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WO2003035221A1 - Procede de production de dioxyde de carbone liquide a partir de gaz de combustion a pression normale - Google Patents

Procede de production de dioxyde de carbone liquide a partir de gaz de combustion a pression normale Download PDF

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Publication number
WO2003035221A1
WO2003035221A1 PCT/FI2002/000814 FI0200814W WO03035221A1 WO 2003035221 A1 WO2003035221 A1 WO 2003035221A1 FI 0200814 W FI0200814 W FI 0200814W WO 03035221 A1 WO03035221 A1 WO 03035221A1
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WO
WIPO (PCT)
Prior art keywords
column
absorption
desorption
concentrate
pressure
Prior art date
Application number
PCT/FI2002/000814
Other languages
English (en)
Inventor
Matti Nurmia
Original Assignee
Cuycha Innovation Oy
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Cuycha Innovation Oy filed Critical Cuycha Innovation Oy
Priority to EP02801921A priority Critical patent/EP1450933A1/fr
Priority to US10/491,857 priority patent/US20040237528A1/en
Publication of WO2003035221A1 publication Critical patent/WO2003035221A1/fr

Links

Classifications

    • 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
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/62—Carbon oxides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/50—Carbon dioxide
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2

Definitions

  • the present invention relates to a process for producing liquid carbon dioxide (C0 2 ) from combustion gas at normal pressure, in which process :
  • the C0 2 is desorbed from the absorption solution led to the upper part of the desorption column to form a gaseous C0 2 concentrate, which is removed from the upper part as the said absorption solution flows to the lower part of the column, from which it is recirculated to the upper part of the said absorption column,
  • One known technique of separating C0 2 from combustion gases is represented by the MEA method, which is disclosed in the publications DE-549556 and DE-606132, among others.
  • the C0 2 is absorbed from the combustion gas into a water solution of monoethylamine (MEA) or other amines. After absorption, the solution is heated to, for example, 120°C and the C0 2 dissolved in it is desorbed at a pressure of about 2 bar.
  • MEA monoethylamine
  • Patent application PCT/FI01/00629 discloses a thermodynamically advantageous method for separating C0 2 from combustion gas. This method exploits the fact that the solubility of C0 2 in, for example, methanol close to its condensation point deviates strongly from Henry's Law. The method works best when the partial pressure of the C0 2 is several bars and, for precisely this reason, is particularly suitable for gas-turbine cycles and other processes in which the pressurization of the combus- tion gas can be used to produce energy.
  • Publication DE-843 545 discloses a process where blast-furnace gas with a C0 2 content of 24 % boosted to a pressure of 2 , 5 bar and scrubbed with ethanol at a temperature of -74 - -67°C.
  • the C0 2 solution obtained is evaporated in two stages at pressures of 0,2 and 0,04 bar, in the same temperature range.
  • the C0 2 obtained at the pressure of 0,2 bar is led to the booster through a regenerator, but the fraction obtained at 0,04 bar is boosted as such, its pressure being too low for a normal regenerator process.
  • the deficit in cooling effect that arises and the rest of the cooling power requirement is covered by expanding the gas fraction, exhausted from the scrubbing process, in a cooling turbine.
  • the present invention is intended to create a process, in which C0 2 can be liquified from normal-pressure combustion gas and by means of which the aforementioned defects can be eliminated.
  • the characteristic features of the process according to the invention are stated in Claim 1.
  • the deviation of the absorption/desorption process from reversibility can be reduced advantageously by using air scavenging in the desorption stage, allowing the air accumulated in the C0 2 concentrate to be used in the liquidization of the C0 2 by exploiting the pressure energy of the remaining waste gas in the liquidization.
  • Cooling is not required in the absorption/desorption process according to the invention, because the processes are carried out chemically in a temperature range advantageous to the process, instead of solution and evaporation taking place in cryogenic temperature conditions. Consequently, the viscosity of the absorption solution is less than one tenth of the viscosity of the solution used in the process of the aforementioned DE publication. The low viscosity of the absorption solution makes thermal and mass transfer more efficient and the circulation of the solution requires less energy.
  • the process according to the invention does not require chemicals that are expensive, volatile, or liable to oxidation.
  • Other advantages achieved through the process according to the invention are itemized in the description section.
  • Figure 1 shows a schematic diagram of one process according to the invention
  • Figure 2 shows a schematic diagram of another embodiment of the process .
  • Figure 1 shows one basic solution of the process according to the invention, in which air scavenging is used advantageously in the desorption stage.
  • the separation unit 10 shown in the left-hand half of this figure comprises an absorption column 11 and a desorption column 12, which are thermally connected to each other to arrange thermal transfer, in the same structure.
  • the absorption and desorption processes are carried out chemically in an advantageous temperature range of 35 - 75°C, which corresponds to the temperature of the combustion gas being brought to the process.
  • the temperature of the desorption column 12 is 2 - 5°C lower than that of the absorption column
  • Combustion gas at normal pressure is brought to the lower part of the absorption column 11, from where is flows upwards against an absorption solution, which absorbs the C0 2 in the combustion gas, and which is brought to the upper part of the column 11 and flows along the column structures (not shown) .
  • a suitable absorption solution is a 2-N water solution of, for example, potassium or sodium carbonate.
  • the relevant compounds are non-volatile and non-oxidizing. In the temperature range referred to, the said solutions have a low viscosity (1,0 - 0,55 cP) , so that thermal and mass transfer take place efficiently and the circulation of the solution requires only a little energy.
  • the C0 2 -rich absorption solution is led from the lower part of the absorption column 11 to the lower part of the desorption column 12, in which, beneath the surface of the absorption solution, a heat exchanger 16 is arranged, in which the absorption solution that has been brought from the lower part of the column 11 transfers heat to the solution in the bottom of the column 12 and desorbs C0 2 from it.
  • the absorption solution is led to the upper part of the desorption column 12, from which it flows downwards along structures (not shown) arranged in the column
  • a pressure of about 0,2 bar prevails, and, according to one preferred embodiment of the invention, scavenging air is led to the lower part of it and flows through the absorption solution in the bottom of the column 12 and rises against the downwards flowing absorption solution in the column.
  • the air flow is used to maintain a constant pressure in the column 12, the partial pressure of the C0 2 being, at each height in the column 12, more or less in equilibrium with the composition of the absorption solution at the same height.
  • the C0 2 released from the solution evaporates into the scavenging air.
  • C0 2 concentrate exhausts from the upper part of the column 12 at a lower pressure than normal, and has a C0 2 concentration of 50 - 55 %, and is led through a steam condenser 13 to be pressurized in a booster-intercooler 14 and from there on to the liquidization process 15.
  • the C0 2 -poor absorption solution that accumulates at the bottom of the column 12 is transferred by a pump 17 back to the absorption column 11, to bind C0 2 .
  • the C0 2 concentrate which has been pressurized, for example, to 100 bar, in the booster-intercooler 14, is taken to the lower part of a liquidization column 18.
  • the C0 2 concentrate flows upwards while the C0 2 liquidizes on the surface of heat exchangers 19.1, 19.2, 19.3, 19.4 arranged in series in the column 18.
  • the liquidized C0 2 is led out of the bottom of the column 18, to be transported farther away, or for other use.
  • the unliquidized waste gas is led from the top of the column 18, through a cooling pipe or group of pipes 19.1 acting as a heat exchanger, to a first cooling turbine 20.1, in which it loses part of its pressure energy. From the cooling turbine 20.1, the cycle continues in a similar manner to a cooling pipe 19.2.
  • the cooling-expansion cycle is repeated in the turbines 20.2, 20.3 and in the heat exchangers 19.3, 19.4, until the pressure of the waste gas has dropped to 1 bar, when it is removed from the cooling-expansion cycle 24 from the lower part 5 of the last hear exchanger 19.4.
  • the heat exchangers 19.1, 19.2, 19.3 19.4 are arranged in the liquidization column 18 in such a way that their temperature levels are essentially set to equal each other and their cooling effect is concentrated in the lower part of the column 18.
  • the cooling turbines 20.1, 10 20.2, 20.3 are connected to a generator 21, or to some other device, in order to exploit the mechanical energy they produce.
  • the C0 2 is liquidized at, for example, a pressure of 100 bar, in a temperature range of +15 - -40°C, the unliquidized waste
  • the combustion gas being processed is often warm (60 - 90°C) , its heat can be exploited by carrying out the absorption and desorption at such a high temperature that the pressure of the water vapour of the combustion gas will have a substantial effect on the process. If, in this second preferred embodiment of the process according to the invention, the temperature of the desorption column 12 is, for example 62,5°C, then the water evaporating from the absorption solution will then maintain a partial pressure of 0,22 bar of the water vapour in it.
  • the total pressure of the C0 2 concentrate at 62,5°C will be 0,42 bar, taking into account the partial pressure of the water vapour. If there is 0,02 bar of water vapour in the C0 2 concentrate after the condenser 13, then its total pressure will still be 0,42 bar, of which 0,2 bar is C0 2 and another 0,2 bar is air. In other words, the partial pressures of the C0 2 and the air double, thus reducing the size and energy requirements of the boosters needed to pressurize the C0 2 .
  • the thermal energy required to evaporate the water in the desorption column 12 can be extracted from the combustion gas in the absorption column 11.
  • Bled steam (not shown) at 0,5 bar, for example, can also be introduced to the desorption column 12.
  • a third embodiment according to the invention shown in Figure 2, instead of the double column shown in Figure 1 there are two separate columns 11' and 12'.
  • a from the cooling cycle 24 separate water- cooled pre-condenser 22, which is close to the inlet connection 27 of the C0 2 concentrate, is located in the lower part of the liquidization column 18.
  • cold ( ⁇ 6°C) cooling water is available from the sea or deep lakes, and in winter from other waterways too. If a temperature of 10°C is maintained in the pre-condenser 22, and the partial pressure in the C0 2 concentrate is 60 bar (the concentrate having, for example, a pressure of 110 bar and a 55 % C0 2 content) , then about 25 % of the C0 2 will liquidize in the pre- condenser 22, the cooling effect required being correspondingly reduced.
  • an additional absorption column 23 in which the C0 2 -rich solution coming from the lower part of the first absorption column 11' absorbs additional C0 2 from the waste gas coming from the cooling cycle 24 of the liquidization, is located at a suitable pressure in the cooling cycle 24 of the liquidization. This increases the C0 2 partial pressure of the concentrate obtained from desorption, while simultaneously returning a considerable part of the waste-gas C0 2 to the liquidization process 15. The impoverished waste gas is returned to the cooling cycle 24 of the liquidization process 15 from the upper part of the column 23.
  • Part of the waste gas of the liquidization can also be led at a suitable pressure to an ejector in connection with the evaporation column 12 ' , in order to raise the pressure of the C0 2 concentrate and to reduce the size of the boosters 14 required.
  • a fourth embodiment of the invention very little or no scavenging air is used, so that the concentrate created in the desorption column 12 is nearly pure C0 2 and most of it can be liquidized at a pressure of 100 bar by water cooling.
  • the separation efficiency without air scavenging would be 67 % .
  • C0 2 pressurized to 100 bar is led to the liquidization column 18, in which it is liquidized in a water-cooled liquidizer (not shown) filling the entire column 18. If there are other gases as impurities in the concentrate, then, when the temperature of the liquidizer (not shown) is 15°C, there will be 50 % C0 2 in the gas exiting from the top of the column 18. If this C0 2 loss is detrimentally large, then the C0 2 is recovered by means of the liquidizing column described in the embodiment shown in Figure 1, the cooling power required by which is produced by expanding the waste gas exhausting from the column 18 in the cooling turbines 20.1, 20.2, 20.3, 20.4.
  • the conditions of the process such as the pressurizing of the C0 2 and the content of the C0 2 concentrate, can be preferably selected so that the cooling power requirement of the liquidization process can be precisely covered using the pressure energy of the unliquidized waste gas of the process and other process-related sources of cooling power.
  • the energy consumption of the process per kilogram of liquidized C0 2 is then brought close to its minimum value.
  • liquidization process according to the invention is its use in connection with oxygen combustion.
  • This embodiment lacks the absorption and desorption cycles described, because in oxygen or oxygen concentrate combustion the C0 2 can be liquidized from the combustion gas without enrichment.
  • One example of this is the liquidization of C0 2 from the pressurized combustion gas of a Vartan-type PFBC power plant.
  • the C0 2 content of the combustion gas is ⁇ 50 %, it is preferable to extend the liquidization to close to the triple point of C0 2 (-56,5°C, 5,1 bar), so that its loss to the waste gas is made small. If the C0 2 content is 30 % and its liquidization pressure is 100 bar, then in the temperature range -5 - -52,5°C about 81 % of the C0 2 will liquidize. In this case, only part of the waste gas pressure energy remaining from the liquidization will be needed to produce the cooling power and there will be only 1 - 2 cooling turbines in the cooling cycle.
  • the waste gas flow exhausting at excess pressure from the cooling cycle is heated, for example, in the process's heat exchanger, before it is led to a separate turbine to produce energy .
  • the nitrogen oxides (NO x s) in the combustion gas in the process according to the present invention are absorbed in the absorption solution and are converted there into nitrate ions.
  • the nitrate ions can be easily separated from the absorption solution as nitrates at the same time as the cations leaving it are replaced with corresponding hydroxides. This gives a degree of freedom in the power plant's combustion, as there is no need to attempt to minimize the N0 X content of the combustion gas. Because nitrates are considerably more valuable that hydroxides, it can even be economically advantageous to attempt to achieve large NO x contents in the combustion gas .

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Biomedical Technology (AREA)
  • Treating Waste Gases (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Gas Separation By Absorption (AREA)

Abstract

La présente invention concerne un procédé de production de dioxyde de carbone liquide (CO2) à partir de gaz de combustion à pression normale. Dans ledit procédé, le CO2 de gaz de combustion amené vers la partie inférieure d'une colonne d'absorption (11) est absorbé dans une solution d'absorption qui s'écoule vers l'aval par rapport à sa partie supérieure, le gaz de combustion pauvre en CO2 est éliminé de la partie supérieure de la colonne d'absorption (11), ladite solution d'absorption est amenée vers la partie supérieure d'une colonne de désorption (12), le CO2 est désorbé de la solution d'absorption amenée vers la partie supérieure de la colonne de désorption (12) pour former un concentré de CO2 gazeux, lequel est éliminé de la partie supérieure lorsque la solution d'absorption s'écoule vers la partie inférieure de la colonne (12), à partir de laquelle elle est recyclée vers la partie supérieure de la colonne d'absorption (11), le concentré de CO2 obtenu est mis sous haute pression, et la majeure partie du CO2 du concentré est liquéfiée. Dans ledit procédé, le CO2 est transféré du gaz de combustion à pression normale, à l'aide d'un procédé d'absorption et de désorption presque réversible, vers le concentré de CO2 à une pression inférieure, à une température proche de celle du gaz de combustion traité, de préférence dans la plage de températures comprise entre 35 et 75 °C, de sorte que les procédés d'absorption et de désorption se produisent dans les colonnes (11,12) à plus ou moins la même température, de préférence sans importation de chaleur externe dans lesdits procédés.
PCT/FI2002/000814 2001-10-22 2002-10-21 Procede de production de dioxyde de carbone liquide a partir de gaz de combustion a pression normale WO2003035221A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP02801921A EP1450933A1 (fr) 2001-10-22 2002-10-21 Procede de production de dioxyde de carbone liquide a partir de gaz de combustion a pression normale
US10/491,857 US20040237528A1 (en) 2001-10-22 2002-10-21 Process for producing liquid carbon dioxide from combustion gas at normal pressure

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FI20015028A FI111607B (fi) 2001-10-22 2001-10-22 Prosessi nestemäisen hiilidioksidin tuottamiseksi normaalipaineisesta savukaasusta
FI20015028 2001-10-22

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WO2003035221A1 true WO2003035221A1 (fr) 2003-05-01

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US (1) US20040237528A1 (fr)
EP (1) EP1450933A1 (fr)
FI (1) FI111607B (fr)
WO (1) WO2003035221A1 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2005087351A1 (fr) * 2004-03-18 2005-09-22 Cuycha Innovation Oy Procede quasi-reversible de separation de dioxyde de carbone d'un gaz de combustion ou gaz produit
WO2006037323A1 (fr) 2004-10-08 2006-04-13 Union Engineering A/S Procede pour recuperer du dioxyde de carbone a partir d'un gaz
RU2495707C2 (ru) * 2009-01-28 2013-10-20 Сименс Акциенгезелльшафт Способ и устройство для отделения диоксида углерода от отходящего газа работающей на ископаемом топливе электростанции

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CA2686969C (fr) * 2007-05-11 2017-01-31 Co2Crc Technologies Pty Ltd Reacteur, installation et procede
AR068841A1 (es) * 2007-10-12 2009-12-09 Union Engeneering As Remocion de dioxido de carbono de un gas de alimentacion
EP2333256B1 (fr) * 2009-12-08 2013-10-16 Alstom Technology Ltd Centrale électrique dotée de capture de CO2 et son procédé d'opération

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WO2000048709A1 (fr) * 1999-02-19 2000-08-24 Norsk Hydro Asa Technique d'elimination et de recuperation du co2 de gaz d'echappement
US6228145B1 (en) * 1996-07-31 2001-05-08 Kvaerner Asa Method for removing carbon dioxide from gases
WO2002004098A1 (fr) * 2000-07-11 2002-01-17 Nurmia, Wendie Procede de separation de dioxyde de carbone (co2) d'un gaz a combustion

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US6228145B1 (en) * 1996-07-31 2001-05-08 Kvaerner Asa Method for removing carbon dioxide from gases
WO2000048709A1 (fr) * 1999-02-19 2000-08-24 Norsk Hydro Asa Technique d'elimination et de recuperation du co2 de gaz d'echappement
CN1261545A (zh) * 1999-12-06 2000-08-02 重庆理想科技有限公司 一种从混合气体中回收co2的方法
WO2002004098A1 (fr) * 2000-07-11 2002-01-17 Nurmia, Wendie Procede de separation de dioxyde de carbone (co2) d'un gaz a combustion

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Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2005087351A1 (fr) * 2004-03-18 2005-09-22 Cuycha Innovation Oy Procede quasi-reversible de separation de dioxyde de carbone d'un gaz de combustion ou gaz produit
WO2006037323A1 (fr) 2004-10-08 2006-04-13 Union Engineering A/S Procede pour recuperer du dioxyde de carbone a partir d'un gaz
WO2006037320A1 (fr) * 2004-10-08 2006-04-13 Union Engineering A/S Procede de recuperation de dioxyde de carbone a partir d'un gaz
JP2008515757A (ja) * 2004-10-08 2008-05-15 ユニオン、エンジニアリング、アクティーゼルスカブ ガスから二酸化炭素を回収する方法
AU2005291723B2 (en) * 2004-10-08 2009-03-19 Union Engineering A/S Method for recovery of carbon dioxide from a gas
EA011604B1 (ru) * 2004-10-08 2009-04-28 Юнион Инджиниринг А/С Способ извлечения диоксида углерода из газа
KR101196015B1 (ko) 2004-10-08 2012-10-30 유니온 엔지니어링 아/에스 가스로부터 이산화탄소를 회수하는 방법
US8475566B2 (en) 2004-10-08 2013-07-02 Union Engineering A/S Method for recovery of carbon dioxide from a gas
RU2495707C2 (ru) * 2009-01-28 2013-10-20 Сименс Акциенгезелльшафт Способ и устройство для отделения диоксида углерода от отходящего газа работающей на ископаемом топливе электростанции

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Publication number Publication date
FI111607B (fi) 2003-08-29
FI20015028A0 (fi) 2001-10-22
EP1450933A1 (fr) 2004-09-01
FI20015028L (fi) 2003-04-23
US20040237528A1 (en) 2004-12-02

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