CN116603380A - Carbon dioxide trapping in-situ utilization method and system based on phase-change solvent - Google Patents
Carbon dioxide trapping in-situ utilization method and system based on phase-change solvent Download PDFInfo
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- CN116603380A CN116603380A CN202310670190.7A CN202310670190A CN116603380A CN 116603380 A CN116603380 A CN 116603380A CN 202310670190 A CN202310670190 A CN 202310670190A CN 116603380 A CN116603380 A CN 116603380A
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 315
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 157
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 157
- 238000000034 method Methods 0.000 title claims abstract description 37
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 25
- 239000002904 solvent Substances 0.000 title claims abstract description 21
- 230000002745 absorbent Effects 0.000 claims abstract description 107
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- 239000003546 flue gas Substances 0.000 claims abstract description 47
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims abstract description 46
- 238000011282 treatment Methods 0.000 claims abstract description 30
- 239000002002 slurry Substances 0.000 claims abstract description 22
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- KRFJLUBVMFXRPN-UHFFFAOYSA-N cuprous oxide Chemical compound [O-2].[Cu+].[Cu+] KRFJLUBVMFXRPN-UHFFFAOYSA-N 0.000 description 2
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- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 description 2
- 229910003437 indium oxide Inorganic materials 0.000 description 2
- PJXISJQVUVHSOJ-UHFFFAOYSA-N indium(iii) oxide Chemical compound [O-2].[O-2].[O-2].[In+3].[In+3] PJXISJQVUVHSOJ-UHFFFAOYSA-N 0.000 description 2
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- 239000012621 metal-organic framework Substances 0.000 description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 2
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- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- OTMSDBZUPAUEDD-UHFFFAOYSA-N Ethane Chemical compound CC OTMSDBZUPAUEDD-UHFFFAOYSA-N 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
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- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical class OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/73—After-treatment of removed components
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/96—Regeneration, reactivation or recycling of reactants
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/80—Organic bases or salts
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
Abstract
The invention belongs to the technical field of carbon capture and utilization, and particularly relates to a carbon dioxide capture in-situ utilization method and a carbon dioxide capture in-situ utilization system based on a phase-change solvent, wherein the method comprises the following steps: after pretreatment of industrial flue gas to be treated, absorbing carbon dioxide in the industrial flue gas by adopting a carbon dioxide absorbent to obtain absorption slurry; performing phase separation treatment on the absorption slurry to obtain CO 2 Rich liquid phase and CO 2 A lean liquid phase; CO is processed by 2 The rich liquid phase is used as a cathode electrolyte for electrocatalytic reduction, and is subjected to electrochemical reduction treatment and then is separated to obtain CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product; CO is processed by 2 Rich liquid regenerated phase and CO 2 Lean liquid phase is re-divided into twoThe carbon oxide absorbent continues to absorb carbon dioxide in the pretreated industrial flue gas. The method solves the problems of high cost of carbon dioxide trapping and regenerating after combustion and low utilization efficiency, and the carbon dioxide is converted into a product with high added value by in-situ utilization after trapping, so that the integration of carbon dioxide trapping and utilization is realized.
Description
Technical Field
The invention relates to the technical field of carbon capture and utilization, in particular to a carbon dioxide capture in-situ utilization method and a carbon dioxide capture in-situ utilization system based on a phase-change solvent.
Background
Carbon dioxide emissions from industrial activities have become a focus of attention worldwide. The harm caused by the large-scale emission of carbon dioxide in industry is widely known, and the harm not only causes great harm to human health, ecological environment and resource utilization, but also brings great challenges to social and economic development and sustainability.
Carbon capture, utilization and sequestration (CCUS) are key technologies for reducing greenhouse gas emissions, achieving carbon neutralization goals in countries around the world, and are also effective solutions to avoid carbon lock-up and large-scale fossil energy capital asset placement.
The method of capturing carbon dioxide can be largely classified into a physical adsorption method, a chemical absorption method, and a membrane separation method. Among the most widely used at present are chemical absorption methods based on the reaction between carbon dioxide and chemical solutions such as carbonates, ammonia, amines, amino acid salts, ionic liquids, phase change absorbers, nanofluids and phenoxides. The typical flow of this process is as follows, the absorption device and the desorption device are operated continuously, and a flue gas stream containing carbon dioxide is introduced at the bottom of the absorption device; introducing an absorbent from the top of the tower to generate countercurrent contact between the flue gas and the absorbent solution and selectively absorb carbon dioxide; the carbon dioxide rich stream is then sent to a regenerator where desorption of carbon dioxide occurs and the carbon dioxide lean regeneration solvent is recycled for further use, and the desorbed carbon dioxide is compressed and sent to storage or utilization. Benefit from chemical solvents and CO 2 The chemical absorption shows a fast carbon dioxide absorption rate and excellent carbon dioxide capturing efficiency, and has high treatment capacity. However, regeneration of the carbon dioxide absorbent is requiredA large amount of energy sources, resulting in an increase in carbon dioxide capture costs.
In order to overcome the technical problems, a new type of carbon dioxide absorbent, namely a phase change solvent, appears in the prior art. The absorbent is characterized in that the absorbent is a single homogeneous solution before absorbing carbon dioxide, and liquid-liquid phase separation occurs along with the increase of load or the change of temperature in the process of absorbing carbon dioxide, wherein the phase of higher load of carbon dioxide is called CO 2 Rich liquid phase, low carbon dioxide load phase is called CO 2 Lean liquid phase.
The carbon dioxide utilization comprises direct utilization and chemical conversion, wherein new energy is utilized in the chemical conversion to generate electricity, the method for electrochemically reducing the carbon dioxide can realize the reaction at normal temperature and normal pressure, and the regulation and control of specific reduction products can be realized by changing a cathode catalyst, an electrolyte and reaction conditions. Electrochemical reduction of carbon dioxide is a method for catalytic reduction of carbon dioxide by using electric energy, and the process generally comprises adsorption of CO on the surface of an electrode 2 Electrochemical reactions occur to produce products such as carbon monoxide or methane, which are then released from the electrode surface and collected. The method has the advantages of high efficiency, cleanliness, strong controllability and the like, but challenges in aspects of catalyst stability, product selectivity, reaction rate and the like still exist at present.
In order to combine carbon dioxide capture and utilization, some carbon capture utilization integration techniques have been proposed. In chinese patent specification CN114000172a, a method for capturing and reducing carbon dioxide and co-producing oxygen or chlorine is disclosed, which uses an absorption solution to convert carbon dioxide into bicarbonate electrolyte and then introduces the bicarbonate electrolyte into a cathode chamber for reduction. However, this method is limited to lower concentration carbon dioxide electrolytes, and carbonate is also easily precipitated in the electrode pores.
Therefore, the invention provides a carbon dioxide capturing in-situ utilization method and a system based on a phase-change solvent.
Disclosure of Invention
In order to solve the defects in the prior art, the invention provides a carbon dioxide capturing in-situ utilization method and a system based on a phase-change solvent.
The invention discloses a carbon dioxide capturing in-situ utilization method and a carbon dioxide capturing in-situ utilization system based on a phase-change solvent, which are realized by the following technical scheme:
the first object of the invention is to provide a method for capturing and in-situ utilizing carbon dioxide based on a phase change solvent, which comprises the following steps:
step 1, after pretreatment of industrial flue gas to be treated, absorbing carbon dioxide in the industrial flue gas by adopting a carbon dioxide absorbent to obtain absorption slurry;
wherein the pretreatment comprises desulfurization, denitrification and dust removal;
step 2, carrying out phase separation treatment on the absorption slurry to obtain CO 2 Rich liquid phase and CO 2 A lean liquid phase;
step 3, the obtained CO 2 The rich liquid phase is used as a cathode electrolyte for electrocatalytic reduction, and is subjected to electrochemical reduction treatment and then is separated to obtain CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product;
step 4, the CO obtained in the step 3 is processed 2 Rich liquid regenerated phase and CO obtained in step 2 2 And (3) returning the lean liquid phase to the step (1) again, and continuously absorbing carbon dioxide in the pretreated industrial flue gas as a carbon dioxide absorbent.
Further, the carbon dioxide absorbent is a liquid absorbent which is subjected to liquid-liquid phase separation after absorbing carbon dioxide and is enriched in one phase of the carbon dioxide;
and the carbon dioxide absorption capacity of the carbon dioxide absorbent is more than or equal to 0.1mol CO 2 An absorption load of 0.1 mol/L CO/L absorbent 2 /mol。
Further, the carbon dioxide absorbent is one or more of a main absorbent, a secondary absorbent and a phase separation promoter;
wherein the main absorbent is a mixture of one or more of primary amine, secondary amine, amino acid salt and ionic liquid in any proportion;
the auxiliary absorbent is a mixture of one or more of amines, amino acid salts, ionic liquid, alcohols, sulfones, piperazines, ethers and imidazoles in any proportion;
the phase separation promoter is one or more of tertiary amine with low carbon dioxide absorption rate, sterically hindered amine and water mixed in any proportion.
Further, in order to facilitate the electrocatalytic reduction of carbon dioxide, the carbon dioxide absorbent further comprises an ionic additive, wherein the addition amount of the ionic additive and the total amount of the carbon dioxide absorbent is 0.05-2 mol:1L;
and the ion additive is a mixture of one or more of potassium ions, sodium ions, lithium ions, rubidium ions and cesium ions mixed in any proportion.
A second object of the present invention is to provide a carbon dioxide capturing and in-situ utilizing system based on the above method, which is characterized by comprising:
the pretreatment device is used for pretreating the industrial flue gas to be treated;
the absorption device is provided with a reaction chamber, the input end of the reaction chamber is communicated with the output end of the pretreatment device, and the reaction chamber is used for receiving the pretreated industrial flue gas output by the pretreatment device;
an absorbent supply device, the output end of which is communicated with the input end of the reaction chamber and is used for providing carbon dioxide absorbent for the reaction chamber so as to form absorption slurry with carbon dioxide in the pretreated industrial flue gas in the reaction chamber;
the input end of the phase separation device is communicated with the output end of the reaction chamber and is used for separating the absorption slurry output by the absorption device; and the phase separation devices are respectively provided with CO 2 Rich liquid phase output port and CO 2 A lean liquid phase output port;
electrocatalytic reduction reactor, the input end of the cathode electrolytic cell of which is connected with the CO 2 A rich liquid phase outlet connected to receive the gas produced by the CO 2 CO output from the rich liquid phase output port 2 Rich liquid phase and will receive CO 2 The rich liquid phase is used as a catholyte for electrochemical reduction treatment;
the input end of the separating device is communicated with the output end of the cathode electrolytic cell and is used for receiving CO after electrochemical reduction treatment 2 Rich liquid phase and the received CO after electrochemical reduction treatment 2 Separating the rich liquid phase; and the output ends of the separation devices are respectively provided with CO 2 A rich liquid regeneration phase output port and a carbon dioxide reduction product output port;
a power transmission device for transmitting the CO 2 CO output from lean liquid phase output port 2 Lean liquid phase and CO produced therefrom 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbent supply.
Further, the power transmission device comprises a power transmission pipeline F and a power transmission pipeline G;
the power transmission pipeline F is respectively connected with the CO 2 A lean liquid phase outlet, an input of the absorbent supply means being in communication to be fed by the CO 2 CO output from lean liquid phase output port 2 Returning a lean liquid phase to the absorbent supply;
the power transmission pipeline G is respectively connected with the CO 2 The rich liquid regeneration phase output port is communicated with the input end of the absorbent supply device so as to be formed by the CO 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbent supply means for resupply by the absorbent supply means into the reaction chamber of the absorbent means.
Further, the pretreatment device comprises a desulfurization mechanism, a denitration mechanism and a dust removal mechanism which are sequentially connected in series.
Further, the phase separation device comprises one or more phase separators;
wherein when a plurality of phase separators are used, the plurality of phase separators are connected in series and/or in parallel.
Further, the phase separator is a separator of one or more components of gravity type, centrifugal type and filtering type.
Further, the electrocatalytic reduction reactor adopts any one of a H-type electrolytic cell, a flow electrolytic cell, a membrane electrode electrolytic cell and a stack type electrolytic cell of a two-electrode or three-electrode system.
Further, a pump body A is arranged between the input end of the absorption device and the output end of the pretreatment device, and the post-flue gas treated by the pretreatment device is pumped into the absorption device through the pump body A.
Further, a pump body B is arranged between the output end of the absorption device and the input end of the phase separation device, and the carbon dioxide absorbent absorbing carbon dioxide smoke is pumped into the phase separation device through the pump body B.
Compared with the prior art, the invention has the following beneficial effects:
the invention provides a carbon dioxide capturing and in-situ utilizing system based on a phase-change solvent, which solves the problems of high cost of capturing, regenerating and transporting carbon dioxide after combustion and low utilization efficiency, and realizes the integration of capturing and utilizing carbon dioxide by converting the captured carbon dioxide into high-added-value products in situ.
Capturing carbon dioxide by a phase change absorbent and replacing CO by electrocatalytic reduction of carbon dioxide 2 The rich liquid phase regeneration unit is used for solving the problem of consumption of a large amount of heat energy in the regeneration process; phase separated CO relative to commercial amine-based carbon dioxide capture electrocatalytic integration 2 Catholyte for electrocatalytic reduction of rich solution, higher CO 2 The concentration is favorable for inhibiting hydrogen evolution reaction and simultaneously completing CO 2 Regenerating the rich liquid phase; in addition, the compression of carbon dioxide is avoided, the volume of electrolyte for power transmission is reduced, and the energy consumption is effectively saved.
Drawings
FIG. 1 is a workflow diagram of a carbon dioxide capture in-situ utilization system based on a phase change solvent of the present invention;
FIG. 2 is an overall schematic of the carbon dioxide capture in-situ utilization system based on phase change solvents of example 2;
FIG. 3 is a schematic view of the phase separator in example 3;
FIG. 4 is a schematic diagram of the electrocatalytic reduction reactor of example 4.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below.
The invention provides a carbon dioxide capturing and in-situ utilizing method based on a phase-change solvent, which comprises the following steps:
step 1, after pretreatment of industrial flue gas to be treated, absorbing carbon dioxide in the industrial flue gas by adopting a carbon dioxide absorbent to obtain absorption slurry;
in order to further improve the capturing effect of the subsequent treatment on the carbon dioxide in the process flue gas, the carbon dioxide in the process flue gas needs to be pretreated before being captured, and the pretreatment comprises desulfurization, denitration and dust removal so as to remove impurities and harmful substances in the flue gas, so that the damage of the flue gas to the subsequent treatment device can be avoided, the purity of the carbon dioxide in the flue gas can be improved, and the subsequent capturing and further utilization of the carbon dioxide in the flue gas can be facilitated.
Wherein, the specific pretreatment is carried out according to the common treatment method in the field.
In the invention, the carbon dioxide absorbent is a liquid absorbent which is separated in liquid-liquid phase after absorbing carbon dioxide and is enriched in one phase of the carbon dioxide, and in order to ensure the capturing effect of the carbon dioxide absorbent on the carbon dioxide, the carbon dioxide absorbent preferably has the carbon dioxide absorption capacity of more than or equal to 0.1mol CO 2 An absorption load of 0.1 mol/L CO/L absorbent 2 /mol to ensure that the expressed carbon dioxide concentration reaches the minimum concentration at which the system can operate.
In order to further improve the capturing effect of the carbon dioxide absorbent adopted by the invention on carbon dioxide, the carbon dioxide absorbent adopted by the invention is one or more of a main absorbent, a secondary absorbent and a phase separation promoter; the main absorbent is a mixture of two or more of primary amine, secondary amine, amino acid salt and ionic liquid with high carbon dioxide absorption rate in any proportion. And the temperature of the carbon dioxide absorbent absorbing carbon dioxide is 40-60 ℃.
The auxiliary absorbent is a mixture of two or more of amines, amino acid salts, ionic liquid, alcohols, sulfones, piperazines, ethers and imidazoles in any proportion.
The phase separation promoter is a mixture of two or more of tertiary amine, sterically hindered amine and water with low carbon dioxide absorption rate.
In order to facilitate the electrocatalytic reduction of carbon dioxide, the absorption liquid also comprises an ion additive, wherein the ion additive is one or a mixture of a plurality of potassium ions, sodium ions, lithium ions, rubidium ions and cesium ions in any proportion. The total addition amount of the ionic additive and the carbon dioxide absorbent is 0.05-2 mol:1L;
step 2, carrying out phase separation treatment on the absorption slurry to obtain CO 2 Rich liquid phase and CO 2 A lean liquid phase;
it should be noted that, since the carbon dioxide absorbent absorbs carbon dioxide and then undergoes liquid-liquid phase separation, and the carbon dioxide is concentrated in one phase, the phase separation herein refers to liquid-liquid phase separation of the absorption slurry, wherein the carbon dioxide concentrated one phase, i.e., the liquid phase with high carbon dioxide content is CO 2 A rich liquid phase, the other liquid phase is CO with less carbon dioxide content 2 Lean liquid phase, thus obtained CO 2 The rich liquid phase realizes the capture of carbon dioxide, and is further beneficial to the utilization of the captured carbon dioxide.
Step 3, the obtained CO 2 The rich liquid phase is used as a cathode electrolyte for electrocatalytic reduction, and is subjected to electrochemical reduction treatment and then is separated to obtain CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product;
in order to achieve the efficiency and effect of recycling captured carbon dioxide, the present invention preferably uses CO obtained 2 The rich liquid phase is used as a catholyte for electrocatalytic reduction, and carbon dioxide electrocatalytic reduction is adopted to replace CO 2 Rich liquid phase regeneration unitThe method avoids the consumption of a large amount of heat energy in the regeneration process of the trapped carbon dioxide in the prior art, solves the problems of high cost of carbon dioxide trapping regeneration and transportation and low utilization efficiency after combustion, directly utilizes the carbon dioxide after absorbing the carbon dioxide by the phase change absorbent, and realizes the integration of carbon dioxide trapping and utilization. And with respect to commercial amine-based carbon dioxide capture electrocatalytic integration, CO after phase separation 2 Catholyte for electrocatalytic reduction of rich liquid phase, higher CO 2 The concentration is favorable for inhibiting hydrogen evolution reaction and simultaneously completing CO 2 Regeneration of the liquid rich phase to obtain CO 2 A rich liquid regenerated phase; in addition, the compression of carbon dioxide is avoided, the volume of electrolyte for power transmission is reduced, and the energy consumption is effectively saved.
Wherein the CO to be obtained 2 The rich liquid phase is used as a cathode electrolyte for electrocatalytic reduction to electrochemically reduce carbon dioxide to produce hydrocarbons or alcohols such as carbon monoxide, methane, methanol, ethane, ethylene, acetylene, ethanol and the like.
Step 4, the CO obtained in the step 3 is processed 2 Rich liquid regenerated phase and CO obtained in step 2 2 Returning the lean liquid phase to the step 1 again, and continuously absorbing carbon dioxide in the pretreated industrial flue gas as a carbon dioxide absorbent;
in order to improve the treatment efficiency and realize the full utilization of resources, the invention uses CO 2 Rich liquid regenerated phase and CO 2 The lean liquid phase returns to the step 1 again and is used as a carbon dioxide absorbent to continuously absorb carbon dioxide in the pretreated industrial flue gas so as to supplement the phase change absorbent consumed in the step 1, thereby improving the recycling of the phase change absorbent, ensuring the forward progress of capturing and utilizing the carbon dioxide and improving the efficiency of treating the carbon dioxide in the flue gas.
The invention also provides a carbon dioxide capturing and in-situ utilizing system based on the phase-change solvent, which comprises a pretreatment device 1, an absorption device 2, an absorbent supply device 3, a phase separation device 4, an electrocatalytic reduction reactor 5, a separation device 6 and a power transmission device.
It should be noted that, the pretreatment device 1 of the present invention is used for pretreating industrial flue gas to be treated to implement treatments such as desulfurization, denitration, and impurity removal of the industrial flue gas to be treated, so that the pretreatment device 1 of the present invention at least includes a desulfurization mechanism, a denitration mechanism, and a dust removal mechanism, where the desulfurization mechanism, the denitration mechanism, and the dust removal mechanism are not limited in order, and can be adjusted according to specific characteristics of different industrial flue gases (such as industrial flue gas generated by coal-fired power plants, biomass power plants, steel plants, petrochemical plants, cement plants, coal chemical industry, etc.). For example, in order to maximally realize pretreatment of industrial flue gas, the invention preferably adopts a coal-fired boiler, cooling energy-saving equipment, a ceramic multi-tube cyclone dust collector, a pulse bag dust collector, an induced draft fan, a denitration tower and a desulfurization and denitration neutralization tower to carry out pretreatment in sequence. The coal-fired boiler, the cooling and energy-saving equipment, the ceramic multi-tube cyclone dust collector, the pulse bag dust collector, the induced draft fan, the denitration tower and the desulfurization and denitration neutralization tower are all in the prior art, and the structure and the working principle of the boiler are known to those skilled in the art, so that the invention is not repeated here.
The absorption device 2 of the invention is provided with a reaction chamber, the input end of the reaction chamber is respectively communicated with the output end of the pretreatment device 1 and the output end of the absorbent supply device 3 through the power transmission pipeline A7 and the power transmission pipeline B8, so that the reaction chamber can receive the pretreated industrial flue gas and the phase change absorbent output by the pretreatment device 1, and the pretreated industrial flue gas and the phase change absorbent react in the reaction chamber to form absorption slurry, thereby realizing the capture of carbon dioxide in the industrial flue gas. Wherein, in order to be convenient for carry the industrial flue gas after the preliminary treatment and phase change absorbent to the reaction chamber, still be provided with pump body A9 and pump body B10 on power delivery pipeline A7 and the power delivery pipeline B8 respectively to be convenient for pump into the reaction chamber with the back flue gas of preprocessing device 1 processing through pump body A9, and be convenient for pump into the reaction chamber with the phase change absorbent in the absorbent feeding device 3 through pump body B10.
The absorption device 2 of the present invention may be a spray tower or a packed tower; the system can also be composed of a plurality of towers which are connected in series, in parallel or in series-parallel.
The input end of the phase separation device 4 is communicated with the output end of the reaction chamber through a power transmission pipeline C11 and is used for carrying out phase separation on the absorption slurry output by the absorption device 2; and the output ends of the phase separation device 4 are respectively provided with CO 2 Rich liquid phase output port and CO 2 And a lean liquid phase output port. In order to facilitate the input of the absorption slurry obtained by the reaction in the reaction chamber into the phase separation device 4, the invention is also provided with a pump body C12 on the power transmission pipeline C11 so as to facilitate the pumping of the absorption slurry into the phase separation device 4 through the pump body C12 for phase separation treatment. The invention is not limited to the particular type or kind of phase separator employed, such as a separator in the form of a combination of any one or more of vertical, horizontal, tubular and spherical. The phase separator is not limited in terms of the mechanism by which the separation is achieved, and may be selected from any one of gravity type, centrifugal type, and filtration type, for example. The number of the phase separators is not limited, one or more phase separators may be used, and when a plurality of phase separators are used, any one or two combinations of series connection and parallel connection may be used between the plurality of phase separators.
Wherein, after the absorbent phase separation, CO 2 Lean liquid phase and CO 2 The rich liquid phase flows out from the outlet respectively, and the CO is different according to the absorbent 2 Lean liquid phase and CO 2 The relative positions of the rich liquid phases can be changed.
The input end of the cathode electrolytic cell of the electrocatalytic reduction reactor 5 and the CO 2 A rich liquid phase outlet connected to receive the gas produced by the CO 2 CO output from the rich liquid phase output port 2 And (3) carrying out electrochemical reduction treatment on the liquid rich phase serving as a catholyte. And the output end of the cathode electrolytic cell is communicated with the input end of the separation device 6 to receive the CO subjected to electrochemical reduction treatment through the separation device 6 2 The rich liquid phase is separated and treated to obtain regenerated CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product; and the output ends are respectively provided with CO 2 Rich liquid regenerated phase output port, and carbon dioxide reduction product output port.
Wherein the CO of the invention 2 The liquid-rich phase undergoes electrochemical reduction of CO at the cathode of the electrocatalytic reduction reactor 5 one or more times 2 The rich liquid phase undergoes electrochemical reduction at the cathode of the electrocatalytic system one or more times. And the electrolytic cell of the electrocatalytic reduction reactor 5 may be selected from any one of a two-electrode or three-electrode system H-type electrolytic cell, a flow electrolytic cell, a membrane electrode electrolytic cell and a stack-type electrolytic cell.
The material of the electrolytic cell of the electrocatalytic reduction reactor 5 can be selected from metal materials or polymer materials, wherein the metal is platinum or other alloy materials, and the polymer materials are polytetrafluoroethylene.
The cell flow channels of the electrocatalytic reduction reactor 5 may be selected from any one of single channel serpentine, straight channel parallel, multi-channel serpentine, mixed serpentine and interdigitated.
The exchange membrane of the electrocatalytic reduction reactor 5 may be selected from any one of proton exchange membrane, cation exchange membrane, anion exchange membrane and bipolar membrane.
And the anode of the electrocatalytic reduction reactor 5 is any one of typical anodic oxidation synthesis reactions such as oxygen evolution reaction, chlor-alkali process, alcohol and nitrogenous organic matter oxidation and the like.
The cathode electrode of the electrocatalytic reduction reactor 5 is made of smooth or foam metal or metal alloy thereof; wherein the metal is one or more of copper, zinc, lead, mercury, cadmium, titanium, indium, tin, silver, gold and bismuth.
The catalyst adopted by the electrocatalytic reduction reactor 5 is any one of a metal oxide catalyst, a molecular catalyst and a heterogeneous catalyst; wherein the metal oxide catalyst is any one of cuprous oxide, tin oxide, indium oxide and titanium dioxide; the molecular catalyst is a molecular catalyst containing any one or more metal centers of iron, cobalt and nickel; the heterogeneous catalyst is any one or more of graphene, carbon nano tubes and metal organic frameworks.
The separation device 6 is a gas-liquid separation device or a liquid-liquid separation device, and the number of the gas-liquid separation device or the liquid-liquid separation device is one or more.
The power transmission device of the present invention includes a power transmission pipe F16 and a power transmission pipe G17; wherein the power transmission pipeline F16 is respectively connected with the CO 2 A lean liquid phase outlet, an input of the absorbent supply 3, to be fed by the CO 2 CO output from lean liquid phase output port 2 The lean liquid phase is returned to the absorbent feed 3. The power transmission pipeline G17 is respectively connected with the CO 2 The rich liquid regeneration phase output port is communicated with the input end of the absorption device 2 so as to be formed by the CO 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbent supply means 3 for resupply by the absorbent supply means into the reaction chamber of the absorbent means.
Example 1
Referring to fig. 2, the present embodiment provides a carbon dioxide capturing and in-situ utilizing system based on a phase-change solvent, which comprises a pretreatment device 1, an absorption device 2, an absorbent supply device 3, a phase separation device 4, an electrocatalytic reduction reactor 5, a separation device 6 and a power transmission device; wherein the power transmission device comprises a plurality of power transmission pipelines.
The pretreatment device 1 is used for pretreatment of industrial flue gas to be treated so as to realize treatments of desulfurization, denitration, impurity removal and the like of the industrial flue gas to be treated, so that the pretreatment device 1 sequentially adopts a coal-fired boiler, cooling energy-saving equipment, a ceramic multi-tube cyclone dust collector, a pulse cloth bag dust collector, an induced draft fan, a denitration tower and a desulfurization and denitration neutralization tower for pretreatment. The coal-fired boiler, the cooling and energy-saving equipment, the ceramic multi-tube cyclone dust collector, the pulse bag dust collector, the induced draft fan, the denitration tower and the desulfurization and denitration neutralization tower are all in the prior art, and the structure and the working principle of the boiler are known to those skilled in the art, so that the invention is not repeated here.
The absorption device 2 of the invention is provided with a reaction chamber, the input end of the reaction chamber is respectively communicated with the output end of the pretreatment device 1 and the output end of the absorbent supply device 3 through the power transmission pipeline A7 and the power transmission pipeline B8, so that the reaction chamber can receive the pretreated industrial flue gas and the phase change absorbent output by the pretreatment device 1, and the pretreated industrial flue gas and the phase change absorbent react in the reaction chamber to form absorption slurry, thereby realizing the capture of carbon dioxide in the industrial flue gas. Wherein, in order to be convenient for carry the industrial flue gas after the preliminary treatment and phase change absorbent to the reaction chamber, still be provided with pump body A9 and pump body B10 on power delivery pipeline A7 and the power delivery pipeline B8 respectively to be convenient for pump into the reaction chamber with the back flue gas of preprocessing device 1 processing through pump body A9, and be convenient for pump into the reaction chamber with the phase change absorbent in the absorbent feeding device 3 through pump body B10.
The input end of the phase separation device 4 of the embodiment is communicated with the output end of the reaction chamber through a power transmission pipeline C11 and is used for carrying out phase separation on the absorption slurry output by the absorption device 2; and the output ends of the phase separation device 4 are respectively provided with CO 2 Rich liquid phase output port and CO 2 And a lean liquid phase output port. In order to facilitate the input of the absorption slurry obtained by the reaction in the reaction chamber into the phase separation device 4, the invention is also provided with a pump body C12 on the power transmission pipeline C11 so as to facilitate the pumping of the absorption slurry into the phase separation device 4 through the pump body C12 for phase separation treatment.
And the phase separation device 4 of the present embodiment includes a primary phase separator 41 and a secondary phase separator 42.
Wherein the primary phase separator 41 is divided into CO 2 Lean liquid separation zone A411 and CO 2 Rich liquid separation zone A412, CO 2 The outlet of the lean liquid separation area A411 is connected with a feed inlet at the top of the absorption device 2 through a lean liquid pump 43; CO 2 The outlet of the rich liquid separation area A412 is connected with the feed inlet of the secondary phase separator 42, and is further used for separating the phase change absorbent.
Wherein the secondary phase separator 42 is divided into CO 2 Lean liquid separation zone B421 and CO 2 Rich liquid separation zone B422, CO 2 The outlet of the lean liquid separation zone B421 is communicated with the input end of the absorbent supply device 3 through a power transmission pipeline F16, and a lean liquid pump 43 is arranged on the power transmission pipeline F16 so as to feed CO through the lean liquid pump 43 2 Lean liquid separationCO obtained by separation in zone A411 2 The lean liquid phase is returned to the absorbent feed 3. And CO 2 The outlet of the rich liquid separation zone B422 is connected with the input end of the cathode electrolytic cell of the electrocatalytic reduction reactor 5 through a power transmission pipeline D13. And an electrolyte pump 14 is provided on the power transmission pipe D13 to separate the CO obtained by the phase separation device 4 by the electrolyte pump 14 2 The liquid rich phase is sent to the catholyte tank of the electrocatalytic reduction reactor 5 to separate the CO obtained by the phase separation device 4 2 And the rich liquid phase is used as a catholyte for electrochemical reduction treatment. And the output end of the cathode electrolytic cell is communicated with the input end of the separation device 6 through a power transmission pipeline E15 to receive CO subjected to electrochemical reduction treatment through the separation device 6 2 Rich in liquid phase and for CO after electrochemical reduction treatment 2 Separating the rich liquid phase to obtain regenerated CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product; and the output ends of the separating devices 6 are respectively provided with CO 2 Rich liquid regenerated phase output port, and carbon dioxide reduction product output port.
The electrocatalytic reduction reactor 5 of this embodiment adopts a membrane electrode electrolytic cell, which includes a cathode chamber 51, a cathode electrode 52, an exchange membrane 53, an anode electrode 54, and an anode chamber 55. The outlet of the cathode chamber 51 is connected to the inlet of the reduction product separation device.
The separation device 6 in this embodiment is a gas-liquid separation device or a liquid-liquid separation device, and the number of the gas-liquid separation device or the liquid-liquid separation device is one or more.
The power transmission device of the invention also comprises a power transmission pipeline F16 and a power transmission pipeline G17, wherein the power transmission pipeline F16 is respectively connected with the CO 2 A lean liquid phase outlet, an input of the absorbent supply 3, to be fed by the CO 2 CO output from lean liquid phase output port 2 The lean liquid phase is returned to the absorbent feed 3. The power transmission pipeline G17 is respectively connected with the CO 2 The rich liquid regeneration phase output port is communicated with the input end of the absorbent supply device 3 so as to be formed by the CO 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbentIn the supply device 3, the phase-change absorbent in the absorbent supply device 3 is pumped into the reaction chamber again through the pump body B10.
Example 2
The present embodiment provides a carbon dioxide capturing and in-situ utilizing system based on a phase-change solvent, and based on the embodiment 1, in the phase separator of the present embodiment, a parallel connection mode is adopted for the primary phase separator 413 and the secondary phase separator 425 as illustrated in fig. 2.
Wherein the absorbent outlet on the other side of the bottom of the absorption device 2 is connected with the feed inlets of the primary phase separator 41 and the secondary phase separator 42.
Wherein the CO of the primary phase separator 41 2 The lean liquid separation zone outlet is communicated with the input end of the absorbent supply device 3 through a power transmission pipeline F16, and the power transmission pipeline F16 is provided with a lean liquid pump 43 for feeding CO through the lean liquid pump 43 2 The CO obtained by separation in the lean liquid separation zone A411 2 The lean liquid phase is returned to the absorbent supply 3. And CO 2 The outlet of the rich liquid separation zone a412 communicates with the input of the secondary phase separator 42 to continue the phase separation process through the secondary phase separator 42.
Wherein the CO of the secondary phase separator 42 2 The outlet of the lean liquid separation zone B421 is also in communication with the lean liquid pump 43 to pass the CO of the secondary phase separator 42 through the lean liquid pump 43 2 CO separated and obtained in lean liquid separation zone B421 2 The lean liquid phase is also returned to the absorbent supply 3. CO 2 The outlet of the rich liquid separation zone B422 is connected with the feed inlet of the cathode chamber of the carbon dioxide electrolytic cell through the electrolyte pump 14. Thereby, a two-phase separation of the phase change absorbent is achieved.
Example 3
The present embodiment provides a carbon dioxide capturing and in-situ utilizing system based on a phase-change solvent, and in the present embodiment, based on the embodiment 1, a primary phase separator 413 and a secondary phase separator 425 as described in fig. 3 are connected in series in the phase separation device 4.
Example 4
The present embodiment provides a carbon dioxide capturing and in-situ utilizing system based on a phase-change solvent, and referring to fig. 4, in this embodiment, based on embodiment 1, a flow electrolytic cell is adopted in the electrocatalytic reduction reactor 5, and the flow electrolytic cell comprises a cathode chamber, a cathode electrode, an exchange membrane, an anode electrode and an anode chamber.
The material of the flowing electrolytic cell can be selected according to actual conditions, and the cathode electrode can be one or more of various metals such as plain or foam copper, zinc, lead, mercury, cadmium, titanium, indium, tin, silver, gold, bismuth and the like or metal alloys thereof; metal oxide catalysts such as cuprous oxide, tin oxide, indium oxide, and titanium oxide; molecular catalysts comprising metal centers such as iron, cobalt or nickel; heterogeneous catalysts of graphene and carbon nanotubes, metal Organic Frameworks (MOFs). The exchange membrane may be a membrane made of polymer materials such as proton exchange membrane, cation exchange membrane, anion exchange membrane, bipolar membrane, etc. The anode electrode can be a platinum electrode, a carbon rod electrode, a foam nickel electrode and the like which are commonly used in oxygen evolution reaction.
Wherein the anode of the carbon dioxide cell in one or more embodiments may be a typical anodic oxidation synthesis reaction of chlor-alkali processes, oxidation of alcohols and nitrogen-containing organics, and the like. The anode electrode may be an electrode commonly used for the corresponding application.
It should be apparent that the embodiments described above are only some, but not all, embodiments of the invention. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
Claims (10)
1. The method for capturing and in-situ utilizing carbon dioxide based on the phase-change solvent is characterized by comprising the following steps of:
step 1, after pretreatment of industrial flue gas to be treated, absorbing carbon dioxide in the industrial flue gas by adopting a carbon dioxide absorbent to obtain absorption slurry;
wherein the pretreatment comprises desulfurization, denitrification and dust removal;
step 2, carrying out phase separation treatment on the absorption slurry to obtain CO 2 Rich liquid phase and CO 2 A lean liquid phase;
step 3, the obtained CO 2 The rich liquid phase is used as a cathode electrolyte for electrocatalytic reduction, and is subjected to electrochemical reduction treatment and then is separated to obtain CO 2 A rich liquid regenerated phase and a carbon dioxide reduction product;
step 4, the CO obtained in the step 3 is processed 2 Rich liquid regenerated phase and CO obtained in step 2 2 And (3) returning the lean liquid phase to the step (1) again, and continuously absorbing carbon dioxide in the pretreated industrial flue gas as a carbon dioxide absorbent.
2. The method of claim 1, wherein the carbon dioxide absorbent is a liquid absorbent that undergoes liquid-liquid phase separation after absorbing carbon dioxide and wherein carbon dioxide is enriched in one of the phases;
the carbon dioxide absorption capacity of the carbon dioxide absorbent is more than or equal to 0.1mol CO 2 An absorption load of 0.1 mol/L CO/L absorbent 2 /mol。
3. The method of claim 1, wherein the carbon dioxide absorbent is one or more of a primary absorbent, a secondary absorbent, and a phase separation promoter;
wherein the main absorbent is a mixture of one or more of primary amine, secondary amine, amino acid salt and ionic liquid in any proportion;
the auxiliary absorbent is a mixture of one or more of amines, amino acid salts, ionic liquid, alcohols, sulfones, piperazines, ethers and imidazoles in any proportion;
the phase separation promoter is one or more of tertiary amine with low carbon dioxide absorption rate, sterically hindered amine and water mixed in any proportion.
4. The method of claim 1, wherein the carbon dioxide absorbent further comprises an ionic additive in an amount of 0.05 to 2mol:1l relative to the total amount of carbon dioxide absorbent;
and the ion additive is a mixture of one or more of potassium ions, sodium ions, lithium ions, rubidium ions and cesium ions mixed in any proportion.
5. A carbon dioxide capture and in-situ utilization system based on the method of any one of claims 1-4, comprising:
the pretreatment device (1) is used for pretreating the industrial flue gas to be treated;
the absorption device (2) is provided with a reaction chamber, the input end of the reaction chamber is communicated with the output end of the pretreatment device (1), and the reaction chamber is used for receiving the pretreated industrial flue gas output by the pretreatment device (1);
an absorbent supply device (3) with an output end communicated with the input end of the reaction chamber, and used for providing carbon dioxide absorbent to the reaction chamber so as to form absorption slurry with carbon dioxide in the pretreated industrial flue gas in the reaction chamber;
a phase separation device (4) with an input end communicated with the output end of the reaction chamber for phase-separating the absorption slurry output by the absorption device (2); and the phase separation devices (4) are respectively provided with CO 2 Rich liquid phase output port and CO 2 A lean liquid phase output port;
an electrocatalytic reduction reactor (5), the input of which is connected to the CO 2 A rich liquid phase outlet connected to receive the gas produced by the CO 2 CO output from the rich liquid phase output port 2 Rich liquid phase and will receive CO 2 The rich liquid phase is used as a catholyte for electrochemical reduction treatment;
a separating device (6) with an input end communicated with the output end of the cathode electrolytic cell and used for receiving CO after electrochemical reduction treatment 2 Rich liquid phase and the received CO after electrochemical reduction treatment 2 Separating the rich liquid phase; and the output ends of the separation device (6) are respectively provided with CO 2 A rich liquid regeneration phase output port and a carbon dioxide reduction product output port;
the power transmission device comprises a power transmission device,for to be used by the CO 2 CO output from lean liquid phase output port 2 Lean liquid phase and CO produced therefrom 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbent supply device (3).
6. The system of claim 5, wherein the power transmission means comprises a power transmission conduit F (16) and a power transmission conduit G (17);
the power transmission pipeline F (16) is respectively connected with the CO 2 A lean liquid phase outlet, an input of the absorbent supply means (3) to be fed by the CO 2 CO output from lean liquid phase output port 2 -returning a lean liquid phase to the absorbent feed means (3);
the power transmission pipeline G (17) is respectively connected with the CO 2 The rich liquid regeneration phase output port is communicated with the input end of the absorbent supply device (3) so as to be formed by the CO 2 CO output from rich liquid regenerated phase output port 2 The rich liquid regenerated phase is returned to the absorbent supply device (3).
7. The system according to claim 5, characterized in that the phase separation device (4) comprises one or more phase separators;
wherein when a plurality of phase separators are used, the plurality of phase separators are connected in series and/or in parallel.
8. The system according to claim 5, wherein the electrocatalytic reduction reactor (5) employs any one of a two-electrode or three-electrode system of H-type cells, flow cells, membrane electrode cells and stack-type cells.
9. The system according to claim 5, characterized in that a pump body a (9) is further arranged between the input end of the reaction chamber and the output end of the pretreatment device (1), and the post-flue gas treated by the pretreatment device (1) is pumped into the reaction chamber through the pump body a (9).
10. The system according to claim 5, characterized in that a pump body C (12) is further arranged between the output of the reaction chamber and the input of the phase separation device (4), through which pump body C (12) absorbent slurry is pumped into the phase separation device (4).
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