US20120067082A1 - Method and apparatus for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid - Google Patents
Method and apparatus for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid Download PDFInfo
- Publication number
- US20120067082A1 US20120067082A1 US13/375,256 US201013375256A US2012067082A1 US 20120067082 A1 US20120067082 A1 US 20120067082A1 US 201013375256 A US201013375256 A US 201013375256A US 2012067082 A1 US2012067082 A1 US 2012067082A1
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- US
- United States
- Prior art keywords
- carbon dioxide
- oxygen
- enriched
- flow
- argon
- Prior art date
- Legal status (The legal status 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 status listed.)
- Abandoned
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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
- B01D53/002—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 condensation
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- F23J15/00—Arrangements of devices for treating smoke or fumes
- F23J15/006—Layout of treatment plant
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- F23J15/00—Arrangements of devices for treating smoke or fumes
- F23J15/02—Arrangements of devices for treating smoke or fumes of purifiers, e.g. for removing noxious material
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- F23L—SUPPLYING AIR OR NON-COMBUSTIBLE LIQUIDS OR GASES TO COMBUSTION APPARATUS IN GENERAL ; VALVES OR DAMPERS SPECIALLY ADAPTED FOR CONTROLLING AIR SUPPLY OR DRAUGHT IN COMBUSTION APPARATUS; INDUCING DRAUGHT IN COMBUSTION APPARATUS; TOPS FOR CHIMNEYS OR VENTILATING SHAFTS; TERMINALS FOR FLUES
- F23L7/00—Supplying non-combustible liquids or gases, other than air, to the fire, e.g. oxygen, steam
- F23L7/007—Supplying oxygen or oxygen-enriched air
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- F25J2270/904—External refrigeration, e.g. conventional closed-loop mechanical refrigeration unit using Freon or NH3, unspecified external refrigeration by liquid or gaseous cryogen in an open loop
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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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- 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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E20/00—Combustion technologies with mitigation potential
- Y02E20/32—Direct CO2 mitigation
-
- 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
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E20/00—Combustion technologies with mitigation potential
- Y02E20/34—Indirect CO2mitigation, i.e. by acting on non CO2directly related matters of the process, e.g. pre-heating or heat recovery
Abstract
The invention relates to a method for producing an argon-enriched fluid and an oxygen-enriched fluid from a fluid resulting from a method for purifying of oxy-fuel combustion fumes, wherein said method comprises purifying the residual gas by a purification method in order to produce a gas enriched with carbon dioxide and a residual gas lean in carbon dioxide, pre-treating the residual gas lean in carbon dioxide in order to obtain a flow enriched with carbon dioxide and a flow lean in carbon dioxide, treating the flow lean in carbon dioxide by a cryogenic technique so as to extract at least an argon-enriched fraction, an oxygen-enriched fraction, and a fraction lean in argon and/or oxygen.
Description
- The present invention relates to a method for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid resulting from a method for purifying a residual gas, the residual gas containing carbon dioxide and either argon or oxygen or both. A particular example would be the production of argon from the incondensables of a method for low-temperature separation of a residual gas produced by an installation consuming oxygen, the residual gas being oxy-fuel combustion fumes.
- Thermal power stations make it possible to release heat, which can be used to produce steam and mechanical or electrical energy, by combustion of fuels. The combustion fumes release large quantities of CO2 into the atmosphere. In order to resolve this environmental problem, the current solution consists in carrying out the combustion inside the boiler in the presence of a gas which is rich in oxygen and above all depleted of nitrogen. This combustion produces combustion fumes having a high concentration of CO2, which is advantageous because the current technologies for removing CO2 from the combustion fumes make it possible to remove the CO2 more easily from fumes with a high concentration of CO2 than from fumes with a low concentration of CO2. This CO2 then needs to be purified and compressed before being sequestered.
- It is an object of the present invention to provide a method for producing argon and oxygen from a residual gas rich in carbon dioxide and also containing argon and/or oxygen, which are incondensables of a unit for purifying fumes with respect to CO2 at low temperature.
- One subject of the invention provides a method for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid resulting from a method for purifying a residual gas containing carbon dioxide and oxygen and/or argon, the residual gas being derived from an installation supplied with oxygen containing argon, which is an oxy-fuel combustion installation, comprising the following steps:
-
- recovering residual gas, consisting of fumes resulting from the oxy-combustion of a fuel by means of a gas rich in oxygen and in carbon dioxide and containing argon in the combustion chamber of a boiler;
- purifying the residual gas, in particular fumes leaving the boiler, by a purification method in particular at low temperature, so as to produce a fluid enriched with carbon dioxide and a residual fluid depleted of carbon dioxide;
- pretreatment of the residual fluid depleted of carbon dioxide in order to obtain a flow enriched with carbon dioxide and a flow lean in carbon dioxide; and
- cryogenic treatment of the flow lean in carbon dioxide so as to extract therefrom at least one fraction enriched or rich in argon, a fraction enriched or rich in oxygen and at least one fraction depleted of argon and/or oxygen.
- According to other optional aspects:
-
- the cryogenic treatment of the flow lean in carbon dioxide comprises a step of cooling in at least one exchanger, optionally a reboiler, optionally a condenser, optionally an exchanger of the reversible type or of the regenerator type, and a step of distillation in a distillation column;
- the purification method is preferably carried out at low temperature, although other known purification methods may be substituted therefor (for example washing with amines);
- the flow lean in carbon dioxide is substantially free of carbon dioxide, and may contain for example a few ppm of carbon dioxide;
- air is separated in an air separation apparatus, preferably by cryogenic distillation, in order to produce an oxygen-rich flow containing at most 99% oxygen, preferably at most 98% oxygen, or at most 97 mol % of oxygen, and argon, preferably at least 2 mol % of argon, or at least 3 mol % of argon, and the oxygen-rich flow is sent to the installation consuming oxygen, preferably the oxy-fuel combustion;
- the oxygen-enriched fraction is used for the oxy-combustion of the fuel and/or for the pretreatment of the residual gas depleted of carbon dioxide;
- the treatment also makes it possible to recover a fraction enriched or rich in nitrogen;
- one or more fluid(s) which come from a unit for separating gas from air or the unit for separating the gases in air, delivering at least part of the oxygen for the oxy-fuel combustion, are used in the treatment of the flow lean in carbon dioxide;
- the flow lean in carbon dioxide is cooled upstream of the cryogenic treatment, the flow lean in carbon dioxide being substantially free of carbon dioxide;
- the flow lean in carbon dioxide is cooled upstream of the cryogenic treatment, and at the same time it is purified with respect to carbon dioxide, the flow lean in carbon dioxide containing carbon dioxide;
- the flow lean in carbon dioxide is cooled in at least one reversible exchanger or in an exchanger of the regenerator type, and the flow produced is sent to a column of the cryogenic treatment unit;
- one of these fluids is a nitrogen-rich liquid which at least partially keeps cold the cryogenic treatment of the flow lean in carbon dioxide;
- no fluid intended for or coming from a column of the treatment unit is expanded in a turbine;
- the flow lean in carbon dioxide is sent to a first column, optionally having a bottom reboiler, and separated to form an oxygen-enriched fluid and a nitrogen-enriched fluid, and an intermediate flow is drawn off from the first column and sent to the bottom of a second column where it is enriched with argon to form a/the argon-enriched fraction;
- an argon-enriched fraction is drawn off from the second column to be sent to a denitrogenation column in order to form an argon-rich fraction;
- one or more fluid(s) which come from a unit for separating gas from air or the unit for separating the gases in air, delivering at least part of the oxygen for the installation supplied with oxygen, for example the oxy-fuel combustion, are used in the treatment of the flow lean in carbon dioxide;
- at least one column of the unit for separating gas from air and at least one column of the treatment unit are contained in a single coldbox;
- one of these fluids is a nitrogen-rich gas which will be used as a cycle gas for at least one reboiler and/or at least one condenser of the cryogenic treatment;
- the pretreatment removes at least 50%, or even substantially 100%, of the carbon dioxide in the residual gas before the cryogenic treatment;
- the pretreatment is carried out at least partially by antisublimation/sublimation of the carbon dioxide in a plurality of exchangers in parallel;
- the sublimation of the carbon dioxide is carried out in the presence of the oxygen-enriched fraction so as to constitute a carbon dioxide/oxygen mixture used for the oxy-combustion of the fuel;
- the pretreatment is carried out at least partly by a process of the TSA, PSA or VPSA type so as to produce a fraction enriched with carbon dioxide and a fraction depleted of carbon dioxide but enriched with argon;
- the pretreatment is carried out at least partly by an absorption process;
- the absorption process uses an aqueous solution of basic pH;
- the basic pH is obtained by injecting NaOH and/or Na2CO3 and/or NH3;
- the pretreatment is carried out at least partly by an adsorption process;
- the pretreatment is carried out at least in part by permeation;
- the flow enriched with carbon dioxide, produced by the pretreatment, is recycled into the boiler, preferably to the combustion chamber.
- Another subject of the invention provides an installation for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid resulting from a method for purifying a residual gas, the residual gas containing carbon dioxide and argon and/or oxygen, the residual gas being derived from an installation supplied with oxygen containing argon, which is an oxy-fuel combustion installation, comprising:
-
- a unit for purifying the residual gas, consisting of fumes leaving a boiler for oxy-combustion of a fuel by means of a gas rich in oxygen and carbon dioxide, in which case the purification unit may be a low-temperature purification unit so as to produce a fluid enriched with carbon dioxide and a residual fluid depleted of carbon dioxide;
- a unit for pretreatment of the residual fluid in order to obtain a flow enriched with carbon dioxide and a flow lean in carbon dioxide; and
- a unit for cryogenic treatment of the flow lean in carbon dioxide so as to extract therefrom a fraction enriched with argon, a fraction enriched with oxygen and a fraction depleted of argon and/or oxygen.
- According to other optional aspects:
-
- the unit for cryogenic treatment of the flow lean in carbon dioxide comprises at least one exchanger and at least one distillation column;
- at least one exchanger is a reboiler;
- at least one exchanger is a condenser;
- the treatment unit makes it possible to recover a fraction enriched or rich in argon and a fraction enriched or rich in oxygen;
- the installation comprises means for sending the oxygen-enriched fraction to the boiler and/or to the pretreatment unit;
- the treatment also makes it possible to recover a nitrogen-enriched fraction;
- the installation comprises means for sending one or more fluid(s), which come from the unit for separating the gases in air, delivering at least part of the oxygen for the installation supplied with oxygen, for example the oxy-fuel combustion, to the unit for cryogenic treatment of the flow lean in carbon dioxide;
- one of these fluids is a nitrogen-rich liquid for keeping the treatment cold;
- one of these fluids is a nitrogen-rich gas which will be used as a cycle gas for at least one reboiler and/or at least one condenser of the unit for cryogenic treatment of the flow lean in carbon dioxide;
- the pretreatment unit is/comprises a carbon dioxide antisublimation/sublimation unit comprising a plurality of exchangers in parallel;
- the sublimation unit is connected to a conduit for conveying the oxygen-enriched fraction so as to form a mixture of carbon dioxide and oxygen, and optionally means for sending the mixture to the fuel oxy-combustion unit;
- the pretreatment unit is/comprises an installation of the TSA, PSA or VPSA type which produces a fraction enriched with carbon dioxide and a fraction depleted of carbon dioxide but enriched with argon;
- the pretreatment unit is/comprises an absorption installation;
- the absorption process uses an aqueous solution of basic pH;
- the basic pH is obtained by injecting NaOH, Na2CO3, NH3;
- the absorption process is a process of washing with methanol;
- the pretreatment unit is/comprises a permeation unit;
- the installation comprises means for recycling the flow enriched with carbon dioxide from the pretreatment unit into the boiler.
- The oxygen sent by the air separation apparatus to the oxy-fuel combustion comprises at most 98 mol % of oxygen, preferably at most 97 mol % of oxygen, or at most 96 mol % of oxygen.
- The oxygen sent by the air separation apparatus to the installation, for example the oxy-fuel combustion, comprises at least 1 mol % of argon, preferably at least 2 mol % of argon, or at least 3 mol % of argon.
- The argon-enriched gas produced by the apparatus comprises at least 50 mol % of argon, preferably at least 70 mol % of argon, or at least 90 mol % of argon.
- The invention will be described in more detail with reference to the figures.
FIG. 1 shows an oxy-fuel combustion installation comprising units for purifying the fumes,FIG. 2 shows the units for purifying the fumes in more detail,FIG. 3 shows a unit for purifying the fumes with respect to CO2 at low temperature,FIG. 4 shows an apparatus for recovering nitrogen and/or oxygen and/or argon from a residual gas of the unit ofFIG. 4 , andFIG. 5 shows a variant ofFIG. 4 . -
FIG. 1 is a schematic view of an oxy-fuel combustion installation. Anair separation apparatus 2 produces anoxygen flow 10 with a typical purity of 95 mol % so as to maximize its argon content, and aresidual nitrogen flow 13. The apparatus also producesgaseous nitrogen 13, andliquid nitrogen 159 which is intended for treatment of the incondensables. Theoxygen flow 10 is divided into twofactions fume recycle flow 15 passes through the units 3 in which thecoal 14 is converted into powder. Thefraction 11 is mixed with the recycle flow downstream of the unit 3, and the mixture is sent to the combustion chamber of the boiler 1. Thefraction 12 is mixed with a secondaryfume recycle flow 16, which provides the burners with ballast in order to maintain the temperatures at acceptable levels.Water 17 is sent to the boiler 1 in order to produce steam 18, which is expanded in a turbine 8.Fumes 19 rich in CO2, typically containing more than 70 mol % (not counting the steam) undergo several treatments in order to remove impurities. The unit 4 removes the NOx, for example by catalysis. Theunit 5 subsequently removes the dust, and after this theunit 6 is a desulfurization system for removing the SO2 and/or the SO3. Theunits 4 and 6 may be superfluous, depending on the composition of the product required. The purifiedflow 24 coming from the unit 6 (or 5 if there is no 6) is sent to a compression and purification unit 7 in order to produce a relatively pure flow ofCO 2 25 and aresidual flow 26. -
FIG. 2 is a schematic view of the compression and purification unit 7 ofFIG. 1 . A flow 110 (corresponding to theflow 24 ofFIG. 1 ) enters aunit 101 in which it is prepared upstream of the compression in theunit 102. In theunit 101, theflow 110 may be purified with respect to dust, SO2 and/or SO3, and/or cooled. - The
residual flow 111 produced by theunit 101 may be condensed water, dust or H2SO4, HNO3, Na2SO4, CaSO4, Na2CO3, CaCO3, etc. - The
compression unit 102 compresses theflow 112 coming from theunit 101, from a pressure close to atmospheric pressure to a high pressure of between 15 and 60 bar abs, preferably around 30 bar abs. This compression may be carried out in a plurality of steps with intermediate cooling. In this case,condensates 113 may be produced. The heat of compression may be recovered in order to preheat thewater 17. Ahot flow 114 leaves thecompression unit 102 and enters theunit 103. This unit cools theflow 114, dries it and optionally purifies it with respect to mercury, producingresiduals 115, 116 and 117. - The
unit 104 is a low-temperature purification unit. In this case, “low-temperature” means a minimum temperature in the cycle of the purification process below 0° C. and preferably below −20° C., or even as close as possible to the triple point of pure CO2 at −56.6° C. In this unit, theflow 118 is cooled and partially condensed in one or more steps. One or more flows enriched with CO2 are expanded and vaporized in order to obtain a product enriched withCO 2 119. A high-pressure flow ofincondensables 120 is recovered from theunit 104 and sent to apretreatment unit 122. Thepretreated flow 123 is sent to atreatment unit 124 in which one or more fluids are produced, which may be liquid and/orgaseous nitrogen 125 and/or liquid and/orgaseous oxygen 126 and/or gaseous and/orliquid argon 127. - The product rich in
CO 2 119 is compressed in acompression unit 105. In theunit 105, thecompressed flow 121 is condensed and may be pumped. -
FIG. 3 shows a low-temperature purification apparatus which corresponds to theunit 104 ofFIG. 2 . Theflow 118 comprising fumes at about 30 bar and at a temperature of between 15° C. and 43° C. is filtered at 3 in order to form theflow 5. Theflow 118 comprises above all carbon dioxide as well as NO2, oxygen, argon and nitrogen. It may be produced directly at high pressure by theunit 103, or it may be compressed by a compressor (in dashes) 2. Theflow 5 is cooled in an exchange line 9 and is partially condensed. A part 7 of theflow 5 is not cooled in the exchange line 9, but instead mixed with the rest of theflow 5 downstream of the exchange line in order to vary the temperature of the mixture. The partially condensed flow is sent to afirst phase separator 11 and separated into agas phase 13 and aliquid phase 17. Thegas phase 13 is divided into two in order to form aflow 15 and aflow 21. Theflow 21 is used for reboiling the column 43 in theexchanger 25, then is sent to a second phase separator 22. Theflow 15 short-circuits the reboilers in order to regulate the reboiling. - The liquid 17 from the
first phase separator 11 is expanded in avalve 19 and theliquid flow 29 of the second phase separator 22 is expanded in a valve 31, and the two expanded flows are then sent to the head of the column 43. The column 43 is used principally to remove the incondensable components (oxygen, nitrogen and argon) from thefeed flow 118. - A flow depleted of
carbon dioxide 33 is drawn off from the head of the column 43 and sent to thecompressor 35. The compressed flow 37 produced in this way is recycled to theflow 5. - A flow enriched or rich in carbon dioxide 67 is drawn off from the bottom of the column 43 and divided into two. One
part 69 is pumped by thepump 71 in order to form aflow 85, subsequently pumped in thepump 87 and then removed from the system. Theflow 85 corresponds to theflow 25 ofFIG. 1 . Theremainder 73 of the flow 67 is used to keep the apparatus cold. - It is recommendable to purify the
flow 118 with respect to NO2. - The incondensables may be separated before or after the NO2 separation.
- In
FIG. 3 , after the split from theflow 69, theremainder 73 of the flow enriched with carbon dioxide is vaporized in the exchange line 9 and sent to a column for purification with respect to NO2 105. - This column may have a head condenser and a bottom reboiler, the
flow 73 being delivered to an intermediate point. Otherwise, if there is no bottom reboiler, the flow is delivered to the bottom. - A flow lean in NO2 79 is drawn off from the
column 105 and returned to the exchange line 9. Thisflow 79 is heated, compressed in thecompressors exchanger 65, drawn off as theflow 78, cooled in the exchangers 81, 83 and mixed with theflow 69 in order to form theflow 85. The exchanger 81 may be used to heat the water intended for a boiler. The exchanger 83 is cooled by a flow ofrefrigerant 185, which may be R134a, ammonia, water, etc., the heated refrigerant being denoted as 187. A flow enriched with NO2 84 is drawn off from the bottom of thecolumn 105. This flow 84 is recycled to a point upstream of the filters 3. - Head gas 32 from the second phase separator 22 is cooled in the exchanger 55 and sent to the
third phase separator 133. A part of the liquid from thethird phase separator 133 is sent to the column 43 and the remainder, as a flow withintermediate purity 45, is divided into twoflows 47, 141. The flow 47 is vaporized in the exchanger 55 and sent to the head of the column 43 or mixed with theflow 33. - The
flow 141 is expanded in a valve, heated in the exchangers 55, 9, compressed in the compressor 59, cooled as aflow 91 in the exchanger 60 and mixed with thecompressed flow 5. The valve which is used to expand theflow 141 may be replaced by a liquid turbine. - The head gas from the
third phase separator 133 is cooled in a heat exchanger 55, optionally after compression in acompressor 134, and sent to afourth phase separator 143. The head gas, lean incarbon dioxide 157, from thefourth phase separator 143 is heated in a heat exchanger 55, then in the exchanger 9, heated in theexchanger 65 and expanded as a flow 23 in theexchanger 63 coupled to thecompressor 35. The gas lean incarbon dioxide 157 comprises between 30 and 45% of carbon dioxide and between 30 and 45% of nitrogen. It also comprises substantial quantities of oxygen and argon. The bottom liquid 51 from thephase separator 143 is sent to the column 43 with the flow 47. - The flow expanded in the
turbine 63 is mixed with theflow 115 which does not pass through the turbine, and subsequently reheated at 89. Apart 97 of the heated flow is expanded in the turbine 61 and sent to the atmosphere as aflow 99. - A
flow 120 rich in incondensables (oxygen and/or argon and/or nitrogen) and containing CO2 is recovered in theunit 104 in order to recover at least one of its components as a product. Thisflow 120 may be a part of theflow 101 coming from the turbine 61 and/or a part of thehead gas 157 from thefourth phase separator 143 upstream of the exchanger 55 and/or a part of the flow expanded in theturbine 63 and/or a part of theflow 157 downstream of the exchanger 9. -
TABLE 1 Molar fractions in percentages (example) for O2, N2, Ar, CO2. FLUIDS/ Components 118 33 67 84 157 141 78 O2 2.5 4.8 0 0 13.3 2.3 0 N2 7.8 11 0 0 43.8 0.1 0 Ar 1.9 4.9 0 0 9.5 2.6 0 CO2 87.8 79.3 99.95 99 33.4 95 100 NOx 250 50 ppm 500 1 5 ppm 500 ppm 0 ppm ppm -
FIG. 4 shows an apparatus for pretreatment and an apparatus for separation by cryogenic distillation of theflow 120. Thisflow 120 is first pretreated in thepretreatment unit 122. This pretreatment unit removes at least 50 mol % of the carbon dioxide in theresidual gas 120, before the cryogenic treatment producing a flow 169 enriched with CO2 which can be recycled to theunit 104 with theflow 118. - The pretreatment may be carried out by antisublimation/sublimation of the carbon dioxide in a plurality of exchangers in parallel. As an alternative, the pretreatment may be carried out by absorption (for example washing with methanol), adsorption, permeation or several of these techniques.
- The sublimation of the carbon dioxide is carried out, for example, in the presence of an oxygen-enriched fraction so as to form a mixture of carbon dioxide and oxygen used for the oxy-combustion of the fuel. By virtue of the anti-sublimation, the temperature of the treated gas falls from −56.6° C. (triple point of CO2) to −170° C/−175° C., a temperature at which cryogenic distillation of the gases in air can be carried out.
- Otherwise, the pretreatment may be carried out by a process of the TSA, PSA or VPSA type so as to produce a fraction enriched with carbon dioxide and a fraction depleted of carbon dioxide but enriched with argon.
- The pretreatment may be carried out by an absorption process, using for example an aqueous solution of basic pH. The basic pH is optionally obtained by injecting NaOH and/or Na2CO3 and/or NH3. The absorption process may also use a non-aqueous fluid such as methanol. In this case, the absorption will be carried out at low temperature and preferably under pressure.
- As an alternative, the pretreatment is carried out by permeation or by a combination of the various processes mentioned.
- It is possible to remove all the carbon dioxide in the pretreatment unit in order then to deliver a flow containing a few ppm of carbon dioxide. This makes it possible to use a plate exchanger and a finned exchanger as exchangers.
- On the other hand, if the
flow 123 still contains carbon dioxide, it is necessary to continue the pretreatment by using reversible exchangers or exchangers of the regenerator type, as described on page 475 of “Tieftemperaturtechnik” [Low-temperature technology], sections 9.4.2.3 and 9.4.2.4, pub. Springer Verlag. Thus, the remaining carbon dioxide may be removed by passing through anexchanger 130 of one of these two types. Clearly, thefeed flow 123 should no longer contain more than a few ppm of carbon dioxide at the entry of the columns. - After the pretreatment, the flow depleted of
carbon dioxide 123 is sent to acryogenic distillation unit 124 as illustrated inFIG. 4 . Theflow 123 is cooled to a cryogenic temperature in anexchanger 130 and sent to the middle of acolumn 131 having abottom reboiler 133. As an alternative, theflow 123 could be cooled by expansion in a turbine with production of work (isentropic expansion). Gaseous oxygen GOX is drawn off from above the bottom of thecolumn 131, heated in theexchanger 130 and used as aproduct 126 and/or recycled to thepretreatment 122 and/or to the boiler 1.Liquid oxygen 136 may be drawn off from the bottom of thecolumn 131, for example as a product. An argon-enrichedflow 141 is sent from thecolumn 131 to thecolumn 137, and a flow ofimpure argon 145 is drawn off from below thecondenser 155 of thiscolumn 137. A flow ofbottom liquid 143 is returned to thecolumn 131. Theimpure argon 145 is purified in adenitrogenation column 139 comprising ahead condenser 153 and abottom reboiler 151.Liquid argon 127 is produced at the bottom of thedenitrogenation column 139. The apparatus is kept cold at least partially by injectingliquid nitrogen 159 coming from theair separation apparatus 2 supplying the oxy-fuel combustion. Theliquid nitrogen 159 is sent to the head of thecolumn 131. Thisair separation apparatus 2 also deliversgaseous nitrogen 13, which is cooled in theexchanger 130 and heats thebottom reboiler 133 of thecolumn 131 in order to form a condensed flow. The condensed flow is sent inpart 147 after expansion to thehead condenser 153 of thedenitrogenation column 139, inpart 165 to thehead condenser 155 of thecolumn 137 and inpart 157 after expansion to the head of thecolumn 131. Thenitrogen 163 vaporized in thecondenser 153 is mixed with thehead gas 135 of thecolumn 131, heated in thesubcooler 160 and theexchanger 130, and forms thegaseous nitrogen 165. Thenitrogen 161 vaporized in thecondenser 155 forms thenitrogen flow 161. - At least one column of the
apparatus 124 may optionally be contained in the same coldbox as at least one column of theapparatus 2. The transfers ofnitrogen 13 and/or 159 can thus take place without having to reheat and cool the nitrogen. For the case ofFIG. 4 , thecolumns -
FIG. 5 shows a variant of the cold part ofFIG. 4 , in which thecold mixture 123 coming from theexchanger 130 is sent to an intermediate level of acolumn 163 without a reboiler or head condenser. Thehead gas 171 from thecolumn 163 constitutes the gaseous nitrogen, and thebottom liquid 173 is sent to acolumn 165 at an intermediate position.Gas 175 is returned from the intermediate position of thecolumn 165 to the bottom of thecolumn 163. Thecolumn 165 has abottom reboiler 175 and ahead condenser 177.Gaseous oxygen 126 and/orliquid oxygen 136 is recovered at the bottom of thecolumn 165, and thehead liquid 145 is sent to adenitrogenation column 167, the liquid argon being formed 127 in the bottom of the latter. The denitrogenation column has abottom reboiler 151 and ahead condenser 153. -
Liquid nitrogen 159 coming from theair separation apparatus 2 is sent to the head of thecolumn 163. Thecolumn 163 has a head condenser which, like all the reboilers and condensers ofFIG. 5 , operates by a cycle of gaseous nitrogen coming from theair separation apparatus 2, which cycle is not illustrated but is similar to that ofFIG. 4 . - Optionally, the delivery of
liquid nitrogen 159 may constitute the only source of cooling for the process. - Ways of separating the
flow 123 by cryogenic distillation other than those illustrated inFIGS. 4 and 5 may of course be envisaged.
Claims (27)
1-18. (canceled)
19. A method for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid resulting from a method for purifying a residual gas, the residual gas containing carbon dioxide and oxygen and/or argon, the residual gas being derived from an installation supplied with oxygen containing argon, which is an oxy-fuel combustion installation, comprising the following steps:
recovering fumes resulting from the oxy-combustion of a fuel by means of a gas rich in oxygen and in carbon dioxide and containing argon in the combustion chamber of a boiler as they leave the boiler,
purifying the fumes by a low-temperature purification method, so as to produce a first stream enriched with carbon dioxide and a residual fluid depleted of carbon dioxide;
pre-treating the residual fluid depleted of carbon dioxide in order to obtain a second stream enriched with carbon dioxide and a stream lean in carbon dioxide; and
cryogenically treating the stream lean in carbon dioxide so as to extract therefrom at least one fraction enriched or rich in argon and at least one fraction enriched or rich in oxygen and at least one fraction depleted of argon and/or oxygen.
20. The method of claim 19 , wherein the cryogenic treatment of the stream lean in carbon dioxide further comprises a step of cooling in at least one exchanger, and a step of distillation in a distillation column.
21. The method of claim 20 , wherein said at least one exchanger is selected from the group consisting of a reboiler, a condenser, a reversible exchanger, and a regenerator exchanger.
22. The method of claim 19 , wherein the air is separated in an air separation apparatus, in order to produce an oxygen-rich flow containing at most 99% oxygen, and argon, and the oxygen-rich flow is sent to the oxy-fuel combustion.
23. The method of claim 22 , wherein the air separation is by cryogenic distillation.
24. The method of claim 22 , wherein the oxygen-rich flow contains at most 98% oxygen.
25. The method of claim 22 , wherein the oxygen-rich flow contains at most 97% oxygen
26. The method of claim 22 , wherein the oxygen-rich flow contains at least 2 mol % of argon.
27. The method of claim 22 , wherein the oxygen-rich flow contains at least 3 mol % argon.
28. The method of claim 19 , wherein the fraction enriched or rich in oxygen is used for the oxy-combustion of the fuel and/or for the pretreatment of the residual gas depleted of carbon dioxide.
29. The method of claim 19 , wherein the cryogenic treatment recovers a fraction enriched or rich in nitrogen.
30. The method of claim 23 , wherein one or more fluid(s) which come from a unit for separating gas from air or the unit for separating the gases in air, delivering at least part of the oxygen for the installation supplied with oxygen, are used in the treatment of the stream lean in carbon dioxide, wherein at least one column of the unit for separating gas from air and at least one column of the treatment unit may be contained in a single coldbox.
31. The method of claim 30 , wherein one of these fluids is a nitrogen-rich liquid which at least partially cools the cryogenic treatment of the flow lean in carbon dioxide.
32. The method of claim 30 wherein one of these fluids is a nitrogen-rich gas which will be used as a cycle gas for at least one reboiler and/or at least one condenser of the cryogenic treatment.
33. The method of claim 23 , wherein the pre-treatment removes at least 50 mol % of the carbon dioxide in the residual gas before the cryogenic treatment.
34. The method of claim 33 , wherein the pre-treatment is carried out at least partially by antisublimation/sublimation of the carbon dioxide in a plurality of exchangers in parallel.
35. The method of claim 34 , wherein the sublimation of the carbon dioxide is carried out in the presence of the oxygen-enriched fraction so as to constitute a carbon dioxide/oxygen mixture used for the oxy-combustion of the fuel.
36. The method of claim 19 , wherein the pre-treatment is carried out at least partly by a process of the TSA, PSA or VPSA type thereby producing a fraction enriched with carbon dioxide and a fraction depleted of carbon dioxide but enriched with argon.
37. The method of claim 19 , wherein the pre-treatment is carried out at least partly by an absorption process.
38. The method of claim 19 , wherein the pre-treatment is carried out by washing with methanol.
39. The method of claim 19 , wherein the pretreatment is carried out at least in part by permeation.
40. The method of claim 19 , wherein the flow enriched with carbon dioxide, produced by the pretreatment, is recycled into the installation consuming oxygen.
41. The method of claim 40 , wherein the flow enriched with carbon dioxide is recycled to the oxy-fuel combustion boiler.
42. The method of claim 40 , wherein the flow enriched with carbon dioxide is recycled to the combustion chamber.
43. An installation for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid resulting from a method for purifying a residual gas, the residual gas containing carbon dioxide and argon and/or oxygen, the residual gas being derived from an installation supplied with oxygen containing argon, which is an oxy-fuel combustion installation, comprising:
a unit for purifying the residual gas, comprising fumes leaving a boiler for oxy-combustion of a fuel by means of a gas rich in oxygen and carbon dioxide, in which case the purification unit may be a low-temperature purification unit so as to produce a fluid enriched with carbon dioxide and a residual fluid depleted of carbon dioxide;
a unit for pretreatment of the residual fluid in order to obtain a flow enriched with carbon dioxide and a flow lean in carbon dioxide; and
a unit for cryogenic treatment of the flow lean in carbon dioxide so as to extract therefrom a fraction enriched with argon, a fraction enriched with oxygen and a fraction depleted of argon and/or oxygen.
44. The installation as claimed in claim 43 , wherein the unit for cryogenic treatment of the flow lean in carbon dioxide comprises at least one exchanger and at least one distillation column.
Applications Claiming Priority (3)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR0953648A FR2946417A1 (en) | 2009-06-03 | 2009-06-03 | METHOD AND APPARATUS FOR PRODUCING AT LEAST ONE ARGON-ENRICHED FLUID AND / OR AT LEAST ONE OXYGEN-ENRICHED FLUID FROM A RESIDUAL FLUID |
FR0953648 | 2009-06-03 | ||
PCT/FR2010/051031 WO2010139884A2 (en) | 2009-06-03 | 2010-05-28 | Method and apparatus for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid |
Publications (1)
Publication Number | Publication Date |
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US20120067082A1 true US20120067082A1 (en) | 2012-03-22 |
Family
ID=41820086
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
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US13/375,256 Abandoned US20120067082A1 (en) | 2009-06-03 | 2010-05-28 | Method and apparatus for producing at least one argon-enriched fluid and at least one oxygen-enriched fluid from a residual fluid |
Country Status (7)
Country | Link |
---|---|
US (1) | US20120067082A1 (en) |
EP (1) | EP2438378A2 (en) |
CN (1) | CN102695935A (en) |
AU (1) | AU2010255559A1 (en) |
CA (1) | CA2762237A1 (en) |
FR (1) | FR2946417A1 (en) |
WO (1) | WO2010139884A2 (en) |
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US20130098244A1 (en) * | 2010-05-31 | 2013-04-25 | Mitsubishi Heavy Industries, Ltd. | Air pollution control system and method |
US20130142712A1 (en) * | 2010-05-31 | 2013-06-06 | Mitsubishi Heavy Industries, Ltd. | Air pollution control system and method |
US8871164B2 (en) | 2010-05-31 | 2014-10-28 | Mitsubushi Heavy Industries, Ltd. | Air pollution control system and method |
US8894941B2 (en) | 2010-05-31 | 2014-11-25 | Mitsubishi Heavy Industries, Ltd. | Air pollution control system and method |
US20160216013A1 (en) * | 2013-09-10 | 2016-07-28 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Method and device for separation at sub-ambient temperature |
US10835862B2 (en) | 2010-05-31 | 2020-11-17 | Mitsubishi Heavy Industries Engineering, Ltd. | Air pollution control system and method |
FR3119227A1 (en) * | 2021-01-27 | 2022-07-29 | L'air Liquide, Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Method and apparatus for separating a stream rich in carbon dioxide by distillation to produce liquid carbon dioxide |
US11913718B2 (en) | 2019-11-27 | 2024-02-27 | L'air Liquide Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Argon and power production by integration with power plant |
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CN105688597B (en) * | 2016-03-31 | 2018-06-05 | 四川天采科技有限责任公司 | A kind of full temperature journey pressure swing absorption process that hydro carbons is recycled from low-temperature methanol washing tail-gas |
US11104576B2 (en) * | 2017-06-27 | 2021-08-31 | Casale Sa | Process for argon and nitrogen production |
US10663224B2 (en) * | 2018-04-25 | 2020-05-26 | Praxair Technology, Inc. | System and method for enhanced recovery of argon and oxygen from a nitrogen producing cryogenic air separation unit |
CN113797700A (en) * | 2021-09-22 | 2021-12-17 | 乔治洛德方法研究和开发液化空气有限公司 | Integrated unit and method for separating air and producing carbon dioxide-rich product |
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US20130142712A1 (en) * | 2010-05-31 | 2013-06-06 | Mitsubishi Heavy Industries, Ltd. | Air pollution control system and method |
US8871164B2 (en) | 2010-05-31 | 2014-10-28 | Mitsubushi Heavy Industries, Ltd. | Air pollution control system and method |
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US11913718B2 (en) | 2019-11-27 | 2024-02-27 | L'air Liquide Societe Anonyme Pour L'etude Et L'exploitation Des Procedes Georges Claude | Argon and power production by integration with power plant |
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Also Published As
Publication number | Publication date |
---|---|
FR2946417A1 (en) | 2010-12-10 |
AU2010255559A1 (en) | 2011-12-22 |
CA2762237A1 (en) | 2010-12-09 |
EP2438378A2 (en) | 2012-04-11 |
WO2010139884A2 (en) | 2010-12-09 |
WO2010139884A3 (en) | 2012-11-15 |
CN102695935A (en) | 2012-09-26 |
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