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WO2010052400A1 - Method and device for capturing carbon dioxide on industrial gases at a low temperature - Google Patents

Method and device for capturing carbon dioxide on industrial gases at a low temperature Download PDF

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Publication number
WO2010052400A1
WO2010052400A1 PCT/FR2009/052010 FR2009052010W WO2010052400A1 WO 2010052400 A1 WO2010052400 A1 WO 2010052400A1 FR 2009052010 W FR2009052010 W FR 2009052010W WO 2010052400 A1 WO2010052400 A1 WO 2010052400A1
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carbon dioxide
reactor
loop
potassium
fluidized
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French (fr)
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Jean-Xavier Morin
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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
    • B01D53/34—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
    • 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
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/81—Solid phase processes
    • B01D53/83—Solid phase processes with moving reactants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/96—Regeneration, reactivation or recycling of reactants
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/30—Alkali metal compounds
    • B01D2251/306—Alkali metal compounds of potassium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2251/00—Reactants
    • B01D2251/60—Inorganic bases or salts
    • B01D2251/604—Hydroxides
    • 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
    • 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 invention relates to a method and a device for capturing carbon dioxide on low temperature industrial gases.
  • This post-capture system of carbon dioxide capture is mainly carried out by gas / liquid and is theoretically adapted to the carbon dioxide capture plant on existing units. But it uses amine-type solvents or ammonia compounds that require very high energies of regeneration. The impact of this regenerative energy consumption causes the large power plants to lose up to 12 points of efficiency, which makes this post-capture system of carbon dioxide capture uneconomical since the cost of such a catch reaches sixty Euros per tonne of carbon dioxide capture, which significantly increases the cost of electricity produced from fossil fuels.
  • the degradation products of these solvents are very toxic and carcinogenic and present risks to the environment and health when they are present even in trace amounts in the capture of carbon dioxide for underground storage in aquifers. Finally, these used solvents are very corrosive to carbon steel pipelines used for economic reasons, for long distance transport to underground storage areas of carbon dioxide capture.
  • the patent document US Pat. No. 5,665,319 describes a method of capturing carbon dioxide on a gas according to which this gas is brought into contact with a metal oxide, in order to fix the carbon dioxide in the form of a carbonate, and the formed carbonate is thermally decomposed into metal oxide by contact with a combustion gas produced by combustion of a fuel with oxygen.
  • the device for implementing this method comprises two reactors, interconnected to allow the realization of a thermochemical loop.
  • the metal oxide is preferably calcium oxide and to achieve the absorption of carbon dioxide and the capture of this carbon dioxide in the so-called absorption reactor, the treated gas must be at a temperature of 600 0 C to 700 0 C at ambient pressure.
  • Such an arrangement of interconnected thermochemical loop reactors using calcium oxide must therefore be inserted into a reactor to treat gases at this temperature.
  • this carbon dioxide capture process can not be adapted to the purification of gases or fumes produced by a boiler without specific design and / or consequent adaptation of the boiler in question.
  • the aim of the invention is to solve this problem by proposing a process for dry capture of carbon dioxide on industrial gases at low temperature, which may be suitable for very high flue gas flows from 1000 MWe plants for example, minimizing the regeneration energy of carbon dioxide transfer media and especially with little impact on existing boiler units.
  • the invention relates to a process for capturing carbon dioxide on industrial gases by means of two thermochemically looped fluidized bed fluidized-bed reactor loops, wherein said gases are brought into contact with a metal compound in the first loop, in order to set the carbon dioxide in the form of a carbonate, characterized in that said metal compound is potassium-based and said carbonate is potassium carbonate.
  • the process according to the invention is perfectly adapted to the low temperature of the order of 80 to 200 ° C. of the gases or fumes to be treated and it makes it possible to achieve total autothermicity by means of specific formulations of the metal compound and by virtue of a flow of solid flows required by large applications.
  • potassium-based metal compound compounds mainly potassium-based, containing possible impurities.
  • the invention also relates to a carbon dioxide capture device for implementing the method as specified above, characterized in that said two reactor loops are fast fluidized bed loops each comprising a reactor connected in part. high to a solids separator connected to its solids outlet to a return line at the bottom of the reactor and in that these two loops are interconnected from each return line of one of the reactors to the lower part of the reactor of the reactor. 'other.
  • the invention finally relates to a use of such a carbon dioxide capture device, characterized in that it is installed at the outlet of fumes or industrial gases from a boiler or a smoke generator.
  • the invention applies to any treatment of gases or fumes containing carbon dioxide, for example fumes from boilers, furnaces or cement plants, blast furnace gas or industrial gases.
  • Figure 1 is a view of a carbon dioxide capture device according to the invention.
  • Figure 2 is a view of a boiler equipped with such a device.
  • the method according to the invention consists in capturing carbon dioxide on industrial gases by means of two gas-mixing reactors and fast fluidized bed fast-interconnected thermochemical loop-type reactors, in which said gases are brought into contact with a gas.
  • potassium-based alkali compound in the first fluidized reactor using the treated industrial gases to fix the carbon dioxide as potassium carbonate.
  • said alkaline compound is potassium hydroxide which reacts with carbon dioxide according to the formula:
  • the potassium carbonate K 2 CO 3 is then thermally decomposed in the second fluidized reactor by means of water vapor, preferably drawn off from a low pressure turbine of the plant equipped with potassium oxide according to the formula:
  • the heat input into the second reactor can also be carried out by hot solids taken from bed systems. fluidized emitters of carbon dioxide or also by sampling hot fumes.
  • the carbon dioxide is thus separated and after cooling, filtration and purification, compressed and transferred by pipeline to an underground geological storage.
  • the potassium oxide is then hydrated to potassium hydroxide at the inlet of the first reactor according to the formula:
  • This last reaction (3) is followed by a new reaction cycle (1), (2), (3) of the thermochemical loop.
  • the potassium compound with a particle size of between 5 and 50 microns is mixed with an auxiliary bed support, preferably alumina or zeolite, in the form of particles having a particle size of between 10 and 100 microns. It is also possible to use auxiliary bed particles coated with potassium compounds by impregnation and which have the advantage of maintaining their physical integrity during the carbonation and decarbonation cycles.
  • This auxiliary bed support is not susceptible to attrition and is inert from the hydration point of view.
  • This auxiliary bed support circulates between the two reactors with the potassium compounds which are of small particle size on the order of 5 to 50 microns.
  • This auxiliary bed support is essential because the nascent potassium oxides and potassium carbonates are extremely cohesive and sticky hence the need to grind and disperse them permanently in all solid loops.
  • This process selectively transfers carbon dioxide from industrial gases, with carbon dioxide corresponding to about
  • These two reactors are interconnected from the bottom of each return line IC, 2C of one of the reactors to the lower part of the reactor 2A, IA of the other reactor, so that the solids have remained in each zone long enough.
  • reaction in terms of temperature and residence time, in order to control the degree of carbonation and decarbonation in the transferred solids.
  • the reactor IA of the first loop receives the gases or fumes loaded with carbon dioxide to be treated and is fluidized by them.
  • the reactor 2A of the second loop is in turn supplied with water vapor withdrawal.
  • gases of the first loop are evacuated fumes low in carbon dioxide.
  • gases of cyclone 2B of the second loop is recovered a mixture of carbon dioxide and water vapor which is filtered, condensed, compressed and transported for storage.
  • Each reactor loop 1, 2 comprises at least one fluidized-bed exchanger in dense phase or in dilute or mobile phase fed with steam or fumes and controlling their temperature.
  • An exchanger E1, E2 may be disposed on each return line IC 2C upstream of the interconnection in the dense phase and / or an exchanger E1 ', E2' may be arranged in the reactor in the dilute phase.
  • the heat generated by the carbonation by carbon dioxide of the fumes in the form of K 2 CO 3 in the first reactor 1 is transferred by the exchanger El and / or El 'of the first reactor 1, to the circulating solids whose Adjustable flow rate makes it possible to precisely adjust the optimal temperature of carbonation in the loop.
  • the decomposition reaction of K 2 CO 3 in the second reactor 2 is endothermic and uses part of the heat of the solids from the first reactor 1 to effect this decomposition.
  • An external supply of heat is provided by the steam drawn off from the cycle or the hot flue gases of the equipped boiler, thanks to the exchanger E2 and / or E2 'of the second reactor 2.
  • This second reactor 2 is thus lined with insulating materials to limit heat loss to the walls.
  • such a device for capturing carbon dioxide may be installed at the outlet of filtered fumes from a boiler, for example from a pulverized coal boiler C.
  • the reactor loops 1 and 2 are diagrammed on this figure. Only the complementary elements of those of Figure 1 will now be specified.
  • a mixture of carbon dioxide and water vapor which is filtered by the filtration device F2, filter bag, condensed, compressed and transported for geological storage underground.
  • the solids recovered by the filtration device F2 are recycled in the first reactor 1.
  • the loss of charge created by the first reactor 1 is compensated by a booster fan Vl on the flue gases before their introduction into this first reactor.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Biomedical Technology (AREA)
  • Analytical Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Sustainable Development (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Treating Waste Gases (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

The invention relates to a method for capturing carbon dioxide on industrial gases by means of two fluidised bed reactors interconnected in a thermochemical loop, according to which said gases are brought into contact with a metallic component in the first reactor (1) in order to fix the carbon dioxide in the form of a carbonate. According to the invention, the metallic component is based on potassium and the carbonate is potassium carbonate.

Description

PROCEDE ET DISPOSITIF DE CAPTURE DE DIOXYDE DE CARBONE SUR DES GAZ INDUSTRIELS A BASSE TEMPERATURE METHOD AND DEVICE FOR CAPTURING CARBON DIOXIDE ON LOW TEMPERATURE INDUSTRIAL GASES

L'invention concerne un procédé et un dispositif de capture de dioxyde de carbone sur des gaz industriels à basse température.The invention relates to a method and a device for capturing carbon dioxide on low temperature industrial gases.

Les nouvelles réglementations en matière de quotas d'émissions de dioxyde de carbone (CO2) ont fait se développer les technologies de capture du dioxyde de carbone contenu dans les fumées de combustion issues des chaudières industrielles et des grandes centrales de production d'électricité utilisant des combustibles fossiles. Plusieurs techniques de capture du dioxyde de carbone sont en développement soit en éliminant l'azote en amont par une oxycombustion soit par une combinaison sélective dans les fumées de combustion principalement constituées d'azote, appelée procédé de post capture.The new regulations on carbon dioxide (CO2) emission quotas have led to the development of technologies for capturing carbon dioxide contained in combustion fumes from industrial boilers and large electricity generating plants using fossil fuels. fossil fuels. Several techniques for capturing carbon dioxide are being developed either by removing nitrogen upstream by oxyfuel combustion or by a selective combination in combustion fumes mainly consisting of nitrogen, called the post-capture process.

Ce système de post capture du capture du dioxyde de carbone est principalement effectué par voie gaz/liquide et est théoriquement adapté à l'installation de capture du dioxyde de carbone sur des unités existantes. Mais elle utilise des solvants de type aminés ou des composés d'ammoniac qui exigent des énergies très importantes de régénération. L'impact de cette consommation d'énergie de régénération fait perdre sur les grandes centrales de production d'électricité jusqu'à douze points de rendement ce qui rend ce système de post capture du capture du dioxyde de carbone peu économique puisque le coût d'une telle capture atteint soixante Euros la tonne de capture du dioxyde de carbone, ce qui augmente très sensiblement le coût de l'électricité produite à partir de combustibles fossiles. D'autre part les produits de dégradation de ces solvants sont très toxiques et cancérigènes et présentent des risques pour l'environnement et la santé quand ils sont présents même à l'état de traces dans la capture du dioxyde de carbone destiné au stockage souterrain dans des nappes aquifères. Enfin ces solvants usagés sont très corrosifs pour les pipelines en acier au carbone utilisés pour des raisons économiques, pour le transport longue distance vers les zones de stockage souterrain du capture du dioxyde de carbone.This post-capture system of carbon dioxide capture is mainly carried out by gas / liquid and is theoretically adapted to the carbon dioxide capture plant on existing units. But it uses amine-type solvents or ammonia compounds that require very high energies of regeneration. The impact of this regenerative energy consumption causes the large power plants to lose up to 12 points of efficiency, which makes this post-capture system of carbon dioxide capture uneconomical since the cost of such a catch reaches sixty Euros per tonne of carbon dioxide capture, which significantly increases the cost of electricity produced from fossil fuels. On the other hand the degradation products of these solvents are very toxic and carcinogenic and present risks to the environment and health when they are present even in trace amounts in the capture of carbon dioxide for underground storage in aquifers. Finally, these used solvents are very corrosive to carbon steel pipelines used for economic reasons, for long distance transport to underground storage areas of carbon dioxide capture.

Le document de brevet US 5 665 319 décrit quant à lui un procédé de capture du dioxyde de carbone sur un gaz selon lequel ce gaz est mis en contact avec un oxyde métallique, afin de fixer le dioxyde de carbone sous forme d'un carbonate, et le carbonate formé est thermiquement décomposé en oxyde métallique par contact avec un gaz de combustion produit par combustion d'un combustible avec de l'oxygène. Le dispositif pour mettre en œuvre ce procédé comporte deux réacteurs, interconnectés pour permettre la réalisation d'une boucle thermochimique.The patent document US Pat. No. 5,665,319 describes a method of capturing carbon dioxide on a gas according to which this gas is brought into contact with a metal oxide, in order to fix the carbon dioxide in the form of a carbonate, and the formed carbonate is thermally decomposed into metal oxide by contact with a combustion gas produced by combustion of a fuel with oxygen. The device for implementing this method comprises two reactors, interconnected to allow the realization of a thermochemical loop.

L'oxyde métallique est de préférence de l'oxyde de calcium et pour réaliser l'absorption du dioxyde de carbone et la capture de ce dioxyde de carbone dans le réacteur dit d'absorption, le gaz traité doit être à une température de l'ordre de 6000C à 700 0C à pression ambiante. Un tel agencement de réacteurs interconnectés en boucle thermochimique utilisant de l'oxyde de calcium doit donc être inséré dans un réacteur pour traiter des gaz à cette température. Il en résulte que ce procédé de capture de dioxyde de carbone ne peut être adapté à l'épuration de gaz ou de fumées produits par une chaudière sans conception spécifique et/ou adaptation conséquente de la chaudière en question.The metal oxide is preferably calcium oxide and to achieve the absorption of carbon dioxide and the capture of this carbon dioxide in the so-called absorption reactor, the treated gas must be at a temperature of 600 0 C to 700 0 C at ambient pressure. Such an arrangement of interconnected thermochemical loop reactors using calcium oxide must therefore be inserted into a reactor to treat gases at this temperature. As a result, this carbon dioxide capture process can not be adapted to the purification of gases or fumes produced by a boiler without specific design and / or consequent adaptation of the boiler in question.

Le but de l'invention est de résoudre ce problème en proposant un procédé de capture par voie sèche du dioxyde de carbone sur des gaz industriels à basse température, pouvant convenir à de très grands débits de fumées provenant de centrales de 1000 MWe par exemple, minimisant l'énergie de régénération des supports transférant le dioxyde de carbone et surtout avec peu d'impact sur les unités de chaudières existantes.The aim of the invention is to solve this problem by proposing a process for dry capture of carbon dioxide on industrial gases at low temperature, which may be suitable for very high flue gas flows from 1000 MWe plants for example, minimizing the regeneration energy of carbon dioxide transfer media and especially with little impact on existing boiler units.

Pour ce faire, l'invention concerne un procédé de capture de dioxyde de carbone sur des gaz industriels au moyen de deux boucles de réacteurs à lit fluidisé interconnectés en boucle thermochimique, selon lequel lesdits gaz sont mis en contact avec un composé métallique dans la première boucle, afin de fixer le dioxyde de carbone sous forme d'un carbonate, procédé caractérisé en ce que ledit composé métallique est à base de potassium et ledit carbonate est du carbonate de potassium.To this end, the invention relates to a process for capturing carbon dioxide on industrial gases by means of two thermochemically looped fluidized bed fluidized-bed reactor loops, wherein said gases are brought into contact with a metal compound in the first loop, in order to set the carbon dioxide in the form of a carbonate, characterized in that said metal compound is potassium-based and said carbonate is potassium carbonate.

Le procédé conforme à l'invention est parfaitement adapté à la basse température de l'ordre de 80 à 200 0C des gaz ou fumées à traiter et il permet d'atteindre la totale autothermicité grâce à des formulations spécifiques du composé métallique et grâce à une circulation de débits de solides exigés par les applications de grande taille.The process according to the invention is perfectly adapted to the low temperature of the order of 80 to 200 ° C. of the gases or fumes to be treated and it makes it possible to achieve total autothermicity by means of specific formulations of the metal compound and by virtue of a flow of solid flows required by large applications.

Ce procédé fonctionne globalement en autothermicité. La capacité à effectuer cette production par une seule unité et non pas des trains multiples amène à des réductions très importantes de coût, d'investissement.This process works globally in autothermicity. The ability to perform this production by a single unit and not multiple trains leads to very significant reductions in cost and investment.

La caractéristique de pouvoir capter le dioxyde de carbone à basse température entraîne l'absence de modifications importantes sur les émetteurs de dioxyde de carbone, que constituent notamment les chaudières industrielles et les grandes centrales de production d'électricité utilisant des combustibles fossiles. Le fait de pouvoir installer de tels systèmes de capture de dioxyde de carbone sans arrêter la production principale d'électricité constitue un gain économique considérable. Par « composé métallique à base de potassium », il est ici entendu les composés principalement à base de potassium, contenant d'éventuelles impuretés.The characteristic of being able to capture carbon dioxide at low temperatures leads to the absence of significant modifications to carbon dioxide emitters, such as industrial boilers and large fossil fuel power plants. Being able to install such carbon dioxide capture systems without stopping the main production of electricity is a considerable economic gain. By "potassium-based metal compound" is meant here compounds mainly potassium-based, containing possible impurities.

L'invention concerne également un dispositif de capture de dioxyde de carbone pour la mise en œuvre du procédé tel que précisé ci-dessus, caractérisé en ce que lesdites deux boucles de réacteurs sont des boucles à lit fluidisé rapide comportant chacun un réacteur connecté en partie haute à un séparateur de solides relié à sa sortie de solides à une conduite de retour en partie basse du réacteur et en ce que ces deux boucles sont interconnectées de chaque conduite de retour de l'un des réacteurs vers la partie basse du réacteur de l'autre. L'invention concerne enfin une utilisation d'un tel dispositif de capture de dioxyde de carbone, caractérisé en ce qu'il est installé en sortie de fumées ou de gaz industriels en provenance d'une chaudière ou d'un générateur de fumée.The invention also relates to a carbon dioxide capture device for implementing the method as specified above, characterized in that said two reactor loops are fast fluidized bed loops each comprising a reactor connected in part. high to a solids separator connected to its solids outlet to a return line at the bottom of the reactor and in that these two loops are interconnected from each return line of one of the reactors to the lower part of the reactor of the reactor. 'other. The invention finally relates to a use of such a carbon dioxide capture device, characterized in that it is installed at the outlet of fumes or industrial gases from a boiler or a smoke generator.

De façon générale, l'invention s'applique à tout traitement de gaz ou fumées contenant du dioxyde de carbone, par exemple les fumées de chaudières, de fours ou de cimenteries, les gaz de haut fourneau sidérurgique ou les gaz industriels.In general, the invention applies to any treatment of gases or fumes containing carbon dioxide, for example fumes from boilers, furnaces or cement plants, blast furnace gas or industrial gases.

L'invention est décrite ci-après à l'aide de figures ne représentant qu'un mode de réalisation préféré de l'invention. La figure 1 est une vue d'un dispositif de capture du dioxyde de carbone conforme à l'invention.The invention is described below with the help of figures representing only a preferred embodiment of the invention. Figure 1 is a view of a carbon dioxide capture device according to the invention.

La figure 2 est une vue d'une chaudière équipée d'un tel dispositif.Figure 2 is a view of a boiler equipped with such a device.

Le procédé conforme à l'invention consiste à capturer du dioxyde de carbone sur des gaz industriels au moyen de deux réacteurs à mélange de gaz et de solides, à lit fluidisé rapide interconnectés en boucle thermochimique, selon lequel lesdits gaz sont mis en contact avec un composé alcalin à base de potassium dans le premier réacteur fluidisé au moyen des gaz industriels traités, afin de fixer le dioxyde de carbone sous forme de carbonate de potassium.The method according to the invention consists in capturing carbon dioxide on industrial gases by means of two gas-mixing reactors and fast fluidized bed fast-interconnected thermochemical loop-type reactors, in which said gases are brought into contact with a gas. potassium-based alkali compound in the first fluidized reactor using the treated industrial gases to fix the carbon dioxide as potassium carbonate.

De préférence, ledit composé alcalin est de l'hydroxyde de potassium qui réagit avec le dioxyde de carbone selon la formule :Preferably, said alkaline compound is potassium hydroxide which reacts with carbon dioxide according to the formula:

(1) 2KOH + CO2 -> K2CO3 + H2O.(1) 2KOH + CO 2 -> K 2 CO 3 + H 2 O.

Il est à noter le caractère inoffensif du carbonate de potassium qui est un additif alimentaire.It is worth noting the harmless nature of potassium carbonate which is a food additive.

Le carbonate de potassium K2CO3 est ensuite thermiquement décomposé dans le second réacteur fluidisé au moyen de vapeur d'eau soutiré de préférence d'une turbine à basse pression de la centrale équipée, en oxyde de potassium selon la formule :The potassium carbonate K 2 CO 3 is then thermally decomposed in the second fluidized reactor by means of water vapor, preferably drawn off from a low pressure turbine of the plant equipped with potassium oxide according to the formula:

(2) K2CO3 -> K2O + CO2.(2) K 2 CO 3 -> K 2 O + CO 2 .

Le cas échéant, l'apport thermique dans le second réacteur peut être également effectué par des solides chauds prélevés à partir de systèmes à lit fluidisés émetteurs de dioxyde de carbone ou également par prélèvement de fumées chaudes.If necessary, the heat input into the second reactor can also be carried out by hot solids taken from bed systems. fluidized emitters of carbon dioxide or also by sampling hot fumes.

Le dioxyde de carbone est ainsi séparé et après refroidissement, filtration et purification, comprimé et transféré par pipeline vers un stockage géologique souterrain.The carbon dioxide is thus separated and after cooling, filtration and purification, compressed and transferred by pipeline to an underground geological storage.

L'oxyde de potassium est ensuite hydraté en hydroxyde de potassium à l'entrée du premier réacteur selon la formule :The potassium oxide is then hydrated to potassium hydroxide at the inlet of the first reactor according to the formula:

(3) K2O + H2O -> 2KOH, la vapeur d'eau H2O étant fournie par les gaz industriels traités, en général des fumées. Il est également possible d'utiliser de l'eau liquide pour cette hydratation.(3) K 2 O + H 2 O -> 2KOH, the water vapor H 2 O being supplied by the treated industrial gases, generally fumes. It is also possible to use liquid water for this hydration.

Cette dernière réaction (3) est suivie d'un nouveau cycle réactionnel (1), (2), (3) de la boucle thermochimique. Le composé de potassium d'une granulométrie comprise entre 5 et 50 microns est mélangé à un support de lit auxiliaire, de préférence de l'alumine ou de la zéolithe, sous forme de particules de granulométrie comprise entre 10 et 100 microns. Il est également possible d'utiliser des particules de lit auxiliaire revêtues de composés de potassium par imprégnation et qui présentent l'avantage de conserver leur intégrité physique lors des cycles de carbonatation et de décarbonatation. Ce support de lit auxiliaire n'est pas susceptible d'attrition et est inerte du point de vue hydratation. Ce support de lit auxiliaire circule entre les deux réacteurs avec les composés de potassium qui sont de faible granulométrie de l'ordre de 5 à 50 microns. Ce support de lit auxiliaire est essentiel car les oxydes de potassium et les carbonates de potassium naissants sont extrêmement cohésifs et collants d'où la nécessité de les broyer et les disperser en permanence dans l'ensemble des boucles solides.This last reaction (3) is followed by a new reaction cycle (1), (2), (3) of the thermochemical loop. The potassium compound with a particle size of between 5 and 50 microns is mixed with an auxiliary bed support, preferably alumina or zeolite, in the form of particles having a particle size of between 10 and 100 microns. It is also possible to use auxiliary bed particles coated with potassium compounds by impregnation and which have the advantage of maintaining their physical integrity during the carbonation and decarbonation cycles. This auxiliary bed support is not susceptible to attrition and is inert from the hydration point of view. This auxiliary bed support circulates between the two reactors with the potassium compounds which are of small particle size on the order of 5 to 50 microns. This auxiliary bed support is essential because the nascent potassium oxides and potassium carbonates are extremely cohesive and sticky hence the need to grind and disperse them permanently in all solid loops.

Ce procédé permet de transférer le dioxyde de carbone contenu dans les gaz industriels de façon sélective, dioxyde de carbone correspondant à environThis process selectively transfers carbon dioxide from industrial gases, with carbon dioxide corresponding to about

14% de teneur en dioxyde de carbone dans des fumées typiques de combustion de charbons, par exemple, en effectuant sur les solides en circulation les échanges de chaleur crées par l'exothermicité de la réaction (1) et l'endothermicité de la réaction (2) de combinaison avec le dioxyde de carbone et de décomposition du dioxyde de carbone.14% of carbon dioxide content in typical fumes burning coal, for example, by performing on the circulating solids the exchanges heat generated by the exothermicity of the reaction (1) and the endothermicity of the reaction (2) of combination with carbon dioxide and decomposition of carbon dioxide.

Comme représenté sur la figure 1, un dispositif de capture de dioxyde de carbone pour la mise en œuvre de ce procédé comportent deux boucles à réacteurs à lit fluidisé rapide 1, 2 fonctionnant à une température de l'ordre de 80 à 2000C et comportant chacun un réacteur IA, 2A connecté en partie haute à un séparateur de solides de type cyclone IB, 2B relié à sa sortie de solides à une conduite de retour IC, 2C en partie basse du réacteur. Ces deux réacteurs sont interconnectés de la partie basse de chaque conduite de retour IC, 2C de l'un des réacteurs vers la partie basse du réacteur 2A, IA de l'autre réacteur, de façon que les solides soient restés suffisamment longtemps dans chaque zone réactionnelle en termes de température et de temps de séjour, afin de contrôler le degré de carbonatation et de décarbonatation dans les solides transférés. Le réacteur IA de la première boucle reçoit les gaz ou fumées chargées de dioxyde de carbone à traiter et est fluidisé par ceux-ci. Le réacteur 2A de la seconde boucle est quant à lui alimenté en vapeur d'eau de soutirage.As shown in Figure 1, a carbon dioxide capture device for the implementation of this method comprise two fluidized bed reactors fast loop 1, 2 operating at a temperature of the order of 80 to 200 0 C and each comprising a reactor IA, 2A connected at the top to a cyclone solids separator IB, 2B connected to its solids outlet to a return line IC, 2C at the bottom of the reactor. These two reactors are interconnected from the bottom of each return line IC, 2C of one of the reactors to the lower part of the reactor 2A, IA of the other reactor, so that the solids have remained in each zone long enough. reaction in terms of temperature and residence time, in order to control the degree of carbonation and decarbonation in the transferred solids. The reactor IA of the first loop receives the gases or fumes loaded with carbon dioxide to be treated and is fluidized by them. The reactor 2A of the second loop is in turn supplied with water vapor withdrawal.

En sortie des gaz du cyclone IB de la première boucle sont évacuées des fumées pauvres en dioxyde de carbone. En sortie des gaz du cyclone 2B de la deuxième boucle est récupéré un mélange de dioxyde de carbone et de vapeur d'eau qui est filtré, condensé, comprimé puis transporté pour stockage.At the exit of the cyclone IB gases of the first loop are evacuated fumes low in carbon dioxide. At the outlet of the gases of cyclone 2B of the second loop is recovered a mixture of carbon dioxide and water vapor which is filtered, condensed, compressed and transported for storage.

Chaque boucle de réacteur 1, 2 comporte au moins un échangeur à lit fluidisé en phase dense ou en phase diluée ou mobile alimenté en vapeur ou en fumées et assurant la commande de leur température. Un échangeur El, E2 peut être disposé sur la chaque conduite de retour IC, 2C en amont de l'interconnexion dans la phase dense et/ou un échangeur El', E2' peut être disposé dans le réacteur dans la phase diluée.Each reactor loop 1, 2 comprises at least one fluidized-bed exchanger in dense phase or in dilute or mobile phase fed with steam or fumes and controlling their temperature. An exchanger E1, E2 may be disposed on each return line IC 2C upstream of the interconnection in the dense phase and / or an exchanger E1 ', E2' may be arranged in the reactor in the dilute phase.

La chaleur dégagée par la carbonatation par le dioxyde de carbone des fumées sous forme de K2CO3 dans le premier réacteur 1 est transférée par l'échangeur El et/ou El' du premier réacteur 1, sur les solides circulants dont le débit réglable permet d'ajuster précisément la température optimale de carbonatation dans la boucle.The heat generated by the carbonation by carbon dioxide of the fumes in the form of K 2 CO 3 in the first reactor 1 is transferred by the exchanger El and / or El 'of the first reactor 1, to the circulating solids whose Adjustable flow rate makes it possible to precisely adjust the optimal temperature of carbonation in the loop.

La réaction de décomposition du K2CO3 dans le deuxième réacteur 2 est endothermique et utilise en partie la chaleur des solides en provenance du premier réacteur 1 pour effectuer cette décomposition. Un apport externe de chaleur est assuré par de la vapeur soutirée du cycle ou des fumées chaudes de la chaudière équipée, grâce à l'échangeur E2 et/ou E2' du second réacteur 2.The decomposition reaction of K 2 CO 3 in the second reactor 2 is endothermic and uses part of the heat of the solids from the first reactor 1 to effect this decomposition. An external supply of heat is provided by the steam drawn off from the cycle or the hot flue gases of the equipped boiler, thanks to the exchanger E2 and / or E2 'of the second reactor 2.

Le débit de solides prélevés du premier réacteur 1 et l'apport externe de chaleur doivent satisfaire à ce besoin de chaleur. Ce deuxième réacteur 2 est donc garni de matériaux isolants pour limiter les pertes de chaleur aux parois.The solids flow taken from the first reactor 1 and the external supply of heat must meet this need for heat. This second reactor 2 is thus lined with insulating materials to limit heat loss to the walls.

Comme représenté sur la figure 2, un tel dispositif de capture de dioxyde de carbone peut être installé en sortie de fumées filtrées d'une chaudière, par exemple d'une chaudière à charbon pulvérisé C. Les boucles à réacteurs 1 et 2 sont schématisées sur cette figure. Seuls les éléments complémentaires de ceux de la figure 1 seront maintenant précisés.As shown in FIG. 2, such a device for capturing carbon dioxide may be installed at the outlet of filtered fumes from a boiler, for example from a pulverized coal boiler C. The reactor loops 1 and 2 are diagrammed on this figure. Only the complementary elements of those of Figure 1 will now be specified.

En sortie des gaz de la première boucle 1 sont évacuées des fumées pauvres en dioxyde de carbone qui sont filtrées au moyen du dispositif de filtration Fl, de type filtre à manches ou électrofiltre, les fumées filtrées étant renvoyées à l'atmosphère et les solides étant recyclés dans le premier réacteur 1.At the outlet of the gases of the first loop 1 are evacuated fumes low in carbon dioxide which are filtered by means of the filtration device Fl, of the bag-filter or electrofilter type, the filtered fumes being returned to the atmosphere and the solids being recycled in the first reactor 1.

De même, en sortie des gaz de la deuxième boucle 2 est récupéré un mélange de dioxyde de carbone et de vapeur d'eau qui est filtré par le dispositif de filtration F2, de type filtre à manches, condensé, comprimé puis transporté pour stockage géologique souterrain. Les solides récupérés par le dispositif de filtration F2 sont recyclés dans le premier réacteur 1.Similarly, at the outlet of the gases of the second loop 2 is recovered a mixture of carbon dioxide and water vapor which is filtered by the filtration device F2, filter bag, condensed, compressed and transported for geological storage underground. The solids recovered by the filtration device F2 are recycled in the first reactor 1.

La perte de charges crée par le premier réacteur 1 est compensée par un ventilateur booster Vl sur les fumées avant leur introduction dans ce premier réacteur. The loss of charge created by the first reactor 1 is compensated by a booster fan Vl on the flue gases before their introduction into this first reactor.

Claims

REVEN DICATIONS REVEN DICATIONS 1. Procédé de capture de dioxyde de carbone sur des gaz industriels au moyen de deux boucles à réacteurs à lit fluidisé interconnectées en boucle thermochimique, selon lequel lesdits gaz sont mis en contact avec un composé métallique dans la première boucle (1), afin de fixer le dioxyde de carbone sous forme d'un carbonate, procédé caractérisé en ce que ledit composé métallique est à base de potassium et ledit carbonate est du carbonate de potassium.A method of capturing carbon dioxide on industrial gases by means of two thermochemically looped fluidized bed fluidized-bed reactor loops, wherein said gases are contacted with a metal compound in the first loop (1), in order to fixing the carbon dioxide in the form of a carbonate, characterized in that said metal compound is based on potassium and said carbonate is potassium carbonate. 2. Procédé selon la revendication 1, caractérisé en ce que ledit composé métallique est de l'hydroxyde de potassium.2. Method according to claim 1, characterized in that said metal compound is potassium hydroxide. 3. Procédé selon la revendication précédente, caractérisé en ce que ledit carbonate de potassium est thermiquement décomposé dans la seconde boucle (2) en oxyde de potassium.3. Method according to the preceding claim, characterized in that said potassium carbonate is thermally decomposed in the second loop (2) in potassium oxide. 4. Procédé selon la revendication précédente, caractérisé en ce que ledit oxyde de potassium est hydraté en hydroxyde de potassium à l'entrée de ladite première boucle (1).4. Method according to the preceding claim, characterized in that said potassium oxide is hydrated to potassium hydroxide at the inlet of said first loop (1). 5. Procédé selon l'une des revendications précédentes, caractérisé en ce que ledit composé métallique est mélangé à un support inerte, de préférence de l'alumine ou de la zéolithe.5. Method according to one of the preceding claims, characterized in that said metal compound is mixed with an inert support, preferably alumina or zeolite. 6. Procédé selon l'une des revendications précédentes, caractérisé en ce que ledit composé métallique est sous forme de particules de granulométrie comprise entre 10 et 100 microns.6. Method according to one of the preceding claims, characterized in that said metal compound is in the form of particle size of between 10 and 100 microns. 7. Procédé selon l'une des revendications précédentes, caractérisé en ce que ladite première boucle (1) est fluidisée au moyen desdits gaz industriels. 7. Method according to one of the preceding claims, characterized in that said first loop (1) is fluidized by means of said industrial gases. 8. Procédé selon l'une des revendications 3 à 7, caractérisé en ce que ladite seconde boucle (2) est fluidisée au moyen de vapeur d'eau.8. Method according to one of claims 3 to 7, characterized in that said second loop (2) is fluidized by means of steam. 9. Dispositif de capture de dioxyde de carbone pour la mise en œuvre du procédé selon l'une de revendications précédentes, caractérisé en ce que lesdites deux boucles de réacteurs (1, 2) sont des boucles à lit fluidisé rapide comportant chacun un réacteur (IA, 2A) connecté en partie haute à un séparateur de solides (IB, 2B) relié à sa sortie de solides à une conduite de retour (IC, 2C) en partie basse du réacteur et en ce que ces deux boucles sont interconnectées de chaque conduite de retour (IC, 2C) de l'un des réacteurs vers la partie basse du réacteur (2A, IA) de l'autre réacteur.9. A carbon dioxide capture device for implementing the method according to one of the preceding claims, characterized in that said two reactor loops (1, 2) are fast fluidized-bed loops each comprising a reactor ( IA, 2A) connected at the top to a solids separator (IB, 2B) connected to its solids outlet to a return line (IC, 2C) in the lower part of the reactor and in that these two loops are interconnected with each return line (IC, 2C) from one of the reactors to the lower part of the reactor (2A, IA) of the other reactor. 10. Dispositif selon la revendication précédente, caractérisé en ce que chaque boucle comporte au moins un échangeur à lit fluidisé ou mobile de contrôle de leur température.10. Device according to the preceding claim, characterized in that each loop comprises at least one fluidized bed or mobile exchanger for controlling their temperature. 11. Dispositif selon la revendication précédente, caractérisé en ce que ledit échangeur (El, E2) est disposé sur la dite conduite de retour (IC, 2C) en amont de l'interconnexion.11. Device according to the preceding claim, characterized in that said exchanger (E1, E2) is disposed on said return line (IC, 2C) upstream of the interconnection. 12. Dispositif selon la revendication 10 ou 11, caractérisé en ce que ledit échangeur (El', E2') est disposé dans le réacteur (IA, 2A).12. Device according to claim 10 or 11, characterized in that said exchanger (El ', E2') is disposed in the reactor (IA, 2A). 13. Dispositif selon l'une des revendications 9 à 12, caractérisé en ce que les deux dites boucles à réacteurs (1, 2) fonctionnent à une température de l'ordre de 80 à 2000C.13. Device according to one of claims 9 to 12, characterized in that the said two reactor loops (1, 2) operate at a temperature of the order of 80 to 200 0 C. 14. Utilisation d'un dispositif de capture de dioxyde de carbone selon l'une des revendications 9 à 13, caractérisé en ce qu'il est installé en sortie de fumées ou de gaz industriels en provenance d'une chaudière (C) ou d'un générateur de fumées. 14. Use of a carbon dioxide capture device according to one of claims 9 to 13, characterized in that it is installed at the outlet of fumes or industrial gases from a boiler (C) or d a smoke generator.
PCT/FR2009/052010 2008-11-04 2009-10-21 Method and device for capturing carbon dioxide on industrial gases at a low temperature Ceased WO2010052400A1 (en)

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