Atmospheric carbon dioxide trapping system

Abstract

A system for capturing atmospheric CO2 includes a reaction reactor having a solid adsorbent; and a mineralization reactor downstream of the reaction reactor, the system having three states, including a first state in which CO2 is sequestered from air into a solid sorbent in the reaction reactor; a second state of releasing sequestered CO2 from the sorbent in the reaction reactor by contacting the CO2-enriched sorbent with an exchange fluid having one or more amino acids and forming a CO2-enriched exchange fluid; and a third state of reacting the sequestered CO2 from the CO2-enriched exchange fluid with a basic feedstock in the mineralization reactor to form carbonate while regenerating the exchange fluid.

Description

Technical Field

[0001] This disclosure relates to systems and methods for capturing atmospheric carbon dioxide (CO2) using a solid adsorbent, regenerating the solid adsorbent using an exchange fluid, and regenerating the exchange fluid in an in-situ CO2 conversion reactor. Background Technology

[0002] CO2 is a notorious greenhouse gas, and its emissions have risen dramatically since the start of the Industrial Revolution in the 18th century. Since then, CO2 emissions have been proven to be a major culprit in global climate change. Recent findings from the International Commission on Climate Change have suggested that CO2 emissions should be halved by 2030 to avoid further negative impacts on the planet. Various technologies have been developed to capture CO2, such as atmospheric CO2, but their limitations hinder the realization of wider CO2 sequestration. Summary of the Invention

[0003] In one or more embodiments, a direct air capture (DAC) system for CO2 is disclosed. The system may include a reactor with a solid adsorbent; and a mineralization reactor downstream of the reactor. The system has three states, including a first state in which CO2 is sequestered from air into the solid adsorbent in the reactor; a second state in which the sequestered CO2 is released from the adsorbent by contacting the CO2-enriched adsorbent with an exchange fluid containing one or more amino acids to form a CO2-enriched exchange fluid; and a third state in which the sequestered CO2 from the CO2-enriched exchange fluid is reacted with an alkaline feedstock in the mineralization reactor to form a carbonate while regenerating the exchange fluid. The solid adsorbent may be amine-functionalized. The exchange fluid may also include a base, alcohol, amine, or a combination thereof. The alkaline feedstock may include a calcium-rich material. The regenerated exchange fluid may be returned to the reactor in the first state for the next CO2 sequestration cycle. The third state can be operated at ambient temperature. The one or more amino acids may include the L-form of the one or more amino acids. The second state may end when the exchange fluid reaches a predetermined saturation point.

[0004] In another embodiment, a direct air capture (DAC) system for CO2 is disclosed. The system may include: a reaction reactor comprising a solid amine-functionalized adsorbent with an affinity for CO2; a first inlet for air having a first concentration of CO2; a first outlet for air having a second concentration of CO2, the second concentration being lower than the first concentration; a mineralization reactor fluidly connected to the reaction reactor, the mineralization reactor comprising an alkaline feedstock source; and an exchange fluid comprising one or more amino acids circulating between the reaction reactor and the mineralization reactor. The exchange fluid may also comprise a base, an alcohol, an amine, or a combination thereof. The one or more amino acids may include L-arginine. The alkaline feedstock may include calcium-rich materials. The alkaline feedstock may include industrial waste. The adsorbent is mobile within the reaction reactor.

[0005] In another embodiment, a direct air capture (DAC) system for CO2 is disclosed. This system may include a reaction reactor with a solid amine-functionalized adsorbent configured to capture CO2 from the air; an in-situ mineralization reactor that reacts the captured CO2 with an alkaline feedstock to produce a carbonate having carbon atoms from the captured CO2 via a mineralization reaction; and an exchange fluid configured to transport the captured CO2 from the reaction reactor to the in-situ mineralization reactor. The exchange fluid may include one or more amino acids. The alkaline feedstock may include CaO. The carbonate may be CaCO3. The exchange fluid may be recycled between the reaction reactor and the mineralization reactor based on a predetermined level of CO2 saturation. The system may be a continuous operating system. Attached Figure Description

[0006] Figure 1 This is a schematic diagram of a non-limiting example of an atmospheric CO2 capture system; Figure 2 This is a schematic diagram of a variation of a non-limiting exemplary atmospheric CO2 capture system according to one or more embodiments disclosed herein; Figure 3 This is a schematic diagram of another variation of a non-limiting exemplary atmospheric CO2 capture system according to one or more embodiments disclosed herein; and Figure 4 This is a schematic diagram of another variation of a non-limiting exemplary atmospheric CO2 capture system according to one or more embodiments disclosed herein. Detailed Implementation

[0007] This document describes embodiments of the present disclosure. However, it should be understood that the disclosed embodiments are merely examples, and other embodiments may take various and alternative forms. These figures are not necessarily to scale; certain features may be enlarged or minimized to show details of specific components. Therefore, the specific structural and functional details disclosed herein should not be construed as limiting, but merely as a representative basis for teaching those skilled in the art to use the embodiments in different ways. As will be understood by those skilled in the art, various features illustrated and described with reference to any of the figures can be combined with features illustrated in one or more other figures to produce embodiments not explicitly illustrated or described. The combinations of features shown provide representative embodiments for typical applications. However, various combinations and modifications of features consistent with the teachings of this disclosure may be desired for a particular application or implementation.

[0008] Unless explicitly stated by example or otherwise, all numerical quantities indicating the amount of material or reaction conditions and / or uses in this specification should be understood to be modified by the word “about” when describing the broadest scope of this disclosure. Practice is generally preferred within the specified numerical limits. Furthermore, unless explicitly stated to the contrary: percentages, “parts”, and ratio values ​​are all by weight; describing a group or class of materials as suitable or preferred for a given purpose related to this disclosure means that a mixture of any two or more members of that group or class is equally suitable or preferred; descriptions of components in chemical terms refer to the components when added to any combination specified in the specification and do not necessarily exclude chemical interactions between the components of the mixture once mixed. Unless otherwise stated, weight % is based on the total weight of the substrate, and volume % is based on the total volume of the substrate.

[0009] The initial definition of an acronym or other abbreviation applies to all subsequent uses of the same abbreviation herein, and with necessary modifications, to the regular grammatical variations of the originally defined abbreviation. Unless explicitly stated to the contrary, the measurement of a property is determined by the same technique referenced previously or later for the same property.

[0010] It should also be noted that, as used in the specification and appended claims, the singular forms “an,” “a,” and “the” include plural references unless the context clearly indicates otherwise. For example, references to a singular component are intended to include multiple components.

[0011] As used herein, the terms “basic,” “approximately,” or “about” mean that the quantity or value in question can be a specified particular value or some other value nearby. Typically, the term “about” indicating a particular value is intended to indicate a range within + / - 5% of that value. As an example, the phrase “about 100” indicates a range of 100 + / - 5, i.e., from 95 to 105. Generally, when the term “about” is used, similar results or effects according to this disclosure can be expected within + / - 5% of the indicated value. The term “basic” may modify a value or related feature disclosed or claimed in this disclosure. In this case, “basic” may mean that the value or related feature it modifies is within ±0%, 0.1%, 0.5%, 1%, 2%, 3%, 4%, 5%, or 10% of that value or related feature.

[0012] It should also be understood that the range of integers explicitly includes all integers in between. For example, the range of integers 1-10 explicitly includes 1, 2, 3, 4, 5, 6, 7, 8, 9, and 10. Similarly, the range 1 to 100 includes 1, 2, 3, 4…97, 98, 99, 100. Similarly, when any range is required, the intermediate number, which is the increment of the difference between the upper and lower limits divided by 10, can be taken as an alternative upper or lower limit. For example, if the range is 1.1 to 2.1, the subsequent numbers 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9, and 2.0 can be chosen as the lower or upper limit. Similarly, whenever an enumerated list of integers is provided herein, it should also be understood that the enumeration of integers explicitly includes the range of any two integers within the enumeration.

[0013] In the examples described herein, concentration, temperature, and reaction conditions (e.g., pressure, pH, flow rate, etc.) can be implemented using the values ​​provided in the examples, rounded or rounded to two significant figures, plus or minus 50%. In one improvement, concentration, temperature, and reaction conditions (e.g., pressure, pH, flow rate, etc.) can be implemented using the values ​​provided in the examples, rounded or rounded to two significant figures, plus or minus 30%. In another improvement, concentration, temperature, and reaction conditions (e.g., pressure, pH, flow rate, etc.) can be implemented using the values ​​provided in the examples, rounded or rounded to two significant figures, plus or minus 10%.

[0014] As used herein, the term "and / or" means that either all or only one element of the group may be present. For example, "A and / or B" means "A only, or B only, or both A and B". In the case of "A only", the term also covers the possibility that B is not present, i.e., "A only, without B".

[0015] It should also be understood that this disclosure is not limited to the specific embodiments and methods described below, as specific components and / or conditions may vary. Furthermore, the terminology used herein is for the purpose of describing specific embodiments of this disclosure only and is not intended to be limiting in any way.

[0016] The term “comprising” is synonymous with “including,” “having,” “containing,” or “characterized as.” These terms are inclusive and open-ended and do not exclude additional, unlisted elements or method steps. The terms “including” or “includes” may cover the phrases “comprising,” “consisting of,” or “substantially consisting of.”

[0017] The phrase “consisting of” excludes any element, step, or component not specified in the claim. When this phrase appears in a body clause of a claim rather than immediately following the preamble, it only limits the element set forth in that clause; other elements are not excluded from the claims as a whole.

[0018] The phrase “consistent essentially of…” limits the scope of the claim to the specified material or step, plus the material or step that does not materially affect one or more of the essential and novel features of the claimed subject matter.

[0019] Regarding the terms “comprising,” “consisting of,” and “substantially composed of,” when one of these three terms is used herein, the subject matter disclosed herein may include the use of any of the other two terms.

[0020] The terms "one or more" mean "at least one," and "at least one" means "one or more." The terms "one or more" and "at least one" include "multiple" as a subset.

[0021] Describing a group or class of materials as suitable for a given purpose in conjunction with one or more embodiments means that a mixture of any two or more members of that group or class is appropriate. Furthermore, describing a group or class of materials as suitable for a given purpose in conjunction with one or more embodiments means that the materials of said group or class may “contain” any or all of the materials of said group or class, “compose of” and / or “substantially constitute” them. The initial definition of acronyms or other abbreviations applies to all subsequent uses of the same abbreviation herein and, where necessary, to the normal grammatical variations of the abbreviations in their initial definitions. Unless expressly stated to the contrary, the measurement of a property is determined by the same technique referenced previously or later for the same property.

[0022] Unless otherwise defined, the term "alkyl" refers to a monovalent alkane-derived group containing 1 to 100 carbon atoms, more preferably 1 to 40 carbon atoms, or even more preferably 1 to 20 carbon atoms. Alkyl groups can be linearly arranged, branched, or cyclic. A branched alkyl group is an alkyl group in which the alkyl group is attached to a straight-chain alkyl chain. Alkyl groups can be saturated or unsaturated hydrocarbons. In other words, alkyl can refer to alkenyl or ynyl. A saturated hydrocarbon is a hydrocarbon containing a single bond, while an unsaturated hydrocarbon is a hydrocarbon containing one or more double or triple bonds. Examples of alkyl groups include, but are not limited to, methyl, ethyl, propyl, isopropyl, butyl, isobutyl, sec-butyl, tert-butyl, pentyl, hexyl, octyl, vinyl, propynyl, butynyl, pentenyl, hexenyl, octenyl, butadienyl, propynyl, butynyl, pentynyl, hexynyl, and propadienyl groups. Alkyl groups can also include cycloalkyl groups, such as cyclopropyl, cyclopentyl, or cyclohexyl. Alkyl is intended to include its isomers. An alkyl group may be substituted with multiple substituents. Substituents may refer to non-hydrogen groups. For example, substituents may be, but are not limited to, halogens, hydroxyl groups, alkoxy groups, acetyl groups, phenyl groups, amino groups, heteroatom or heteroatomic groups.

[0023] The term "alkoxy" refers to alkyl ethers or aryl ethers, such as methoxy, ethoxy, n-propoxy, isopropoxy, n-butoxy, isobutoxy, sec-butoxy, tert-butoxy, and phenoxy.

[0024] The term "aryl" refers to a carbon-containing aromatic ring, such as a phenyl group, and a heteroaryl group refers to a carbon ring in which at least one carbon atom is replaced by a heteroatom, such as a nitrogen atom, an oxygen atom, or a sulfur atom.

[0025] The term "alkylaryl" refers to an aryl group in which at least one hydrogen group is replaced by an alkyl group.

[0026] The term “amino” or “amine” refers to the group -NR'R” (or NRR'R”), where R, R' and R” are independently selected from hydrogen, alkyl, aryl, alkylaryl or heteroaryl.

[0027] Unless otherwise stated, the term "R" may refer to hydrogen, alkyl, aryl, alkylaryl, heteroatom, alkoxy, or heteroaryl.

[0028] Many aim for net-zero global carbon emissions to avoid, prevent, or mitigate human impacts on the climate. One developing technology that can be used to achieve carbon emission reduction is carbon capture, utilization, and storage (CCUS). Conventionally, this involves the process of separating carbon emissions, such as CO2, for storage or further utilization before they are released into the atmosphere; this can also be called point-source carbon capture or source-point carbon capture. These technologies typically rely on high concentrations of CO2 at the carbon emission source. For example, these technologies may be common in oil and gas companies or energy companies involved in the extraction and / or combustion of fossil fuels. For example, flue gas can be a point source of carbon emissions. Source-point technologies can be incorporated into certain combustion technologies or are better suited to existing industrial facilities such as power plants.

[0029] Alternatively, atmospheric carbon capture or direct air capture (DAC) of carbon emissions (such as CO2) can be used to offset emissions from industries where reductions or prevention of releases may be more difficult (i.e., industries where emissions are harder to reduce), such as transportation (e.g., shipping and aviation). In some respects, DAC can be more challenging because it involves extracting carbon emissions, such as CO2, under environmental conditions (e.g., temperature, pressure, concentration) far below those of point-of-use technologies. The differences between point-of-use and DAC often make point-of-use technologies unsuitable for DAC, and vice versa. For example, technologies used for point-of-use capture may have slow kinetics under environmental conditions, making them inefficient or ineffective for DAC. Furthermore, storing and / or further utilizing captured carbon (e.g., CO2) is often limited to point-of-use capture because effectively extracting sufficient quantities from ambient air makes storage and further utilization difficult and / or expensive. In yet another instance, DAC technologies can be implemented as large-scale facilities, while point-of-use technologies can be adapted to existing facilities. In any case, significant advancements in these technologies make them more promising for ultimately achieving carbon neutrality. For example, U.S. Patent Application No. 18 / 162,326, filed January 31, 2023, describes some advancements in DAC, the entire contents of which are hereby incorporated by reference.

[0030] Traditional CO2 capture involves the use of liquid adsorbents, particularly amine-based solutions. Monoethanolamine (MEA) is the benchmark solvent due to its high reactivity with CO2. However, traditional amine solvents have several significant drawbacks. Liquid amine solvents require high energy consumption for regeneration, and the process of releasing captured CO2 from the amine solution typically involves applying heat, which can account for a considerable portion of the total energy consumption of the CO2 capture process. This high energy requirement reduces the overall efficiency of the system and increases operating costs. The combined effects of high energy consumption, corrosion, and solvent degradation result in high overall operating costs for using liquid amines for CO2 capture. These costs can be a major obstacle to the widespread adoption of this technology, especially for industries with narrow profit margins.

[0031] Solid amine adsorbents and amine stripping techniques used for regeneration are generally incompatible. Thus, solid adsorbents (e.g., metal-organic frameworks, zeolites, or other porous materials) are typically limited to DAC (Distillation-Drying) technologies, while liquid storage is generally limited to source-point technologies. For example, solid adsorbent technologies have been tested with thermal regeneration techniques. However, heating and pressurizing regeneration techniques can be inefficient and / or lead to degradation of the stored material, resulting in a limited lifetime. Liquid technologies may also exhibit slow kinetics at low temperatures, low pressures, and / or low concentrations, making them unsuitable for environmental conditions.

[0032] Therefore, conventional carbon capture technologies need improvement because they can be inefficient, costly, involve expensive or rare materials, and / or include many drawbacks, such as those discussed above. For example, some challenges include energy requirements for regeneration, limited lifetime, scale of deployment, material cost, and material degradation. Degradation of adsorbent materials during carbon capture is a significant challenge affecting the overall efficiency and cost-effectiveness of carbon capture methods. Factors such as exposure to contaminants, high temperatures, and the cyclical nature of the capture and release processes can lead to physical and chemical changes in adsorbent materials, resulting in reduced CO2 capture capacity and selectivity. Contaminants present in flue gas or ambient air, such as sulfur compounds and particulate matter, can interact with adsorbent materials, leading to fouling and performance degradation over time. Furthermore, the high temperatures and pressures during the regeneration step can cause mechanical stress and thermal degradation of the adsorbent materials. These costs can be a major obstacle to the widespread adoption of this technology, especially for industries with narrow profit margins.

[0033] Furthermore, in terms of utilization and storage, CO2 emissions captured through conventional carbon capture technologies are generally not directly usable as valuable products, and currently only a few specific applications are available. Beyond the implementation of carbon credits, more sustainable and economically viable methods for generating revenue from atmospheric CO2 removal include converting captured CO2 into more useful and marketable end products. These end products include carbon monoxide (CO), formic acid, methanol, and various other carbon-based substances. By converting CO2 into valuable chemicals, industries can generate revenue streams that help offset the costs associated with carbon capture methods. For example, methanol can be used as a fuel or feedstock in chemical manufacturing, while formic acid has applications in agriculture and leather production. On the other hand, carbon monoxide is a key component in synthetic fuel production and various industrial processes. Carbonates can be used in various industries, such as construction or fertilizers.

[0034] Traditionally, to efficiently convert CO2 into a useful final product, captured emissions must first be purified, pressurized, and transported to a conversion facility. Each of these steps incurs additional costs, losses, and challenges. Purifying CO2 is the step required to remove impurities that may hinder the efficiency of subsequent chemical reactions. This process typically involves advanced filtration and separation technologies, which can be energy-intensive and expensive. Once purified, the CO2 must be pressurized to facilitate its transport and subsequent chemical conversion. Pressurization requires a significant energy input, increasing the overall cost and carbon footprint of the process. Transporting CO2 to the conversion facility presents another set of logistical challenges. Depending on the distance and mode of transport (e.g., pipeline, truck, or ship), there are varying degrees of complexity, risk, and costs involved. Once at the conversion facility, the purified and pressurized CO2 undergoes chemical reactions to convert it into a valuable final product. This stage requires sophisticated technologies and catalysts to ensure high conversion efficiency and product yield.

[0035] Therefore, a CO2 capture system that overcomes one or more of the drawbacks mentioned in this paper is needed.

[0036] In one or more embodiments, a CO2 capture system is disclosed. The system may be configured to sequester CO2 from a dilution source. The system may be a DAC (Dilute-Dependent Acquisition) system. The system is arranged to capture CO2 from air, the atmosphere. The capture may be direct capture. The CO2 may be anthropogenic CO2, residual CO2, naturally occurring CO2, CO2 from various sources such as decomposition CO2, ocean-released CO2, respired CO2, industrial CO2, deforestation CO2, fossil fuel combustion CO2, transport CO2, fuel combustion CO2, exhaust CO2, etc., or combinations thereof. Other sources of CO2 may also be suitable for the sequestration described herein. Unless explicitly stated otherwise, it should be understood that the mechanisms for CO2 sequestration can occur through adsorption or absorption and are not particularly limited.

[0037] The capture systems and methods disclosed herein are a hybrid of conventional source-point and DAC technologies, enhancing and integrating the benefits of both while overcoming many of their drawbacks. The capture systems disclosed herein may include a solid adsorbent and a regeneration process that repeatedly circulates one or more exchange fluids. Separating carbon sequestration from its source and endothermic regeneration provides greater versatility and incorporates the benefits of both technologies while creating new advantages. Furthermore, the systems and related methods disclosed herein offer one or more advantages. The systems and methods can help mitigate adsorbent degradation that traditionally occurs during temperature and pressure fluctuations in the regeneration phase. Moreover, the integration of capture, conversion, mineralization, or a combination thereof eliminates separate regeneration and compression steps, contributing to overall efficiency. The systems also utilize alternative compounds for the exchange fluid (e.g., amino acids), achieving alternative and beneficial chemistry.

[0038] The system may have one or more parts, stages, states, or combinations thereof. The system can fuse a solid adsorbent with a liquid exchange fluid for regenerating the solid adsorbent. The system comprises several components. The various components described herein may cooperate mechanically, physically, chemically, fluidly, or in combination thereof, such that they are described as being in mechanical, chemical, and / or fluid communication to achieve the structures, functions, and instances described herein. Figure 1-4 Non-limiting examples of the systems disclosed in this paper are shown.

[0039] The systems disclosed herein include at least one container. The systems may include 2, 3, 4, 5, 6, or more containers. However, the systems may include a single container or only two containers. The containers may be reaction reactors, tanks, vessels, compartments, cylinders, capsules, barrels, chambers, water tanks, flasks, reservoirs, etc. The containers may be closed, sealable, openable, sealable, and / or resealable.

[0040] The container may include or contain a solid CO2 adsorbent. The adsorbent may include a porous support functionalized with one or more amine functional groups, molecules, or polymers attached to a support. The attachment may include immobilization, grafting, direct bonding, or incorporation of a non-volatile polymer component such as a coating. The porous support material itself may include functionalized amines. The porous material may include (mesoporous) porous silica, cellulose, zeolite, polymers such as polymethyl methacrylate (PMMA) or polystyrene (PS). The porous material may have a high surface area (e.g., at least about 100, 250, or 500 m²). 2 / g). Non-limiting exemplary adsorbents include monolithic cellulose coated with polyethyleneimine (PEI).

[0041] The adsorbent can be configured as a solid material, such as particles, within the reactor. The adsorbent can be configured as a bulk material, pad, plate, sheet, film, membrane, fabric, etc. The adsorbent can be configured as beads or particles fixed in a fixed bed that is mobile within the closed environment of the reactor / vessel. The non-limiting average particle size of the adsorbent can be approximately 100 μm to 5 mm, 500 μm to 2 mm, or 1000 μm to 1 mm.

[0042] The adsorbent is configured to have selectivity and / or affinity for CO2, such that it sequesters CO2 from its gaseous state (e.g., atmospheric air). For example, the adsorbent may be configured to consume a volume of atmospheric air to less than about 380, 350, 300, 280, 250, 225, or 200 ppm.

[0043] The system may include several states, stages, or phases. In a first state, the functionalized portion of the adsorbent spontaneously reacts with CO2 to separate CO2 from the air, while a porous support material provides a high surface area for the amine / air interface, ensuring that air can flow through the adsorbent and immobilizing the amines in the solid adsorbent, preventing their volatilization. Effective contact between the CO2-filled air and the adsorbent (especially its amine functionalization) should be maintained at sufficient time intervals to maximize CO2 sequestration. During the first phase, the adsorbent is effectively loaded with CO2. During the first phase, the incoming ambient air has a first CO2 concentration, which is higher than the second CO2 concentration after CO2 has bound to the adsorbent. The air leaving the reactor and system thus has a second CO2 concentration lower than the first concentration.

[0044] The adsorbent is then regenerated via an exchange fluid in a second stage or state. In the second state, the adsorbent material is exposed to the exchange fluid, where it chemically adsorbs CO2 bound to the amine end groups. Once the exchange fluid is loaded with CO2, it is removed, and the adsorbent material is rinsed with water, dried, and prepared for a new adsorption cycle. The adsorbent may be rinsed (e.g., with water) and / or dried periodically, or it may be rinsed and dried before each new CO2 adsorption cycle. CO2 may be bound in the exchange fluid in the form of carbamate, bicarbonate, carbonate, or a combination thereof.

[0045] In the third stage or state, the exchange fluid is regenerated in a regeneration device. The regenerated exchange fluid can be reintroduced into the system. The regeneration device may provide additional functionality, such as converting CO2 into carbonate for further utilization or storage in solid form. A non-limiting exemplary regeneration device may include a mineralization reactor.

[0046] Figure 1A non-limiting example of the system is shown. It can be seen that... Figure 1 System 100 can utilize an exchange fluid 102 shared and circulated between a reaction reactor 108, comprising adsorbent 104, and a regeneration unit 106. The adsorbent 104 and the regeneration unit 106 can be separated from each other. In various embodiments, CO2 is captured by the adsorbent 104 from a CO2-containing input stream described at point A. The adsorbent 104 can then be regenerated in the reaction reactor 108 by immersing it in the exchange fluid 102. The exchange fluid 102 can sequester CO2 from the adsorbent 104, thereby removing CO2 from the adsorbent 104. The adsorbent 104 can be regenerated for further sequestering CO2 from a source of CO2 (e.g., atmospheric air). After regeneration of the adsorbent 104, the CO2-enriched exchange fluid 102 can be transferred to the regeneration unit 106, where CO2 is separated from the exchange fluid 102. The exchange fluid 102 can then be recycled back to the reaction reactor 108 for another regeneration cycle.

[0047] The regeneration device 106 can provide two functions: (1) regeneration of the exchange fluid and (2) in-situ conversion of captured CO2 into a final product, which includes consuming the sealed / captured CO2. The device 106 (206, 306, 406) is thus a dual-function device. Functions (1) and (2) can be simultaneous or continuous. The regeneration of the exchange fluid can utilize one or more intermediates or products from the conversion reaction, such as hydroxide ions (OH-). - The final product may be non-gaseous, gaseous, liquid, solid, high-value, non-CO2, or a combination thereof. The final product may include carbon atoms from sealed and captured CO2, thereby combining carbon from ambient air in a non-CO2 form. The final product may include oxygen, carbon monoxide, alcohols (e.g., methanol), carboxylic acids (e.g., formic acid), or another carbon-based substance.

[0048] The regeneration unit 106 (which also provides the function of converting CO2 into useful chemical compounds, products, or intermediates for further production) is an in-situ reactor. In other words, the unit 106 is physically part of the disclosed system, adjacent to or close to the regeneration unit 106. Because the system includes an in-situ conversion unit, it thereby avoids the need for purified CO2 intermediates, pressurization, and transportation, thus improving efficiency. The system can operate in a loop, allowing continuous recycling of the adsorbent and exchange fluid. The system can be configured as a batch process or a continuous operating system. The system can thus support a circular economy and contribute to mitigating climate change.

[0049] The regeneration device may be a mineralization reactor, and non-limiting examples are shown in Figure 2 A mineralization reactor is a vessel used to chemically convert CO2 into carbonates, such as calcium carbonate (CaCO3), through a process called mineralization. Unlike naturally occurring mineralization (which takes hundreds or thousands of years, in which minerals inside rocks react with atmospheric CO2 to produce carbonates), the process in a mineralization reactor promotes an accelerated reaction between CO2 and minerals, resulting in the safe storage of CO2.

[0050] The mineralization process may utilize alkaline feedstocks to react with concentrated CO2. Alkaline feedstocks may include fly ash, steel slag, industrial alkaline waste, alkaline tailings, industrial byproducts, mined rocks such as alkaline rocks rich in iron, calcium, and magnesium, calcium-rich materials, or combinations thereof. The alkaline feedstock may include one or more oxides, such as calcium oxide (CaO). The alkaline feedstock may contribute to the regeneration of calcium ion sources, be a calcium ion source, or both. The alkaline feedstock may be in the form of pulverized particles.

[0051] The mineralization reaction can be promoted at ambient temperature and relatively low or relatively high pressure, high temperature, or both. The temperature of the mineralization reaction can be approximately 15-90, 25-80, or 35-70°C. Compared with methods that require high temperatures and high pressures above ambient conditions, reactions at ambient temperature for storing CO2 in solid form have advantages.

[0052] In a mineralization reactor, CO2 reacts with divalent cations to produce stable carbonate minerals. The resulting carbonate minerals can then be used in a variety of applications, such as as a component of cement, fertilizer, and a source material for paper and paint.

[0053] The system may include a settling tank to remove carbonate products in solid form. The system may also include a filter to separate the regenerated exchange fluid before it is returned for further storage.

[0054] Figure 2 The embodiments illustrate a method for producing carbonates from CO2. A specific, non-limiting example could be the production of CaCO3 from CO2 and CaO. Figure 2 As shown in system 200, reaction reactor 208 can promote Figure 1 The system is shown in its first and second states. Air with a higher CO2 concentration is contacted with a CO2 adsorbent for sequestration. Subsequently, an exchange fluid is submerged in reactor 208 to remove CO2 from the adsorbent. The CO2-enriched exchange fluid is then introduced into mineralization reactor 206. An alkaline feedstock is also introduced into mineralization reactor 206 to promote the reaction with CO2. The exchange fluid is regenerated by removing the CO2 reacted with the alkaline feedstock. The exchange fluid can be returned to reactor 208 for further CO2 sequestration.

[0055] In another embodiment, Figure 1 The regeneration device 106 may be a conversion unit 306, a non-limiting example of which is shown in Figure 3 and 4 In the conversion unit, the captured CO2 can be reduced via thermal, chemical, thermochemical, or electrochemical pathways.

[0056] In a thermochemical pathway, a CO2-filled fluid can be subjected to temperatures between approximately 50 and 200 °C and / or pressures above approximately 1 bar in the presence of a catalyst, such as those based on silver (Ag), copper (Cu), nickel (Ni), platinum (Pt), palladium (Pd), or ruthenium (Ru) on various supports including zinc oxide or alumina (ZnO and Al2O3). Other catalysts and oxides are also considered. Appropriate combinations of catalytic systems, temperatures, and pressures can be selected to produce the desired final product. The thermochemical pathway can be implemented in a regeneration unit 306. The catalytic system, increased temperature, increased pressure, or combinations thereof can be present in or supplied to the reactor, as... Figure 3 As shown in the diagram. The chemistry of the final product depends on the type of catalyst, temperature, and pressure introduced into reactor 306. The final product may include gaseous, liquid, solid products, or combinations thereof.

[0057] A non-limiting description of the thermochemical reaction pathway is shown in Figure 3 The system 300 includes a reaction reactor 308 containing a solid adsorbent. The first and second stages occur in the reaction reactor 308. The third stage occurs in an adjacent regeneration reactor 306, which is also a conversion reactor for capturing CO2.

[0058] In an electrochemical approach, the exchange fluid can be introduced into the electrolytic cell, a non-limiting example of which is shown in... Figure 4 In the process, oxidation occurs at the anode (e.g., oxygen evolution), while at the cathode, CO2 is electrochemically reduced to various final products in the presence of a catalyst. The two electrode compartments can be separated by either a proton exchange membrane, an anion exchange membrane, or a bipolar membrane obtained by combining proton and anion exchange membranes.

[0059] Figure 4 A non-limiting exemplary system including an electrolytic cell is shown. The system 400 includes a reaction reactor 408 in which first and second stages occur. A third stage occurs in a conversion reactor 406, which in this embodiment is an electrolytic cell 406. The electrolytic cell 406 includes a cathode 430, an anode 432, and a membrane 434 separating electrodes 430 and 432. The final product may include various reaction products, including gaseous products such as oxygen. The regenerated exchange fluid may be returned to the reaction reactor 408.

[0060] In the systems disclosed herein, the exchange fluid can deplete the chemically bound CO2 to a degree determined by the overall system requirements, typically between approximately 10-100%, 20-90%, or 30-70%, and is subsequently regenerated for the next adsorption cycle. Meanwhile, the desired end product can be collected, purified, stored, used in production, or a combination thereof.

[0061] Reactors 108, 208, 308, 408 and regeneration devices 106, 206, 306, 406 may include one or more inlets and one or more outlets. For example, reactor 208 may include a first inlet 210 for receiving a gaseous supply stream / input and a first outlet 212 for discharging or releasing the gaseous supply. Reactor 208 may further include a second inlet 214 for receiving exchange fluid from a regeneration module (e.g., mineralization reactor 206) and a second outlet 216 for discharging CO2-enriched exchange fluid from the adsorbent compartment / reactor 208 and transferring it to the regeneration module 206.

[0062] Similarly, the regeneration reactors, devices, or modules 106, 206, 306, and 406 may include one or more inlets and one or more outlets. For example, device 206 may include a first inlet 218 for entering the CO2-enriched exchange fluid and a second inlet 220 for feed input. The reactor 206 may also include a first outlet 222 for discharging the exchange fluid after regeneration and a second outlet 224 for collecting carbonates. Figure 3 and 4 Similar entrances and exits are also depicted in the text.

[0063] The reactors 108, 208, 308, and 408 may also include inlets for any raw materials or chemical compounds required to assist in CO2 sequestration. The chemical compounds may be part of the exchange fluid. Alternatively, or additionally, as needed, such as after regeneration of the exchange fluid, additional chemical compounds may be supplied to the reactors.

[0064] The reactor and regeneration device may further include one or more conduits connecting the reactor to the regeneration device. For example, the system may share a single conduit that guides the exchange fluid back and forth between the reactor and the regeneration device. Alternatively, the system may include two separate conduits, a first conduit for conveying the enriched exchange fluid from the reactor to the regeneration device, and a second conduit for conveying the regenerated exchange fluid from the regeneration device to the reactor.

[0065] The first and second inlets can be separate and sealable, such that during a first time period, the first inlet allows the gaseous stream to enter the compartment and contact the adsorbent, while the second inlet is sealed. During a second time period, the first inlet can be sealed, while the second inlet is open to immerse the adsorbent / compartment with the exchange fluid. Similarly, the first and second outlets can be selectively sealable for filling or draining the compartment with the gaseous stream / exchange fluid.

[0066] The first inlet or gaseous input can be positioned such that the input stream passes along the adsorbent (e.g., above or through the adsorbent). The same orifice or port can serve as both an inlet and outlet for the gaseous stream and / or the exchange fluid. The container can provide a closed environment by selective inclusion, sealability, or sealing, preventing the release of movable adsorbent (e.g., beads / granules) and / or volatile components (e.g., in the exchange fluid). In other words, the gas supply can be fixed in the reactor for a duration sufficient to allow the adsorbent to remove and sequester CO2. Alternatively, a continuous stream of air can be supplied.

[0067] During the first state, CO2 may be exposed to the adsorbent until a threshold saturation level and / or capacity is reached, or for a duration sufficient for adsorption. During the second state, the exchange fluid may be exposed to the adsorbent until a threshold saturation level / limit / point and / or capacity is reached, or for a duration sufficient for regeneration. Exposure in either state may be carried out for a predetermined amount of time.

[0068] The threshold point / limit can be a decrease / increase in the encapsulation capacity of at least approximately 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 98, or 99%. The threshold saturation level / limit / point can be at least approximately 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 98, or 99% of the adsorption capacity. A time period sufficient to achieve the threshold limit or range can be used. For example, the adsorbent may be exposed to a gaseous component and / or the exchange fluid may be exposed to the adsorbent for a duration sufficient to utilize at least approximately 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 98, or 99% of the adsorption capacity. In a non-limiting example, based on real, historical, or predicted conditions, such as temperature, humidity, pressure, and atmospheric air composition, exposure may occur for a duration sufficient to utilize approximately 20 to 90, 30 to 85, or 45 to 80% of the adsorption capacity.

[0069] The exchange fluid can then be contacted with the adsorbent after the adsorbent reaches saturation or a threshold saturation level for CO2 adsorption, or after a (predetermined and / or predicted) duration. Before immersing the adsorbent in the exchange fluid, the adsorbent may be exposed to atmospheric air for a duration sufficient to adsorb CO2 exceeding the threshold. Similarly, before removing the exchange fluid containing sequestered CO2, the exchange fluid may be contacted with the adsorbent for a duration sufficient to reach the threshold saturation level of the exchange fluid or release the threshold capacity of the adsorbent. The CO2-loaded / filled exchange fluid can be removed, discharged, or extracted from the adsorbent after reaching the threshold level and / or after a (predetermined / predicted) duration. The step of contacting the exchange fluid with the adsorbent can be repeated once or multiple times to extract CO2 from the adsorbent. The same or different exchange fluids in different streams / volumes can be used.

[0070] The dimensions of the reactor can be adjusted to accommodate a volume of exchange fluid configured to regenerate the adsorbent in one, two, three, or more passes. The reactor dimensions can also be adjusted to accommodate a volume of exchange fluid such that the transfer of CO2 from the adsorbent to the exchange fluid is kinetically more efficient (i.e., the ratio of CO2 sequestered by the exchange fluid to the adsorbent is greater than 1:1, for example, the ratio of the total sequestered capacity of the exchange fluid to the CO2 sequestered in the adsorbent is greater than 1:1 or at least 2:1, 5:1, 10:1, 25:1, 50:1, 100:1, or at least 1,000:1). The reactor dimensions can also be adjusted to accommodate excess exchange fluid such that the exchange fluid in the reactor has a larger total capacity for CO2 sequestration than the CO2 sequestered (or to be sequestered) by the adsorbent. For example, the compartment containing the adsorbent can be submerged in the exchange fluid.

[0071] Because the adsorbent can spontaneously sequester CO2 from ambient air under environmental conditions, the adsorbent, reaction reactor, CO2 sequestration reactor, system, or combination thereof may not have a heating element for heating the adsorbent. In conventional systems, a heating element may be present in the CO2 adsorption device, for example, for the regeneration of the adsorbent.

[0072] The systems disclosed herein may include heating elements, either entirely or solely in the third stage or in devices 106, 206, 306, and 406. In one or more embodiments, even devices 106, 206, 306, and 406 may not have heating elements. For example, if the device is a mineralization reactor, device 206 may not have heating elements and thus not have increased temperature, pressure, or both. If the device is a conversion device 306, 406, or both, the device may include one or more heating elements to facilitate temperatures sufficient for conversion processes involving thermal, thermochemical, or electrochemical reactions.

[0073] The heating element can be placed inside, outside, or both of the regeneration device. The heating element can be inside or outside the device. The device can be constructed as a pressure vessel.

[0074] The reactor may be submerged in an exchange fluid such that it is filled to approximately, at least approximately, or at most approximately 30, 50, 60, 75, 80, 85, 90, 95, 98, or 99% of its volumetric capacity.

[0075] The method described herein can be repeated continuously or in batches. In one variation, the first and second stages can be repeated multiple times (e.g., 2, 3, 4, 5, 6, 7, 8, 9, 10 times) before regeneration. Regeneration can be repeated multiple times (e.g., 2, 3, 4, 5, 6, 7, 8, 9, 10) to fully regenerate the exchange fluid before it is brought back into contact with the adsorbent. The regenerated exchange fluid can be cooled before being reintroduced into the adsorbent.

[0076] The adsorbent can sequester CO2 from a gaseous stream, such as atmospheric air, while simultaneously regenerating the exchange fluid. Conventional systems without an integrated intermediate exchange fluid cannot separate the task of removing CO2 from the air from the task of simultaneously removing CO2 from the system for further utilization or storage.

[0077] One or more steps described herein can be performed by a controller, which includes non-volatile memory having computer-executable instructions stored thereon and a processor for executing the computer-executable instructions. For example, the sealing or regeneration step can be based on predicted conditions rather than actual conditions or on proxy parameters. The prediction can be based on algorithms such as machine learning algorithms. Machine learning algorithms can be implemented using artificial intelligence. Machine learning algorithms can be algorithms that improve their accuracy through experience. Machine learning algorithms can enable one or more implementations to learn and improve from previous experience and / or the data described herein without explicit programming. The machine learning algorithm can be a neural network algorithm. Neural network algorithms, random forest algorithms, support vector algorithms, k-nearest neighbor algorithms, and symbolic regression algorithms can be trained to identify complex patterns within data and learn to represent non-linear relationships between data and predict trends. Machine learning algorithms can be implemented as machine instructions stored in non-volatile memory on a computer, wherein the machine instructions will be executed by the computer.

[0078] For example, historical, forecast, or current weather or environmental conditions can be used to predict CO2 concentrations in ambient air, the appropriate duration for sequestration, improve the efficiency of the systems described herein, or a combination thereof.

[0079] The processor may include one or more devices selected from high-performance computing systems, including high-performance cores, microprocessors, microcontrollers, digital signal processors, microcomputers, central processing units, field-programmable gate arrays, programmable logic devices, state machines, logic circuits, analog circuits, digital circuits, or any other device that manipulates signals (analog or digital signals) based on computer-executable instructions residing in memory. The memory may include a single memory device or multiple memory devices, including but not limited to random access memory (RAM), volatile memory, non-volatile memory, static random access memory (SRAM), dynamic random access memory (DRAM), flash memory, cache memory, or any other device capable of storing information. Non-volatile memory may include one or more permanent data storage devices, such as hard disk drives, optical disk drives, magnetic tape drives, non-volatile solid-state devices, cloud storage, or any other device capable of permanently storing information.

[0080] Executable instructions may reside in a software module. The software module may include an operating system and applications. The software module may be compiled or interpreted from computer programs created using various programming languages ​​and / or technologies, including but not limited to Java, C, C++, C#, Objective C, Fortran, Pascal, JavaScript, Python, Perl, and PL / SQL, individually or in combination. Non-volatile memory may also include data supporting the aforementioned functions, features, calculations, and processing.

[0081] Computer-readable storage media (e.g., memory) that are inherently non-volatile can include tangible media that are volatile or non-volatile, and removable or non-removable, implemented in any method or technique for storing information (e.g., computer-readable instructions, data structures, program modules, or other data). Computer-readable storage media may further include RAM, ROM, erasable programmable read-only memory (EPROM), electronically erasable programmable read-only memory (EEPROM), flash memory or other solid-state memory technologies, portable optical disc read-only memory (CD-ROM) or other optical storage, magnetic tape cassettes, magnetic tape, disk storage or other magnetic storage devices, or any other medium that can be used to store desired information and is readable by a computer. Computer-readable program instructions may be downloaded to a computer via a network, another type of programmable data processing device, or another device form of computer-readable storage media, or downloaded to an external computer or external storage device.

[0082] Computer-readable program instructions stored in a computer-readable medium can be used to instruct a computer, other type of programmable data processing apparatus, or other device to operate in a particular manner, causing the instructions stored in the computer-readable medium to produce an article of writing that includes instructions to implement the functions, actions, and / or operations described herein. The functions, actions, and / or operations described herein can be reordered, processed serially, and / or processed concurrently.

[0083] The exchange fluid used to regenerate the adsorbent may have at least one component with an affinity and / or selectivity for CO2, such that the exchange fluid sequesters CO2 from the adsorbent. Thus, the exchange fluid can be used to regenerate the adsorbent after contact with it for a sufficient duration (e.g., at least 1, 5, 15, 30, 45, or 60 minutes). The exchange fluid may be configured to sequester CO2 from the adsorbent at relatively low temperatures (e.g., below about 50, 75, or 100°C), at relatively low pressures (e.g., below about 1, 2, 3, 4, or 5 atmospheres), and / or under ambient conditions (e.g., about 20 to 25°C and 0.5 to 1.5 atm). CO2 sequestration at relatively low temperatures and pressures or under ambient conditions can be spontaneous, such that energy input is not required to facilitate sequestration / adsorption.

[0084] The exchange fluid (or a component thereof) can be selected such that CO2 has a greater affinity for the exchange fluid (or a component thereof) compared to the adsorbent. In various embodiments, the exchange fluid (or a component thereof) can be selected based on its binding energy with CO2. The exchange fluid (or a component thereof) can be selected such that the binding energy between the exchange fluid (or a component thereof) and CO2 is greater than the binding energy between the adsorbent and CO2.

[0085] CO2 can bind to one or more components in the exchange fluid, such as one or more functional groups in the exchange fluid. Functional groups in the exchange fluid can form complexes with CO2.

[0086] The exchange fluid may be primarily a liquid, such as a solution, emulsion, or dispersion. The exchange fluid may be an water-based solution. The exchange fluid may include one or more compounds having one or more nitrogen atoms. The exchange fluid may include one or more nitrogen-containing compounds or compounds with nitrogen-containing groups. The exchange fluid may include one or more amines, amino acids, neutralizing agents, or combinations thereof. The exchange fluid may not contain one or more amines, amino acids, or neutralizing agents.

[0087] The one or more nitrogen-containing compounds or nitrogen-containing groups may include amines. The exchange fluid may include one or more amines. An amine is a compound having a nitrogen atom with a lone pair of electrons. The nitrogen atom in the exchange fluid is not limited to nitrogen gas (e.g., N2). The amine may include primary amines, secondary amines, tertiary amines, or combinations thereof. The amine may have the formula R-NH2, R2-NH, or R3-N. CO2 can be sequestered such that the ionic form has a -1 charge, i.e., one extra electron per mole of CO2 or a near-such form, for example, less than 5, 3, or 2 electrons per mole. In other words, CO2 can be sequestered such that the addition of one electron (per sequestered CO2 molecule) can be added to release the bound CO2. For example, CO2 can be sequestered in the form of carbamate, bicarbonate, etc., or mixtures thereof.

[0088] The one or more amines may include one or more (or selected from) aqueous amines, water-depleted amines, amino acids, amidines, guanidines and their derivatives, and / or mixtures thereof.

[0089] Aqueous amines include amines that can be used to form water-based solutions of amines. Aqueous amines may include amines that are miscible and / or soluble in water. Aqueous amines may have a solubility of at least 1, 10, 100, 500, or 1000 mg / L at 25°C. Non-limiting examples of suitable aqueous amines may include monoethanolamine (MEA), diethanolamine (DEA), triethylamine (TEA), triethanolamine (TEOA), ethylenediamine (EDA), diethylenetriamine (DETA), triethylenetetramine (TETA), 2-(2-aminoethyl-amino)ethanol (AEEA), 2-amino-2-methyl-1-propanol (AMP), piperazine (PZ), piperazine derivatives, or combinations thereof.

[0090] Aqueous depletion can refer to a compound that does not intentionally include water, contains only negligible or trace amounts of water, or is anhydrous. For example, aqueous depletion amines can include mixtures of organic diluents and amines. Aqueous depletion can also refer to a compound having a low water content, such as less than about 0.01, 0.1, 0.5, or 1% by weight based on the total weight of the compound. Aqueous depletion components can include organic solvents, alcohols, or mixtures thereof. One or more aqueous depletion amines can be liquid at room temperature and are referred to as amines or aqueous depletion amine solvents. For example, suitable aqueous depletion amines can include N-(2-ethoxyethyl)-3-morpholinopropyl-1-amine (EEMPA), N1-(2-ethoxyethyl)-N2,N2-diisopropylethane-1,2-diamine (EEDIDA), 3-methoxy-N-(pyridin-2-ylmethyl)propyl-1-amine (MPMPA), or 2-morpholino-N-(pyridin-2-ylmethyl)ethyl-1-amine (MPMEA). The water-deficient amine may include compounds represented by formula (1): (1).

[0091] The dehydrated amine may include compounds represented by formula (2): (2).

[0092] The water-deficient amine may include compounds represented by formula (3): (3).

[0093] The dehydrated amine may include compounds represented by formula (4): (4).

[0094] The dehydrated amine may be a mixture of two or more compounds represented by formulas 1-4.

[0095] The exchange fluid may include at least one or more amino acids (e.g., a mixture of amino acids). Amino acids are organic compounds having an amino functional group (-NH2) and a carboxylic acid functional group (-COOH). Suitable amino acids may include alanine, arginine, asparagine, aspartic acid, cysteine, glycine, glutamic acid, glutamine, histidine, isoleucine, leucine, lysine, methionine, phenylalanine, proline, pyrrolidone, serine, selenocysteine, threonine, tryptophan, tyrosine, and valine. The R or L stereochemical configuration of the amino acid may be used. In a non-limiting example, L-arginine may be used. The amino acid may include a primary or secondary amino group (proline). The amino acid may include an amino group in its "R" chain. The amino acid may include one or two primary amine groups in its structure.

[0096] Amidones are organic compounds having the functional group RC(NR)NR2, where R can be the same or different. Amidones include two nitrogen atoms. Amidones are imine derivatives of amides (RC(O)NR2). Non-limiting exemplary amidones include formamidinium having the formula HC(=NH)NH2, diamidinium, benzylamidinium having the formula C6H5C(NH)NH2, pentamidine, paranyline, etc.

[0097] Guanidine is a compound having the formula HNC(NH2)2. Guanidine is a strong base soluble in polar solvents. Guanidine derivatives, or guanidines, are a group of organic compounds that share a common functional group with the general structure (R1R2N)(R3R4N)C=N−R5 and have an imine central bond. Examples of guanidines include arginine, triazabicyclodecene, and creatine.

[0098] One or more nitrogen-containing components or nitrogen-containing groups (e.g., one or more amines) may be present in an amount of about, at least about, or at most about 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 99, or 100% by weight of the exchange fluid. The one or more nitrogen-containing components or nitrogen-containing groups (e.g., one or more amines) may be present in an amount of about 5-90, 10-75, or 25-45% by weight based on the total weight of the exchange fluid. The weight and / or concentration described herein with respect to the exchange fluid may be before or after CO2 sequestration; however, unless explicitly stated otherwise, the amount refers to the weight or concentration before sequestration.

[0099] In one or more embodiments, the nitrogen-containing compound (e.g., one or more amines) may be present at a concentration of about, at least about, or at most about about 0.5, 1, 1.5, 2, 2.5, 3, 3.5, 4, 4.5, 5, 5.5, 6, 6.5, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, 21, 22, 23, 24, or 25 M. The amine may be present in amounts of about 2-20, 4-15, or 6-9 M. In a non-limiting example, 7.0 M MEA and / or 8.0 M PZ may be used.

[0100] The exchange fluid may comprise an alcohol or a mixture of alcohols. The exchange fluid may comprise a mixture of water and one or more alcohols. For example, suitable alcohols may include methanol, ethanol, propanol (e.g., 1-propanol or prop-2-ol / isopropanol), butanol, pentanol, and / or hexanol. Other suitable alcohols include glycols (e.g., ethylene glycol, propylene glycol), glycerol, xylitol, sorbitol, or other suitable alcohols. The alcohol may comprise up to 20 carbon atoms (C1-C2). 20 ), or at most 16 carbons (C1-C1). 16 ), or at most 14 carbons (C1-C1). 14 ), or 12 carbons (C1-C 12 ), or 10 carbons (C1-C 10 (1) or 8 carbons (C1-C8). Straight-chain alcohols can be used.

[0101] The exchange fluid may also include a neutralizing agent, such as a neutralizing base. A neutralizing agent, such as a neutralizing base, is a substance with the general formula MOH. xThe compound, wherein M belongs to an alkali metal or alkaline earth metal. For example, salts of, for instance, sodium hydroxide (NaOH) and / or potassium hydroxide (KOH) can be used in an amount sufficient to neutralize one or more nitrogen-containing groups. In various embodiments, the base can promote CO2 adsorption, CO2 transfer from the adsorbent to the exchange fluid, and / or affect the chemical form of CO2 sequestered in the exchange fluid. For example, sequestering CO2 in the form of carbamate and / or bicarbonate can reduce regeneration requirements.

[0102] The components in the exchange fluid, such as nitrogen-containing compounds or amines, may have an adsorption energy / enthalpy of about, at least about, or at most about 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85, 90, 95, 100, 102, 110, 115, or 120 kJ / mol.

[0103] One or more volumes of exchange fluid can be used. These volumes can be the same or different, for example, regarding their composition, the presence or absence of neutralizing agents, or combinations thereof. A first volume of exchange fluid can be contacted with the adsorbent to regenerate it and then removed, followed by contact with a second volume of exchange fluid for further regeneration. The second volume of exchange fluid can have the same or different composition as the first volume. For example, the first and second volumes of exchange fluid can comprise the same amino acid mixture. Having multiple fresh (unexposed) volumes can improve the kinetics of CO2 sequestration from the adsorbent.

[0104] The second volume of exchange fluid may have a different composition than the first volume. In a non-limiting example, the first volume of exchange fluid may exhibit better kinetics when the adsorbent has a high saturation, and the second volume of exchange fluid may exhibit better kinetics when the adsorbent has a low saturation. In a non-limiting example, the first volume of exchange fluid may comprise an alcohol-amidine mixture, and the second volume of exchange fluid may comprise an amino acid mixture. The first and second volumes of exchange fluid may have different storage capacities, i.e., one may have a greater storage capacity than the other. Example

[0105] Examples 1 and 2 The system includes, for example Figure 1 and 2 The method begins with a monolith coated with polyethyleneimine (PEI), which is exposed to an ambient air stream until the amine-based adsorbent becomes fully loaded and chemically binds CO2 in the form of carbamate. Once the adsorption step is complete, the monolith is immersed in an exchange fluid. The exchange fluid is a water-based solution containing at least one deprotonated amino acid having the general formula (5): H x N-CHR-COOH (5), Or its deprotonated form can be represented by equation (6): H x N-CHR-COO - (6), in x is 2; and R is a hydrogen or carbon group.

[0106] In equations (5) and (6), R can be hydrogen, C1-C 100 Alkyl, aryl, or alkylaryl. R can be C1-C2. 40 Alkyl, C1-C 20 Alkyl, or C1-C8 alkyl.

[0107] One or more amino acids are encapsulated by the nitrogen-containing functional groups (e.g., amine or imine groups) of the solid adsorbent to form carbamate from CO2. This reaction is represented by formula (7): 2 - OOC-CHR-NH2+ CO2→ - OOC-CHR-NHCOO - + - OOC-CHR-NH3 + (7), in R is a hydrogen or carbon group. R can be hydrogen, C1-C... 100 Alkyl, aryl, or alkylaryl. R can be C1-C2. 40 Alkyl, C1-C 20 Alkyl, or C1-C8 alkyl.

[0108] In the presence of water or alkali, the carbamate ion further reacts to form bicarbonate, at which point the free amino group can react with CO2 again. At high pH, ​​the reaction proceeds further, producing carbonate ions. The reaction is represented by equation (8): - OOC-CHR-NHCOO - + - OOC-CHR-NH3 + + H2O→ - OOC-CHR-NH2+ - OOC-CHR-NH3 + + HCO3 - (8), in R can be a hydrogen or carbon group. R can be hydrogen, C1-C 100 Alkyl, aryl, or alkylaryl. R can be C1-C2.40 Alkyl, C1-C 20 Alkyl, or C1-C8 alkyl. This can be rewritten as shown in formula (9), which indicates that in (8), amino acids ( - OOC-CHR-NH2) is reformed and can subsequently react with another CO2 and H2O to form another bicarbonate ion and - OOC-CHR-NH3 + : - OOC-CHR-NH2+ CO2+ H2O→ - OOC-CHR-NH3 + + HCO3 - (9), in R can be a hydrogen or carbon group. R can be hydrogen, C1-C 100 Alkyl, aryl, or alkylaryl. R can be C1-C2. 40 Alkyl, C1-C 20 Alkyl, or C1-C8 alkyl.

[0109] Various exchange fluids can be used. The exchange fluids may include amidines, such as 1,8-diazabicyclo[5.4.0]undec-7-ene (DBU), diamidinium, benzylamidinium, pentamidine, and / or paranyline. Mixtures of the exchange fluid components described herein can be used. For example, a mixture of nitrogen-containing compounds (e.g., amines, amides, amino acids, imines, amidines, guanidines) and water-poor solvents (e.g., organic solvents and / or alcohols) can be used.

[0110] In another non-limiting example, a suitable amino acid with a sufficiently high adsorption energy (enthalpy) disclosed herein may be selected. In one non-limiting example, an aqueous solution of 1 M L-glycine (where R: H) or 1 M L-arginine (where R: HN=C(NH2)-NH-(CH2)3) may be used.

[0111] Example 1 After sufficient time to allow the adsorption process, the CO2-loaded fluid is then transferred to the next step: CO2 mineralization and exchange fluid regeneration. In this step, CaO is added to the solution to release Ca and hydroxide ions, as shown in reaction (10): CaO + H₂O → Ca(OH)₂ → Ca 2+ + 2OH - (10).

[0112] Ca ions further react with carbonate ions to produce insoluble CaCO3, which is then precipitated and separated. In parallel, one of the two hydroxide ions regenerates the amino acid solution, which is then removed and supplied to a sealed reaction reactor for continuous adsorption cycles. The second hydroxide ion forms carbonate. The carbonate generation reactions are shown in equations (11a) and (11b), and the amino acid regeneration is shown in equation (12): HCO3 - +OH - → CO3 2- + H2O (11a), Ca 2+ + CO3 2- → CaCO3(11b), - OOC-R-CH-NH3 + + OH - → H2O + - OOC-R-CH-NH2(12).

[0113] Example 2 After sufficient time to allow the adsorption process, the CO2-loaded fluid is then transferred to the next step: electrolysis and exchange fluid regeneration. At the anode, oxygen is evolved in the presence of an iridium oxide catalyst system, producing protons and electrons (13): 2H₂O → 4H + + 4e - + O2(13), Meanwhile, at the cathode, CO2 in the form of carbamate (14) or bicarbonate (15) is directly reduced to carbon monoxide on a silver-based catalyst, consuming the protons and electrons generated at the other electrode: 2 - OOC-R-CH-NHCOO - +2 - OOC-R-CH-NH3 + + 4H + + 4e - → 2CO + 2OH - +2 - OOC-R-CH-NH2+ 2 - OOC-R-CH-NH3 + (14).

[0114] 2 - OOC-R-CH-NH3 + + 2HCO3 - + 4H + + 4e- → 2CO + 2H₂O + 2OH⁻ - +2 - OOC-R-CH-NH3 + (15).

[0115] Once CO is formed, the amino acids further react with the generated hydroxide ions, regenerating the solution to its original state (16, 17): 2CO + 2OH - +2 - OOC-R-CH-NH2+ 2 - OOC-R-CH-NH3 + → 2CO + 2H2O + 4 - OOC-R-CH-NH2(16), 2CO + 2H₂O + 2OH⁻ - +2 - OOC-R-CH-NH3 + → 2CO + 4H2O + 2 - OOC-R-CH-NH2(17).

[0116] The generated CO is separated and collected, while the regenerated solution is removed as a ready-to-use fluid for continuous adsorption cycles.

[0117] Example 3 A solid amine-functionalized ion exchange resin adsorbent is exposed to ambient air for a duration sufficient to become saturated with CO2 (e.g., at least 1 minute and up to 3 hours). Subsequently, a mixture of hexanol and DBU in a 1:1 molar ratio is introduced as the exchange fluid into the saturated adsorbent for a duration sufficient to sequester CO2 from the solid adsorbent (e.g., 1 to 60 minutes). The loaded exchange fluid is then mixed with a carbon-supported palladium catalyst in a thermochemical reactor at 50°C and 60 bar with pressurized hydrogen (H2) for 8 hours to produce formic acid. Gas-liquid and liquid-liquid separations are followed by distillation and reboiler to recover the formic acid and the regenerated exchange fluid, which are then recycled back to the adsorbent for further adsorbent regeneration.

[0118] Example 4 A solid amine-functionalized ion exchange resin adsorbent is exposed to ambient air for a duration sufficient to become saturated with CO2 (e.g., at least 1 minute and up to 3 hours). EEMPA is then introduced as an exchange fluid into the saturated adsorbent for a duration sufficient to sequester CO2 from the solid adsorbent (e.g., 1 to 60 minutes). The loaded exchange fluid (6-10 wt% loading) is then mixed with 5 wt% platinum catalyst (i.e., Pt / TiO2 and Pt / CeO2) in a thermochemical reactor at 170-190°C and 60 bar under pressurized hydrogen (H2) for 12 hours to produce methanol. Following gas-liquid and liquid-liquid separation, methanol and the regenerated exchange fluid are recovered and subsequently recycled back to the adsorbent for further adsorbent regeneration.

[0119] Example 5 A solid amine-functionalized ion exchange resin adsorbent is exposed to ambient air for a duration sufficient to become fully saturated with CO2 (e.g., at least 1 minute and up to 3 hours). A mixture of TEA and ethanol in a 1:1 molar ratio is then introduced as the exchange fluid to the saturated adsorbent for a duration sufficient to sequester CO2 from the solid adsorbent (e.g., 1 to 60 minutes). The loaded exchange fluid is then mixed with an activated catalyst mixture of 55.7 wt% Cu, 26.8 wt% ZnO, and 5 wt% Al2O3 in a thermochemical reactor at 170 °C and 60 bar under pressurized hydrogen (H2) supply for 16 hours to produce methanol. Following gas-liquid and liquid-liquid separation, methanol and the regenerated exchange fluid are recovered and subsequently recycled back to the adsorbent for further adsorbent regeneration.

[0120] Example 6 A solid amine-functionalized ion exchange resin adsorbent is exposed to ambient air for a duration sufficient to become fully saturated with CO2 (e.g., at least 1 minute and at most 3 hours). EEMPA is then introduced as an exchange fluid into the saturated adsorbent for a duration sufficient to sequester CO2 from the solid adsorbent (e.g., 1 to 60 minutes). The loaded exchange fluid is then mixed with a heterogeneous ruthenium catalyst in a thermochemical reactor at 170°C and a pressure less than 15 bar for 16 hours with a pressurized hydrogen (H2) supply to produce methanol (methane). Gas-liquid separation is performed to recover methane, and subsequent liquid-liquid separation is performed to recover the regenerated exchange fluid, which is then recycled back to the adsorbent for further adsorbent regeneration.

[0121] Example 7 A solid amine-functionalized ion exchange resin adsorbent is exposed to ambient air for a duration sufficient to become completely saturated with CO2 (e.g., at least 1 minute and at most 3 hours). An amino acid exchange fluid containing L-lysine is then introduced as the exchange fluid into the saturated adsorbent for a duration sufficient to sequester CO2 from the solid adsorbent (e.g., 1 to 60 minutes). The loaded exchange fluid is then mixed with a ruthenium complex in a thermochemical reactor at 145°C and 2–20 bar for at least 30 minutes to produce formate. Separation and purification methods are then used to separate and purify the formate and the exchange fluid.

[0122] The following applications are related to this application: U.S. Patent Application Serial No. 18 / 162,326 (RBPA0421PUS), filed January 31, 2023, and U.S. Patent Application Serial No. 18 / 347,614 (RBPA0421PUS1), filed July 6, 2023, and U.S. Patent Application Serial No. 18 / 960,017 (RBPA0527PUS), U.S. Patent Application Serial No. 18 / 960,257 (RBPA0528PUS), U.S. Patent Application Serial No. 18 / 960,217 (RBPA0529PUS), U.S. Patent Application Serial No. 18 / 960,033 (RBPA0530PUS), U.S. Patent Application Serial No. 18 / 960,045. U.S. Patent Application Serial No. 18 / 960,078 (RBPA0534PUS), both filed on November 26, 2024, are incorporated herein by reference in their entirety.

[0123] The processes, methods, or algorithms disclosed herein can be delivered to, or implemented by, a processing device, sensor, transponder, controller, or computer, which may include any existing programmable electronic control unit or dedicated electronic control unit. Similarly, the processes, methods, or algorithms can be stored in many forms as data or instructions executable by a controller or computer, including but not limited to information permanently stored on non-writable storage media such as ROM devices and information reproducibly stored on writable storage media such as floppy disks, magnetic tapes, CDs, RAM devices, and other magnetic and optical media. The processes, methods, or algorithms can also be implemented in a software executable object. Alternatively, the processes, methods, or algorithms can be implemented, wholly or partially, using suitable hardware components such as application-specific integrated circuits (ASICs), field-programmable gate arrays (FPGAs), state machines, controllers, or other hardware components or devices, or a combination of hardware, software, and firmware components.

[0124] While exemplary embodiments have been described above, it is not intended that these embodiments describe all possible forms covered by the claims. The language used in this specification is descriptive rather than restrictive, and it should be understood that various changes may be made without departing from the spirit and scope of this disclosure. As previously stated, features of various embodiments may be combined to form further embodiments of the invention that may not be explicitly described or shown. While various embodiments may have been described as offering advantages or being preferred over other embodiments or prior art implementations in one or more desired characteristics, those skilled in the art will recognize that one or more features or characteristics may be compromised to achieve desired overall system properties depending on the specific application and implementation. These properties may include, but are not limited to, cost, strength, durability, lifecycle cost, merchantability, appearance, packaging, size, suitability, weight, manufacturability, ease of assembly, etc. Therefore, to the extent that any embodiment is described as less desirable compared to other embodiments or prior art implementations, it is not outside the scope of this disclosure and may be desirable for a particular application.

Claims

1. A system for capturing atmospheric CO2, the system comprising: Reactors with solid adsorbents; and The mineralization reactor is located downstream of the reaction reactor. The system has three states, including In the reaction reactor, CO2 is sequestered from the air into the solid adsorbent in a first state; In the reactor, a second state of sequestered CO2 is released from the adsorbent by contacting a CO2-enriched adsorbent with an exchange fluid containing one or more amino acids to form a CO2-enriched exchange fluid. and In the mineralization reactor, the sealed CO2 from the CO2-enriched exchange fluid is reacted with an alkaline feedstock to form carbonates, while simultaneously regenerating the exchange fluid to a third state.

2. The system according to claim 1, wherein the solid adsorbent is amine-functionalized.

3. The system of claim 1, wherein the exchange fluid further comprises an alkali, an alcohol, an amine, or a combination thereof.

4. The system according to claim 1, wherein the alkaline raw material comprises a calcium-rich material.

5. The system of claim 1, wherein the regenerated exchange fluid is returned to the reaction reactor in a first state for the next CO2 sequestration cycle.

6. The system of claim 1, wherein the third state operates at ambient temperature.

7. The system of claim 1, wherein the one or more amino acids comprise the L-form of the one or more amino acids.

8. The system of claim 1, wherein the second state ends when the exchange fluid reaches a predetermined saturation point.

9. A direct air capture (DAC) system for CO2, comprising: The reaction reactor comprises: Solid amine-functionalized adsorbents with an affinity for CO2; The first inlet is used to allow air with a first concentration of CO2 to enter; A first outlet for air with a second concentration of CO2, which is lower than the first concentration; A mineralization reactor, fluidly connected to the reaction reactor, the mineralization reactor comprising an alkaline feedstock source; and An exchange fluid, comprising one or more amino acids, circulates between the reaction reactor and the mineralization reactor.

10. The system of claim 9, wherein the exchange fluid further comprises an alkali, an alcohol, an amine, or a combination thereof.

11. The system of claim 9, wherein one or more amino acids comprise L-arginine.

12. The system according to claim 9, wherein the alkaline raw material comprises a calcium-rich material.

13. The system according to claim 9, wherein the alkaline raw material comprises industrial waste.

14. The system of claim 9, wherein the adsorbent is movable within the reaction reactor.

15. A direct air capture (DAC) system for CO2, comprising: A reaction reactor having a solid amine functionalized adsorbent configured to capture CO2 from the air; An in-situ mineralization reactor that reacts captured CO2 with an alkaline feedstock to produce carbon carbonates from the captured CO2 via a mineralization reaction; and An exchange fluid configured to transport captured CO2 from the reaction reactor to the in-situ mineralization reactor.

16. The system of claim 15, wherein the exchange fluid comprises one or more amino acids.

17. The system according to claim 15, wherein the alkaline raw material comprises CaO.

18. The system of claim 15, wherein the carbonate is CaCO3.

19. The system of claim 15, wherein the exchange fluid is recirculated between the reaction reactor and the mineralization reactor based on a predetermined level of CO2 saturation.

20. The system of claim 15, wherein the system is a continuous operating system.

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