WO2010037825A1 - Amines - Google Patents

Amines Download PDF

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Publication number
WO2010037825A1
WO2010037825A1 PCT/EP2009/062776 EP2009062776W WO2010037825A1 WO 2010037825 A1 WO2010037825 A1 WO 2010037825A1 EP 2009062776 W EP2009062776 W EP 2009062776W WO 2010037825 A1 WO2010037825 A1 WO 2010037825A1
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WO
WIPO (PCT)
Prior art keywords
absorbent
mea
concentration
weight
gas
Prior art date
Application number
PCT/EP2009/062776
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English (en)
Inventor
Thor Mejdell
Karl Anders Hoff
Olav Juliussen
Hallvard F. Svendsen
Andrew Tobiesen
Terje Vassbotn
Original Assignee
Aker Solvent As
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 Aker Solvent As filed Critical Aker Solvent As
Priority to EP09736584A priority Critical patent/EP2349533A1/fr
Publication of WO2010037825A1 publication Critical patent/WO2010037825A1/fr

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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
    • B01D53/1493—Selection of liquid materials for use as absorbents
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2257/00—Components to be removed
    • B01D2257/50—Carbon oxides
    • B01D2257/504—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

Definitions

  • the present invention relates to an improved method for capturing of CO2 from a combustion gas, and to an improved amine absorbent for CO 2 .
  • Capture of CO 2 from a mixture of gases in an industrial scale has been known for decades, i.e. for separation of natural gas and CO 2 from sub terrain gas wells to give natural gas for export and CO 2 for return to the sub terrain structure.
  • Industrial CO 2 capturing plants include an absorber, in which a liquid absorbent is brought into countercurrent contact with the gas to be treated.
  • a "purified" or low CO 2 gas is withdrawn at the top of the absorber and is released into the atmosphere, whereas a CO 2 rich absorbent is withdrawn from the bottom of the absorber.
  • the rich absorbent is regenerated in a regeneration column where the rich absorbent is stripped by countercurrent flow with steam that is generated by heating of regenerated absorbent at the bottom of the regeneration column.
  • the regenerated absorbent is withdrawn from the bottom of the regeneration column and is recycled into the absorber.
  • a CO 2 rich gas mainly comprising steam and CO 2 is withdrawn from the top of the regeneration column.
  • the CO 2 rich gas is treated further to remove water, and compressed before the CO2 is sent for deposition or other use.
  • Capture of CO 2 is, however, an energy demanding process, as the binding of CC> 2 to the absorbent is an exothermal reaction and the regeneration is an endothermal reaction. Accordingly, heat is lost in the absorber and heat is to be added to the regeneration column to regenerate the absorbent and release the CO 2 .
  • This heat demand is a major operating cost for a plant for CO 2 capture. A reduction of the heat requirement for regeneration of the absorbent is therefore sought to reduce the energy cost for the CO 2 capture.
  • Amines having a less exothermic reaction when absorbing CO 2 do normally have slower reaction kinetics and will thus require a longer contact time between the CO 2 containing gas and the absorbent. A longer contact time will require a larger absorber for the same gas volume.
  • amines and combinations have been suggested as absorbents for CO 2 , the different amines having CO 2 absorption capabilities, see e.g. the above mentioned patents.
  • suggested amines for the aqueous solutions to be used as absorbents are alkanolamines such as e.g. monoethanol amine (MEA), diethanol amine (DEA) , triethanol amine, dimethyldiethanolamine, diisopropanol amine, diglycol amine, methyl monoethanol amine (MMEA), 2- amino-2-methyl-1-propanole (AMP).
  • MEA is also commonly used as a reference absorbent in tests for possible new absorbents.
  • reaction kinetics, heat demand, heat of reaction, amine equilibrium loading, degradation, stability, solubility in water and absorption capacity of the different amines are of interest when selecting a potential absorbent for industrial scale CO 2 capture.
  • the objective of the present invention is to provide an improved absorbent and an improved method for capturing of CO 2 from a CO 2 containing gas, where the improved absorbents has improved characteristics compared with the prior used absorbents, such as exemplified with the MEA reference absorbent. Specifically, it is an object to provide an absorbent having a lower energy demand for regeneration of the absorbent, at the same time as acceptable reaction kinetics and absorption capacity is obtained. It is also an object to provide a method for use of the new absorbent. Summary of the invention
  • the present invention relates to an aqueous CO2 absorbent comprising a combination of a sterically hindered amine and a monoalkanolamine, wherein the concentration of the sterically hindered amine is from 10 to 35 % by weight and the concentration of the monoalkanolamine is from 10 to 35 % by weight.
  • the sterically hindered amine is, according to one embodiment, 2-amino-2-methyl-1-propanol (AMP).
  • the monoalkanolamine is methyl monoethanolamine (MMEA) or monoethanolamine (MEA)
  • the invention relates to a process for removing CO 2 from a CO2-containing gas, comprising the step of bringing the CO 2 - containing gas in contact with an aqueous solution of a sterically hindered amine, and a monoalkanolamine, where the concentration of the sterically hindered amine is from 10 to 35 % by weight and the concentration of the monoalkanolamine is from 10 to 35 % by weight.
  • the sterically hindered amine is, according to one embodiment, 2-amino-2-methyl-1-propanol (AMP).
  • the monoalkanolamine is methylmonoethanolamine (MMEA) or monoethanolamine (MEA).
  • Figure 1 is a graph illustrating reaction rate as a function of concentration of CO 2 for different CO 2 absorbents
  • Figure 2 is a graph illustrating absorption rate versus loading for different absorbents
  • Figure 3 is a graph illustrating desorption rate versus loading for different absorbents
  • Figure 4 is a graph illustrating desorption rate versus concentration for different absorbents
  • Figure 5 is a graph illustrating absorption rate in lean loading versus net absorption capacity for different absorbents
  • Figure 6 is a graph illustrating equilibrium data for 30 % by weight of MEA at different temperatures
  • Figure 7 is a principle drawing of a pilot plant used for testing absorbents
  • Figure 8a and b illustrates loading and gas inlet concentration of CO 2 , respectively, for different runs
  • Figure 9 is a graph illustrating the results for the specific reboiler duty versus loading.
  • the present invention relates to an improved amine absorbent for CO 2 capture and a method for capturing CO 2 using the improved amine absorbent.
  • the invention is based on mixing two different amines having different reaction kinetics, one being a sterically hindered amine, such as e.g. 2-amino-2-methyl-1- propanol (AMP) and the other being a monoalkanolamine, such as e.g. methyl monoethanolamine (MMEA) or monoethanolamine (MEA).
  • a sterically hindered amine such as e.g. 2-amino-2-methyl-1- propanol (AMP)
  • MMEA methyl monoethanolamine
  • MEA monoethanolamine
  • AMP being a sterically hindered amine
  • the slow reaction kinetics have a negative impact in the absorber as it requires a longer contact time between the CO 2 containing gas and the absorbent in the absorber.
  • MMEA and MEA at the other side are known to have high energy requirement but faster reaction kinetics.
  • an aqueous CO 2 absorbent comprising from 10 to 35 % by weight of a sterically hindered amine and from 10 to 35 % by weight of a monoalkanolamine has a substantially lower energy requirement than the industry standard absorbent MEA. Additionally, the novel absorbent shows good reaction kinetics and absorption capacity.
  • At least 15% by weight, such as e.g. at least 20 % by weight or at least 25 % by weight, such as about 30 % by weight, of the sterically hindered amine is present in the absorbent. It is also preferred that at least 15% by weight, such as e.g. at least 20 % by weight or at least 25 % by weight such as about 30 % by weight, of the monoalkanolamine, is present in the absorbent.
  • concentrations of the amines corresponds to a weight ratio of sterically hindered amine to the monoalkanolamine from 10:35 to 35: 10, such as e.g. 15:35 to 35:15, 20:35 to 35:20, 25:35 to 35:25, or 30:35 to 35:30, such as e.g. 35:35.
  • a series of screening experiments were performed for an initial screening of possible absorbent mixtures for further examinations.
  • the objective of screening tests is to carry out simple mass transfer absorption and stripping tests of candidate absorbents as alternatives to 30% (5M) mono-ethanol-amine (MEA).
  • the rate of absorption is a measure of the mass transfer enhancement properties of an absorbent, which is directly related to the height required for the absorber. With a faster reacting absorbent the absorber tower height can be reduced.
  • the screening tests give only relative data for the absorption/stripping process.
  • the tests were performed at an apparatus designed to give a fast relative comparison of the rate of absorption and the absorption capacity of solvents with a potential for utilization in an industrial absorption process.
  • the method of comparison has been used for comparative studies since 1993 (see e.g. Erga et al., 1995). Being an apparatus for relative comparison, the interpretation of results relies on the specification of a base-case amine with a specific concentration.
  • the rate of absorption is a measure of the mass transfer enhancement properties of an absorbent, which is directly related to the height required for the absorber. With a faster reacting absorbent the tower heights can normally be reduced.
  • the absorption capacity of the solvent is an important property as a premise for a high cyclic capacity of the process. Additional observations from the screening experiments can be made regarding the extent of foaming, possible precipitation, and discoloration upon CO 2 loading which may be indicative of solvent degradation. In this project the purpose of the screening is to select appropriate concentration levels of both AMP and MMEA / MEA.
  • the absorption capacity of the solvent is an important premise for maximizing the cyclic capacity of the process.
  • the capacity for absorption is limited by the reaction stoichiometry to about 0.5 mole CO 2 /mole amine at ambient pressure.
  • AMP is a sterically hindered amine and forms bicarbonate, it can be loaded to more than 0.5 mole CO 2 /mole amine depending of the CO 2 partial pressure with a theoretical maximum loading of 1.0. It must, however, be noted that for the cyclic capacity to be high, a high CO 2 equilibrium pressure at desorption conditions is also necessary.
  • the mass transfer screening apparatus is used to measure the absorption rate of CO 2 at 4O 0 C followed by desorption rate measurements with nitrogen at 8O 0 C.
  • the gas is distributed through the diffuser of sintered glass which creates gas- bubbles rising up through the liquid. From the surface of these bubbles, CO 2 is first absorbed into the liquid at 40 0 C until 95% of equilibrium, corresponding to 9.5% CO 2 in the effluent gas, is obtained. Afterwards the rich solution is heated to 8O 0 C, and desorption starts with pure nitrogen until the CO 2 concentration in the effluent gas decreases to 1 vol%.
  • a computer controls the solenoid valve system for gas supply and cooling or heating of the water bath.
  • the CO 2 -content of the effluent gas is measured by an IR CO 2 analyzer. After each experiment the accumulated weight of liquid is measured and compared with the net absorbed amount of CO 2 . This is to assure that no solvent is lost by evaporation. Samples of the solvent are also taken for CO 2 analysis after the absorption and desorption sequence.
  • Figures 2 illustrate the results for absorption rate vs. loading and absorption rate vs. concentration, respectively, for 30% MEA and different combinations of AMP and MEA.
  • the highest absorption rate is measured for 30% MEA when the comparison is made on a CO 2 loading basis.
  • the absorption capacity is increased from 2.5 mole/I to 3.5 mole/1 when the feed gas contains 10 vol% C ⁇ 2 (as shown in Figure 3). It must be noted that the loading for all mixtures are limited to about 0.5 mole C ⁇ 2/mole amine even though AMP forms bicarbonate due to the low inlet CO 2 partial pressure
  • Figures 3 and 4 show desorption rate vs. loading and desorption rate vs. concentration, respectively, for the 5 different MEA/AMP mixtures compared with 30% MEA.
  • the stripping curves indicate the achievable net CO 2 absorption capacity (rich-lean CO 2 concentration) for the tested solvent.
  • the mixture 20% AMP + 30% MEA and 25% AMP + 25% MEA seem to be promising alternatives as the net CO 2 capacities are higher than for 30% MEA. Also the mixture 30% AMP + 20% MEA shows to be promising.
  • the highest absorption rate is measured for 30% MEA when the comparison is made on a net CO 2 loading basis.
  • the net absorption capacity is increased from 1.38 mole CO 2 /! (30% MEA) to 1.73-2.18 CO 2 /I for the AMP/MEA mixtures. This is a favorable and important factor to reduce the heat requirement and pump duty.
  • the absorption rate is reduced by about 10% compared with 30% MEA, but is at the same level for all the AMP/MEA mixtures. It must be noted that the loading for all mixtures are close to about 0.5 mole CO 2 /mole amine even though AMP forms bicarbonate. This is according with theory for MEA, while sterically hindered AMP might be loaded to a higher level depending on the CO 2 partial pressure.
  • the equilibrium data for 30 wt% MEA and the solution 2.5M AMP and 2.5M MMEA were measured at temperatures of 40, 60, 80, 100 and 120 0 C. These data were used to obtain an equilibrium model, i.e. a model that calculates the partial pressure of CO2 as a function of loading and temperature. As an example the data for 30wt% MEA is shown in Figure 6 along with the model.
  • the sensible heat is proportional to ⁇ T, and inversely proportional to the cyclic capacity, the number of moles of CO 2 per litre which is transported by the circulating liquid, defined as c Am (a nch -a lean ) .
  • Artificial exhaust gas mainly comprising nitrogen, CO 2 and water is introduced into an absorber 2 through an exhaust gas line 3.
  • the exhaust gas is brought in countercurrent flow to an absorbent to be tested in a contact zone 4 in the absorber 2.
  • the absorbent is introduced through an absorbent line 5 at the top of the absorber, flows trough the contact section and absorbs CO 2 from the exhaust gas, and is collected at the bottom of the absorber 2.
  • the CO 2 rich absorbent collected at the bottom of the absorber is withdrawn through a rich absorbent line 6 and is heated in a heat exchanger 7 and a cooler 8 before the absorbent is introduced at the top of a contact zone 9 of a regenerator 10, where the absorbent is brought in countercurrent flow to steam introduced at the bottom of the contact section 9 to strip the absorbent for CO 2 .
  • the stripped absorbent is collected at the bottom of the regenerator 10 and withdrawn trough an absorbent line 11 and introduced into a reboiler 12, heating the absorbent to produce steam that is introduced into the regenerator 10 through a steam line 13.
  • Regenerated, or lean, absorbent is withdrawn from the reboiler 12 through a lean absorbent line 14 and is cooled against the rich absorbent in the heat exchanger 7 before it is introduced into a storage and mixing tank 15.
  • the lean absorbent is withdrawn through line 5.
  • the temperature of the absorbent in line 5 is controlled by a heater 17 and a cooler 18.
  • the absorbent is thereafter filtered through a coal filter 19 and a particle filter 20 before the lean absorbent is introduced at the top of the contact section of the absorber as described above.
  • CO 2 and steam are collected at the top of the regenerator 10 and is withdrawn through a line 21.
  • the withdrawn gas is cooled and condensed water is collected in a condenser 22.
  • Water collected in the condenser is withdrawn through a condensate line 23 and is introduced into the reboiler, or is introduced at the top of the contact zone 9 of the regenerator 10 through a line 23'
  • Dried CO 2 is withdrawn from the condenser through a CO 2 line 24 and is recycled in the plant as CO 2 for the artificial exhaust gas as described in more detail below.
  • CO 2 depleted exhaust gas here mainly nitrogen
  • CO 2 depleted exhaust gas here mainly nitrogen
  • a pump 26 is withdrawn from the top of the absorber 2 through a line 25 by means of a pump 26 and introduced to a washing section 27 for washing of the gas with water that is introduced through a water line 28.
  • the washing water is withdrawn from the bottom of the washing section into a water tank 29.
  • the water in the water tank 29 is recycled to the washing section via water line 28.
  • the washed gas is leaving the washing section through a line 30, into which CO 2 from the CO 2 line 24 is mixed to make up the artificial exhaust gas.
  • the artificial exhaust gas is heated in a heater 31 before it is introduced into the absorber.
  • sampling point S1 is arranged to withdraw samples for testing the gas in line 3
  • sampling point S2 is arranged to withdraw liquid from line 6
  • samling point S3 is arranged to withdraw gas from line 25
  • sampling point S4 is arranged to withdraw liquid from line 11
  • sapling point S5 is arranged to withdraw liquid from line 14
  • sampling point S6 is arranged to withdraw liquid from the tank 15.
  • the pilot absorber only has 4.3 meter of structured packing, and consequently a capture efficiency of 90 % can not be tested directly.
  • the tests were performed such that the upper part of a full size CO2 column was tested first.
  • the main operational parameter was to have a CO2-content out from the absorber near 0.4 vol-% (90 % recovery).
  • the lean loading of the liquid and the temperature in the absorber were varied.
  • Table 2 shows that these three runs cover the upper part (Run2) the middle part (Run 11 ) and the lower part (Run 17). There are only minor mismatches between the different parts (especially, the liquid temperatures for each run do not match exactly, as described below), and we see that an exhaust gas with 4.4% CO 2 (which is 10% higher than normal concentrations) will be captured down to 0.2 % CO 2 which is 95 % recovery of a normal gas of 4%.
  • the liquid temperature into the absorber was 40 0 C for all these 3 sets. This actually mimics a situation with two intercooling points, and might give a too optimistic absorption rate. Nevertheless, because the column showed more than 90% CO 2 recovery, it might be concluded that an absorber with about 14-15 meter Mellapak 250Y packing will be adequate for this solvent provided similar superficial gas flow (2.2 m/s) and liquid load (10 m 3 /m 2 h).

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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)
  • Treating Waste Gases (AREA)
  • Gas Separation By Absorption (AREA)

Abstract

L'invention porte sur un absorbant aqueux de CO2 comprenant une association d'une amine stériquement encombrée et d'une monoalcanolamine, la concentration de l'amine stériquement encombrée étant de 10 à 35 % en poids et la concentration de la monoalcanolamine étant de 10 à 35 % en poids. De plus, l'invention porte sur un procédé pour l'élimination de CO2 à partir d'un gaz brûlé à l'aide de l'absorbant.
PCT/EP2009/062776 2008-10-01 2009-10-01 Amines WO2010037825A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP09736584A EP2349533A1 (fr) 2008-10-01 2009-10-01 Amines

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
NO20084144 2008-10-01
NO20084144A NO20084144L (no) 2008-10-01 2008-10-01 Aminer for CO2-absorpsjon

Publications (1)

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WO2010037825A1 true WO2010037825A1 (fr) 2010-04-08

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014086988A1 (fr) * 2012-12-07 2014-06-12 Aker Engineering & Technology As Absorbant aqueux de co2 comprenant du 2-amino-2-méthyl-1-propanol et du 3-amino-propanol ou du 2-amino-2-méthyl-1-propanol et du 4-amino-butanol

Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0558019A2 (fr) * 1992-02-27 1993-09-01 The Kansai Electric Power Co., Inc. Méthode d'élimination de l'anhydride carbonique de gaz d'échappement de combustion
JPH06343858A (ja) * 1993-06-08 1994-12-20 Mitsubishi Heavy Ind Ltd 二酸化炭素吸収剤

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0558019A2 (fr) * 1992-02-27 1993-09-01 The Kansai Electric Power Co., Inc. Méthode d'élimination de l'anhydride carbonique de gaz d'échappement de combustion
JPH06343858A (ja) * 1993-06-08 1994-12-20 Mitsubishi Heavy Ind Ltd 二酸化炭素吸収剤

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
ANINDO DEY ET AL: "Carbon Dioxide Absorption Characteristics of Blended Monoethanolamine and 2-Amino-2-methyl-1-propanol", EIC CLIMATE CHANGE TECHNOLOGY, 2006 IEEE, IEEE, PI, 1 May 2006 (2006-05-01), pages 1 - 5, XP031005176, ISBN: 978-1-4244-0218-2 *
SAKWATTANAPONG ET AL: "Behavious of reboiler heat duty for CO2 capture plants using regenerable single and blended alkanolamines", INDUSTRIAL AND ENGINEERING CHEMISTRY RESEARCH, vol. 44, no. 12, 8 June 2005 (2005-06-08), American Chemical Society US, pages 4465 - 4473, XP002560572 *

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014086988A1 (fr) * 2012-12-07 2014-06-12 Aker Engineering & Technology As Absorbant aqueux de co2 comprenant du 2-amino-2-méthyl-1-propanol et du 3-amino-propanol ou du 2-amino-2-méthyl-1-propanol et du 4-amino-butanol
CN104853830A (zh) * 2012-12-07 2015-08-19 阿克工程及技术股份公司 一种含有2-氨基-2-甲基-1-丙醇和3-氨基丙醇或2-氨基-2-甲基-1-丙醇和4-氨基丁醇的含水的co2吸收剂
CN104853830B (zh) * 2012-12-07 2018-04-27 阿克工程及技术股份公司 一种含有2-氨基-2-甲基-1-丙醇和3-氨基丙醇或2-氨基-2-甲基-1-丙醇和4-氨基丁醇的含水的co2吸收剂

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Publication number Publication date
EP2349533A1 (fr) 2011-08-03
NO20084144L (no) 2010-04-06

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