CN115672020B - Device for capturing, separating and catalyzing carbon dioxide in flue waste gas and control method thereof - Google Patents
Device for capturing, separating and catalyzing carbon dioxide in flue waste gas and control method thereof Download PDFInfo
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- CN115672020B CN115672020B CN202211587428.1A CN202211587428A CN115672020B CN 115672020 B CN115672020 B CN 115672020B CN 202211587428 A CN202211587428 A CN 202211587428A CN 115672020 B CN115672020 B CN 115672020B
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Abstract
The invention provides a device for capturing, separating and catalyzing carbon dioxide in flue waste gas and a control method thereof, relating to the technical field of waste gas treatment. In the device for capturing, separating and catalyzing the carbon dioxide in the flue waste gas, an air inlet pipe is used for inputting the flue waste gas with the carbon dioxide, the air inlet pipe is wound on a high-temperature area of an outer cylinder reactor, the air inlet pipe, a condensed water collector, a waste gas storage device, an injection pump and the high-temperature area of the outer cylinder reactor are sequentially communicated, and an exhaust valve is arranged on the outer cylinder reactor; the inner cylinder reactor is arranged in the low-temperature zone of the outer cylinder reactor, the rotating chassis is rotatably arranged at the bottom of the inner cylinder reactor, condensed water dripped by a condensed water dripping head sequentially passes through the high-temperature zone and the low-temperature zone and reaches a metal mesh on the rotating chassis, catalyst powder is loaded on the metal mesh, and the cathode electrolyte, the anode electrolyte and solid carbon dioxide hydrate are subjected to electrocatalysis reaction under the action of the catalyst powder on the metal mesh to generate industrial raw materials.
Description
Technical Field
The invention relates to the technical field of waste gas treatment, in particular to a device for capturing, separating and catalyzing carbon dioxide in flue waste gas and a control method thereof.
Background
Carbon dioxide is an important substance causing greenhouse effect, fossil fuel still occupies a dominant position in world energy supply in the next decades, and carbon emission reduction still faces huge challenges, so that the deep development of carbon dioxide capture and sequestration (CCS) technology is widely considered to be of great significance for relieving global warming according to relevant requirements in the environmental field in the current international society, and how to capture and separate carbon dioxide from mixed gas is a premise and a basis for reducing carbon dioxide emission.
The traditional carbon capture method comprises an absorption method, an adsorption method, a low-temperature separation method, a metal oxide method, a membrane separation method and the like, wherein the chemical absorption method is mature and is suitable for the state of low carbon dioxide concentration and normal pressure, but the dosage of an absorbent is large, the supplement is needed in the circulation process, the requirement on the reagent is high, and the energy consumption in the regeneration process is high. The membrane separation method has simple process and simple operation, but has high requirement on raw material gas, and needs pretreatment, dehydration and filtration, and the obtained product has low purity. Therefore, there is a need for methods and apparatus with high capture efficiency and low capture cost.
Due to the physicochemical property and the gas storage characteristic of the hydrate structure, the technology for recovering and storing carbon dioxide by using a gas hydrate method becomes an emerging research hotspot in recent years. The method utilizes the hydrate method to separate the carbon dioxide gas in the flue gas, and compared with the traditional separation method, the method can greatly reduce the separation cost on the premise of effectively improving the separation efficiency. The principle of separating mixed gas by using hydrate method is that the phase equilibrium difference of binary and multicomponent gases when producing hydrate is large, so that the gas which is easy to form gas hydrate can be fed into hydrate phase, and the gas which is difficult to form gas hydrate can be retained in gas phase so as to implement separation of mixed gas.
In the hydrate method carbon capture technology, the conditions required for forming the carbon dioxide hydrate are milder than those required for forming the nitrogen hydrate, for example, at 273.15K, the pressure required for forming the carbon dioxide hydrate is 1.24MPa, and the pressure required for forming the nitrogen hydrate is 16.3MPa. Therefore, the hydrate method is applicable to the capture of greenhouse gases such as carbon dioxide. In addition, the energy density of gas hydrates is high, and 1 volume of hydrate can release about 170 volumes of gas under standard conditions. However, the hydrate nucleation process is characterized by randomness, and a long induction period is accompanied before nucleation. And the hydrate forms and releases heat, and if the generated heat cannot be removed in time, the hydrate is inhibited from further generation. This means that hydrate formation is generally less efficient. The hydrate layer formed at the water-gas interface significantly reduces the gas permeability as hydrates are formed, and thus the mass transport capability of the gas gradually decreases significantly during the growth phase after hydrate nucleation. This means that the resulting energy storage capacity of hydrates is generally low. In addition, most of the hydrates generated in the prior art are in loose snowflake shapes or form hydrate slurry, which occupies most of the growth space and is not beneficial to the efficient and continuous reaction. Therefore, although gas hydrate has great potential in the aspects of capture and sequestration of carbon dioxide, the problems of relatively low capture rate, low gas capture capacity and the like in the carbon capture process by adopting the general hydrate method limit the commercial application scale of the carbon capture technology by adopting the hydrate method.
For this reason, many researchers have conducted basic experimental studies on the hydrate method carbon capture technology, and the used medium is mainly pure water or a solution system. The strengthening methods used include both mechanical strengthening and chemical-physical strengthening. The mechanical strengthening process is usually achieved by increasing the contact area of gas and liquid, such as stirring, bubbling, spraying, atomizing, etc. Through a series of external environment disturbances, the mass transfer and heat transfer efficiency of the hydrate can be increased, and the hydrate generation rate is further improved. In a pure water or solution stirring system, the gas-liquid contact area is improved, but the mass transfer efficiency and the heat transfer efficiency are lower than those of a spraying system. The chemical and physical strengthening method is to add chemical additives (such as surfactant) into water to strengthen gas-liquid contact from the level of nano scale and molecular scale and promote the nucleation growth process of the hydrate.
The existing hydrate method carbon capture technology, no matter forming hydrate in pure water or solution, or forming in porous medium, increases the air/liquid contact area by continuously disturbing liquid phase (such as stirring, spraying, bubbling, etc.), or the liquid stably exists in porous medium to continuously obtain huge air/liquid contact surface.
In addition, most hydrate formation method researches are quantitative intermittent water supply, and no continuous water replenishing measure exists. The feasibility of the hydrate-process carbon capture application technology depends not only on the associated phase equilibrium issues but also on whether rapid hydrate formation is feasible. The hydrate method carbon capture technology which is more widely concerned, such as a hydrate membrane method, a TBAB/THF hydrate method, an external field hydrate method and the like, has the hydrate formation time of over 60min and longer reaction time.
Disclosure of Invention
The invention aims to provide a catalytic device for capturing and separating carbon dioxide in flue waste gas and a control method thereof, which can efficiently capture and separate carbon dioxide in flue waste gas by using a hydrate method and convert generated solid carbon dioxide hydrate into industrial raw materials in situ.
Embodiments of the invention may be implemented as follows:
the invention provides a catalytic device for capturing, separating and catalyzing carbon dioxide in flue waste gas, which comprises an air inlet pipe, a condensate water collector, a condensate water dripping head, a waste gas storage device, an injection pump, an outer cylinder reactor, an inner cylinder reactor, a rotary chassis, an exhaust valve, a cathode reservoir, an infusion pump, an injection conduit, a metal mesh, an anode lead, an anode reservoir and a power supply, wherein the outer cylinder reactor comprises a high-temperature area and a low-temperature area which are arranged up and down;
the air inlet pipe is used for inputting flue waste gas with carbon dioxide, the air inlet pipe is wound on a high-temperature region of the outer cylinder reactor, the air inlet pipe, the condensate water collector, the waste gas storage, the injection pump and the high-temperature region of the outer cylinder reactor are sequentially communicated, and the exhaust valve is installed on the outer cylinder reactor;
the condensed water collector is used for converting water vapor in the flue waste gas into condensed water and collecting the condensed water, the waste gas storage is used for storing the flue waste gas after the water vapor is removed, the flue waste gas is injected into the outer cylinder reactor through the injection pump, and carbon dioxide is removed in the outer cylinder reactor and then is discharged through the exhaust valve;
the condensed water dripping head is arranged at the bottom of the condensed water collector and is inserted into the high-temperature area of the outer cylinder reactor;
the inner cylinder reactor is arranged in the low-temperature zone of the outer cylinder reactor, the rotating chassis is rotatably arranged at the bottom of the inner cylinder reactor, the metal mesh is arranged on the rotating chassis, catalyst powder is loaded on the metal mesh, and condensed water dripped by the condensed water dripping head sequentially passes through the high-temperature zone and the low-temperature zone and reaches the metal mesh on the rotating chassis to form solid carbon dioxide hydrate;
the cathode reservoir is internally stored with a cathode electrolyte, the anode reservoir is stored with an anode electrolyte, the cathode reservoir, the infusion pump and the injection conduit are sequentially communicated, the injection conduit is sequentially inserted into the outer cylinder reactor, the inner cylinder reactor and the metal mesh from top to bottom, the metal mesh, the power supply, the anode reservoir and the anode lead are sequentially connected, the anode lead is connected to the inner wall of the inner cylinder reactor, and the connection position of the anode lead is higher than that of the metal mesh;
wherein, the catholyte, the anolyte and the solid carbon dioxide hydrate are subjected to electrocatalysis reaction under the action of the catalyst powder on the metal mesh to generate industrial raw materials.
In an alternative embodiment, the device for capturing, separating and catalyzing carbon dioxide in flue waste gas further comprises a heat dissipation fin, and the heat dissipation fin is arranged outside the low-temperature zone of the outer cylinder reactor.
In an optional embodiment, the device for capturing, separating and catalyzing carbon dioxide in flue waste gas further comprises an electric rotating machine and a linkage shaft, the electric rotating machine is arranged below the outer cylinder reactor, and the electric rotating machine is connected to the rotating chassis through the linkage shaft so as to drive the rotating chassis to rotate.
In an alternative embodiment, a conductive part is arranged in the universal driving shaft, and the metal mesh is connected to a power supply through the conductive part and a wire.
In an optional embodiment, the catalytic device for capturing and separating carbon dioxide in flue waste gas further comprises an electric valve, the electric valve is connected to the condensed water dripping head, and the electric valve is used for controlling the speed of the condensed water dripping head for dripping condensed water.
In an alternative embodiment, the device for capturing, separating and catalyzing carbon dioxide in flue gas further comprises a switch, and the switch is arranged between the power supply and the anode reservoir.
In an alternative embodiment, the condensate collector, the condensate dripping head, the outer cylinder reactor, the inner cylinder reactor and the rotating base plate are located on the same center line.
In an alternative embodiment, the injection pump and the exhaust valve are both connected to the upper part of the outer cylinder reactor.
In an alternative embodiment, the air inlet tube is wound from bottom to top in the high temperature zone.
In a second aspect, the present invention provides a control method for a catalyst device for capturing and separating carbon dioxide in flue gas, the control method being applied to the catalyst device for capturing and separating carbon dioxide in flue gas of the foregoing embodiment, the control method including:
utilizing an electric valve to control a condensed water dripping head to drip condensed water, and utilizing an injection pump to inject flue waste gas into the outer cylinder reactor;
controlling the rotation of the rotating chassis by using a motor-driven rotating machine, and adsorbing carbon dioxide in flue waste gas by using condensed water borne on the metal mesh to form solid carbon dioxide hydrate;
controlling an infusion pump to inject catholyte into the bottom of the metal mesh at the position where the height of the solid carbon dioxide hydrate reaches the anode lead;
starting a power supply, enabling direct current to flow out from the positive electrode of the power supply, passing through an anode liquid storage device and flowing into the solid carbon dioxide hydrate in the inner cylinder reactor through an anode lead, and enabling the cathode electrolyte and the solid carbon dioxide hydrate to generate an electrocatalytic reaction under the action of the catalyst powder on the metal mesh to generate an industrial raw material.
The device for capturing, separating and catalyzing carbon dioxide in flue waste gas and the control method thereof provided by the embodiment of the invention have the beneficial effects that:
and rapidly trapping and separating carbon dioxide in flue gas by using a hydrate method. Specifically, flue waste gas is condensed, water vapor in the flue waste gas is collected and recycled, and then the flue waste gas except the water vapor is pressurized to maintain a high-pressure environment in the outer cylinder reactor. The waste heat in the flue waste gas is utilized to maintain the high-temperature area of the outer cylinder reactor in a high-temperature state, and simultaneously, the low-temperature area of the outer cylinder reactor and the rotating chassis are in a low-temperature state. And (3) dripping condensed water condensed and collected from flue waste gas from the top of the outer cylinder reactor to the bottom, wherein the condensed water sequentially passes through the high-temperature zone and the low-temperature zone. In the high temperature zone, the viscosity of the droplets is greatly reduced and the condensed water does not convert to solid hydrates in the high temperature zone. In a low-temperature area, the rotating chassis does high-speed rotation movement, once condensed water touches the metal mesh on the rotating chassis, the condensed water can be diffused into a large number of small droplets under the action of huge centrifugal force, at the moment, carbon dioxide in flue gas has high diffusion rate in the droplets on the metal mesh, the droplets and the carbon dioxide can be quickly converted into carbon dioxide hydrate, the process is continuously carried out, the carbon dioxide hydrate can be continuously formed on the metal mesh, and finally, large blocks of carbon dioxide hydrate with high gas density are formed, so that the efficient trapping and separation of the carbon dioxide in flue waste gas by a hydrate method are realized. And then, converting the separated solid carbon dioxide hydrate into an industrial raw material in situ by adopting an electrocatalysis method, thereby further increasing the commercial additional value of the hydrate method for capturing carbon dioxide in the waste gas of power plants and chemical plants.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings required in the embodiments will be briefly described below, it should be understood that the following drawings only illustrate some embodiments of the present invention and therefore should not be considered as limiting the scope, and those skilled in the art can also obtain other related drawings based on the drawings without inventive efforts.
FIG. 1 is a schematic structural diagram of a catalytic device for capturing and separating carbon dioxide in flue gas according to an embodiment of the present invention;
FIG. 2 is a schematic structural diagram of two devices for capturing, separating and catalyzing carbon dioxide in flue gas, which work in series.
Icon: 100-a carbon dioxide capturing, separating and catalyzing device in flue waste gas; 1, an air inlet pipe; 2-a condensate collector; 3-condensed water dropping head; 4-an exhaust gas reservoir; 5-a syringe pump; 6-an external cylinder reactor; 7-internal barrel reactor; 8-rotating the chassis; 9-an exhaust valve; 10-heat dissipation fins; 11-an electric rotating machine; 12-a linkage shaft; 13-an electrically operated valve; 14-carbon dioxide hydrate; 15-a cathode reservoir; 16-an infusion pump; 17-an injection catheter; 18-a metal mesh; 19-anode lead; 20-an anode reservoir; 21-a power supply; 22-a switch; 23-overflow outlet; 24-a discharge outlet; 25-a heating plate; 26-filling opening.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are some, but not all embodiments of the present invention. The components of embodiments of the present invention generally described and illustrated in the figures herein may be arranged and designed in a wide variety of different configurations.
Thus, the following detailed description of the embodiments of the present invention, presented in the figures, is not intended to limit the scope of the invention, as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be obtained by a person skilled in the art without inventive step based on the embodiments of the present invention, are within the scope of protection of the present invention.
It should be noted that: like reference numbers and letters refer to like items in the following figures, and thus, once an item is defined in one figure, it need not be further defined and explained in subsequent figures.
In the description of the present invention, it should be noted that if the terms "upper", "lower", "inside", "outside", etc. indicate an orientation or a positional relationship based on that shown in the drawings or that the product of the present invention is used as it is, this is only for convenience of description and simplification of the description, and it does not indicate or imply that the device or the element referred to must have a specific orientation, be constructed in a specific orientation, and be operated, and thus should not be construed as limiting the present invention.
Furthermore, the appearances of the terms "first," "second," and the like, if any, are only used to distinguish one description from another and are not to be construed as indicating or implying relative importance.
It should be noted that the features of the embodiments of the present invention may be combined with each other without conflict.
Referring to fig. 1, the embodiment provides a catalytic apparatus 100 for capturing and separating carbon dioxide in flue gas, the catalytic apparatus 100 for capturing and separating carbon dioxide in flue gas includes an air inlet pipe 1, a condensed water collector 2, a condensed water dripping head 3, a waste gas storage 4, an injection pump 5, an outer barrel reactor 6, an inner barrel reactor 7, a rotating chassis 8, an exhaust valve 9, a heat dissipation fin 10, an electric rotating machine 11, a linkage shaft 12, an electric valve 13, a cathode reservoir 15, an infusion pump 16, an injection conduit 17, a metal mesh 18, an anode lead 19, an anode reservoir 20, a power supply 21, and a switch 22. Wherein, the outer cylinder reactor 6 can bear the gas pressure less than or equal to 15MPa, the outer cylinder reactor 6 comprises a high-temperature area and a low-temperature area which are arranged up and down, the height of the outer cylinder reactor 6 can be 250cm, the outer diameter can be 200cm, and the height of the inner cylinder reactor 7 can be 150cm. The metal mesh 18 may be a multi-layered mesh structure. The volume of the exhaust gas storage 4 at normal pressure may be 200L.
The air inlet pipe 1 is used for inputting flue waste gas with carbon dioxide, the air inlet pipe 1 is wound on a high-temperature area of the outer cylinder reactor 6, the distance between the air inlet pipe 1 wound on the outer cylinder reactor 6 can be 5cm, the outer diameter of the air inlet pipe 1 can be 10cm, the ratio of the winding height of the air inlet pipe 1 on the outer cylinder reactor 6 to the height of the outer cylinder reactor 6 is 2, and the flue waste gas in the air inlet pipe 1 can heat the high-temperature area of the outer cylinder reactor 6. Preferably, the air inlet pipe 1 is wound from bottom to top in a high-temperature area, so that the flue waste gas can efficiently heat the high-temperature area of the outer cylinder reactor 6.
The heat radiation fins 10 are disposed outside the low temperature region of the outer tube reactor 6. Specifically, the ratio of the height of the heat dissipation fins 10 to the height of the outer tube reactor 6 is 0.5 to 0.6. And cold air in winter can be used for radiating the low-temperature region of the outer cylinder reactor 6. If the device is applied in summer, the device can be cooled by a method of winding a condensation hose outside the outer cylinder reactor 6, and the condensation hose is externally connected with a constant temperature water tank, so that the manual control cooling of the low-temperature area of the outer cylinder reactor 6 and the rotating chassis 8 can be realized.
The air inlet pipe 1, the condensed water collector 2, the waste gas storage 4, the injection pump 5 and the high-temperature area of the outer cylinder reactor 6 are communicated in sequence, and the exhaust valve 9 is arranged on the outer cylinder reactor 6. The condensed water collector 2 is used for converting water vapor in flue waste gas into condensed water and collecting the condensed water, the waste gas storage 4 is used for storing the flue waste gas after the water vapor is removed, the flue waste gas is injected into the outer cylinder reactor 6 through the injection pump 5, and carbon dioxide is removed in the outer cylinder reactor 6 and then is discharged through the exhaust valve 9. Wherein, the injection pump 5 and the exhaust valve 9 are both connected on the upper part of the outer cylinder reactor 6, so that the flue waste gas entering the outer cylinder reactor 6 is in full contact with the condensed water dripped from the condensed water dripping head 3.
The condensed water dripping head 3 is installed at the bottom of the condensed water collector 2 and inserted into the high temperature zone of the outer cylinder reactor 6. The electric valve 13 is connected to the condensate dripping head 3, and the electric valve 13 is used for controlling the dripping speed of the condensate dripping head 3.
The inner cylinder reactor 7 is arranged in the low-temperature region of the outer cylinder reactor 6, the rotary chassis 8 is rotatably arranged at the bottom of the inner cylinder reactor 7, the metal mesh 18 is arranged on the rotary chassis 8, and the metal mesh 18 carries catalyst powder which can be selected from bismuth trioxide. The condensed water dripped by the condensed water dripping head 3 sequentially passes through a high-temperature region and a low-temperature region and reaches the metal mesh 18 on the rotating chassis 8 to form solid carbon dioxide hydrate. The electric rotating machine 11 is arranged below the outer cylinder reactor 6, and the electric rotating machine 11 is connected to the rotating chassis 8 through a linkage shaft 12 so as to drive the rotating chassis 8 to rotate.
The condensed water collector 2, the condensed water dripping head 3, the outer cylinder reactor 6, the inner cylinder reactor 7 and the rotating chassis 8 are positioned on the same central line.
The cathode reservoir 15 stores catholyte, the anode reservoir 20 stores anolyte, the cathode reservoir 15, the infusion pump 16 and the injection conduit 17 are sequentially communicated, the injection conduit 17 is sequentially inserted into the outer cylinder reactor 6, the inner cylinder reactor 7 and the metal mesh 18 from top to bottom, the metal mesh 18, the power supply 21, the switch 22, the anode reservoir 20 and the anode lead 19 are sequentially connected, and the anode lead 19 is connected to the inner wall of the inner cylinder reactor 7 and is higher than the metal mesh 18. Wherein, a conductive part is arranged in the linkage shaft 12, and the metal mesh 18 is connected to a power supply 21 through the conductive part and a lead. The outer wall of the infusion pump 16 is provided with a heating plate 25 to heat the catholyte flowing through the infusion pump 16.
Wherein the catholyte, the anolyte and the solid carbon dioxide hydrate undergo an electrocatalytic reaction under the action of the catalyst powder on the metal mesh 18 to produce the industrial raw material.
In the embodiment, the industrial raw material generated by the electrocatalytic reaction is formic acid, and the catholyte is 0.5mol/L KHCO 3 The solution and the anolyte are 1mol/L KOH solution. The volume of the cathode reservoir 15 at atmospheric pressure may be 100L and the volume of the anode reservoir 20 at atmospheric pressure may be 50L.
The present embodiment also provides a control method of the above-mentioned device 100 for capturing, separating and catalyzing carbon dioxide in flue gas, the control method including the steps of:
(1) Flue waste gas is connected into the gas inlet pipe 1, so that high-temperature flue waste gas enters the part of the gas inlet pipe 1 surrounded by the outer wall of the outer cylinder reactor 6, and the high-temperature area of the outer cylinder reactor 6 is externally heated.
(2) The heated flue gas enters the condensate collector 2, where the water vapor or liquid moisture in the flue gas is condensed and separated and stored in the condensate collector 2.
(3) And the residual flue waste gas after the water vapor is removed enters a waste gas storage 4 for storage.
(4) And starting the injection pump 5, injecting the flue waste gas in the waste gas storage 4 into the outer cylinder reactor 6, and reaching the required pressure value, wherein the required pressure value can be 8.0MPa.
(5) At this time, the high temperature zone of the outer cylindrical reactor 6 can be continuously maintained in a high temperature state, which may be 60 ℃ or more, by the heating action of the gas inlet pipe 1. On the other hand, the low temperature region of the outer cylinder reactor 6 continuously maintains the low temperature state under the cooling effect of the low temperature airflow in winter and the heat dissipation effect of the heat dissipation fins 10 distributed outside the low temperature region of the outer cylinder reactor 6, wherein the low temperature state can be below-5 ℃.
(6) The electric rotating machine 11 is started to drive the linkage shaft 12 to enable the rotating chassis 8 to be in a high-speed rotating state.
(7) The electric valve 13 is opened to drop the condensed water collected in the condensed water collector 2 onto the metal mesh 18 on the rotating base plate 8.
(8) At this time, the rotating chassis 8 is in a high-speed rotating state, and the whole set of the outer cylinder reactor 6 is in a high-pressure state, so that the heat radiating fins 10 outside the outer cylinder reactor 6 can cool the inner cylinder reactor 7 by virtue of a low-temperature environment in winter, and the rotating chassis 8 is maintained in a low-temperature state.
(9) At this time, the insides of the outer tube reactor 6 and the inner tube reactor 7 are in a high-pressure state, the rotating base plate 8 is in a low-temperature state, and the high-temperature region of the outer tube reactor 6 is in a high-temperature state. When the condensed water drops from the condensed water collector 2 at the top gradually and passes through a high-temperature region of the outer cylinder reactor 6, the internal temperature is higher, the condensed water cannot be converted into hydrate, when the condensed water drops on the metal mesh 18 on the rotating base plate 8, the rotating base plate 8 is in a high-speed rotating state, once the condensed water contacts the metal mesh 18 on the rotating base plate 8, the condensed water can be rapidly diffused to the periphery under the action of huge centrifugal force and is attached to catalyst powder on the surface of the metal mesh 18, the gas-liquid contact area of the dropped condensed water is rapidly enlarged, and the temperature of the condensed water is rapidly reduced under the cooling action of the metal mesh 18 to reach the formation condition of carbon dioxide hydrate 14. Since the process occurs under the high pressure condition of the outer tube reactor 6 and the gas concentration of carbon dioxide in the flue waste in the outer tube reactor 6 is very high, carbon dioxide will rapidly diffuse from the flue waste gas to a large number of droplets formed by expansion, and at this time, the droplets and carbon dioxide will be instantaneously converted into carbon dioxide hydrate 14.
(10) After the metal mesh 18 is gradually filled with the solid carbon dioxide hydrate, the solid carbon dioxide hydrate covers the metal mesh 18, and under the action of the huge centrifugal force generated by the electric rotating machine 11, the solid carbon dioxide hydrate formed later spreads out on the top of the metal mesh 18 to form a new solid carbon dioxide hydrate. At this time, when the condensed water gradually drops down along the injection conduit 17 again, once the liquid drops contact with the new solid carbon dioxide hydrate, the liquid drops rapidly spread under the action of a huge centrifugal force to form a thin water film layer, and further a huge gas-liquid contact area is obtained, which is consistent with the former formation process in the metal mesh 18, and the liquid water drops rapidly convert into the solid carbon dioxide hydrate.
(11) The above process (10) is continued, and the carbon dioxide hydrate 14 is continuously and rapidly formed in the inner cylindrical reactor 7 in a continuous laminated manner.
(12) With the formation of a large amount of solid carbon dioxide hydrate 14, carbon dioxide in flue gas is captured and separated and stored in the solid carbon dioxide hydrate 14, and flue gas containing low-concentration carbon dioxide treated by the hydrate method is discharged to the atmosphere through a safety valve.
(13) The size and the dripping speed of water drops can be adjusted by adjusting the electric valve 13, the thickness of a water film layer spread on the rotating chassis 8 can be adjusted by correspondingly adjusting the rotating speed of the rotating chassis 8, the two parts are adjusted in a matching way, and finally the reaction efficiency of converting liquid water drops into solid carbon dioxide hydrate 14 can be adjusted, so that the hydrate method trapping and separating efficiency of carbon dioxide in flue waste gas can be adjusted. In addition, the high temperature zone of the outer cylinder reactor 6 is in a high temperature state, and the low temperature zone is in a low temperature state, so that strong heat convection can be formed inside the outer cylinder reactor 6, which is beneficial to the heat transfer and diffusion of the water film layer on the rotating chassis 8, and thus the conversion reaction efficiency from liquid water drops to the solid carbon dioxide hydrate 14 can be further improved.
(14) When the solid carbon dioxide in the inner cylinder reactor 7 is hydratedWhen the height of the substance grows to exceed the height of the anode wire 19, the infusion pump 16 and the heating plate 25 are started, and the high-temperature cathode electrolytic solution (formic acid is the electrocatalytic reaction product in the embodiment, 0.5mol/L KHCO is selected as the cathode electrolytic solution) 3 Solution exemplified) is slowly injected through the injection conduit 17 to the bottom of the metal mesh 18. Under the high temperature action of the catholyte, the solid carbon dioxide hydrate filled in the metal mesh 18 is decomposed and releases a large amount of carbon dioxide gas, and the carbon dioxide is rapidly dissolved in the catholyte under the high pressure environment condition of the external cylindrical reactor 6. At this time, the switch 22 is turned on, the power supply 21 is turned on, and the electrocatalytic carbon dioxide activation function is started. Direct current flows out from the positive electrode of the power supply 21, passes through the anode reservoir 20 and flows into the carbon dioxide hydrate in the inner cylinder reactor 7 through the anode lead 19, then is guided into the metal mesh 18 carrying the catalyst powder under the action of liquid water remained in the solid carbon dioxide hydrate to start catalytic reduction of carbon dioxide gas molecules dissolved in the catholyte, and then flows back to the negative electrode of the power supply 21 through the conductive component embedded in the universal driving shaft 12. In addition, since the metal mesh 18 and the bottom of the inner cylindrical reactor 7 and the peripheral structure thereof are provided with the insulator material, the electrocatalytic reaction can be performed only when the height of the solid carbon dioxide hydrate in the inner cylindrical reactor 7 reaches the anode wire 19. Otherwise, the power supply 21 cannot be connected to form a current closed loop, and the electrocatalytic reaction cannot take effect. The catholyte is continuously consumed during the catalytic reaction and fresh catholyte is continuously replenished to the cathode reservoir 15 through the fill port 26.
(15) When the solid carbon dioxide hydrate is continuously formed on the rotating base plate 8, the rotating base plate 8 is always in a high-speed rotating state under the driving action of the electric rotating machine 11, so that the formed solid carbon dioxide hydrate cannot stick to the injection conduit 17, and further the rotating speed of the rotating base plate 8 cannot be influenced. In addition, the formed catalytic product can be thrown out into the outer cylinder reactor 6 through the overflow outlet 23 by means of the high-speed rotation of the rotating base plate 8, so that the subsequent reaction product collection is convenient. Wherein the aperture of the overflow outlet 23 may be 1cm.
(16) After the electrocatalytic reaction is performed for a period of time, the discharge opening 24 of the outer cylinder reactor 6 is opened slowly, and the catalytic product (formic acid in this embodiment) can be discharged from the outer cylinder reactor 6 rapidly under the high-pressure environment condition inside the outer cylinder reactor 6, so as to complete the rapid collection of the reaction product.
In addition, referring to fig. 2 (some parts of the device 100 for capturing, separating and catalyzing carbon dioxide in flue gas are omitted in the figure, only for showing the serial form of two devices), in order to effectively improve the capturing, separating and catalyzing efficiency of carbon dioxide in flue gas as a whole, a plurality of single sets of the devices 100 for capturing, separating and catalyzing carbon dioxide in flue gas can be connected in series to form a continuous working mode capable of processing flue gas in batch.
Specifically, the safety valve of the carbon dioxide capturing, separating and catalyzing device 100 in the first flue gas is communicated with the intake pipe 1 of the carbon dioxide capturing, separating and catalyzing device 100 in the second flue gas, or the safety valve of the carbon dioxide capturing, separating and catalyzing device 100 in the first flue gas can be directly omitted, and the outlet of the outer tube reactor 6 in the first device is directly connected to the intake pipe 1 in the second device.
It is easy to understand that, in this embodiment, the industrial raw material is taken as formic acid, and during the use of the apparatus, formic acid is not limited to be formed by electrocatalysis, and according to different required carbon dioxide electrocatalysis products, a suitable catalyst, a cathode electrolyte and an anode electrolyte are selected and used, and the corresponding industrial raw material is generated by using the electrocatalysis activation function of the apparatus.
The beneficial effects of the device 100 for capturing, separating and catalyzing carbon dioxide in flue gas and the control method thereof provided by the embodiment include:
firstly, inputting flue waste gas discharged by a flue into an air inlet pipe 1, condensing water vapor in the flue waste gas and storing the condensed water in a condensed water collector 2, and then recycling the flue waste gas; then, the waste heat carried in the flue waste gas is recycled and used for heating a high-temperature area of the outer cylinder reactor 6; in addition, the low-temperature air flow in winter is recycled and used for cooling and heating the low-temperature area of the outer cylinder reactor 6 and the rotating chassis 8. The condensed water obtained by condensation drips in the outer cylinder reactor 6 with a certain frequency and size, the water drops vertically and sequentially pass through a high-temperature area and a low-temperature area inside the outer cylinder reactor 6, the viscosity of the water drops in the high-temperature area is low, and the water drops are not easy to be converted into hydrates under the high-temperature condition, so when the water drops touch the metal mesh 18 on the rotating chassis 8, the rotating chassis 8 rotates at a high speed, the water drops can be quickly spread in the pore structure of the metal mesh 18 under the action of huge centrifugal force, a large number of small drops adhered in pores are formed, the contact area between gas and liquid is greatly increased, and carbon dioxide and a water film layer can be instantly converted into carbon dioxide hydrates 14. Then, the liquid drops drop on the solid carbon dioxide hydrate and can be quickly spread to form a thin water film layer with the thickness reaching micron order. The process is carried out under high pressure, after water drops are spread into a thin water film layer, the diffusion rate of gas molecules (mainly carbon dioxide in flue gas) to the water film layer under the high pressure condition is greatly improved, and the carbon dioxide and the water film layer are instantly converted into carbon dioxide hydrate 14. The process is continuously carried out, so that a large block of carbon dioxide hydrate 14 formed in a laminated manner can be obtained, and the efficient capture and separation of carbon dioxide in flue gas by using a hydrate method can be further completed; when the height of the solid carbon dioxide hydrate accumulated at the bottom of the inner cylinder reactor 7 reaches the anode wire 19, the switch 22 can be closed, the power supply 21 is connected, the current is conducted to the metal mesh 18 carrying the catalyst powder through the accumulated large carbon dioxide hydrate and flows back to the power supply 21 in parallel, a complete current closed loop is formed, the formed solid carbon dioxide hydrate 14 is subjected to in-situ electrocatalytic reduction activation, the processes of capturing, separating and activating the carbon dioxide in the flue gas by the hydrate method are finally completed, and the commercial additional value of the process for treating the carbon dioxide in the waste gas by the hydrate method is improved.
The above description is only for the specific embodiments of the present invention, but the scope of the present invention is not limited thereto, and any changes or substitutions that can be easily conceived by those skilled in the art within the technical scope of the present invention are included in the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the claims.
Claims (10)
1. The catalytic device for capturing, separating and catalyzing carbon dioxide in flue waste gas is characterized by comprising an air inlet pipe (1), a condensed water collector (2), a condensed water dripping head (3), a waste gas storage device (4), an injection pump (5), an outer cylinder reactor (6), an inner cylinder reactor (7), a rotating chassis (8), an exhaust valve (9), a cathode liquid storage device (15), an infusion pump (16), an injection conduit (17), a metal net (18), an anode lead (19), an anode liquid storage device (20) and a power supply (21), wherein the outer cylinder reactor (6) comprises a high-temperature area and a low-temperature area which are arranged up and down;
the air inlet pipe (1) is used for inputting flue waste gas with carbon dioxide, the air inlet pipe (1) is wound on the high-temperature area of the outer cylinder reactor (6), the air inlet pipe (1), the condensate water collector (2), the waste gas storage (4), the injection pump (5) and the high-temperature area of the outer cylinder reactor (6) are communicated in sequence, and the exhaust valve (9) is installed on the outer cylinder reactor (6);
the condensed water collector (2) is used for converting water vapor in flue waste gas into condensed water and collecting the condensed water, the waste gas storage (4) is used for storing the flue waste gas after the water vapor is removed, the flue waste gas is injected into the outer cylinder reactor (6) through the injection pump (5), and carbon dioxide is removed in the outer cylinder reactor (6) and then is discharged through the exhaust valve (9);
the condensed water dripping head (3) is arranged at the bottom of the condensed water collector (2) and is inserted into the high-temperature area of the outer cylinder reactor (6);
the inner cylinder reactor (7) is arranged in the low-temperature region of the outer cylinder reactor (6), the rotating chassis (8) is rotatably arranged at the bottom of the inner cylinder reactor (7), the metal net (18) is arranged on the rotating chassis (8), catalyst powder is loaded on the metal net (18), and the condensed water dripped by the condensed water dripping head (3) sequentially passes through the high-temperature region and the low-temperature region and reaches the metal net (18) on the rotating chassis (8) to form solid carbon dioxide hydrate;
the cathode liquid storage device (15) is internally stored with catholyte, the anode liquid storage device (20) is internally stored with anolyte, the cathode liquid storage device (15), the infusion pump (16) and the injection conduit (17) are sequentially communicated, the injection conduit (17) is sequentially inserted into the outer cylinder reactor (6), the inner cylinder reactor (7) and the metal mesh (18) from top to bottom, the metal mesh (18), the power supply (21), the anode liquid storage device (20) and the anode lead (19) are sequentially connected, and the anode lead (19) is connected to the inner wall of the inner cylinder reactor (7) and is higher than the metal mesh (18);
wherein the catholyte, the anolyte and the solid carbon dioxide hydrate undergo an electrocatalytic reaction under the action of the catalyst powder on the metal mesh (18) to produce an industrial raw material.
2. The apparatus for capturing, separating and catalyzing carbon dioxide in flue gas according to claim 1, further comprising heat dissipating fins (10), wherein the heat dissipating fins (10) are disposed outside the low temperature region of the outer tube reactor (6).
3. The device for capturing, separating and catalyzing carbon dioxide in flue gas as recited in claim 1, further comprising an electric rotating machine (11) and a linkage shaft (12), wherein the electric rotating machine (11) is disposed below the outer tube reactor (6), and the electric rotating machine (11) is connected to the rotating chassis (8) through the linkage shaft (12) to drive the rotating chassis (8) to rotate.
4. The apparatus for capturing, separating and catalyzing carbon dioxide in flue-gas according to claim 3, wherein an electrically conductive member is provided inside the linkage shaft (12), and the metal mesh (18) is connected to the power source (21) through the electrically conductive member and a wire.
5. The apparatus for capturing, separating and catalyzing carbon dioxide in flue gas according to claim 3, further comprising an electric valve (13), wherein the electric valve (13) is connected to the condensed water dripping head (3), and wherein the electric valve (13) is configured to control a dripping speed of the condensed water dripping head (3) on the condensed water.
6. The apparatus for trapping and separating carbon dioxide in flue-gas according to claim 1, further comprising a switch (22), wherein the switch (22) is provided between the power source (21) and the anode reservoir (20).
7. The apparatus for capturing, separating and catalyzing carbon dioxide in flue gas according to claim 1, wherein the condensed water collector (2), the condensed water dropping head (3), the outer drum reactor (6), the inner drum reactor (7) and the rotating base plate (8) are located on the same center line.
8. The apparatus for capturing, separating and catalyzing carbon dioxide in flue-gas according to claim 1, wherein the injection pump (5) and the exhaust valve (9) are connected to an upper portion of the outer drum reactor (6).
9. The apparatus for capturing, separating and catalyzing carbon dioxide in flue gas according to claim 1, wherein the intake pipe (1) is wound from bottom to top in the high temperature zone.
10. A control method of a device for capturing, separating and catalyzing carbon dioxide in flue gas, which is applied to the device for capturing, separating and catalyzing carbon dioxide in flue gas according to claim 5, the control method comprising:
controlling the condensed water dripping head (3) to drip the condensed water by using the electric valve (13), and injecting flue waste gas into the outer cylinder reactor (6) by using the injection pump (5);
the electric rotating machine (11) is used for controlling the rotating chassis (8) to rotate, and the condensed water received on the metal net (18) adsorbs carbon dioxide in flue gas to form solid carbon dioxide hydrate (14);
controlling the infusion pump (16) to inject catholyte into the bottom of the metal mesh (18) at the position where the height of the solid carbon dioxide hydrate (14) reaches the anode lead (19);
and starting the power supply (21), enabling direct current to flow out from the positive electrode of the power supply (21), pass through the anode liquid storage device (20) and flow into the solid carbon dioxide hydrate in the inner cylinder reactor (7) through the anode lead (19), and enabling the catholyte and the solid carbon dioxide hydrate to generate an electrocatalytic reaction under the action of the catalyst powder on the metal mesh (18) to generate an industrial raw material.
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| CN116196741B (en) * | 2023-04-27 | 2023-07-25 | 中国科学院西北生态环境资源研究院 | Device and method for forming carbon dioxide hydrate by ball milling method |
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