DE1174861B - Process for the production of catalyst electrodes for fuel and air oxygen elements - Google Patents
Process for the production of catalyst electrodes for fuel and air oxygen elementsInfo
- Publication number
- DE1174861B DE1174861B DEA35088A DEA0035088A DE1174861B DE 1174861 B DE1174861 B DE 1174861B DE A35088 A DEA35088 A DE A35088A DE A0035088 A DEA0035088 A DE A0035088A DE 1174861 B DE1174861 B DE 1174861B
- Authority
- DE
- Germany
- Prior art keywords
- compounds
- fuel
- catalytically active
- active metals
- production
- 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
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Classifications
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- 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
- H01M4/88—Processes of manufacture
- H01M4/8875—Methods for shaping the electrode into free-standing bodies, like sheets, films or grids, e.g. moulding, hot-pressing, casting without support, extrusion without support
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- 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
- B01J37/00—Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
- B01J37/08—Heat treatment
- B01J37/082—Decomposition and pyrolysis
-
- 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
- H01M4/88—Processes of manufacture
- H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
- H01M4/8882—Heat treatment, e.g. drying, baking
-
- 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
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
-
- 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
- H01M4/9041—Metals or alloys
-
- 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
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
- H01M2004/8684—Negative electrodes
-
- 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
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
- H01M2004/8689—Positive electrodes
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M2300/00—Electrolytes
- H01M2300/0002—Aqueous electrolytes
- H01M2300/0014—Alkaline electrolytes
-
- 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)
- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Physics & Mathematics (AREA)
- Thermal Sciences (AREA)
- Organic Chemistry (AREA)
- Inert Electrodes (AREA)
- Catalysts (AREA)
Description
DEUTSCHESGERMAN
PATENTAMTPATENT OFFICE
AUSLEGESCHRIFTEDITORIAL
Internat. Kl.: H Ol raBoarding school Kl .: H Ol ra
Deutsche Kl.: 21b-14/01 German class: 21b -14/01
Nummer: 1174 861Number: 1174 861
Aktenzeichen: A35088VIb/21bFile number: A35088VIb / 21b
Anmeldetag: 9. Juli 1960 Filing date: July 9, 1960
Auslegetag: 30. Juli 1964Opening day: July 30, 1964
Die vorliegende Erfindung betrifft ein Verfahren zur Herstellung von Katalysatorelektroden, die sich zur Verwendung in Brennstoff- und Luftsauerstoffelementen eignen.The present invention relates to a method for producing catalyst electrodes, which suitable for use in fuel and atmospheric oxygen elements.
Derartige Elektroden sind an sich bekannt. Im allgemeinen bestehen sie aus einem porösen Körper, beispielsweise aus Kohle oder einem gesinterten Metallpulver. Zur Erhöhung der katalytischen Wirksamkeit der Elektroden ist schon vielfach der Weg beschriften worden, diese porösen Körper mit katalytisch aktivem Metall zu imprägnieren. Dabei ist es jedoch immer erforderlich, eine ganze Reihe von Arbeitsgängen nacheinander vorzunehmen, so daß sich die Herstellung hochbelastbarer Katalysatorelektroden bisher stets als sehr kostspielig und als mit hohem Zeitaufwand verbunden erwiesen hat. Dies gilt insbesondere auch für Elektroden, deren aktiver Bestandteil aus einem Raney-Katalysator besteht, da die inaktive Ausgangslegierung durch Behandlung mit Alkalilaugen aktiviert werden muß.Such electrodes are known per se. Generally they consist of a porous body, for example from coal or a sintered metal powder. To increase the catalytic effectiveness The way of electrodes has already been marked many times, these porous bodies with catalytic impregnate active metal. However, it is always necessary to do a number of To carry out operations one after the other, so that the production of heavy-duty catalyst electrodes has always proven to be very costly and time-consuming. this applies in particular to electrodes whose active component consists of a Raney catalyst, since the inactive starting alloy must be activated by treatment with alkaline solutions.
Es war daher Aufgabe der vorliegenden Erfindung,1 hier Abhilfe zu schaffen und ein einfaches Verfahren zu finden, mit dessen Hilfe sich Katalysatorelektroden für Brennstoff- und Luftsauerstoffelemente herstellen lassen.It is an object of the present invention, 1 to remedy this situation and to find a simple method which can be produced catalyst electrodes for fuel and oxygen elements which helps.
Gemäß der Erfindung wird diese Aufgabe dadurch gelöst, daß aus einer oder einem Gemisch mehrerer leicht zersetzlicher Verbindungen eines oder mehrerer katalytisch aktiver Metalle ein fester Körper gepreßt wird, worauf die Verbindungen bei einer Temperatur unterhalb des Schmelzpunktes der betreffenden Metalle in sauerstofffreier Atmosphäre zersetzt werden.According to the invention, this object is achieved in that from one or a mixture of several easily decomposable compounds of one or more catalytically active metals pressed into a solid body whereupon the compounds at a temperature below the melting point of the relevant Metals are decomposed in an oxygen-free atmosphere.
Als besonders geeignete Ausgangsmaterialien für das erfindungsgemäße Verfahren haben sich durch Temperaturerhöhung leicht zersetzliche anorganische Verbindungen, wie z. B. die Oxyde, Hydroxyde, Nitrate und Carbonate, katalytisch aktiver Metalle erwiesen. Mit Vorteil lassen sich weiterhin eine Reihe organischer Verbindungen katalytisch aktiver Metalle, wie z. B. die Salze organischer Säuren oder metallorganische Verbindungen, verwenden.Particularly suitable starting materials for the process according to the invention have proven to be Increase in temperature easily decomposable inorganic compounds such. B. the oxides, hydroxides, Nitrates and carbonates, proven catalytically active metals. A number can still be advantageously used organic compounds of catalytically active metals, such as. B. the salts of organic acids or organometallic Connections, use.
Die Zersetzung aller dieser Verbindungen erfolgt mit besonderem Vorteil in einer reinen Wasserstoffatmosphäre. Dabei lagert sich in erheblichem Maße Wasserstoff in die Fehlstellen des Gitters der katalytisch aktiven Metalle ein, so daß die fertigen Sinterkörper eine besonders hohe katalytische Aktivität aufweisen.The decomposition of all these compounds takes place with particular advantage in a pure hydrogen atmosphere. A considerable amount of hydrogen is stored in the flaws in the lattice of the catalytic system active metals, so that the finished sintered body has a particularly high catalytic activity exhibit.
Als katalytisch aktive Metalle kommen für das erfindungsgemäße Verfahren insbesondere Silber und Nickel in Betracht.Suitable catalytically active metals for the process according to the invention are in particular silver and Nickel into consideration.
Verfahren zur Herstellung von Katalysatorelektroden für Brennstoff- und Luftsauerstoffelemente Process for the production of catalyst electrodes for fuel and atmospheric oxygen elements
Anmelder:Applicant:
Varta Aktiengesellschaft,
Hagen (Westf.), Dieckstr. 42Varta Aktiengesellschaft,
Hagen (Westphalia), Dieckstr. 42
Als Erfinder benannt:Named as inventor:
Margarete Jung, Nieder-Eschbach,Margarete Jung, Nieder-Eschbach,
Dipl.-Chem. Dr. Hanns H. Kroger, Frankfurt/M.Dipl.-Chem. Dr. Hanns H. Kroger, Frankfurt / M.
Nachstehend seien noch einige Ausführungsbeispiele für das erfindungsgemäße Verfahren im einzelnen beschrieben.A few more detailed examples of the method according to the invention are given below described.
Aus Nickelcarbonat wurden in einer Matrize bei einem Druck von 200 kg/cm2 Tabletten der Abmessungen von 20 mm Durchmesser und einer Dicke von 5 mm hergestellt. Bei einer Temperatur von 275° C wurden die Preßkörper im Wasserstoff strom zu metallischem Nickel reduziert. Nach dieser Reduktion waren die Körper so stark pyrophor, daß das Einbringen in stromableitende Halterungen nur unter Verwendung von Schutzgas bzw. in angefeuchtetem Zustande durchzuführen war.From nickel carbonate, tablets with a diameter of 20 mm and a thickness of 5 mm were produced in a die at a pressure of 200 kg / cm 2. At a temperature of 275 ° C, the compacts were reduced to metallic nickel in a stream of hydrogen. After this reduction, the bodies were so strongly pyrophoric that they could only be introduced into current-dissipating holders using protective gas or in a moistened state.
Diese Körper wurden als negative Elektroden in Knallgas-Brennstoffzellen eingebaut und hatten bei einer Dauerbelastung von 100 mA/cm2 eine vom reversiblen Wasserstoffpotential nur unwesentlich abweichende Spannungslage.These bodies were installed as negative electrodes in oxyhydrogen fuel cells and, when subjected to a continuous load of 100 mA / cm 2, had a voltage level that deviated only insignificantly from the reversible hydrogen potential.
Aus Silberoxyd wurden bei einem Druck von 250 kg/cm2 Formkörper von 20 mm Durchmesser und 4 mm Dicke kalt gepreßt. Sodann wurden die Körper bei 500° C im Wasserstoff strom leicht gesintert. Nach Abkühlung auf Zimmertemperatur und Einbau in eine stromableitende Halterung, die gleichzeitig zur Sauerstoffzufuhr dient, wurde die Elektrode in Alkalilauge durch eine anodische Belastung von 5 mA/cm2 partiell wieder oxydiert.Moldings 20 mm in diameter and 4 mm thick were cold-pressed from silver oxide at a pressure of 250 kg / cm 2. The bodies were then lightly sintered at 500 ° C. in a stream of hydrogen. After cooling to room temperature and installation in a current-conducting holder, which also serves to supply oxygen, the electrode was partially re-oxidized in alkali metal by an anodic load of 5 mA / cm 2.
Bei anschließendem Einsatz als positive Elektrode in einer Brennstoffzelle zeigte das Material bei einer Belastung von 100 mA/cm2 ein Potential von — 150 mV gegen eine gesättigte Kalomelelektrode.When subsequently used as a positive electrode in a fuel cell, the material showed a potential of −150 mV against a saturated calomel electrode at a load of 100 mA / cm 2.
'■''':''r'° 409 638/106'■''' : '' r '° 409 638/106
Aus einem innigen Gemisch von 25 Gewichtsteilen Nickelformiat und 1 Gewichtsteil Kaliumpalladium(II)-chlorid wurden unter einem Druck von 280 kg/cm2 Scheiben mit einem Radius von 2 cm und einer Stärke von 3,5 mm gepreßt und bei 350° C einem Wasserstoffstrom ausgesetzt.From an intimate mixture of 25 parts by weight of nickel formate and 1 part by weight of potassium palladium (II) chloride, discs with a radius of 2 cm and a thickness of 3.5 mm were pressed under a pressure of 280 kg / cm 2 and a stream of hydrogen at 350 ° C exposed.
Als Wasserstoffelektrode in einer Halbzellenschaltung wies sie bei Zimmertemperatur und einer Belastung von 100 mA/cm2 ein um 110 mV vom reversiblen Wasserstoffpotential abweichendes Potential auf.As a hydrogen electrode in a half-cell circuit, it had a potential deviating from the reversible hydrogen potential by 110 mV at room temperature and a load of 100 mA / cm 2.
40 Gewichtsteile frisch gefälltes Nickelhydroxyd, 10 Gewichtsteile Silberoxalat und 1 Gewichtsteil Kaliumosmat wurden gut miteinander vermischt und aus dem erhaltenen Pulver durch Pressen unter einem Druck von 320 kg/cm2 Scheiben mit einem Durchmesser von 4 cm und einer Stärke von 4 mm hergestellt. Eine Scheibe wurde nach dem Erhitzen auf 260° C 50 Minuten lang im Wasserstoffstrom belassen und nach dem Abkühlen als Sauerstoffelektrode in eine Brennstoffzellen-Elektrodenhalterung eingebaut.40 parts by weight of freshly precipitated nickel hydroxide, 10 parts by weight of silver oxalate and 1 part by weight of potassium osmate were mixed well and disks with a diameter of 4 cm and a thickness of 4 mm were produced from the powder obtained by pressing under a pressure of 320 kg / cm 2. After heating to 260 ° C., a disk was left in a stream of hydrogen for 50 minutes and, after cooling, was installed as an oxygen electrode in a fuel cell electrode holder.
Als Wasserstoffelektrode diente eine Scheibe mit gleichen Abmessungen, deren Ausgangsmaterial aus 10 Gewichtsteilen Nickelnitrat, 10 Gewichtsteilen Kupferphenyl und 1 Gewichtsteil Platindiamminnitrit bestand. Die Wärmebehandlung des Preßlings erfolgte bei 270° C im Kohlenmonoxydstrom für 70 Minuten.A disk with the same dimensions, the starting material of which was used, served as the hydrogen electrode 10 parts by weight of nickel nitrate, 10 parts by weight of copper phenyl and 1 part by weight of platinum diamine nitrite duration. The compact was heat treated at 270 ° C. in a stream of carbon monoxide for 70 minutes.
Das mit den beschriebenen Elektroden ausgerüstete Brennstoffelement lieferte bei einer Belastung von 50 mA/cm2 und Zimmertemperatur im Dauerbetrieb eine Spannung von 0,84 V.The fuel element equipped with the electrodes described delivered a voltage of 0.84 V in continuous operation at a load of 50 mA / cm 2 and room temperature.
Claims (4)
Deutsche Auslegeschriften Nr. 1 019 361,
099;Considered publications:
German Auslegeschrift No. 1 019 361,
099;
Priority Applications (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
NL266573D NL266573A (en) | 1960-07-09 | ||
DEA35088A DE1174861B (en) | 1960-07-09 | 1960-07-09 | Process for the production of catalyst electrodes for fuel and air oxygen elements |
GB23805/61A GB985900A (en) | 1960-07-09 | 1961-06-30 | Catalyst electrodes for fuel cells |
FR867554A FR1315033A (en) | 1960-07-09 | 1961-07-10 | Process for preparing catalysts, in particular for fuel cells, electrodes and cells conforming to those obtained |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DEA35088A DE1174861B (en) | 1960-07-09 | 1960-07-09 | Process for the production of catalyst electrodes for fuel and air oxygen elements |
Publications (1)
Publication Number | Publication Date |
---|---|
DE1174861B true DE1174861B (en) | 1964-07-30 |
Family
ID=6928841
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
DEA35088A Pending DE1174861B (en) | 1960-07-09 | 1960-07-09 | Process for the production of catalyst electrodes for fuel and air oxygen elements |
Country Status (3)
Country | Link |
---|---|
DE (1) | DE1174861B (en) |
GB (1) | GB985900A (en) |
NL (1) | NL266573A (en) |
Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE15620C (en) * | F. WINDHAUSEN in Berlin, Chausseestrafse 38 | Steam water lifter with float piston | ||
DE14941C (en) * | M. MERKELBACH in Grenzhausen bei Coblenz | Clay pots with transparent walls | ||
DE1019361B (en) * | 1954-10-23 | 1957-11-14 | Ruhrchemie Ag | Double skeleton catalyst electrode |
DE1023099B (en) * | 1955-12-29 | 1958-01-23 | Nat Res Dev | Fuel element |
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0
- NL NL266573D patent/NL266573A/xx unknown
-
1960
- 1960-07-09 DE DEA35088A patent/DE1174861B/en active Pending
-
1961
- 1961-06-30 GB GB23805/61A patent/GB985900A/en not_active Expired
Patent Citations (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE15620C (en) * | F. WINDHAUSEN in Berlin, Chausseestrafse 38 | Steam water lifter with float piston | ||
DE14941C (en) * | M. MERKELBACH in Grenzhausen bei Coblenz | Clay pots with transparent walls | ||
DE1019361B (en) * | 1954-10-23 | 1957-11-14 | Ruhrchemie Ag | Double skeleton catalyst electrode |
DE1023099B (en) * | 1955-12-29 | 1958-01-23 | Nat Res Dev | Fuel element |
Also Published As
Publication number | Publication date |
---|---|
NL266573A (en) | |
GB985900A (en) | 1965-03-10 |
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