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Systems and methods for carbon dioxide capture — Peter Eisenberger (US20230149896A1)

Peter Eisenberger · Google Patents

Google Patents · Patents · License: Open Access

patent, google patents, intellectual property, US20230149896A1, Peter Eisenberger, en, 2023

ABSTRACT

Abstract

There is provided a structurally stable monolith substrate, suitable to provide carbon dioxide capture structure for removing carbon dioxide from air, having two major opposed surfaces, and further having a plurality of longitudinal channels extending between and opening through the two major opposed surfaces of the structurally stable monolith substrate; and a macroporous coating, adhered to the interior wall surfaces of the longitudinal channels, comprising an adherent, coating formed of cohered, compact mesoporous particles each being formed of a material that is compatible with the material forming the underlying substrate structure so as to become adherent thereto when coated. The mesoporous particles are capable of supporting in their mesopores a sorbent for CO2 There is also provided a method for forming the monolith and a system for utilizing the monolith as part of a CO2 capture structure, within the system, to remove CO2 from the atmosphere.

Description

INTRODUCTION AND BACKGROUND OF THE INVENTION

The prior art teach us that there may be myriad methods products, apparatus and systems capable of capturing and sequestering carbon dioxide, and other acidic gases from mixtures of gases. However, the art has not as yet found a product that can be used in different systems and apparatus in a highly effective and efficient manner, both from the view of capital and operating costs and from the view of energy efficiency. The following patents disclose some of the apparatus and systems in which the product of the present invention can be used.

There is much attention currently focused upon trying to achieve three somewhat conflicting energy related objectives: 1) provide affordable energy for economic development; 2) achieve energy security; and 3) avoid the destructive climate change caused by global warming. However, it is believed by experts in the energy field that it is unlikely that our society will be able to avoid using fossil fuels at least during a significant part of this century.

It is also clear that there is a continuing need for further improvement in the efficiency of the systems and methods for removing additional CO2 from the atmosphere, known as Direct Air Capture (or DAC). All of the following patents and patent applications are directed and relate to the capture of carbon dioxide from ambient air and mixtures of gases, some of which contain ambient air.

U.S. Pat. No. 10,512,880 granted Dec. 24, 2019 entitled âRotating multi-monolith capture structure movement system for removing carbon dioxide from the atmosphere.â U.S. Pat. No. 10,413,866 granted Sep. 17, 2019 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 10,239,017 granted Mar. 26, 2019 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 9,975,087 granted Mary 22, 2018 entitled âSystem and method for carbon dioxide capture and sequestration from relatively high concentration carbon dioxide mixtures.â U.S. Pat. No. 9,937,461 granted Apr. 10, 2018 entitled âSystem and method for carbon dioxide capture and sequestration utilizing an improved substrate structure.â U.S. Pat. No. 9,925,488 granted Mar. 27, 2018 entitled âRotating multi-monolith capture structure movement system for removing carbon dioxide from the atmosphere.â U.S. Pat. No. 9,908,080 granted Mar. 6, 2018 entitled âSystem and method for removing carbon dioxide from an atmosphere and global thermostat using the same.â U.S. Pat. No. 9,878,286 granted Jan. 30, 2018 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 9,776,131 granted Oct. 3, 2017 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 9,630,143 granted Apr. 25, 2017 entitled âSystem and method for carbon dioxide capture and sequestration utilizing an improved substrate structure.â U.S. Pat. No. 9,616,378 granted Apr. 11, 2017 entitled âSystem and method for carbon dioxide capture and sequestration from relatively high concentration carbon dioxide mixtures.â U.S. Pat. No. 9,555,365 granted Jan. 31, 2017 entitled âSystem and method for removing carbon dioxide from an atmosphere and global thermostat using same.â U.S. Pat. No. 9,433,896 granted Sep. 6, 2016 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 9,227,153 granted Jan. 5, 2016 entitled âCarbon dioxide capture/regeneration method using monolith.â U.S. Pat. No. 9,061,237 granted Jun. 23, 2015 entitled âSystem and method for removing carbon dioxide from an atmosphere and global thermostat using same.â U.S. Pat. No. 9,028,592 granted May 12, 2015 entitled âSystem and method for carbon dioxide capture and sequestration from relatively high concentration carbon dioxide mixtures.â U.S. Pat. No. 8,894,747 granted Nov. 25, 2014 entitled âSystem and method for removing carbon dioxide from an atmosphere and global thermostat using the same.â U.S. Pat. No. 8,696,801 granted Apr. 15, 2014 entitled âCarbon dioxide capture/regeneration apparatus.â U.S. Pat. No. 8,500,861 granted Aug. 6, 2013 entitled âCarbon dioxide capture/regeneration method using co-generation.â U.S. Pat. No. 8,500,860 granted Aug. 6, 2013 entitled âCarbon dioxide capture/regeneration method using effluent gas.â U.S. Pat. No. 8,500,859 granted Aug. 6, 2013 entitled âCarbon dioxide capture/regeneration method using vertical elevator and storage.â U.S. Pat. No. 8,500,858 granted Aug. 6, 2013 entitled âCarbon dioxide capture/regeneration method using vertical elevator.â U.S. Pat. No. 8,500,857 granted Aug. 6, 2013 entitled âCarbon dioxide capture/regeneration method using gas mixture.â U.S. Pat. No. 8,500,855 granted Aug. 6, 2013 entitled âSystem and method for carbon dioxide capture and sequestration.â U.S. Pat. No. 8,491,705 granted Jul. 23, 2013 entitled âApplication of amine-tethered solid sorbents for carbon dioxide fixation from air.â U.S. Pat. No. 8,163,066 granted Apr. 24, 2012 entitled âCarbon dioxide capture/regeneration structures and techniques.â

The present invention provides a monolith product that will be useful in improving the operation of the above and many other products and systems previously used for the removal of CO2 from the atmosphere.

GENERAL STATEMENT OF THIS INVENTION

The present invention teaches a novel and surprisingly effective product, that can be associated and combined with many systems, apparatus and methods of capturing carbon dioxide or other acidic gases, from ambient air or from mixtures of other gases mixed with ambient air, mixtures such as ambient air with a minor proportion of an effluent gas, or flue gas, from processes powered by, e.g., the oxidation of hydrocarbons. In one embodiment of the present invention disclosed herein, carbon dioxide is captured using a system comprising a rotating multi-capture movement system, described in more detail below. In another embodiment of the invention, carbon dioxide is removed from a stream of gas that includes ambient air, combined with flue gas from a fossil fuel combustion source. In yet another system in which the present invention of a defined product is used for removing CO2 from mixed gases; the product of this invention is supported within a stationary system, which alternates as the CO2 separation chamber and the regeneration chamber; this stationary system is operated by the automated opening and closing of valves controlling flow through conduits into or out from the stationary chamber, and out from or into sources of the desired gas or vapor or destinations for the outputs from the system, as well as for other fluids for treating the feed gases or for regenerating the sorption systems.

Additionally, and in one embodiment, the present invention teaches the combination of a structural, rigid, substrate, defined further as having longitudinal channels extending between opposing surfaces of the substrate, the channels have walls that support, within the longitudinal channels, an applied dried and sintered coating of defined predetermined characteristics. In one preferred embodiment of the present invention, the rigid substrate is formed in the general shape of a solid form having a generally polyhedral shape, or a tubular shape. In more preferred embodiments, for space efficiency reasons under most circumstances, in the shapes of regular polyhedrons. In all geometrical shape embodiments, the rigid substrates are formed with longitudinal channels extending therethrough, the channels having outer surfaces through which the gas mixture to be treated flows. The walls of the channels are coated with a solid macro-mesoporous coating formed of sintered coherent mesoporous particles adhered to the wall of the channel, leaving a central channel for passage of the ambient air or the mixed gases.

One method for forming the macro-mesoporous coating is to apply a liquid slurry comprising mesoporous particles, binders and rheologically effective materials, to form a viscous slurry that adheres to the walls of the channels in the substrate, so that the slurry can be dried and sintered to the walls of the channels. The sintered adhered coating has characteristics that can be defined as a sintered, coherent, mass of porous particles, providing a combination of macropores and mesopores, both of defined sizes.

In one embodiment the macropores are provided by the spacing between the individual sintered particles forming the coating and the mesopores are formed as pores within each particle. In preferred embodiments, the macropore separation of the particles is preferably at least about 200 nm, and in another embodiment the separation is between 200 and 500 nanometers. In other preferred embodiments, the mesopores within each particle have pore diameters of at least about 10 nm and in another preferred embodiment a pore size of preferably between 20 and 50 nm in diameter.

The aforementioned channel wall coatings, in another embodiment, can be formed from a liquid slurry of particles suspended in a liquid, and where particles have a diameter of at least about 200 nm and preferably a particle diameter of between 200 and 900 nm. It is contemplated by the present invention that the said slurry, when applied on the surface of the channels through a stable solid substrate and then sintered, the particles cohere together and adhere to the stable substrate channel walls. In one embodiment, the individual mesoporous particle diameter can be substantially the same size as the macropore diameter, especially when the particles are compact in shape, and are sintered together. The macropores can be slightly larger than the original compact particle size. The actual predetermined macropore size is a function of the particle size, the distribution of particle sizes, and the other materials present in the slurry, as well as the sintering process. The individual particles making up the slurry are formed such that they have internal porosity in the range of the desired mesoporosity of the finished sintered washcoat. In preferred embodiments, the overall diameters of the coating particles have a particle size that varies by not more than about 20% and more preferably of not greater than 10%.

It is further contemplated by this invention that, in order to achieve a desired predetermined macropore size throughout the sintered washcoat, the individual particles are relatively compact in substantially all directions.

In another embodiment, the aforementioned individual particles are preferably formed of a metal oxide, such as alumina or titania, although other such metal oxides are contemplated as coming within the scope of the present invention.

The slurried washcoat can be applied as a single coating or in multiple coats. When sintering the slurry coated upon the channel walls of the structurally stable substrate, the preferred sintering temperature of the sintering temperature will be a function of the material of the particle, as well as the materials forming the liquid suspension and the material forming the structural substrate; such a temperature, in one embodiment of the preparation is as low as 250Â° F. The slurrying liquid is preferably an aqueous liquid containing a desired binder material, such as boehmite, to assist in forming the desired sintered structure.

DISCUSSION

It is now clear that there are many technically feasible methods available to directly capture carbon dioxide from the atmosphere utilizing, e.g., a single capture large monolithic unit operating together with a regeneration system, whereby the CO2 is directly adsorbed onto the monolith, as described above. These systems, as well as others to be developed in the future can be greatly improved by using the channel containing monoliths of the present invention, which contain a plurality of separate sorbent supporting particle-coated channels extending therethrough. In one embodiment a large monolithic unit can be formed of a plurality of smaller monoliths formed in accordance with the present invention, by combining and holding together, either by adhesively binding a plurality of small monoliths together or by binding them together by an outside framework within which the individual small monoliths are held together.

A preferred embodiment can be formed of a plurality of smaller modular tubular monoliths, stacked together, or by forming a single large monolith. In all cases, it is necessary to provide channels extending through each portion of the monolith or through each of the modular smaller monoliths. The total size of the individual capture structures, which can be formed of a plurality of any number of smaller modules having the individual channels extending therethrough. The individual modules can be adhesively bound together, and/or held together within an outer frame. The individual modular monoliths can have, for example only, cross-sections of polygons, such as polygons such as squares, hexagons, octagons, or rounded shapes such as circular or ovoidal.

Each monolith or modular small monolith is provided with longitudinal channels extending between the opposing sides of the monolith or modular small monolith, and can have substantially any cross-sectional shape, including, by way of example only, polygons such as triangular, or parallelograms, including without limitation, squares, rectangles, hexagons, or octagons, or rounded shapes such as circular or ovoidal.

The critical portion of each capture structure is the density of the channels extending through the single monolith or bound individual modular monolithic capture structure. Preferably the channels are substantially parallel in the entire structure. The channels can have cross-sections that are of almost any configuration, as long as the flow of air is not overly constricted. Exemplary channel cross-sections include triangular, or parallelograms, including without limitation, squares, rectangles, hexagons, or octagons, or rounded shapes such as circular or ovoidal, bell-curves (think corrugated cardboard), diamonds/rhomboids.

In one preferred embodiment of this invention the total capture structure monolith can be formed of a plurality tubular modules having one of the above cross-sectional shapes.

In one embodiment, the monolith is moved between a location where it is exposed to the ambient air, or to mixture of gases, and then moved to a separate regeneration unit; in another embodiment the monolith is maintained within the same chamber and by the use of automatically operating valved conduits the same chamber can be used for passing the CO2-rich gas mixture through the channels of the monolith and for regeneration of the sorbent held within the mesopores of the particles coated on the channel walls in the monolith, to release the CO2 and to regenerate the sorbent for future use.

INTRODUCTION AND BACKGROUND OF THE INVENTION

GENERAL STATEMENT OF THIS INVENTION

DISCUSSION

In one preferred embodiment of this invention the total capture structure monolith can be formed of a plurality tubular modules having one of the above cross-sectional shapes.

In both embodiments, the sorbent-supporting monolith is treated with process heat preferably in the form of steam generated from the secondary energy output of some type of a primary system, such as a power generating unit, a cement plant, or other manufacturing facility. In each of these cases the mesoporous substrate structure for the sorbent will contain sufficient sorbent to permit the economical removal of carbon dioxide from air and produce substantially pure CO2 during regeneration; the substantially pure CO2 can be available, for example, for the manufacture of hydrocarbon fuels, or available for improving the agricultural output of greenhouses or other applications requiring merchant CO2.

These and other features of this invention are described in, or are apparent from, the following more detailed description, related to the accompanying drawings.

BRIEF DESCRIPTION OF THE FIGURES/EXHIBITS

FIG. 1 is a diagrammatic top view of one preferred embodiment of this invention showing a mutually interactive pair of rotating multi-capture structure systems for removing carbon dioxide from the atmosphere according to an exemplary embodiment of this invention, illustrating in sketch form a grade level regeneration chamber for each loop and a plurality of capture structures, the two capture structures immediately upstream from each of the regeneration chambers being provided with sealable conduits for feeding cleaned flue gas to the capture structures;

FIG. 2 is a schematic illustration of a track level version of a pair of regenerating chambers for removing carbon dioxide from the capture structures medium of FIG. 1 , showing the movement of the capture structures along the track level, air or flue gas contact positions (where the gas flow can be aided by a mechanical blower) into the regeneration chamber position;

FIG. 3 is a top plan [schematic elevation] view of the regeneration chambers of FIG. 2 , and capture structures on adjacent capture structures, showing the piping system arrangement for each chamber and between the chambers;

FIG. 4 is a schematic elevation view showing fans which are stationary relative to one of the capture structures, and which rotate with its respective capture structure;

FIG. 5 is a diagrammatic side elevation view of a design for Dual Induced Axial Fans and Plenums of FIG. 4 ;

FIG. 6 is a diagrammatic representation of an all-around seal between a regeneration box and monolith structure;

FIG. 7 is a diagrammatic elevation view of one of the mutually interactive pair of rotating multi-capture structures system, showing the track level regeneration chamber for removing carbon dioxide from the atmosphere, and the immediately successive capture structure treating a flue gas for CO2 capture;

FIG. 8 is a block diagram depicting the basic concept of direct air capture from ambient air where the adsorption unit is exposed to ambient air for a predetermined period of time, that is 9 times longer in duration than the time each unit spends in the desorption or regeneration unit; The monolith product of the present invention improves the effectiveness of a system such as this compared to prior such sorbent-supporting structures;

FIG. 9 is a block diagram of the improved CO2 capture system of the present invention wherein ambient air is passed over the direct air adsorption unit for a period of time 8 times longer than each unit spends in the CO2 desorption unit and in the final, ninth stage, before desorption the ambient air is admixed with flue gas to form a gas mixture containing about 1% CO2 in the final stage before being placed in the CO2 desorption or regeneration unit; The monolith product of the present invention improves the effectiveness of a system such as this compared to prior such sorbent-supporting structures;

FIG. 9 A is a further variation of the direct air capture unit wherein the exhaust from the 9 th stage is passed back to be mixed with the ambient air in the 8 th stage before the 8 th stage passes into the 9 th stage where it is blended with the mixture of fresh flue gas and air to form a feed of 1% CO2;

FIG. 10 depicts an idealized drawing of the sintered macro-mesoporous coating of the walls of the longitudinal channels through the monolithic carrier of the present invention, in a situation where the size of the compact individual sintered particles are fairly uniform;

10 A depicts a diagrammatic comparison showing the effect of a greater distribution of different sized particles on the macropore size openings existing between the particles of the sintered particulate porous coating;

10 B depicts the internal mesopores extending into the individual particles of the sintered coating;

FIG. 11 is a cross-sectional diagram depicting an individual longitudinal channel through each monolith, showing the channel wall 760 , the sintered washcoat for supporting the CO2- sorbent 763 , and the open longitudinal channel through the monolith for the passage of the CO2-rich gases;

FIG. 11 A depicts three sizes of the basic monoliths 760 , and the protective and in some cases supporting screen connected to the opposing faces between which the longitudinal channels extend;

FIG. 11 B depicts in diagrammatic form the flow of the ambient air through the monolith longitudinal channels 765 , with the CO2 molecules being absorbed by the sorbent supported in the sintered coating and aa partial cross-section showing the channels and the walls between the channels extending between opposing sides of a monolith in cubic form;

FIG. 11 C depicts a cordierite monolith, containing 230 longitudinal channels per square inch (âCPSIâ), with 8 mil walls between the channels, providing 77.2% OFA;

FIG. 11 D depicts a cordierite monolith, containing 230 longitudinal channels CPSI, with 7.5 mil walls between the channels, providing 77.2% OFA;

FIG. 11 E depicts an aluminum hex cell monolith, containing 100 longitudinal channels CPSI, with 1.2 mil walls between the channels, providing 97.6% OFA;

FIG. 11 F depicts an alumina-fiberglass corrugated cell monolith, containing 70 longitudinal channels CPSI, with 13 mil walls between the channels, providing 79% OFA;

FIG. 11 G depicts a porous titania extrudate monolith, containing 170 longitudinal channels CPSI, with 9 mil walls between the channels, providing 77.9% OFA;

FIG. 12 shows the change in efficiency with increased loading of the sorbent based upon percent of amine sorbent loading in the mesopores of the sintered coating on the channel walls;

FIG. 13 shows the change in amine efficiency with increased loading ratio of the sorbent based upon percent of amine sorbent loading in the mesopores of the sintered SiO2 coating on the channel walls;

FIG. 14 shows the effect of particle size on the diffusion of the CO2 from the surface of the monolith wall to the particle holding the sorbent;

FIGS. 15 - 18 depict the graphical results of the Examples 1-4 in the specification.

DETAILED DESCRIPTION OF THE INVENTION

In an embodiment of this invention, the sintered coating is from a viscous slurry comprising mesoporous particles and ancillary materials, such as binders and rheological materials that provide sufficient viscosity and adhesion to adhere in an even coating on the channels of the solid monolith.

In another embodiment of the present invention, the capture structures for exposure to the flow of CO2-rich gases a single structure formed from a plurality of the individual small monoliths secured together by an adhesive or an outer framework pressing the individual small monoliths together, to form a single large monolith providing the desired open longitudinal channels to the flow of CO2-rich gases to be cleaned of CO2. Preferably all of the small monoliths joined together have the same CPSI and the same amount of sorbent in the channel wall coating.

The monoliths can be exposed to the mixed gases while moving and moved into a separate regeneration chamber for regenerating the sorbent by stripping the sorbed CO2 from the coated walls on the channel walls of the monolith.

In another embodiment, the monolith with the coated longitudinal channel walls can be immovable while exposed to the CO2-rich gases and then a sealable chamber can be moved around the monolith, within which it can be regenerated to strip and capture the CO2 sorbed on the walls coated with the sorbent-supporting coating.

In yet another embodiment of this invention, the monolith can be maintained within a single sealable chamber and alternatively exposed to the CO2-rich gases and then the process heat steam for stripping the CO2, and regenerating the sorbent, by the automatic operation of valving to change the materials entering and leaving the chamber. Specifically, the automatic operation of the valved conduits connected to the closed and sealed structure, are designed by known methods to be capable of switching between a source of ambient air, i.e., the atmosphere, for example, and a source of process heat steam, for example. Steam sourced from preferably the secondary process heat of a primary plant, can be used in these carbon capture systems at temperatures of not greater than 120Â° Celsius and preferably below 100Â° C., to as low as 60Â° C., so that the operating costs for the system would be lowered.

In yet another embodiment of the present invention, a non-coated monolith, such as, by way of example only, a fully porous monolith provided with the longitudinal channels where the walls are formed of the sintered mesoporous particles and the space between particles provide the necessary macroporous openings. In this embodiment, porous titania extrusions are useful, as well as porous alumina or porous silica or other porous metal oxides.

In one embodiment, the use of a fully porous extrusion, formed as individual bricks, provide a useful construction for a desired non-coated monolith comprising a stack of monolithic bricks having the desired structural durability and rigidity, preferably having a porous surface and narrow channels extending longitudinally through each brick, that will provide the necessary volume for the required reservoir of the desired sorbent. In this situation adsorbency is by the amount of sorbent present in the pores on the surface of the walls of the longitudinal channels through each brick.

In all of the embodiments of this invention, the amount of porosity, i.e., the macroporosity and the mesoporosity, required is a function of the time period required for the sorbent action to be accomplished for a given amount of sorbent material. This allows for the greatest economy of scale when adsorbing CO2 using a sorbent-containing porous substrate. In one embodiment, relatively small bricks, in a hexahedral shape, such as one where all of the surfaces are squares or one in which the four largest faces are rectangular, are piled into a tetrahedral shape where the two largest faces are rectangular, and the piled shape is supported by a surrounding frame to provide the necessary structural strength of the overall monolithic structure. Alternatively, or in addition, the individual brick monoliths, may be adhesively connected. In some embodiments, this large monolithic structure formed of the piled bricks comprises the capture structures in the system and methods for air capture, described herein.

In the preferred embodiment, the structural substrate is formed so as to include straight longitudinal channels running axially between the two exposed major surfaces. In the more common case, the walls of the channels are coated with a sintered coating having a thickness of at least 2 mils. The coating is preferably formed of compact mesoporous particles having a diameter of at least about 200 nm.

The internal structural substrate can be formed of a structurally strong Cordierite, aluminum, fiberglass, fecralloy, other metals, inorganic oxides (alumina, titania, silica, etc.), ceramic, polymers (polyethylene, polypropylene, polycarbonate, etc.), carbon, etc. Some of these materials should be used under certain circumstances, where the temperatures are maintained at a lower value, such as fiberglass impregnated polymers, other plastics and carbon fiber enhanced such materials.

All of these structural substrates can be manufactured by extrusion, aggregation, corrugating, templating, 3D printing, molding, etc. The structural substrate is to provide structurally stable geometry, at the operating temperatures for the sorbent apparatus as it is exposed to ambient air or mixtures of ambient air with an effluent gas such as that sourced from a hydrocarbon fuel heating system, or while the sorbent is being regenerated. The structural substrate must be capable of stably supporting a cell density and channel shape, for the combination with a porous coating. The porous coating must be formed of porous particles that can be sintered together to form what will be referred to as the macroporous coating structure supported on the channel walls of the structural substrate. It must form a stable porous coating having good physical and chemical adhesion with the structural substrate in order to form the desired mesoporous structure within which the sorbent will be primarily maintained.

a. The monolith structural substrate with straight channels running axially, can be formed of Cordierite, aluminum, fiberglass, fecralloy, other metals, inorganic oxides (alumina, titania, silica, etc.), ceramic, polymers (polyethylene, polypropylene, polycarbonate, etc.), carbon, etc. The substrate can be formed by being extruded, corrugated, templated, 3D printed, molded, etc. to form the monolith structure. The material forming the substrate can be porous or nonporous. The cell density (channel openings), in preferred embodiments of this invention can be 50-400 CPSI. The channel wall thickness, in preferred embodiments of this invention, can be 0.2 mil-20 mil. The OFA of the faces into which the channels open, in preferred embodiments of this invention can be 0.5-0.98th. The channel cross section geometry, in preferred exemplary embodiments of this invention, can be polygons such as squares, hexagons, octagons, or circular or ovoidal, bell-curves (think corrugated cardboard), diamonds/rhomboids. The individual channels can have a length of, in preferred embodiments of this invention, 3-24â³. The channels, in preferred embodiments of this invention, can be coated with a macro-mesoporous coating, via dipcoating (single or sequential) or some other coating method with a washcoat slurry containing mesoporous particles applied to a substrate channel walls as defined above, to form a macro-mesoporous coating. The coating comprises mesoporous particles of inorganic oxide (alumina, silica, titania, etc.), porous mineral/ceramic (e.g., boehmite), etc. The porosity is in the range 0.7-0.96, in preferred embodiments of this invention, and have a mesopore volume range of 0.4 cc/g-1.5 cc/g. The most prevalent mesopore diameter is 10-50 nm, with a coating thickness range of 2-15 mil after sintering. The macropore diameter range, in preferred embodiments of this invention, is 0.1-2 microns; and the macropore/mesopore ratio range is 1:5-2:1 (20% macro-80% meso to 66% macro-33% meso).

The porous coatings on the channel walls can accept, in preferred embodiments of this invention, an active sorbent material, preferentially in the mesopores. The sorbent can be physically impregnated or chemically bonded to the mesoporous particles and can be aminopolymers (pei, ppi, paa, pva, pgam, etc), blends of polymers (aminopolymers with each other, aminopolymers with PEGs, etc.), chemically modified polymers, polymers+ additive blends, MOFs, zeolites, etc.

The polymers can be branched, linear, hyperbranched, or dendritic, and a molecular weight range of 500-25000 Da, depending upon the polymer structure. Mesopore volume occupancy of the sorbent (pore filling), in preferred embodiments of this invention, can range from 40-100%. The macropore volume occupancy (pore filling) range can be 0-15%.

In another preferred embodiment of this invention, the entire monolith substrate with longitudinal channels, is formed of the macro-mesoporous media described as a coating above. In other words, the entire monolith is a homogeneous porous body, having no distinct interface between substrate and channel wall washcoat, but containing meso-macroporous particles throughout the monolith. One example of such a homogeneous porous body, includes homogeneous porous monolith formed of a fibrous network, the fibers providing the body structural integrity and the adhered particles providing the entire body with meso and macroporosity:

The material forming the embedded particles can include, in some embodiments, the same inorganic oxides (alumina, titania, silica, etc.), ceramic, carbon, polymer, binders and fillers.

The cell density of the channel openings are preferably in the range of 64-400 cpsi. The channel wall thickness is preferably 3-30 mil, with an OFA of 0.5-0.8; and the channel opening cross section geometry in some of these embodiments can be, for example, square, hexagonal, cylindrical, bell-curve (as in corrugated cardboard), diamond/rhomboid, etc.; other preferred parameters of these homogeneous monoliths are:

Channel length of 3-24â³; Porosity range of 0.3-0.9 Mesopore volume range of 0.2 cc/g-1.5 cc/g The preferred range of most prevalent mesopore diameter is in the range of 10-50 nm; The preferred macropore diameter range is 0.15-2 micron; and Macropore/mesopore ratio range is 1:5-3:1 (20% macro-80% meso to 75% macro-25% meso) Cell, or channel opening density of 64-400 cpsi; wall thickness, between the channel openings of 3-30 mil; an OFA of 0.5-0.8

As previously explained, the particles on the walls of the channels can accept the same active sorbent materials as described above for the coated wall structures.

A system for that purpose of capturing CO2 has been developed that includes the above structures and a method for achieving the efficient and effective capture of CO2 from ambient air and other mixtures of gases.

In most embodiments of this invention, except as described immediately above, the structural substrate is substantially inert with regard to sorbent activity or to the slurried washcoat, so that the mass of the substrate monolith should be minimized by forming the channel walls at a minimum thickness sufficient to maintain its structural strength and stable structure. In one preferred embodiment, the substrate will be provided with straight channels connecting two opposed surfaces of the monolith. The wall thickness separating the longitudinal channels should be preferably from 0.2 mil-20 mil, as long as it is sufficient to maintain structural integrity. This effectively minimizes the thermal mass of the monolith structure, and thus minimize the costs of the heating or cooling required during adsorption or desorption, while maintaining sufficient structural strength to maintain the shape of the porous walls, which maintains the structure of the macropores to permit the mixed gas to reach the sorbent in the mesopores of the particles. Maintaining the shape of the channel walls also prevents the collapsing of the channels, so as to maintain the flow of the gas without requiring increasing pressure drop. Pressure drop is a function of the hydraulic diameter and lengths of the open channels through the structural substrate. The channel openings density is preferably in the range of 50-400 CPSI.

In another preferred embodiment, the commercial monolith will be formed of individual bricks stacked together in a stable geometry, where the individual bricks are as described above, preferably, e.g., polyhedrons such as hexahedrons or decahedrons, or tubular shapes, in all cases having longitudinal channels extending between opposing faces, with the interior walls separating the channels being coated with the macro-mesoporous coating; the length of each individual brick is preferably in the range of 3-24 ins.; the individual bricks can have equal sides or four of the sides can be rectangular; the macro-mesoporous coatings can be as described above.

The porosity of the individual particles in the slurry is preferably in the range of 0.7-0.96; the mesopore volume range is 0.4 cc/g-1.5 cc/g; the most prevalent mesopore diameter is in the range of 10-50 nm; the thickness of the final dried and sintered coating is in the range 2-15 mil. The sorbents can be aminopolymers, such as polypropylenimine (PPI), polyallylamine (PAA), polyvinylamine (PVA), polyglycidylamine (PGA), zeolites, etc.), blends of polymers (aminopolymers with each other, aminopolymers with PEGs, phenyl core polyamines (PhXYY), etc.), chemically modified polymers, polymers+ additive blends, metal organic frameworks (MOFs), porous organic frameworks (POFs), and covalent organic frameworks (COFs).

The amino polymers can be branched, linear, hyperbranched, or dendritic; the polymers can have a molecular weight in the range of from 500-25000 Da; the mesopore volume occupancy (pore filling) range can be from 40 to 100%; the macropore volume occupancy (pore filling) is in the range of from 0-15%, and should be minimized to avoid interfering with the flow of the mixed gases through the coating and into the mesopores of the individual particles, and ultimately out through the channels extending through the structural substrate.

The cost for heating the structural substrate as a thermal mass, of all of these monoliths, should be minimized, especially by minimizing the mass of any structural substrate. Furthermore, the thinner the wall thickness between channels, of the structural substrate, the higher the capacity for CO2 adsorption, as more macro-mesopore coating can be applied for the same pressure drop, yielding a higher volume of the sorbent within the porous system that can be reached by the flow of the CO2-laden air or other mixed gas flow.

The macroporous structure of macro-mesopore coating is formed on the surface of the channel walls. The macroporous structure of the porous coating is intended to provide the higher support volume for holding the sorbent in a morphology that is accessible to CO2 over the timescales needed to maximize production of CO2 per volume of a full-size monolith. The slurry of mesoporous particles is wash-coated onto the channel walls of the preformed structural substrate in either a single or multiple sequential coating steps, to build the macro-mesopore coating to the thickness that is desired.

The macro-mesopore coating is preferably formed from a slurry of mesoporous particles by drying and sintering together the particle slurry coated on the surface of the channel walls. The inter-particle volumes within the sintered coating define the macropores, which are formed by the spaces between the sintered particles.

The mesopore volume within the sintered coating in some embodiments of this invention contains mesopores preferably within the range of 10 nm to 50 nm diameter and optimally within the 20-40 nm range.

Further Aspects of the Present Invention:

The present invention provides further new and useful improvements to previously described DAC systems, apparatus and methods for removing carbon dioxide from a mass or stream of carbon dioxide-laden air, at higher efficiencies and lower overall costsâincluding lower capital expenses (âCAPEXâ) and lower operating expenses (âOPEXâ).

In accordance with one of several preferred embodiments of the present invention, a novel process and system has been developed utilizing an assembly of a plurality of separate CO2 capture structures, each supporting substrate capture structure, as described above, or capture structures of substrate particles, are combined with a single regeneration box, in a ratio dependent upon the ratio of the speed of adsorption from ambient air, or from whichever gas mixture is being treated to remove CO2, compared to the speed of regeneration of the captured CO2-laden sorbent. In preferred embodiments, the CO2 capture structures are supported on a closed loop track, preferably forming a closed curve; the CO2 capture structures move longitudinally along a loop defined by the track, in succession, while being exposed to a moving stream of ambient air or a mixture of gases comprising ambient air. Alternatively, the capture structures can be moved longitudinally back and forth along an open-ended track.

At one location along the track, one of the CO2 capture structures is moved into a sealed chamber for processing, i.e., to strip CO2 from the sorbent and to regenerate the sorbent. When the sorbent is regenerated, the capture structure being regenerated leaves the regeneration chamber and the capture structures are rotated around the track until the next CO2 capture structure is in position to enter the regeneration box, and so on. The improvement of this invention provides for at least one of the capture structures to receive flue gas in place of ambient air, and preferably at least a majority of the other capture structures would be fed ambient air. Most preferably it would be substantially the last station before the regeneration box where the capture structures would receive the flue gas, or a mixture of ambient air with flue gas as the input.

In a preferred example the monoliths can complete one complete rotation along the track loop in about 1,000 seconds.

The velocity and concentration of the input flue gas mixture is independently controlled on the input side, though the output from the channels can be assisted by exhaust fans adjacent the exhaust side of the monolith. Ideally this could be a retrofit on to a pure DAC unit. It would enable the sorption of additional CO2, and preheat the sorbent array, by the sorption heat of reaction, before entering the regeneration box. The cool down of the array after the regeneration box could remain unchanged, though the heat removed might be used for other purposes, since the array was already preheated before regeneration began. The advantages of this integrated approach over a separate DAC and system for mixing a flow of ambient air and flue gas are as follows.

This approach, using a flue gas mixture at the last station before regeneration, increases the overall production of CO2 per DAC plant by an expected 30 to 50% and thus reduces the capex per yielded metric ton of captured CO2.

This approach reduces the capital cost of the flue gas capture component by using the same capital plant as the DAC.

The energy used per tonne of CO2 produced is reduced

(A) because the amine sites binding the high concentration CO2 flue gas mixture increase the amounts of CO2 held by the sorbent per unit time; (B) because this system has more CO2 being captured for the same sensible heat; and (C) because the higher temperature flue gas mixture will preheat the array. Examples of a system as described above is shown in the drawing FIGS. 1 - 10 .

There are three cases to consider for this system:

(A) The standalone case where a heat & power cogeneration unit (hereafter: Cogen) is sized to provide the heat and power for the GT facility. (B) as an adjunct to larger Cogen facility so the heat and flue gas CO2 available is larger than will be used for the DAC unit and excess electricity and heat will be generated. (C) The case of a negative carbon power plant where one will be capturing the CO2 from the power source and sizing the DAC provided based upon the need to remove the flue gas CO2 as well. (In this case one can choose the amount of flue gas CO2 captured based upon costs because the facility overall is carbon negative (e.g., removing more CO2 than would otherwise have been emitted without capture). (D) The interesting observation is that for all three cases the same design holds; all that one is changing is the size of the Cogen plant being determined in [A] by our DAC energy needs, in [B] the energy needs of the specific application (compression, etc.), and in [C] by the size of the carbon negative power plant.

When an adjacent plant is a power plant, the product of such plant including cogenerated or surplus steam and electricity for operating the DAC plant is provided. The effluent flue gas from such power plant is at least partially cleaned before the effluent is fed to the final stage of CO2 capture, immediately prior to entry into the regeneration chamber. In addition, a partially pre-treated, CO2 reduced effluent can be used either alone or in admixture with ambient air in the eighth position, i.e., the position or stage immediately preceding, the flue gas capture stage of the system shown especially in the attached drawing figures of FIGS. 1 , 7 , and 9 ; it is understood of course that where there are, for example, 10 capture structures, with a single regeneration chamber, the regeneration chamber is the 10 th stage and the immediately preceding capture structure stage, before the capture structure enters the regeneration chamber, is the 9 th stage, and the second preceding stage is the 8 th stage. Examples of suitable structures for the system is shown in the drawings and descriptive text below.

Another preferred embodiment provides for the CO2-laden feed to include a previously partially captured flue gas, for example the exhaust from the final or last capture structure or the exhaust from a conventional CO2 removal system, conventionally used in industries having large CO2 containing exhaust, such as fuel burning power plants, cement manufacturing plants, steelmaking plants, and the like. Such systems involving the pretreatment of the effluent, are especially important when dealing with the exhaust from either solid, e.g., coal, or liquid e.g., petroleum oil, combustion process, which often include fine particulate matter, solid or liquid particles, and noxious gases.

A further preferred embodiment is a situation where a plant produces fuel intended for sale or use in other locations, from the CO2 produced from the plant of the present invention (e.g., via synthetic fuel production with H2).

Porous Substrate:

As explained above, the present process however is a low temperature (e.g., preferably ambientâ100Â° C.) semi-continuous process, with mass transport of the gas through the pores and sorbent at each phase of the process. Further, in one preferred embodiment the sorption reaction occurs on a sorbent impregnated within the macro-mesoporous coatings on the channel walls through a monolithic substrate. In such circumstances, the macroporosity is most preferably tuned to maximize pore volume rather than surface area. In order to accomplish this preferred situation, the preferred substrates are formed of structurally stable substrate having porous coatings covering the channel wall surfaces of the substrate. Although such coatings have been used in the production of catalytic structures, the preferred sorbent capture structures of this invention require significantly thicker porous coatings than traditional catalytic contactors with completely different preferred pore size and distribution due to the importance of total pore volume rather than total surface area of the channel walls.

CLAIMS

Claims ( 21 )

1 - 20 . (canceled)

21 . A method for removing CO 2 from a gas stream, the method comprising:

contacting a gas stream with a honeycomb monolith containing a CO 2 sorbent;

wherein the honeycomb monolith is comprised of longitudinal channels connecting two opposed surfaces of the monolith;

wherein the longitudinal channels comprise macropore and mesopore containing walls;

wherein the CO 2 sorbent occupies a fraction of a mesopore volume within the macropore and mesopore containing walls;

removing CO 2 from the gas stream by sorbing CO 2 using the CO 2 sorbent as the gas stream flows through the longitudinal channels; and removing the sorbed CO 2 from the CO 2 sorbent by heating the honeycomb monolith to about 60Â° C. to 130Â° C.;

wherein an amount of time taken for removing the CO 2 from the gas stream is about 3 to 10 times an amount of time taken for removing the sorbed CO 2 .

22 . The method of claim 21 , wherein the honeycomb monolith has a channel opening density of about 50 channels per square inch to 400 channels per square inch;

wherein the open face area (OFA) of the opposed surfaces is about 0.5 to 0.9; and wherein a length of the honeycomb monolith is about 3 inches to 24 inches.

23 . The method of claim 21 , wherein the macropore and mesopore containing walls comprise mesopores and macropores;

wherein a macropore diameter is about 0.15 microns to 2 microns; wherein a mesopore diameter is about 10 nm 50 nm; wherein a mesopore volume is about 0.4 cc/g to 1.5 cc/g; and wherein a ratio of macropores to mesopores is about 1:5 to about 2:1.

24 . The method of claim 23 , wherein the macropore and mesopore containing walls comprises sintered mesoporous particles having macropores separating the mesoporous particles, wherein the sorbent comprises an amine.

25 . The method of claim 23 , wherein the longitudinal channels comprise a solid macro-mesoporous coating that forms the macropore and mesopore containing walls.

26 . The method of claim 25 , wherein the macropore and mesopore containing walls is comprised of an inorganic oxide or a porous mineral/ceramic.

27 . The method of claim 26 , wherein the mesopores are physically impregnated with or chemically bonded to a sorbent comprising an amine.

28 . The method of claim 25 , wherein the amine is an aminopolymer, and wherein the aminopolymer is branched, hyperbranched, dendritic, or linear.

29 . The method of claim 21 , wherein the fraction is about 40% to 100%.

30 . The method of claim 21 , wherein the heating occurs by contacting the honeycomb monolith with steam.

31 . The method of claim 31 , wherein the gas stream has an approach velocity of about 2 m/s to 10 m/s.

32 . The method of claim 31 , wherein the gas stream comprises a CO 2 concentration of about 10% or less, and wherein the gas is selected from ambient air, flue gas, or a combination thereof.

33 . The method of claim 31 , wherein the amount of time taken for removing the CO 2 from the gas stream is about 3 times the amount of time taken for removing the sorbed CO 2 , about 9 times the amount of time taken for removing the sorbed CO 2 , or about 10 times the amount of time taken for removing the sorbed CO 2 .

34 . A system for removing CO 2 from a gas stream, the system comprising:

a loop of capture structures, each capture structure comprised of a honeycomb monolith, wherein the honeycomb monolith contains a CO 2 sorbent; and wherein the number of capture structures is equal to a ratio, wherein the ratio is an amount of time taken for removing the CO 2 from the gas stream and an amount of time taken for removing the sorbed CO 2 .

35 . The system of claim 34 , wherein the gas stream comprises a CO 2 concentration of about 10% or less, and wherein the gas is selected from ambient air, flue gas, or a combination thereof.

36 . The system of claim 34 , wherein the honeycomb monolith is comprised of longitudinal channels connecting two opposed surfaces of the monolith;

wherein the channels comprise macropore and mesopore containing walls; and wherein the CO 2 sorbent occupies about 40% to 100% of a mesopore volume within the macropore and mesopore containing walls.

37 . The system of claim 34 , wherein the honeycomb monolith has a channel opening density of about 50 channels per square inch to 400 channels per square inch; wherein the open face area (OFA) of the opposed surfaces is about 0.5 to 0.9; and wherein a length of the honeycomb monolith is about 3 inches to 24 inches.

38 . The system of claim 36 , wherein the macropore and mesopore containing walls comprise mesopores and macropores; wherein a macropore diameter is about 0.15 microns to 2 microns; wherein a mesopore diameter is about 10 nm 50 nm; wherein a mesopore volume is about 0.4 cc/g to 1.5 cc/g; wherein a ratio of macropores to mesopores is about 1:5 to about 2:1.

39 . The system of claim 36 , wherein the macropore and mesopore containing walls comprises sintered mesoporous particles having macropores separating the mesoporous particles, wherein the sorbent comprises an amine.

40 . The system of claim 33 , wherein the macropore and mesopore containing walls is comprised of an inorganic oxide or a porous mineral/ceramic; and wherein the mesopores are physically impregnated with or chemically bonded to a sorbent comprising an amine.

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