WO2013159215A1 - Capture de co2 à l'aide de solutions d'absorption à base d'ammoniac à faible concentration en présence d'enzymes - Google Patents

Capture de co2 à l'aide de solutions d'absorption à base d'ammoniac à faible concentration en présence d'enzymes Download PDF

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Publication number
WO2013159215A1
WO2013159215A1 PCT/CA2013/050201 CA2013050201W WO2013159215A1 WO 2013159215 A1 WO2013159215 A1 WO 2013159215A1 CA 2013050201 W CA2013050201 W CA 2013050201W WO 2013159215 A1 WO2013159215 A1 WO 2013159215A1
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Prior art keywords
absorption solution
kmol
absorption
liquid loading
flow rate
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PCT/CA2013/050201
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English (en)
Inventor
Albert Rikus Johannes ARENDSEN
Geert Frederik Versteeg
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Co2 Solutions Inc.
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Publication of WO2013159215A1 publication Critical patent/WO2013159215A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/14—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by absorption
    • B01D53/1456—Removing acid components
    • B01D53/1475—Removing carbon dioxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/46—Removing components of defined structure
    • B01D53/62—Carbon oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
    • B01D2252/10—Inorganic absorbents
    • B01D2252/102—Ammonia
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
    • B01D2252/60—Additives
    • B01D2252/602—Activators, promoting agents, catalytic agents or enzymes
    • 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
    • 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 generally relates to the field of gaseous C0 2 capture. More particularly, the present invention concerns processes for C0 2 capture using low concentration ammonia based absorption solutions in combination with enzymes.
  • GHGs man-made greenhouse gas
  • C0 2 carbon dioxide
  • the CCS process involves selective removals of C0 2 from a C0 2 -containing flue gas, and production of a highly concentrated C0 2 gas stream which is then compressed and transported to a geologic sequestration site.
  • This site may be a depleted oil field or a saline aquifer.
  • Sequestration as mineral carbonates is an alternate way to sequester C0 2 that is in the development phase. Captured C0 2 can also be used for enhanced oil recovery, for injection into greenhouses, for chemical reactions and production, and for other useful applications.
  • aqueous solutions currently in use in this regard are alkanolamine-based solutions.
  • an alternative approach is based on the use of aqueous ammonia, known as the "chilled ammonia" process.
  • CAP chilled ammonia process
  • US patent No. 7,862,788 hereinafter referred to as Gal et al
  • Gal et al describe a promoter enhanced chilled ammonia based system for removal of C0 2 from a flue gas stream.
  • Gal et al describe a CAP process in which a promoter is used to help accelerate certain chemical reactions that occur between C0 2 and ammoniated ionic solutions.
  • the promoter may be an amine such as piperazine or an enzyme or enzyme system.
  • CAP installations have used relatively low temperatures, e.g. between 0-20°C or between 0-10°C, along with relatively high ammonia concentrations.
  • the low temperature minimizes ammonia losses to evaporation and the high ammonia concentration enables adequate absorption of C0 2 from the flue gas.
  • Conventional wisdom has indeed suggested that decreasing NH 3 concentration would result in a proportional increase of the overall solvent circulation rate in the absorption tower for a given C0 2 capture rate.
  • Increasing solvent circulation rate within the system would, in turn, increase the overall equipment and operational cost significantly.
  • a lower NH 3 concentration can induce an increase of solvent circulation rate to maintain the C0 2 loading capacity, thereby inducing a significant increase in energy consumption and equipment size.
  • the present invention responds to the above need by providing a processes and methods for capturing carbon dioxide using ammonia based absorption solutions.
  • a method for reducing a size of C0 2 capture equipment for capturing C0 2 from a C0 2 containing gas with an ammonia based absorption solution at low ammonia concentrations includes:
  • the operation window is defined by operating conditions comprising an absorption temperature, a lean C0 2 liquid loading range of the absorption solution, an ammonia concentration range in the absorption solution and an absorption solution flow rate.
  • the method may include managing an ammonium bicarbonate saturation percentage of the absorption solution for increasing or maximizing a rich C0 2 liquid loading in the absorption solution.
  • the method may include managing a C0 2 partial pressure in the absorption solution for increasing or maximizing the rich C0 2 liquid loading in the absorption solution.
  • a process for removing C0 2 from a C0 2 containing gas includes:
  • an operation window enabling operation near or at an elevated or maximized rich C0 2 liquid loading, the operation window being defined by an operating ammonia concentration range and an operating absorption solution flow rate range, at a given absorption temperature and a given lean C0 2 liquid loading range; providing an ammonia based absorption solution having an ammonia concentration selected in the operating ammonia concentration range and having a C0 2 liquid loading selected in the lean C0 2 liquid loading range;
  • the absorption solution having a flow rate selected in the operating absorption solution flow rate range;
  • a method of using low ammonia concentrations in an ammonia based C0 2 capture process includes:
  • an operation window for the C0 2 capture process enabling capture near or at an elevated or maximized rich C0 2 liquid loading, the operation window being defined by an operating ammonia concentration range and an operating absorption solution flow rate range, at a given absorption temperature and a given lean C0 2 liquid loading range;
  • the method may include using at least one enzyme or analogue thereof for accelerating the hydration reaction of C0 2 into the absorption solution and thereby reduce equipment sizing within the operation window.
  • a method for maximizing absorption of C0 2 from a C0 2 -containing gas using an ammonia based absorption solution includes: determining a maximum rich C0 2 liquid loading in the ammonia based absorption solution in accordance with given operating conditions;
  • the selecting of the absorption solution flow rate may be performed according to the following equation:
  • C m is the NH 3 concentration in the absorption solution in kmol/m 3 .
  • a process for capturing C0 2 from a C0 2 containing gas with an ammonia based C0 2 capture system includes:
  • the process may include controlling or reducing an absorption solution flow rate for operating near or at a maximum C0 2 capture at low ammonia concentrations.
  • the process may include controlling the ammonia concentration, an absorption temperature, a lean C0 2 liquid loading or an absorption solution flow rate or a combination thereof, to reduce or avoid formation of precipitated solids in the absorption solution.
  • an ammonia based absorption solution for use in a C0 2 capture system, the absorption solution having an ammonia concentration sufficiently low as to be enhanced by the presence of an enzyme while reaching an enhanced or maximized C0 2 liquid loading.
  • the lean C0 2 liquid loading may be between about 0.1 and about 0.5, optionally between about 0.2 and about 0.45, and further optionally between 0.35 and 0.4.
  • the absorption temperature may be between about 0°C and about 50°C, optionally between about 10°C and about 30°C, and further optionally between about 15°C and about 25°C.
  • the ammonia concentration may be between about 1 kmol/m 3 and about 8 kmol/m 3 .
  • the ammonia concentration may be between about 2 kmol/m 3 and about 5 kmol/m 3 when the absorption temperature is about 10°C.
  • the ammonia concentration may be between about 2 kmol/m 3 and about 3 kmol/m 3 .
  • the ammonia concentration may be between about 4 kmol/m 3 and about 8 kmol/m 3 when the absorption temperature is about 25°C.
  • the ammonia concentration may be between about 5 kmol/m 3 and about 7 kmol/m 3 .
  • the ammonia concentration may be about 6 kmol/m 3 .
  • the absorption solution flow rate may be between about 0.5 and about 3 m 3 /kmol, optionally between about 1 m 3 /kmol and about 2 m 3 /kmol.
  • the enzyme may comprise a recombinant enzyme, a variant enzyme or a naturally occurring enzyme or a combination thereof.
  • the enzyme may be derived from archeal source enzyme, bacterial source enzyme or fungal source enzyme or a combination thereof.
  • the enzyme may include carbonic anhydrase or analogues thereof.
  • the operation window may be defined for the given absorption temperature and the given lean C0 2 liquid loading by:
  • the operating ammonia concentration range between about 1 kmol/m 3 and 8 kmol/m 3 ; and the operating absorption solution flow rate range wherein the absorption solution flow rate is within 0.5 m 3 /kmol above or below a corresponding solvent flow rate at the given lean C0 2 liquid loading.
  • the operation window may be defined for the given absorption temperature and the given lean C0 2 liquid loading by:
  • the operating ammonia concentration range wherein the ammonia concentration is within 1.5 kmol/m 3 above or below a transitional ammonia concentration
  • the operating absorption solution flow rate range wherein the absorption solution flow rate is within 0.5 m 3 /kmol above or below a corresponding solvent flow rate at the given lean C0 2 liquid loading.
  • methods and processes may include determining the transitional ammonia concentration at a transition point for the given absorption temperature and the given lean C0 2 liquid loading.
  • the operation window may be pre-determined, calculated, estimated and/or determined during start-up, turndown or regular operation.
  • the operation window may be based on models, simulations, experiments or representations or a combination thereof, as represented in the appended figs for example.
  • Fig. 1 is a process flow diagram of a C0 2 capture process including absorption and desorption units according to an optional embodiment of the present invention.
  • Fig. 2 is a graph of rich C0 2 liquid loading versus NH 3 concentration at a temperature of 10C with iso-lines of the logarithm of C0 2 partial pressure according to an optional embodiment of the present invention.
  • Fig. 3 is a graph of rich C0 2 liquid loading versus NH 3 concentration at a temperature of 25'C with iso-lines of NH 4 HC0 3 saturation according to an optional embodiment of the present invention.
  • Fig. 4 is a graph of NH 3 concentration versus rich C0 2 liquid loading at a temperature of 10C with iso-lines of the logarithm of C0 2 partial pressure according to an optional embodiment of the present invention.
  • Fig. 5 is a graph of NH 3 concentration versus rich C0 2 liquid loading at a temperature of 10C with iso-lines of NH 4 HC0 3 saturation according to an optional embodiment of the present invention.
  • Fig. 6 is a graph of NH 3 concentration versus rich C0 2 liquid loading at a temperature of 10C with iso-lines of the logarithm of NH 3 partial pressure according to an optional embodiment of the present invention.
  • Fig. 7 is a graph of rich and lean C0 2 liquid loadings versus NH 3 concentration at a temperature of 25'C, a C0 2 partial pressure of 1 bar and a NH 4 HC0 3 saturation of 100%, according to an optional embodiment of the present invention.
  • Fig. 8 is a graph of absorption solution flow rate versus the NH 3 concentration at a temperature of 25'C for several lean CO 2 liquid loadings at constant C0 2 capture with operation windows according to an optional embodiment of the present invention.
  • Fig. 9 is a graph of NH 3 concentration versus absorption solution flow rate at a temperature of 100 for several lean C0 2 liquid loadings at constant C0 2 capture with operation windows according to an optional embodiment of the present invention.
  • Fig. 10 is a graph of NH 3 concentration versus absorption solution flow rate at a temperature of 25'C for several lean C0 2 liquid loadings at constant C0 2 capture according to an optional embodiment of the present invention.
  • Fig. 1 1 is a graph of NH 3 concentration versus absorption solution flow rate at a temperature of I OC for a lean C0 2 liquid loading of 0.4 at constant C0 2 capture with an operation window according to an optional embodiment of the present invention.
  • Fig. 12 a graph of NH 3 concentration versus absorption solution flow rate at a temperature of ⁇ 0 for several lean C0 2 liquid loadings at constant C0 2 capture with operation windows according to an optional embodiment of the present invention.
  • Fig. 13 is a process flow diagram of a C0 2 capture process including absorption and desorption units according to an optional embodiment of the present invention.
  • the present invention relates to techniques for absorbing C0 2 from a C0 2 -containing gas with an ammonia based absorption solution in combination with an enzyme.
  • Equation (1) may therefore be written as follows:
  • ammonium bicarbonate is in chemical equilibrium between its solid state NH HC0 3 (S) and its solute [NH + ; HC0 3 " ] (aq) .
  • the degree of saturation of the absorption solution may be expressed in percentage of the NH C0 3 solute (also referred as solubility product) at a given absorption solution composition.
  • rates of dissolution and precipitation are equal to one another and the absorption solution is said to be saturated.
  • a rise of temperature increases the solubility (according to Le Chatelier's principle).
  • the process comprises feeding the absorption solution into an absorber reactor, to contact the C0 2 -containing gas so as to dissolve C0 2 from the C0 2 -containing gas into the absorption solution in presence of the enzyme, thereby catalyzing the hydration of dissolved C0 2 into bicarbonate ions and hydrogen ions, and producing a gas stream and a liquid stream.
  • the gas stream is a C0 2 -depleted gas and the liquid stream is an ion-rich solution comprising bicarbonate ions and ammonium ions.
  • the overall C0 2 capture process 10 may include an absorption unit 12 and a desorption unit 14.
  • the absorption unit 12 may include the absorber reactor 16 which receives the C0 2 -containing gas 18 that can come from a variety of sources.
  • the C0 2 -containing gas 18 is an effluent gas such as power plant flue gas, industrial exhaust gas, aluminum refining flue gas, aluminum smelting off-gas, steel production flue gas, chemical production flue gas, combustion gas from in-situ oil sands production, etc.
  • the C0 2 -containing gas 18 is a naturally occurring gas such as ambient air.
  • the absorber reactor 16 also receives the absorption solution 20.
  • the absorber reactor 16 the conversion of C0 2 into bicarbonate and hydrogen ions takes place in the presence of at least one enzyme or analogue thereof, thereby producing the C0 2 -depleted gas 22 and the ion-rich solution 24.
  • the absorber reactor 16 is a direct-contact type reactor, such as a packed tower or spray scrubber or otherwise, allowing the gas and liquid phases to contact and mix together.
  • the ion-rich solution 24 may be pumped by a pump 26 to downstream parts of the process, such as heat exchangers, desorption units, regeneration towers and the like.
  • Part of the ion-rich solution 24 may be recycled back to the absorber reactor 16 via an ion-rich solution return line, which can improve mixing of the bottoms of the absorber reactor to avoid accumulation of precipitates and reactor deadzones, as the case may be.
  • the absorber 16 may also have other recycle or return lines, as desired, depending on operating conditions and reactor design.
  • the process may be operated according to process operating conditions including an absorption temperature, a NH 3 concentration in the ammonia based absorption solution, an absorption solution flow rate, a rich C0 2 liquid loading and a lean C0 2 liquid loading.
  • the lean C0 2 liquid loading is defined as the ratio of C0 2 molarity over NH 3 molarity in the absorption solution entering the absorber, also referred to herein after as ai ean -
  • the rich C0 2 liquid loading is defined as the ratio of C0 2 molarity over NH 3 molarity in the ion-rich solution exiting the absorber, also referred to herein after as a rich .
  • Fig. 2 is a graph providing iso-lines of C0 2 partial pressure as a function of the NH 3 concentration and the rich C0 2 liquid loading at an absorption temperature of 25°C.
  • each iso-line provides the corresponding maximum rich C0 2 liquid loading at 25'C.
  • the C0 2 partial pressure is 0.1 bar (10,000 Pa)
  • the corresponding iso-line of C0 2 partial pressure is the iso-line with a value of 4.
  • the maximum rich C0 2 liquid loading is 0.7 at 25 .
  • Fig. 3 is a graph providing iso-lines of NH HC0 3 saturation percentage as a function of the NH 3 concentration and rich C0 2 liquid loading at an absorption temperature of 25'C.
  • each iso-line provides the corresponding maximum rich C0 2 liquid loading at 25'C.
  • the saturation percentage i n the absorption solution is 50%
  • the corresponding iso-line has a value of 50.
  • the maximum rich C0 2 liquid loading is 0.62 at 25 t C.
  • Figs. 4 to 6 are graphs respectively providing iso-lines of C0 2 partial pressure, iso-lines of NH HC0 3 saturation and iso-lines of NH 3 partial pressure as a function of the NH 3 concentration and the rich C0 2 liquid loading at an absorption temperature of 10°C.
  • Fig. 7 is a graph based on a combination of the graphs of Figs. 2 and 3 for a C0 2 partial pressure of 1 bar and a NH HC0 3 saturation of 100%. Indeed, Fig. 7 provides the maximum a rich at 25'C as a function of NH 3 concentration based on the combination of a given C0 2 partial pressure (one iso-line of Fig. 2) and a given NH HC0 3 saturation at equilibrium (one iso-line of Fig. 3).
  • the NH 3 concentration has a transition value under which the maximum a rich is limited by the given C0 2 partial pressure; and above which the maximum a rich is limited by the given NH HC0 3 saturation.
  • Fig. 7 shows that under a transition value NH 3 concentration of 6.3 kmol/m 3 , the maximum a rich is limited by the given C0 2 partial pressure and above 6.3 kmol/m 3 the maximum a rich is limited by the given NH4HCO 3 saturation.
  • Fig. 7 shows that under a transition value NH 3 concentration of 6.3 kmol/m 3 , the maximum a rich is limited by the given C0 2 partial pressure and above 6.3 kmol/m 3 the maximum a rich is limited by the given NH4HCO 3 saturation.
  • the process may comprise controlling the absorption solution flow rate for operating near or at a maximum rich C0 2 liquid loading of the ion- rich solution at the exit of the absorber.
  • the required absorption solution flow rate may be determined according to the following equation (1). ⁇ ⁇ ⁇ is the absorption solution flow rate in m 3 /kmol;
  • ncft max is the maximum rich C0 2 liquid loading
  • a lean is the lean C0 2 liquid loading of the absorption solution entering the absorber; and C m is the NH 3 concentration in the absorption solution in kmol/m 3 .
  • Fig. 8 is a graphical representation of equation (1) showing the required absorption solution flow rate for attaining the maximum rich C0 2 liquid loading as a function of the NH 3 concentration for 5 different lean C0 2 liquid loadings ranging from 0.1 to 0.5.
  • Each of the five curves includes a transition point T at which the maximum rich C0 2 liquid loading is the same for a given C0 2 partial pressure and a given NH4HCO 3 saturation.
  • the NH 3 concentration at the transition point T for each lean C0 2 liquid loading is 6.3 kmol/m 3 .
  • the required absorption solution flow rate is limited by the C0 2 partial pressure.
  • the required absorption solution flow rate is limited by the NH4HCO 3 saturation.
  • the process may comprise controlling or providing process operating conditions according to an operation window enabling to maximize the rich C0 2 liquid loading, also referred to hereinafter as maximum C0 2 capture.
  • the operation window may be chosen so as to maximize the rich C0 2 liquid loading at low NH 3 concentrations.
  • the operation window may be chosen so as to maximize the rich C0 2 liquid loading at low NH 3 concentrations at which the maximum rich C0 2 liquid loading is limited by a given C0 2 partial pressure.
  • the operation window may be chosen so as to maximize the rich C0 2 liquid loading at low NH 3 concentrations at which the maximum rich C0 2 liquid loading is limited by a given NH 4 HC0 3 saturation.
  • the operation window may be chosen so as to maximize the rich C0 2 liquid loading at low NH 3 concentrations at which the maximum rich C0 2 liquid loading is limited either by a given C0 2 partial pressure or a given NH 4 HC0 3 saturation.
  • the operation window may be determined by an operating NH 3 concentration range and an operating absorption solution flow rate range enabling to maximize the rich C0 2 liquid loading.
  • the operation NH 3 concentration range may include low NH 3 concentrations.
  • the operation window may also be defined for a given absorption temperature, a given C0 2 partial pressure, a given NH 4 HC0 3 saturation and a given range of lean C0 2 liquid loading.
  • the operation window defined for a given lean C0 2 liquid loading is referred to as W a in the Figs.
  • NH 3 concentration may be lowered without causing a significant increase of the solvent flow rate required to attain or come closer a maximum rich C0 2 liquid loading.
  • a variation of the NH 3 concentration from 6.3 kmol/m 3 to 4 kmol/m 3 implies a slight increase of the absorption solution flow rate from 0.5 m 3 /kmol to 0.7 m 3 /kmol so as to maintain a maximum rich C0 2 liquid loading.
  • the operation window may be defined for enabling to operate at low NH 3 concentrations without increasing the absorption solution flow rate above a targeted threshold.
  • the NH 3 concentration may be at most 8 kmol/m 3 .
  • the NH 3 concentration may be at most 6 kmol/m 3 range between about 1 to about 8 kmol/m 3 .
  • the NH 3 concentration may range from about 2 to about 4 kmol/m 3 .
  • the lean C0 2 liquid loading may range from about 0.1 to about 0.5.
  • the lean C0 2 liquid loading may range from about 0.2 to about 0.45.
  • the lean C0 2 liquid loading may be about 0.4.
  • the absorption solution flow rate may range from about 0.5 to about 3 m 3 /kmol.
  • the operation window may include a plurality of individual operation windows for each optional operating range of NH 3 concentration and absorption solution flow rate defined above.
  • the operation window may also be defined to operate with a ratio of the operating NH 3 concentration range over the operating absorption solution flow rate range between 1 and 10.
  • the operating NH 3 concentration range may or may not include the transition value of NH 3 concentration depending on the limitation imposed to the process, i.e. C0 2 partial pressure limitation, NH 4 HC0 3 saturation limitation or a combination thereof.
  • the operating NH 3 concentration range of the operation window W 0 .i does not include the transition value of NH 3 concentration of 6.3 kmol/m 3 .
  • the maximizing of the rich C0 2 liquid loading for a lean C0 2 liquid loading of 0.1 at the entrance of the absorber is performed under a C0 2 partial pressure limitation only.
  • maximizing the rich C0 2 liquid loading would imply operating at an absorption solution flow rate of 0.25 m 3 /kmol, which is an inoperable absorption solution flow rate.
  • operating within the operating window W 0 .i at lower NH 3 concentrations, for example 3 kmol/m 3 enables to maximize the rich C0 2 liquid loading with an acceptable value of flow rate of 0.6 m 3 /kmol.
  • the process may include contacting the C0 2 containing gas with the ammonia based absorption solution in presence of a biocatalyst, such as an enzyme.
  • a biocatalyst such as an enzyme.
  • the enzyme may include carbonic anhydrase and analogues thereof.
  • the presence of a biocatalyst allows catalyzing the hydration of C0 2 into hydrogen ions and bicarbonate ions in the absorption solution.
  • the size of the absorber While operating within the operating window at low NH 3 concentrations, the size of the absorber may have to be adapted in accordance with the required absorption solution flow rate for maximizing the rich C0 2 liquid loading. When the required absorption solution flow rate is decreased, the size of the absorber may have to be increased accordingly.
  • the enzyme may therefore be advantageously used so as to reduce the size of the absorber within the chosen operating window.
  • carbonic anhydrase and analogues thereof may include naturally occurring, modified or evolved carbonic anhydrase enzymes; and analogues thereof may be variants or non-biological small molecules that are naturally occurring or synthesized to achieve or mimic the effect of the enzyme.
  • the process may include controlling solid formation of NH 4 HC0 3 within the absorber.
  • an increase of the absorption temperature e.g. from 10 ⁇ to 25 ⁇
  • the absorption temperature may be chosen accordingly so as to preserve the activity of the enzyme.
  • the absorption temperature may be further chosen so as to minimize the ammonia losses by evaporation and maximize the solubility of NH 4 HC0 3 .
  • the absorption temperature may range from about 0 ⁇ to about 50 ⁇ .
  • the absorption temperature may range from about 10 ⁇ to about 30 ⁇ .
  • the absorption temperature may be 15 ⁇ .
  • the operation window may be defined with a varying operating absorption solution flow rate range.
  • the operating absorption solution flow rate may vary.
  • this latter range may be from 1.2 to 1.6 m 3 /kmol for 1 kmol/m 3 , and from 1 to 1.4 m 3 /kmol for 5 kmol/m 3 .
  • This optional embodiment of the operation window may enable to operate in accordance with an operating absorption solution flow rate range which is within 0.2 m 3 /kmol above or below the corresponding absorption solution flow rate at a constant C0 2 capture.
  • the operating absorption solution flow rate range could be within 0.5 m 3 /kmol to 0.1 m 3 /kmol above or below the corresponding absorption solution flow rate at a constant C0 2 capture, so as to operate near or at the maximum rich C0 2 liquid loading.
  • a total operation window may include a plurality of operation windows in accordance with the plurality of lean C0 2 liquid loadings that are expected at the entrance of the absorber.
  • each total operation window of Fig. 12 may have a shape which varies so as to follow the trend of the curves according to the lean C0 2 liquid loading range.
  • W T 3 is defined by an operating absorption solution flow rate range which is within 0.50 m 3 /kmol above or below the corresponding absorption solution flow rate at a constant lean C0 2 liquid loading, and by an operating NH 3 concentration range which is within 1.5 kmol/m 3 above or below the transition value of NH 3 concentration on the line L.
  • W T2 is defined by an operating solvent flow rate range which is within 0.35 m 3 /kmol above or below the corresponding absorption solution flow rate at a constant lean C0 2 liquid loading, and by an operating NH 3 concentration range which is within 1 kmol/m 3 above or below the transition value of NH 3 concentration on the line L.
  • W T1 is defined by an operating absorption solution flow rate range which is within 0.15 m 3 /kmol above or below the corresponding absorption solution flow rate at a constant lean C0 2 liquid loading, and by an operating NH 3 concentration range which is within 0.50 kmol/m 3 above or below the transition value of NH 3 concentration on the line L.
  • the operation line L is defined by an operating absorption solution flow rate range which is within 0.05 m 3 /kmol above or below the transition value of the absorption solution flow rate.
  • the process may be operated within an operation window which enables to provide or manage the absorption solution flow rate in accordance to the transitional value of NH 3 concentration at a given absorption temperature and a given range of lean C0 2 liquid loading.
  • the absorption temperature may be minimized so as to consequently lower the transitional value of NH 3 concentration and therefore operate at low NH 3 concentration.
  • the process further includes regenerating the captured C0 2 as a C0 2 gas which can be separated for sequestration, storage or various uses.
  • the ion-rich solution 24 may then be fed to the desorption unit 14, in which it can be regenerated.
  • the ion-rich solution 24 is preferably heated, which may be done by one or more heat exchanger 32, to favor the desorption process.
  • the heat exchanger may use heat contained in one or more downstream process streams in order to heat the ion-rich solution 32, e.g. ion-depleted solution 42.
  • the heated ion-rich solution 34 is fed into a desorption reactor 36.
  • the at least one enzyme or analogue thereof may be present within the ion-rich solution 34, allowing the at least one enzyme to flow with the ion-rich solution 34 while promoting the conversion of the bicarbonate ions into C0 2 gas 38 and generating an ion-depleted solution 40.
  • the at least one enzyme could also be fixed or immobilized within reactors or particles passing within and/or through the reactors. Alternatively, the enzymes could also be removed from the ion-rich stream prior to feeding it to the desorption reactor 36.
  • the process also includes releasing the C0 2 gas 38 and the ion-depleted solution 40 from the desorption unit 14 and, preferably, sending a recycled ion-depleted solution 42 to make up at least part of the absorption solution 20.
  • a make-up stream 50 introducing the at least one enzyme further makes up the absorption solution 20.
  • the ion-depleted solution 42 is preferably cooled prior to re-injection into the absorption unit, which may be done by the heat exchanger 32.
  • the desorption reactor 36 may also include various recycle or return streams (not illustrated) as desired.
  • the desorption unit 14 may also include one or more reboilers each of which takes a fraction of the liquid flowing through a corresponding one of the desorption reactors and heats it to generate steam that will create a driving force such that C0 2 will be further released from the solution.
  • the process further includes managing a NH 4 HC0 3 solids content in the ion rich solution for optimizing desorption.
  • the reduction of the size of the desorption unit 14 may result from the separation, in a separation unit 52, of the ion-rich solution 24 into a pure liquid stream 54 and a solid/liquid slurry 56.
  • the pure liquid stream 54 has a relatively low C0 2 content and the solid/liquid slurry 56 has a high C0 2 content.
  • the size of the desorption reactor 36 is reduced (comparing to the process according to Fig. 1).
  • Embodiments or aspects of the above-mentioned processes and methods can provide several advantages, some of which are as follows; decrease of ammonia slip or loss in the absorber reactor; ability to operate the process at higher temperatures; optimization of the stripping performance based on the net energy consumption as an optimization parameter; better control of solids formation; less complicated process set-up and less process units.

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  • Oil, Petroleum & Natural Gas (AREA)
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Abstract

La présente invention concerne des méthodes et des processus se rapportant à la capture du CO2 avec des solutions d'absorption à base d'ammoniac à faible concentration. Les conditions de fonctionnement peuvent être établies de sorte qu'elles puissent être mises en œuvre à l'intérieur d'une fenêtre de fonctionnement permettant une plage maximale de capture du CO2 ; et la solution d'absorption à base d'ammoniac peut être améliorée par l'ajout d'au moins une enzyme ou ses analogues, afin d'accélérer l'hydratation du CO2 provenant du gaz contenant le CO2 dans la solution d'absorption pour réduire par exemple, la taille de l'équipement de capture du CO2 à l'intérieur de la fenêtre de fonctionnement. Les conditions de fonctionnement peuvent comprendre une pression partielle de CO2 dans la solution d'absorption, une température d'absorption, une plage de chargement de liquide pauvre en CO2 de la solution d'absorption, une plage de concentration d'ammoniac dans la solution d'absorption et un débit de la solution d'absorption. Les méthodes et les processus peuvent comprendre l'étape consistant à sélectionner le débit de la solution d'absorption en fonction d'un chargement maximal de liquide riche en CO2 de la solution d'absorption.
PCT/CA2013/050201 2012-04-24 2013-03-14 Capture de co2 à l'aide de solutions d'absorption à base d'ammoniac à faible concentration en présence d'enzymes WO2013159215A1 (fr)

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006022885A1 (fr) * 2004-08-06 2006-03-02 Eig, Inc. Ultra nettoyage de gaz de combustion englobant l’enlèvement de co2
WO2010003961A1 (fr) * 2008-07-07 2010-01-14 Arcelik Anonim Sirketi Agencement de rinçage de boîte de détergent pour machine à laver
US7862788B2 (en) * 2007-12-05 2011-01-04 Alstom Technology Ltd Promoter enhanced chilled ammonia based system and method for removal of CO2 from flue gas stream
US20110061533A1 (en) * 2009-09-15 2011-03-17 Black Sean E Method and system for removal of carbon dioxide from a process gas
US20120063975A1 (en) * 2010-09-14 2012-03-15 Peter Ulrich Koss Process gas treatment system
US20120258031A1 (en) * 2011-04-06 2012-10-11 Alstom Technology Ltd. Carbon dioxide capture system

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2006022885A1 (fr) * 2004-08-06 2006-03-02 Eig, Inc. Ultra nettoyage de gaz de combustion englobant l’enlèvement de co2
US7862788B2 (en) * 2007-12-05 2011-01-04 Alstom Technology Ltd Promoter enhanced chilled ammonia based system and method for removal of CO2 from flue gas stream
WO2010003961A1 (fr) * 2008-07-07 2010-01-14 Arcelik Anonim Sirketi Agencement de rinçage de boîte de détergent pour machine à laver
US20110061533A1 (en) * 2009-09-15 2011-03-17 Black Sean E Method and system for removal of carbon dioxide from a process gas
US20120063975A1 (en) * 2010-09-14 2012-03-15 Peter Ulrich Koss Process gas treatment system
US20120258031A1 (en) * 2011-04-06 2012-10-11 Alstom Technology Ltd. Carbon dioxide capture system

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