodiments, the liquid mist can be exposed to the gas stream under conditions facilitating transfer of at least some of the gaseous carbon dioxide from the gas stream to the mist. Conditions that facilitate the transfer of gaseous carbon dioxide to the mist may include but are not limited to temperature, flow rate of carbon dioxide in the gas flow pathway, pressure of carbon dioxide in the gas flow pathway, quantity of liquid mist introduced into the absorption zone, concentration of any reactive components in the liquid mist, pH of the liquid mist, and / or the flow rate of the gas stream in the gas flow pathway. A person of ordinary skill in the art, with the totality of this disclosure, may recognize the conditions that are necessary to facilitate the transfer of carbon dioxide into the liquid mist. Other conditions that facilitate the transfer of gaseous carbon dioxide to the mist are possible.

[0049] In some embodiments, the transfer of gaseous carbon dioxide to the liquid mist can occur in various forms. In certain instances, the gaseous carbon dioxide can react with the liquid mist and / or a reactive component in the liquid mist thereby producing an intermediary product. As an example, carbon dioxide can react with liquid mist comprising potassium hydroxide to form an intermediate product of potassium bicarbonate. In this example, the intermediate product may continue to be in a liquid mist form factor. In some embodiments, gaseous carbon dioxide may be transferred into the liquid mist in solution. That is, in some embodiments, the gaseous carbon dioxide may not immediately react with the liquid mist but may nevertheless be transferred to the liquid mist as aqueous carbon dioxide.

[0050] As an example, FIG. 2 depicts gaseous carbon dioxide absorption zone 110 along gas flow pathway 105 with source of liquid mist 115, fluidically connected to gaseous carbon dioxide absorption zone 110, introducing liquid mist 116 into gas flow pathway 105. Source of liquid mist 115 introduces and / or dispenses liquid mist comprising reactant component 205 into absorption zone 110 such that gaseous carbon dioxide reacts with reactant component 205 to form intermediate compound 205A. Intermediate compound 205A remains in a mist form factor within the absorption zone and can be entrained along gas flow pathway 105 with the gas stream. Absorption zone 110 facilitates the transfer of gaseous carbon dioxide from the gas stream into intermediate product 205A.

[0051] In some embodiments, the integrated system comprises a source of liquid mist. The source of liquid mist, according to certain embodiments, is configured to introduce the liquid mist into the gaseous carbon dioxide absorption zone. Spray heads, jets, and / or other fluidic dispensing and / or atomizing devices may be used to introduce the liquid into the absorption zone. Auxiliary equipment such as pumps, flow rate sensors, pressure sensors may be used to introduce the liquid mist into the absorption zone. In some embodiments, the source of liquid mist if fluidically connected to the gas flow pathway and / or the absorption zone.

[0052] In some embodiments, the source of liquid mist is configured to at least partially react with the gaseous carbon dioxide. In some embodiments, the source of liquid mist can be configured to introduce the liquid mist into the absorption zone in a manner that facilitates the absorption of carbon dioxide into the mist. To facilitate the absorption of carbon dioxide into the mist, the liquid mist can be present in a form factor that has sufficient interfacial area between the liquid mist and the gaseous carbon dioxide. That is, the liquid mist may comprise a plurality of droplets with sufficiently small diameters to enable relatively enhanced uptake of gaseous carbon dioxide from the gas stream. It is important to note, as one of ordinary skill in the art may understand based on the totality of this disclosure, that the absorption of gaseous carbon dioxide into the mist may effectively involve a chemical reaction and / or transformation, but may, at least in part, also involve at least some dissolution of gaseous carbon dioxide into the liquid mist.

[0053] The liquid mist, once introduced into the absorption zone from the source of liquid mist, can, in some embodiments, comprise a plurality of droplets. Each of the plurality of droplets, in some embodiments, may have a maximum dimension that provide sufficient interfacial area between the droplet and the gaseous carbon dioxide to effectively react and / or uptake the gaseous carbon dioxide at relatively high rates. In some embodiments, each of the plurality of droplets can have a maximum dimension that is sufficiently small to be entrained within the gas stream. That is, the plurality of droplets may be able to follow the flow path of the gas stream through the integrated system.

[0054] In some embodiments, the liquid mist comprises an absorbent (e.g., a sorbent). In some embodiments, the absorbent comprises a reactive component and / or reactant. In some embodiments, the reactive component and / or reactant is configured to react with the carbon dioxide to produce a carbonate or bicarbonate in a liquid (e.g. mist) state. Any of a variety of suitable reactive components may be employed. According to certain embodiments, virtually any absorbent may be used in the system described herein. In some embodiments, the absorbent comprises an amine-containing compound (e.g., monoethanolamine (MEA), 2-amino-2-methyl- 1-propanol (AMP)), a hydroxide (e.g., potassium hydroxide (KOH)), ammonia, a quinone, an amino acid, an ionic liquid, and / or combinations thereof. Other absorbents are also possible. In some embodiments, the reactive component and / or the reactant comprises potassium hydroxide (KOH). In some embodiments, the reactive component and / or the reactant comprises aqueous amine-based solutions (e.g. monoethanolamine). The gaseous carbon dioxide, once reacted with the liquid mist, can, in some embodiments, undergo a chemical transformation that effectively removes the gaseous carbon dioxide from the gas stream. That is, the reaction between the liquid mist and the carbon dioxide may transfer gaseous carbon dioxide to the liquid mist by creating an intermediate product that is within the liquid mist in the absorption zone. The intermediate product may maintain a mist form factor and therefore may entrain with the gas stream along the gas flow pathway.

[0055] According to some embodiments, the reactive component (e.g., the absorbent) may be configured such that the gaseous carbon dioxide dissolves in the absorbent. In some embodiments, the reactive component causes and / or facilitates a reaction of the gaseous carbon dioxide, thereby changing (e.g., chemically changing) the gaseous carbon dioxide and / or removing the gaseous carbon dioxide at least in part from the gas stream. In some embodiments, for example, the reactive component may react (e.g., chemically react) with the gaseous carbon dioxide in the gas stream. In some such embodiments, the reactive component may interact with the gaseous carbon dioxide and remove the gaseous carbon dioxide from the gas stream. In certain embodiments, the interaction between the reactive component and the gaseous carbon dioxide is one or more bonding interactions (e.g., chemical bonding interactions). Any of a variety of suitable bonding interactions between the reactive component and the gaseous carbon dioxide are possible, including, for example, covalent bonds, ionic bonds, dipole-dipole interactions, van der Waals interactions, London dispersion forces, and / or hydrogen bonds.

[0056] In certain embodiments, the reactive component may be in liquid form (e.g., the reactive component exists as a liquid at standard temperature and pressure). The reactive component may, in some embodiments, comprise a mixture (e.g., a reactive mixture). In some embodiments, for example, the reactive mixture comprises a reactant component (e.g., any of the reactive components described above) dissolved and / or dispersed in a liquid (e.g., water).

[0057] The reactive mixture may comprise the reactive components in any of a variety of suitable amounts. In certain embodiments, for example, the reactive mixture comprises the reactant in an amount greater than or equal to 5 weight percent (wt.%), greater than or equal to 10 wt.%, greater than or equal to 20 wt.%, greater than or equal to 30 wt.%, or greater than or equal to 40 wt.% versus the total weight of the reactive mixture. In some embodiments, the reactive mixture comprises the reactant in an amount less than or equal to 50 wt.%, less than or equal to 40 wt.%, less than or equal to 30 wt.%, less than or equal to 20 wt.%, or less than or equal to 10 wt.% versus the total weight of the reactive mixture. Combinations of the above recited ranges are possible (e.g., the reactive mixture comprises the reactant in an amount greater than or equal to 5 wt.% and less than or equal to 50 wt.% versus the total weight of the reactive mixture, the reactive mixture comprises the reactant in an amount greater than or equal to 20 wt.% and less than or equal to 30 wt.% versus the total weight of the reactive mixture). Other ranges are also possible.

[0058] In certain embodiments, the reactive mixture may comprise one or more additives. In certain embodiments, for example, the reactive mixture comprises nanoparticles configured to adsorb the gaseous carbon dioxide, thereby enhancing the removal efficiency of reactive mixture towards the gaseous carbon dioxide. The nanoparticles may, in some embodiments, be optionally functionalized with one or more functional groups configured to adsorb the gaseous carbon dioxide. Other additives are also possible, including, for example, surfactants.

[0059] According to certain embodiments, the system may comprise an adsorbent (e.g., in addition to or instead of the absorbent). The adsorbent may, in some embodiments, be configured to adsorb the gaseous carbon dioxide from the gas stream. Suitable adsorbents include, for example, a nanofluid. In certain embodiments, the nanofluid comprises a fluid comprising nanoparticles. The nanoparticles may, in some embodiments, be optionally functionalized with one or more functional groups configured to adsorb the gaseous carbon dioxide.

[0060] In certain embodiments, the separation zone comprises one or more surfaces that are configured to absorb and / or adsorb the liquid mist. In some embodiments, for example, the gas stream comprising entrained liquid mist may be flowed directly through a surface (e.g., a mesh and / or porous surface) in the separation zone (e.g., a collector electrode, a non-electrode surface, etc.) that captures at least some of the liquid mist. In other embodiments, the gas stream comprising the entrained liquid mist is flowed proximate a surface (e.g., a mesh and / or porous surface) in the separation zone (e.g., a collector electrode, a non-electrode surface, etc.), but need not pass through the surface. In certain embodiments, for example, a surface may be arranged as an enclosure and / or wall of the separation zone, and the gas stream comprising the entrained liquid mist can be directed at and / or tangential to the enclosure and / or wall such that the entrained liquid mist diffuses proximate the enclosure and / or wall. In one set of embodiments, the gas stream comprising entrained liquid mist is circulated and repeatedly flowed by one or more walls of an enclosure of the separation zone, for example a mesh surface defining an enclosure of the separation zone that is configured to separate the liquid mist from the gas stream.

[0061] According to some embodiments, the separation zone may be configured as a tube, column, and / or cylinder. Configuring the separation zone as a tube, column, and / or cylinder may advantageously facilitate the flow of the gas stream along the gas flow pathway through the separation zone. Other configurations for the separation zone are also possible, however, as the disclosure is not meant to be limiting in this regard, including, for example, a cube, prism, and / or cone configuration.

[0062] In some embodiments, the liquid mist can be separated from the gas stream in a separation zone. In some embodiments, the separation zone can be positioned along the gas flow pathway. The separation zone, in some embodiments, removes, separates, collects, and / or otherwise isolates the liquid mist from the gas stream. That is, the separation zone allows for the removal of carbon dioxide and / or the intermediate product from the gas stream thus limiting the amount of carbon dioxide exiting the outlet of the gas flow pathway. In some embodiments, the separation zone is along the gas flow pathway. In some embodiments, the separation zone is associated with the gas flow pathway. In some embodiments, the separation zone is fluidly connected to the gaseous carbon dioxide absorption zone.

[0063] According to some embodiments, the separation zone is configured to separate at least some of the liquid mist from the gas stream. The separation zone, in some embodiments, can impart suitable conditions onto the gas stream to remove, collect, separate, and / or otherwise isolate the liquid mist from the gas stream. In some embodiments, the separation zone electrostatically separates at least some of the liquid mist from the gas stream. As would be recognizable by a person of ordinary skill in the art, the separation zone may comprise any of a myriad of devices configured to remove the liquid mist from the gas stream flowing through the gas flow pathway.

[0064] The separation zone may have any of a variety of suitable lengths. In some embodiments, for example, the length of the separation zone is greater than or equal to 10 centimeters, greater than or equal to 50 centimeters, greater than or equal to 1 meter, greater than or equal to 2 meters, greater than or equal to 3 meters, or greater than or equal to 4 meters. In certain embodiments, the length of the separation zone is less than or equal to 5 meters, less than or equal to 4 meters, less than or equal to 3 meters, less than or equal to 2 meters, less than or equal to 1 meter, or less than or equal to 50 centimeters. Combinations of the above recited ranges are possible (e.g., the length of the separation zone is greater than or equal to 10 centimeters and less than or equal to 5 meters, the length of the separation zone is greater than or equal to 1 meter and less than or equal to 2 meters). Other ranges are also possible.

[0065] In certain embodiments wherein the separation zone is configured as a tube, column, and / or cylinder, the separation zone may have any of a variety of suitable diameters. In certain embodiments, for example, the separation zone has a diameter greater than or equal to 1 centimeter, greater than or equal to 5 centimeters, greater than or equal to 10 centimeters, greater than or equal to 20 centimeters, or greater than or equal to 50 centimeters. In some embodiments, the separation zone has a diameter less than or equal to 1 meter, less than or equal to 50 centimeters, less than or equal to 20 centimeters, less than or equal to 10 centimeters, or less than or equal to 5 centimeters. Combinations of the above recited ranges are possible (e.g., the separation zone has a diameter greater than or equal to 1 centimeter and less than or equal to 1 meter, the separation zone has a diameter greater than or equal to 10 centimeters and less than or equal to 20 centimeters). Other ranges are also possible. According to certain embodiments, the separation zone may be configured as a honeycomb structure. In some embodiments, for example, the separation zone may comprise a plurality of tubes, columns, and / or cylinders. In some such embodiments, each tube, column, and / or cylinder of the honeycomb separation zone may be fluidly connected to the gaseous carbon dioxide absorption zone such that each tube, column, and / or cylinder is configured to receive the gas stream after the gas stream has flowed through the gaseous carbon dioxide absorption zone. In certain embodiments wherein the separation zone is an electrostatic separation zone, each tube, column, and or cylinder of the honeycomb separation zone may comprise at least one emitter electrode and at least one collector electrode, as described herein. According to some embodiments, each tube, column, and / or cylinder of the honeycomb separation zone may have a length as described herein (e.g., greater than or equal to 10 centimeters and less than or equal to 5 meters) and / or a diameter as described herein (e.g., greater than or equal to 1 centimeter and less than or equal to 1 meter). Each tube, column, and / or cylinder of the honeycomb separation zone may, in some embodiments, have a comparatively smaller diameter than the tube, column, and / or cylinder of the gaseous separation zone.

[0066] The separation zone may comprise any of a variety of suitable materials. According to some embodiments, for example, the separation zone may comprise a metal, a metal alloy, a clad material, a ceramic, a plastic, a carbon-based material, and / or combinations thereof. Other materials are also possible. In certain embodiments, the separation zone material may be at least partially coated. For example, in some embodiments, the separation zone material is coated with a corrosion resistant material (e.g., a plastic coated with a corrosion resistant metal or alloy).

[0067] As an example, FIG. 2 depicts electrostatic separation zone 120 along gas flow pathway 105 receives intermediate product 205A and / or reactive component 105 from the absorption zone. Electrostatic separation zone 120 separates intermediate product 205A and / or reactive component 205 from the gas stream such that the gas stream exiting gas flow pathway 105 via outlet 105B contains a limited amount of intermediate product 205A and / or reactive component 205 entrained in the exiting gas stream. After intermediate product 205A is separated from the gas stream in electrostatic separation zone 120, intermediate product 205A can be collected to form mist-captured feedstock 205B.

[0068] In some embodiments, the separation zone separates at least a portion of the liquid mist from the gas stream to form a mist-captured feedstock. When liquid mist is introduced into the gas stream in the absorption zone, a reaction between the gaseous carbon dioxide and the liquid mist may produce an intermediate product in a mist form factor. After the gas stream passes through the separation zone, the intermediate product can, in some embodiments, be separated from the gas stream to form a mist-captured feedstock. That is, at least a portion of the mist- captured feedstock comprises the product of the reaction between the liquid mist and the gaseous carbon dioxide. In some embodiments, the mist-captured feedstock has essentially identical chemical components as the intermediate product in a different form factor (e.g. the intermediate products typically can exist as a mist in the gas flow pathway while the mist-captured feedstock can exist as a collected liquid derived from mist). In some embodiments, the intermediate product undergoes a chemical transformation and / or a chemical reaction to form the mist- captured feedstock. In some embodiments, the intermediate product does not undergo a chemical transformation and / or a chemical reaction to form the mist-captured feedstock (e.g. the form factor, not the chemical composition, of the mist-captured feedstock and the intermediate product can change).

[0069] According to some embodiments, the mist-captured feedstock may be advantageously used as a feedstock for conversion into at least one product. Mist-captured feedstock, as opposed to feedstock used for conversion captured via other means, may be particularly advantageous for conversion due to the mist-captured feedstock’s relatively high concentration. Additionally, the mist-captured feedstock, being in a liquid state rather than a gaseous state, does not need to undergo time and energy-intensive compression processes. Such compression processes often lead an unnecessary cost burden on the design and construction of carbon capture and conversion systems, and by eliminating the need of such compression processes, in some embodiments, the cost burden may be substantially reduced using a mist-captured feedstock in a liquid state.

[0070] In some embodiments, the mist-captured feedstock comprises potassium bicarbonate (KHCO3). In some embodiments, the mist captured feedstock comprises potassium bicarbonate in an amount greater than or equal to 1 wt.%, greater than or equal to 5 wt.%, greater than or equal to 10 wt.%, greater than or equal to 15 wt.%, greater than or equal to 20 wt.%, greater than or equal to 40 wt.%, greater than or equal to 60 wt.%, greater than or equal to 80 wt.%, or greater than or equal to 99 wt.%. In some embodiments, the mist captured feedstock comprises potassium bicarbonate in an amount less than or equal to 99 wt.%, less than or equal to 80 wt.%, less than or equal to 60 wt.%, less than or equal to 40 wt.%, less than or equal to 20 wt.%, less than or equal to 15 wt.%, less than or equal to 10 wt.%, less than or equal to 5 wt.%, or less than or equal to 1 wt.%. Combination of these ranges are also possible (e.g. greater than or equal to 1 wt.% and less than or equal to 99% wt.%). Other ranges are also possible. In some embodiments, the mist-captured feedstock comprises potassium carbonate (K2CO3). In some embodiments, the mist captured feedstock comprises potassium carbonate in an amount greater than or equal to 1 wt.%, greater than or equal to 5 wt.%, greater than or equal to 10 wt.%, greater than or equal to 15 wt.%, greater than or equal to 20 wt.%, greater than or equal to 40 wt.%, greater than or equal to 60 wt.%, greater than or equal to 80 wt.%, or greater than or equal to 99 wt.%. In some embodiments, the mist captured feedstock comprises potassium carbonate in an amount less than or equal to 99 wt.%, less than or equal to 80 wt.%, less than or equal to 60 wt.%, less than or equal to 40 wt.%, less than or equal to 20 wt.%, less than or equal to 15 wt.%, less than or equal to 10 wt.%, less than or equal to 5 wt.%, or less than or equal to 1 wt.%. Combination of these ranges are also possible (e.g. greater than or equal to 1 wt.% and less than or equal to 99% wt.%). Other ranges are also possible.

[0071] In some embodiments, the mist-captured feedstock has a pH. In some embodiments, the mist-captured feedstock has a pH greater than or equal to 8, greater than or equal to 9, greater than or equal to 10, greater than or equal to 11, greater than or equal to 12, greater than or equal to 13. In some embodiments, the mist-captured feedstock has a pH less than or equal to 14, less than or equal to 13, less than or equal to 12, less than or equal to 11, less than or equal to 10, less than or equal to 9, or greater than or equal to 8. Combination of these ranges are also possible (e.g. greater than or equal to 8 and less than or equal to 14). Other ranges are also possible.

[0072] According to some embodiments, the chemical properties of the mist-captured feedstock (e.g. pH, concentration, composition, etc.) can be tailored, tuned, or otherwise controlled to allow for relatively efficient conversion processes. That is, the mist-captured feedstock comprises properties that can be considered favorable and / or desirable for conversion of the mist-captured feedstock to at least one product. In some embodiments, as previously mentioned, the mist-captured feedstock can be highly concentrated. In some embodiments, the mist-captured feedstock can have pH that is amenable for conversion into at least one product.

[0073] According to some embodiments, the gaseous carbon dioxide from the gas stream can be converted into at least one product by the conversion apparatus. The conversion apparatus, in some embodiments, can be configured to receive a mist-captured feedstock. Once received, the conversion apparatus can convert the mist-captured feedstock into at least one product (e.g. carbon monoxide, ethanol, and / or ethylene). In some embodiments, the conversion apparatus is configured to expose at least some of the mist-captured feedstock to conditions that facilitate its conversion into at least one product. In some embodiments, the conversion apparatus is configured to expose at least some of the feedstock to conditions that facilitate its conversion into at least one product. Those of ordinary skill in the art will recognize, based on the totality of this disclosure, the conditions necessary to facilitate the conversion of the feedstock into at least one product. Such conditions may include and / or involve but are not limited to temperature, pressure, pH, electrical stimuli, and / or photo stimuli. The conditions, in some embodiments, may facilitate the conversion of the mist-captured feedstock into products at a rate and efficiency that may be advantageous compared to the conversion of other feedstocks from non-mist capture technologies under otherwise essentially identical conditions.

[0074] The conversion apparatus can comprise any of a myriad of devices configured to convert captured carbon dioxide. In some embodiments, the conversion apparatus comprises an electrochemical cell. In some embodiments, the electrochemical cell is configured to electrolyze the mist-captured feedstock. That is, the electrochemical cell may impart conditions to allow for the electrolysis of the mist-captured feedstock to produce at least one product. In some embodiments, the electrochemical cell is configured to facilitate carbonate electrolysis on the mist-captured feedstock.

[0075] The conversion apparatus, in some embodiments, can convert the mist-captured feedstock to at least one product despite not undergoing a stripping process (e.g. removal of gaseous carbon dioxide from the mist-captured feedstock via a stripper). Advantageously, the conversion apparatus does not require the feedstock to be stripped prior to conversion to at least one product. Accordingly, stripper columns, large towers that separate carbon dioxide from a captured feedstock, are no longer thereby reducing the overall cost and complexity of the integrated capture and conversion system. Stripper columns are typically a large additional expense for conventional, non-integrated capture and conversion systems. In some embodiments, the conversion apparatus can receive the mist-captured feedstock, separate gaseous carbon dioxide from the mist-captured feedstock and converts gaseous carbon dioxide into at least one product.

[0076] In some embodiments, the conversion apparatus comprises an inlet configured to receive the mist-captured feedstock. The conversion apparatus may be associated with the gas flow pathway. That is, the conversion apparatus may be fluidly connected to the gas flow pathway or the separation zone in a manner that allows the mist-captured feedstock at the separation zone to flow into the conversion apparatus. In some embodiments, auxiliary equipment may be necessary to ensure the mist-captured feedstock is directed into the conversion apparatus appropriately including but not limited to fluidic pumps, vacuums, tubing, valves, flow meters, and / or temperature sensors.

[0077] Any of a myriad of conversion apparatuses can be used. Those of ordinary skill in the art will recognize, based on the totality of this disclosure, that the conversion apparatus can efficiently convert mist-captured feedstock into at least one product in a manner that is amenable for scalable carbon dioxide conversion systems. Those of ordinary skill in the art will also recognize that the conditions that the mist-captured feedstock may be exposed to in the conversion apparatus can be controlled (e.g. modified) to implement carbon dioxide conversion via electrical energy, thermal energy, chemical energy, and / or other energy input. In some embodiments, the conversion apparatus is an electrochemical cell. In some embodiments, the electrochemical cell comprises a cathode, an anode, one or more catalysts (e.g., a Pt catalyst), and / or a membrane (e.g., an anion exchange membrane, a cation exchange membrane, a bipolar membrane). In some cases, the electrolyte solution that the electrochemical cell relies on is the mist-captured feedstock. Examples of electrochemical cells that may be used to convert the mist- captured feedstock into one or more products are shown in Example 1 and FIGS. 7 A and 8. In some embodiments, the anode comprises a gas diffusion layer (GDL) as shown in FIG. 7A (e.g., an ePTFE GDL).

[0078] As an example, FIG. 1 depicts integrated capture and conversion system 100 comprising conversion apparatus 125 fluidically connected to electrostatic separation zone 120. Conversion apparatus 125 is fluidically connected to electrostatic separation zone 120 via fluidic connector 130. In FIG. 2, conversion apparatus 125 receives mist-captured feedstock 205B and exposes mist-captured feedstock 205B to conditions that facilitate conversion into at least one product 210 that exit conversion apparatus 125 via conversion apparatus outlet 125A. In FIG. 3, a schematic of conversion apparatus 125 is shown. Mist captured feedstock 205B enters conversion apparatus 125 and is exposed to conditions that facilitate its conversion into at least one product 210. Mist-captured feedstock 205B can chemically transformed into aqueous carbon dioxide 305 and recycled reactive component 310. Aqueous carbon dioxide 305 can then be exposed to conditions that facilitate its conversion into at least one product 210. Recycled reactive component 310 can be collected and reused and / or repurposed.

[0079] The types of products that can produced by converting the mist-captured feedstock may be evident to a person of ordinary skill in the art. The feedstock can be converted to at least one product that, in some embodiments, are commercially and economically advantageous. For example, gaseous carbon dioxide may be captured and converted using the integrated system to produce products including but not limited to carbon monoxide, ethanol, and / or ethylene. Such products can be commercially valuable as precursors to various polymeric materials and / or as fuel for various combustion processes. Such products may also reduce and / or mitigate the limited the capital and / or energetic expenditures associated with carbon capture and conversion systems. Accordingly, the inventors have realized an integrated system capable of valorizing gaseous carbon dioxide emitted as a byproduct of combustion processes. In some embodiments, the at least one product comprises carbon monoxide (CO), formate (HCCL ), methanol (CHsOH), glyoxal (C2H2O2), methane (CH4), acetate (C2H3O2’), glycolaldehyde (C2H4O2), ethylene glycol (C2H6O2), acetaldehyde (C2H4O), ethanol (C2H6O), ethylene (C2H4), hydroxyacetone (C3H6O2), acetone (CsHeO), allyl alcohol (CaHeO, propionaldehyde (C3H6O), and / or 1-proponal (CsHsO). In some embodiments, gaseous carbon dioxide may be captured and converted back into gaseous carbon dioxide for subsequent use and / or storage. That is, the gaseous carbon dioxide may react mist comprising the sorbent (e.g., KOH) and separated from the gas flow pathway to form the mist-captured feedstock. The feedstock may then be fed into the conversion apparatus which converts the feedstock back into gaseous carbon dioxide for subsequent use. In some embodiments, the conversion apparatus separated the carbon dioxide from the mist-captured feedstock for subsequent use.

[0080] In some embodiments, the conversion apparatus is configured to convert the mist- captured feedstock into at least one product at a relatively high rate. In some embodiments, the conversion apparatus is configured to convert the mist-captured feedstock into at least one product at a rate greater than or equal to 10 mL / min, greater than or equal to 50 mL / min, greater than or equal to 100 mL / min, greater than or equal to 500 mL / min, greater than or equal to 1000 mL / min, greater than or equal to 2 L / min, greater than or equal to 5 L / min, greater than or equal to 10 L / min, or greater than or equal to 50 L / min. In some embodiments, the conversion apparatus is configured to convert the mist-captured feedstock into at least one product at a rate less than or equal to 50 L / min, less than or equal to 10 L / min, less than or equal to 5 L / min, less than or equal to 2 L / min, less than or equal to 1000 mL / min, less than or equal to 500 mL / min, less than or equal to 100 mL / min, less than or equal to 50 mL / min, or less than or equal to 10 mL / min. Combinations of these ranges are possible (e.g. greater than or equal to 10 mL / min and less than or equal to 50 L / min). Other ranges are also possible.

[0081] In some embodiments, the conversion apparatus converts the mist-captured feedstock into at least one product at a conversion efficiency. In some embodiments, the conversion efficiency, expressed as a percent, can be calculated by dividing the amount of product produced by the conversion apparatus by the amount of feedstock received by the conversion apparatus and multiplying the quotient by 100. In some embodiments, the conversion efficiency is greater than or equal to 0.5%, greater than or equal to 1.0%, greater than or equal to 1.5%, greater than or equal to 2.0%, greater than or equal to 2.5%, greater than or equal to 3.0%, greater than or equal to 3.5%, greater than or equal to 4.0%, greater than or equal to 4.5%, greater than or equal to 5%, greater than or equal to 10%, greater than or equal to 15%, greater than or equal to 20%, greater than or equal to 25%, greater than or equal to 30%, greater than or equal to 40%, greater than or equal to 50%, greater than or equal to 75%, or greater than or equal to 99% conversion efficiency. In some embodiments, the conversion efficiency is less than or equal to 99%, less than or equal to 75%, less than or equal to 50%, less than or equal to 40%, less than or equal to 30%, less than or equal to 25%, less than or equal to 20%, less than or equal to 15%, less than or equal to 10%, less than or equal to 5%, less than or equal to 4.5%, less than or equal to 4%, less than or equal to 3.5%, less than or equal to 3.0%, less than or equal to 2.5%, less than or equal to 2.0%, less than or equal to 1.5%, less than or equal to 1.0%, or less than or equal to 0.5% conversion efficiency. Combinations of these ranges are possible (e.g. greater than or equal to 0.5% and less than or equal to 99%). Other ranges are also possible.

[0082] In some embodiments, the conversion apparatus can convert the mist-captured feedstock into at least one product a conversion rate. In some embodiments, the conversion rate depicts the amount of product produced by the conversion apparatus per unit time. In some embodiments, the conversion rates can be at least 0.1 grams of product per hour, at least 1 grams of product per hour, at least 10 grams of product per hour, at least 100 grams of product per hour, at least 1 kilograms of product per hour, at least 10 kilograms of product per hour, or at least 100 kilograms of product per hour.

[0083] PCT Application No. PCT / US2022 / 048105, filed October 27, 2022, and entitled “Systems and Methods for Removing Species from Gas Streams,” is incorporated herein by reference in its entirety for all purposes.

[0084] The following examples are intended to illustrate certain embodiments of the present invention, but do not exemplify the full scope of the invention.

[0085] EXAMPLE 1

[0086] In this example, a capture system is demonstrated that operates using a relatively high concentration of potassium hydroxide (KOH) and a relatively low concentration of potassium carbonate. Air containing 400 ppm of carbon dioxide was directed into a chamber and exposed to a carbon capture sorbent (e.g., KOH), as shown in FIG. 6A. The carbonate loading of the sorbent was varied to determine the effect of carbonate loading on capture rate. As the air flowed out of the chamber, the concentration of carbon dioxide was measured using a infrared carbon dioxide sensor. By measuring the carbon dioxide concentration of the air flowing out of the chamber, it is possible to determine the carbonate loading of the carbon capture sorbent. The carbonate loading generally refers to the degree of carbonation of the sorbent (e.g., KOH), and can be expressed according to equation 1. 2 • [CO32-]

[0087] Carbonate Loading = — — — : — Equation 1

[0088] I J

[0089] FIG. 6B shows the effect of carbonate loading on capture rate of carbon dioxide when exposed to a sorbent. Accordingly, the steady state carbon dioxide capture rate is a function of the carbonate loading, as sorbents having higher carbonate concentration generally capture carbon dioxide at a slower rate. The relative absorption rate is plotted as a function of carbonate loading of the sorbent in FIG. 6C. As the carbonate loading of the sorbent increases, the absorption rate of carbon dioxide decreases (See I and II of FIG. 6C). Without wishing to be bound by any particular theory, at relatively high carbonate concentrations, the sorbent may not have sufficient reactive hydroxide groups to capture additional carbon dioxide. On the other hand, at relatively low carbonate loadings, carbon dioxide may readily react with hydroxide groups within the sorbent allowing for carbon dioxide to be captured at relatively high rates. The relatively poor absorption rate for highly carbonate solutions poses a significant integration challenge with a subsequent electrochemical conversion step, because, while relatively high carbonate loadings are desirable for electrochemical conversion, the low absorption rate of such sorbents may reduce the overall throughput of the system.

[0090] Conversion systems (e.g., electrochemical conversion systems) generally operate at relatively efficiencies using feedstock having high carbonate loading. As shown in FIG. 7A, an electrochemical cell was demonstrated to determine the conversion efficiency of a carbonate feedstock as a function of carbonate loading. The cell shown in FIG. 7A relies on a hydrogen looping mechanism, but other mechanisms (e.g., water electrolysis, bipolar membrane electrodialysis, active material such as Bismuth, organic redox materials, etc.) are also possible. The electrochemical cell of FIG. 7A receives a solution of carbonate, hydroxide, and optionally bicarbonate and exposed the solution to an electric field. Under the electric field, the anions are pulled over the anion exchange membrane (AEM) to the anode of the electrochemical cell. The anions then react with protons released from the electrochemical reaction. In the case of carbonate and / or bicarbonate, carbon dioxide is released thereby completing the carbon dioxide capture process. The cathode releases hydroxides which can then be used to capture more carbon dioxide when transported to the capture system. The effluent of the electrochemical cell may be returned to the capture stage to complete a cycle of the capture-conversion process. Generally, migration of hydroxides reduce current efficiency, as water is undesirable compared to the production of carbon dioxide. As shown in FIG. 7B, the current efficiency of the electrochemical shown in FIG. 7A increases with increased carbonate loading. At relatively low carbonate loadings, the production water is favored over the production of carbon dioxide, whereas at relatively high carbonate loadings, the production of carbon dioxide is favored over the production of water. Accordingly, the electrochemical cell of 7A may convert carbonate and / or bicarbonate solutions into gaseous carbon dioxide, as opposed to other conversion products (e.g., carbon monoxide, ethylene, ethanol).

[0091] As shown in FIG. 8A, an electrochemical cell comprising an anode, cathode, and cation exchange membrane (CEM) is shown. Such an electrochemical is capable of converting carbonate and / or bicarbonate solutions into one or more conversion products (e.g., carbon monoxide, ethylene, ethanol). This electrochemical cell is configured to receive a mist-captured feedstock comprising carbonate, hydroxide, and, optionally, bicarbonate. Under an electric field, protons generated at the anode are pulled over the CEM to the catholyte chamber and react with any anions that are present (e.g., carbonate and / or bicarbonate ions). While a cation exchange membrane is used in this example, other membranes, including but not limited to a bipolar exchange membrane may be used. This reactions leads to the formation of carbon dioxide which may be in an aqueous dissolved phase or a bulk gas phase. The carbon dioxide is then electrochemically reduced at the cathode thereby producing one or more derivative products (e.g., carbon monoxide, ethanol, ethylene). The effluent of the catholyte is then recirculated to the capture stage (e.g., mist capture) to complete the cycle. In some cases, separation of products from the catholyte effluent may be necessary prior to recirculation.

[0092] By increasing the capture rate of carbon dioxide, it may be possible at least partially remedy the challenges related to integrating carbon capture systems with carbon conversion systems. The system described herein uses mists of micrometric droplets to expose the carbon dioxide to liquid sorbent which thereby increases the gas-liquid interfacial area. The specific interfacial area of mist can be described equation 2:

[0093] SA Pq L 6

[0094] - = - r • — Equation 2 Vtot Pi G 6 where SA is the liquid-gas surface area, V_tot is the total volume, pgis the gas density, ptis the liquid density, is the ratio of liquid mass flow rate to gas mass flow rate into the capture vessel, and 8 is the surface-area- weighted mean diameter of the mist droplets. For a typical - of 2, and a droplet size of 10 microns, an interfacial area per volume of 1,500 m2 / m3is achieved, relatively higher than conventional packed beds, which have around 250m2 / m3. Use of mists to capture carbon dioxide may have surprising synergies with direct electrochemical conversion performed on sorbents containing captured carbon dioxide. As shown in FIGS. 9A-9C, mist can effectively capture gaseous carbon dioxide at relatively high rates. By capturing carbon dioxide at high rates using mist capture, it is possible to rely on sorbents that have a high carbonate concentration for efficient electrochemical separation and / or conversion. This resolves a key issue in the economic viability of the process. Mist capture can lead to increased surface areas and increased capture rates, which in turn allow for the economical capture of a more carbonated sorbent, which in turn increases the efficiency of the subsequent electrochemical CO2 separation or electrochemical conversion to products.

[0095] While several embodiments of the present invention have been described and illustrated herein, those of ordinary skill in the art will readily envision a variety of other means and / or structures for performing the functions and / or obtaining the results and / or one or more of the advantages described herein, and each of such variations and / or modifications is deemed to be within the scope of the present invention. More generally, those skilled in the art will readily appreciate that all parameters, dimensions, materials, and configurations described herein are meant to be exemplary and that the actual parameters, dimensions, materials, and / or configurations will depend upon the specific application or applications for which the teachings of the present invention is / are used. Those skilled in the art will recognize, or be able to ascertain using no more than routine experimentation, many equivalents to the specific embodiments of the invention described herein. It is, therefore, to be understood that the foregoing embodiments are presented by way of example only and that, within the scope of the appended claims and equivalents thereto, the invention may be practiced otherwise than as specifically described and claimed. The present invention is directed to each individual feature, system, article, material, and / or method described herein. In addition, any combination of two or more such features, systems, articles, materials, and / or methods, if such features, systems, articles, materials, and / or methods are not mutually inconsistent, is included within the scope of the present invention.

[0096] The indefinite articles “a” and “an,” as used herein in the specification and in the claims, unless clearly indicated to the contrary, should be understood to mean “at least one.”

[0097] The phrase “and / or,” as used herein in the specification and in the claims, should be understood to mean “either or both” of the elements so conjoined, i.e., elements that are conjunctively present in some cases and disjunctively present in other cases. Other elements may optionally be present other than the elements specifically identified by the “and / or” clause, whether related or unrelated to those elements specifically identified unless clearly indicated to the contrary. Thus, as a non-limiting example, a reference to “A and / or B,” when used in conjunction with open-ended language such as “comprising” can refer, in one embodiment, to A without B (optionally including elements other than B); in another embodiment, to B without A (optionally including elements other than A); in yet another embodiment, to both A and B (optionally including other elements); etc.

[0098] As used herein in the specification and in the claims, “or” should be understood to have the same meaning as “and / or” as defined above. For example, when separating items in a list, “or” or “and / or” shall be interpreted as being inclusive, i.e., the inclusion of at least one, but also including more than one, of a number or list of elements, and, optionally, additional unlisted items. Only terms clearly indicated to the contrary, such as “only one of’ or “exactly one of,” or, when used in the claims, “consisting of,” will refer to the inclusion of exactly one element of a number or list of elements. In general, the term “or” as used herein shall only be interpreted as indicating exclusive alternatives (i.e. “one or the other but not both”) when preceded by terms of exclusivity, such as “either,” “one of,” “only one of,” or “exactly one of.” “Consisting essentially of,” when used in the claims, shall have its ordinary meaning as used in the field of patent law.

[0099] As used herein in the specification and in the claims, the phrase “at least one,” in reference to a list of one or more elements, should be understood to mean at least one element selected from any one or more of the elements in the list of elements, but not necessarily including at least one of each and every element specifically listed within the list of elements and not excluding any combinations of elements in the list of elements. This definition also allows that elements may optionally be present other than the elements specifically identified within the list of elements to which the phrase “at least one” refers, whether related or unrelated to those elements specifically identified. Thus, as a non-limiting example, “at least one of A and B” (or, equivalently, “at least one of A or B,” or, equivalently “at least one of A and / or B”) can refer, in one embodiment, to at least one, optionally including more than one, A, with no B present (and optionally including elements other than B); in another embodiment, to at least one, optionally including more than one, B, with no A present (and optionally including elements other than A); in yet another embodiment, to at least one, optionally including more than one, A, and at least one, optionally including more than one, B (and optionally including other elements); etc.

[0100] Some embodiments may be embodied as a method, of which various examples have been described. The acts performed as part of the methods may be ordered in any suitable way. Accordingly, embodiments may be constructed in which acts are performed in an order different than illustrated, which may include different (e.g., more or less) acts than those that are described, and / or that may involve performing some acts simultaneously, even though the acts are shown as being performed sequentially in the embodiments specifically described above.

[0101] In the claims, as well as in the specification above, all transitional phrases such as “comprising,” “including,” “carrying,” “having,” “containing,” “involving,” “holding,” and the like are to be understood to be open-ended, i.e., to mean including but not limited to. Only the transitional phrases “consisting of’ and “consisting essentially of’ shall be closed or semi-closed transitional phrases, respectively, as set forth in the United States Patent Office Manual of Patent Examining Procedures, Section 2111.03.

Claims

CLAIMSWhat is claimed is:

1. An integrated system for converting gaseous carbon dioxide into at least one product, comprising: a gas flow pathway having an inlet for receiving a gas stream comprising gaseous carbon dioxide and an outlet for releasing the gas stream containing less of the gaseous carbon dioxide than is contained in the gas stream at the inlet; a gaseous carbon dioxide absorption zone along the gas flow pathway; a source of a liquid mist configured to introduce the liquid mist into the gaseous carbon dioxide absorption zone, wherein the gaseous carbon dioxide absorption zone is configured to expose the liquid mist to the gas stream under conditions facilitating transfer of at least some of the gaseous carbon dioxide from the gas stream to the mist; an electrostatic separation zone along the gas flow pathway, fluidly connected to the gaseous carbon dioxide separation zone and configured to electrostatically separate at least some of the liquid mist from the gas stream to form a mist-captured feedstock; and a conversion apparatus configured to receive the mist-captured feedstock and expose at least some of the feedstock to conditions that facilitate the conversion of the feedstock into at least one product.

2. An integrated system for converting gaseous carbon dioxide into at least one product, comprising: a separation zone, fluidically connected to a gas flow pathway, configured to separate at least a portion of liquid mist from a gas stream flowing through the gas flow pathway; and a conversion apparatus configured to receive a mist-captured feedstock and expose at least some of the mist-captured feedstock to conditions that facilitate its conversion into at least one product, wherein the liquid mist is configured to at least partially react with the gaseous carbon dioxide in the gas stream to form the mist-captured feedstock.

3. A method for converting gaseous carbon dioxide into at least one product, comprising:exposing a gas stream, comprising gaseous carbon dioxide, in a gas flow pathway to a liquid mist, wherein a reactive component of the liquid mist is configured to at least partially react with the gaseous carbon dioxide; in a gaseous carbon dioxide absorption zone, reacting the reactive component and the gaseous carbon dioxide to produce a mist-captured feedstock; in a separation zone fluidly connected to the gaseous carbon dioxide absorption zone, separating at least some of the liquid mist and / or the mist-captured feedstock from the gas stream; and feeding the mist-captured feedstock into a conversion apparatus configured to expose at least some of the mist-captured feedstock to conditions that facilitate its conversion into at least one product.

4. A system or method as in any one of the preceding claims, wherein the conversion apparatus is configured to convert the mist-captured feedstock product into at least one product at a rate greater than or equal to 10 mL / min.

5. A system or method as in any one of the preceding claims, wherein the mist- captured feedstock comprises potassium bicarbonate (KHCO3) and / or potassium carbonate (K2CO3).

6. A system or method as in any one of the preceding claims, wherein the mist- captured feedstock comprises potassium bicarbonate (KHCO3) in an amount greater than or equal to 1 wt.%.

7. A system or method as in any one of the preceding claims, wherein the mist- captured feedstock comprises potassium carbonate (K2CO3) in an amount greater than or equal to 1 wt.%.

8. A system or method as in any one of the preceding claims, wherein the mist- captured feedstock has a pH between 8 and 14.

9. A system or method as in any one of the preceding claims, wherein the overall energy consumption of theintegrated system is less than or equal to 1000 kilojoules per mole of the carbon dioxide.

10. A system or method as in any one of the preceding claims, wherein the conversion apparatus converts the mist-captured feedstock into at least one product via electrolysis.

11. A system or method as in any one of the preceding claims, wherein the liquid mist is electrostatically separated from the gas stream.

12. A system or method as in any one of the preceding claims, wherein the conversion apparatus comprises an electrochemical cell.

13. A system or method as in any one of the preceding claims, wherein the at least one product comprises carbon monoxide (CO), ethanol (C2H6O), and / or ethylene (C2H4).

14. A system or method as in any one of the preceding claims, wherein the gas flow pathway comprises an inlet for receiving a gas stream comprising gaseous carbon dioxide and an outlet for releasing the gas stream containing less of the gaseous carbon dioxide than is contained in the gas stream at the inlet.

15. A system or method as in any one of the preceding claims, wherein the liquid comprises potassium hydroxide (KOH).

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