CN110152452B - Ternary non-aqueous solid-liquid phase change absorption system and application thereof - Google Patents
Ternary non-aqueous solid-liquid phase change absorption system and application thereof Download PDFInfo
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- CN110152452B CN110152452B CN201910393822.3A CN201910393822A CN110152452B CN 110152452 B CN110152452 B CN 110152452B CN 201910393822 A CN201910393822 A CN 201910393822A CN 110152452 B CN110152452 B CN 110152452B
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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
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/20—Organic absorbents
- B01D2252/202—Alcohols or their derivatives
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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
- B01D2252/20—Organic absorbents
- B01D2252/204—Amines
- B01D2252/20436—Cyclic amines
- B01D2252/20447—Cyclic amines containing a piperazine-ring
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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
Abstract
The invention discloses a ternary non-aqueous solid-liquid phase change absorption system and application thereof, wherein the absorption system is prepared from 2-amino-2-methyl-1-propanol, dipropylene glycol dimethyl ether and piperazine, which absorbs CO2The former is a uniform transparent liquid solution for absorbing CO2Then become solid-liquid two phases, and CO2The enriched liquid is only needed to be regenerated after the solid phase is separated, and the regenerated rich liquid amount can be greatly reduced, so that the regeneration energy consumption of the technology is reduced. The solid-liquid phase change ternary absorption system has the greatest advantage that the saturated rich liquid solid phase is granular crystals, and compared with the traditional solid-liquid phase change system solid phase viscous rich liquid, the solid-liquid phase change ternary absorption system is easy to separate and operate; and the regeneration temperature of the phase change system is far lower than that of the traditional solid-liquid phase change system, so that the phase change system has better application prospect.
Description
Technical Field
The invention belongs to the technical field of carbon dioxide capture, and particularly relates to a ternary non-aqueous solid-liquid phase change absorption system and application thereof.
Background
Carbon dioxide (CO)2) As the most important greenhouse gas, its control and emission reduction are the hot spots of interest in various countries in recent years. Carbon emission reduction is mainly aimed at energy systems, such as CO in thermal power plants and the like2The key of the concentrated emission source is to CO in the flue gas2The collection and separation of (1). However, the traditional organic amine aqueous solution absorption method has the problem of high regeneration energy consumption. Taking 30 wt% ethanolamine (MEA) as an example, the energy consumption of thermal desorption of the saturated solution is as high as 3.7GJ/t CO2A large amount of energy is consumed in the heating and evaporation process of the solvent water.
Phase change absorbents, a new type of absorbent, have received much attention from researchers in recent years. The novel absorbent is used for absorbing CO2The former is homogeneous solution, absorbs CO2Then the absorbent can generate liquid-liquid or solid-liquid phase separation and CO through regulation by a certain means2Mainly enriches in one phase, only needs to enrich CO2And the rich phase is sent to a regeneration tower for desorption, so that the regeneration volume of the absorbent is greatly reduced, and the regeneration energy consumption of the system is further reduced. At present, the existing phase change absorbents are mainly focused on liquid-liquid phase change absorption systems, but actually, the research on the systems is not yet completedThe problems such as inconvenient separation of liquid-liquid two phases and high viscosity of rich solution still need to be solved by further research and exploration. In addition to liquid-liquid phase separation, the development of solid-liquid phase separation systems can overcome the problems faced by liquid-liquid phase separation systems to some extent. Due to CO2The absorption product is continuously precipitated from the solution in the form of solid, which is beneficial to the rapid separation of the product. In the existing research on the solid-liquid phase change absorbent, a polyamine non-aqueous solid-liquid phase change system based on organic amine forms a viscous solid product which is not beneficial to separation; non-aqueous solid-liquid phase change system of poly (amine) group, which enables CO2The absorption product is completely precipitated from the solvent, so that the phase separation effect is better, but the oxidative degradation of amine and the corrosion of equipment are easily accelerated by excessively high regeneration temperature. Therefore, how to construct a novel solid-liquid phase change absorbent is a key problem.
As can be seen from the above, the phase change absorbent is due to CO2Mainly enriches in one phase, only needs to enrich CO2The rich phase is sent to a regeneration tower for desorption, thereby greatly reducing the regeneration volume of the absorbent and having huge energy-saving potential. Compared with a liquid-liquid phase change absorbent, the solid-liquid phase change absorbent has the advantages that the product is relatively easy to separate, the actual operation is facilitated, related researches are few, and how to construct a novel solid-liquid phase change system is still a difficult problem. The invention provides a ternary non-aqueous solid-liquid phase change absorption system and application thereof in carbon dioxide capture, which overcome the defects that the rich solution of the existing phase change absorbent is viscous and difficult to separate or the regeneration temperature is high, and provide a new idea for carbon dioxide capture.
Disclosure of Invention
The invention aims to overcome the defects of the prior art, provides a ternary non-aqueous solid-liquid phase change absorption system and application thereof, and solves the problems of low carbon dioxide capture efficiency, difficult absorbent regeneration and the like in the background technology.
The technical scheme adopted by the invention for solving the technical problems is as follows: a ternary non-aqueous solid-liquid phase change absorption system is provided, and the ternary mixed system is composed of 2-amino-2-methyl-1-propanol (AMP), dipropylene glycol dimethyl ether (DME) and Piperazine (PZ), wherein the molar ratio of the 2-amino-2-methyl-1-propanol to the piperazine is 7:3-9:1, the total concentration of the two is 1-2mol/L, and the dipropylene glycol dimethyl ether is used as a solvent.
Wherein AMP (formula I) is used as a main absorbent, and due to the steric effect, the excellent regeneration performance of the system is ensured; non-aqueous liquid solid phase systems based on AMP absorb CO2Then, the product is generated in a form of a small amount of solid, the volume amount of the absorbent to be regenerated is greatly reduced, the absorbent can be efficiently regenerated at a lower temperature, and the energy-saving potential is huge;
DME (formula II) as a phase-splitting reagent ensuring that the absorbent absorbs CO2Then solid-liquid phase change is easy to occur, and the solvent is not easy to volatilize during regeneration due to the characteristics of high boiling point and low vapor pressure;
pz (formula III) as CO2The deprotonation activator of the absorption reaction, and the addition of the nucleophilic organic base deprotonation activator Pz can obviously improve the CO treatment of the system2The absorption performance of the catalyst can compensate the absorption of CO by AMP2Deficiencies in absorption rate and absorption load.
In a preferred embodiment of the present invention, the ternary mixed system is used for absorbing 5-20% by volume of carbon dioxide in pure carbon dioxide or mixed gas.
In a preferred embodiment of the invention, the absorption temperature of carbon dioxide in the ternary mixed system is 30-60 ℃, and the absorption load is 0.5-1.0mol of CO2Per mol of absorbent.
In a preferred embodiment of the present invention, the ternary mixed system has phase-splitting performance. Binary system consisting of AMP or Pz alone dissolved in DME absorbs CO2The front and the back have no phase separation capability, but the ternary system consisting of AMP + PZ + DME absorbs CO2The former is a uniform transparent liquid solution for absorbing CO2Then becomes a solid-liquid two-phase.
In a preferred embodiment of the present invention, the ternary mixing system absorbs CO2The former is homogeneous solution, absorbs CO2Then becomes solid-liquidTwo phases, in which the solid phase is a granular crystal and CO2The enriched liquid is only needed to be regenerated after the solid phase is separated, and the regenerated rich liquid amount can be greatly reduced, so that the regeneration energy consumption of the technology is reduced. The volume of the rich solution of the solid-liquid two phases accounts for 20-50% of the total volume, the amount of the rich solution required to be regenerated is reduced, and the regeneration energy consumption is further effectively reduced.
In a preferred embodiment of the present invention, the solid phase of the solid-liquid two-phase is regenerated by thermal desorption.
In a preferred embodiment of the invention, the regeneration temperature is 90-120 ℃, the regeneration time is 50-100min, and the regeneration efficiency is 40-95%.
The invention also provides application of the ternary non-aqueous solid-liquid phase change absorber system in carbon dioxide capture.
In a preferred embodiment of the invention, 2-amino-2-methyl-1-propanol is used as the main absorbent, dipropylene glycol dimethyl ether is used as the phase separation agent, and piperazine is used as CO2The deprotonation activator of the absorption reaction forms a ternary mixed system, absorbs 5-20% of carbon dioxide in volume ratio in pure carbon dioxide or mixed gas, the absorption temperature is 30-60 ℃, and the absorption load is 0.5-1.0mol of CO2Per mol of absorbent.
In a preferred embodiment of the invention, the absorption of CO will be carried out2After solid phase in the system which is changed into solid-liquid two-phase is filtered and separated, the regeneration is carried out by a thermal desorption mode, the regeneration temperature is 90-120 ℃, the regeneration time is 50-100min, and the regeneration efficiency is 40-95%.
Compared with the background technology, the technical scheme has the following advantages:
1. the scheme effectively utilizes the advantages of each component to obtain the effect that 1+1+1 is more than 3, and the AMP is used as a main absorbent to ensure the excellent regeneration performance of the system due to the steric effect; DME as phase separation agent to ensure CO absorption by the absorbent2Then solid-liquid phase change is easy to occur, and the solvent is not easy to volatilize during regeneration due to the characteristics of high boiling point and low vapor pressure; pz as CO2The deprotonation activator of the absorption reaction can greatly improve the CO content of the system2Absorption properties of CO2The trapping performance is 0.5-1.0mol CO2Per mol of absorbent;
2. by CO2The load regulation and control can realize the characteristic of system phase change, and is simple, convenient and quick;
3. the saturated rich liquid solid phase is a granular crystal, and compared with the traditional solid-liquid phase change system solid phase viscous rich liquid, the saturated rich liquid solid phase is easy to separate and operate, and the regeneration temperature is far lower than that of the traditional solid-liquid phase change system, so that the defect that the existing phase change absorbent rich liquid is viscous and difficult to separate or has high regeneration temperature is overcome.
Drawings
FIG. 1 shows CO capture when the molar ratio of AMP to Pz is 7:32The phase change effect diagrams before and after a-absorption, b-absorption and c-solid phase rich solution;
FIG. 2 shows three solid-liquid phase change systems CO of AMP-PZ-DME with different ratios2Comparison of absorption capacity of (c);
FIG. 3 shows the regeneration performance of the ternary solid-liquid phase change system AMP-PZ-DME at different regeneration temperatures.
Detailed Description
Example 1
In the ternary non-aqueous solid-liquid phase change absorption system of this example, 2-amino-2-methyl-1-propanol is used as the main absorbent, dipropylene glycol dimethyl ether is used as the phase separation agent, and piperazine is used as CO2The deprotonation activator of the absorption reaction forms a ternary mixed system, wherein the molar ratio of the 2-amino-2-methyl-1-propanol to the piperazine is 7:3-9:1, the total concentration of the two is 1-2mol/L, and the dipropylene glycol dimethyl ether is used as a solvent.
The device is used for absorbing 5-20% of carbon dioxide by volume in pure carbon dioxide or mixed gas; in the embodiment, the proportion of the carbon dioxide and the nitrogen mixed gas is 0-20%, and the absorption temperature is 30-60 ℃.
The ternary system consisting of AMP-PZ-DME absorbs CO2The former is a uniform transparent liquid solution for absorbing CO2Then becomes a solid-liquid two-phase, and the solid phase is granular crystal. Will absorb CO2After solid phase in the system which is changed into solid-liquid two-phase is filtered and separated, the regeneration is carried out by a thermal desorption mode, the regeneration temperature is 90-120 ℃, the regeneration time is 50-100min, and the regeneration efficiency is 40-95 percent。
Comparative examples 1 to 3
A binary mixed system was prepared as comparative examples using 1mol/L, 1.5mol/L, 2mol/L aqueous AMP and DME solutions, respectively.
Absorption of CO2Detecting afterload and split-phase effect: detection of CO absorption at 40 ℃ in example 1 and comparative examples 1 to 32Performance and phase splitting effect of
The method comprises the following steps: respectively preparing 30g of AMP-PZ-DME ternary system in example 1 and binary mixed systems of AMP aqueous solution and DME solution in comparative examples 1-3, respectively pouring the ternary systems and the AMP aqueous solution into a three-neck flask, stirring the three-neck flask on a magnetic stirrer at the temperature of 40 ℃ for 150r/min, and introducing 60mL min-1CO of2The absorption test was started until the absorbent was saturated. Through this experiment, different absorbent systems for absorbing CO can be obtained2Is the rate of change over time. The absorption rate is integrated with the time relation, so that the absorption of CO by the absorbent at different times can be obtained2The load situation of (2).
As a result: FIG. 1 shows that the AMP-PZ-DME ternary solid-liquid phase-change system absorbs CO when the molar ratio of AMP to Pz is 7:32Front and back and photographs of the solid phase enriched solution. As can be seen from the figure, AMP-PZ-DME absorbs CO2The former is a uniform liquid phase, absorbs CO2Become a solid-liquid two phase after saturation, CO2Mainly concentrates in solid phase and is granular white crystal. Unlike the existing solid-liquid phase change absorption solid phase sticky state, the solid phase of the particulate matter is very easy to separate by filtration, and the volume of the particles accounts for 47 percent of the total volume. The solid phase is transferred, pyrolyzed and regenerated, and then mixed with barren liquor to become homogeneous phase again.
As shown in figure 2, the ternary phase change system composed of AMP and Pz with different molar ratios absorbs CO2There are significant differences in their ability. As the Pz content increases, the absorption load gradually increases, but the volume of the rich liquid-solid phase also increases. When the ratio of AMP to PZ is 7:3, carbon dioxide is enriched in the solid phase of the crystal particles, the volume of the solid phase after phase separation only accounts for 47 percent of the total volume, and CO accounts for2The content was 94% of the total absorption. The binary mixed system of AMP aqueous solution and DME solution of the comparative example absorbs CO2No phase separation after the reaction, and AMP is water aloneSolution absorption of CO2And then has no phase separation capability.
Second, example 1 testing of regeneration Performance
Due to the large amount of industrial waste gas, the regeneration and recycling of the absorbent are critical links, and the process cost is influenced. The regeneration method of the absorbent is commonly known as thermal desorption, membrane filtration, pressure change method and the like. The regeneration method used in this experimental example was thermal desorption, and the regeneration capacity of the absorbent was examined by comparing the absorption load before and after regeneration of the absorbent.
The method comprises the following steps: the solution of AMP-PZ-DME ternary solid-liquid phase change system (1M, 7:3) from example 1 was taken and CO was absorbed at 40 ℃ as in Experimental example 12To saturation. The saturated absorbent is thermally desorbed for 60min at different regeneration temperatures (90, 100, 110 and 120 ℃), and the regenerated absorbent is subjected to repeated absorption experiments according to the method in the experimental example 1, and the influence of different regeneration temperatures on the absorption performance is examined.
As a result: as shown in FIG. 3, the solution of the AMP-PZ-DME ternary solid-liquid phase change system (1M, 7:3) can be regenerated at 90-120 ℃, but the regeneration efficiency is increased along with the increase of the temperature, wherein the solid is not completely converted into liquid between 90 ℃ and 110 ℃; and desorption is carried out for 60 minutes at 120 ℃, the solid is completely converted into liquid, and the maximum regeneration efficiency can reach 92%. The regeneration temperature of the traditional organic amine aqueous solution is generally 120 ℃, the traditional phase-change amine absorbent can hardly be regenerated without nitrogen purging, and the regeneration efficiency is only 70-80% under nitrogen purging; the solid phase regeneration temperature of the prior polyamine solid-liquid phase change absorbent is generally higher than 120 ℃. Therefore, the AMP-PZ-DME ternary solid-liquid phase change system disclosed by the patent not only has the advantage of low regeneration energy consumption of the phase change absorbent, but also effectively overcomes the defects of difficult regeneration and high regeneration temperature of the existing phase change amine.
The above description is only a preferred embodiment of the present invention, and therefore should not be taken as limiting the scope of the invention, which is defined by the appended claims and their equivalents.
Claims (9)
1. Ternary non-aqueous solid-liquid phase change absorberThe collecting system is characterized in that: the composite material is a ternary mixed system consisting of 2-amino-2-methyl-1-propanol, dipropylene glycol dimethyl ether and piperazine, wherein the molar ratio of the 2-amino-2-methyl-1-propanol to the piperazine is 7:3-9:1, the total concentration of the two is 1-2mol/L, and the dipropylene glycol dimethyl ether is a solvent; the ternary mixed system has split-phase performance and absorbs CO2The former is homogeneous solution, absorbs CO2Then becomes a solid-liquid two phase, wherein the solid phase is granular crystal, and CO2Enriched in the solid phase.
2. The ternary non-aqueous solid-liquid phase change absorbent system of claim 1, wherein: the ternary mixed system is used for absorbing 5-20% of carbon dioxide in volume ratio in pure carbon dioxide or mixed gas.
3. The ternary non-aqueous solid-liquid phase change absorbent system of claim 2, wherein: the absorption temperature of the carbon dioxide of the ternary mixed system is 30-60 ℃, and the absorption load is 0.5-1.0mol of CO2Per mol of absorbent.
4. The ternary non-aqueous solid-liquid phase change absorbent system of claim 1, wherein: the volume of the rich liquid of the solid-liquid two phases accounts for 20-50% of the total volume.
5. The ternary non-aqueous solid-liquid phase change absorbent system of claim 1, wherein: the solid phase of the solid-liquid two phases is regenerated by means of thermal desorption.
6. The ternary non-aqueous solid-liquid phase change absorbent system of claim 5, wherein: the regeneration temperature is 90-120 ℃, the regeneration time is 50-100min, and the regeneration efficiency is 40-95%.
7. Use of a ternary non-aqueous solid-liquid phase change absorber system as claimed in any one of claims 1 to 6 in carbon dioxide capture.
8. Use according to claim 7, characterized in that: 2-amino-2-methyl-1-propanol is used as a main absorbent, dipropylene glycol dimethyl ether is used as a phase separation reagent, and piperazine is used as CO2The deprotonation activator of the absorption reaction forms a ternary mixed system, absorbs 5-20% of carbon dioxide in volume ratio in pure carbon dioxide or mixed gas, the absorption temperature is 30-60 ℃, and the absorption load is 0.5-1.0mol of CO2Per mol of absorbent.
9. Use according to claim 7, characterized in that: will absorb CO2After solid phase in the system which is changed into solid-liquid two-phase is filtered and separated, the regeneration is carried out by a thermal desorption mode, the regeneration temperature is 90-120 ℃, the regeneration time is 50-100min, and the regeneration efficiency is 40-95%.
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| EP1062999A2 (en) * | 1993-10-06 | 2000-12-27 | The Kansai Electric Power Co., Inc. | Method for removing carbon dioxide from combustion exhaust gas |
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