US20070056247A1 - Combustion of gaseous fuel - Google Patents

Combustion of gaseous fuel Download PDF

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Publication number
US20070056247A1
US20070056247A1 US10/557,994 US55799404A US2007056247A1 US 20070056247 A1 US20070056247 A1 US 20070056247A1 US 55799404 A US55799404 A US 55799404A US 2007056247 A1 US2007056247 A1 US 2007056247A1
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channels
metal
particles
ceramic
gas
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US10/557,994
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Michael Joseph Bowe
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CompactGTL PLC
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CompactGTL PLC
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Priority claimed from GB0315180A external-priority patent/GB0315180D0/en
Priority claimed from GB0320513A external-priority patent/GB0320513D0/en
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Assigned to ACCENTUS PLC reassignment ACCENTUS PLC ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: BOWE, MICHAEL JOSEPH
Publication of US20070056247A1 publication Critical patent/US20070056247A1/en
Assigned to COMPACTGTL PLC reassignment COMPACTGTL PLC ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: ACCENTUS PLC
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    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C13/00—Apparatus in which combustion takes place in the presence of catalytic material
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10J—PRODUCTION OF PRODUCER GAS, WATER-GAS, SYNTHESIS GAS FROM SOLID CARBONACEOUS MATERIAL, OR MIXTURES CONTAINING THESE GASES; CARBURETTING AIR OR OTHER GASES
    • C10J3/00—Production of combustible gases containing carbon monoxide from solid carbonaceous fuels
    • C10J3/72—Other features
    • C10J3/86—Other features combined with waste-heat boilers
    • 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
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/002—Removal of contaminants
    • C10K1/003—Removal of contaminants of acid contaminants, e.g. acid gas removal
    • C10K1/004—Sulfur containing contaminants, e.g. hydrogen sulfide
    • 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
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/02—Dust removal
    • C10K1/024—Dust removal by filtration
    • 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
    • C10K1/00—Purifying combustible gases containing carbon monoxide
    • C10K1/02—Dust removal
    • C10K1/026—Dust removal by centrifugal forces
    • 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
    • C10K3/023—Reducing the tar content
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C13/00—Apparatus in which combustion takes place in the presence of catalytic material
    • F23C13/08—Apparatus in which combustion takes place in the presence of catalytic material characterised by the catalytic material
    • 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
    • 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
    • C10J2300/093—Coal
    • 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
    • C10J2300/0953—Gasifying agents
    • C10J2300/0956—Air or oxygen enriched air
    • 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
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1861—Heat exchange between at least two process streams
    • C10J2300/1884—Heat exchange between at least two process streams with one stream being synthesis 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
    • C10J2300/18—Details of the gasification process, e.g. loops, autothermal operation
    • C10J2300/1861—Heat exchange between at least two process streams
    • C10J2300/1892—Heat exchange between at least two process streams with one stream being water/steam
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F23—COMBUSTION APPARATUS; COMBUSTION PROCESSES
    • F23C—METHODS OR APPARATUS FOR COMBUSTION USING FLUID FUEL OR SOLID FUEL SUSPENDED IN  A CARRIER GAS OR AIR 
    • F23C2900/00—Special features of, or arrangements for combustion apparatus using fluid fuels or solid fuels suspended in air; Combustion processes therefor
    • F23C2900/99008—Unmixed combustion, i.e. without direct mixing of oxygen gas and fuel, but using the oxygen from a metal oxide, e.g. FeO
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E20/00—Combustion technologies with mitigation potential
    • Y02E20/34—Indirect CO2mitigation, i.e. by acting on non CO2directly related matters of the process, e.g. pre-heating or heat recovery
    • 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

  • the invention relates to an apparatus and a method suitable for performing combustion of gaseous fuel, and which may be used for producing hydrogen.
  • Steam reforming is a common method of hydrogen production. The main process step involves the reaction of steam with a hydrocarbon over a catalyst to form hydrogen and carbon oxides. However, the subsequent process steps that are needed to separate the hydrogen from the carbon oxides and any impurities are complicated and expensive. Likewise, it is difficult to separate out hydrogen from the combustion gases that are formed upon the air gasification of a fuel such as a fossil based hydrocarbon or solid biomass.
  • the present invention enables pure hydrogen to be produced, while overcoming these problems.
  • an apparatus for performing combustion of a gaseous fuel comprising a compact reactor consisting of a plurality of metal sheets arranged to define first and second gas flow channels, the channels being arranged alternately to ensure good thermal contact between the gases in them and each channel containing a removable metallic heat conducting insert coated with a support ceramic, in one set of channels the ceramic incorporating particles comprising an oxide of a transition metal and in the other set of channels the ceramic incorporating particles of a transition metal.
  • Suitable materials for the ceramic are those which are stable at the reaction temperatures and do not react irreversibly with the transition metal, for example alumina or zirconia.
  • the ceramic may also be doped with a material such as lanthanum, cerium or gadolinium to enhance its stability.
  • the “metal” particles might actually be a metal oxide in which the metal is in a low oxidation state, whereas in the “metal oxide” particles the metal is in a higher oxidation state.
  • both the first and the second gas flow channels are preferably less than 8 mm deep in the direction normal to the sheets. More preferably both the first and the second gas flow channels are less than 5 mm deep, but preferably at least 0.5 mm deep.
  • the heat-conducting insert may comprise a corrugated or dimpled foil, a wire mesh, or a corrugated metal felt.
  • the ceramic coating is of thickness typically in the range between 30 and 300 ⁇ m, and is porous, the transition metal or metal oxide particles being dispersed within the porous ceramic, and the ceramic being sufficiently porous that the gaseous reagents can diffuse to the surface of the particles.
  • the specific surface area of the ceramic is preferably in the range 50-340 m 2 /g, and the ceramic may be, for example, lanthanum-stabilised gamma-alumina.
  • the materials of which the reactor are made are subjected to a severely corrosive atmosphere in use, for example the temperature may be as high as 900° C., although more typically around 850° C.
  • the reactor may be made of a metal such as an aluminium-bearing ferritic steel, in particular of the type known as Fecralloy (trade mark) which is iron with up to 20% chromium, 0.5-12% aluminium, and 0.1-3% yttrium. For example it might comprise iron with 15% chromium, 4% aluminium, and 0.3% yttrium.
  • each step being carried out for sufficient time that a substantial proportion of the oxide particles have been reduced, and the gas flows then being exchanged so the other step is carried out.
  • the gaseous fuel comprises at least one gas which reduces the transition metal oxide particles to metal particles. It may comprise more than one reductant and may also include a diluent such as nitrogen and or carbon dioxide. If the combustion gas does not contain a diluent such as nitrogen, the output from the combustion channels can be substantially pure CO 2 (once any water-vapour has been condensed).
  • the oxidizing gas may comprise oxygen, for example it may be air.
  • the oxidizing gas may comprise an oxygen-containing compound, such as water vapour. If the oxidizing gas is steam, then the method provides an output of hydrogen gas, which can be over 99% pure.
  • the gaseous fuel may be the result of gasifying a hydrocarbon or a biomass product.
  • biomass such as forestry waste, coppiced willow or rice/corn husk may be decomposed autothermally (partial oxidation), typically in a fluidized bed gasifier, so as to produce hydrogen, carbon monoxide, methane, water, nitrogen and ash.
  • a typical gas composition for a 20 % moisture wood feed is 50-54% N 2 , 17-22% CO, 9-15% CO 2 , 12-20% H 2 and 2-3% CH 4 .
  • Such a gas has a typical heating value of 5-5.9 MJ/Nm 3 .
  • the fluidized bed gasifier may be fed with pre-heated air so that partial oxidation of the biomass occurs which produces the heat for the remaining thermal decomposition of the biomass.
  • the gasifier may in addition be fed with steam.
  • the gas resulting from the gasification of the biomass is typically cleaned, for example using catalytic tar removal, cyclonic ash removal and filtration.
  • the gas is then fed into the channels of the reactor.
  • the reductants in the gas such as carbon monoxide, hydrogen and methane, react with the transition metal oxide to produce carbon dioxide and water, and the transition metal oxide is reduced to the metal.
  • the reaction is exothermic, and is effectively combustion of the gas. Typically the reaction proceeds at about 300-800° C.
  • This process enables an impure mixture of gases to be used to generate hydrogen indirectly, by reducing the metal oxide to the metal.
  • the metal oxide is re-formed by the reaction between hot steam and the metal, which results in the generation of pure hydrogen without the need for complicated separation techniques.
  • the first set of channels may be fed with a gaseous fuel which undergoes combustion in the channels, but which does not include any diluent gases.
  • a gaseous fuel which undergoes combustion in the channels, but which does not include any diluent gases.
  • Any gaseous fuel that is capable of reducing the metal oxide may be used, for example synthesis gas produced from coal or heavy oil gasification.
  • the fuel is oxidized in the channels, thereby reducing the metal oxide to metal.
  • the metal oxide acts as an oxygen donor for the reaction thus producing the fully oxidized pure combustion products carbon dioxide and water.
  • the carbon dioxide is not diluted with nitrogen because the source of oxygen for the combustion is not air but a metal oxide.
  • the pure carbon dioxide can then be sequestrated by compression and injection into a suitable sub-surface storage volume without the need to remove any nitrogen.
  • the oxidizing gas is steam, this may be produced by heating water.
  • the steam reacts with the dispersed transition metal particles at elevated temperature, typically 300-800° C., to produce transition metal oxide and hydrogen.
  • the reaction is endothermic and heat for the reaction is provided from the exothermic reaction of the gaseous fuel with the transition metal oxide in the adjacent set of channels.
  • the oxidizing gas is air
  • the oxygen from the air reacts exothermally to generate the metal oxide.
  • the temperature may reach above 800° C., and heat is transferred into adjacent channels.
  • the fuel reacts with the metal oxide, and is itself oxidized.
  • the absence of a flame front and the good thermal control result in low NO x generation.
  • the overall chemical reaction is that the gaseous fuel is oxidized, so the overall process is strongly exothermic.
  • the reactor may incorporate a third set of channels which in this case may carry a coolant fluid.
  • the gas streams feeding each set of channels are changed over so that the reactions proceed in alternating quasi-continuous cycles.
  • the gas flows are exchanged when a substantial proportion of the metal oxide particles have been reduced, and this proportion is preferably at least 30%, more preferably 50%, more preferably 70% and most preferably 90% of the particles.
  • the hot product gases, hydrogen, carbon dioxide and water vapour from the reactor are used to pre-heat the air that is fed to the fluidised bed gasifier.
  • the hot hydrogen product and/or the hot exhaust gas from the transition metal oxide reduction reaction may be used in this way.
  • FIG. 1 shows a flow diagram for the plant and process of the invention
  • FIG. 2 shows a sectional view of a compact reactor for use in the plant of FIG. 1 , showing one metal plate in plan;
  • FIG. 3 shows a flow diagram for an alternative plant and process of the invention.
  • a plant 10 for combustion of a fuel gas is shown, where the fuel gas may be for example methane, or a mixture of hydrogen and carbon monoxide resulting from the gasification of coal or other fossil fuels.
  • the plant 10 incorporates a compact reactor 12 which defines two sets of gas flow channels 14 and 15 which alternate with each other and are in good thermal contact (the reactor is described in greater detail with reference to FIG. 2 ).
  • a removable metallic heat-conducting insert coated with a ceramic initially the inserts in flow channels 14 contain particles of cobalt metal, while the inserts in flow channels 15 contain particles of cobalt oxide.
  • the reactor 12 incorporates headers 18 in communication with the flow channels 14 , and incorporates headers 19 in communication with the flow channels 15 .
  • the fuel gas is supplied through a valve 20 to the inlet header 19 to flow through the channels 15 , and at the same time air is supplied through a valve 22 to the inlet headers 18 to flow through the flow channels 14 .
  • Oxygen from the air reacts vigorously and exothermically with the particles of cobalt metal, oxidising them to cobalt oxide, this reaction increasing the temperature in the channels 14 to about 800° C.
  • the inserts in the channels 15 are also heated to a high temperature, typically about 750° C. At this high temperature the fuel gas reduces the cobalt oxide particles to cobalt metal, this reaction being somewhat exothermic; the fuel gas undergoes combustion, by taking oxygen from the oxide particles.
  • the hot gases emerging from the outlet headers 18 and 19 are consequently at about 750° C., and are then supplied via respective valves 24 and 25 to respective heat exchangers 26 to generate steam. This may be used for electricity generation.
  • the exhaust gases from the channels 15 in which the fuel gas has been oxidised, are then cooled still further to condense water vapour, as indicated at 28 , and the resulting carbon dioxide is subjected to sequestration treatment.
  • the gas flows are exchanged by operating the valves 20 and 22 and the valves 24 and 25 .
  • the fuel gas flows through the channels 14 and the air flows through the channels 15 .
  • These two phases then alternate whenever substantially all the metal oxide particles in the channel carrying the fuel gas have been reduced to metal.
  • combustion of the fuel gas is substantially continuous, though taking place alternately in the two sets of channels.
  • the cycle time for switching between the two phases depends on the operating temperature, the metal loading and the degree of metal dispersion.
  • a reactor 40 suitable for use as the reactor 12 comprises a stack of Fecralloy steel plates 41 , each plate being generally rectangular, 450 mm long and 150 mm wide and 3 mm thick, these dimensions being given only by way of example. There may for example be forty plates 41 in the stack. On the upper surface of each such plate 41 are rectangular grooves 42 of depth 2 mm separated by lands 43 (eight such grooves being shown), but there are three different arrangements of the grooves 42 . In the plate 41 shown in the drawing the grooves 42 extend diagonally at an angle of 45° to the longitudinal axis of the plate 41 , from top left to bottom right as shown.
  • the grooves 42 a (as indicated by broken lines) follow a mirror image pattern, extending diagonally at 45° from bottom left to top right as shown.
  • the grooves 42 b (as indicated by chain dotted lines) extend parallel to the longitudinal axis.
  • the plates 41 are assembled in a stack, plates 41 of the third type (with the longitudinal grooves 42 b ) alternating with plates of the first or second types, which are themselves used alternately so that each plate of the third type is between a plate with diagonal grooves 42 and a plate with mirror image diagonal grooves 42 a, and after assembling many plates 41 the stack is completed with a blank rectangular plate.
  • the plates 41 are compressed together during diffusion bonding, so they are sealed to each other.
  • Inserts 44 comprising corrugated Fecralloy alloy foils (only one is shown) 50 ⁇ m thick coated with a ceramic coating, of appropriate shapes and with corrugations 2 mm high, can be slid into each such groove 42 , 42 a and 42 b.
  • each three-compartment header 18 there might instead be three adjacent header chambers, each being a rectangular cap like the headers 19 .
  • the longitudinal grooves 42 b define the channels 15
  • the diagonal grooves 42 and 42 a define the channels 14 .
  • the flow path for the mixture supplied to the top-left compartment of the header 18 is through the diagonal grooves 42 into the bottom-middle header compartment, and then to flow through the diagonal grooves 42 a in other plates in the stack into the top-right compartment of the header 18 .
  • the gas flows in the channels 15 and 14 are at least partially co-current.
  • the headers 18 and 19 each comprise a simple rectangular cap sealed around its periphery to the outside of the stack so as to cover part of one face of the stack. They may be welded onto the outside of the stack. Alternatively, if neither of the gas flows are at elevated pressures, it may be adequate to clamp them onto the outside of the stack. In either case it will be appreciated that after a period of use, if the metal or metal oxide particles in either or both of the channels has lost reactivity, then the headers 18 and 19 may be removed or cut off and the corresponding inserts 44 removed and replaced. The headers 18 , 19 can then be re-attached.
  • the inserts 44 may have a coating of stabilised gamma alumina of thickness 100 ⁇ m, to which cobalt metal is added in the proportion 30% by weight. After deposition of the ceramic coating, the coating is saturated with a solution of cobalt nitrate, and this is then decomposed by heat treatment. For those inserts 44 that are required to contain cobalt oxide, the heat treatment can be carried out in an atmosphere containing oxygen, whereas for the inserts 44 that are required to contain cobalt metal the heat treatment would be carried out in a reducing atmosphere, for example containing hydrogen. This process may be repeated to increase the proportion of cobalt. This process can produce particles of size less than 50 nm, which are highly reactive.
  • the alumina support maintains the high degree of dispersion of the cobalt (or cobalt oxide) preventing sintering during high temperature operation; it may incorporate additives such as lanthanum to improve hydrothermal stability.
  • the reactor 12 may take a different form to that shown in FIG. 2 , but that it is essential that the channels 14 and 15 are in good thermal contact with each other.
  • the reactor should define a multiplicity of alternating flow channels, and these are preferably defined between metal sheets in a stack, either by flat sheets with grooves or slots, or by corrugated sheets.
  • the channels are not in transverse directions, so the flows are at least partly parallel, but the headers for the different gases must be separate.
  • the inserts must be removable, once the headers are removed, so they can be replaced if necessary without replacing the entire reactor.
  • the reactor may also incorporate a third set of flow channels for generating steam.
  • the reactor may comprise a stack of hexagonal plates each defining a set of straight grooves between a pair of opposite sides; plates arranged with their grooves in different orientations provide flow paths for different fluids, so there are flow paths for three different fluids: water/steam; fuel (to reduce metal oxide particles); and air (to oxidize metal particles).
  • These three fluid flow paths may be defined by three successive plates, such groups of three successive plates being repeated to form the stack. This enables superheated steam to be generated directly from the reactor.
  • the reactor may operate at a lower temperature to that discussed above, for example 400-600° C., or even as low as about 300° C. if the metal is highly dispersed and a reduction promoter such as ruthenium and platinum is included in the ceramic.
  • the fuel gas in this case is made from a supply of biomass 33 .
  • the biomass 33 is fed to a gasifier 34 where it undergoes partial oxidation in the presence of air.
  • the resulting fuel gas is then cleaned and sulphur is removed 35 from it.
  • the gas is fed through a heat exchanger 36 so as to heat water to produce the steam for channels 15 , and then fed through the valve 31 to the channels 14 .
  • the hot fuel gas reduces the cobalt oxide particles to cobalt metal, this reaction being somewhat exothermic. Thermal balance in the reactor may be achieved by the control of reactant gas flowrate within each set of channels 14 and 15 .
  • the hot gases emerging from the channels 14 and 15 are typically at about 750° C., and are then supplied to heat exchangers 26 .
  • the heat exchangers are positioned so as to provide some or all of the heat required to heat the air that is fed to the fuel gasifier 34 .
  • the exhaust gases from the channels 14 in which the fuel gas has been oxidised, may then be cooled still further to condense water vapour, if this water is required in the steam generating process, and the remaining gases are vented to the atmosphere.
  • One or both of the heat exchangers 26 may alternatively be positioned so as to heat the steam for the compact reactor.
  • the gas flows are exchanged by operating the valves 31 and 32 and valves 37 and 38 in the outlet ducts.
  • the fuel gas flows through the channels 15 , and the steam flows through the channels 14 .
  • These two operational phases then alternate whenever substantially all the metal particles in the channel carrying the steam have been oxidised to metal oxide.
  • hydrogen production is substantially continuous, though taking place alternately in the two sets of channels.
  • the cycle time for switching between the two phases depends on the operating temperature, the metal loading and the degree of metal dispersion and the space velocity of the feed gases. So as to maintain a substantially pure flow of hydrogen the exhaust gases from the channels fed by steam may initially be vented to the atmosphere after changeover until sufficiently pure hydrogen is being produced.
  • a compact reactor may be supplied with a fuel gas with no diluent gases (as described in relation to the plant 10 ), fed to the channels containing metal oxide particles, and with steam (as described in relation to the plant 30 ) fed to the channels containing metal particles.
  • a fuel gas with no diluent gases as described in relation to the plant 10
  • steam as described in relation to the plant 30
  • the resulting CO 2 from the combustion of the fuel gas can readily be sequestered (as with the plant 10 ).

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • General Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Hydrogen, Water And Hydrids (AREA)
US10/557,994 2003-06-28 2004-06-21 Combustion of gaseous fuel Abandoned US20070056247A1 (en)

Applications Claiming Priority (5)

Application Number Priority Date Filing Date Title
GB0315180.0 2003-06-28
GB0315180A GB0315180D0 (en) 2003-06-28 2003-06-28 Combustion of gaseous fuel
GB0320513A GB0320513D0 (en) 2003-09-02 2003-09-02 Production of hydrogen
GB0320513.5 2003-09-02
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