WO2011021944A1 - Procédés combinés permettant d'utiliser un gaz de synthèse à faible émission de co2 et à rendement énergétique élevé - Google Patents

Procédés combinés permettant d'utiliser un gaz de synthèse à faible émission de co2 et à rendement énergétique élevé Download PDF

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WO2011021944A1
WO2011021944A1 PCT/NO2010/000310 NO2010000310W WO2011021944A1 WO 2011021944 A1 WO2011021944 A1 WO 2011021944A1 NO 2010000310 W NO2010000310 W NO 2010000310W WO 2011021944 A1 WO2011021944 A1 WO 2011021944A1
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process according
energy
gasification
gas
synthesis gas
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PCT/NO2010/000310
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Erik Fareid
Lars Erik Fareid
Skule Pedersen
Tommy Schierning
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Eicproc As
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • 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
    • C01B3/12—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 by reaction of water vapour with carbon monoxide
    • C01B3/16—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 by reaction of water vapour with carbon monoxide using catalysts
    • C—CHEMISTRY; METALLURGY
    • C07—ORGANIC CHEMISTRY
    • C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
    • C07C29/00—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring
    • C07C29/15—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively
    • C07C29/151—Preparation of compounds having hydroxy or O-metal groups bound to a carbon atom not belonging to a six-membered aromatic ring by reduction of oxides of carbon exclusively with hydrogen or hydrogen-containing gases
    • C07C29/1516—Multisteps
    • C07C29/1518—Multisteps one step being the formation of initial mixture of carbon oxides and hydrogen for synthesis
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • 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
    • C10G2/32—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts
    • C10G2/33—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon from carbon monoxide with hydrogen with the use of catalysts characterised by the catalyst used
    • 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
    • C10J3/466—Entrained flow processes
    • C—CHEMISTRY; METALLURGY
    • 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
    • C10K3/04—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 reducing the carbon monoxide content, e.g. water-gas shift [WGS]
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10L—FUELS NOT OTHERWISE PROVIDED FOR; NATURAL GAS; SYNTHETIC NATURAL GAS OBTAINED BY PROCESSES NOT COVERED BY SUBCLASSES C10G, C10K; LIQUEFIED PETROLEUM GAS; ADDING MATERIALS TO FUELS OR FIRES TO REDUCE SMOKE OR UNDESIRABLE DEPOSITS OR TO FACILITATE SOOT REMOVAL; FIRELIGHTERS
    • C10L3/00—Gaseous fuels; Natural gas; Synthetic natural gas obtained by processes not covered by subclass C10G, C10K; Liquefied petroleum gas
    • C10L3/06—Natural gas; Synthetic natural gas obtained by processes not covered by C10G, C10K3/02 or C10K3/04
    • C10L3/08—Production of synthetic natural gas
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    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • 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
    • C01B2203/0288—Processes for making hydrogen or synthesis gas containing a CO-shift step, i.e. a water gas shift step containing two CO-shift steps
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/061—Methanol production
    • C—CHEMISTRY; METALLURGY
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/062—Hydrocarbon production, e.g. Fischer-Tropsch process
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    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/068—Ammonia synthesis
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1041—Composition of the catalyst
    • C01B2203/1076—Copper or zinc-based catalysts
    • 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
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/0916—Biomass
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
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    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0913—Carbonaceous raw material
    • C10J2300/095—Exhaust gas from an external process for purification
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    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
    • C10J2300/0953—Gasifying agents
    • C10J2300/0956—Air or oxygen enriched air
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    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
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    • C10J2300/00—Details of gasification processes
    • C10J2300/09—Details of the feed, e.g. feeding of spent catalyst, inert gas or halogens
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    • C10J2300/0973—Water
    • 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
    • C10J2300/1246—Heating the gasifier by external or indirect heating
    • 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
    • C10J2300/1253—Heating the gasifier by injecting hot gas
    • 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
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1659—Conversion of synthesis gas to chemicals to liquid hydrocarbons
    • 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
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1662—Conversion of synthesis gas to chemicals to methane (SNG)
    • 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
    • C10J2300/16—Integration of gasification processes with another plant or parts within the plant
    • C10J2300/164—Integration of gasification processes with another plant or parts within the plant with conversion of synthesis gas
    • C10J2300/1656—Conversion of synthesis gas to chemicals
    • C10J2300/1665—Conversion of synthesis gas to chemicals to alcohols, e.g. methanol or ethanol
    • 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
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/10—Biofuels, e.g. bio-diesel
    • 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
    • Y02E50/00—Technologies for the production of fuel of non-fossil origin
    • Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
    • 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
    • Y02P20/145—Feedstock the feedstock being materials of biological origin

Definitions

  • One of the items of the present invention is to present a chemical process for providing energy in the form of electrical energy or synthesized products which may be combusted releasing usable chemical energy.
  • the process according to the present invention combines combustion gas (CO + CO 2 ) with hydrogen (preferably originating from water) for producing organic molecules (e.g. methane) and energy.
  • the process according to the present invention combines the processes of (1) power production from any combustion of organic fuels, (2) the process of gasification and or pyrolysis and (3) any process of utilizing synthesis gas, such as methanation, methanol production, ammonia production, urea production, Fischer-Tropsch synthesis and any other utilization of the above in the production of energy and energy-harboring compounds.
  • the term "neutral" concerning emitted CO 2 means that the carbon involved neither increases nor reduces the total carbon emission to the atmosphere.
  • biofuels where plants assimilate the same amount of carbon from the atmosphere (in the form of CO 2 ) storing it in the form of e.g. cellulose and sugars, as the amount emitted to the atmosphere when combusting these materials, making the total carbon balance to the atmosphere zero.
  • PCT/NO2007/000387 may be summarized as a catalytic gas reactor including a catalyzer or process creating hydrogen and oxygen by splitting of water and a process with catalyzer creating methane from reactions wherein CO, CO 2 and hydrogen participate.
  • Seng Sing Tan, Linda Zou and Eric Hu "Photosynthesis of hydrogen and methane as key components for clean energy system” Science and Technology of Advanced Materials, Volume 8, no. 1-2, January-March 2007, page 89-92, APNF International Symposium on Nanotechnology in Environmental Protection and Pollution
  • the present invention combines the processes of (1) power production from any combustion of organic fuels, with (2) the process of gasification and or pyrolysis with (3) any process of utilizing synthesis gas, such as methanation, methanol production, ammonia production, urea production, Fischer-Tropsch synthesis and any other utilization of the above in energy production.
  • synthesis gas such as methanation, methanol production, ammonia production, urea production, Fischer-Tropsch synthesis and any other utilization of the above in energy production.
  • the excess heat from the exhaust gas from the power production together with any heat from the synthesis gas utilization will supply all or parts of the heat necessary to gasify the organic substances to synthesis gas. Though this process it is possible to gasify organic/Bio waste as the CO 2 from these wastes are neutral.
  • reaction loop By combining said chemical reactions it is possible to create a "reaction loop" wherein the recapture of the reaction energy provides usable energy in the form of electrical or chemical energy in the form of a gas that may be combusted directly or that harbours large amounts of potential chemical energy.
  • organic fuels is to mean materials comprising any number carbon atoms and hydrogen atoms in their structure that may be converted to or processed to a fluid or gaseous form or which may remain in a solid form, and which in their solid, fluid or gaseous form may be combusted with oxygen to form karbonmonoxide and/or carbondioxide and/or methane (see the reaction equations infra).
  • organic fuel is to include any carbonaceous material that may react through combustion for producing energy.
  • combustion is to mean any reaction involving a reaction between oxygen and a carbonaceous material within the temperature intervals indicated infra.
  • gasification is to mean the evaporation and/or combustion of organic fuel.
  • chemical energy refers to the latent or potential energy of a compound that may be released through a chemical process that lowers the potential energy of the relevant compound forming one or more reaction products with a lower net potential energy and releasing the energy difference between the original compound(s) and the product(s).
  • electrical energy refers to energy that may be utilized by an electrical storage unit (battery, condenser, etc.) or be converted to other forms of energy, e.g. mechanical energy, through the use of an electrical appliance.
  • the term "large amounts of energy” refers to energy within the range 10-50 MJ/kg
  • the term "about” refers to a relative deviation from the indicated amount of up to + 10%, i.e. an interval of one unit per ten units of the relevant number.
  • the deviation may also be smaller, e.g. 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8% or 9% or any number in between or any interval combination thereof.
  • One of the possibilities realized by the present invention is through energy recapture to provide usable energy as well as providing a gas that may be combusted or that contains large amounts of chemical energy.
  • the waste from power production based on combustion of organic fuels may have a temperature in the range of 100-2000°C.
  • Examples of possible temperature intervals in such a combustion are 200-1800°C, 30O-150O°C, 400-1300 0 C, 500-1250 0 C, 550- 1200 0 C, 600-1100 0 C, 700-1000 0 C or any combination of said intervals.
  • step (2) of the present invention there may be used gasifiers for providing gas from the organic combustion material.
  • gasifiers examples include: counter- current fixed bed gasifisers; co-current fixed bed gasifisers, fluidized bed gasifiers and entrained flow gasifers.
  • the counter-current fixed bed (“up draft") gasifier includes a fixed bed of carbonaceous fuel (e.g. coal or biomass) through which the "gasification agent” (steam, oxygen and/or air) flows in counter-current configuration.
  • the co-current fixed bed (“down draft”) gasifier is similar to the counter-current type, but the gasification agent gas flows in co-current configuration with the fuel (downwards, hence the name “down draft gasifier”).
  • the fuel In the fluidized bed reactor, the fuel is fluidized in oxygen and steam or air.
  • the ash is removed dry or as heavy agglomerates that defluidize.
  • the temperatures are relatively low in dry ash gasifiers, so the fuel must be highly reactive; low-grade coals are particularly suitable.
  • the agglomerating gasifiers have slightly higher temperatures, and are suitable for higher rank coals. Fuel throughput is higher than for the fixed bed, but not as high as for the entrained flow gasifier.
  • Gasifiers used in the present invention gasify organic waste into gaseous organic material to be further combusted into CO and/or CO 2 included in the combined process according to the present invention.
  • Gasification of organic material in the process according to the present invention is preferably performed at low amounts of O 2 present, i.e. at O 2 concentrations of the inlet gas in the range of 0,5-15% O 2 (v/v).
  • the gasification of the organic material in the gasifiers is conveniently done in a temperature interval of 500-2000 0 C, preferably within the temperature interval 800-1200°C, e.g. within the temperature intervals 500-800°C, 700-1000°C, 900-1 100°C, 850-1150°C, 1000-1200°C or 1 100-1200°C.
  • a methanation reaction is one of the reactions for utilizing the synthesis gas.
  • the methanation reaction may be performed with the catalysts infra with different compositions depending on the condition of the gas that is to be treated, but all methanation catalysts may be used in the temperature interval 150 to 600 0 C;
  • step (3) of the process according to the present invention another of the possible reactions is methanol production.
  • Most synthesis gas for methanol production is produced by team reforming of natural gas.
  • the ideal synthesis gas composition for this application in the process according to the present invention has a H 2 /CO ratio of about 2.
  • a small amount of CO 2 (about 5%) increases the catalyst activity using a catalyst comprising the elements Cu/ZnO/Al 2 O 3 .
  • step (3) of the process according to the present invention another of the possible ways to convert synthesis gas to a wide range of hydrocarbons and/or alcohols is through the Fisher-Tropsch (F-T) process.
  • F-T Fisher-Tropsch
  • the F-T process was discovered in 1923 but it is in the recent years that it has been perceived as a possible way to convert natural gas into liquid fuels.
  • the chemistry behind the F-T process is rather complex, the fundamental aspects can be represented by he major overall reactions in the Fischer-Tropsch synthesis:
  • nCO + (2n + 1 ) H 2 C n H 2n+2 + nH 2 0
  • nCO + 2nH 2 H(-CH 2 -) n OH + (n- 1 )H 2 O
  • a characteristic of the F-T reactions is their high exothermicity. For example, the formation of 1 mol of -CH 2 - is accompanied by a heat release of 165 kJ/mol. From the overall reactions it can be seen that both hydrocarbons and alcohols can be formed. Therefore, the choice of catalyst and process conditions is very important.
  • the hydrocarbons are formed by a chain-growth process, with the length of the chain being determined by the catalyst selectivity and the reaction conditions. Selecting such conditions lies, however, within the competence of the person skilled in the art or requires no unreasonable amount of experimentation to determine.
  • Suitable catalysts for performing the F-T reaction include e.g. a mixture of Co and Ni or pure Co or pure Ni optionally including support materials like carbon nanofibers or carbon nanotubes or Al 2 O 3 or TiO 2 .
  • CO 2 is transformed to methane through the aid of hydrogen and may consequently be used again as a fuel or as a raw material for a number of other processes.
  • Some of these processes may be the production of methane, methanol, ammonia, urea, nitric acid, ammonium nitrate, NPK, PVC, etc.
  • the present invention may be used in all forms of gases wherein fossil or biological fuel is used.
  • the present invention solves the problem with emission of VOC (volatile organic compounds), NOx (nitrogen oxides), N 2 O (laughing gas), NH 3 (ammonia) and other greenhouse and in other ways polluting gases.
  • NOx-gases e.g. from combusted proteins
  • SNCR selective non-catalytic reduction
  • SCR selective catalytic reduction
  • other NOx-reducing processes according to procedures known to the skilled artisan.
  • the present invention produces also energy far more effectively than similar processes today, and has far lower CO 2 emission per kWh than contemporary processes with CO 2 harvesting.
  • Table 1 infra is presented as an comparative example presenting parameters and cost-effectiveness of the process according to the present invention.
  • Table 1 Comparison between the present invention and a similar power plant (LM Ericsson 2500 gas turbine) with and without CO 2 collection. All numbers* are relative to today's without CO 2 collection:
  • the present invention may be used within the general area OfCO 2 purification, collection and sequestering.
  • the present reactions are also disclosed as the application of specific reactor designs providing catalytic and physical characteristics allowing and emphasizing the hydrogenation of CO and CO 2 to CH 4 (methane).
  • the present invention may be considered as a triple one, the one part producing hydrogen and CO according to reaction 5.
  • the second part will take advantage of the produced hydrogen from the first part, but may also individually produce hydrogen from reaction 1.
  • the produced hydrogen will in the third part react with CO and CO 2 according to reaction 2 and 3 and produce methane.
  • the produced methane may either be re-circulated and combusted in a continuous loop or the methane may be separated out and be used as a raw material for producing other chemicals.
  • the produced hydrogen and CO may be used as raw materials for other uses and processes.
  • Part 1 of the present invention may contain combustion and/or oxidation processes where fossil or organic substances are used as fuel.
  • Part 2 of the present invention may contain catalysts and other devices making it possible to produce synthesis gas.
  • Synthesis gas contains hydrogen and carbon monoxide, however synthesis gas may also contain carbon doxide, water, nitrogen and methane.
  • Part 3 of the present invention is to contain a catalyst being suited for performing the methanation reaction, reactions 2 and 3, and suppressing the reverse shift reaction, reaction 4.
  • Part 1 , part 2 and part 3 may be integrated with each other or may be separate entities.
  • Part 1 is the section where the organic or fossil fuel is combusted and/or oxidized and is described by the well known reaction 6.
  • Part 2 is the section wherein the gasification is performed. Gasification is an energy demanding process. This energy may be taken from Part 3 developing large amounts of energy or the energy may be provided from external sources, or part 1.
  • the organic substances may be split into hydrogen and CO according to reaction 5 through several different processes. As mentioned supra, some of these may be:
  • the counter-current fixed bed (“up draft”) gasifier consists of a fixed bed of carbonaceous fuel (e.g. coal or biomass) through which the "gasification agent” (steam, oxygen and/or air) flows in counter-current configuration.
  • carbonaceous fuel e.g. coal or biomass
  • the "gasification agent” steam, oxygen and/or air
  • the co-current fixed bed (“down draft”) gasifier is similar to the counter-current type, but the gasification agent gas flows in co-current configuration with the fuel (downwards, hence the name “down draft gasifier”).
  • the fuel In the fluidized bed reactor, the fuel is fluidized in oxygen and steam or air.
  • the ash is removed dry or as heavy agglomerates that defluidize.
  • the temperatures are relatively low in dry ash gasifiers, so the fuel must be highly reactive; low-grade coals are particularly suitable.
  • the agglomerating gasifiers have slightly higher temperatures, and are suitable for higher rank coals.
  • Fuel throughput is higher than for the fixed bed, but not as high as for the entrained flow gasifier.
  • a dry pulverized solid an atomized liquid fuel or a fuel slurry is gasified with oxygen (much less frequent: air) in co-current flow. The gasification reactions take place in a dense cloud of very fine particles.
  • Most coals are suitable for this type of gasifier because of the high operating temperatures and because the coal particles are well separated from one another.
  • Part 3 the transforming of CO 2 with hydrogen to methane is performed in a reactor with a catalyst.
  • the heat being developed may be used for heating Part 2 or in any other way.
  • the shape of the catalyst is not essential and may inter alia comprise coated monoliths, different nano materials and other types and forms of carriers.
  • the carriers may be selected from e.g. TiO 2 , Al 2 O 3 , cordierite, Gd-doped CeO and other types of carrier materials.
  • the catalytic material may also be present in any form as a "pure" catalyst material. The form and composition of the reactor and the catalyst will depend on which emission gas it is wanted to purify.
  • An impure exhaust gas with large amounts of dust may have a monolithic catalyst carrier whereas a pure exhaust gas (from a natural gas turbine) may have a catalyst in the form of pellets. All types of exhaust gases from all types of combustions of organic material may be treated.
  • the methanation reaction may be performed with the catalyzers infra with different compositions depending on the condition of the gas that is to be treated, but all methanation catalyst may be used in the temperature interval 150 to 600 0 C.
  • examples of usable catalysts are:
  • a methanation reaction is selected in the combined process according to the present invention, such a methantion reaction is conducted according to standard procedus, taking into account e.g. the efficiency and optimal operating conditions of the catalysts used, but the methanation reaction is normally conducted at temperatures indicated supra and at pressures in the range of about. 1 to 50 bar.
  • the CO having been produced at the gasification may be used as a source for other applications e.g. for producing energy or as a starting material for the production of more hydrogen.
  • Another possibility for using of the formed synthesis gas may be to produce methanol as disclosed supra. This production may conceivably happen according to commercial processes being available today, and the methanol may have several areas of use such as e.g. fuel for transportation vehicles.
  • This process may be realized in the following way: Fuel is combusted with air in a burner. Electricity, being another form of energy, is taken out from the combustion process in a conventional manner. The CO 2 produced is used, as disclosed in the present invention, for producing methane. The methane is recirculated while the hydrogen and CO produced by the gasification is used for producing methanol.
  • the present invention is not limited to these two fields, but may be used in all processes wherein natural gas or other hydrocarbons and organic compounds are one of the raw materials.
  • the present invention also produces energy far more efficiently than comparable processes today, and has a far lower CO 2 emission per kWh than today's processes with capture of CO 2 .
  • the other advantages of the present process as compare to others are observed in the table infra (being equal to table 1 supra, but emphasizing other aspects of the present invention).
  • Table 1 Comparison between the present invention and comparable power plants with and without capture of CO 2 . All numbers a relative to today's without capture of CO 2 :
  • This exhaust gas consists mainly of CO 2 and water.
  • This composition makes it very simple to capture CO 2 without using chemicals (e.g. amines and others), since the water may be condensed out while the CO 2 still is in a gaseous state. CO 2 may then be used for other purposes or may be stored. The cost for capture and optionally storage of such CO 2 then becomes very small.
  • the CO 2 may be captured and used or stored in any possible way described.
  • the disclosed reactions are common reactions (equilibrium reactions) happening in the production of ammonia over different catalytic layers and in the gasification of the organic compounds.
  • the shift reaction happens in the LT (low temperature being known to the person skilled in the art) or HT (high temperature being known to the person skilled in the art) shift reactors wherein carbon monoxide reacts to produce carbon dioxide and hydrogen over an iron oxide/chromium oxide respectively a copper oxide/zinc oxide catalyst may be used.
  • the methanation reaction happens in a methane reactor (operating under the conditions temperature up to 600 °C, pressure 1 to 50 bar, space velocity 10 000 h '1 ) wherein carbon monoxide and carbon dioxide is reacted into methane and water over a nickel, ruthenium, tungsten or other metal-containing catalyst according to several total reactions (equilibrium reactions), inter alia:
  • ammonia process is a process for producing ammonia via hydrogen from methane and nitrogen from air
  • the reactions 2. and 3. disclosed supra are reactions that are not wanted and which give losses of in the production of ammonia. In the present invention all of these reactions are wanted since they produce methane being a product or intermediates participating in producing methane.
  • the waste gases may contain different types of contaminants. These contaminants may be, but are not limited to N 2 O, NO, NO 2 , volatile compounds (VOCs), SO 2 , etc.
  • FIG. 1 Gasification of biomass with flue gas.
  • FIG. 1 Biomass heat exchanged with flue gas.
  • Figure 1 Gasification of biomass with flue gas.
  • the figure shows air and fossil fuel (e.g. methane) being fed to a combustion unit (2).
  • the flue gas from the combustion is mixed with biomass and fed to the gasification reactor (4).
  • the biomass together with the oxygen and water in the flue gas is converted to synthesis gas.
  • the synthesis gas is heat exchanged (if necessary in 5) and either used as raw material and converted to the synthesis gas conversion (6) unit, or burned to generate energy.
  • FIG. 1 Biomass heat exchanged with flue gas.
  • the figure shows biomass, air and water being heat exchanged (3) with hot flue gas from a combustion unit (1) before entering a gasification reactor (4).
  • the reactants are converted to synthesis gas, and the synthesis gas is heat exchanged (in necessary in 5) and either used as raw material and converted in the synthesis gas conversion unit (6) or burned to generate energy.
  • FIG. 1 Conventional gasification process.
  • the figure shows a conventional gasification process where biomass, air and water is mixed and heated (if necessary in 2) before entering a gasification reactor (3).
  • the synthesis gas is heat exchanged (if necessary in 4) and either used as raw material and converted in the synthesis gas conversion unit (5), or burned to generate energy.
  • Detailed use of the invention are described below.
  • FIG. 1 The figure shows air and fossil fuel (e.g. methane) being fed to a combustion unit (2).
  • the flue gas from the combustion is mixed with biomass and fed to the gasification reactor (4).
  • the biomass together with the oxygen and water in the flue gas is converted to synthesis gas.
  • the synthesis gas is heat exchanged (if necessary in 5) and either used as raw material and converted in the synthesis gas conversion (6) unit, or burned to generate energy.
  • FIG. 2 The figure shows biomass, air and water being heat exchanged (3) with hot flue gas from a combustion unit (1) before entering a gasification reactor (4).
  • the reactants are converted to synthesis gas, and the synthesis gas is heat exchanged (if necessary in 5) and either used as raw material and converted in the synthesis gas conversion unit (6), or burned to generate energy.
  • FIG. 3 The figure shows a conventional gasification process where biomass, air and water is mixed and heated (if necessary in 2) before entering a gasification reactor (3).
  • the synthesis gas is heat exchanged (if necessary in 4) and either used as raw material and converted in the synthesis gas conversion unit (5), or burned to generate energy.
  • CO 2 may be compressed and stored in a suitable way.
  • gasification for H 2 and CO production based on entrained flow gasifier may be used in a combined process with water dissociation and CO 2 methanation. It consists of three chemical steps:
  • the hydrogen recovery step is performed in any type of gasification reactor in the temperature range 300-1200 0 C but according to this example the gasification reactor is an entrained flow gasifier with the following operating conditions: temperature 1600 - 2200 K, atmospheric pressure.
  • the gases that are developed are hydrogen, carbon monoxide and carbon dioxide.
  • the carbon monoxide may be reacted with water to further develop more hydrogen in the water-gas shift reaction.
  • the water-gas shift reaction is carried out using to adiabatic fixed-bed reactors with cooling between the two reactors.
  • the first reactor (High Temperature Shift) operates at high temperature (350 "C) and contains a classical catalyst (iron oxide promoted with chromium oxide).
  • the second reactor contains a more active catalyst (copper on a mixed support of zinc oxide and aluminum oxide) and operates at lower temperature (Low Temperature Shift, 190 - 210 "C).
  • the hydrogen will be used together with the CO 2 -containing exhaust gas and reacted over a methanation catalyst being specifically in the present example Nickel on aluminum oxide support for providing methane and water.
  • the parameters under which this methanation catalyst operates are: Temperature: 350 0 C and atmospheric pressure.
  • the electrical efficiency for the whole set up may be as high as 70%
  • Example 2 of gasification combined with methanation Large amounts of hydrogen and CO may be produced at moderate temperatures (300- 1200 0 C).
  • the Hydrogen and CO may be used as described in example 1 or the gas mixture can be used to produce other chemicals like, but not limited to, methanol ethanol and diesel fuels.
  • the excess of heat from the Sabatier reaction (methanation of CO 2 and hydrogen for providing methane and water) will be used either to heat the gasification or for creating any type of energy.
  • the heat from the waste- or flue-gases will also assist in heating the gasification process.

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Abstract

Grâce à la combinaison de l'énergie produite par la combustion dans l'oxygène d'un matériau organique avec la gazéification et la pyrolyse ainsi qu'avec tout autre procédé utilisant un gaz de synthèse (par exemple, méthanation, production de méthanol, production d'ammoniac, production d'urée, synthèse de Fischer-Tropsch, etc.), une énergie utilisable peut être extraite à l'issu du procédé global, par exemple, sous la forme d'énergie électrique ou de produits pouvant être soumis à combustion pour libérer l'énergie contenue dans les composés produits.
PCT/NO2010/000310 2009-08-19 2010-08-19 Procédés combinés permettant d'utiliser un gaz de synthèse à faible émission de co2 et à rendement énergétique élevé WO2011021944A1 (fr)

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CN103252238A (zh) * 2013-05-17 2013-08-21 浙江大学 一种用于合成气选择性合成汽柴油组分的催化剂及其制备方法
WO2015011503A1 (fr) * 2013-07-26 2015-01-29 Advanced Plasma Power Limited Procédé de production d'un substitut du gaz naturel
CN104341322A (zh) * 2013-07-30 2015-02-11 热选择有限公司 由具有任何组成的废弃物,优选家庭废弃物,制备尿素的方法
US9458099B2 (en) 2013-07-25 2016-10-04 Thermoselect Aktiengesellschaft Method of manufacturing urea from refuse, preferably domestic waste, of any composition
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CN109181771A (zh) * 2018-10-09 2019-01-11 新奥科技发展有限公司 一种煤催化气化方法及煤催化气化装置
CN110665507A (zh) * 2019-09-18 2020-01-10 盐城工学院 一种高分散负载型钴基催化剂及其制备方法
CN112774682A (zh) * 2019-11-11 2021-05-11 中国科学院城市环境研究所 一种铝钴复合催化剂及其制备方法与应用

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WO2012130450A1 (fr) * 2011-03-29 2012-10-04 Haldor Topsøe A/S Procédé de purification d'un gaz brut
CN103252238A (zh) * 2013-05-17 2013-08-21 浙江大学 一种用于合成气选择性合成汽柴油组分的催化剂及其制备方法
US9458099B2 (en) 2013-07-25 2016-10-04 Thermoselect Aktiengesellschaft Method of manufacturing urea from refuse, preferably domestic waste, of any composition
WO2015011503A1 (fr) * 2013-07-26 2015-01-29 Advanced Plasma Power Limited Procédé de production d'un substitut du gaz naturel
CN104341322A (zh) * 2013-07-30 2015-02-11 热选择有限公司 由具有任何组成的废弃物,优选家庭废弃物,制备尿素的方法
CN108822877A (zh) * 2018-05-29 2018-11-16 柳州东侯生物能源科技有限公司 城市生活垃圾裂解制备燃气的方法
CN109181771A (zh) * 2018-10-09 2019-01-11 新奥科技发展有限公司 一种煤催化气化方法及煤催化气化装置
CN109181771B (zh) * 2018-10-09 2020-10-23 新奥科技发展有限公司 一种煤催化气化方法及煤催化气化装置
CN110665507A (zh) * 2019-09-18 2020-01-10 盐城工学院 一种高分散负载型钴基催化剂及其制备方法
CN110665507B (zh) * 2019-09-18 2022-06-10 盐城工学院 一种高分散负载型钴基催化剂及其制备方法
CN112774682A (zh) * 2019-11-11 2021-05-11 中国科学院城市环境研究所 一种铝钴复合催化剂及其制备方法与应用
CN112774682B (zh) * 2019-11-11 2023-04-07 中国科学院城市环境研究所 一种铝钴复合催化剂及其制备方法与应用

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