CN107213753B - CO in flue gas or syngas2Removing method and device - Google Patents
CO in flue gas or syngas2Removing method and device Download PDFInfo
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- CN107213753B CN107213753B CN201710316363.XA CN201710316363A CN107213753B CN 107213753 B CN107213753 B CN 107213753B CN 201710316363 A CN201710316363 A CN 201710316363A CN 107213753 B CN107213753 B CN 107213753B
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Abstract
The invention discloses CO in flue gas or synthetic gas2A method for removing. Comprises introducing the flue gas or synthesis gas into an absorption tower, contacting with absorption liquid in countercurrent for decarbonization, and removing CO from the discharged gas2Flue gas or synthesis gas, liquid phase being CO2Enriching liquid, wherein the absorption liquid is organic amine solution containing phenol; in CO2Introducing excessive carbon dioxide into the enriched solution to make CO2Further acidifying the enriched solution, standing the solution for layering to obtain crude phenol oil and CO2An organic amine solution; introducing the CO into the reactor2Organic amine solution is heated for desorption, and CO released2CO partially used in phenol regeneration step2Acidifying the enriched liquid, and recycling the regenerated organic amine solution as an extracting agent for extracting phenolic substances in the coal tar or the direct coal liquefaction oil. The CO in the flue gas or the synthesis gas provided by the invention2The removal method has good absorption effect of the regenerated absorption liquid and reduces the process operation cost. The invention also provides CO in the flue gas or the synthesis gas2And a removing device.
Description
Technical Field
The invention relates to the technical field of flue gas purification, in particular to CO in flue gas or synthetic gas2A method and apparatus for removal.
BackgroundThe increasing greenhouse gases in the atmosphere are a direct cause of warming the climate. With the rapid development of modern industry, carbon dioxide generated by burning a large amount of fossil fuels is a main source causing greenhouse effect, and in order to reduce environmental pollution and natural disasters caused by the increase of carbon dioxide, the carbon dioxide must be absorbed and enriched to reduce the emission of carbon dioxide into the atmosphereThe living environment of human is protected, and the sustainable development of ecological environment is promoted. In the related art, methods for absorbing carbon dioxide mainly include a physical absorption method, a chemical absorption method, a membrane absorption method, a low-temperature fractionation method, and the like. The chemical absorption method using ammonia water as absorption liquid has the characteristics of strong absorption capacity, low corrosivity, low regeneration energy consumption, low replenishment cost and capability of simultaneously removing various acidic gas pollutants, becomes a mature technology of a decarburization process, and is widely applied in recent years. However, in practical application of ammonia decarburization process, the higher the concentration of the absorption liquid is, incomplete desorption and CO generation can occur during desorption2The lower the desorption rate is, the lower the absorption capacity of the regenerated absorption liquid is, and the problems of ammonia escape and the like are easily caused, so that the process operation cost is increased. Therefore, there is a need to provide a new technology to solve the above technical problems.
Disclosure of Invention
The object of the present invention is to overcome the above technical problems and to provide a process for the production of CO from flue gas or synthesis gas2The removing method comprises extracting phenols and CO from coal tar or direct coal liquefaction oil2Wherein a phenol-containing organic amine solution produced in the extraction of the phenolic substances is used as the absorption of CO2The absorbed solution is completely desorbed in the desorption process, the regenerated absorption solution has good absorption effect, and the process operation cost is reduced.
The technical scheme of the invention is as follows:
CO in flue gas or synthetic gas2The removing method comprises the following steps:
CO2absorption: introducing the flue gas or synthetic gas into an absorption tower, contacting with absorption liquid in countercurrent for decarbonization, and removing CO from the discharged gas2Flue gas or synthesis gas, liquid phase being CO2Enriching liquid; wherein the absorption liquid is a phenol-containing organic amine solution obtained by extracting phenolic substances in coal tar or direct coal liquefaction oil by using an organic amine solution as an extracting agent;
and (3) phenol regeneration: in CO2Introducing excessive dioxygen into the enriched liquidBy conversion of carbon to CO2Further acidifying the enriched solution, standing the solution for layering to obtain crude phenol oil and CO2An organic amine solution;
CO2regeneration: introducing the CO into the reactor2Organic amine solution is heated for desorption, and CO released2CO partially used in phenol regeneration step2Acidifying the enriched liquid, and recycling the regenerated organic amine solution as an extracting agent for extracting phenolic substances in the coal tar or the direct coal liquefaction oil.
Preferably, CO2In the absorption step, the absorption liquid absorbs CO in the flue gas or the synthesis gas2The absorption temperature of (A) is 30-55 ℃.
Preferably, in the phenol regeneration step, CO2The acidification temperature of the enrichment liquid is 30-60 ℃.
Preferably, in CO2The molar ratio of the carbon dioxide absorbed in the absorption step to the organic amine is 0.01-2: at CO 12In the regeneration step, the CO is introduced2CO circulating in enriched liquor2The molar ratio of the amount to the organic amine is 0.01-2: 1.
preferably, CO2In the regeneration step, CO is contained2The temperature for heating and desorbing the organic amine solution is 120-150 ℃.
Preferably, the method is characterized in that CO2In the absorption step, the mass fraction of organic amine in the absorption liquid is 30-80%, the mass fraction of phenol is 15-40%, and the mass fraction of water is 5-30%.
Preferably, the organic amine is at least one of ethylenediamine, monoethanolamine, diethanolamine, triethanolamine, triethylamine and N-methyldiethanolamine.
The invention also provides CO in the flue gas or the synthesis gas2And a removing device. CO in the flue gas or syngas2The removing device comprises an extraction tower used for extracting phenolic substances in the coal tar or the direct coal liquefaction oil to obtain a phenol-containing organic amine solution; is connected with the extraction tower and takes the organic amine solution containing the phenol as an absorption liquid to absorb CO in flue gas or synthesis gas2The absorption tower of (4); is connected with the absorption tower and is used for discharging CO discharged by the absorption tower2The enrichment solution enters intoAcidifying, namely releasing phenolic substances contained in the phenol regeneration tower; the substance discharged from the phenol regeneration tower is statically separated to obtain crude phenol oil and CO-containing substance2A separator for the organic amine solution; connected to the separator and used for separating CO2Organic amine solution for CO2Regenerating the desorbed organic amine decarbonizing tower, introducing the regenerated carbon dioxide part into the phenol regenerating tower, and returning the regenerated organic amine solution serving as an extracting agent into the extracting tower.
Compared with the prior art, the method provided by the invention has the advantages that CO in the flue gas or the synthetic gas2The removing method and the device have the following beneficial effects:
CO in flue gas or synthesis gas2In the removal process, CO is absorbed2The absorption liquid is phenol-containing organic amine solution generated by extracting phenolic substances in coal tar or direct coal liquefaction oil by taking organic amine solution as an extracting agent to absorb CO2The later absorption liquid is sequentially subjected to phenol regeneration and CO2And in the regeneration process, the organic amine solution obtained by regeneration is used as an extracting agent for extracting phenolic substances in coal tar or direct coal liquefaction oil for recycling. Thereby extracting phenolic substances and CO from coal tar or direct coal liquefaction oil2The absorption and the combination of the two are integrated, so that the process operation cost is reduced; and CO in organic amine solution regeneration process2The desorption rate is high, the absorption effect of the regenerated absorption liquid is good, and the supplement amount of the organic amine solution is small.
Second, CO in flue gas or synthesis gas2In the removal process, the CO is removed2CO released after desorption of the organic amine solution2Part of the CO is used in the phenol regeneration process and can be completely replaced2The phenolic substances in the solution are enriched, the extraction rate of the phenolic substances is improved, the phenol content in the regenerated organic amine solution is reduced, and the efficiency of extracting the phenolic substances by the organic amine solution is further ensured.
Drawings
FIG. 1 shows CO in flue gas or syngas provided by the present invention2The structure of the removing device is shown schematically.
Detailed Description
The invention will be further explained with reference to the drawings and the embodiments.
Referring to FIG. 1, the invention provides a method for producing CO from flue gas or syngas2The structure of the removing device is shown schematically. CO in the flue gas or syngas2The removing device 100 comprises an extraction tower 11, an absorption tower 12, a phenol regeneration tower 13, a separator 14 and an organic amine decarbonization tower 15. Wherein:
the extraction tower 11 is used for extracting phenolic substances in coal tar or direct coal liquefaction oil, the raffinate phase is dephenolized oil, and the extract phase is organic amine solution containing phenol.
The absorption tower 12 is connected with the extraction tower 11, and an extraction phase in the extraction tower 11 is used as the absorption of CO in the absorption tower 122The absorbent solution of (1). Absorption of CO2The gas phase is then CO-depleted2Flue gas or synthesis gas, liquid phase being CO2Enriching the liquid.
The phenol regeneration tower 13 is connected to the absorption tower 12, and CO discharged from the absorption tower 122Introducing the enriched solution into the phenol regeneration tower 13, and continuously acidifying with carbon dioxide to make CO2The phenolic substances in the enrichment liquid are completely released.
The separator 14 is connected to the phenol regeneration column 13, CO2The enriched liquid flows into the separator 14 after being further acidified, and is kept stand and layered in the separator 14 to obtain crude phenol oil and CO2Organic amine solution.
The organic amine decarbonization tower 15 is connected with the separator 14 and contains CO2Discharging the organic amine solution into the organic amine decarbonizing tower 15, and carrying out CO treatment in the organic amine decarbonizing tower 152Regenerated, released CO2A portion of the recycle is introduced into the phenol regeneration column 13 for CO2The enriched liquid is further acidified, and one part of the enriched liquid is used for synthesizing urea or other purposes; the regenerated organic amine solution is returned to the extraction tower 11 as an extracting agent for recycling. Namely, CO released in the organic amine decarbonizing tower 152The device is divided into two branches, one branch is connected with the phenol regeneration tower 13, and carbon dioxide discharged from the other branch is used for urea synthesis or other purposes.
Wherein the flue gas has the main components of nitrogen, carbon dioxide, oxygen, water vapor and sulfides; the synthesis gas is composed mainly of hydrogen, carbon monoxide, carbon dioxide, methane and nitrogen. The phenolic compound is one or more of phenol, o-cresol, p-cresol, m-cresol, ethylphenol, diethylphenol, dimethylphenol and p-phenylphenol.
Based on CO in said flue gas or synthesis gas2The invention provides a removing device 100, and the invention provides CO in flue gas or synthesis gas2A method for removing.
The following examples illustrate the CO in flue gas or syngas provided by the present invention2The removal process is described in detail.
Example 1
CO in flue gas or synthetic gas2The removing method comprises the following steps:
step S1: CO 22Absorption of
Extracting phenolic substances in coal tar or direct coal liquefaction oil by taking an organic amine solution as an extracting agent to obtain an extract phase which is a phenol-containing organic amine solution; introducing the flue gas or the synthesis gas subjected to desulfurization, dedusting and cooling into the absorption tower 12, introducing the organic amine solution containing phenol into the absorption tower 12 as absorption liquid, carrying out decarburization treatment by countercurrent contact with the flue gas or the synthesis gas, wherein the discharged gas phase is CO removal2Flue gas or synthesis gas, liquid phase being CO2Enriching liquid;
specifically, the components in the organic amine solution containing phenol comprise organic amine, phenol and water, wherein the mass fraction of the organic amine is 30-80%, the mass fraction of the phenol is 15-40%, and the mass fraction of the water is 5-30%; the organic amine is at least one of ethylenediamine, monoethanolamine, diethanolamine, triethanolamine, triethylamine and N-methyldiethanolamine.
In this embodiment, the mass percentages of the components in the phenol-containing organic amine solution are: 60% of organic amine, 20% of phenol and 20% of water.
The distillation range of the coal tar or the direct coal liquefaction oil is 120-340 ℃, and the phenol content is 50.42%;
the extraction conditions were: the temperature is 25 ℃, and the reaction is carried out under the condition of normal pressure;
CO in flue gas or syngas2The content of (A) is 15%;
CO absorption by organic amine solution containing phenol2Conditions are as follows: the absorption temperature is 30 ℃, the gas-liquid flow ratio is 18:1, and the absorption is carried out under the normal pressure condition; the molar ratio of the absorbed carbon dioxide to the organic amine is 0.5;
step S2: phenol regeneration
In CO2Introducing excessive carbon dioxide into the enriched solution to make CO2Further acidifying the enriched solution, standing the solution for layering to obtain crude phenol oil and CO2An organic amine solution;
in particular, CO2The acidification temperature of the enrichment solution is 60 ℃;
step S3: CO 22Regeneration
Introducing the CO into the reactor2Organic amine solution is heated for desorption, and CO released2CO partially used in phenol regeneration step2Acidifying the enrichment liquid, and taking the regenerated organic amine solution as an extracting agent for extracting phenolic substances in coal tar or direct coal liquefaction oil;
in particular, containing CO2The temperature for heating and desorbing the organic amine solution is 120 ℃, and the pressure is normal pressure;
introducing the CO2CO circulating in enriched liquor2The molar ratio of the amount to the organic amine was 0.6.
With CO in the flue gas or syngas of example 12The removal method is based on the formation of CO in the flue gas or syngas of examples 2-9 by varying specific parameters2The specific conditions for the removal are shown in Table 1:
table 1: conditions for carrying out examples 2 to 9
The results of the tests of examples 1-9 were examined as shown in Table 2:
table 2: examples 1-9 test results data
| Purity of crude phenol oil | Yield of crude phenol oil | CO2Absorption rate | CO2Resolution ratio | |
| Example 1 | 95.37％ | 53.74％ | 99.9％ | 99.9％ |
| Example 2 | 95.84％ | 54.36％ | 98.85％ | 97.6％ |
| Example 3 | 96.21％ | 58.27％ | 99.6％ | 99.1％ |
| Example 4 | 96.78％ | 60.54％ | 94.2％ | 98.2％ |
| Example 5 | 95.78％ | 55.42％ | 88.6％ | 98.7％ |
| Example 6 | 96.53％ | 59.25％ | 85.4％ | 98.5％ |
| Example 7 | 95.84％ | 50.48％ | 98.85％ | 97.6％ |
| Example 8 | 96.21％ | 51.61％ | 99.6％ | 99.1％ |
| Example 9 | 96.78％ | 58.67％ | 94.2％ | 98.2％ |
It can be seen from the above test data that under the same extraction conditions, different absorption temperatures, gas-liquid flow ratios, and CO2Has a large influence on the absorption rate of (A), wherein CO is absorbed at an absorption temperature of 30-45 DEG C2The absorption rate of (A) is higher; and CO2In the regeneration process, the heating temperature is 120-150 ℃ to CO2The influence of the resolution ratio is small, which shows that organic amine solution is used as absorption liquid to absorb CO2After that, the desorption effect is good.
CO2In the absorption step, the solution containing organic amine phenol absorbs CO2While being coated with CO2Acidifying to release the phenol moiety; recycling the introduced CO during the phenol regeneration step2Facilitating further release displacement of the phenol. When CO is present2The molar ratio of carbon dioxide and organic amine absorbed in the absorption step is 0.8: 1, CO2In the regeneration step, CO is introduced2CO circulating in enriched liquor2The molar ratio of the amount to the organic amine is 0.4: 1, the yield of the crude phenol oil can be effectively improved; CO 22The acidification temperature of the enrichment liquid has certain influence on the yield of the crude phenol oil, and when the acidification temperature is 60 ℃, the corresponding yield of the crude phenol oil is higher than that when the acidification temperature is 30 ℃.
With CO in said flue gas or syngas of example 12The removal method is based on the above optimal technical parameters as quantification, and the concentration of the organic amine solution as an extracting agent is changed to further illustrate the concentration of the organic amine solution to CO2The effect of the stripping effect results in examples 10-14, as shown in Table 3.
It should be noted that: to facilitate detection of organic amine concentration vs. CO2The influence of the absorption rate is actually measured by the concentration of the organic amine in the absorption liquid in the present invention.
Table 3: conditions and test results for examples 10-14
As can be seen from the test data of examples 10 to 14, the organic amine concentrationTo CO2The absorption rate of the absorption rate and the yield of the crude phenol oil have great influence, and the optimal concentration of the organic amine solution in the absorption liquid is 60-80%.
Compared with the prior art, the method provided by the invention has the advantages that CO in the flue gas or the synthetic gas2The removing method and the device have the following beneficial effects:
CO in flue gas or synthesis gas2In the removal process, CO is absorbed2The absorption liquid is phenol-containing organic amine solution generated by extracting phenolic substances in coal tar or direct coal liquefaction oil by taking organic amine solution as an extracting agent to absorb CO2The later absorption liquid is sequentially subjected to phenol regeneration and CO2And in the regeneration process, the organic amine solution obtained by regeneration is used as an extracting agent for extracting phenolic substances in coal tar or direct coal liquefaction oil for recycling. Thereby extracting phenolic substances and CO from coal tar or direct coal liquefaction oil2The absorption and the combination of the two are integrated, so that the process operation cost is reduced; and CO in organic amine solution regeneration process2The desorption rate is high, the absorption effect of the regenerated absorption liquid is good, and the supplement amount of the organic amine solution is small.
Second, CO in flue gas or synthesis gas2In the removal process, the CO is removed2CO released after desorption of the organic amine solution2Part of the CO is used in the phenol regeneration process and can be completely replaced2The phenolic substances in the solution are enriched, the extraction rate of the phenolic substances is improved, the phenol content in the regenerated organic amine solution is reduced, and the efficiency of extracting the phenolic substances by the organic amine solution is further ensured.
The above description is only an embodiment of the present invention, and not intended to limit the scope of the present invention, and all modifications of equivalent structures and equivalent processes, which are made by using the contents of the present specification and the accompanying drawings, or directly or indirectly applied to other related technical fields, are included in the scope of the present invention.
Claims (8)
1. CO in flue gas or synthetic gas2The removing method is characterized by comprising the following steps:
CO2absorption: the smoke after being desulfurized, dedusted and cooledIntroducing the channel gas or synthetic gas into absorption tower, and performing decarburization treatment by countercurrent contact with absorption liquid to obtain CO-removed gas2Flue gas or synthesis gas, liquid phase being CO2Enriching liquid; wherein the absorption liquid is a phenol-containing organic amine solution obtained by extracting phenolic substances in coal tar or direct coal liquefaction oil by using an organic amine solution as an extracting agent;
and (3) phenol regeneration: in CO2Introducing excessive carbon dioxide into the enriched solution to make CO2Further acidifying the enriched solution, standing the solution for layering to obtain crude phenol oil and CO2An organic amine solution;
CO2regeneration: introducing the CO into the reactor2Organic amine solution is heated for desorption, and CO released2CO partially used in phenol regeneration step2Acidifying the enriched liquid, and recycling the regenerated organic amine solution as an extracting agent for extracting phenolic substances in the coal tar or the direct coal liquefaction oil.
2. Flue gas or syngas CO according to claim 12The method of removing CO is characterized in that2In the absorption step, the absorption liquid absorbs CO in the flue gas or the synthesis gas2The absorption temperature of (A) is 30-55 ℃.
3. Flue gas or syngas CO according to claim 12Characterized in that, in the phenol regeneration step, CO is removed2The acidification temperature of the enrichment liquid is 30-60 ℃.
4. Flue gas or syngas CO according to claim 12A process for the removal of CO from a gas stream2The molar ratio of the carbon dioxide absorbed in the absorption step to the organic amine is 0.01-2: at CO 12In the regeneration step, the CO is introduced2CO circulating in enriched liquor2The molar ratio of the amount to the organic amine is 0.01-2: 1.
5. flue gas or syngas CO according to claim 12The method of removing CO is characterized in that2In the regeneration step, containCO2The temperature for heating and desorbing the organic amine solution is 120-150 ℃.
6. Flue gas or syngas CO according to any of claims 1-52The method of removing CO is characterized in that2In the absorption step, the mass fraction of organic amine in the absorption liquid is 30-80%, the mass fraction of phenol is 15-40%, and the mass fraction of water is 5-30%.
7. Flue gas or syngas CO according to claim 62The removing method is characterized in that the organic amine is at least one of ethylenediamine, monoethanolamine, diethanolamine, triethanolamine, triethylamine and N-methyldiethanolamine.
8. CO in flue gas or synthetic gas2The removing device is characterized by comprising an extraction tower for extracting phenolic substances in coal tar or coal direct liquefaction oil to obtain a phenolic organic amine solution; is connected with the extraction tower and takes the organic amine solution containing the phenol as an absorption liquid to absorb CO in flue gas or synthesis gas2The absorption tower of (4); is connected with the absorption tower and is used for discharging CO discharged by the absorption tower2A phenol regeneration tower for further acidifying the enriched liquid and releasing phenolic substances contained in the enriched liquid; the substance discharged from the phenol regeneration tower is statically separated to obtain crude phenol oil and CO-containing substance2A separator for the organic amine solution; connected to the separator and used for separating CO2Organic amine solution for CO2Regenerating the desorbed organic amine decarbonizing tower, introducing the regenerated carbon dioxide part into the phenol regenerating tower, and returning the regenerated organic amine solution serving as an extracting agent into the extracting tower.
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Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101143805A (en) * | 2006-09-15 | 2008-03-19 | 中国石油化工股份有限公司 | Method for separating phenols compounds from phenol-containing raw material oil |
| CN101417200A (en) * | 2007-10-22 | 2009-04-29 | 辽河石油勘探局 | Carbon dioxide, nitrogen gas recovering method in boiler flue gas |
| WO2010037109A3 (en) * | 2008-09-29 | 2010-05-27 | Akermin, Inc. | Process for accelerated capture of carbon dioxide |
| CN101804264A (en) * | 2010-05-12 | 2010-08-18 | 中冶东方工程技术有限公司 | Treatment method of industrial waste acid |
| CN102241453A (en) * | 2010-09-25 | 2011-11-16 | 仲恺农业工程学院 | Method for treating coal gasification wastewater containing phenol and ammonia |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101143805A (en) * | 2006-09-15 | 2008-03-19 | 中国石油化工股份有限公司 | Method for separating phenols compounds from phenol-containing raw material oil |
| CN101417200A (en) * | 2007-10-22 | 2009-04-29 | 辽河石油勘探局 | Carbon dioxide, nitrogen gas recovering method in boiler flue gas |
| WO2010037109A3 (en) * | 2008-09-29 | 2010-05-27 | Akermin, Inc. | Process for accelerated capture of carbon dioxide |
| CN101804264A (en) * | 2010-05-12 | 2010-08-18 | 中冶东方工程技术有限公司 | Treatment method of industrial waste acid |
| CN102241453A (en) * | 2010-09-25 | 2011-11-16 | 仲恺农业工程学院 | Method for treating coal gasification wastewater containing phenol and ammonia |
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