CN117065519A - A method for capturing carbon dioxide using ionic liquid composite absorbent - Google Patents

A method for capturing carbon dioxide using ionic liquid composite absorbent Download PDF

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Publication number
CN117065519A
CN117065519A CN202311206378.2A CN202311206378A CN117065519A CN 117065519 A CN117065519 A CN 117065519A CN 202311206378 A CN202311206378 A CN 202311206378A CN 117065519 A CN117065519 A CN 117065519A
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ionic liquid
composite absorbent
liquid composite
carbon dioxide
proton
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葛春亮
卢晗锋
张威
陈瑶姬
范雯阳
崔国凯
张力
丁得龙
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Zhejiang University of Technology ZJUT
Zhejiang Tiandi Environmental Protection Technology Co Ltd
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Zhejiang University of Technology ZJUT
Zhejiang Tiandi Environmental Protection Technology Co Ltd
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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
    • 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
    • B01D53/1425—Regeneration of liquid absorbents

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Gas Separation By Absorption (AREA)
  • Treating Waste Gases (AREA)

Abstract

本发明涉及一种离子液体复合吸收剂捕集二氧化碳方法，包括：制备多氢键调节的质子型碱性离子液体复合吸收剂；所述质子型碱性离子液体复合吸收剂具有不同结构阴阳离子及不同比例的氢键供体；采用所述质子型碱性离子液体复合吸收剂对二氧化碳进行吸收；对二氧化碳进行脱附。本发明的有益效果是：本发明制备的质子型碱性离子液体复合吸收剂具有粘度低、稳定性好的优点，可以避免有机胺挥发和损失。

The invention relates to a method for capturing carbon dioxide with an ionic liquid composite absorbent, which includes: preparing a proton-type alkaline ionic liquid composite absorbent regulated by multiple hydrogen bonds; the proton-type alkaline ionic liquid composite absorbent has different structures of anions and cations and Different proportions of hydrogen bond donors; using the proton-type alkaline ionic liquid composite absorbent to absorb carbon dioxide; and desorbing carbon dioxide. The beneficial effects of the present invention are: the protonic alkaline ionic liquid composite absorbent prepared by the present invention has the advantages of low viscosity and good stability, and can avoid the volatilization and loss of organic amines.

Description

Method for capturing carbon dioxide by using ionic liquid composite absorbent
Technical Field
The invention relates to the technical field of absorption, in particular to a method for capturing carbon dioxide by using an ionic liquid composite absorbent.
Background
As a C1 resource, various high-added-value products can be synthesized by starting from carbon dioxide. In order to achieve the strategic goals of carbon peak and carbon neutralization, new technologies for carbon dioxide capture and utilization and sequestration are required to be developed.
At present, organic amine and a compound system thereof are generally adopted as an absorbent in industry, and carbon dioxide is captured by a chemical absorption method. However, the method has the defects of equipment corrosion, high desorption energy consumption, easy solvent volatilization and the like, and does not accord with the principle of green sustainable development.
The ionic liquid (ionic liquid) is a novel green solvent composed of organic cations and organic or inorganic anions, has the advantages of high thermal stability, high chemical stability, incombustibility, designability structure and the like, and has great potential in the fields of acid gas absorption, catalysis and the like. For example, blancard et al measured the solubility of carbon dioxide in various imidazoles ionic liquids at various pressures, indicating that carbon dioxide can be physically dissolved in ionic liquids, but is less soluble at atmospheric pressure (Nature 1999,28). Another approach is to perform chemical capture of carbon dioxide gas by functionalized ionic liquids. For example, davis et al first used amino functionalized ionic liquids to capture carbon dioxide, and can capture 0.5 moles of carbon dioxide per mole of ionic liquid at atmospheric pressure (j.am.chem.soc., 2002,926). Thereafter, many researchers have developed other quaternary phosphonium, imidazole, quaternary ammonium, pyridine-type ionic liquids containing amino groups for capturing carbon dioxide. However, in 2, which is subject to amine and carbon dioxide: the absorption mechanism of 1 has low absorption capacity, difficult desorption, high desorption temperature up to 120 ℃, and high preparation cost, so that the method is not suitable for large-scale industrial popularization at present.
Therefore, based on the characteristic of function ion liquid action site regulation, a green absorbent with high stability, easy adsorption and easy desorption is developed, which is a key problem for realizing the trapping and utilization of green low-energy-consumption carbon dioxide.
Disclosure of Invention
The invention aims at overcoming the defects of the prior art, and provides a method for capturing carbon dioxide by using an ionic liquid composite absorbent.
In a first aspect, a method for capturing carbon dioxide by using an ionic liquid composite absorbent is provided, which comprises the following steps:
step 1, preparing a proton type alkaline ionic liquid composite absorbent with multiple hydrogen bond regulation; the proton type alkaline ionic liquid composite absorbent has anions and cations with different structures and hydrogen bond donors with different proportions;
step 2, absorbing carbon dioxide by adopting the proton type alkaline ionic liquid composite absorbent;
and 3, desorbing the carbon dioxide.
Preferably, in the step 2, the pressure of the absorbed gas is 0.0001-0.1MPa, the absorption temperature is 30-60 ℃ and the absorption time is 0.5-10h.
Preferably, in the step 3, the desorption temperature is 60-120 ℃ and the desorption time is 0.5-5h.
In a second aspect, there is provided an ionic liquid composite absorber according to the first aspect, consisting of an ionic liquid and a hydrogen bond donor; the ionic liquid is prepared according to the following steps of 1: the proton acceptor and the proton donor are mixed at normal temperature and normal pressure according to the molar ratio of 1, and are compounded with the hydrogen bond donor.
Preferably, the proton acceptor includes: 1, 5-diazabicyclo [4.3.0] -5-nonene (DBN), 1, 8-diazabicyclo [5.4.0] undec-7-ene (DBU), 1, 3-Tetramethylguanidine (TMG), N' -dimethylpiperazine (MPZ), 7-methyl-1, 5, 7-triazabicyclo [4.4.0] dec-5-ene (MTBD) and 1, 4-diazabicyclo [2.2.2] octane (DABCO); the proton donor includes: pyrazole (Pyra), 4-methylpyrazole (4-Me-Pyra), 4-bromopyrazole (4-Br-Pyra), 4-phenylpyrazole (4-Ph-Pyra) and benzopyrazole (BenPyra).
Preferably, the hydrogen bond donor includes Ethylene Glycol (EG) and glycerol (Gly).
Preferably, the ionic liquid has a decomposition temperature of greater than 120 ℃.
Preferably, the proton acceptor is 1, 5-diazabicyclo [4.3.0] -5-nonene, the proton donor is pyrazole, and the hydrogen bond donor is ethylene glycol.
In a third aspect, there is provided a method for preparing the ionic liquid composite absorbent according to the first aspect, comprising:
step 1, according to 1: mixing a proton acceptor and a proton donor at normal temperature and normal pressure in a molar ratio of 1 to obtain a proton type alkaline ionic liquid;
and step 2, compounding proton type alkaline ionic liquid hydrogen bond donors, and stirring at 90 ℃ for 1-3h to prepare the ionic liquid composite absorbent.
In a fourth aspect, there is provided the use of an ionic liquid composite absorber according to the first aspect for capturing carbon dioxide.
The beneficial effects of the invention are as follows:
1. the proton type alkaline ionic liquid composite absorbent prepared by the invention has the advantages of low viscosity and good stability, and can avoid volatilization and loss of organic amine.
2. The invention adopts the proton type alkaline ionic liquid composite absorbent with multiple hydrogen bonds for absorbing carbon dioxide, the absorption capacity is obviously increased, and the absorption capacity under normal pressure can reach 1.1mol -1 。
Drawings
FIG. 1 is a flow chart of a method for capturing carbon dioxide by using an ionic liquid composite absorbent.
Detailed Description
The invention is further described below with reference to examples. The following examples are presented only to aid in the understanding of the invention. It should be noted that it will be apparent to those skilled in the art that modifications can be made to the present invention without departing from the principles of the invention, and such modifications and adaptations are intended to be within the scope of the invention as defined in the following claims.
Example 1:
adding 0.005mol of ionic liquid composite absorbent of the same EG hydrogen bond donor, a strong alkaline proton acceptor (DBN) and different weak alkaline proton donors into a 4ml glass container with an inner diameter of 1.5cm, slowly introducing carbon dioxide gas, controlling the molar ratio (proton acceptor: proton donor) by 20ml/min at the pressure of 0.1 MPa: hydrogen bond donor= (1:1): 1. The absorption temperature was 40℃and the absorption time was controlled to 4 hours, and the sample was weighed by an analytical balance during the trapping process. The amount of carbon dioxide captured is shown in table 1.
TABLE 1 influence of different classes of weakly basic proton donors on carbon dioxide capture behavior of ionic liquids
Example 2:
similar to example 1, the absorption capacity was measured by absorbing carbon dioxide with the same EG hydrogen bond donor, pyrazole (Pyra) proton donor, and an ionic liquid composite absorber composed of different proton acceptors. Control of the molar ratio (proton acceptor: proton donor): hydrogen bond donor= (1:1): 1. The amount of carbon dioxide captured is shown in table 2.
TABLE 2 Effect of different classes of strongly basic proton acceptors on carbon dioxide capture behavior of ionic liquids
Example 3
Similar to example 1, the absorption capacity was measured by absorbing carbon dioxide with an ionic liquid composite absorber composed of the same Pyra proton donor, DBN proton acceptor, and different hydrogen bond donors. The amount of carbon dioxide captured is shown in table 3.
TABLE 3 influence of different kinds of Hydrogen bond donors and ratios on carbon dioxide capturing behavior of ionic liquids
As can be seen from table 3, the hydrogen bond acceptors: the molar ratio of the hydrogen bond donors is different, the absorption amount of the carbon dioxide gas can be obviously changed, wherein the greater the number of the hydrogen bond donors is, the greater the absorption amount of the carbon dioxide gas is by the ionic liquid system.
Example 4:
similar to example 1, an ionic liquid composite absorbent [ DBN ] [ Pyra ]/EG (1:1) was selected, the carbon dioxide gas pressure was controlled to 0.1MPa, the absorption temperature was 20 ℃, 30 ℃, 40 ℃, 50 ℃, 60 ℃ and the carbon dioxide capturing amount was as shown in Table 4.
TABLE 4 influence of different absorption temperatures on carbon dioxide capture by ionic liquids
As can be seen from Table 4, the absorption amount of carbon dioxide gas varies significantly depending on the temperature of the absorption gas, wherein the higher the absorption temperature is, the smaller the amount of carbon dioxide gas absorbed by the ionic liquid system is.
Example 5:
similar to example 1, an ionic liquid composite absorbent [ DBN ] [ Pyra ]/EG (1:1) was selected, the absorption temperature was controlled to 40 ℃, the carbon dioxide gas pressures were 0.01, 0.02, 0.04, 0.06, 0.08, 0.1MPa, and the carbon dioxide capturing amounts were as shown in Table 5.
TABLE 5 influence of different carbon dioxide pressures on carbon dioxide capture by ionic liquids
As can be seen from Table 5, the amount of carbon dioxide absorbed varies significantly with the pressure of the absorbed gas, wherein the higher the gas pressure, the higher the amount of carbon dioxide absorbed by the ionic liquid system.
Example 6:
similar to example 1, an ionic liquid composite absorbent [ DBN ] [ Pyra ]/EG (1:1) was selected, the absorption temperature was controlled to 40 ℃, the carbon dioxide gas pressure was controlled to 0.1MPa, and the absorption times were 0.5, 1, 1.5, 2, and 4 hours, and the carbon dioxide capturing amounts were as shown in Table 6.
TABLE 6 influence of different absorption times on carbon dioxide capture by ionic liquids
As can be seen from table 6, the absorption amount of carbon dioxide gas increases with the increase in the absorption time before the absorption equilibrium is not reached; after the absorption equilibrium is reached, the absorption amount of carbon dioxide gas is hardly changed with the absorption time.
Example 7:
nitrogen was slowly introduced into the ionic liquid composite absorbent having absorbed carbon dioxide gas in example 2 at 80℃and a flow rate of 60ml/min at a pressure of 0.1MPa. Control of the molar ratio (proton acceptor: proton donor): hydrogen bond donor= (1:1): 1. The desorption results are shown in Table 7.
TABLE 7 influence of different ionic liquids on carbon dioxide desorption
Example 8
Similarly to examples 2 and 7, the carbon dioxide gas pressure was controlled to be 0.1MPa, the flow rate was controlled to be 20ml/min, the absorption temperature was controlled to be 40 ℃, the nitrogen gas pressure was controlled to be 0.1MPa, the flow rate was controlled to be 60ml/min, the desorption temperature was controlled to be 80 ℃, and the ionic liquid composite absorbent [ DBN ] [ Pyra ]/EG (1:1) was selected, and the trapping amounts thereof were as shown in Table 8.
TABLE 8 ion liquid cycle absorption and desorption results

Claims (10)

1.一种离子液体复合吸收剂捕集二氧化碳方法，其特征在于，包括：1. A method for capturing carbon dioxide using an ionic liquid composite absorbent, which is characterized by comprising: 步骤1、制备多氢键调节的质子型碱性离子液体复合吸收剂；所述质子型碱性离子液体复合吸收剂具有不同结构阴阳离子及不同比例的氢键供体；Step 1. Prepare a proton-type alkaline ionic liquid composite absorbent regulated by multiple hydrogen bonds; the proton-type alkaline ionic liquid composite absorbent has different structures of anions and cations and different proportions of hydrogen bond donors; 步骤2、采用所述质子型碱性离子液体复合吸收剂对二氧化碳进行吸收；Step 2. Use the proton-type alkaline ionic liquid composite absorbent to absorb carbon dioxide; 步骤3、对二氧化碳进行脱附。Step 3. Desorb carbon dioxide. 2.根据权利要求1所述的离子液体复合吸收剂捕集二氧化碳方法，其特征在于，步骤2中，吸收气体压力为0.0001-0.1MPa，吸收温度为30-60℃，吸收时间为0.5-10h。2. The method for capturing carbon dioxide with an ionic liquid composite absorbent according to claim 1, characterized in that in step 2, the absorbed gas pressure is 0.0001-0.1MPa, the absorption temperature is 30-60°C, and the absorption time is 0.5-10h. . 3.根据权利要求2所述的离子液体复合吸收剂捕集二氧化碳方法，其特征在于，步骤3中，脱附温度为60-120℃，脱附时间为0.5-5h。3. The method for capturing carbon dioxide with an ionic liquid composite absorbent according to claim 2, characterized in that in step 3, the desorption temperature is 60-120°C and the desorption time is 0.5-5h. 4.一种如权利要求1所述的离子液体复合吸收剂，其特征在于，由离子液体及氢键供体组成；所述离子液体按照1：1摩尔比常温常压下混合质子受体和质子供体得到，并与氢键供体复配。4. An ionic liquid composite absorbent as claimed in claim 1, characterized in that it is composed of an ionic liquid and a hydrogen bond donor; the ionic liquid is mixed with a proton acceptor and a hydrogen bonding agent at a molar ratio of 1:1 at normal temperature and pressure. The proton donor is obtained and compounded with the hydrogen bond donor. 5.根据权利要求4所述的离子液体复合吸收剂，其特征在于，所述质子受体包括：1,5-二氮杂双环[4.3.0]-5-壬烯、1,8-二氮杂双环[5.4.0]十一碳-7-烯、1,1,3,3-四甲基胍、N,N’-二甲基哌嗪、7-甲基-1,5,7-三氮杂二环[4.4.0]癸-5-烯、1,4-二氮杂二环[2.2.2]辛烷；所述质子供体包括：吡唑、4-甲基吡唑、4-溴吡唑、4-苯基吡唑和苯并吡唑。5. The ionic liquid composite absorbent according to claim 4, wherein the proton acceptor includes: 1,5-diazabicyclo[4.3.0]-5-nonene, 1,8-bis Azabicyclo[5.4.0]undec-7-ene, 1,1,3,3-tetramethylguanidine, N,N'-dimethylpiperazine, 7-methyl-1,5,7 -Triazabicyclo[4.4.0]dec-5-ene, 1,4-diazabicyclo[2.2.2]octane; the proton donor includes: pyrazole, 4-methylpyrazole , 4-bromopyrazole, 4-phenylpyrazole and benzopyrazole. 6.根据权利要求5所述的离子液体复合吸收剂，其特征在于，所述氢键供体包括乙二醇和丙三醇。6. The ionic liquid composite absorbent according to claim 5, wherein the hydrogen bond donor includes ethylene glycol and glycerol. 7.根据权利要求6所述的离子液体复合吸收剂，其特征在于，所述离子液体的分解温度大于120℃。7. The ionic liquid composite absorbent according to claim 6, wherein the decomposition temperature of the ionic liquid is greater than 120°C. 8.根据权利要求4所述的离子液体复合吸收剂，其特征在于，所述质子受体为1,5-二氮杂双环[4.3.0]-5-壬烯，所述质子供体为吡唑，所述氢键供体为乙二醇。8. The ionic liquid composite absorbent according to claim 4, wherein the proton acceptor is 1,5-diazabicyclo[4.3.0]-5-nonene, and the proton donor is Pyrazole, the hydrogen bond donor is ethylene glycol. 9.一种如权利要求1所述的离子液体复合吸收剂的制备方法，其特征在于，包括：9. A method for preparing the ionic liquid composite absorbent according to claim 1, characterized in that it includes: 步骤1、按照1：1摩尔比常温常压下混合质子受体和质子供体得到质子型碱性离子液体；Step 1. Mix the proton acceptor and the proton donor according to a 1:1 molar ratio under normal temperature and pressure to obtain a proton-based alkaline ionic liquid; 步骤2、将质子型碱性离子液体氢键供体复配，在90℃下搅拌1-3h制得离子液体复合吸收剂。Step 2: Compound the proton-type alkaline ionic liquid hydrogen bond donor and stir at 90°C for 1-3 hours to prepare an ionic liquid composite absorbent. 10.一种如权利要求1所述的离子液体复合吸收剂的应用，其特征在于，所述离子液体复合吸收剂用于捕集二氧化碳。10. Application of the ionic liquid composite absorbent according to claim 1, characterized in that the ionic liquid composite absorbent is used to capture carbon dioxide.
CN202311206378.2A 2023-09-18 2023-09-18 A method for capturing carbon dioxide using ionic liquid composite absorbent Pending CN117065519A (en)

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