CN114870570A - Liquid-solid phase separation absorbent for carbon dioxide separation - Google Patents
Liquid-solid phase separation absorbent for carbon dioxide separation Download PDFInfo
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- CN114870570A CN114870570A CN202210608707.5A CN202210608707A CN114870570A CN 114870570 A CN114870570 A CN 114870570A CN 202210608707 A CN202210608707 A CN 202210608707A CN 114870570 A CN114870570 A CN 114870570A
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- 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
- B01D53/14—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 by absorption
- B01D53/1456—Removing acid components
- B01D53/1475—Removing carbon dioxide
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- 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
- B01D53/14—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 by absorption
- B01D53/1493—Selection of liquid materials for use as absorbents
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/50—Combinations of absorbents
- B01D2252/504—Mixtures of two or more absorbents
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- 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
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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- 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
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- Gas Separation By Absorption (AREA)
Abstract
The invention relates to a method for CO 2 The separated liquid-solid phase separation absorbent takes N-methyldiethanolamine as a main body and comprises activator piperazine, organic solvent and water, wherein the mass percent of the N-methyldiethanolamine is 20-40%; the mass percent of the activating agent piperazine is 3-15%; the mass percent of the organic solvent is 30-60%, and the mass percent of the water is 0-40%; the liquid-solid phase separation absorbent absorbs CO 2 The gas source is a uniform liquid phase to absorb CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Enriching in solid phase, separating to obtain solid phase, desorbing only solid phase, and recycling the desorbed absorbent. Only solid needs to be heated in the desorption process, and temperature rise sensible heat and water evaporation latent heat are avoided, so that CO is reduced 2 And (5) desorbing energy consumption.
Description
Technical Field
The invention belongs to the technical field of gas separation, and particularly relates to a method for separating CO 2 Separated liquidSolid phase absorbent.
Background
At present, those skilled in the art are constantly developing new high efficiency absorbents in an attempt to reduce CO in chemical absorption processes 2 And (5) capturing energy consumption. A new class of absorbents, phase change absorbents, is proposed. Absorption of CO by phase change absorbents 2 Pre-homogeneous, absorbing CO 2 Two phases are formed later to obtain CO 2 Very high loaded CO 2 Rich phase, CO only 2 The enriched phase enters the desorption unit, so that the amount of the enriched phase entering the desorption unit is reduced, and the energy consumption in the desorption process is reduced.
Chinese patent application "MDEA composite absorbent and separation method for acid gas separation" (application No. 201610035154.3, published 2016, 5, 4), chinese patent application "liquid-liquid phase change absorbent and application for carbon dioxide capture" (application No. 201910378327.5, published, 2019, 7, 26), and chinese patent application "a reaction phase change CO 2 The absorbent and the preparation method thereof (application No. 201910771297.4, published as 9/22/2020) and Chinese patent application "a phase change absorbent for capturing carbon dioxide and a method for capturing carbon dioxide" (application No. 201911218162.1, published as 2/18/2020) both propose a phase change absorbent which absorbs CO 2 Then liquid-liquid phase separation is formed, and CO is enriched 2 The liquid phase of (a) enters a desorption unit. The energy in the desorption process is not fully used for CO 2 The desorption, and the other part for the solution temperature rise and solvent evaporation.
For further CO reduction 2 Trapping energy consumption, a class of phase change absorbents for liquid-solid phase separation were developed by those skilled in the art. The phase change absorbent absorbs CO 2 Then liquid-solid phase separation is formed, and CO is enriched 2 The solid phase enters a desorption unit, and the energy of desorption is totally used for CO 2 And (4) desorbing. Chinese patent application "system and method for capturing carbon dioxide" (application No. 201310046925.5, published 2013, 8.14) proposes the use of amino-siloxane compounds to obtain solid reaction products after absorption of CO 2. Chinese patent application' preparation of two-phase absorbent by using ethylenediamine and DMA (direct memory access) for removing CO from biological hydrogen alkane gas 2 Method of (1) (application No. 2)01711311798.1, published 2018, 6.19) proposed mixing ethylenediamine with DMA to obtain a liquid two-phase absorbent, which reacts with CO2 to form a solid precipitate. Chinese patent application "a method for removing carbon dioxide from a gas mixture by two-phase absorption" (application No. 201310631961.8, published 2014, 3, 26) proposes that enamine and an organic solvent form a two-phase absorbent, the organic solvent is C1-C10 alcohols, toluene, DMF, DMAC, and carbon dioxide in the gas mixture is removed by precipitation after contacting with the absorbent. The components of the phase change absorbent of the liquid-solid phase separation are volatile or are not common amine, the price is high, and the economical efficiency needs to be investigated.
In review, it is of practical interest to develop a mature liquid-solid phase-change absorbent based on industrial applications.
Disclosure of Invention
In view of the disadvantages of the prior art, it is an object of the present invention to provide a method for CO 2 A separated liquid-solid phase separation absorbent which absorbs CO 2 The former is a uniform liquid phase, absorbs CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Enriching in solid phase, separating to obtain solid phase, desorbing only solid phase, and recycling the desorbed absorbent. Only solid needs to be heated in the desorption process, and temperature rise sensible heat and water evaporation latent heat are avoided, so that CO is reduced 2 And (5) desorbing energy consumption.
In order to achieve the above purposes, the invention adopts the technical scheme that:
for CO 2 The separated liquid-solid phase separation absorbent takes N-methyldiethanolamine as a main body and comprises activator piperazine, organic solvent and water, wherein the mass percent of the N-methyldiethanolamine is 20-40%; the mass percent of the activating agent piperazine is 3-15%; the mass percent of the organic solvent is 30-60%, the mass percent of the water is 0-40%, and the sum of the total mass percent is 100%. The liquid-solid phase separation absorbent absorbs CO 2 The gas source is a uniform liquid phase to absorb CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Enriching in solid phase, separating to obtain solid phase, desorbing only solid phase, and desorbingThe absorbent can be recycled.
Preferably, in the liquid-solid phase separation absorbent, the mass percent of N-methyldiethanolamine is 30-40%, the mass percent of activator piperazine is 3-10%, the mass percent of organic solvent is 40-60%, the mass percent of water is 0-20%, and the sum of the total mass percent is 100%.
Preferably, in the liquid-solid phase separation absorbent, the mass percent of N-methyldiethanolamine is 32%, the mass percent of activator piperazine is 8%, the mass percent of organic solvent is 40%, the mass percent of water is 20%, and the sum of the total mass percent is 100%.
Preferably, in the liquid-solid phase separation absorbent, the mass percent of N-methyldiethanolamine is 37%, the mass percent of activator piperazine is 3%, the mass percent of organic solvent is 40%, the mass percent of water is 20%, and the sum of the total mass percent is 100%.
Preferably, in the liquid-solid phase separation absorbent, the mass percent of N-methyldiethanolamine is 32%, the mass percent of activating agent piperazine is 8%, the mass percent of organic solvent is 60%, and the sum of the total mass percent is 100%.
Preferably, the organic solvent is selected from any one or more of dimethyl sulfoxide, N-methyl pyrrolidone, N-methyl formamide and N, N-dimethyl formamide, preferably N-methyl pyrrolidone.
Further, the liquid-solid phase separation absorbent absorbs CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Is enriched in the solid phase.
Further, the solid phase of the liquid-solid phase separation absorbent accounts for 5-50% of the liquid-solid phase separation absorbent in volume percentage.
Further, the liquid-solid phase separation absorbent absorbs CO 2 A liquid-solid two phase is spontaneously formed after the gas source, and the solid phase accounts for 5 to 50 percent of the volume percentage of the liquid-solid phase separation absorbent; separating to obtain solid phase, desorbing only the solid phase, and recycling the absorbent obtained by desorption.
Preferably, the liquid-solid phase separation absorptionCO absorption by agents 2 The gas source conditions were: the pressure is normal pressure to 3.0MPaG, and the temperature is 20-80 ℃.
CO is carried out by utilizing the liquid-solid phase separation absorbent 2 A method of separation comprising the steps of: at a temperature of 20-80 deg.C, CO 2 The pressure of the gas source is normal pressure to 3.0MPaG, and the absorbent and CO are mixed 2 Gas source contact reaction to absorb CO 2 The gas source is a uniform liquid phase to absorb CO 2 Spontaneously forms a liquid-solid two phase after air source, and the solid phase is CO 2 The volume percentage of the solid phase in the enriched rich liquid phase accounts for 5-50% of the liquid-solid phase separation absorbent; and (4) enabling the rich liquid phase to enter a desorption unit for desorption, and recycling the absorbent obtained by desorption.
Still further, the CO is 2 The gas source is flue gas, natural gas, shift gas or synthesis gas.
Compared with the prior art, the method for preparing CO provided by the invention 2 The separated liquid-solid phase separation absorbent has the following advantages:
firstly, the main body of the liquid-solid phase separation absorbent is N-methyldiethanolamine, which has the advantage of low regeneration energy consumption and can reduce CO 2 Desorbing energy consumption; the activator component can improve the absorption of CO by the liquid-solid phase separation absorbent 2 The absorption equipment height is reduced, and the equipment investment is reduced.
Secondly, the liquid-solid phase separation absorbent of the invention absorbs CO 2 The gas source is a uniform liquid phase to absorb CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Enriching in solid phase, separating to obtain solid phase, desorbing only solid phase, and recycling the desorbed absorbent. In the desorption process, only solid needs to be heated, and sensible heat of temperature rise and latent heat of water evaporation are avoided, so that CO is reduced 2 And (5) desorbing energy consumption.
Detailed Description
The invention is further described below with reference to specific embodiments and examples.
Example 1
Mixing N-methyldiethanolamine, activating agent piperazine, N-dimethylformamide and water to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamineThe content of the N, N-dimethylformamide is 32%, the mass fraction of the activating agent piperazine is 8%, the mass fraction of the N, N-dimethylformamide is 40%, and the mass fraction of the water is 20%; at 40 deg.C and normal pressure, mixed gas CO 2 The content is 50 percent, and the absorbent is used for absorbing to saturation; absorption of CO 2 The latter absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 5.0 mL. CO2 2 The solid phase accounts for 5 percent of the volume of the liquid-solid phase separation absorbent.
Example 2
Mixing N-methyldiethanolamine, activator piperazine, dimethyl sulfoxide and water to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamine is 32%, the mass fraction of the activator piperazine is 8%, the mass fraction of the dimethyl sulfoxide is 40%, and the mass fraction of the water is 20%; at 40 deg.C and normal pressure, mixed gas CO 2 Content 15%, absorbing to saturation with the absorbent; absorption of CO 2 The latter absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 17.0 mL. CO2 2 The volume percentage of the solid phase in the liquid-solid phase separation absorbent is 17%.
Example 3
Mixing N-methyldiethanolamine, activator piperazine, N-methylpyrrolidone and water to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamine is 37%, the mass fraction of the activator piperazine is 3%, the mass fraction of the N-methylpyrrolidone is 50%, and the mass fraction of the water is 10%; at 40 deg.C and normal pressure, mixed gas CO 2 Content 15%, absorbing to saturation with the absorbent; absorption of CO 2 The latter absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 40.0 mL. CO2 2 The solid phase accounts for 40 percent of the volume of the liquid-solid phase separation absorbent.
Example 4
Mixing N-methyldiethanolamine, activator piperazine, N-methylpyrrolidone and water to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamine is 30%, the mass fraction of the activator piperazine is 10%, the mass fraction of the N-methylpyrrolidone is 50%, and the mass fraction of the water is 10%; at 40 deg.C and normal pressure, mixed gas CO 2 Content 15%, absorbing to saturation with the absorbent; absorption of CO 2 The absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 7.0 mL. CO2 2 The solid phase accounts for 7 percent of the volume of the liquid-solid phase separation absorbent.
Example 5
Mixing N-methyldiethanolamine, activator piperazine, N-methylpyrrolidone and water to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamine is 32%, the mass fraction of the activator piperazine is 8%, the mass fraction of the N-methylpyrrolidone is 60%, and the mass fraction of the water is 0%; at 40 deg.C and normal pressure, mixed gas CO 2 Content 15%, absorbing to saturation with the absorbent; absorption of CO 2 The latter absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 20.0 mL. CO2 2 The solid phase accounts for 20 percent of the volume of the liquid-solid phase separation absorbent.
Example 6
Mixing N-methyldiethanolamine, activator piperazine, an organic solvent and water, wherein the organic solvent is a mixture of N, N-dimethyl amide and N-methyl formamide to prepare 100g of the absorbent, the mass fraction of the N-methyldiethanolamine is 30%, the mass fraction of the activator piperazine is 10%, the mass fraction of the N, N-dimethyl amide is 25%, the mass fraction of the N-methyl formamide is 10%, namely the mass fraction of the organic solvent is 35%, and the mass fraction of the water is 25%; pure CO at 40 deg.C and normal pressure 2 Absorbing to saturation with the absorbent; absorption of CO 2 The latter absorbent forms two phases of liquid and solid, and the solid phase is CO 2 Phase enriched, volume 15.0 mL. CO2 2 The solid phase accounts for 15 percent of the volume of the liquid-solid phase separation absorbent.
Comparative example 1:
the liquid-solid phase separation absorbent was prepared by the same procedure as in example 1 except that the organic solvent was replaced with n-propanol and the remaining conditions were identical. But the resulting absorbent is in any CO 2 No phase separation occurs under partial pressure.
Comparative example 2:
mixing N-methyldiethanolamine and organic solventMixing a solvent and water, wherein the organic solvent is polyethylene glycol dimethyl ether to prepare 100g of absorbent, wherein the mass fraction of the N-methyldiethanolamine is 30%, the mass fraction of the polyethylene glycol dimethyl ether is 20%, and the mass fraction of the water is 40%; disposing the resulting absorbent in any CO 2 No phase separation occurs under partial pressure.
Comparative example 3:
mixing N-methyldiethanolamine, activating agent piperazine, organic solvent and water, wherein the organic solvent is N-methylpyrrolidone, preparing 100g of absorbent, the mass fraction of the N-methyldiethanolamine is 35%, the mass fraction of the piperazine is 5%, the mass fractions of the N-methylpyrrolidone are respectively 10%, 20% or 25% for experiment, and the mass fractions of the rest water are 100%. Disposing the resulting absorbent in any CO 2 No phase separation occurs under partial pressure.
Comparative example 4:
the absorbent is prepared by mixing N-methyldiethanolamine, activating agent piperazine, organic solvent and water, wherein the organic solvent is N-methylpyrrolidone, and 100g of the absorbent is prepared, the mass fraction of the N-methyldiethanolamine is 39%, the mass fraction of the piperazine is 1%, the mass fraction of the N-methylpyrrolidone is 50%, and the mass fraction of the water is 10%. Disposing the resulting absorbent in any CO 2 No phase separation occurs under partial pressure.
Comparative example 5:
the absorbent is prepared by mixing N-methyldiethanolamine, activator piperazine, organic solvent and water, wherein the organic solvent is polyethylene glycol dimethyl ether, and the absorbent is prepared into 100g, the mass fraction of the N-methyldiethanolamine is 30%, the mass fraction of the piperazine is 5%, the mass fraction of the polyethylene glycol dimethyl ether is 10%, and the mass fraction of the water is 55%. Disposing the resulting absorbent in any CO 2 No phase separation occurs under partial pressure.
Comparative example 6:
mixing N-methyldiethanolamine, an activator morpholine, an organic solvent and water, wherein the organic solvent is polyethylene glycol dimethyl ether or sulfolane, and preparing 100g of absorbent, the mass fraction of the N-methyldiethanolamine is 30%, the mass fraction of the morpholine is 5%, and the mass fraction of the polyethylene glycol is 5%The mass fraction of the alcohol dimethyl ether or sulfolane is 10 percent, and the mass fraction of the water is 55 percent. The obtained absorbent (organic solvent is polyethylene glycol dimethyl ether or sulfolane) is prepared in any CO 2 No phase separation occurs under partial pressure.
The above-described embodiments are merely illustrative of the present invention, which may be embodied in other specific forms or in other specific forms without departing from the spirit or essential characteristics thereof. The described embodiments are, therefore, to be considered in all respects as illustrative and not restrictive. The scope of the invention should be indicated by the appended claims, and any changes that are equivalent to the intent and scope of the claims should be construed to be included therein.
Claims (10)
1. For CO 2 Separated liquid-solid phase separation absorbent, characterized in that said liquid-solid phase separation absorbent absorbs CO 2 The gas source is a uniform liquid phase to absorb CO 2 Spontaneously form two phases of liquid and solid, CO, after gas supply 2 Enriching in a solid phase, separating to obtain a solid phase, desorbing only the solid phase, and recycling the absorbent obtained by desorption; the liquid-solid phase separation absorbent takes N-methyldiethanolamine as a main body and comprises activator piperazine, organic solvent and water, wherein the mass percent of the N-methyldiethanolamine is 20-40%; the mass percent of the activating agent piperazine is 3-15%; the mass percent of the organic solvent is 30-60%, the mass percent of the water is 0-40%, and the sum of the total mass percent is 100%.
2. The liquid-solid phase separation absorbent according to claim 1, wherein the mass percent of N-methyldiethanolamine is 30-40%, the mass percent of activator piperazine is 3-10%, the mass percent of organic solvent is 40-60%, the mass percent of water is 0-20%, and the sum of the total mass percent is 100%.
3. The liquid-solid phase separation absorbent according to claim 1, wherein the organic solvent is selected from any one or more of dimethylsulfoxide, N-methylpyrrolidone, N-methylformamide and N, N-dimethylformamide.
4. The liquid-solid phase-separated absorbent according to claim 3, wherein said organic solvent is N-methylpyrrolidone.
5. The liquid-solid phase separation absorbent according to claim 1, wherein the mass percent of N-methyldiethanolamine, the mass percent of the activator piperazine, the mass percent of the organic solvent and the total mass percent of the liquid-solid phase separation absorbent are respectively 32%, 8% and 60%, respectively, and the sum of the mass percent of the N-methyldiethanolamine and the total mass percent of the organic solvent is 100%.
6. The liquid-solid phase separation absorbent according to claim 1, wherein the liquid-solid phase separation absorbent absorbs CO 2 The gas source conditions were: the pressure is normal pressure to 3.0 MPaG.
7. The liquid-solid phase separation absorbent according to claim 6, wherein the liquid-solid phase separation absorbent absorbs CO 2 The gas source is 20-80 ℃.
8. The liquid-solid phase separation absorbent according to claim 1, wherein the solid phase accounts for 5-50% of the liquid-solid phase separation absorbent by volume after the liquid-solid phase separation absorbent forms the liquid-solid two phases.
9. The liquid-solid phase-separated absorbent as claimed in claim 1, wherein said CO is present in a gas phase 2 The gas source is flue gas, natural gas, shift gas or synthesis gas.
10. CO-separation using the liquid-solid phase-separated absorbent according to any of claims 1 to 9 2 A method of separation characterized by the steps of: at a temperature of 20-80 deg.C, CO 2 The pressure of the gas source is normal pressure to 3.0MPaG, and the absorbent and CO are mixed 2 Gas source contact reaction to absorb CO 2 The gas source is a uniform liquid phase in front of which CO is absorbed 2 Spontaneously forms a liquid-solid two phase after air source, and the solid phase is CO 2 The volume percentage of the solid phase in the enriched rich liquid phase accounts for 5-50% of the liquid-solid phase separation absorbent; and (4) enabling the rich liquid phase to enter a desorption unit for desorption, and recycling the absorbent obtained by desorption.
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| CN110801711A (en) * | 2019-12-03 | 2020-02-18 | 中冶京诚工程技术有限公司 | Phase change absorbent for capturing carbon dioxide and method for capturing carbon dioxide |
| CN111569612A (en) * | 2020-06-03 | 2020-08-25 | 西南化工研究设计院有限公司 | Anhydrous chemical absorbent for absorbing acid gas and application thereof |
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