EP0153235B1 - Process for the production of synthesis gas - Google Patents

Process for the production of synthesis gas Download PDF

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Publication number
EP0153235B1
EP0153235B1 EP19850400229 EP85400229A EP0153235B1 EP 0153235 B1 EP0153235 B1 EP 0153235B1 EP 19850400229 EP19850400229 EP 19850400229 EP 85400229 A EP85400229 A EP 85400229A EP 0153235 B1 EP0153235 B1 EP 0153235B1
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Prior art keywords
reactor
gas
temperature
production
hydrogen
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EP19850400229
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German (de)
French (fr)
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EP0153235A1 (en
Inventor
Gérard Chrysostome
Jean-Michel Lemasle
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Areva NP SAS
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Framatome SA
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    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/54—Gasification of granular or pulverulent fuels by the Winkler technique, i.e. by fluidisation
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/46—Gasification of granular or pulverulent flues in suspension
    • C10J3/463—Gasification of granular or pulverulent flues in suspension in stationary fluidised beds
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/58—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels combined with pre-distillation of the fuel
    • C10J3/60—Processes
    • C10J3/64—Processes with decomposition of the distillation products
    • C10J3/66—Processes with decomposition of the distillation products by introducing them into the gasification zone
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J2300/00—Details of gasification processes
    • C10J2300/12—Heating the gasifier
    • C10J2300/123—Heating the gasifier by electromagnetic waves, e.g. microwaves
    • C10J2300/1238—Heating the gasifier by electromagnetic waves, e.g. microwaves by plasma

Definitions

  • the subject of the invention is a process for the production, from a hydrocarbon material, of a synthesis gas based on CO and H 2 which can be used for the synthesis of a chemical substance such as for example methanol, or else as combustible.
  • synthesis gas consisting essentially of carbon monoxide and hydrogen and which can be used as raw material for the synthesis of bodies.
  • chemicals such as methanol or ammonia, or industrial fuel, or even allow reduction and hydrogenation reactions to be carried out.
  • the production of synthesis gas takes place in two successive stages.
  • the gasification proper of the hydrocarbon substance is first carried out, with the production of a gaseous mixture based on CO and H 2 also containing significant proportions of other so-called "fatal” species such as dioxide. carbon, water vapor, methane, unburnt carbon and, in particular in the case of gasification of a biomass product, CnHm hydrocarbons and grouds.
  • agglomerating ash processes the process is carried out at high temperature, which makes it possible to increase the gasification yield.
  • the agglomeration and the evacuation of the ash pose problems which are difficult to solve, in particular in the case of large reactors and this is why, in many cases, it is preferred to maintain in the fluidized bed a moderate temperature, of l '' order of 700 to 800 ° C which allows to remain below the melting or softening temperature of the ash, the latter being close to 1000 ° C in the case of wood.
  • This tempera- ture operating mode Moderate ture is simpler to implement but nevertheless leads, in the case of wood in particular, to the production of relatively large quantities of methane and of hydrocarbon.
  • the gas obtained can have, for example, the following composition, expressed in% by volume on the raw gas: + Traces of tar + unburnt carbon
  • a second reactor is used for this purpose in which a conversion is carried out where the main reactions can be as follows:
  • the partial combustion of the gas produces significant amounts of C0 2 at the expense of CO.
  • approximately 35% of the carbon originating from the raw material can be found in the form of C0 2 , which represents a potential carbon loss of approximately one third.
  • the subject of the invention is a new process which is simpler to implement and which makes it possible to carry out on the one hand the gasification reaction at moderate temperature and on the other hand the conversion reaction at higher temperature without partial combustion of the CO and by therefore without loss of carbon.
  • the method according to the invention makes it easier to adjust the relative proportions of the constituents of the gas produced.
  • a rise in the conversion temperature in the second reactor is obtained by blowing a stream of gas previously brought to a temperature between 3000 and 5000 ° C. by passing it through a plasma torch placed at the outlet of a gas blowing circuit in the conversion reactor, the blown gas flow is adjusted as a function of the temperature and of the proportions of carbon monoxide and hydrogen already existing in the mixture coming from the first reactor gasification.
  • the blown gas is hydrogen
  • the blown gas is nitrogen.
  • the invention also relates to an installation in which the conversion reactor is equipped on the one hand with a plasma torch placed at the outlet of a hydrogen insufflation lance carried by said plasma torch at a temperature comprised between 3000 and 5000 ° C and means for adjusting the flow rate of the blown hydrogen taking into account the flow rate and the temperature of the gases coming from the gasification reactor so that the average temperature of the gas mixture in the conversion reactor is raised to a level sufficient for the conversion of fatal species.
  • Figure 1 is a diagram of an improved installation according to the invention.
  • Figure 2 is a detail view schematically showing the gas blowing lance in the conversion reactor, provided with a plasma torch for heating the gas.
  • FIG 1 there is shown schematically a synthesis gas production installation comprising two reactors 1 and 2 respectively of gasification and conversion.
  • the reactor 1 operates, in a conventional manner, in a fluidized bed or in a circulating bed. It therefore consists of a vertical cylindrical enclosure provided at its base with means for fluidizing the hydrocarbon raw material introduced at 11, by ascending circulation of a gas introduced at 12.
  • the fluidizing gas is preferably a gas useful for reaction, for example water vapor.
  • Oxidizing gas, air or oxygen is injected at 13 to carry out the partial combustion of the hydrocarbon material in the fluidized bed. As indicated, the respective flow rates of hydrocarbon raw material and oxygen are adjusted so that the gasification reaction takes place at moderate temperature, the gases produced leaving at 14, at the top of reactor 1, at a temperature of 700 to 800 ° C.
  • the conversion reactor 2 which consists of a vertical enclosure furnished with refractories and at the end of which are introduced at 21, the gases coming from the gasification reactor 1.
  • the conversion reactor is provided with a lance 3 for blowing a gas brought to very high temperature.
  • the lance 3 is connected to a circuit 31 for injecting pressurized gas and is provided with means 4 for heating the gas to very high temperature before it enters the reactor 2.
  • the means 4 for heating the gas advantageously consists of a plasma torch.
  • a plasma torch which may be commercially available, does not need to be described in detail. It suffices to indicate that it may comprise electrodes 41, 42 offset in the direction of circulation of the gas, between which an electric arc blown by the gas is formed and which allows, at the outlet of the lance 3 in the reactor 2, to produce a zone 43 at very high temperature, of the order of 3000 to 5000 ° C.
  • the inlet 21 of the gases from the gasification reactor 1 takes place at substantially the same level as the inlet of the high temperature gases so that the very high temperature zone is limited around the injection orifice 32 which can be made of a material capable of withstanding such temperatures. It is also possible to use known means for mixing the two gas streams as soon as they enter the reactor, for example by injecting the gas at high temperature in the axis of a vortex formed by the gases introduced by the inlet. 21. The flow rates of the two gas streams are adjusted in suitable proportions so that the temperature inside the reactor 2 is homogeneous and maintained at an average level of between 1200 and 1500 ° C. which favors the conversion reactions (1) to (5) indicated above.
  • a gas is thus obtained very simply free of methane, higher hydrocarbons, and whose carbon dioxide content is lower than that obtained for example by a catalytic process of oxygen reforming.
  • carbon dioxide content is lower than that obtained for example by a catalytic process of oxygen reforming.
  • 10 to 20% of the carbon originating from the starting material is found in the form of CO 2 , the rest, ie 80 to 90% being in the CO form.
  • Another advantage is that the oxygen consumption is lower than in known methods.
  • the high temperature heating of the injected gas leads to an increase in energy consumption, in particular electrical energy for the supply of the plasma torch 4.
  • the association of a plasma torch with the conversion reactor will be advantageous in many cases, in particular whenever there is a large and inexpensive source of energy, for example example of hydroelectric origin.
  • the process makes it possible to save the biomass for the production of synthesis gas and this saving can be significant even in countries where there is a large amount of biomass because it is not possible to conceive the realization of gasification installation.
  • these should not be exploited from the gasification installation and this is why, even in a country very favored from the point of view of the renewal of the biomass, it is useful to draw the maximum potential energy, including CO and H2 of this substance.
  • the consumption, even important, of electric energy can thus be advantageous, and it is in particular the case when important installations of production of hydroelectric or nuclear power are placed in relatively isolated regions which can also be suitable for crops energetic.
  • the gas injected at high temperature, after passing through the plasma torch, can simply be synthetic gas recycled in suitable proportions.
  • the gas leaving at 22 from the conversion reactor 2 contains practically only CO + H 2 + C0 2 + H 2 0 but the H 2 / CO ratio must be adjusted to the appropriate value before the chemical synthesis carried out in a installation 5 provided for this purpose.
  • this ratio must be close to 2 whereas it is generally close to 1 at the outlet of the conversion reactor 2.
  • this gas can be converted subsequently by the known conversion reaction of CO:
  • the reaction therefore consumes part of the CO and also generates additional CO 2 .
  • the blown gas is hydrogen. Taking into account the flow rate and the temperature of the gases resulting from the gasification, and the temperature which makes it possible to obtain the plasma torch 4, it is possible to inject by the lance 3 a controlled flow of hydrogen, so as to control the H 2 / CO ratio in the gas produced. The CO conversion step is then saved and it suffices to eliminate the water vapor in a simple condensing device 51.
  • the installation can operate only with a source of hydrocarbon material and a source of electrical energy because the electrolysis of water makes it possible to generate at the same time, in sufficient quantity, the oxygen injected in 13 in the reactor 1 to supply the quantity of heat necessary for the gasification reaction. It will even be possible to produce a certain amount of excess oxygen, recovered at 15.
  • the use of an electrolysis device will therefore make it possible to avoid the production of oxygen by distillation of the air.
  • electrolysis lies in the fact that there are electrolysis devices supplying hydrogen under a pressure which can be up to 70 bars. The hydrogen can therefore be led directly, through the circuit 31 in the plasma torch 4 without prior compression.
  • gasification and conversion in reactors 1 and 2 can be carried out under pressure and therefore more economically thanks to the resulting reduction in the dimensions of the equipment and the savings made on gas compression. before the synthesis, this must, in all cases, be carried out under pressure.
  • the high temperature gas injected into the conversion reactor could, in general, be any gas useful for synthesis, for example nitrogen in the case of the production of ammonia.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Description

L'invention a pour objet un procédé de production, à partir d'une matière hydrocarbonée, d'un gaz de synthèse à base de CO et H2 utilisable pour la synthèse d'une substance chimique comme par exemple le méthanol, ou bien comme combustible.The subject of the invention is a process for the production, from a hydrocarbon material, of a synthesis gas based on CO and H 2 which can be used for the synthesis of a chemical substance such as for example methanol, or else as combustible.

Par gazéification d'une substance carbonée, par exemple un produit de biomasse ou du charbon, on peut obtenir un gaz dit "de synthèse" constitué essentiellement de monoxyde de carbone et d'hydrogène et qui peut servir de matière première pour la synthèse de corps chimiques tels que le méthanol ou l'ammoniac, ou bien de combustible industriel, ou bien encore permettre de réaliser des réactions de réduction et d'hydrogénation.By gasification of a carbonaceous substance, for example a product of biomass or of coal, one can obtain a so-called "synthesis" gas consisting essentially of carbon monoxide and hydrogen and which can be used as raw material for the synthesis of bodies. chemicals such as methanol or ammonia, or industrial fuel, or even allow reduction and hydrogenation reactions to be carried out.

Normalement la production du gaz de synthèse se fait en deux étapes successives. Dans un premier réacteur, on réalise tout d'abord la gazéification proprement dite de la substance hydrocarbonée, avec production d'un mélange gazeux à base de CO et H2 contenant également des proportions notables d'autre espèces dites "fatales" comme du dioxyde de carbone, de la vapeur d'eau, du méthane, du carbone imbrûlé et, notamment dans le cas de gazéification d'un produit de biomasse, des hydrocarbures CnHm et des grou- drons.Normally, the production of synthesis gas takes place in two successive stages. In a first reactor, the gasification proper of the hydrocarbon substance is first carried out, with the production of a gaseous mixture based on CO and H 2 also containing significant proportions of other so-called "fatal" species such as dioxide. carbon, water vapor, methane, unburnt carbon and, in particular in the case of gasification of a biomass product, CnHm hydrocarbons and grouds.

Dans de nombreux procédés, on a jugé avantageux de réaliser la gazéification de la substance hydrocarbonée en lit fluidisé en présence d'oxygène. Dans le cas par exemple d'un produit de biomasse, l'utilisation du lit fluidisé permet d'utiliser des déchets de bois de granulométries variables et donc d'économiser sur le broyage de la matière première, mais aussi d'admettre des matériaux variés comme des bois de diverses origines, de l'écorce, de la paille, de la bagasse, ou différents déchets végétaux.In many processes, it has been found advantageous to carry out gasification of the hydrocarbon substance in a fluidized bed in the presence of oxygen. In the case for example of a biomass product, the use of the fluidized bed makes it possible to use wood waste of variable particle sizes and therefore to save on the grinding of the raw material, but also to admit various materials like wood of various origins, bark, straw, bagasse, or different vegetable waste.

L'injection d'oxygène dans le réacteur permet de travailler en mode "autothermique", l'oxygène injecté apportant l'énergie nécessaire à la gazéification par combustion partielle du bois. Toutefois, le gaz produit dans ces conditions contient des proportions significatives de C02 et H20 produit par la combustion partielle.The injection of oxygen into the reactor makes it possible to work in "autothermal" mode, the oxygen injected providing the energy necessary for gasification by partial combustion of the wood. However, the gas produced under these conditions contains significant proportions of C0 2 and H 2 0 produced by partial combustion.

Dans certains procédés dits en cendres agglo- mérantes, on travaille à haute température ce qui permet d'augmenter le rendement de gazéification. Cependant, l'agglomération et l'évacuation des cendres posent des problèmes difficiles à résoudre notamment dans le cas des réacteurs de grandes dimensions et c'est pourquoi, dans de nombreux cas, on préfère maintenir dans le lit fluidisé une température modérée, de l'ordre de 700 à 800°C qui permet de rester en-dessous de la température de fusion ou de ramollissement des cendres, celle-ci étant proche de 1000°C dans le cas du bois. Ce mode de fonctionnement à tempéra-. ture modérée est plus simple à mettre en oeuvre mais conduit cependant, dans le cas du bois notamment, à la production de quantités relativement importantes de méthane et d'hydrocarbure.In certain so-called agglomerating ash processes, the process is carried out at high temperature, which makes it possible to increase the gasification yield. However, the agglomeration and the evacuation of the ash pose problems which are difficult to solve, in particular in the case of large reactors and this is why, in many cases, it is preferred to maintain in the fluidized bed a moderate temperature, of l '' order of 700 to 800 ° C which allows to remain below the melting or softening temperature of the ash, the latter being close to 1000 ° C in the case of wood. This tempera- ture operating mode. Moderate ture is simpler to implement but nevertheless leads, in the case of wood in particular, to the production of relatively large quantities of methane and of hydrocarbon.

A titre d'exemple, à la sortie d'un réacteur de gazéification du bois à température modérée, comprise entre 700 et 800°C, le gaz obtenu peut avoir par exemple la composition suivante, exprimée en % volumique sur le gaz brut:

Figure imgb0001
+Traces de goudrons+carbone imbrûléBy way of example, at the outlet of a gasification reactor for wood at a moderate temperature, between 700 and 800 ° C., the gas obtained can have, for example, the following composition, expressed in% by volume on the raw gas:
Figure imgb0001
 + Traces of tar + unburnt carbon

Le gaz ainsi produit présente donc l'inconvénient d'être tout à fait impropre, en l'état, à une synthèse chimique. En revanche, ce procédé de gazéification à température modérée présente l'avantage d'être bien maitrisé, aisément contrôlable, et apte à traiter une variété étendue de matières hydrocarbonées, sans conditionnement préalable souvent très couteux.The gas thus produced therefore has the drawback of being entirely unsuitable, as it stands, for chemical synthesis. On the other hand, this gasification process at moderate temperature has the advantage of being well controlled, easily controllable, and capable of treating a wide variety of hydrocarbon materials, without prior conditioning which is often very expensive.

Il faut alors, dans une seconde étape, ajuster la composition du gaz pour le rendre propre à une synthèse chimique avec un bon rendement, c'est-à-dire en maximisant la production de CO et H2.It is then necessary, in a second step, to adjust the composition of the gas to make it suitable for chemical synthesis with good yield, that is to say by maximizing the production of CO and H 2 .

On utilise à cet effect un second réacteur dans lequel on réalise une conversion où les principales réactions peuvent être les suivantes:A second reactor is used for this purpose in which a conversion is carried out where the main reactions can be as follows:

Figure imgb0002
Figure imgb0003
Figure imgb0004
Figure imgb0005
Figure imgb0006
Ces réactions, dont la vitesse augmente avec la température, sont toutes endothermiques et nécessitent donc un apport de chaleur qui, jusqu'à présent, était obtenu par injection d'oxygène dans le second réacteur de conversion, de façon à réaliser une combustion partielle du gaz brut provenant du premier réacteur, pour libérer la chaleur nécessaire à la réalisation des réactions (1) à (5).
Figure imgb0002
Figure imgb0003
Figure imgb0004
Figure imgb0005
Figure imgb0006
 These reactions, whose speed increases with temperature, are all endothermic and therefore require a supply of heat which, until now, was obtained by injecting oxygen into the second conversion reactor, so as to achieve a partial combustion of the raw gas from the first reactor, to release the heat necessary for carrying out reactions (1) to (5).

Ces réactions de combustion partielles sont du type:

Figure imgb0007
Figure imgb0008
Figure imgb0009
etc.These partial combustion reactions are of the type:
Figure imgb0007
Figure imgb0008
Figure imgb0009
 etc.

On peut ainsi obtenir à l'intérieur du réacteur de conversion une température de 1200 à 1500°C qui permet, en favorisant les réactions de conversion, de disposer d'un gaz ne contenant pratiquement plus de méthane, d'hydrocarbures supérieurs ou de carbone imbrûlé. En revanche, comme l'indiquent les réactions de combustion données ci- dessus, la combustion partielle du gaz produit des quantités significatives de C02 su détriment du CO. En pratique, 35% environ du carbone provenant de la matière première peut se retrouver sous forme de C02 ce qui représente une perte en carbone potentielle d'un tiers environ.One can thus obtain inside the conversion reactor a temperature of 1200 to 1500 ° C which allows, by promoting the conversion reactions, to have a gas containing practically no more methane, higher hydrocarbons or carbon unburnt. On the other hand, as indicated by the combustion reactions given above, the partial combustion of the gas produces significant amounts of C0 2 at the expense of CO. In practice, approximately 35% of the carbon originating from the raw material can be found in the form of C0 2 , which represents a potential carbon loss of approximately one third.

On peut aussi, dans un autre mode de conversion, faire passer les gaz sur un catalyseur dont la présence permet la réalisation des réactions de conversion à des températures plus modérées, de l'ordre de 950 à 1100°C, ce qui réduit la quantité d'oxygène à injecter dans le gaz et par conséquent la combustion partielle de ce dernier peut produire l'élévation de température nécessaire. On produit ainsi un gaz exempt de méthane et d'hydrocarbures supérieurs et contenant moins de C02 avec une consommation d'oxygène plus réduite. Cependant, ce procède catalytique nécessite la présence d'un dépoussiérage à haute température du gaz avant son entrée dans le réacteur de conversion pour protéger le cataly- seυr.·It is also possible, in another conversion mode, to pass the gases over a catalyst whose presence allows conversion reactions to be carried out at more moderate temperatures, of the order of 950 to 1100 ° C., which reduces the quantity of oxygen to be injected into the gas and consequently the partial combustion of the latter can produce l temperature increase required. This produces a gas free of methane and higher hydrocarbons and containing less C0 2 with reduced oxygen consumption. However, this catalytic process requires the presence of a high temperature dusting of the gas before it enters the conversion reactor to protect the catalyst.

L'invention a pour objet un nouveau procédé plus simple à mettre en oeuvre et permettant de réaliser d'une part la réaction de gazéification à température modérée et d'autre part la réaction de conversion à température plus élevée sans combustion partielle du CO et par conséquent sans perte de carbone. En outre, le procédé selon l'invention permet de régler plus facilement les proportions relatives des constituants du gaz produit.The subject of the invention is a new process which is simpler to implement and which makes it possible to carry out on the one hand the gasification reaction at moderate temperature and on the other hand the conversion reaction at higher temperature without partial combustion of the CO and by therefore without loss of carbon. In addition, the method according to the invention makes it easier to adjust the relative proportions of the constituents of the gas produced.

Conformément à l'invention, une élévation à la température de conversion dans le second réacteur est obtenure par insufflation d'un courant de gaz préalablement porté à une température comprise entre 3000 et 5000°C par passage de ce dernier dans une torche à plasma placée au débouché d'un circuit d'insufflation du gaz dans le réacteur de conversion, le débit de gaz insufflé est réglé en fonction de la température et des proportions de monoxyde de carbone et d'hydrogène déjà existant dans le mélange issu du premier réacteur de gazéification.In accordance with the invention, a rise in the conversion temperature in the second reactor is obtained by blowing a stream of gas previously brought to a temperature between 3000 and 5000 ° C. by passing it through a plasma torch placed at the outlet of a gas blowing circuit in the conversion reactor, the blown gas flow is adjusted as a function of the temperature and of the proportions of carbon monoxide and hydrogen already existing in the mixture coming from the first reactor gasification.

Selon une autre caractéristique de l'invention, le gaz insufflé est de l'hydrogène.According to another characteristic of the invention, the blown gas is hydrogen.

Selon encore une autre caractéristique de l'invention, le gaz insufflé est de l'azote.According to yet another characteristic of the invention, the blown gas is nitrogen.

L'invention a également pour objet une installation dans laquelle le réacteur de conversion est équipé d'une part d'une torche à plasma placée au débouché d'une lance d'insufflation d'hydrogène porté par ladite torche à plasma à une température comprise entre 3000 et 5000°C et de moyens de réglage du débit-de l'hydrogène insufflé en tenant compte du débit et de la température des gaz issus du réacteur de gazéification de façon que la température moyenne du mélange gazeux dans le réacteur de conversion soit élevée à un niveau suffisant pour la conversion des espèces fatales.The invention also relates to an installation in which the conversion reactor is equipped on the one hand with a plasma torch placed at the outlet of a hydrogen insufflation lance carried by said plasma torch at a temperature comprised between 3000 and 5000 ° C and means for adjusting the flow rate of the blown hydrogen taking into account the flow rate and the temperature of the gases coming from the gasification reactor so that the average temperature of the gas mixture in the conversion reactor is raised to a level sufficient for the conversion of fatal species.

Mais l'invention sera mieux comprise par la description détaillée d'un mode de réalisation donné à titre d'exemple en se référant aux dessins annexés.However, the invention will be better understood from the detailed description of an embodiment given by way of example with reference to the accompanying drawings.

La figure 1 est un schéma d'une installation perfectionnée selon l'invention.Figure 1 is a diagram of an improved installation according to the invention.

La figure 2 est une vue de détail représentant schématiquement la lance d'insufflation de gaz dans le réacteur de conversion, munie d'une torche à plasma pour le chauffage du gaz.Figure 2 is a detail view schematically showing the gas blowing lance in the conversion reactor, provided with a plasma torch for heating the gas.

Sur la figure 1, on a représenté schématiquement une installation de production de gaz de synthèse comportant deux réacteurs 1 et 2 respectivement de gazéification et de conversion.In Figure 1, there is shown schematically a synthesis gas production installation comprising two reactors 1 and 2 respectively of gasification and conversion.

Le réacteur 1 fonctionne, de façon classique, en lit fluidisé ou en lit circulant. Il est donc constitué d'une enceinte cylindrique verticale munie à sa base de moyens de fluidisation de la matière première hydrocarbonée introduite en 11, par circulation ascendante d'un gaz introduit en 12. Le gaz de fluidisation est de préférence un gaz utile à la réaction, par exemple de la vapeur d'eau. Un gaz comburant, de l'air ou de l'oxygène, est injecté en 13 pour réaliser la combustion partielle de la matière hydrocarbonée dans le lit fluidisé. Comme on l'a indiqué, les débits respectifs de matière première hydrocarbonée et d'oxygène sont réglés de telle sorte que la réaction de gazéification se produise à température modérée, les gaz produits sortant en 14, à la partie supérieure de réacteur 1, à une température de 700 à 800°C.The reactor 1 operates, in a conventional manner, in a fluidized bed or in a circulating bed. It therefore consists of a vertical cylindrical enclosure provided at its base with means for fluidizing the hydrocarbon raw material introduced at 11, by ascending circulation of a gas introduced at 12. The fluidizing gas is preferably a gas useful for reaction, for example water vapor. Oxidizing gas, air or oxygen, is injected at 13 to carry out the partial combustion of the hydrocarbon material in the fluidized bed. As indicated, the respective flow rates of hydrocarbon raw material and oxygen are adjusted so that the gasification reaction takes place at moderate temperature, the gases produced leaving at 14, at the top of reactor 1, at a temperature of 700 to 800 ° C.

De tels réacteurs en lit fluidisé sont bien connus et ne nécessitent pas une description détaillée.Such fluidized bed reactors are well known and do not require a detailed description.

Il en est de même du réracteur de conversion 2 qui est constitué d'une enceinte verticale garnie de réfractaires et à l'extrémité de laquelle sont introduits en 21, les gaz issus du réacteur de gazéification 1.It is the same for the conversion reactor 2 which consists of a vertical enclosure furnished with refractories and at the end of which are introduced at 21, the gases coming from the gasification reactor 1.

Comme on l'a indiqué, le réacteur de conversion est muni d'une lance 3 d'insufflation d'un gaz porté à très haute température. A cet effet, la lance 3 est reliée à un circuit 31 d'injection de gaz sous pression et est munie de moyen 4 de chauffage du gaz à très haute température avant son entrée dans le réacteur 2.As indicated, the conversion reactor is provided with a lance 3 for blowing a gas brought to very high temperature. To this end, the lance 3 is connected to a circuit 31 for injecting pressurized gas and is provided with means 4 for heating the gas to very high temperature before it enters the reactor 2.

Comme on l'a représenté schématiquement sur la figure 2, le moyen 4 de chauffage du gaz est constitué avantageusement par une torche à plasma. Un tel dispositif, qui peut se trouver dans le commerce, n'a pas besoin d'être décrit en détail. Il suffit d'indiquer qu'il peut comporter des électrodes 41, 42 décalées dans le sens de circulation du gaz en entre lesquelles se forme un arc électrique soufflé par le gaz et qui permet, au débouché de la lance 3 dans le réacteur 2, de réaliser une zone 43 à très haute température, de l'ordre de 3000 à 5000°C.As shown diagrammatically in FIG. 2, the means 4 for heating the gas advantageously consists of a plasma torch. Such a device, which may be commercially available, does not need to be described in detail. It suffices to indicate that it may comprise electrodes 41, 42 offset in the direction of circulation of the gas, between which an electric arc blown by the gas is formed and which allows, at the outlet of the lance 3 in the reactor 2, to produce a zone 43 at very high temperature, of the order of 3000 to 5000 ° C.

L'entrée 21 des gaz issus du réacteur de gazéification 1 se fait sensiblement au même niveau que l'entrée des gaz à haute température de façon que la zone à température très élevée soit limitée autour de l'orifice d'injection 32 qui peut être réalisée en une matière susceptible de résister à de telles températures. On peut d'ailleurs utiliser des moyens connus pour réaliser un mélange des deux courants gazeux dès leur entrée dans le réacteur, par exemple en injectant le gaz à haute température dans l'axe d'un tourbillon formé par les gaz introduits par l'entrée 21. Les débits des deux courants gazeux sont réglés en proportions convenables de façon que la température à l'intérieur du réacteur 2 soit homogène et maintenue à un niveau moyen compris entre 1200 et 1500°C qui favorise les réactions de conversion (1) à (5) indiquées plus haut.The inlet 21 of the gases from the gasification reactor 1 takes place at substantially the same level as the inlet of the high temperature gases so that the very high temperature zone is limited around the injection orifice 32 which can be made of a material capable of withstanding such temperatures. It is also possible to use known means for mixing the two gas streams as soon as they enter the reactor, for example by injecting the gas at high temperature in the axis of a vortex formed by the gases introduced by the inlet. 21. The flow rates of the two gas streams are adjusted in suitable proportions so that the temperature inside the reactor 2 is homogeneous and maintained at an average level of between 1200 and 1500 ° C. which favors the conversion reactions (1) to (5) indicated above.

On obtient ainsi de façon très simple un gaz exempt de méthane, d'hydrocarbures supérieurs, et dont la teneur en dioxyde de carbone est inférieure à celle obtenue par exemple par un procédé catalytique de réformage à l'oxygène. De la sorte, seulement 10 à 20% du carbone provenant du matériau de départ se retrouve sous forme de CO2, le reste, soit 80 à 90% étant sous la forme CO. Un autre avantage réside dans le fait que la consommation d'oxygène est moins élevée que dans les procédés connus.A gas is thus obtained very simply free of methane, higher hydrocarbons, and whose carbon dioxide content is lower than that obtained for example by a catalytic process of oxygen reforming. In this way, only 10 to 20% of the carbon originating from the starting material is found in the form of CO 2 , the rest, ie 80 to 90% being in the CO form. Another advantage is that the oxygen consumption is lower than in known methods.

Bien entendu, le chauffage à haute température du gaz injecté entraine un surcroît de consommation d'énergie, en particulier d'énergie électrique pour l'alimentation de la torche à plasma 4.Of course, the high temperature heating of the injected gas leads to an increase in energy consumption, in particular electrical energy for the supply of the plasma torch 4.

Cependant, compte tenu des avantages apportés, l'association d'une torche à plasma au réacteur de conversion sera intéressante dans de nombreux cas, en particulier chaque fois que l'on dispose d'une source importante et bon marché d'énergie, par exemple d'origine hydroélectrique. En effet, le procédé permet d'économiser la biomasse pour la production du gaz de synthèse et cette économie peut être importante même dans les pays où l'on dispose de grande quantité de biomasse car on ne peut concevoir la réalisation d'installation de gazéification importante qu'en les associant à des cultures énergétiques rapidement renouvelables réalisées à cet effet. Pour être exploitées dans de bonnes conditions, celles-ci ne devraient pas être exploitées de l'installation de gazéification et c'est pourquoi, même dans un pays très favorisé du point de vue du renouvellement de la biomasse, il est utile de tirer le maximum d'énergie potentielle, dont de CO et de H2 de cette substance. La consommation, même importante, d'énergie électrique, peut donc être avantageuse, et c'est en particulier le cas lorsque des installations imporantes de production d'énergie hydroélectrique ou électronucléaire sont placées dans des régions relativement isolées qui peuvent également convenir à des cultures énergétiques.However, in view of the advantages provided, the association of a plasma torch with the conversion reactor will be advantageous in many cases, in particular whenever there is a large and inexpensive source of energy, for example example of hydroelectric origin. Indeed, the process makes it possible to save the biomass for the production of synthesis gas and this saving can be significant even in countries where there is a large amount of biomass because it is not possible to conceive the realization of gasification installation. important than by combining them with rapidly renewable energy crops produced for this purpose. To be exploited in good conditions, these should not be exploited from the gasification installation and this is why, even in a country very favored from the point of view of the renewal of the biomass, it is useful to draw the maximum potential energy, including CO and H2 of this substance. The consumption, even important, of electric energy, can thus be advantageous, and it is in particular the case when important installations of production of hydroelectric or nuclear power are placed in relatively isolated regions which can also be suitable for crops energetic.

Le gaz injecté à haute température, après passage dans la torche à plasma, peut, être, simplement, du gaz du synthèse recyclé en proportions convenables. Dans ce cas, le gaz sortant en 22 du réacteur de conversion 2 ne contient pratiquement que CO+H2+C02+H20 mais le rapport H2/ CO doit être ajusté à la valeur adéquate avant la synthèse chimique réalisée dans une installation 5 prévue à cet effet. Pour la synthèse du méthanol, par exemple, ce rapport doit être voisin de 2 alors qu'il est généralement voisin de 1 à la sortie du réacteur de conversion 2. Pour cela, on peut convertir ultérieurement ce gaz par la réaction connue de conversion du CO:

Figure imgb0010
The gas injected at high temperature, after passing through the plasma torch, can simply be synthetic gas recycled in suitable proportions. In this case, the gas leaving at 22 from the conversion reactor 2 contains practically only CO + H 2 + C0 2 + H 2 0 but the H 2 / CO ratio must be adjusted to the appropriate value before the chemical synthesis carried out in a installation 5 provided for this purpose. For the synthesis of methanol, for example, this ratio must be close to 2 whereas it is generally close to 1 at the outlet of the conversion reactor 2. For this, this gas can be converted subsequently by the known conversion reaction of CO:
Figure imgb0010

Pour générer de l'hydrogène la réaction consomme donc une partie du CO et gènère en outre du C02 supplémentaire.To generate hydrogen, the reaction therefore consumes part of the CO and also generates additional CO 2 .

Pour éviter cet inconvénient, dans un mode de réalisation particulièrement avantageux, le gaz insuflé est de l'hydrogène. Compte tenu du débit et de la température des gaz issus de la gazéification, et de la température que permet d'obtenir la torche à plasma 4, on peut on effet injecter par la lance 3 un débit contrôlé d'hydrogène, de façon à maitriser le rapport H2/CO dans le gaz produit. On fait alors l'économie de l'étape de conversion du CO et il suffit d'éliminer le vapeur d'eau dans un simple dispositif de condensation 51.To avoid this drawback, in a particularly advantageous embodiment, the blown gas is hydrogen. Taking into account the flow rate and the temperature of the gases resulting from the gasification, and the temperature which makes it possible to obtain the plasma torch 4, it is possible to inject by the lance 3 a controlled flow of hydrogen, so as to control the H 2 / CO ratio in the gas produced. The CO conversion step is then saved and it suffices to eliminate the water vapor in a simple condensing device 51.

Comme on peut difficilement disposer, en particulier dans un endroit isolé, d'une réserve d'hydrogène, il est particulièrement intéressant d'associer l'installation à un dispositif 6 d'électrolyse de l'eau. De la sorte, en effet, d'installation peut fonctionner uniquement avec une source de matière hydrocarbonée et une source d'énergie électrique car l'électrolyse de l'eau permet de générer en même temps, en quantité suffisante, l'oxygène injecté en 13 dans le réacteur 1 pour y apporter la quantité de chaleur nécessaire à la réaction de gazéification. On pourra même produire une certaine quantité d'oxygène en excès, récupéré en 15. L'utilisation d'un dispositif d'électrolyse permettra donc d'éviter la production d'oxygène par distillation de l'air.As it is difficult to have, in particular in an isolated location, a reserve of hydrogen, it is particularly advantageous to associate the installation with a device 6 for electrolysis of water. In this way, in fact, the installation can operate only with a source of hydrocarbon material and a source of electrical energy because the electrolysis of water makes it possible to generate at the same time, in sufficient quantity, the oxygen injected in 13 in the reactor 1 to supply the quantity of heat necessary for the gasification reaction. It will even be possible to produce a certain amount of excess oxygen, recovered at 15. The use of an electrolysis device will therefore make it possible to avoid the production of oxygen by distillation of the air.

En outre, un autre avantage de l'utilisation de l'électrolyse réside dans le fait qu'il existe des dispositifs d'électrolyse fournissant de l'hydrogène sous une pression qui peut aller jusqu'à 70 bars. L'hydrogène peut donc être conduit directement, par le circuit 31 dans la torche à plasma 4 sans compression préalable.In addition, another advantage of using electrolysis lies in the fact that there are electrolysis devices supplying hydrogen under a pressure which can be up to 70 bars. The hydrogen can therefore be led directly, through the circuit 31 in the plasma torch 4 without prior compression.

D'autre part, la gazéification et la conversion dans les réacteurs 1 et 2 pourront être réalisées sous pression et par conséquent de façon plus économique grâce à la réduction qui en résulte des dimensions des équipements et à l'économie faite sur la compression des gaz avant la synthèse, celle-ci devant, dans tous les cas, être réalisée sous pression.On the other hand, gasification and conversion in reactors 1 and 2 can be carried out under pressure and therefore more economically thanks to the resulting reduction in the dimensions of the equipment and the savings made on gas compression. before the synthesis, this must, in all cases, be carried out under pressure.

Bien entendu, l'invention ne se limite pas aux modes de réalisation qui viennent d'être décrits à titre d'exemple, d'autres variantes pouvant être imaginées en restant dans le cadre de la protection revendiquée.Of course, the invention is not limited to the embodiments which have just been described by way of example, other variants which can be imagined while remaining within the framework of the claimed protection.

C'est ainsi que le gaz à haute température injecté dans le réacteur de conversion pourrait être, d'une façon générale, tout gaz utile à la synthèse, par exemple de l'azote dans le cas de la production d'ammoniac.Thus, the high temperature gas injected into the conversion reactor could, in general, be any gas useful for synthesis, for example nitrogen in the case of the production of ammonia.

Claims (5)

1. A process for the production of synthesis gas, wherein a hydrocarbon substance of vegetable origin, such as a biomass product, is first gasified in a first reactor (1) at a moderate temperature lower than the melting temperature of the ash, with the production, in addition to usable carbon monoxide and hydrogen, of "inevitable" species such as unconverted carbon, hydrocarbons and tars, whereafter the inevitable species are converted at high temperature in a second reactor (2) into hydrogen and carbon monoxide, characterized in that an increase to the conversion temperature in the second reactor (2) is obtained by blowing in a gas flow previously heated to a temperature of between 3000 and 5000°C by passing such gas through a plasma torch (4) disposed at the outlet of a circuit (3) via which gas is blown into the conversion reactor (2), the flow rate of the blown-in gas being controlled in dependence on the temperature and proportions of carbon monoxide and hydrogen already existing in the mixture leaving the first gasification reactor (1).
2. A process for the production of synthesis gas according to claim 1, characterized in that the gas blow in is hydrogen.
3. A process for the production of synthesis gas according to claim 1, characterized in that the gas blown in is nitrogen.
4. A process for the production of synthesis gas according to claim 1, characterized in that the gasification temperature in the first reactor (1) is between 700 and 800°C.
5. An installation for the production of synthesis gas, comprising a first reactor (1) for the gasification of a hydrocarbon substance of vegetable origin such as a biomass product, and a second reactor (2) for converting the inevitable species contained in the gas mixture leaving the first reactor (1), characterized in that the conversion reactor (2) has a plasma torch (4) disposed at the outlet of a nozzle (3) for blowing in hydrogen heated by the plasma torch to a temperature of between 3000 and 5000°C. and means for controlling the flow rate of the blown-in hydrogen in relation to the flow rate and temperature of the gases leaving the gasification reactor (1), so as to raise the mean temperature of the gas mixture in the conversion reactor (2) t6 a level adequate for the conversion of the invevitable species.
EP19850400229 1984-02-16 1985-02-12 Process for the production of synthesis gas Expired EP0153235B1 (en)

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