KR101406711B1 - Carbon dioxide separation method using mixture of solvent - Google Patents
Carbon dioxide separation method using mixture of solvent Download PDFInfo
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 176
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 88
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 88
- 239000002904 solvent Substances 0.000 title abstract description 54
- 238000000926 separation method Methods 0.000 title abstract description 4
- 239000000203 mixture Substances 0.000 title description 5
- 238000000034 method Methods 0.000 claims abstract description 62
- 238000010521 absorption reaction Methods 0.000 claims abstract description 60
- 239000012046 mixed solvent Substances 0.000 claims abstract description 44
- 238000001704 evaporation Methods 0.000 claims abstract description 5
- WYTZZXDRDKSJID-UHFFFAOYSA-N (3-aminopropyl)triethoxysilane Chemical compound CCO[Si](OCC)(OCC)CCCN WYTZZXDRDKSJID-UHFFFAOYSA-N 0.000 claims description 21
- 238000006243 chemical reaction Methods 0.000 claims description 12
- 239000007864 aqueous solution Substances 0.000 claims description 7
- 239000006096 absorbing agent Substances 0.000 claims description 5
- 238000010438 heat treatment Methods 0.000 claims description 2
- 230000008569 process Effects 0.000 abstract description 38
- FZHAPNGMFPVSLP-UHFFFAOYSA-N silanamine Chemical group [SiH3]N FZHAPNGMFPVSLP-UHFFFAOYSA-N 0.000 abstract description 24
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 abstract description 2
- 229910052799 carbon Inorganic materials 0.000 abstract description 2
- 238000011112 process operation Methods 0.000 abstract description 2
- 239000007789 gas Substances 0.000 description 27
- 239000000126 substance Substances 0.000 description 25
- 230000002745 absorbent Effects 0.000 description 9
- 239000002250 absorbent Substances 0.000 description 9
- 230000002378 acidificating effect Effects 0.000 description 9
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 8
- XTHFKEDIFFGKHM-UHFFFAOYSA-N Dimethoxyethane Chemical compound COCCOC XTHFKEDIFFGKHM-UHFFFAOYSA-N 0.000 description 7
- 239000002253 acid Substances 0.000 description 7
- 230000008901 benefit Effects 0.000 description 6
- 230000008859 change Effects 0.000 description 6
- 230000000694 effects Effects 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 125000003277 amino group Chemical group 0.000 description 3
- 238000007086 side reaction Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- HZAXFHJVJLSVMW-UHFFFAOYSA-N 2-Aminoethan-1-ol Chemical compound NCCO HZAXFHJVJLSVMW-UHFFFAOYSA-N 0.000 description 2
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 2
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- 229910002808 Si–O–Si Inorganic materials 0.000 description 2
- -1 amine compound Chemical class 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 229910002091 carbon monoxide Inorganic materials 0.000 description 2
- 238000001816 cooling Methods 0.000 description 2
- 230000007797 corrosion Effects 0.000 description 2
- 238000005260 corrosion Methods 0.000 description 2
- LVTYICIALWPMFW-UHFFFAOYSA-N diisopropanolamine Chemical compound CC(O)CNCC(C)O LVTYICIALWPMFW-UHFFFAOYSA-N 0.000 description 2
- 229940043276 diisopropanolamine Drugs 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 239000007788 liquid Substances 0.000 description 2
- CRVGTESFCCXCTH-UHFFFAOYSA-N methyl diethanolamine Chemical compound OCCN(C)CCO CRVGTESFCCXCTH-UHFFFAOYSA-N 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 125000004430 oxygen atom Chemical class O* 0.000 description 2
- 230000009257 reactivity Effects 0.000 description 2
- 230000008929 regeneration Effects 0.000 description 2
- 238000011069 regeneration method Methods 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 238000003786 synthesis reaction Methods 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- JCVAWLVWQDNEGS-UHFFFAOYSA-N 1-(2-hydroxypropylamino)propan-2-ol;thiolane 1,1-dioxide;hydrate Chemical group O.O=S1(=O)CCCC1.CC(O)CNCC(C)O JCVAWLVWQDNEGS-UHFFFAOYSA-N 0.000 description 1
- TUGGFUSCPLPUFY-UHFFFAOYSA-N 3-triethoxysilylpropan-1-amine Chemical compound CCO[Si](OCC)(OCC)CCCN.CCO[Si](OCC)(OCC)CCCN TUGGFUSCPLPUFY-UHFFFAOYSA-N 0.000 description 1
- RWSOTUBLDIXVET-UHFFFAOYSA-N Dihydrogen sulfide Chemical compound S RWSOTUBLDIXVET-UHFFFAOYSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 150000001299 aldehydes Chemical class 0.000 description 1
- 150000001335 aliphatic alkanes Chemical class 0.000 description 1
- 150000001413 amino acids Chemical class 0.000 description 1
- 238000009835 boiling Methods 0.000 description 1
- 150000001720 carbohydrates Chemical class 0.000 description 1
- 235000014633 carbohydrates Nutrition 0.000 description 1
- 239000003034 coal gas Substances 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 238000004332 deodorization Methods 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- 230000018109 developmental process Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000007613 environmental effect Effects 0.000 description 1
- 239000003546 flue gas Substances 0.000 description 1
- 230000008570 general process Effects 0.000 description 1
- 159000000011 group IA salts Chemical class 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910000037 hydrogen sulfide Inorganic materials 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 239000003112 inhibitor Substances 0.000 description 1
- 150000002576 ketones Chemical class 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000009149 molecular binding Effects 0.000 description 1
- 238000006386 neutralization reaction Methods 0.000 description 1
- 239000012074 organic phase Substances 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- 230000000704 physical effect Effects 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 230000001172 regenerating effect Effects 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 239000011550 stock solution Substances 0.000 description 1
- HXJUTPCZVOIRIF-UHFFFAOYSA-N sulfolane Chemical compound O=S1(=O)CCCC1 HXJUTPCZVOIRIF-UHFFFAOYSA-N 0.000 description 1
- 239000011593 sulfur Substances 0.000 description 1
- 229930195735 unsaturated hydrocarbon Natural products 0.000 description 1
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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
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
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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
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/96—Regeneration, reactivation or recycling of reactants
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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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- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Health & Medical Sciences (AREA)
- Biomedical Technology (AREA)
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Abstract
Description
본 발명은 혼합용매를 이용하여 이산화탄소를 분리하는 방법에 관한 것으로, 보다 상세하게는 흡수탑과 탈거탑을 포함하는 이산화탄소 분리 장치에서 혼합용매로 아미노 실란계를 이용하는 방법에 관한 것이다.
The present invention relates to a method of separating carbon dioxide using a mixed solvent, and more particularly, to a method of using aminosilane as a mixed solvent in a carbon dioxide separator including an absorption tower and a stripping column.
산업 공정에서 가스 상에 존재하는 산성가스 (Acid Gas) 제거공정은 다양하게 개발되어 석유화학 및 발전계통에 이용되고 있으며 각 공정은 사용 용매에 따라서 화학 용매 공정, 물리 용매 공정, 혼합 화학/물리 용매 공정, 직접 전환 공정 등으로 나누어진다. Acid gas removal processes that exist in the gas phase in industrial processes have been developed in various ways and are used in petrochemical and power generation systems. Each process is divided into chemical solvent process, physical solvent process, mixed chemical / physical solvent Process, and direct conversion process.
물리용매공정의 대표적인 예는 Selexol공정으로 유기용매를 이용하여 고압의 석탄가스에서 산성가스를 물리적으로 흡수시킨다. 즉 화학반응이 개입되지 않으므로 열이나 압력감소, 가스 Stripping 등의 방법으로 용매를 재생시킨다. A typical example of a physical solvent process is the Selexol process, which uses organic solvents to physically absorb acid gases in high pressure coal gas. That is, the chemical reaction is not intervened, so the solvent is regenerated by heat, pressure reduction, gas stripping and the like.
화학용매공정은 메틸디에탄올아민(MDEA, Methyldiethanolamine)과 같은 아민류 화합물과 산성가스와의 화학반응을 이용하는 공정으로 알칼리성염 수용액이 용매로 사용된다. 아민용매의 재생은 열이나 증기를 가하여 H2S, CO2를 제거한다. The chemical solvent process uses a chemical reaction between an amine compound such as methyldiethanolamine (MDEA) and an acidic gas, and an alkaline salt aqueous solution is used as a solvent. Regeneration of the amine solvent removes H 2 S and CO 2 by applying heat or steam.
또한, 혼합용매공정은 물리용매와 화학용매를 혼합사용하는 공정으로, 예를 들어, 산성가스를 설포레인(Sulfolane)에 물리적으로 흡수시킴과 동시에 디이소프로파놀아민(DIPA, Diisopropanolamine)에 화학적으로 흡수시키는 원리를 이용한다. 특히 이러한 혼합용매는 고압의 강산성가스를 처리하는데 적합하며 대표적인 예는 셸(Shel)사가 개발한 가스 중 탄산가스, 황화수소 제거법인 설피놀(Sulfinol) 공정이다. In addition, the mixed solvent process is a process in which a physical solvent and a chemical solvent are used in combination. For example, the acidic gas is physically absorbed into sulfolane and the diisopropanolamine (DIPA) The principle of chemical absorption is used. Particularly, these mixed solvents are suitable for treatment of high-pressure strongly acidic gas. Representative example is Sulfinol process which is carbon dioxide gas and hydrogen sulfide removal method developed by Shel.
물리 흡수 공정은 산성가스 용해도가 높은 유기용매에 물리적으로 산성가스를 흡착시켜 제거하는 방식으로 산성가스의 분압이 높을수록 보다 많은 양의 산성가스가 제거된다. 따라서 산성가스의 분압이 높은 경우 (76psi 이상)에는 물리 용매공정이 화학용매 공정보다 훨씬 유리하다. 그러나 물리용매 공정의 흡수탑 운전온도는 화학용매 공정보다 낮기 때문에 냉각에너지가 많이 요구된다. 따라서 공급가스중의 산성가스 분압이 낮아도 계통의 운전 온도가 상당히 낮을 경우 (약 -60℃정도) 물리용매 공정이 경제적으로 우수한 경우가 종종 나타난다. 대표적인 물리용매 공정으로는 메탄올을 사용하는 렉티솔(Rectisol) 공정과 디메틸에테르를 사용하는 셀렉솔(Selexol) 공정이 있다. 물리 용매공정의 경우 장치설비를 위한 투자비용이 높고, 흡수제 재생을 위한 압력손실과정에서 오는 고비용 등이 꾸준히 문제점으로 지적되어 왔다. In the physical absorption process, an acidic gas is physically adsorbed to an organic solvent having a high acidic gas solubility and is removed. The higher the partial pressure of the acidic gas, the more acidic gas is removed. Therefore, the physical solvent process is more advantageous than the chemical solvent process when the partial pressure of acid gas is high (76psi or more). However, since the absorption tower operation temperature of the physical solvent process is lower than that of the chemical solvent process, a large amount of cooling energy is required. Therefore, even if the partial pressure of the acid gas in the feed gas is low, the physical solvent process is often economically superior when the operating temperature of the system is considerably low (about -60 ° C). Representative physical solvent processes include the Rectisol process using methanol and the Selexol process using dimethyl ether. The physical solvent process has been pointed out as a problem with a high investment cost for the equipment and a high cost coming from the pressure loss process for regenerating the absorbent.
이에 비해, 모노에탄올아민(MEA, monoethanolamine)으로 대표되는 화학 용매공정의 경우, 물리용매 공정에 비해 상대적으로 초기 투자비가 저렴하며, 빠른 반응속도, 높은 흡수능, 낮은 분자량 등의 장점을 가지고 있다. 그러나 흡수제로 인한 장치 부식의 문제가 상존하며 배가스 내의 여러 부가스와의 부반응문제가 초기부터 꾸준히 존재 하였다. 최근의 연구는 이러한 단점을 상쇄 개선하기 위한 연구에 초점이 맞추어져 있으며, 그러한 노력의 일환으로 화학 용매의 반응성을 낮추는 반응 억제제(inhibator)와 반대로 반응을 더욱 향상시키는 첨가제(promotor)등의 개발이 이루어지고 있다. 이에 따른 반대급부로 이산화탄소 분리 회수 시 부반응과 높은 증기압으로 인한 휘발이 환경적인 위해를 야기하기도 한다. 이러한 단점이 있지만 화학적 흡수법은 정유공정 등에서 오랜 기간 광범위하게 응용되고 있다. In contrast, the chemical solvent process represented by monoethanolamine (MEA) has advantages such as relatively low initial investment cost as compared with the physical solvent process, fast reaction rate, high absorption capacity and low molecular weight. However, there is a problem of corrosion of the device due to the absorbent, and the side reaction problems of various gases in the flue gas have been present from the beginning. Recent studies have focused on studies to improve the offset of these disadvantages. As part of such efforts, the development of inhibitors that lower the reactivity of chemical solvents and the promoters that further improve the reaction . As a countermeasure, volatilization due to the side reaction and high vapor pressure during the recovery of carbon dioxide may cause environmental harm. Although these drawbacks exist, the chemical absorption method has been widely used for a long time in the refining process and the like.
물리 용매는 산성가스 제거 시 고압 저온 상태를 유지해야 하므로 이로 인해 용매의 냉각 비용이 많이 소요되는 단점을 갖고 있다. 화학 용매의 경우는 화학 결합된 산성가스를 제거하는데 많은 재생에너지가 필요하고, 특히 고압에서 산성가스를 제거할 때 높은 휘발도로 인해 안전에 큰 문제점을 갖고 있다. 높은 휘발도는 보충해야할 용매의 양도 증가시키므로 경제성이 떨어지는 단점을 갖고 있다.The physical solvent has a disadvantage in that the cooling cost of the solvent is high because the high-pressure and low-temperature state must be maintained when the acid gas is removed. In the case of chemical solvents, a large amount of renewable energy is required to remove chemically bonded acidic gases, and particularly, there is a serious problem in safety due to high volatility when removing acidic gas at high pressure. The high volatility increases the amount of the solvent to be supplemented, which is disadvantageous in that the economical efficiency is low.
대한민국 공개특허 10-2011-0129848은 기체혼합물을 탈산하는 방법 및 시스템에 관한 기술을 개시하고 있으며, 이산화탄소를 물리적 및 화학적으로 흡수하는 유기상 전달매질로 알칸, 불포화탄화수소, 알코올, 글리콜, 에테르, 알데히드, 케톤, 탄수화물, 아민, 알칸올아민, 아미노산 등을 포함한다. 그러나 상기 용매의 경우 물리적 특징이 우수하면 화학적 특징이 열등하고, 반대로 화학적 특징이 우수할 경우 물리적 특징이 열위에 오는 문제가 있다. 따라서 한 용매가 물리 용매와 화학 용매의 장점을 갖추면서 특히 산성가스 중 이산화탄소 제거 능력이 우수한 용매를 이용한 이산화탄소 분리, 제거 방법의 개발이 요구된다.
Korean Patent Laid-open Publication No. 10-2011-0129848 discloses a technique and system for deoxidizing a gas mixture, which comprises an organic phase transfer medium for physically and chemically absorbing carbon dioxide, an alkane, an unsaturated hydrocarbon, an alcohol, a glycol, an ether, an aldehyde, Ketones, carbohydrates, amines, alkanolamines, amino acids and the like. However, in the case of the above solvent, when the physical property is excellent, the chemical characteristic is inferior, and when the chemical characteristic is excellent, there is a problem that the physical characteristic is inferior. Therefore, it is required to develop a method of separating and removing carbon dioxide using a solvent having excellent ability to remove carbon dioxide from an acid gas while one solvent has advantages of a physical solvent and a chemical solvent.
본 발명은 상기와 같은 문제점을 감안하여 안출된 것으로, 물리용매의 장점과 화학흡수의 장점을 고루 가지도록, 고압 공정에서 낮은 휘발성을 가지는 혼합용매를 사용하여 이산화탄소가 함유된 혼합가스로부터 이산화탄소를 분리하는 방법을 제공하고자 한다.
SUMMARY OF THE INVENTION The present invention has been made in view of the above problems, and it is an object of the present invention to separate carbon dioxide from a mixed gas containing carbon dioxide by using a mixed solvent having low volatility in a high pressure process so as to have the advantages of physical solvents and advantages of chemical absorption .
상기 과제를 해결하기 위하여, 본 발명자들은 액상 원액을 사용하는 대신 수용액 상태의 아미노 실란 용매를 종래의 연속식 이산화탄소 분리공정에 적용하면, 물리적 및 화학적 흡수제의 장점을 모두 얻을 수 있음을 발견하여 본 발명을 완성하였다. In order to solve the above problems, the present inventors have found that the advantages of the physical and chemical absorbents can be obtained by applying the aminosilane solvent in the aqueous solution state to the conventional continuous carbon dioxide separation process instead of using the liquid raw stock solution, .
본 발명은 혼합용매를 이용하여 이산화탄소를 분리하는 방법으로, 이산화탄소 혼합용매를 흡수탑의 상부로 공급하고 상기 흡수탑의 하부로 이산화탄소가 함유된 혼합가스를 도입하여 혼합가스에 함유된 이산화탄소를 혼합용매에 흡수시키는 단계; 상기 이산화탄소가 흡수된 혼합용매를 재증발 탱크(flash tank)로 보내고 압력차를 이용해 이산화탄소를 탈거시키는 단계; 및 상기 재증발 탱크를 통과한 혼합용매를 탈거탑으로 보내고 가열하여 이산화탄소를 탈거시키는 단계를 포함하고, 상기 혼합용매는 아미노실란(Amino silane)계인, 혼합용매를 이용하여 이산화탄소를 분리하는 방법을 제공한다.
The present invention relates to a method for separating carbon dioxide using a mixed solvent, comprising the steps of supplying a carbon dioxide mixed solvent to an upper part of an absorption tower, introducing a carbon dioxide-containing mixed gas into the lower part of the absorption tower, ; Sending the mixed solvent in which the carbon dioxide has been absorbed to a flash tank and removing carbon dioxide using a pressure difference; And discharging the mixed solvent having passed through the re-evaporation tank to the deodorization tower and heating the mixture to remove carbon dioxide. The mixed solvent is a method of separating carbon dioxide using an aminosilane-based mixed solvent do.
본 발명은 또한, 상기 혼합용매는 30 wt% 아미노프로필트리에톡시실란 (Aminoprorpyltriethoxysilane, APTS) 수용액인, 혼합용매를 이용하여 이산화탄소를 분리하는 방법을 제공한다.
The present invention also provides a method for separating carbon dioxide using a mixed solvent, which is an aqueous solution of 30 wt% aminopropyltriethoxysilane (APTS).
본 발명은 또한, 상기 흡수탑의 반응 온도는 -10℃ 내지 40℃인, 혼합용매를 이용하여 이산화탄소를 분리하는 방법을 제공한다.
The present invention also provides a method for separating carbon dioxide using a mixed solvent, wherein the reaction temperature of the absorption tower is -10 ° C to 40 ° C.
본 발명은 또한, 상기 흡수탑의 반응 압력은 1bat 내지 20bar인, 혼합용매를 이용하여 이산화탄소를 분리하는 방법을 제공한다.
The present invention also provides a method for separating carbon dioxide using a mixed solvent, wherein the reaction pressure of the absorber is from 1 to 20 bar.
본 발명의 아미노 실란 용매는 기존 상용의 용매와 비교하여, 높은 이산화탄소 흡수 성능 및 제거 효율로 인해 공정 적용시 포집비용을 절감할 수 있다. 또한 휘발도가 낮아 공정 운전 시 안전성 및 경제성이 우수하다.The aminosilane solvent of the present invention can reduce the collection cost in process application due to high carbon dioxide absorption performance and removal efficiency as compared with conventional commercial solvents. In addition, it has low volatility and is excellent in safety and economy in process operation.
또한, 수분 존재 하에서도 부반응을 일으키지 않아, 화학적인 안정성이 높으며, 화학 용매와는 달리 장치 부식을 야기하지 않음으로 공정 적용상의 큰 장점을 가진다.
In addition, it does not cause side reactions even in the presence of water, has high chemical stability, and has a great advantage in process application because it does not cause device corrosion, unlike chemical solvents.
도 1은 본 발명의 아미노 실란계 혼합용매인 Aminopropyltriethoxysilane의 화학 구조를 나타내는 도면이다.
도 2는 본 발명의 연속식 이산화탄소 제거공정의 개요를 나타내는 도면이다.
도 3은 본 발명의 온도 변화에 따른 아미노 실란계 혼합용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능을 나타내는 그래프이다.
도 4는 20℃에서 압력 변화에 따른 아미노 실란계 혼합용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능을 나타내는 그래프이다.
도 5는 40℃에서 압력 변화에 따른 아미노 실란계 혼합용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능을 나타내는 그래프이다.1 is a view showing the chemical structure of aminopropyltriethoxysilane which is an aminosilane-based mixed solvent of the present invention.
2 is a diagram showing an outline of the continuous carbon dioxide removing step of the present invention.
FIG. 3 is a graph showing carbon dioxide absorption performance of aminopropyltriethoxysilane, which is an aminosilane-based mixed solvent according to the temperature change of the present invention.
4 is a graph showing carbon dioxide absorption performance of Aminopropyltriethoxysilane, which is an aminosilane-based mixed solvent, at 20 ° C.
5 is a graph showing carbon dioxide absorption performance of aminopropyltriethoxysilane, which is an aminosilane-based mixed solvent, at 40 ° C.
이하에서, 본 발명에 따른 이산화탄소가 함유된 혼합가스로부터 이산화탄소를 분리하는 방법을 상세하게 설명한다. 본 발명은 아미노 실란계 용매, 특히 Aminopropyltriethoxysilane를 이산화탄소 혼합용매로 사용하여 이산화탄소를 분리하는 방법에 관한 것이다. Hereinafter, a method for separating carbon dioxide from a gas mixture containing carbon dioxide according to the present invention will be described in detail. The present invention relates to a method for separating carbon dioxide using an aminosilane-based solvent, particularly Aminopropyltriethoxysilane, as a carbon dioxide-based solvent.
기존 산성가스 특히 이산화탄소 흡수 용매의 단점은 액상 원액을 사용하며, 물리 화학적 흡수 중 선택적으로 작용하는 것이므로, 본 발명에서는 혼합용매를 사용하여 물리적 흡수와 화학적 흡수를 동시에 수행하도록 하여 흡수능을 향상시킨다. 본 발명의 일 구현예에서, 상기 혼합용매로 아미노 실란을 선택하고 그 사용은 수용액 상태로 기존의 연속식 이산화탄소 제거공정에 적용한다.The disadvantage of the conventional acid gas, particularly the carbon dioxide absorption solvent, is that the liquid raw stock is used and selectively acts on the physicochemical absorption. Therefore, the present invention improves the absorption ability by simultaneously performing physical absorption and chemical absorption using a mixed solvent. In one embodiment of the present invention, the aminosilane is selected as the mixed solvent and its use is applied to an existing continuous carbon dioxide removal process in the form of an aqueous solution.
도 2에 연속식 이산화탄소 제거공정의 개요를 나타내었다. 이는 일반적인 공정에 관한 것으로 The Dow Chemical Company의 Sidney F. Bosen박사가 전자통신회선(http://www.dow.com/PublishedLiterature/dh_0119/0901b80380119094.pdf)에 공개한 "Causes of Amine Plant Corrosion-Design Considerations" 자료를 참조하였다. 이산화탄소를 포함하는 합성가스(syngas)를 탈황장치(desulfurizer)에 통과시켜 황을 제거하고, 증기(steam)와 가열기(heater)를 이용해 가온한 뒤 전환반응기(shift reactor)에 통과시켜 합성가스 중에 포함된 일산화탄소를 수소와 이산화탄소로 전환한다. 상기 전환과정을 거친 합성가스는 냉각기(cooler)에서 온도를 낮춰준 뒤 흡수탑(absorber) 하부로 주입하여 흡수탑 상부에서 내려오는 혼합용매와 접촉하여 이산화탄소가 상기 혼합용매에 흡수되도록 하고, 수소 기체는 흡수탑을 통해 배출시킨다. Fig. 2 shows an outline of the continuous carbon dioxide removal process. This is related to a general process and is described by Dr Sidney F. Bosen of The Dow Chemical Company in Causes of Amine Plant Corrosion-Design (http://www.dow.com/PublishedLiterature/dh_0119/0901b80380119094.pdf) Considerations ". The synthesis gas (syngas) containing carbon dioxide is passed through a desulfurizer to remove sulfur, heated with steam and a heater, passed through a shift reactor, Carbon monoxide to hydrogen and carbon dioxide. The synthesis gas having undergone the conversion process is lowered in temperature by a cooler and then injected into the lower part of the absorber to be contacted with a mixed solvent coming down from the upper part of the absorption tower so that carbon dioxide is absorbed into the mixed solvent, Is discharged through the absorption tower.
상기 흡수탑은 고압을 유지하여 혼합용매가 화학적 흡수와 함께 고압 환경에서 물리적 흡수를 진행하도록 한다. 이와 같이 이산화탄소를 흡수한 혼합용매는 이산화탄소 흡수 혼합용액이 되어 재증발 탱크(Flash Tank)로 주입되어 급격하게 압력이 낮추어지게 된다. 상기 재증발 탱크에서 압력차에 의해 혼합용매에 물리적으로 흡수되어 되어 있던 이산화탄소가 분리된다. 물리흡수 이산화탄소를 제거한 흡수 혼합용액은 가열기(heater)를 통과시켜 온도를 높인 뒤 탈거탑으로 주입되고, 탈거탑의 재가열기(reboiler)에서 끓여 재생시킨다. 고온에서 혼합용매에 화학적으로 결합되어 있던 이산화탄소를 분리시킨 뒤 재생된 상기 혼합용매는 냉각기(cooler)를 거쳐서 다시 흡수탑으로 주입된다. 상기 냉각기를 거친 뒤 흡수탑에 주입되는 과정에서 재증발기에서 재생된 혼합용매가 일부 더해지며, 냉각기를 거친 뒤에도 상대적으로 온도가 높기 때문에 흡수탑에서 이산화탄소를 흡수하여 재증발기로 주입되는 흡수 혼합용액과 열교환기(Heat Exchanger)를 통해 열을 교환하여 에너지를 절감한다. The absorber maintains a high pressure to allow the mixed solvent to conduct physical absorption in a high pressure environment with chemical absorption. The mixed solvent absorbing the carbon dioxide becomes a carbon dioxide absorbing mixed solution and injected into the flash tank, so that the pressure is suddenly lowered. The carbon dioxide which has been physically absorbed in the mixed solvent is separated by the pressure difference in the re-evaporation tank. Physical absorption The absorbing mixed solution from which carbon dioxide is removed is injected into a deck tower after passing through a heater to increase the temperature, and boiled and regenerated from the reboiler of the deck. After the carbon dioxide chemically bound to the mixed solvent is separated at a high temperature, the regenerated mixed solvent is injected into the absorption tower again through a cooler. In the process of being injected into the absorption tower after passing through the cooler, some of the mixed solvent regenerated in the evaporator is added. Since the temperature is relatively high even after passing through the cooler, the absorption mixture solution absorbed in the absorption tower and injected into the re- Heat is exchanged through a heat exchanger to save energy.
본 발명의 아미노실란의 물리 용매로서의 작용을 살펴보면, 도 1의 아미노실란 구조에서 보는 바와 같이 oxysilane은 비교 대상인 ether에 비해 전하 분리가 확연히 크다. 이는 CO2 분자와 분자간 결합을 하는 oxysilane의 산소 원자 Mulliken charge가 거의 -1에 가까워 ether의 산소 원자 Mulliken charge값 -0.5에 비해 크기 때문에 CO2와 oxysilane의 분자간 결합 에너지가 CO2와 ether의 분자간 결합에너지에 비해 크기 때문이다. Si-O-Si 결합을 보이는 oxysilane의 분자구조가 이산화탄소와 물리적인 결합이 클 것으로 예상되기 때문에 이로 인해 CO2 흡수능이 증대되는 것으로 판단된다. 또한 이러한 구조는 분자 내의 원자단의 공간적 배열이 분자 반응성에 미치는 효과인 입체장애 효과가 크기 때문에, 재생할 때 결합된 이산화탄소가 쉽게 떨어지는 효과가 있다. As shown in the aminosilane structure of FIG. 1, the oxysilane has a markedly higher charge separation than the ether to which it is compared, as a physical solvent of the aminosilane of the present invention. This oxygen atom Mulliken charge is almost close to -1, because the oxygen atoms of the intermolecular bonding size than the Mulliken charge value is -0.5 molecular binding energy of the CO 2 and CO 2 oxysilane ether and the ether to the oxysilane to intermolecular bond and CO 2 molecules Because it is larger than energy. The molecular structure of oxysilane, which shows Si-O-Si bond, is predicted to have a strong physical bond with carbon dioxide, which leads to an increase in CO 2 absorption capacity. Furthermore, this structure has a large effect of steric hindrance, which is the effect of the spatial arrangement of atomic groups in the molecule on the molecular reactivity, so that the combined carbon dioxide is easily dropped when regenerated.
화학 용매로서의 작용을 살펴보면, 아미노실란은 분자 구조 내에 아미노기(-NH2)를 가지고 있다. 이와 같은 아미노기는 이산화탄소와 직접 반응하거나 산-염기 중화반응에 의하여 이온성 중간체를 생성하는 화학반응에 의하여 이산화탄소의 물질 전달을 증진시키는 역할을 한다. 이러한 아미노기의 역할을 원활하게 해 주기 위해서는 물이 필요하다. 따라서 본 발명의 일 구현예에서는 물과 아미노실란을 혼합하여 사용한다.Looking at the action as a chemical solvent, aminosilane has an amino group (-NH 2 ) in its molecular structure. Such an amino group promotes the mass transfer of carbon dioxide by a chemical reaction which directly reacts with carbon dioxide or generates an ionic intermediate by an acid-base neutralization reaction. Water is needed to facilitate the role of these amino groups. Therefore, water and aminosilane are mixed in one embodiment of the present invention.
또한 아미노실란은 Si-O-Si 구조를 갖고 있어 잘 휘발이 되지 않아 물리 또는 화학 재생 시 안전성과 경제적인 측면에서 유리하다.Also, aminosilane has a Si-O-Si structure and is not well volatilized, which is advantageous in terms of safety and economy in physical or chemical regeneration.
기존 흡수제가 가지는 수용액 상태에서의 사용상의 문제점과 물리 화학적 흡수의 선택적 적용에 따른 흡수능 저하 문제를 해결하기 위하여, 아미노 실란계 용매를 적용함으로써 기존 물리 또는 화학 용매의 문제점을 해결함과 동시에 높은 수준의 이산화탄소 흡수 효율을 제공하고자 하였다. 아미노 실란계 흡수 용매는 끓는점이 217℃ 이상이고, 분자량이 220 g/mol 이상이다. In order to solve the problem of the use of the conventional absorbent in the aqueous solution state and the problem of the lowering of the absorption ability due to the selective application of the physicochemical absorption, the problem of the existing physical or chemical solvent is solved by applying the aminosilane- And to provide carbon dioxide absorption efficiency. The aminosilane-based absorption solvent has a boiling point of 217 ° C or higher and a molecular weight of 220 g / mol or higher.
본 발명에서는 아미노 실란계 용매를 이산화탄소 흡수 용매에 새로이 적용하였으며, 이때의 이산화탄소 흡수 효과를 기존 물리 용매인 Selexol, Purisol과 비교함으로써, 아미노 실란계 흡수 용매의 이산화탄소 흡수성능을 확인하였다. 하기 실시예는 다양한 온도와 압력의 운전 조건에서, 아미노 실란계 흡수 용매와 기존 물리 용매간의 이산화탄소 흡수 효과를 비교하였다.
In the present invention, an aminosilane-based solvent was newly applied to a carbon dioxide-absorbing solvent, and the carbon dioxide absorption performance of the aminosilane-based absorption solvent was confirmed by comparing the carbon dioxide absorption effect at this time with the existing physical solvents Selexol and Purisol. The following example compares the carbon dioxide absorption effect between an aminosilane-based absorption solvent and a conventional physical solvent under various conditions of temperature and pressure.
[실시예 1] 온도변화에 따른 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능 변화[Example 1] Carbon dioxide absorption performance of aminopropyltriethoxysilane according to temperature change
온도 변화에 따른 아미노 실란계 용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능 변화를 도 3에 나타내었다. 닫힌 반응기안에 아미노 실란계 용매인 Aminopropyltriethoxysilane 30 wt% 수용액 9.5ml를 주입한 후, 순도 99.99%의 이산화탄소를 직접 접촉시켜 이산화탄소 흡수 성능을 실험하였다. 실험은 압력을 고정하고, 온도에 변화를 주며 3회 반복 실험하여 데이터의 신뢰성을 확보하였다. 공정상의 온도는 -10도~40℃ 범위로 가정하였으며, 실험 시 압력은 연소전 압력조건을 가정하여 10 bar 조건에서 모사하였다. 주입된 이산화탄소의 양은 모두 취합하여 최종 적산하였으며, 이렇게 얻어진 결과치에 공실험(blank) 결과치를 보정하여 용매의 최종적인 이산화탄소 흡수성능을 계산하였다. 반응기는 닫힌계이므로 반응기안의 흡수제가 이산화탄소 흡수성능이 크다면 주입되는 이산화탄소의 양이 증가하게 되며, 이 때의 결과를 항상 동일한 값을 가지는 공실험 결과에 감산하여 최종 이산화탄소 흡수량을 계산하였다. 이렇게 얻어진 최종적인 이산화탄소 흡수성능을 각 용매의 몰수를 고려하여 표준화하였다. 동일한 과정으로 Selexol과 Purisol의 이산화탄소 흡수성능을 계산하였다. 상호 비교 결과, 아미노 실란계 용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수성능은 -10도~40℃의 전 실험구간에서 Selexol과 Purisol을 상회하는 가장 높은 이산화탄소 흡수 성능을 나타내었다. 가장 높은 이산화탄소 흡수능은 -10℃, 10bar 조건일 때 2.91 mol CO2/mol absorbent로 확인되었으며, Purisol대비 227%의 이산화탄소 흡수 성능 증가를 확인하였다.
FIG. 3 shows changes in carbon dioxide absorption performance of aminopropyltriethoxysilane, which is an aminosilane-based solvent, according to temperature change. In the closed reactor, 9.5 ml of Aminopropyltriethoxysilane 30 wt% aqueous solution was injected. Experiments were carried out three times by fixing the pressure, changing the temperature, and ensuring the reliability of the data. The temperature of the process is assumed to be in the range of -10 to 40 ℃. The pressure during the experiment was simulated under the pre-combustion pressure condition at 10 bar. The amounts of injected carbon dioxide were all collected and finally added. The final carbon dioxide absorbing performance of the solvent was calculated by correcting the blank results of the obtained results. Since the reactor is a closed system, the amount of carbon dioxide injected increases when the absorber in the reactor has a high carbon dioxide absorption capacity. The result is always subtracted from the experimental results having the same value to calculate the final carbon dioxide absorption amount. The final carbon dioxide absorption performance thus obtained was standardized in consideration of the number of moles of each solvent. The carbon dioxide absorption capacity of Selexol and Purisol was calculated by the same procedure. As a result of the mutual comparison, the absorption capacity of aminopropyltriethoxysilane, the aminopropyltriethoxysilane, showed the highest carbon dioxide absorption performance over Selexol and Purisol in the entire experimental range from -10 ° C to 40 ° C. The highest carbon dioxide absorption capacity was confirmed to be 2.91 mol CO 2 / mol absorbent at -10 ° C and 10 bar, and 227% increase in carbon dioxide absorption performance compared to Purisol.
[실시예 2] 압력변화에 따른 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능 변화(운전 온도 20 ℃)[Example 2] Carbon dioxide absorption performance of aminopropyltriethoxysilane according to pressure change (operation temperature: 20 ° C)
반응기 온도를 20℃로 고정한 상태에서 압력을 변화시키며(1, 10, 20 bar) 공정을 모사한 내용을 도 4에 나타내었다. 대상이 된 Selexol, Purisol과 마찬가지로 아미노 실란계 용매인 Aminopropyltriethoxysilane도 압력의 증가에 따라서 흡수능이 동반하여 증가하는 것을 확인하였다. 특히 일반적인 이산화탄소 제거 공정 조건인 상압(1 bar)조건에서, 아미노 실란계 용매인 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능은 알카놀 아민계 물리 흡수제인 Selexol 대비 10.91배, Purisol 대비 18.71배의 매우 높은 이산화탄소 흡수 성능을 확인하였다. FIG. 4 shows the results of simulating the process of varying the pressure (1, 10, 20 bar) with the reactor temperature being fixed at 20 ° C. Aminopropyltriethoxysilane (Aminopropyltriethoxysilane), as well as Selexol and Purisol, were found to increase with increasing pressure. In particular, under the normal atmospheric pressure (1 bar) condition, which is a common carbon dioxide removal process condition, Aminopropyltriethoxysilane, an aminopropyltriethoxysilane, exhibits a very high carbon dioxide absorption performance of 10.91 times as compared with Seloxol as an alkanolamine-based physical absorbent and 18.71 times as much as Purisol Respectively.
이때의 이산화탄소 흡수 성능은 1.31 mol CO2/mol absorbent였으며, 압력의 증가에 따라 더불어 상승하여 20bar조건에서 2.75mol CO2/mol absorbent로 증가하였다.
At this time, the carbon dioxide absorption performance was 1.31 mol CO 2 / mol absorbent, which increased with increasing pressure and increased to 2.75 mol CO 2 / mol absorbent at 20 bar.
[실시예 3] 압력변화에 따른 Aminopropyltriethoxysilane의 이산화탄소 흡수 성능 변화 (운전 온도 40 ℃) [Example 3] Carbon dioxide absorption performance change of aminopropyltriethoxysilane according to pressure change (operation temperature: 40 ° C)
반응기 온도를 40℃로 고정하고 압력을 변화시키며(1, 10, 20bar) 공정을 모사한 내용을 도 5에 나타내었다. 그 결과 상압조건에서 아미노 실란계 용매인 Aminopropyltriethoxysilane의 흡수 성능은 Selexol대비 13.18배, Purisol대비 29배의 이산화탄소 흡수 성능 향상을 확인하였다. The reactor temperature was fixed at 40 ° C, the pressure was varied (1, 10, 20 bar) and the process was simulated. As a result, the absorption performance of aminopropyltriethoxysilane, which is an aminosilane solvent at atmospheric pressure, was 13.18 times higher than Selexol and 29 times higher than Purisol.
40 조건에서 아미노 실란계 용매인 Aminopropyltriethoxysilane이 가장 높은 이산화탄소 흡수성능을 나타내는 압력 조건은 20bar조건이며, 3.11 mol CO2/mol absorbent 값을 확인하였다.
Aminopropyltriethoxysilane (Aminopropyltriethoxysilane) showed the highest carbon dioxide absorption performance under the condition of 20 bar and 3.11 mol CO 2 / mol absorbent.
Claims (4)
이산화탄소 혼합용매를 흡수탑의 상부로 공급하고 상기 흡수탑의 하부로 이산화탄소가 함유된 혼합가스를 도입하여 혼합가스에 함유된 이산화탄소를 혼합용매에 흡수시키는 단계;
상기 이산화탄소가 흡수된 혼합용매를 재증발 탱크(flash tank)로 보내고 압력차를 이용해 이산화탄소를 탈거시키는 단계; 및
상기 재증발 탱크를 통과한 혼합용매를 탈거탑으로 보내고 가열하여 이산화탄소를 탈거시키는 단계를 포함하고,
상기 혼합용매는 30 wt% 아미노프로필트리에톡시실란 (Aminoprorpyltriethoxysilane, APTS) 수용액인,
혼합용매를 이용하여 이산화탄소를 분리하는 방법.
As a method for separating carbon dioxide using a mixed solvent,
Supplying a mixed gas of carbon dioxide to the upper part of the absorption tower and introducing a mixed gas containing carbon dioxide into the lower part of the absorption tower to absorb carbon dioxide contained in the mixed gas into the mixed solvent;
Sending the mixed solvent in which the carbon dioxide has been absorbed to a flash tank and removing carbon dioxide using a pressure difference; And
And transferring the mixed solvent having passed through the re-evaporation tank to a de-stripping tower and heating to remove carbon dioxide,
The mixed solvent was an aqueous solution of 30 wt% aminopropyltriethoxysilane (APTS)
A method for separating carbon dioxide using a mixed solvent.
상기 흡수탑의 반응 온도는 -10℃ 내지 40℃인,
혼합용매를 이용하여 이산화탄소를 분리하는 방법.
The method according to claim 1,
Wherein the reaction tower has a reaction temperature of -10 캜 to 40 캜,
A method for separating carbon dioxide using a mixed solvent.
상기 흡수탑의 반응 압력은 1bar 내지 20bar인,
혼합용매를 이용하여 이산화탄소를 분리하는 방법.
The method according to claim 1,
The reaction pressure of the absorber is from 1 bar to 20 bar,
A method for separating carbon dioxide using a mixed solvent.
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