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  • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
  • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
  • C01B3/36—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents
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  • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
  • C01B3/36—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents
  • C01B3/363—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using oxygen or mixtures containing oxygen as gasifying agents characterised by the burner used
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  • C01B3/06—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen, e.g. water, acids, bases, ammonia, with inorganic reducing agents
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  • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
  • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
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  • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
  • C10G2/30—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen
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  • C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions
  • C10G47/22—Non-catalytic cracking in the presence of hydrogen
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  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
  • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
  • C10K3/001—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by thermal treatment
  • C10K3/003—Reducing the tar content
  • C10K3/008—Reducing the tar content by cracking
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  • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
  • C10K—PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
  • C10K3/00—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide
  • C10K3/02—Modifying the chemical composition of combustible gases containing carbon monoxide to produce an improved fuel, e.g. one of different calorific value, which may be free from carbon monoxide by catalytic treatment
  • C10K3/026—Increasing the carbon monoxide content, e.g. reverse water-gas shift [RWGS]
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  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/00049—Controlling or regulating processes
  • B01J2219/00051—Controlling the temperature
  • B01J2219/0015—Controlling the temperature by thermal insulation means
  • B01J2219/00155—Controlling the temperature by thermal insulation means using insulating materials or refractories
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/00049—Controlling or regulating processes
  • B01J2219/00051—Controlling the temperature
  • B01J2219/00157—Controlling the temperature by means of a burner
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  • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
  • B01J2219/00049—Controlling or regulating processes
  • B01J2219/00051—Controlling the temperature
  • B01J2219/00159—Controlling the temperature controlling multiple zones along the direction of flow, e.g. pre-heating and after-cooling
• • B—PERFORMING OPERATIONS; TRANSPORTING
  • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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  • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
  • C01B2203/02—Processes for making hydrogen or synthesis gas
  • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
  • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
  • C01B2203/0238—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a carbon dioxide reforming step
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  • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
  • C01B2203/0255—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a non-catalytic partial oxidation step
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  • C01B2203/02—Processes for making hydrogen or synthesis gas
  • C01B2203/0283—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step
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  • C01B2203/08—Methods of heating or cooling
  • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
  • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
  • C01B2203/0816—Heating by flames
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  • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
  • C01B2203/1205—Composition of the feed
  • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
  • C01B2203/1235—Hydrocarbons
  • C01B2203/1241—Natural gas or methane
• • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
  • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
  • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
  • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
  • Y02E60/30—Hydrogen technology
  • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
• • 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
  • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
  • Y02P20/00—Technologies relating to chemical industry
  • Y02P20/141—Feedstock

Definitions

• the present application relates to a method and a reactor for producing synthesis gas from a source of carbon and hydrogen (H2). More particularly, the synthesis gas production method is carried out in the direct presence of an Oxy-flame to transform a flow comprising a source of carbon and hydrogen into synthesis gas.
• CO2 as well captured can be used as a carbon source for the production of a broad spectrum of products that can be considered carbon neutral, ie, whose production and use cycle involves virtually no net emissions of GHGs. It is thus possible to produce carbon neutral synthetic fuels that can be used in existing infrastructure.
• syngas By reacting CO2 with excess hydrogen (H2), mixtures of hydrogen and CO can be produced. Such mixtures are called “synthesis gas” or “syngas” in English. These syngas may also contain some residual CO2.
• Synthesis gases can be used to produce a spectrum of basic chemicals. These products include methanol and hydrocarbons such as those found in motor gasoline, diesel, kerosene.
• Methanol is a platform molecule that can be used as a raw material for a large number of other commodities such as formaldehyde. Methanol is also known for its use in windshield washer fluid and as an industrial solvent. It can also be used as a fuel. Methanol can even be transformed into synthetic hydrocarbons. Finally, methanol can be transformed into dimethyl ether (DME), itself a chemical intermediate. DME is used, among other things, as a propellant for aerosols. DME can be used as a diesel engine fuel or as an alternative to propane.
• DME dimethyl ether
• Synthetic hydrocarbons can be produced from synthesis gas, according to Fischer-Tropsch reaction (C):
• the CO / H2 mixtures useful as synthesis gas for these products must be balanced, i.e., they must contain the correct proportions of H2 and CO.
• the synthesis gas syngas
• the molar proportions of the gases to be able to carry out the reactions (B) or (C) generally correspond to the ratios R1 or R2 of the following equations (D) and (E):
• a very large number of chemical and hydrocarbon syntheses can be carried out with syngas that can meet the criteria of R1 or R2 molar composition. It should also be noted that it is possible to produce methane, CPU, from synthesis gas. One mole of methane can be formed from 1 mole of CO and 3 moles of H2.
• RWGS (A) The reaction of RWGS (A) is endothermic (reaction enthalpy of 41 kJ / mole at room temperature). According to the stoichiometry of this reaction, to produce 1 kg of CO, it takes 1.57 kg of CO2 and 0.07 kg of H2 and it is necessary to provide 1465 kJ or 0.4 kWh of thermal energy. To carry out this reaction, use is generally made of catalytic bed reactors. However, the use of conventional catalysts to carry out reaction (A) does not make it possible to obtain high conversion rates. This means that the conversion per pass, that is, the conversion during the passage of CO2 through a catalytic bed, turns out to be rather low.
• reaction (A) becomes rather favorable at higher temperature levels. This is illustrated by Table 1 which presents the value of the equilibrium constant as a function of temperature (at atmospheric pressure).
• the present technology relates to a method of producing synthesis gas comprising carbon monoxide (CO) and hydrogen (hte), in which the synthesis gas is produced by a reduction reaction of a. first flow comprising a source of carbon and an excess of hydrogen in contact with an Oxy-flame, and in which: the hydrogen comes from a reducing current, a first part of which is found in the first flow and a second part is used to generate Oxy-flame by combustion of hydrogen in the presence of a second stream comprising oxygen (O2), the second stream coming from an oxidizing stream, the first stream and the second stream are at a distance from each other such that the Oxy-flame sustains the reaction between the carbon source and the hydrogen.
• CO carbon monoxide
• hte hydrogen
• the method is such that the reduction reaction is carried out in the absence of solid catalyst.
• the method is such that the Oxy-flame generates ionic species and free radicals which promote the conversion of the carbon source to CO.
• the method is such that the carbon source comprises:
• the carbon source comprises CO2 and the reduction reaction comprises a reverse reaction of gas to water or “Reverse Water Gas Shift”.
• the method is such that the reducing current is hydrogen.
• the reducing stream includes hydrogen and the carbon source.
• the reducing stream comprises hydrogen and CO2.
• the method is such that the reducing current comprises hydrogen, CO2 and at least one type of oxygenated molecules of formula CaHpO Y where a is between 1 and 5, b is between 2 and 10 and y is between 1 and 4.
• the method is such that the oxidizing current is oxygen.
• the oxidizing stream comprises oxygen and CO2.
• the method is such that the reducing current comprises only hydrogen, the oxidizing current comprises only oxygen and the carbon source is supplied by an independent current.
• the independent current comprises CO2.
• the independent stream comprises CO2 and methane.
• the method is such that the oxygen comes from an electrolysis reaction of water.
• the method is such that the hydrogen comes from an electrolysis reaction of water.
• the method is such that the carbon source comes from a gas mixture resulting from a process for gasification or pyrolysis of biomass.
• the method is such that the reduction reaction is carried out at an average temperature of at least 600 ° C.
• the reduction reaction is carried out at an average temperature of at least 1200 ° C.
• the reduction reaction is carried out at an average temperature of at most 2200 ° C.
• the method is such that the first stream and the second stream are at a distance from each other of between 0.1 mm and 100 mm. According to another embodiment, the first stream and the second stream are at a distance from each other of between 0.3 mm and 50 mm. According to another embodiment, the first flow and the second flow are spaced from each other between 0.6 mm and 30 mm.
• the method is such that the carbon source comprises CO2 and the reduction reaction is carried out using an H2 / CO2 molar ratio of between 2 and 7.
• the method is such that the carbon source comprises CO2 and the reduction reaction is carried out using an O2 / CO2 molar ratio of between 0.35 and 0.9.
• the method is such that the reduction reaction is carried out using an O2 / H2 molar ratio of between 0.1 and 0.3.
• the method is such that the synthesis gas produced has an H2 / CO molar ratio of at least 1.8. According to another embodiment, the synthesis gas produced has an H2 / CO molar ratio of at least 2. According to another embodiment, the synthesis gas produced has an H2 / CO molar ratio of between 1.8 and 5.0.
• the method is such that the synthesis gas produced further comprises CO2.
• the method is such that the synthesis gas produced has a molar ratio of host, CO and CO2 such that (H2 - CO2) / (CO + CO2) 3 2.
• the method further comprises cooling the synthesis gas to form a cooled synthesis gas.
• the method further comprises condensing water contained in the cooled synthesis gas and recovering the water. According to another embodiment, at least part of the recovered water is recycled to the cooling step.
• the present technology relates to the use of a synthesis gas produced by the method according to the present technology, for the manufacture of chemicals or fuels.
• the present technology relates to the use of a synthesis gas produced by the method according to the present technology, for the manufacture of methanol or synthetic hydrocarbons.
• the present technology relates to a reactor for producing a synthesis gas comprising carbon monoxide (CO) and hydrogen (H2), said reactor comprising: a reaction chamber in which the synthesis gas is produced by a reduction reaction of a first flow comprising a source of carbon and an excess of hydrogen in contact with an oxy-flame, at least one first means for supplying the reaction chamber with a reducing current comprising hydrogen, a first part of the reducing current being found in the first flow and a second part being used to generate the Oxy-flame in the combustion chamber, by combustion of hydrogen in the presence of a second flow comprising oxygen ( O2), at least one second means for supplying the reaction chamber with an oxidizing current forming the second flow, the first flux and the second flux being at a distance from each other such that the Oxy-flame supports the reaction between the carbon source and the hydrogen.
• CO carbon monoxide
• H2 hydrogen
• the reactor is such that the reduction reaction is carried out in the absence of solid catalyst.
• the reactor is such that the Oxy-flame generates ionic species and free radicals which promote the conversion of the carbon source to CO.
• the reactor is such that the carbon source comprises:
• the reactor is such that the carbon source comprises CO2 and the reduction reaction is the reverse reaction of gas to water or "Reverse Water Gas Shift".
• the reactor is such that the reducing stream is hydrogen.
• the reducing stream includes hydrogen and the carbon source.
• the reducing stream comprises hydrogen and CO2.
• the reactor is such that the reducing current comprises hydrogen, CO 2 and at least one type of oxygenated molecules of formula CaHpO Y where a is between 1 and 5, b is between 2 and 10 and g is between 1 and 4.
• the reactor is such that the oxidizing current is oxygen.
• the oxidizing current comprises oxygen and CO2.
• the reactor is such that the first means for supplying the reducing current and the second means for supplying the oxidizing current are tubes.
• the reactor comprises a plurality of second means consisting of a plurality of tubes allowing the injection of the oxidizing current into the reaction chamber, and a plurality of first means consisting of a plurality of openings allowing the injection of the reducing current into the reaction chamber.
• each opening is defined by an annular space bounded by the outer diameter of one of the plurality of tubes and extending perpendicularly from the outer wall of the tube.
• the reactor further comprises a reducing current distribution chamber separated from the reaction chamber by a separation wall, said distribution chamber and said separation wall being crossed by the plurality of tubes, the annular space extending perpendicularly from the outer wall of each tube also passing through the partition wall.
• the reactor is such that the reducing current is hydrogen which is supplied to the reaction chamber by the first means consisting of a first tube, the oxidizing current is oxygen which is supplied to the reaction chamber.
• reaction chamber by the second means consisting of a second tube, and the carbon source is supplied by an independent current which is injected into the reaction chamber through at least one opening located in a wall of the reaction chamber.
• the opening is formed by a third tube concentric with the first tube and the second tube, the second tube forming the inner tube, the first tube forming an intermediate tube and the third tube forming an outer tube.
• the opening is formed by an annular space delimited by an internal diameter of the third tube and an external diameter of the first tube.
• the reactor further comprises a distribution chamber separated from the reaction chamber by a separation wall, said distribution chamber serving to supply the independent current comprising the carbon source and being traversed by the first tube. and the second tube.
• the reactor is such that the independent stream comprises CO2.
• the reactor is such that the independent stream comprises CC and methane.
• the reactor is such that the oxygen originates from an electrolysis reaction of water.
• the reactor is such that the hydrogen originates from a reaction of electrolysis of water.
• the reactor is such that the carbon source comes from a gas mixture resulting from a process for gasification or pyrolysis of biomass.
• the reactor is such that the reaction chamber reaches a temperature of at least 600 ° C during the reduction reaction. In another embodiment, the reaction chamber reaches a temperature of at least 1200 ° C during the reduction reaction. In another embodiment, the reaction chamber reaches a temperature of at most 2200 ° C during the reduction reaction.
• the reactor is such that the first flow and the second flow are at a distance from each other of between 0.1 mm and 100 mm. According to another embodiment, the first flow and the second flow are at a distance from each other of between 0.3 mm and 50 mm. According to another embodiment, the first flow and the second flow are at a distance from each other of between 0.6 mm and 30 mm. According to another embodiment, the reactor is such that the carbon source comprises CO2 and the reduction reaction is carried out using an H2 / CO2 molar ratio of between 2 and 7. According to another embodiment, the source of carbon comprises CC and the reduction reaction is carried out using an O2 / CO2 molar ratio of between 0.35 and 0.9.
• the reactor is such that the reduction reaction is carried out using an O2 / H2 molar ratio of between 0.1 and 0.3.
• the reactor is such that the synthesis gas produced has an H2 / CO molar ratio of at least 1.8. According to another embodiment, the synthesis gas produced has an H2 / CO molar ratio of at least 2. According to another embodiment, the synthesis gas produced has an H2 / CO molar ratio of between 1.8 and 5.0.
• the reactor is such that the synthesis gas produced further comprises CO2.
• the reactor is such that the synthesis gas produced has a molar ratio of H2, CO and CO2 such that (H2 - CO2) / (CO + CO2) 3 2.
• the present technology relates to a system comprising the reactor as defined according to the present technology, coupled to a device for cooling the synthesis gas to form a cooled synthesis gas.
• the system is such that the cooling device is a direct contact cooler.
• the system further comprises a water condensing apparatus for recovering water from the cooled syngas.
• the system is such that the condensing apparatus is a cooler-condenser. According to another embodiment, the system further comprises equipment for recycling at least part of the recovered water to the cooling device.
• Figure 1 is a schematic of the general principle of operation of the present method to produce syngas.
• Figure 2 shows a sectional view along the vertical of a reactor which can be used to carry out the method of producing syngas according to a first embodiment.
• Figure 3 shows certain distance parameters between the different flows and / or between different elements of the reactor according to one embodiment of the syngas production method.
• Figure 4 shows a sectional view along the vertical of a reactor which can be used to carry out the syngas production method according to another embodiment.
• Figure 5 shows a sectional view along the vertical of a reactor which can be used to carry out the method of producing syngas according to another embodiment.
• Figure 6a shows a sectional view along the vertical of a reactor which can be used to carry out the syngas production method according to another embodiment.
• Figure 6b shows a top cross-sectional view of the reactor of Figure 6a.
• An enlarged view of two concentric tubes is also shown in Figure 6b to explain the distance parameter according to this embodiment.
• Figure 7 shows a diagram of the syngas production process according to yet another embodiment.
• Figure 8 shows a schematic sectional view along the vertical of a mini reactor used for the examples. The figure shows the general arrangement of the tubes for this mini-reactor.
• the terms “synthesis gas” and “syngas” are used interchangeably to identify a gas mixture comprising at least carbon monoxide (CO) and hydrogen (H2).
• the syngas or syngas can include CO2.
• the H2 / CO molar ratio in the synthesis gas is greater than or equal 1.
• the synthesis gas can have an H2 / CO molar ratio of at least 1.8, for example between 1.8 and 5.0.
• the H2 / CO molar ratio in the synthesis gas is greater than or equal
• the H2 / CO molar ratio in the synthesis gas can be 1, 8 or 1, 9 or 2.0 or 2.1 or 2.2 or 2.3 or 2.4 or 2.5 or 2.6 or 2.7 or 2.8 or 2.9 or 3.0 or 3.1 or 3.2 or 3.3 or 3.4 or 3.5 or 3.6 or 3.7 or 3, 8 or 3.9 or 4.0 or 4.1 or 4.2 or 4.3 or 4.4 or 4.5 or 4.6 or 4.7 or 4.8 or 4.9 or 5.0.
• synthesis gases with different and varied H2 / CO molar ratios can be obtained.
• the term “stream” is used to describe the different gas streams which will feed the reaction chamber in which the formation of synthesis gas is carried out.
• the method uses at least one stream containing hydrogen (H2) and at least one stream containing oxygen (O2).
• the carbon source used in the method can be supplied either by an independent current, or by the current containing GO2, or by the current containing I ⁇ 2.
• the streams entering the reaction chamber are in the gaseous state. If necessary, the reagents in the liquid state can be vaporized so that they arrive in the reaction chamber in gaseous form.
• the term "stream” is used to describe the various gas streams that are involved in carrying out the synthesis gas production reaction, inside the reaction chamber.
• the reaction involves a reducing stream containing hydrogen (H2) and the carbon source which will react with each other to form synthesis gas, and an oxidizing stream containing hydrogen (H2). oxygen (O2) which will react with hydrogen (H2) to form an Oxy-flame.
• carbon source describes the chemical compound (s) that are used to provide the carbon that ends up in the synthesis gas produced.
• the carbon source provides at least the carbon that ends up in the carbon monoxide (CO) produced.
• CO carbon monoxide
• the carbon source can comprise CO2.
• the carbon source can comprise one or more types of oxygenated carbon-based molecules of formula CaHpO Y where a is between 1 and 5, b is between 2 and 10 and y is between 1 and 4
• the carbon source can also comprise one or more hydrocarbons such as, for example, alkanes, alkenes and / or aromatics.
• the carbon source used to produce the synthesis gas is a combination of two or more of the different sources described above.
• the carbon source can comprise CO2 and one or more oxygenated molecules of the CaHpO Y type.
• the carbon source can comprise CO2 and one or more hydrocarbons, for example CO2 and methane.
• This oxygen can be supplied by CO2, but it can also be supplied in the form of water vapor.
• the carbon source can comprise one or more hydrocarbons, CO2 and water vapor. The water vapor, when required, can come from the reaction which generates the Oxy-flame (see reaction (G) below) and / or can be fed into the reaction chamber.
• the carbon source can vary.
• the carbon source includes CO2 which can generally come from two main categories of sources: anthropogenic sources, linked to human activities and natural sources, known as biogenic.
• This method can use CO2 from both types of sources and can also use pure CO2.
• a gas mixture comprising CO2 and one or more types of oxygenated molecules of formula CaHpO Y where a is between 1 and 5, b is between 2 and 10 and g is between 1 and 4 can be used.
• the carbon source may simply include one or more types of CaHpO Y molecules.
• a gas mixture comprising CO2 and hydrocarbons, such as alkanes (eg, methane), alkenes and / or aromatic molecules, can also be used.
• hydrocarbons such as alkanes (eg, methane), alkenes and / or aromatic molecules
• the carbon source can comprise CO2, one or more types of CaHpO Y molecules and one or more types of hydrocarbons.
• a wide range of organic molecules, including products from a fossil source, which may optionally contain sulfur, can be present in the gas mixture providing the carbon source.
• an "Oxy-flame” is understood to mean a flame produced by the combustion of hydrogen in the presence of an oxidant such as oxygen (O2) according to the following reaction (F):
• This flame is bright and radiant and provides the heat required to support the reaction that will produce synthesis gas from the carbon source.
• This flame can generate ionic species and free radicals which can catalyze the conversion of the carbon source to CO.
• the Oxy-flame can make it possible to reach an average temperature, in the reaction chamber, of at least about 600 ° C.
• the average temperature reached in the reaction chamber is at least about 1200 ° C.
• the temperature reached in the reaction chamber can be up to about 2200 ° C.
• the reaction of producing synthesis gas in the reaction chamber can be carried out at an average temperature of at least 600 ° C up to about 2200 ° C.
• Oxy-flame can be qualified as a “reduction oxy-flame” because the combustion reaction between hydrogen and oxygen takes place in the presence of an excess of hydrogen.
• the oxidant which is used to produce the Oxy-flame can be a mixture based on oxygen (O2), preferably pure oxygen.
• oxygen oxygen
• pure oxygen it is understood that this does not necessarily mean a purity of 100%, but that the oxygen-based mixture substantially comprises GO2 and may be accompanied by certain impurities such as N2, H2O for example.
• the reaction to form synthesis gas is carried out in the presence of excess hydrogen.
• excess hydrogen it will be understood that the quantity of hydrogen (H2) must be sufficient on the one hand to allow the combustion reaction (F) to produce the oxy-flame and on the other hand to be able to carry out the combustion reaction.
• reaction for converting the carbon source into synthesis gas The amount of hydrogen required can be determined depending on the carbon source used and taking into account the stoichiometry of the reactions involved.
• the hydrogen required in the present method as well as the oxygen used to produce the Oxy-flame can, at least in part, result from a reaction. electrolysis of water. This can be even more beneficial if the water electrolysis system is powered by renewable electricity.
• the combustion which produces the Oxy-flame can be initiated using an ignition device, such as an electric arc, a glowing wire, or any other known source of energy.
• the present method can produce a syngas essentially containing H2 and CO in an H2 / CO molar ratio close to 2.
• the present method is suitable for the production of syngas whose composition meets the conditions. presented by equations (D) and (E) reported above. This is made possible by varying the proportions of the different gas streams producing the oxidizing stream and the reducing stream.
• Figure 1 illustrates the general principle of how the method works. A reducing flow (on the right in the figure) comprising at least hydrogen and the carbon source is found in a reaction chamber (10).
• the heat required to convert the carbon source to CO is provided by means of a hot flame, called an Oxy-flame, which is produced by the combustion of hydrogen in the presence of an oxidant such as oxygen. (left part of the figure).
• Part of the hydrogen supplied to the reaction chamber can be used to produce the Oxy-flame (bottom arrow in the figure).
• Another part of the hydrogen supplied to the reaction chamber is used as such for the production of the synthesis gas.
• the Oxy-flame in addition to providing the heat required for the reaction to convert the carbon source to CO, can generate ionic species and free radicals which can promote this conversion.
• the hydrogen is introduced in excess in the reaction chamber and a part is evacuated with the CO to form the syngas. Taken together, the entire process can be termed an “autothermal” process.
• the reaction chamber (10) there are therefore two distinct flows: a first which comes from an oxidizing gas based on pure oxygen called oxidizing flow, and another flow, called reducing flow, resulting from a mixture reducing gas based on hydrogen and containing the carbon source. These two flows are close to each other.
• the two flows can be separated by a distance “d” from each other such that 0.1 mm ⁇ d ⁇ 100 mm.
• the distance d separating the two flows may be such that 0.3 mm ⁇ d ⁇ 50 mm. This distance can preferably be such that 0.6 mm ⁇ d ⁇ 30 mm.
• the distance d separating the two streams can be 0.1mm, 0.2mm, 0.3mm, 0.4mm, 0.5mm, 0.6mm, 0.7mm, 0.8 mm, 0.9mm, 1mm, 5mm, 10mm, 15mm, 20mm, 25mm, 35mm, 40mm, 45mm, 50mm, 55mm, 60mm, 65mm, 70mm, 75 mm, 80 mm, 85 mm, 90 mm, 95 mm, 100 mm, or any distance between these values.
• the reducing and oxidizing flows which are found in the reaction chamber can be obtained from various currents.
• the reducing flow comes from a reducing current comprising at least H2 and the flow oxidant originates from an oxidizing stream comprising at least oxygen.
• the source of carbon which is found in the reducing flow in the reaction chamber, can be supplied either by the reducing current, or by an independent current, or by the oxidizing current if this carbon source comprises CO2 only. .
• a first realization of the syngas production method is shown on the Error! Source of the referral not found. This realization is particularly suited to the production of syngas from CO2 as a carbon source.
• a stream comprising oxygen (1) is mixed with a stream comprising CO2 (2) to produce an oxidizing stream (3) comprising a mixture of O2 and CO2.
• the oxidizing stream (3) is passed through a tube (4) allowing the injection of the mixture of O2 and CO2 inside the reaction chamber (10) of a reactor. Inside the reaction chamber (10), the mixture of O2 and CO2 forms an oxidizing flow (6), of which GO2 will be used to produce the Oxy-flame (9).
• a stream comprising hydrogen (5) is injected inside the reaction chamber, through an annular space defined between the outer wall of the tube (4) and the circumference of an opening (7) in the chamber. entrance to the reaction chamber.
• the hydrogen stream (5) constitutes a reducing stream which, once inside the chamber, will form a reducing stream which itself divides into two parts: a first part (8a) of the reducing stream will react with the oxidizing flux (6) according to the hydrogen combustion reaction (F) to produce the Oxy-flame (9).
• the second part (8b) of the hydrogen stream serves as the reagent ingredient for the reaction of RWGS (A).
• the heat required for this reaction comes from the Oxy-flame (9).
• Reactions (F) and (A) take place inside the reaction chamber (10) to form a gas mixture (12) consisting of hydrogen, carbon monoxide, carbon dioxide and vapor. water.
• the gas mixture (12) is also called wet syngas.
• This gas mixture (12) is discharged through the opening (13) of the reactor.
• the reactor used for this embodiment comprises a wall (14) which can be lined with refractory and insulating materials (11).
• the volume of the reaction chamber (10) is determined by the cylindrical space defined by the length L and the diameter D.
• combustion can be initiated using a conventional ignition device as per example an electric arc, an incandescent wire (not shown in the figure).
• the reactor can be equipped with a device making it possible to measure the temperature inside the reaction chamber.
• Such a device can for example be a thermocouple (not shown in the figure).
• the injection tube (4) of the oxidizing stream (3) can be fixed by means of a device (15).
• the fixing device (15) can serve both as a guide for the injection tube (4) and as a sealing system.
• the fixing device (15) can for example comprise clamps with cable glands.
• the length L of the reaction chamber may be between 1 cm and 300 cm, preferably between 10 cm and 100 cm.
• the diameter D of the reaction chamber can for example be between 0.3 cm and 100 cm, preferably between 1 cm and 50 cm. According to some embodiments, these values of length and diameter of the reaction chamber can also be applied to the reactors shown in Figures 2 to 5.
• the different gas streams can be characterized by certain parameters which will be defined below. Some of these parameters depend on different distances which are shown for example in Figure 3.
• v1 n ⁇ / ((p / 4) ⁇ i L 2)
• the diameter Di is such that the speed v1 characterizing the oxidizing flow (6) is at least 1 m / s, based on the volume flow V1. According to another embodiment, the diameter Di is such that the speed v1 is between 5 m / s and 150 m / s, preferably between 5 and 100 m / s.
• the speed v1 can therefore be for example between 5 m / s and 90 m / s, between 5 m / s and 80 m / s, between 5 m / s and 70 m / s, between 5 m / s and 60 m / s, between 5 m / s and 50 m / s, between 5 m / s and 40 m / s, between 5 m / s and 30 m s, between 5 m / s and 20 m / s, or between 5 m / s and 10 m / s.
• the opening (7) characterized by (D / 2-DV2) can be such that the speed v2 of the reducing current flowing in the annular space defined between the outer wall of the tube (4) and the circumference of the opening (7 ), will be at least 1 m / s based on the V2 volume flow.
• the opening (7) (D / 2-DV2) is such that the speed v2 is between 5 m / s and 150 m / s, preferably between 10 and 100 m / s.
• the speed v2 can therefore be for example between 10 m / s and 90 m / s, between 10 m / s and 80 m / s, between 10 m / s and 70 m / s, between 10 m / s and 60 m / s, between 10 m / s and 50 m / s, or between 10 m / s and 40 m / s.
• the distance d may be between 0.1 mm and 100 mm, preferably between 0.3 mm and 50 mm, and preferably between 0.6 mm and 30 mm.
• the distance d can also be any distance within these ranges of values.
• the volume of the reaction chamber (10) of the reactor will allow a certain residence time of all the reactants inside the reaction chamber (10) of at least 0.01 second.
• V1 can be between 2 L / min (3.33E-5 m 3 / s) and 100,000 L / min (1.67 m 3 / s), preferably between 5 L / min (8.33E -05 m 3 / s) and 50,000 L / min (0.84 m 3 / s).
• V2 can be between 10 L / min (1.67E-04 m 3 / s) and 300000 L / min (5 m 3 / s), preferably between 25 L / min (4.17E-04 m 3 / s) and 200,000 L / min (3.33 m 3 / s).
• the method for producing the syngas can be carried out using an H2 / CO2 molar ratio of between 2 and 7.
• the O2 / CO2 molar ratio can for example be between 0.35 and 0.9.
• the production of syngas can be carried out using, for example, an O2 / H2 molar ratio of between 0.1 and 0.3.
• the method for producing the syngas can be carried out using the following molar proportions of the different reagents:
• the temperature reached inside the reaction chamber during syngas production can be at least 600 ° C. This temperature can be at most 2200 ° C. It will be understood that the temperature can therefore vary between a value of 600 ° C and 2200 ° C, and can therefore be for example 1000 ° C, 1100 ° C, 1200 ° C, 1300 ° C, 1400 ° C, 1500 ° C, 1600 ° C, 1700 ° C, 1800 ° C, 1900 ° C, 2000 ° C, 2100 ° C and 2200 ° C or any temperature between these values. It is understood that inside the reaction chamber, a temperature profile is established during the reaction. Thus, the temperature is not necessarily the same at one point relative to another point inside the reaction chamber. In other words, there are warmer and cooler places inside the reaction chamber. When we talk about the temperature reached in the reaction chamber, we are therefore talking about a representative average temperature.
• the temperature can vary depending on the pressure in the reaction chamber during the syngas production reaction.
• the pressure to carry out the syngas production reaction can be at least 0.5 atm.
• the production of syngas can be carried out at a pressure of not more than 3 atm.
• the pressure can therefore be 0.5 atm, 1 atm, 1.5 atm, 2 atm, 2.5 atm or 3 atm, or even any pressure between these values.
• the pressure can be between 1 atm and 3 atm.
• the O 2 feed rate can be adjusted so as to obtain a desired level of temperature and heat inside the reactor to operate the RWGS reaction.
• the flow rate of H2 can be adjusted so as to obtain the H2 / CO ratio or the R2 ratio defined by equation (E) that it is desired to have for the gas mixture (12) discharged by the opening (13).
• This realization is suitable for the production of syngas from any possible carbon source.
• a stream comprising a carbon source (2) is mixed with a stream of hydrogen (5a) to form a reducing stream (5b) which is then sent to the reactor.
• the carbon source comprises CO2 which is an oxidant
• the mixture (5b) formed by mixing the gas comprising the CO2 and the hydrogen is however a reducing mixture since it consists mainly of hydrogen.
• the carbon source is CO2 and the H2 / CO2 molar ratio in the reducing stream may be at least about 2, and preferably at least 3.
• the stream reducing agent (5b) becomes the reducing flux (8a, 8b).
• An oxidizing stream comprising GO2 (1) is fed into the reactor by means of the tube (4) to form the oxidizing stream (6).
• a first part (8a) of the reducing flux reacts with the oxidizing flux (6) to produce the Oxy-flame (9).
• the second part (8b) of the hydrogen stream which also contains the carbon source reacts using heat from the Oxy-flame (9).
• the gas mixture (12) which is formed at the outlet of the reactor consists of hydrogen, carbon monoxide, carbon dioxide and water vapor. This gas stream, or wet syngas, is discharged through the opening (13) of the reactor.
• the carbon source forming the stream (2) can essentially comprise CO2 and the reaction which takes place in the reaction chamber is the RWGS reaction (A).
• the carbon source forming the current (2) can comprise organic molecules of chemical formula CaHpOy where a can vary between 1 and 5, b can vary between 2 and 10 and g can vary between 1 and 4.
• D 'other types of organic molecules can also form the stream (2), such as hydrocarbons such as alkanes (eg, methane), alkenes, aromatics. These organic molecules can optionally be mixed with CO2 in the stream (2).
• the carbon source includes organic molecules of the CaHpOy type
• the following reactions can occur in the reaction chamber:
• stream (2) can comprise a mixture of CO2 and organic molecules of formula CaHpO Y.
• both reactions (A) and (M) can occur in the reaction chamber to form the syngas.
• the carbon source includes a hydrocarbon
• production of syngas can take place in the reaction chamber in the presence of an oxidant to allow oxidation of the hydrocarbon.
• an oxidant can include water vapor and / or CO2.
• the water vapor can be generated by the combustion reaction (F) of Fh during the formation of the Oxy-flame and / or can be fed independently into the reaction chamber.
• the carbon source includes methane as a hydrocarbon
• the following reactions can occur in the reaction chamber, depending on the oxidant involved (water vapor, CO2):
• the carbon source comprises a hydrocarbon of the formula C n H m , the following reaction can occur in the reaction chamber:
• the present method of producing syngas offers the possibility of using various carbon sources.
• the carbon source can be a gas mixture produced by industrial processes such as biomass gasification or pyrolysis processes.
• FIG. 5 shows another embodiment of the method for producing syngas and of a reactor which can be used, among others, for this embodiment.
• that of FIG. 5 is suitable for the production of syngas from any possible carbon source (eg, CO2, molecules of formula CaHpO Y , hydrocarbons or their mixtures).
• the Oxy-flame (9) can be produced by injecting oxygen and hydrogen by means of two separate concentric tubes (4a and 4b), as will be explained in more detail below. below.
• the reactor comprises in its lower part a central tube (4a) which fits into a second tube of larger diameter (4b).
• the central tube (4a) can be attached to the larger tube (4b) by means of a fixing device (15b) such as a sealing device.
• the second, wider tube (4b) can itself be attached to the wall (14) of the reactor by means of a fastening device (15a) which is preferably similar to the fastening device (15b).
• the interior of the reactor is divided into two compartments (10a and 10b).
• the two compartments (10a, 10b) are separated by a wall (16) provided with an opening (7b).
• the first compartment (10a) constitutes the reaction chamber of the reactor.
• an oxidizing stream (1) based on oxygen is injected into the central tube (4a), while a stream comprising hydrogen (5) is injected into the second tube. (4b).
• the hydrogen stream (5) passes through an opening defined by the annular space (7a) between the inner wall of the middle tube (4b) and the outer wall of the central tube (4a).
• a stream (2) comprising a carbon source is injected inside the compartment (10b) which can be termed a distribution chamber, and then passes through the opening (7b) to enter the reaction chamber ( 10a).
• the stream of O2 (1) becomes an oxidizing stream (6)
• the stream of H2 (5) becomes a stream of hydrogen (8c)
• the stream (2) comprising the carbon source ends up in a third stream (8d).
• the oxygen flow (6) and part of the hydrogen flow (8c) are used for the production of the Oxy-flame (9), while the excess hydrogen, ie which is not burned, comes reacting with the flow comprising the carbon source (8d).
• the excess hydrogen ie which is not burned, comes reacting with the flow comprising the carbon source (8d).
• the stream comprising the carbon source (2) can be CO2.
• the stream (2) can also include other compounds such as organic molecules and / or hydrocarbons as described above while being free of CO2.
• the stream (2) can also include hydrogen.
• a certain quantity of hydrogen can be fed into the middle tube (4b) to serve to form the hydrogen stream (8c) while another part of hydrogen can be mixed with CO2 and / or vapors. organic and / or hydrocarbon to form the flow (8d).
• FIGS. 6a and 6b show an embodiment of the syngas production method using a high capacity reactor.
• the reactor can comprise a wall (14) and an insulating and refractory material (11) to protect the reaction chamber (10a).
• a distribution chamber (10b) is arranged in the lower part of the reactor in communication with the reaction chamber (10a).
• the distribution chamber receives the reducing stream (5) comprising hydrogen before it enters the reaction chamber.
• the reaction chamber (10a) is separated from the reducing current distribution chamber (10b) by a wall.
• the wall can be made of refractory material with insulation and be supported by a plate (16).
• the plate (16) can for example be a metal plate.
• the compartment (10b) can be crossed by a multitude of concentric tubes (4) which can be fixed to the wall (14) of the reactor in the lower part of the compartment (10b).
• the tubes (4) can be fixed to the wall (14) by means of a sealing device (15).
• the fixing and sealing devices (15) can also serve as guides to maintain the position of the tubes (4).
• the concentric tubes (4) extend through the distribution chamber (10b) to the lower part of the reaction chamber (10a) to form a multitude of inlet ports (7b) through which the oxidizing current (3 ) is injected into the reaction chamber.
• the wall between the distribution chamber and the reaction chamber is provided with openings forming a multitude of inlet ports (7a) of radius n through which the reducing current (5) can penetrate inside the chamber. reaction chamber.
• the openings (7a) form a ring around the tubes (4) as can be seen in Figure 6b.
• the entry ports (7b) of radius G2 can be concentric with respect to the entry ports (7a).
• the reducing current (5) can be injected into the distribution chamber (10b) through more than one input port.
• the reactor can be provided with at least 4 inlet ports for the reducing current (5).
• the reactor can include a multitude of tubes (4) for injecting the oxidizing current (3) into the reaction chamber (10a).
• the reactor according to this embodiment also comprises an outlet (13) to allow the evacuation of the syngas produced in the reaction chamber.
• Oxy-flames can form in the reaction chamber.
• the distance d may preferably be between 0.1 mm and 100 mm. According to another embodiment, the distance d separating the two flows may be between 0.3 mm and 50 mm, or even preferably between 0.6 mm and 30 mm. The distance d can also be any distance within these ranges of values.
• the hydrogen which is needed in the reducing stream and which is used to obtain the syngas can be produced from renewable resources.
• hydrogen can be produced from a water electrolysis system powered by electricity from renewable sources.
• the stream comprising the carbon source (e.g. CO2) which is also needed as a reagent, can itself be a gas mixture resulting from biomass gasification or pyrolysis techniques, as mentioned above.
• Figure 7 also shows additional steps, comprising for example the recovery of water formed during the reaction of production of gas. synthesis.
• Figure 7 shows the following steps: • electrolysis (20) of the water supplied (FteO-a) by electricity from renewable sources (E);
• the electrolysis system (20) is fed with water (FteO-a) to produce hydrogen (Fte) and oxygen.
• the hydrogen (H2) produced by electrolysis is mixed with a gas comprising CO2 and / or another carbon source, preferably CO2.
• This gas comprising CO2 and / or another carbon source can come, at least in part, from a process of gasification or pyrolysis of biomass.
• the resulting mixture (G0) forms a reducing stream which can then be used for the production of syngas (30).
• Some of the oxygen (O2-a) produced by electrolysis (20) is sent to the production of syngas (30), where it can be used to generate Oxy-flame.
• the other part of the oxygen ( ⁇ 2-b) produced by electrolysis (20) can be removed.
• the gas (G1) resulting from the production of syngas (30) is then cooled (40) rapidly in order to limit / prevent the reverse reaction of reaction (A) from occurring. Cooling can be carried out using a conventional method. According to a preferred embodiment, the cooling (40) can be carried out by means of a cooler in direct contact with a stream of water (H2O- b). According to one embodiment, the gas (G1) is cooled to a temperature above the dew point of the hot gas and not exceeding 250 ° C. According to some embodiments, the dew point of the hot gas (G1) is less than 90 ° C at atmospheric pressure. For example, the dew point of hot gas (G1) is included between 60 ° C and 90 ° C at atmospheric pressure. According to some embodiments, the gas (G1) can be cooled to a temperature between 90 ° C and 250 ° C.
• the cooled gas (G2) obtained after the cooling (40) is a wet gas.
• This gas (G2) can then undergo a second cooling which can be carried out by condensation (50).
• this condensation can be carried out using a cooler-condenser.
• the condensation step (50) can be carried out such that the gas (G2) is cooled to a temperature of 35 ° C and below.
• Part of the condensed water (hteO-c) can be recycled (flow hteO-b) to the cooling stage (40) while the other part of the condensed water can be discharged (flow hhO-d) .
• the hteO-d flow can be used, at least in part, to supply water to the electrolysis system (20).
• the syngas production method described in this document can make it possible to produce gas mixtures based on CO and hte (syngas) which are balanced, ie, with appropriate proportions of CO and hte, to then allow the production of a variety of products by conventional chemical syntheses.
• CO and hte syngas
• It is also possible to play on the proportion of CO and hte in the syngas by controlling the temperature, the pressure and the O2 feed rate in the reaction chamber.
• the temperature in the reactor can be controlled by the flow of oxygen supplied.
• the syngas produced contains host and CO in a molar ratio H2 / CO> 2.
• the syngas produced by the method described can also contain CO2.
• the molar ratios of H2, CO and CO2 in the syngas can be such that (H2-CO2) / (CO + CO2)> 2.
• the syngas produced by the present method can be used to produce a large number of basic chemicals. These products include methanol and hydrocarbons such as those found in motor gasoline, diesel, kerosene, to name a few examples.
• the syngas production method described above and the reactor that can be used to achieve this method therefore have several advantages.
• the reagents are easily accessible and can be derived from renewable sources. It is not necessary to resort to the use of solid catalysts.
• the rate of conversion of the reactants may also be greater than the rate of conversion observed in the case of a RWGS reaction carried out in a conventional manner in the presence of a catalyst.
• the present method is characterized by its robustness, in that it is versatile and simple to implement.
• This example is based on a small reactor as shown schematically in Figure 8.
• This mini-reactor operates according to a scenario involving the co-injection of pre-mixed O2 and CO2, inside the inner tube, ie, in space A, and injection of H2 into annular space B.
• the reactor was built from small tubes in Inconel 600 TM.
• thermocouples An ignition system used to ignite a pulsoreactor, ie, a 20 kV spark plug with ignition, was inserted inside the reactor, very close to the upper end of the inner and middle tubes. . A perforation was made to allow the spark plug to be inserted (not shown in the figure for clarity).
• the change in the temperature level in the reactor is monitored using thermocouples. The temperature is measured in a lower part and also in an upper part of the reaction zone inside the mini-reactor. That is, one temperature reading near the base of the reaction zone (where gases are injected) specifically 13 mm higher than the line at the start of the reaction zone (see Figure 8) and another reading at 89 mm higher than the line at the start of the reaction zone (see figure 8), are carried out.
• the thermocouples were installed by means of T-fittings (not shown in the figure).
• the experimental set-up includes the following: the reactor itself, a tube and jacket heat exchanger allowing rapid cooling of the gases leaving the reactor, a condensate recovery tank, a relative humidity (RH) analysis system gases, and finally, an analysis system (C02 / C0 / CxH y / 02) making it possible to measure the contents of CO, CO2, hydrocarbons (CxH y ) as well as the oxygen content of the gas produced, at the outlet of the gas cooling system.
• RH relative humidity
• a system of mass flow meters with automated control valves is also implemented.
• the system is accompanied by software for programming changes in the composition of the gas mixture introduced into the reactor.
• manual valves are used to direct each of the gases into the desired reactor tube.
• ignition is carried out in stages (lasting approximately 1 second).
• the main stages of the sequence ignition include: 1) start the injection immediately, 2) after a few seconds, inject the oxygen in successive stages until the desired flow rate, each stage lasting a few seconds, 3) start the injection of CO2.
• the input flow rates (standard liters (SL) at 25 ° C, 1 atm per min) are as follows:
• the CO2 and O2 flows are premixed.
• the operating pressure is almost 1 atm.
• the concentration of H2 is calculated from an atomic balance.
• the atomic balance is itself carried out taking into account all the inputs (CO2, H2, O2) and taking into account the composition of the outgoing gas (CO and CO2 content, hydrocarbon content expressed in CH4 equivalent, gas humidity, residual oxygen content).
• CO2 content hydrocarbon content expressed in CH4 equivalent, gas humidity, residual oxygen content.
• the atomic balance on the hydrogen atoms makes it possible to calculate the hydrogen composition of the gas at the outlet of the reactor.
• the same device as for example 1 is used, but with injection of O2 into the inner tube (space A), injection of H2 into the annular space between the middle tube and the inner tube (space B) , and injection of a CO2 / CH4 equimolar mixture into the annular space between the outer tube and the middle tube (space C).
• the input flow rates (standard liters at 25 ° C, 1 atm per min) are as follows:
• Example 2 the same reactor as that of Example 1 is used, but the outer Inconel TM tube is replaced by a quartz tube.
• the length of the reaction chamber is the same.
• the CO2 and O2 flow rates are premixed.
• the resulting mixture is injected inside the inner tube (space A), while hydrogen is injected inside space B.
• the operating pressure is nearly 1 atm. Since the temperature cannot be measured directly, the temperature used is a thermodynamic equilibrium temperature value calculated to obtain a gas with the same CO / CO2 ratio as what has been measured.
• the input flow rates (standard liters at 25 ° C, 1 atm per min) are as follows:
• This example uses the same equipment as Example 3, i.e., based on using a quartz tube as the outer tube.
• O2 is injected into space A
• H2 is injected into space B
• CO2 is injected into space C. Since the temperature cannot be measured directly, the temperature used is a calculated thermodynamic equilibrium temperature value. to obtain a gas having the same CO / CO2 ratio as what has been measured.
• the input flow rates (standard liters (SL) at 25 ° C, 1 atm) per min) are as follows:
• R2 (H2-CO2) / (CO + CO2): 2.26
• concentration of H2 in the gas leaving the reactor is calculated from an atomic balance.
• CO2 is a very chemically stable molecule, and much more stable than a CaHpO Y molecule where a is between 1 and 5. Since the above examples have shown that the process is applicable for CO2 which turns out to be more difficult in chemically transforming a molecule of the CaHpO Y type, it is reasonable to conclude that the method is also applicable to molecules of the CaHpO Y type as a carbon source.

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