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WO2007060480A1 - Appareil de reformage de carburant - Google Patents

Appareil de reformage de carburant Download PDF

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Publication number
WO2007060480A1
WO2007060480A1 PCT/GB2006/050402 GB2006050402W WO2007060480A1 WO 2007060480 A1 WO2007060480 A1 WO 2007060480A1 GB 2006050402 W GB2006050402 W GB 2006050402W WO 2007060480 A1 WO2007060480 A1 WO 2007060480A1
Authority
WO
WIPO (PCT)
Prior art keywords
fuel
oxygen
reaction chamber
reforming
gas permeable
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/GB2006/050402
Other languages
English (en)
Inventor
John Sydney Carlow
Robert Frew Gillespie
Stuart Leigh Jones
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Qinetiq Ltd
Accentus Medical PLC
Original Assignee
Qinetiq Ltd
Accentus Medical PLC
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Qinetiq Ltd, Accentus Medical PLC filed Critical Qinetiq Ltd
Priority to GB0807420A priority Critical patent/GB2448084A/en
Publication of WO2007060480A1 publication Critical patent/WO2007060480A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • 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
    • C01B2203/80—Aspect of integrated processes for the production of hydrogen or synthesis gas not covered by groups C01B2203/02 - C01B2203/1695
    • C01B2203/82—Several process steps of C01B2203/02 - C01B2203/08 integrated into a single apparatus
    • 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
    • Y02P20/10—Process efficiency
    • Y02P20/129—Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Definitions

  • the present invention relates to an apparatus for fuel reforming in order to produce hydrogen from hydrocarbon fuels.
  • the invention also relates to the use of the apparatus for fuel reforming.
  • the main routes known for the production of hydrogen from hydrocarbons are steam reforming, partial oxidation and carbon dioxide reforming.
  • Partial oxidation requires that reaction conditions have to be set up for a hydrocarbon to react with oxygen according to the equations
  • Partial oxidation reforming reactions are highly exothermic and are an extremely efficient method of providing base process heating. This is useful where endothermic steam reforming reactions are utilised further along in the process stream so minimising the external heat inputs required.
  • US patent no. 6,245,309 discloses a system for reforming a fuel gas to produce a stream of hydrogen for a fuel cell.
  • the system comprises a combustion chamber and a plasma reforming chamber. Fuel is combusted in the combustion chamber and the heat of combustion is used to preheat the reactive gases for plasma reforming. No other form of integrated preheating is disclosed in the patent.
  • the present invention provides an apparatus for use in fuel reforming, which apparatus comprises a first reaction chamber having an inlet for a fuel and oxygen mixture, the inlet being provided with a gas permeable ceramic and/or metal body, and a means of ignition, and a second reaction chamber, communicating with the first reaction chamber, said second reaction chamber comprising a fuel reforming device.
  • the fuel is generally a hydrocarbon. It is typically a liquid or gaseous hydrocarbon such as methane, natural gas, petrol or diesel fuel. It may also be, for example, an alcohol such as ethanol, a glycol, such as polyethylene glycol, such as glycerol, or biodiesel.
  • the hydrocarbon may be pure or impure. In particular it may contain sulphurous impurities. However, in general any liquid or gaseous hydrocarbon may be used.
  • a hydrocarbon that is solid at room temperature may be used if it can be provided to the reactor in the form of a liquid or gas, or as a solid when entrained as small particles in a fluidised bed.
  • Partial oxidation of the fuel takes place in the first reaction chamber.
  • oxygen must be supplied.
  • the oxygen may be in the form of oxygen alone or oxygen mixed with one or more other gases, for example the oxygen may be provided as air. It is generally preferred to mix the fuel with air rather than oxygen due to cost.
  • the gas permeable ceramic or metal body is a body that has a plurality of channels or paths in it through which the fuel and oxygen mixture can pass. Typically the channels run the entire length of the burner without interconnecting with one another but some interconnections may be present. As the fuel/oxygen mixture flows through the gas permeable body the fuel and oxygen undergo thorough mixing.
  • An example of a suitable body is a flowthrough (open at both ends) ceramic honeycomb of the type used in conjunction with 3-way catalysts for control of emissions from petrol engines. These honeycombs are typically made out of a low thermal expansion glass ceramic, cordierite, and have channels with a rectangular or square cross section. The channels could also be any other shape such as circular, hexagonal or triangular in cross-section.
  • Honeycombs are produced by, for example, Corning and NGK. (A tradename of the Corning product is Celcor.)
  • the channel density often ranges from 50 to 400 channels or cells per square inch (0.625 x 10 ⁇ 3 m 2 ) .
  • the walls separating the channels may be impervious to gas, or are gas permeable, for example when used as filters for diesel exhaust gases, .
  • the gas permeable ceramic and/or metal body is a block of ceramic material preferably a ceramic monolith with communication of gas between channels to aid mixing.
  • Alternative ceramic or metal bodies are an open structured ceramic foam, a metal mesh or gauze, a rigid ceramic fibre blanket or sintered metal and/or ceramic material.
  • Suitable sintered materials include sintered metal fibre, sintered metal powder and sintered ceramics.
  • Metal matrix and composite materials may also be used for example a metal-reinforced ceramic where the metal reinforcement involves use of metal fibres or rods as examples.
  • An example of a ceramic composite is silicon carbide, for example fibres, dispersed in an alumina matrix.
  • a ceramic reinforced metal matrix may also be used for example a ceramic powder dispersed in a metal matrix.
  • the gas permeable body aids fuel mixing and locating of the flame front.
  • the flame front is located immediately at the exit of the gas permeable body in the first reaction chamber.
  • some burning may take place just inside the gas permeable body, for example, up to a depth equivalent to the width of a channel.
  • the gas permeable body typically takes heat away from the flame itself and therefore the gas mixture is typically not hot enough to burn in the gas permeable body.
  • there is a foam or sponge positioned immediately before the ceramic monolith to aid mixing of the fuel and oxygen prior to entry to the monolith. This is particularly important where longitudinal monolithic flow forms are used, as mixing of fuel and the air is further enhanced.
  • the fuel is ignited in the first reaction chamber.
  • the ignition source may be electrical, mechanical or chemical/mechanical.
  • the ignition source may be piezoelectric, a laser pulse, UV light, radio- frequency (r . f .) /microwave heating or a tesla coil spark igniter.
  • the ignition source is typically placed immediately downstream of the gas permeable ceramic or metal body. Ignition may take place within the gas permeable body. Ignition may be caused by a catalyst which may be coated on the inside of the gas permeable body.
  • the initial burning of the fuel may take place at least partially in the monolith to a small extent.
  • ignition may be caused by a catalyst which may be coated on the inside of the gas permeable body.
  • the fuel typically burns substantially without a flame.
  • the reactor may further comprise a flash-back arrestor upstream of the gas permeable body to prevent oxidation of the fuel occurring in the inlet pipe.
  • the arrestor may be made of, for example, high conductivity metallic mesh.
  • the arrestor can be a separate body, or more conveniently be provided by the sponge or foam used at the mixing position immediately ahead of the gas permeable ceramic or monolith.
  • further fuel mixed with oxygen is added to the partially oxidised fuel and oxygen mixture through a second inlet before it enters the second reaction chamber in order to change the composition of the fuel and oxygen mixture.
  • the amount of fuel and oxygen (which may be in the form of air) added is controlled so as to alter the composition of gases in the reaction chamber so that the resulting composition of gases is such that the partial oxidation process is favoured.
  • the fuel and oxygen composition for ignition is typically richer in oxygen than the composition required for partial oxidation. This addition of fuel and oxygen will typically be necessary when the correct composition of gases is often not achieved by ignition of the initial fuel and oxygen mixture.
  • the partial oxidation stage is used to heat the gases to a temperature close to that at which reforming can take place.
  • the fuel/oxygen mixture may be heated before entering the first reaction chamber.
  • the fuel/oxygen mixture may be passed through a heat exchanger to heat the mixture.
  • the heat exchanger may be located within the reaction chamber so as to use excess heat from the partial oxidation reaction to heat the fuel/oxygen mixture before it enters the reactor.
  • a heat exchanger may be used for the fuel/oxygen entering through the first, second or both inlets.
  • the gases are then transferred to the second reaction chamber.
  • the second oxidation chamber is connected to the first reaction chamber, for example by a pipe.
  • further fuel and oxygen may be added in order to alter the gas composition so as to be suitable for reforming. This will typically be necessary if the gas composition resulting from the partial oxidation process is not suitable for reforming.
  • the further fuel/oxygen and or the water vapour may pass through a flash-back arrestor and/or a heat exchanger before entering the apparatus.
  • the second reaction chamber comprises a fuel reforming device.
  • the fuel reforming device is any device which can reform the partially oxidised fuel and oxygen mixture to produce hydrogen (and carbon dioxide/ carbon monoxide) .
  • the fuel reforming device may be a plasma device. Any plasma device which activates the gases is appropriate.
  • the plasma device may be, for example, a microwave plasma generator, a non-thermal plasma dielectric barrier reactor, a corona discharge reactor or a gliding arc plasma reactor.
  • the fuel reforming device may also be a microwave heat source or radio-frequency (r.f.) heating may be used to heat the fuel/gas mixture to a temperature at which fuel reforming takes place.
  • r.f. radio-frequency
  • a microwave heating source or radio-frequency heating is that is possible to vary the power input using one of these devices and they do not suffer from the thermal lag that is present if a thermal heat source were used.
  • the gases are passed through the fuel reforming device. This activates the gas molecules providing them with enough energy to reform amongst themselves.
  • the products of the reforming reaction are carbon dioxide, carbon monoxide and hydrogen.
  • the hydrogen may be separated from other products by known methods such as pressure swing absorption or membrane separation.
  • the carbon monoxide is typically converted to carbon dioxide in the presence of a catalyst.
  • water vapour may be added to the fuel and oxygen mixture in order to perform a steam reforming reaction in the second chamber.
  • the water vapour may be added as the gases enter the second chamber or at or near the exit from the first reaction chamber.
  • steam reforming is an endothermic reaction further heating may be required in the second reaction chamber in order for the reaction to proceed.
  • Any part of the process may be enhanced by the presence of a catalyst.
  • a catalyst for the partial oxidation of the fuel may be included in the first reaction chamber. This may be, for example, nickel when the fuel is natural gas or methane or platinum, platinum/rhodium or ruthenium for heavier fuels, in particular diesel. In addition or alternatively, a catalyst may be present in the gas permeable body.
  • a catalyst for the reforming of the activated species may be present in the plasma device or downstream of the plasma device such that the activated gas molecules pass over the catalyst after leaving the second reaction chamber. If the catalyst is placed downstream of the plasma device it may be within the reaction chamber, in the exit pipe or in a further reaction chamber.
  • Suitable catalysts to catalyse the reforming reaction include, for example, nickel or rhodium.
  • the present invention also provides a method of fuel reforming using the apparatus of the present invention.
  • the present invention further provides a method of fuel reforming comprising supplying fuel and oxygen to a reactor, mixing the fuel and oxygen, igniting the fuel such that partial oxidation occurs and then reforming the partially oxidised fuel.
  • the present invention also provides a gas permeable body comprising a) one or more channels arranged for fuel and/or oxygen to pass, as inlet stream, therethrough; and b) one or more central channels communicating with the inlet channel (s) and arranged in the counter- current direction to the inlet channel for the inlet stream, optionally to mix or further mix the fuel and oxygen, and pass through and from the body.
  • the mixed gases then exit from the centre of the gas permeable body.
  • the fuel and oxygen (which may be provided as air) or fuel/oxygen mixture is heated on passing through the gas permeable body prior to ignition of the fuel.
  • water may be added through a further channel or with the fuel or oxygen.
  • the body provides at least two channels through which the fuel/oxygen mixture passes, typically outer channels of the body, before mixing in the body.
  • the body provides separate channels for fuel and oxygen and the fuel and oxygen mix on leaving the separate channels and entering central channel (s) of the gas permeable body.
  • the fuel is ignited in or on leaving the gas permeable body.
  • the position of ignition of the fuel depends on the gas flow velocities and the size of the channels. Channels with a diameter of ⁇ 0.5mm typically extinguish a flame, whereas a flame can continue in a channel with a diameter of >0.5mm.
  • the specific critical dimensions are dependent on the fuel, those cited herein being relevant to natural gas as a feed.
  • the diameter of the inlet channel (s) is ⁇ 0.5mm and the diameter of the central channel (s) is >0.5mm.
  • the gas flow velocity is also typically regulated so that the flame is not pushed away from the end of the gas permeable body. Ignition of the fuel may be caused by a catalyst coated on the inside of the gas permeable body.
  • a flashback arrestor is incorporated into the fuel and/or fuel/oxygen channels, for example just before the point at which the channel enters the gas permeable body.
  • a gas permeable body which preheats the inlet gases may be used in the fuel reforming apparatus of the present invention or in any apparatus where ignition occurs in or on leaving a gas permeable body.
  • the gas permeable body is a monolith.
  • the central channel of the gas permeable body is filled with a foam or ceramic wool to aid mixing of the fuel and oxygen.
  • outer channels for preheating the gases may be attached to the ceramic sponge or foam.
  • the gas permeable body is in the form of a foam cylinder surrounded by a foam annulus and separated by a solid material (separator sheet) .
  • the central part of the gas permeable body is filled with a foam or wool so as to induce turbulent flow.
  • Figure 1 is a diagrammatic cross-section of one embodiment of the present invention.
  • Figure 2 is a diagrammatic perspective view of a gas permeable body of the present invention
  • Figure 3 is diagrammatic cross-section of the gas permeable body of figure 2.
  • Figure 1 shows an apparatus according to the present invention.
  • the apparatus comprises a first reaction chamber (1), and a second reaction chamber (2) and a downstream further reaction zone (3) .
  • the final section of the reactor is an exit cone (4) .
  • the fuel and air mixture for ignition is fed in through pipe (5) in the direction of the arrows.
  • the mixture passes through a heat exchanger (6), a flash-back arrestor (7) and a ceramic monolith (8) in turn and then enters the first reaction chamber (1) .
  • the ignition source (9) for the fuel/air mixture is located just downstream of the ceramic monolith.
  • the first reaction chamber also has a second inlet of fuel and air from pipe (10) and this fuel/air mixture is used to adjust the composition of gases in the first reaction chamber for partial oxidation before the gases pass into the second reaction chamber (2) .
  • the second reaction chamber (2) contains a plasma device (or an alternative reforming device) .
  • the further reaction zone (3) may optionally contain a catalyst.
  • Both the first and second pipes (5,10) for fuel and air pass the fuel and air through a flashback arrestor (11) and a heat exchanger (6) before entering the reaction chamber.
  • the combined apparatus is also insulated (12) so as to reduce heat losses during operation.
  • Figure 2 shows a ceramic monolith (20) through which gas inlet streams (22,24) pass before ignition (not shown) .
  • Gas enters the inlets (22,24) and is then heated as it passes along the channels (261,281) .
  • the inlet streams are then routed (26,28) round to enter the centre of the monolith (30) .
  • the centre of the monolith is sealed with a plate (34) .
  • the gases mix and pass through the centre of the monolith undergoing ignition either within the monolith or on leaving it.
  • the centre of the monolith (30) is preferably filled with a ceramic wool to promote good mixing of the gas streams.
  • one stream is a fuel stream and the other is air.
  • Figure 3 is a cross sectional view of the monolith shown in Figure 2.
  • the same numerals are used to refer to the same structures.
  • the apparatus may be fed with a mixture of fuel and oxygen rather than a mixture of fuel and air.
  • the apparatus may be fed with a mixture of fuel and oxygen rather than a mixture of fuel and air.
  • the gas permeable body of Figures 2 and 3 may be used.
  • the body may comprise, for example, concentric cylinders where an outer cylinder is used for the counter-current gas flow and the gases then pass through the centre of the body.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Physics & Mathematics (AREA)
  • Fluid Mechanics (AREA)
  • Toxicology (AREA)
  • Hydrogen, Water And Hydrids (AREA)

Abstract

Appareil destiné à être utilisé dans le reformage de carburant, ledit appareil comportant une première chambre de réaction dotée d'une entrée pour un mélange de carburant et d'oxygène, l'entrée étant pourvue d'un corps en céramique perméable aux gaz et / ou en métal et d'un moyen d'allumage, et une deuxième chambre de réaction communiquant avec la première chambre de réaction, ladite deuxième chambre de réaction comportant un dispositif de reformage de carburant.
PCT/GB2006/050402 2005-11-22 2006-11-21 Appareil de reformage de carburant Ceased WO2007060480A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
GB0807420A GB2448084A (en) 2005-11-22 2006-11-21 Fueling reforming apparatus

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB0523646.8 2005-11-22
GBGB0523646.8A GB0523646D0 (en) 2005-11-22 2005-11-22 Fuel reforming apparatus

Publications (1)

Publication Number Publication Date
WO2007060480A1 true WO2007060480A1 (fr) 2007-05-31

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ID=35580395

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/GB2006/050402 Ceased WO2007060480A1 (fr) 2005-11-22 2006-11-21 Appareil de reformage de carburant

Country Status (2)

Country Link
GB (2) GB0523646D0 (fr)
WO (1) WO2007060480A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2009126229A3 (fr) * 2008-04-07 2010-03-04 Florida Syngas Dispositif convertissant une matière carbonée en gaz de synthèse et procédés associés
CN109896501A (zh) * 2017-12-11 2019-06-18 中国科学院大连化学物理研究所 一种重整制氢装置及采用该装置制氢的方法

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5112527A (en) * 1991-04-02 1992-05-12 Amoco Corporation Process for converting natural gas to synthesis gas
US5762658A (en) * 1994-06-24 1998-06-09 Johnson Matthey Public Limited Company Self-sustaining hydrogene generator
EP1118583A2 (fr) * 1996-08-26 2001-07-25 Arthur D Little, Inc. Procédé et appareil pour transformer du carburant hydrocarbure en gaz hydrogène et en dioxyde de carbone
EP1382382A1 (fr) * 2002-07-19 2004-01-21 Conoco Phillips Company Distributeur de gaz avec une pluralité de canaux et son utilisation dans un réacteur catalytique
US20060219735A1 (en) * 2002-11-06 2006-10-05 Ian Faye Dosing device

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US5112527A (en) * 1991-04-02 1992-05-12 Amoco Corporation Process for converting natural gas to synthesis gas
US5762658A (en) * 1994-06-24 1998-06-09 Johnson Matthey Public Limited Company Self-sustaining hydrogene generator
EP1118583A2 (fr) * 1996-08-26 2001-07-25 Arthur D Little, Inc. Procédé et appareil pour transformer du carburant hydrocarbure en gaz hydrogène et en dioxyde de carbone
EP1382382A1 (fr) * 2002-07-19 2004-01-21 Conoco Phillips Company Distributeur de gaz avec une pluralité de canaux et son utilisation dans un réacteur catalytique
US20060219735A1 (en) * 2002-11-06 2006-10-05 Ian Faye Dosing device

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2009126229A3 (fr) * 2008-04-07 2010-03-04 Florida Syngas Dispositif convertissant une matière carbonée en gaz de synthèse et procédés associés
CN109896501A (zh) * 2017-12-11 2019-06-18 中国科学院大连化学物理研究所 一种重整制氢装置及采用该装置制氢的方法

Also Published As

Publication number Publication date
GB2448084A (en) 2008-10-01
GB0523646D0 (en) 2005-12-28
GB0807420D0 (en) 2008-05-28

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