EP1144302A1 - Cuve de reaction et procede permettant d'eliminer le monoxyde de carbone dans l'hydrogene - Google Patents

Cuve de reaction et procede permettant d'eliminer le monoxyde de carbone dans l'hydrogene

Info

Publication number
EP1144302A1
EP1144302A1 EP99956238A EP99956238A EP1144302A1 EP 1144302 A1 EP1144302 A1 EP 1144302A1 EP 99956238 A EP99956238 A EP 99956238A EP 99956238 A EP99956238 A EP 99956238A EP 1144302 A1 EP1144302 A1 EP 1144302A1
Authority
EP
European Patent Office
Prior art keywords
reactor
selective oxidation
feedstock
hydrogen
reactor according
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.)
Withdrawn
Application number
EP99956238A
Other languages
German (de)
English (en)
Inventor
Peter Geoffrey Gray
John Frederick Pignon
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.)
Johnson Matthey PLC
Original Assignee
Johnson Matthey 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 Johnson Matthey PLC filed Critical Johnson Matthey PLC
Publication of EP1144302A1 publication Critical patent/EP1144302A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/2485—Monolithic reactors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0403—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the fluid flow within the beds being predominantly horizontal
    • B01J8/0407—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds the fluid flow within the beds being predominantly horizontal through two or more cylindrical annular shaped beds
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/04—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds the fluid passing successively through two or more beds
    • B01J8/0496—Heating or cooling the reactor
    • 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
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/56—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids
    • C01B3/58—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction
    • C01B3/583—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by contacting with solids; Regeneration of used solids including a catalytic reaction the reaction being the selective oxidation of carbon monoxide
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00168—Controlling the temperature by indirect heat exchange with heat exchange elements outside the bed of solid particles
    • B01J2208/00194—Tubes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
    • B01J2208/00168—Controlling the temperature by indirect heat exchange with heat exchange elements outside the bed of solid particles
    • B01J2208/00256—Controlling the temperature by indirect heat exchange with heat exchange elements outside the bed of solid particles in a heat exchanger for the heat exchange medium separate from the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00796—Details of the reactor or of the particulate material
    • B01J2208/00823—Mixing elements
    • B01J2208/00831—Stationary elements
    • B01J2208/00849—Stationary elements outside the bed, e.g. baffles
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/18—Details relating to the spatial orientation of the reactor
    • B01J2219/182—Details relating to the spatial orientation of the reactor horizontal
    • 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
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0435—Catalytic purification
    • C01B2203/044—Selective oxidation of carbon monoxide
    • 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
    • C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
    • C01B2203/0465—Composition of the impurity
    • C01B2203/047—Composition of the impurity the impurity being carbon monoxide

Definitions

  • the present invention concerns an improved reactor, more particularly it concerns a reactor particularly adapted for and suitable for certain selective oxidation reactions.
  • the present invention provides a reactor for catalytic selective oxidation, comprising a reactor vessel with counter current cooling and at least one stage, each stage provided with an inlet for a first feedstock, e.g. CO contaminated hydrogen, an inlet for a second feedstock, e.g. oxygen-containing gas, gas mixing means and a catalytic reaction zone, preferably comprising a selective oxidation catalyst deposited on a substrate having good heat conduction properties.
  • a first feedstock e.g. CO contaminated hydrogen
  • a second feedstock e.g. oxygen-containing gas
  • gas mixing means e.g. oxygen-containing gas
  • the invention also provides a process for the removal of quantities of CO from a hydrogen feedstock by partial oxidation, comprising at least one step of admixing said feedstock with a quantity of oxygen, passing the resulting mixture over a selective oxidation catalyst in a selective oxidation zone and recovering a hydrogen product with reduced content of CO, whilst simultaneously cooling the selective oxidation zone, preferably to maintain the selective oxidation zone at a temperature in the range 100 to 250°C, by counter- current coolant flow.
  • the reactor in its most preferred embodiment, has four stages and this is effective to reduce a reformate having a CO content of 1 to 2% to below lOppm. In other embodiments, there may be 2 to 10 stages.
  • the reactor is suitably in the form of a vessel in which the reaction zones are generally annular in shape, and provided with internal and/or external liquid cooling. Cooling is preferably provided by internal cooling using water, which is suitably under pressure to prevent boiling at the temperatures generated. Other liquid coolants, or forced air cooling may be used if desired. According to specific reactor designs, heat removal may be enhanced by increasing heat exchange surface areas by corrugation or other established means. Heat removal may be altered by altering the flow of coolant and/or altering the quantity of heat removed from the coolant by means of a heat exchanger.
  • Each reaction zone suitably comprises a metallic catalyst support (“monolith”) of generally honeycomb construction, as is in common use in automobile exhaust gas catalysis. These may have 50 to 1200 cells per square in cell density, preferably 200 to 600 cpsi, and may be of a variety of types of stainless steel. In general, the present invention does not result in the reaction stages reaching the higher temperatures generally met with in exhaust gas catalysis (e.g. 500-900°C), but the material should be capable of resisting temperature excursions.
  • An alternative reaction zone design utilises what has become known as "static mixers" which combine a very high degree of gas agitation and mixing, resulting in non- laminar flow, with relatively low pressure drop. Such static mixers may be manufactured from a variety of metals and are commercially available. However, it is presently preferred to use a honeycomb monolith.
  • the reaction zone desirably carries a selective oxidation catalyst comprising a platinum group metal, especially comprising platinum and/or rhodium, carried on a high surface area metal oxide support, such as alumina.
  • a selective oxidation catalyst comprising a platinum group metal, especially comprising platinum and/or rhodium, carried on a high surface area metal oxide support, such as alumina.
  • the metallic catalyst support may be coated by generally known methods with a slurry of oxide support, dried and fired, and then impregnated with the catalytically active components, before a final firing. Such procedures are in themselves known, and do not form part of this invention.
  • An essentially cylindrical metal vessel made by pressing two halves and seam-welding, has a main gas inlet, 2, for reformate gas, and an outlet, 3, for cleaned gas.
  • the vessel has a number of annular reaction zones, 4, each consisting of an annular wound corrugated catalyst support.
  • the vessel further has an internal water jacket, 5, between a spacer and the shell and this is supplied with cooling water by means of a water circuit comprising a circulating pump, 6, and a heat exchanger, 7.
  • the heat exchanger is desirably used to recover heat in an integrated system e.g. in an integrated combined heat and power system.
  • the vessel further is provided with four air inlets, 8, each providing pre-determined (for a steady-state operation) levels of air (that is reaction oxygen; air is generally suitable).
  • controlled amounts of oxygen may be used downstream of each air inlet.
  • Zone 9a is suitably a static mixer, but zones 9b, 9c and 9d are preferably alternating annular mixing vanes, 10, and discs, 11, having gas flow holes, as illustrated in Figs 2 and 3. It should be noted that for simplicity only four vanes and four holes are shown, but more, e.g. six or eight, may be used.
  • vanes and discs may be manufactured by pressing to form a sleeve which may be fitted and brazed or welded onto the jacket 5 with the intention that each gas mixing zone also serves to remove hear from the reaction gases leaving each reaction zone.
  • each reaction zone may incorporate different and/or different loadings, of catalyst.
  • Each metal catalyst support monolith suitably has 300-400 cells per sq.in. and is coated with a washcoat comprising ⁇ 36wt% alumina solids of D50 of approx 5 ⁇ m and D90 of approx 16 ⁇ m, to deposit approx 3g/m 3 . After drying and firing, the coated monolith was impregnated with a platinum salt solution to result in 5% by wt of Pt deposited on the alumina. The resulting coated monolith was again dried and fired before being assembled into the reactor.
  • the reactor of the invention is compact and exhibits relatively low pressure drop. Manufacturing costs are relatively low.
  • the reactor is believed to be suitable for mobile or automobile uses as well as stationery uses. It is presently envisaged that the reactor shell will be lagged to control heat loss and prevent injury.
  • the reactor can be manufactured simply and inexpensively, using pressed and welded parts. It is desirably operated to achieve low pressure drop, and the particular embodiment illustrated is designed for a gas hourly space velocity of approx. 30,000h " ' gas throughput.
  • the reactor as described may be altered in a variety of ways without departing from the central inventive concept.
  • the invention is now illustrated below in a working example of a two-stage reactor, fed with a synthetic reformate gas mixture containing N 2 , H 2 , CO, CO 2 and H O.
  • Each of the two stages consists of a mixing zone with three off-set spiral vanes, followed by air injection accomplished through a number of apertures in an annular ring, producing a swirling, mixing gas.
  • the thus mixed hydrogen and air mixture passes through an annular metal honeycomb support mounted on a central cooling jacket.
  • the cooling jacket is fed counter-current to the flow of hydrogen with a heat transfer fluid, conveniently water under pressure, and the metal honeycomb support is mounted in good heat exchange contact with the cooling jacket.
  • the metal honeycomb carries a selective oxidation catalyst.
  • Gas may be extracted for analysis between the two stages and/or after the second stage.
  • the test two-stage reactor can model a three or four stage reactor.
  • the detailed operating conditions and other experimental detail for one typical run of the above reactor now follow. It was remarkable that the pressure drop across the whole of the est reactor was about the measurement limit of the gauges being used, and was of the order of 1.5-3mbar (150-300Pa), at the two throughputs tested. This indicates that the reactor is very efficient, compact and requires very little energy to operate.
  • Each catalyst support was an annular of internal diameter 3.85in (9.78cm), external diameter 5.85in (14,86cm) and 3.0in(7.62cm) length, made from "Fecralloy" steel and having 500 cells per sq in.
  • Each support had been washcoated with alumina washcoat as used in exhaust gas catalytic convertors, followed by loading with 5% by wt of the alumina of Pt. Conventional manufacturing techniques were used.
  • the synthetic reformate had the compositions: 48%N 2 (dry), 40%H 2 (dry), 10%CO 2 (dry), 0.5-1.5%CO (dry) and 13% H 2 O (of total flow).

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Fluid Mechanics (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)
  • Industrial Gases (AREA)

Abstract

L'invention concerne une cuve de réaction (1) à un ou plusieurs étages d'oxydation sélective, avec refroidissement en contre-courant (5, 6, 7), chaque étage ayant une admission pour charge du type hydrogène contaminé par CO (2), une admission pour seconde charge du type oxygène ou air (8) un système de mélange de gaz (9a, 9b) et une zone de réaction catalytique (4), renfermant de préférence un support métallique à catalyseur d'oxydation sélective. Ce type de reformeur compact à chute de pression très basse est approprié à la production d'hydrogène pour une pile à combustible.
EP99956238A 1998-12-01 1999-11-29 Cuve de reaction et procede permettant d'eliminer le monoxyde de carbone dans l'hydrogene Withdrawn EP1144302A1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
GB9826222 1998-12-01
GBGB9826222.3A GB9826222D0 (en) 1998-12-01 1998-12-01 Improved reactor
PCT/GB1999/003958 WO2000032513A1 (fr) 1998-12-01 1999-11-29 Cuve de reaction et procede permettant d'eliminer le monoxyde de carbone dans l'hydrogene

Publications (1)

Publication Number Publication Date
EP1144302A1 true EP1144302A1 (fr) 2001-10-17

Family

ID=10843323

Family Applications (1)

Application Number Title Priority Date Filing Date
EP99956238A Withdrawn EP1144302A1 (fr) 1998-12-01 1999-11-29 Cuve de reaction et procede permettant d'eliminer le monoxyde de carbone dans l'hydrogene

Country Status (5)

Country Link
EP (1) EP1144302A1 (fr)
JP (1) JP2002531247A (fr)
CA (1) CA2352776A1 (fr)
GB (1) GB9826222D0 (fr)
WO (1) WO2000032513A1 (fr)

Families Citing this family (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE10240953A1 (de) * 2002-09-02 2004-03-18 Viessmann Werke Gmbh & Co Kg Apparat zur Erzeugung von Wasserstoff
JP4641115B2 (ja) * 2001-03-30 2011-03-02 東京瓦斯株式会社 Ｃｏ除去器
JP4929548B2 (ja) * 2001-09-10 2012-05-09 トヨタ自動車株式会社 改質ガスの流路交換装置またはガス混合部を備えた燃料改質装置
US20030086852A1 (en) * 2001-10-15 2003-05-08 Ballard Generation Systems Inc. Apparatus for the selective oxidation of carbon monoxide in a hydrogen-containing gas mixture
JP3815355B2 (ja) 2002-03-27 2006-08-30 日産自動車株式会社 燃料電池システム
JP5047548B2 (ja) 2006-07-06 2012-10-10 ユニ・チャーム株式会社 着用物品の止着構造
US8398731B2 (en) 2008-05-30 2013-03-19 Panasonic Corporation Fuel treatment device with gas supply and diffusion regions
ES2431491B1 (es) * 2013-08-07 2014-09-29 Abengoa Hidrógeno, S.A. Reactor de oxidación preferencial de monóxido de carbono
US11883810B2 (en) 2017-06-27 2024-01-30 Syzygy Plasmonics Inc. Photocatalytic reactor cell

Family Cites Families (6)

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Publication number Priority date Publication date Assignee Title
GB2075859A (en) * 1980-04-29 1981-11-25 Humphreys & Glasgow Ltd Catalytic reactor with internal heat exchanger
DE3631642A1 (de) * 1986-09-17 1988-04-07 Linde Ag Verfahren zur durchfuehrung katalytischer reaktionen
DK156701C (da) * 1987-08-27 1990-01-29 Haldor Topsoe As Fremgangsmaade til gennemfoerelse af heterogene katalytiske kemiske reaktioner
EP0873967B1 (fr) * 1992-03-19 2003-08-20 International Fuel Cells Corporation Procédé et dispositif pour éliminer l'oxyde de carbone contenu dans les gaz
DE4334981C2 (de) * 1993-10-14 1998-02-26 Daimler Benz Ag Verwendung eines Reaktors zur katalytischen Entfernung von CO in H¶2¶-reichem Gas
DE19544895C1 (de) * 1995-12-01 1997-02-27 Daimler Benz Ag Verfahren und Vorrichtung zur selektiven katalytischen Oxidation von Kohlenmonoxid

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO0032513A1 *

Also Published As

Publication number Publication date
JP2002531247A (ja) 2002-09-24
WO2000032513A1 (fr) 2000-06-08
GB9826222D0 (en) 1999-01-20
CA2352776A1 (fr) 2000-06-08

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