EP0021456A1 - Electrode for the electrolysis of water - Google Patents
Electrode for the electrolysis of water Download PDFInfo
- Publication number
- EP0021456A1 EP0021456A1 EP80200266A EP80200266A EP0021456A1 EP 0021456 A1 EP0021456 A1 EP 0021456A1 EP 80200266 A EP80200266 A EP 80200266A EP 80200266 A EP80200266 A EP 80200266A EP 0021456 A1 EP0021456 A1 EP 0021456A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- surface layer
- electrode
- mol
- titanium
- catalyst
- 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.)
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- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
- C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
- C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
- C25B11/091—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds
- C25B11/093—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of at least one catalytic element and at least one catalytic compound; consisting of two or more catalytic elements or catalytic compounds at least one noble metal or noble metal oxide and at least one non-noble metal oxide
Definitions
- the invention relates to an electrode according to the preamble of claim 1.
- Electrodes and processes for their production are known primarily from the technology developed for fuel cells (e.g. Carl Berger, Handbook of Fuel Cell Technology pp. 401-406, Prentice Hall 1968; HA Liebhafsky and EJ Cairns, Fuel Cells and Fuel Batteries, p 289-294, John Wiley & Sons, 1968).
- the requirement for precisely defined reaction zones requires a multilayer structure and special treatment processes for such fuel cell electrodes.
- the structure of the electrodes described above is too complicated for water decomposition and their manufacturing methods are too complex and costly. This applies in particular with regard to manufacturing methods for large industrial plants for the economical production of hydrogen.
- Electrodes for water decomposition cells have already been proposed (eg US Pat. No. 4,039,409). To accelerate the electrochemical reactions, they are usually used with kata dysers doped.
- the described electrodes leave something to be desired in terms of their mechanical and chemical properties. The same applies to the catalysts used.
- the invention has for its object to provide an electrode for water electrolysis, which with good mechanical and chemical stability, high electrical conductivity and good permeability to water and gas has a long life and the property to catalytically accelerate the water decomposition reaction in an optimal manner.
- the figure shows
- the shape of the plate 1 can be circular, square, rectangular, hexagonal or octagonal.
- this surface layer 3 is large thanks to local oxidation; Part made of titanium, the smaller one made of titanium dioxide. As a result, the underlying carbon (graphite) of the plate 1 is effectively protected against corrosive attack (oxidation by the formation of oxygen).
- the plate 1 prepared in this way was now immersed in an alcoholic solution for 10 sec. Wt .-% ruthenium chloride (RuCl3) and 85 rel. Wt .-% iridium chloride (IrCl 3 ) contained. After draining for 1 min, plate 1 was oxidized in air for 10 min at a temperature of 375 ° C. This immersion and oxidizing process was repeated 5 times in total. Finally, plate 1 was oxidized again in air for 4 h at a temperature of 375 ° C. In this way, the catalyst doping 4 consisting of approximately 20 mol% ruthenium oxide (Ru0 2 ) and 80 mol% iridium oxide was formed on the plate surface. As has been shown in practice, such an oxide mixture has optimal catalyst properties.
- the electrode is particularly impressive due to its extremely simple structure. In addition, their production is relatively cheap, since carbon (electric coal, graphite) is an inexpensive starting material.
- the described method can be used in a particularly advantageous manner in the production of electrodes for high-performance water decomposition apparatus for the production of hydrogen. Thanks to the simplicity and economy of the product manufactured in this way, it is ideally suited for standard, large-area electrodes for large industrial plants.
- the electrodes manufactured in this way are characterized by high chemical resistance and a favorable decomposition voltage.
Abstract
Elektrode für die Wasserelektrolyse, bestehend aus einer auf einer Seite mit Rillen (2) versehenen porösen Graphitplatte (1), welche auf der anderen Seite mit einer aus Titan und Titandioxyd bestehenden dünnen Oberflächenschicht (3) versehen ist. Die Oberflächenschicht (3) ist in vorteilhafter Weise mit einem zu 20 mol-% aus Rutheniumoxyd und zu 80 mol-% aus Iridiumoxyd bestehenden Katalysator (4) dotiert.Electrode for water electrolysis, consisting of a porous graphite plate (1) provided with grooves (2) on one side, which is provided on the other side with a thin surface layer (3) made of titanium and titanium dioxide. The surface layer (3) is advantageously doped with a catalyst (4) consisting of 20 mol% of ruthenium oxide and 80 mol% of iridium oxide.
Description
Die Erfindung geht aus von einer Elektrode nach der Gattung des Anspruchs l.The invention relates to an electrode according to the preamble of
Elektroden sowie Verfahren zu deren Herstellung sind vor allem von der für Brennstoffzellen entwickelten Technologie her bekannt (z.B. Carl Berger, Handbook of Fuel Cell Technology S. 401-406, Prentice Hall 1968; H.A. Liebhafsky and E.J. Cairns, Fuel Cells and Fuel Batteries, S. 289-294, John Wiley & Sons, 1968). Die Forderung nach genau definierten Reaktionszonen bedingt einen vielschichtigen Aufbau und spezielle Behandlungsverfahren derartiger Brennstoffzellen-Elektroden.Electrodes and processes for their production are known primarily from the technology developed for fuel cells (e.g. Carl Berger, Handbook of Fuel Cell Technology pp. 401-406, Prentice Hall 1968; HA Liebhafsky and EJ Cairns, Fuel Cells and Fuel Batteries, p 289-294, John Wiley & Sons, 1968). The requirement for precisely defined reaction zones requires a multilayer structure and special treatment processes for such fuel cell electrodes.
Für die Wasserzersetzung sind die oben beschriebenen Elektroden in ihrem Aufbau zu kompliziert und ihre Fertigungsmethoden zu aufwendig und kostspielig. Dies gilt insbesondere im Hinblick auf Herstellungsmethoden für industrielle Grossanlagen zur wirtschaftlichen Erzeugung von Wasserstoff.The structure of the electrodes described above is too complicated for water decomposition and their manufacturing methods are too complex and costly. This applies in particular with regard to manufacturing methods for large industrial plants for the economical production of hydrogen.
Elektroden für Wasserzersetzungszellen sind bereits vorgeschlagen worden (z.B. US-PS 4 039 409). Zur-Beschleunigung der elektrochemischen Reaktionen werden sie meist mit Katalysatoren dotiert.Electrodes for water decomposition cells have already been proposed (eg US Pat. No. 4,039,409). To accelerate the electrochemical reactions, they are usually used with kata dysers doped.
Die beschriebenen Elektroden lassen sowohl bezüglich ihrer mechanischen und chemischen Eigenschaften zu wünschen übrig. Das gleiche gilt bezüglich der verwendeten Katalysatoren.The described electrodes leave something to be desired in terms of their mechanical and chemical properties. The same applies to the catalysts used.
Der Erfindung liegt die Aufgabe zugrunde, eine Elektrode für die Wasserelektrolyse anzugeben, welche bei guter mechanischer und chemischer Stabilität, hoher elektrischer Leitfähigkeit und guter Durchlässigkeit für Wasser und Gas eine hohe Lebensdauer sowie die Eigenschaft besitzt, die Wasserzersetzungsreaktion katalytisch in optimaler Weise zu beschleunigen.The invention has for its object to provide an electrode for water electrolysis, which with good mechanical and chemical stability, high electrical conductivity and good permeability to water and gas has a long life and the property to catalytically accelerate the water decomposition reaction in an optimal manner.
Diese Aufgabe wird erfindungsgemäss durch die Merkmale des Anspruchs 1 gelöst.According to the invention, this object is achieved by the features of
Es hat sich gezeigt, dass es vorteilhaft ist, als Elektrodenmaterial einen porösen, durchlässigen Werkstoff auf-Kohlenstoffbasis zu benutzen und seine dem Elektrolyt zugewandte Oberfläche durch Titan/Titandioxyd vor korrosivem Angriff zu schützen. Als Katalysator ist eine aus Platinmetalloxyden bestehende Imprägnierung, vorzugsweise eine Mischung von Rutheniumoxyd und Iridiumoxyd, vorgesehen.It has been shown that it is advantageous to use a porous, permeable carbon-based material as the electrode material and to protect its surface facing the electrolyte from corrosive attack by means of titanium / titanium dioxide. An impregnation consisting of platinum metal oxides, preferably a mixture of ruthenium oxide and iridium oxide, is provided as the catalyst.
Die Erfindung wird anhand des nachfolgenden, durch eine Figur erläuterten Ausführungsbeispiels näher beschrieben.The invention is described in more detail with reference to the following exemplary embodiment explained by a figure.
Dabei zeigt die FigurThe figure shows
den Querschnitt durch eine Elektrode.the cross section through an electrode.
1 ist eine Platte aus porösem Graphit, deren der Wasserzufuhr zugekehrte Seite mit einem Raster von Rillen 2 versehen ist. 3 stellt die aus einer Mischung von Titan und Titandioxyd bestehende elektrolytseitige Oberflächenschicht dar. 4 ist die in der Oberflächenschicht enthaltene Katalysator-Dotierung bestehend aus einer Mischung von 20 mol-% Rutheniumoxyd und 80 mol-% Iridiumoxyd. Die Platte 1 kann in ihrer Grundrissform kreisrund, quadratisch, rechteckig, sechseckig oder achteckig ausgeführt sein.1 is a plate made of porous graphite, the side facing the water supply is provided with a grid of grooves 2. 3 represents the electrolyte-side surface layer consisting of a mixture of titanium and titanium dioxide. 4 is the catalyst doping contained in the surface layer consisting of a mixture of 20 mol% ruthenium oxide and 80 mol% iridium oxide. The shape of the
In eine fein-poröse Graphitplatte 1 von 60 mm Durchmesser und 4 mm Dicke (z.B. Qualität S 1602 von Le Carbone AG) wurden mit Hilfe eines Fräsers Rillen 2 in Form eines Rasters aus einer der Oberflächen herausgearbeitet. Bei einer gesamten Oberfläche von 28cm2 war die Breite und Tiefe der Rillen quadratischen Querschnitts je 1 mm, ihr gegenseitiger Abstand je 2 mm. Hierauf wurde die glatte Oberfläche der Platte 1, welche im Betrieb dem Feststoffelektrolyten zugewandt ist, im Vakuum von 10-5 bis 10 torr durch Glimmentladungen während 5 Minuten gereinigt. Danach wurde bei einer Aufdampfgeschwindigkeit von 10 bis 20 9/sec eine Titan-Schicht von total ca. 1000 R auf diese Oberfläche der Platte aufgedampft. Im Betrieb besteht diese Oberflächenschicht 3 dank örtlicher Oxydation zum grossen ; Teil aus Titan, zum kleineren aus Titandioxyd. Dadurch wird der darunterliegende Kohlenstoff (Graphit) der Platte 1 vor korrosivem Angriff (Oxydation durch entstehenden Sauerstoff) wirksam geschützt.In a fine-
Die auf diese Art und Weise vorbereitete Platte 1 wurde nun während 10 sec in eine alkoholische Lösung getaucht, welche ca. 15 rel. Gew.-% Rutheniumchlorid (RuCl3) und 85 rel. Gew.-% Iridiumchlorid (IrCl3) enthielt. Nach dem Abtropfen während 1 min wurde die Platte 1 während 10 min bei einer Temperatur von 3750C in Luft oxydiert. Dieser Prozess des Eintauchens und Oxydierens wurde insgesamt 5 Mal wiederholt. Zum Schluss wurde die Platte 1 nochmals während 4 h bei einer Temperatur von 375°C in Luft oxydiert. Derart wurde auf der Plattenoberfläche die Katalysator-Dotierung 4, bestehend aus ca. 20 mol-% Rutheniumoxyd (Ru02) und 80 mol-% Iridiumoxyd gebildet. Wie sich in der Praxis gezeigt hat, weist eine derartige Oxydmischung optimale Katalysatoreigenschaften auf.The
Die Elektrode besticht vor allem durch ihren ausserordentlich einfachen Aufbau. Zudem ist ihre Herstellung verhältnismässig billig, da Kohlenstoff (Elektrokohle, Graphit) ein preiswertes Ausgangsmaterial darstellt.The electrode is particularly impressive due to its extremely simple structure. In addition, their production is relatively cheap, since carbon (electric coal, graphite) is an inexpensive starting material.
Das beschriebene Verfahren lässt sich in besonders vorteilhafter Weise bei der Herstellung von Elektroden für Hochleistungs-Wasserzersetzungsapparate zur Herstellung von Wasserstoff anwenden. Dank der Einfachheit und Wirtschaftlichkeit des auf diese Art und Weise hergestellten Produkts eignet sich dieses vorzüglich für serienmässige, grossflächige Elektroden für industrielle Grossanlagen.The described method can be used in a particularly advantageous manner in the production of electrodes for high-performance water decomposition apparatus for the production of hydrogen. Thanks to the simplicity and economy of the product manufactured in this way, it is ideally suited for standard, large-area electrodes for large industrial plants.
Die auf diese Art hergestellten Elektroden zeichnen sich durch hohe chemische Beständigkeit und eine günstige Zersetzungsspannung aus.The electrodes manufactured in this way are characterized by high chemical resistance and a favorable decomposition voltage.
- 1 = Platte aus porösem Graphit1 = plate made of porous graphite
- 2 = Rillen2 = grooves
- 3 = Oberflächenschicht aus Ti/Ti02 3 = surface layer made of Ti / Ti0 2
- 4 = Katalysator-Dotierung aus 20 Ru02/80 Ir02 (Mol-Verhältnis)4 = catalyst doping of 20 Ru0 2/80 Ir0 2 (molar ratio)
Claims (4)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
CH6082/79 | 1979-06-29 | ||
CH608279 | 1979-06-29 |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0021456A1 true EP0021456A1 (en) | 1981-01-07 |
EP0021456B1 EP0021456B1 (en) | 1983-05-18 |
Family
ID=4303966
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP80200266A Expired EP0021456B1 (en) | 1979-06-29 | 1980-03-24 | Electrode for the electrolysis of water |
Country Status (3)
Country | Link |
---|---|
US (1) | US4348268A (en) |
EP (1) | EP0021456B1 (en) |
DE (2) | DE2928911A1 (en) |
Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0683247A1 (en) * | 1994-05-20 | 1995-11-22 | Bayer Ag | Process for manufacturing stable graphite cathodes for the electrolysis of chlorhydric acid |
EP0768390A1 (en) * | 1995-09-21 | 1997-04-16 | Karpov Institute of Physical Chemistry | Electrodes and methods of preparation thereof |
WO2007119130A1 (en) * | 2006-04-14 | 2007-10-25 | Toyota Jidosha Kabushiki Kaisha | Fuel cell |
CN106222694A (en) * | 2016-08-25 | 2016-12-14 | 山东清大银光金属海绵新材料有限责任公司 | The preparation method of sponge structure Alloy ternary oxide layer hydrogen evolution electrode material |
Families Citing this family (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4707229A (en) * | 1980-04-21 | 1987-11-17 | United Technologies Corporation | Method for evolution of oxygen with ternary electrocatalysts containing valve metals |
US4457824A (en) * | 1982-06-28 | 1984-07-03 | General Electric Company | Method and device for evolution of oxygen with ternary electrocatalysts containing valve metals |
JPS5937662A (en) * | 1982-08-24 | 1984-03-01 | Kureha Chem Ind Co Ltd | Electrode substrate for monopolar type fuel cell with two-layer structure |
US4849254A (en) * | 1988-02-25 | 1989-07-18 | Westinghouse Electric Corp. | Stabilizing metal components in electrodes of electrochemical cells |
US5332496A (en) * | 1993-04-12 | 1994-07-26 | Electrocom Gard, Ltd. | System for performing catalytic dehalogenation of aqueous and/or non-aqueous streams |
DE19844329B4 (en) * | 1998-09-28 | 2010-06-17 | Friedrich-Schiller-Universität Jena | Process for the treatment of microorganisms and pollutants |
US6936370B1 (en) * | 1999-08-23 | 2005-08-30 | Ballard Power Systems Inc. | Solid polymer fuel cell with improved voltage reversal tolerance |
US20040013935A1 (en) * | 2002-07-19 | 2004-01-22 | Siyu Ye | Anode catalyst compositions for a voltage reversal tolerant fuel cell |
US7241691B2 (en) * | 2005-03-28 | 2007-07-10 | Freescale Semiconductor, Inc. | Conducting metal oxide with additive as p-MOS device electrode |
US7510956B2 (en) * | 2006-01-30 | 2009-03-31 | Fressscale Semiconductor, Inc. | MOS device with multi-layer gate stack |
US20080187813A1 (en) * | 2006-08-25 | 2008-08-07 | Siyu Ye | Fuel cell anode structure for voltage reversal tolerance |
US7608358B2 (en) * | 2006-08-25 | 2009-10-27 | Bdf Ip Holdings Ltd. | Fuel cell anode structure for voltage reversal tolerance |
AT511433B1 (en) * | 2011-11-03 | 2012-12-15 | Pro Aqua Diamantelektroden Gmbh & Co Kg | ELECTRODE, ITS USE AND ELECTROCHEMICAL CELL |
CN103088362B (en) * | 2012-12-13 | 2015-12-23 | 苏州赛斯德工程设备有限公司 | A kind of Tubular titanium anode |
PT106779A (en) * | 2013-02-13 | 2014-08-13 | José Jo O Santana Campos Rodrigues | ELECTROLYTEER AND PRODUCTION PROCESS OF SYNTHESIS GAS, BY ELECTROLYSIS OF WATER, USING GRAPHITE / CARBON ELECTRODES |
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FR1398388A (en) * | 1963-06-10 | 1965-05-07 | Imp Metal Ind Kynoch Ltd | Electrolyser |
DE1286513B (en) * | 1966-03-18 | 1969-01-09 | Bayer Ag | Anode for electrolytic processes |
AT313313B (en) * | 1971-01-08 | 1974-02-11 | Metallgesellschaft Ag | Electrode, in particular anode, for chlor-alkali electrolysis and method for producing the electrode |
US3928150A (en) * | 1974-04-02 | 1975-12-23 | Ppg Industries Inc | Method of operating an electrolytic cell having hydrogen gas disengaging means |
FR2308701A1 (en) * | 1975-04-25 | 1976-11-19 | Battelle Memorial Institute | GASEOUS ELECTROLYZER |
US4011149A (en) * | 1975-11-17 | 1977-03-08 | Allied Chemical Corporation | Photoelectrolysis of water by solar radiation |
US4039409A (en) * | 1975-12-04 | 1977-08-02 | General Electric Company | Method for gas generation utilizing platinum metal electrocatalyst containing 5 to 60% ruthenium |
Family Cites Families (6)
Publication number | Priority date | Publication date | Assignee | Title |
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GB1195871A (en) * | 1967-02-10 | 1970-06-24 | Chemnor Ag | Improvements in or relating to the Manufacture of Electrodes. |
US3616445A (en) * | 1967-12-14 | 1971-10-26 | Electronor Corp | Titanium or tantalum base electrodes with applied titanium or tantalum oxide face activated with noble metals or noble metal oxides |
US3647641A (en) * | 1970-10-26 | 1972-03-07 | Gen Electric | Reactant sensor and method of using same |
GB1403183A (en) * | 1973-05-25 | 1975-08-28 | Hooker Chemicals Plastics Corp | Bipolar electrodes |
US3824175A (en) * | 1973-05-25 | 1974-07-16 | Hooker Chemical Corp | Bipolar electrode |
GB1529989A (en) * | 1976-10-15 | 1978-10-25 | Johnson & Co Ltd A | Electrolytic cells |
-
1979
- 1979-07-18 DE DE19792928911 patent/DE2928911A1/en not_active Withdrawn
-
1980
- 1980-03-24 EP EP80200266A patent/EP0021456B1/en not_active Expired
- 1980-03-24 DE DE8080200266T patent/DE3063253D1/en not_active Expired
- 1980-06-17 US US06/160,176 patent/US4348268A/en not_active Expired - Lifetime
Patent Citations (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR1398388A (en) * | 1963-06-10 | 1965-05-07 | Imp Metal Ind Kynoch Ltd | Electrolyser |
DE1286513B (en) * | 1966-03-18 | 1969-01-09 | Bayer Ag | Anode for electrolytic processes |
AT313313B (en) * | 1971-01-08 | 1974-02-11 | Metallgesellschaft Ag | Electrode, in particular anode, for chlor-alkali electrolysis and method for producing the electrode |
US3928150A (en) * | 1974-04-02 | 1975-12-23 | Ppg Industries Inc | Method of operating an electrolytic cell having hydrogen gas disengaging means |
FR2308701A1 (en) * | 1975-04-25 | 1976-11-19 | Battelle Memorial Institute | GASEOUS ELECTROLYZER |
US4011149A (en) * | 1975-11-17 | 1977-03-08 | Allied Chemical Corporation | Photoelectrolysis of water by solar radiation |
US4039409A (en) * | 1975-12-04 | 1977-08-02 | General Electric Company | Method for gas generation utilizing platinum metal electrocatalyst containing 5 to 60% ruthenium |
Cited By (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP0683247A1 (en) * | 1994-05-20 | 1995-11-22 | Bayer Ag | Process for manufacturing stable graphite cathodes for the electrolysis of chlorhydric acid |
US5575985A (en) * | 1994-05-20 | 1996-11-19 | Bayer Aktiengesellschaft | Preparation of stable graphite |
CN1052038C (en) * | 1994-05-20 | 2000-05-03 | 拜尔公司 | Preparation of stable graphite cathodes for the electrolysis of hydrochloric acid |
EP0768390A1 (en) * | 1995-09-21 | 1997-04-16 | Karpov Institute of Physical Chemistry | Electrodes and methods of preparation thereof |
WO2007119130A1 (en) * | 2006-04-14 | 2007-10-25 | Toyota Jidosha Kabushiki Kaisha | Fuel cell |
CN106222694A (en) * | 2016-08-25 | 2016-12-14 | 山东清大银光金属海绵新材料有限责任公司 | The preparation method of sponge structure Alloy ternary oxide layer hydrogen evolution electrode material |
CN106222694B (en) * | 2016-08-25 | 2018-01-02 | 山东清大银光金属海绵新材料有限责任公司 | Sponge structure alloy loads the preparation method of ternary oxide layer hydrogen evolution electrode material |
Also Published As
Publication number | Publication date |
---|---|
EP0021456B1 (en) | 1983-05-18 |
US4348268A (en) | 1982-09-07 |
DE2928911A1 (en) | 1981-01-29 |
DE3063253D1 (en) | 1983-07-07 |
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