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DE1916340A1 - Tungsten carbide for fuel cells - Google Patents

Tungsten carbide for fuel cells

Info

Publication number
DE1916340A1
DE1916340A1 DE19691916340 DE1916340A DE1916340A1 DE 1916340 A1 DE1916340 A1 DE 1916340A1 DE 19691916340 DE19691916340 DE 19691916340 DE 1916340 A DE1916340 A DE 1916340A DE 1916340 A1 DE1916340 A1 DE 1916340A1
Authority
DE
Germany
Prior art keywords
tungsten
tungsten carbide
fuel cells
carbon monoxide
elevated temperature
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.)
Pending
Application number
DE19691916340
Other languages
German (de)
Inventor
Dieter Baganz
Harald Dr Boehm
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.)
Licentia Patent Verwaltungs GmbH
Original Assignee
Licentia Patent Verwaltungs GmbH
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 Licentia Patent Verwaltungs GmbH filed Critical Licentia Patent Verwaltungs GmbH
Priority to DE19691916340 priority Critical patent/DE1916340A1/en
Publication of DE1916340A1 publication Critical patent/DE1916340A1/en
Pending legal-status Critical Current

Links

Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • 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
    • B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
    • B01J27/20—Carbon compounds
    • B01J27/22—Carbides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/90—Carbides
    • C01B32/914—Carbides of single elements
    • C01B32/949—Tungsten or molybdenum carbides
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/51—Particles with a specific particle size distribution
    • C01P2004/52—Particles with a specific particle size distribution highly monodisperse size distribution
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/60—Particles characterised by their size
    • C01P2004/62—Submicrometer sized, i.e. from 0.1-1 micrometer
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/21—Attrition-index or crushing strength of granulates
    • 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
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Landscapes

  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Inert Electrodes (AREA)
  • Catalysts (AREA)

Abstract

This is prepared by carburising tungsten or tungsten oxide with carbon monoxide at elevated temperature. The carbon monoxide may be mixed with carbon dioxide preferably 0.1-60%. Suitable temperatures are between 600 and 1500 degrees C. Tungsten carbide electrodes are suitable for use in fuel cells with acid electrolytes, particularly for the oxidation of hydrogen or carbon monoxide.

Description

Verfahren zur Herstellung eines Wolfraicarbidkatalysator für Brennstoffsellen Bei Brennstoffzellen mit saurem Elektrolyten wird zur anodischen Oxydation von Wasserstoff z0B. Wolframcarbid als Katalysator eingesetzt. Zur Herstellung von porösen Gasdiffusionselektroden wird Wolframcarbid kleiner Korngröße in einem thermoplastischen Kunststoff eingelagert. Die Herstellung des Wolframcarbide selbst kann nach verschiedenen Verfahren erfolgen. Es ist s.B. Process for the production of a Wolfraicarbidkatalysator for fuel cells In fuel cells with acidic electrolytes, hydrogen is anodically oxidized z0B. Tungsten carbide used as a catalyst. For the production of porous gas diffusion electrodes Tungsten carbide with a small grain size is embedded in a thermoplastic material. The tungsten carbide itself can be produced by various methods. It's s.B.

bekannt, Wolframcarbid durch Reaktion von litivkohle mit Wolframpulver oder pulverförmigen Wolframoxiden zu erzeugen, oder die vorgenannten Ausgangsstoffe mit Kohlenwassestoff zu carburieren.known, tungsten carbide through the reaction of litive carbon with tungsten powder or powdered tungsten oxides generate, or the aforementioned Carburizing starting materials with hydrocarbons.

Die bei dem genannten Verfahren erzielbare katalytische Aktivität reicht Jedoch für einen wirtschaftlichen Einsatz in Brennstoffzellen nicht aus.The catalytic activity that can be achieved in the process mentioned However, it is not sufficient for economic use in fuel cells.

Der Erfindung liegt daher die Aufgabe zugrunde, ein Verfahren zur Herstellung von Wolframcarbid anzugeben, das die für einen wirtschaftlichen Einsatz notwendige Aktivität aufweist.The invention is therefore based on the object of a method for Manufacture of tungsten carbide to indicate which is the most economical use has necessary activity.

Es wurde nun überraschend gefunden, daß diese Auf gabe dadurch gelöst wird, daß Wolfram oder Wolframoxid bei erhöhter Temperatur mit Kohlenmonoxid carburiert wird.It has now been found, surprisingly, that this task is solved is that tungsten or tungsten oxide carburized with carbon monoxide at an elevated temperature will.

In einer Abwandlung des Verfahrens werden die genannten Ausgangsstoffe bei erhöhter Temperatur mit einem Gemisch aus Kohlenmonoxid mit Kohlendioxid behandelt. Be sonders günstige Ergebnisse werden dabei mit einem Gasgemisch erzielt, daß 0,1 bis 60 56 Kohlendioxid enthält. Die Carburierung erfolgt vorteilhaft bei einer Temperatur im Bereich von 600 bis 15000 a, wobei bei Behandlungszeiten von 4 bis 16 Stunden als ausreichend und notwendig anzusehen sind.In a modification of the process, the starting materials mentioned treated at elevated temperature with a mixture of carbon monoxide with carbon dioxide. Be particularly favorable results are achieved with a gas mixture that 0.1 contains up to 60 56 carbon dioxide. The carburization is advantageously carried out at one temperature in the range from 600 to 15000 a, with treatment times of 4 to 16 hours are to be regarded as sufficient and necessary.

Zur Durchführung des Verfahrens wird das Ausgangsmaterial, z. B. pulverförmiges Wolfram, in einen Drehrohrofen mit z.B. Kohlenmonoxid carburiert. Die Behandlungszeit richtet sich nach der Korngröße des Ausgangsmaterials. Bei einer Korngröße von 0, 3 ist bei einer Temperatur von 700° C zur vollständigen Carburierung eine Behandlungszeit von 7 bis 10 Stunden notwending.To carry out the process, the starting material, e.g. B. powdery Tungsten, carburized in a rotary kiln with e.g. carbon monoxide. The treatment time depends on the grain size of the starting material. With a grain size of 0, 3 is a treatment time at a temperature of 700 ° C for complete carburization from 7 to 10 hours necessary.

Durch die ständige Umwäl ung in dem Drohrohrofen wird ein homogenes Endprodukt erzielt, daß ohne weitere Aktivierung nach bekannten Verfahren zu Gasdiffusions elektroden verarbeitet werden kann.The constant circulation in the tubular furnace makes it homogeneous End product achieved that without further activation by known methods to gas diffusion electrodes can be processed.

In der Figur sind 3 Stromspannungskurven dargestellt, wie sie sich in einer Brennstoffzelle bei der anodischen Oxydation von Wasserstof an einer Gasdiffusionselektrode aus Wolframcarbid ergeben. Während die Kurven 1 und 2 an naoh bekannten Verfahren hergestellten Wolframcarbidelektroden erhalten wurden, gibt die Stromspannungscharakteristik der Kurve 3 den Verlauf wieder, der mit einer Gasdiffusionselektrode unter Verwendung von Wolfra.cartid gemäß der Erfinduiag erhalten wurde.In the figure, 3 current-voltage curves are shown as they are in a fuel cell during the anodic oxidation of hydrogen on a gas diffusion electrode from tungsten carbide. While curves 1 and 2 are based on well-known processes manufactured tungsten carbide electrodes were obtained, gives the voltage characteristic the curve 3 shows the course again, using a gas diffusion electrode from Wolfra.cartid according to the invention.

Aus der Figur ist ohne weiteres die Fortschrittlichkeit des Verfahrens gemäß der Erfindung bezüglich der erhöhten katalyischen Aktivität zu entnehmen.The progressiveness of the process is readily apparent from the figure to be found according to the invention with respect to the increased catalytic activity.

Gasdiffusionselektroden aus Wolframcarbid gemäß der Erfindung werden besonders vorteilhaft in Brennstoffzellen mit saurem Elektrolyten eingesetzt, wobei als Brennstoff bevorzugt Wasserstoff oder Kohlenmonoxid oxydiert wird.Tungsten carbide gas diffusion electrodes according to the invention used particularly advantageously in fuel cells with acidic electrolytes, wherein hydrogen or carbon monoxide is preferably oxidized as fuel.

Claims (6)

P a t e n t a n s p r ü c h eP a t e n t a n s p r ü c h e 1. Verfahren zur Herstellung von Wolframcarbid als Katalysator für Brennstoffzellen, d a d u r c h g e k e n n z e i c h n e t, daß Wolfram oder Wolframoxid bei erhöhter Temperatur mit Kohlenmonoxid carburiert wird.1. Process for the production of tungsten carbide as a catalyst for Fuel cells, noting that tungsten or tungsten oxide is carburized with carbon monoxide at an elevated temperature. 2. Verfahren zur Herstellung von Wolframcarbid als Katalysator für Brennstoffzellen, d a d u r c h g e k e n n z-e i c h n e t, daß Wolfram oder Wolframoxid bei erhöhter Temperatur mit einem Gemilch aus Kohlenmonoxid und Kohlendioxid carburiert wird.2. Process for the production of tungsten carbide as a catalyst for Fuel cells, d u r g e k e n n n z-e i c h n e t, that tungsten or tungsten oxide carburized at elevated temperature with a milk made from carbon monoxide and carbon dioxide will. 3. Verfahren nach Anspruch 2, d a d u r ch g ek e n n z e i c h n e t, daß in dem Gasgemisch 0,1 bis 60 % Kohlendioxid enthalten ist.3. The method according to claim 2, d a d u r ch g ek e n n z e i c h n e t that the gas mixture contains 0.1 to 60% carbon dioxide. 4. Verfahren nach den Ansprächen 1 bis 3, dad u r c h g e k e n n z e i c h n e t, daß die Carburierung bei einer Temperatur im Bereich von 600 bis 1500 0C erfolgt.4. The method according to claims 1 to 3, dad u r c h e k e n n indicates that the carburization takes place at a temperature in the range of 600 to 1500 0C takes place. 5. Wolframcarbid nach den Ansprüchen 1 bis 4, g ek e n n z e i c h n e t durch seine Verwendung als Elektrode in einer Brennstoffzelle mit saurem Elektrolyt.5. tungsten carbide according to claims 1 to 4, g ek e n n z e i c h n e t through its use as an electrode in a fuel cell with acidic electrolyte. 6. Wolframcarbid nach den Ansprüchen 1 bis 5, g ek e n n z e i c h n e t durch seine Verwendung zur Oxydation von Wasserstoff oder Kohlenmonoxid.6. tungsten carbide according to claims 1 to 5, g ek e n n z e i c h n e t through its use to oxidize hydrogen or carbon monoxide. LeerseiteBlank page
DE19691916340 1969-03-29 1969-03-29 Tungsten carbide for fuel cells Pending DE1916340A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
DE19691916340 DE1916340A1 (en) 1969-03-29 1969-03-29 Tungsten carbide for fuel cells

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
DE19691916340 DE1916340A1 (en) 1969-03-29 1969-03-29 Tungsten carbide for fuel cells

Publications (1)

Publication Number Publication Date
DE1916340A1 true DE1916340A1 (en) 1971-04-08

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
DE19691916340 Pending DE1916340A1 (en) 1969-03-29 1969-03-29 Tungsten carbide for fuel cells

Country Status (1)

Country Link
DE (1) DE1916340A1 (en)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1293721B (en) * 1966-09-01 1969-04-30 Brandes Emil Device for pressing stored documents onto the base of an upright letter folder
FR2384542A1 (en) * 1977-03-25 1978-10-20 Licentia Gmbh PROCESS FOR PREPARING A TUNGSTENE CARBIDE CATALYST
DE3814112A1 (en) * 1987-08-13 1989-02-23 Ts Lab Elektrochimitscheski Is Device for the recombination of hydrogen and oxygen separating out in lead-acid batteries
WO2000029325A1 (en) * 1998-11-13 2000-05-25 H.C. Starck Gmbh & Co. Kg Method for producing wolfram carbides by gas-phase carburetion

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1293721B (en) * 1966-09-01 1969-04-30 Brandes Emil Device for pressing stored documents onto the base of an upright letter folder
US4172808A (en) * 1977-03-24 1979-10-30 Licentia Patent-Verwaltungs-G.M.B.H. Process for the production of a tungsten carbide catalyst by carburization of tungsten oxides
FR2384542A1 (en) * 1977-03-25 1978-10-20 Licentia Gmbh PROCESS FOR PREPARING A TUNGSTENE CARBIDE CATALYST
DE3814112A1 (en) * 1987-08-13 1989-02-23 Ts Lab Elektrochimitscheski Is Device for the recombination of hydrogen and oxygen separating out in lead-acid batteries
WO2000029325A1 (en) * 1998-11-13 2000-05-25 H.C. Starck Gmbh & Co. Kg Method for producing wolfram carbides by gas-phase carburetion
US7118635B1 (en) 1998-11-13 2006-10-10 H. C. Starck Gmbh & Co. Kg Method for producing tungsten carbides by gas-phase carburization

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