WO2007042246A2 - Procede de vaporisation et de reformage de combustibles liquides - Google Patents

Procede de vaporisation et de reformage de combustibles liquides Download PDF

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Publication number
WO2007042246A2
WO2007042246A2 PCT/EP2006/009742 EP2006009742W WO2007042246A2 WO 2007042246 A2 WO2007042246 A2 WO 2007042246A2 EP 2006009742 W EP2006009742 W EP 2006009742W WO 2007042246 A2 WO2007042246 A2 WO 2007042246A2
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WO
WIPO (PCT)
Prior art keywords
air
supplied
reforming
reaction space
volume
Prior art date
Application number
PCT/EP2006/009742
Other languages
German (de)
English (en)
Other versions
WO2007042246A3 (fr
Inventor
Thomas Aicher
Lothar Griesser
Original Assignee
Fraunhofer Gesellschaft Zur Förderung Der Angewandten Forschung E. V.
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 Fraunhofer Gesellschaft Zur Förderung Der Angewandten Forschung E. V. filed Critical Fraunhofer Gesellschaft Zur Förderung Der Angewandten Forschung E. V.
Priority to EP06806121A priority Critical patent/EP1940737A2/fr
Priority to CA002624762A priority patent/CA2624762A1/fr
Priority to JP2008533950A priority patent/JP2009511648A/ja
Publication of WO2007042246A2 publication Critical patent/WO2007042246A2/fr
Publication of WO2007042246A3 publication Critical patent/WO2007042246A3/fr
Priority to US12/099,319 priority patent/US20080229662A1/en

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • 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
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • 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
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/386—Catalytic partial combustion
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • 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
    • C01B3/22—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
    • 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
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0244—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being an autothermal reforming step, e.g. secondary reforming processes
    • 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
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0255—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a non-catalytic partial oxidation step
    • 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
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/025—Processes for making hydrogen or synthesis gas containing a partial oxidation step
    • C01B2203/0261—Processes for making hydrogen or synthesis gas containing a partial oxidation step containing a catalytic partial oxidation step [CPO]
    • 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
    • C01B2203/1005—Arrangement or shape of catalyst
    • C01B2203/1011—Packed bed of catalytic structures, e.g. particles, packing elements
    • 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
    • C01B2203/1005—Arrangement or shape of catalyst
    • C01B2203/1023—Catalysts in the form of a monolith or honeycomb
    • 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
    • C01B2203/1047—Group VIII metal catalysts
    • C01B2203/1052—Nickel or cobalt catalysts
    • C01B2203/1058—Nickel catalysts
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1276—Mixing of different feed components
    • C01B2203/1282—Mixing of different feed components using static mixers
    • 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
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1288—Evaporation of one or more of the different feed components

Definitions

  • the invention relates to a process for the evaporation and reforming of liquid fuels, in particular the catalytic and non-catalytic partial oxidation and the autothermal reforming of liquid fuels with the addition of air or air-steam mixtures or air-water mixtures.
  • the invention solves the problems of mixture formation, soot formation and conversion to low hydrocarbons and hydrogen in connection with reforming processes known from the prior art.
  • DE 199 51 585 A1 describes a reforming device in which a hydrocarbon-air-vapor mixture is catalytically converted to a hydrogen-rich product gas.
  • the fuel is injected by means of a nozzle in liquid form with droplet formation in the Eduktgemischaufleungsraum.
  • the method described here can not ensure that the educts mix homogeneously over a wide range of load conditions because, due to the nature of the nozzle (also two-fluid nozzle or three-fluid nozzle), the droplet size varies greatly with the fuel throughput through the nozzle. Therefore, the reactants mix differently depending on the operating state and thus the droplet size.
  • EP 0 199 587 B1 describes an autothermal reforming reactor which likewise introduces liquid fuels into a reactor with the aid of a nozzle, wherein the atomized fuel is partially oxidized directly after mixing with oxygen and steam in a catalyst-occupied reaction space, before a second, also catalyst-occupied reaction space that uses steam reforming.
  • This method also has the disadvantage that the droplet size varies so much depending on the throughput through the reactor that a homogeneous mixing of all educt streams is not guaranteed at all times.
  • EP 0 716 225 describes a process for the evaporation of liquid fuels by partial catalytic oxidation and heat supply to the liquid by thermal radiation. This process can not be used directly for reforming because the conversion of the fuel to low-chain hydrocarbons and hydrogen is insufficient.
  • Another method is based on the phenomenon of the so-called. Cold flame for mixture formation. These are exothermic pre-reactions that partially convert and vaporize the fuel with heat release. The reaction is limited to a characteristic temperature specific to each fuel due to kinetic self-limitation. Below this characteristic temperature, auto-ignition of the fuel-oxidant mixture can be safely avoided (see, for example, A. Naidja, CR Krishna, T. Butcher, D. Mahajan, Progr.
  • Another common way of forming a mixture is to introduce the liquid fuel into liquid water or superheated steam, to vaporize this mixture in the first case, and then to contact it with (atmospheric) oxygen.
  • a process for the evaporation and reforming of liquid fuels in which the fuel is vaporized and partially oxidized in a first reaction space with the aid of a first catalyst (as set out in EP 0 716 225) and in a second reaction space the vaporized one Fuel is mixed with additionally supplied air and then reformed.
  • a ratio of the air volume supplied in the first reaction chamber to the air volume supplied in the second reaction chamber is set between 30:70 and 70:30.
  • the ratio of the volume of air supplied in the first reaction space to that in the second Response room supplied volume of air adjusted via distributor structures is adjusted via distributor structures.
  • the air is supplied via pipelines, wherein the pipelines have openings and / or nozzles and these are dimensioned such that the ratio of the volume of air supplied in the first reaction space to the volume of air supplied in the second reaction space is adjusted can.
  • nozzles or porous structures such as, for example, porous sintered metal bodies, are used as the distributor structure.
  • a preferred variant provides that in the second reaction space in the reforming, a second catalyst is used.
  • catalysts catalytically active noble metals or nickel are preferably used here on ceramic supports (for example honeycomb bodies or fillings).
  • ceramic supports for example honeycomb bodies or fillings.
  • a further preferred variant provides that corresponding carrier
  • Metal structures e.g. Honeycomb body, are used. Likewise, it is also possible that the reforming takes place without a catalyst.
  • the reforming can be carried out in this case by partial oxidation in a preferred variant.
  • Another preferred variant relates to the reforming by autothermal reforming.
  • the catalyst used for the reforming is in particular a packed bed, a honeycomb body or a coated metal mesh.
  • the mixing of fuel and supplied air after the first and in the second reaction space may preferably be assisted by static mixing devices.
  • a first variant for the evaporation and reforming of liquid fuels is shown. This is based on a catalytic partial oxidation with air supply through a tube in one stage.
  • the process for supplying air must be designed in such a way that the air is introduced in a defined ratio into the first reaction space, ie the evaporator, and into the second reaction space, ie the reformer.
  • the ratio of the air introduction in the evaporator to that in the reformer can be done by appropriately sized holes in the pipe.
  • the reactor is divided into the first reaction space, which has the evaporation catalyst 3, and the reaction space with the reforming catalyst 4.
  • a heater 5 may be used to preheat the device.
  • the product gas 6 after the reformer then leaves the reactor.
  • the partial oxidation shown here can also be carried out without tor 4 are performed.
  • the catalysts 3 and 4 and the tube 2 are e.g. preheated by external heating. Then, the air supply 1 and the fuel supply 7 are started. The preheating can be stopped after the onset of evaporation and reforming. In the first reaction chamber, the fuel is vaporized and partially oxidized, then in the second reaction chamber the fuel is reformed with the additional air supply.
  • Fig. 2 shows a device with two separate
  • Pipes 2 and 8 for the air supply can be set independently and thus also the ratio of the air flows to the evaporator and reformer.
  • water vapor can also be introduced into the second reaction space through the second tube. This makes it possible to implement the fuel by autothermal reforming.
  • the location of the air supply in the second reaction space ie the reformer, is variable.
  • the air supply 10 takes place before the second reaction space.
  • the air can be introduced into the reaction space through small openings or nozzles in the pipe for supplying air or through porous sintered metal bodies.
  • annular distributor structures are possible.
  • the air supply 12 takes place before the second reaction space through a supply arranged on the side.
  • a static mixer is additionally provided in comparison with FIG. 3 as a supplementary variant. This can be before and / or after the air supply and serves to mix the vaporized, partially oxidized fuel with the remaining air and optionally the water vapor.
  • FIG. 5 shows a variant in which the second reaction space is separated from the first reaction space, wherein both reaction spaces are connected by a tube with a smaller diameter.
  • the air supply also takes place via a lateral inlet, but it is also possible to choose other locations for the air supply.

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

Abstract

La présente invention concerne un procédé de vaporisation et de reformage de combustibles liquides, selon lequel, dans une première chambre de réaction, le combustible (7) est vaporisé au moyen d'un catalyseur (3) avec adjonction d'air (1) et oxydé de manière fortement substoechiométrique et, dans une deuxième chambre de réaction, le combustible vaporisé est mélangé à l'air introduit avant d'être reformé, le rapport du volume d'air introduit dans la première chambre de réaction relativement au volume d'air introduit dans la deuxième chambre de réaction étant réglé entre 30:70 et 70:30.
PCT/EP2006/009742 2005-10-10 2006-10-09 Procede de vaporisation et de reformage de combustibles liquides WO2007042246A2 (fr)

Priority Applications (4)

Application Number Priority Date Filing Date Title
EP06806121A EP1940737A2 (fr) 2005-10-10 2006-10-09 Procede de vaporisation et de reformage de combustibles liquides
CA002624762A CA2624762A1 (fr) 2005-10-10 2006-10-09 Procede de vaporisation et de reformage de combustibles liquides
JP2008533950A JP2009511648A (ja) 2005-10-10 2006-10-09 液体燃料を気化及び改質する方法
US12/099,319 US20080229662A1 (en) 2005-10-10 2008-04-08 Method for vaporising and reforming liquid fuels

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102005048385.2 2005-10-10
DE102005048385A DE102005048385A1 (de) 2005-10-10 2005-10-10 Verfahren zur Verdampfung und Reformierung flüssiger Brennstoffe

Related Child Applications (1)

Application Number Title Priority Date Filing Date
US12/099,319 Continuation US20080229662A1 (en) 2005-10-10 2008-04-08 Method for vaporising and reforming liquid fuels

Publications (2)

Publication Number Publication Date
WO2007042246A2 true WO2007042246A2 (fr) 2007-04-19
WO2007042246A3 WO2007042246A3 (fr) 2007-07-05

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PCT/EP2006/009742 WO2007042246A2 (fr) 2005-10-10 2006-10-09 Procede de vaporisation et de reformage de combustibles liquides

Country Status (7)

Country Link
US (1) US20080229662A1 (fr)
EP (1) EP1940737A2 (fr)
JP (1) JP2009511648A (fr)
KR (1) KR20080049811A (fr)
CA (1) CA2624762A1 (fr)
DE (1) DE102005048385A1 (fr)
WO (1) WO2007042246A2 (fr)

Cited By (1)

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DE102018204456A1 (de) 2017-11-24 2019-05-29 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Verfahren zum Betrieb eines katalytischen Verdampfers und Anwendungen des Verfahrens

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DE102010012945B4 (de) * 2010-03-26 2013-08-14 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Vorrichtung zur Verdampfung von flüssigen Kraftstoffen und brennbaren Flüssigkeiten, Verfahren zum Betreiben sowie Verwendungszwecke
US9199846B2 (en) 2010-10-05 2015-12-01 Precision Combustion, Inc. Process and apparatus for reforming a high sulfur-containing liquid fuel
DE102011100417A1 (de) * 2011-05-04 2012-11-08 Vaillant Gmbh Reformer
DE102011113699A1 (de) 2011-09-20 2013-03-21 Lurgi Gmbh Verfahren zur Herstellung von Synthesegas
DE102012204649A1 (de) * 2012-03-22 2013-09-26 Volkswagen Aktiengesellschaft Motoraggregat mit gasbetriebenen Verbrennungsmotor und Wasserstoffreformer und Verfahren zum Betreiben eines solchen Motoraggregats
TWI501462B (zh) * 2012-07-19 2015-09-21 Atomic Energy Council 可以防止產生積碳的重組器
DE102017107295A1 (de) * 2017-04-05 2018-10-11 Elringklinger Ag Reformiervorrichtung und Verfahren zum Bereitstellen eines Reformats für eine Brennstoffzellenvorrichtung
KR20210142112A (ko) 2019-03-27 2021-11-24 프라운호퍼-게젤샤프트 츄어 푀르더룽 데어 안게반텐 포르슝에.파우. 배기 가스 배출 제어 장치, 이를 구비한 내연 기관 및 배기 가스 배출 제어 방법

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WO2004000724A1 (fr) * 2002-06-20 2003-12-31 Nissan Motor Co., Ltd. Dispositif de reformage de combustible
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Publication number Priority date Publication date Assignee Title
DE102018204456A1 (de) 2017-11-24 2019-05-29 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Verfahren zum Betrieb eines katalytischen Verdampfers und Anwendungen des Verfahrens
WO2019101846A1 (fr) 2017-11-24 2019-05-31 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Procédé de fonctionnement d'un évaporateur catalytique et applications du procédé
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Also Published As

Publication number Publication date
JP2009511648A (ja) 2009-03-19
EP1940737A2 (fr) 2008-07-09
CA2624762A1 (fr) 2007-04-19
DE102005048385A1 (de) 2007-04-19
US20080229662A1 (en) 2008-09-25
KR20080049811A (ko) 2008-06-04
WO2007042246A3 (fr) 2007-07-05

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