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GB2095025A - Acid electrolyte fuel cell - Google Patents

Acid electrolyte fuel cell Download PDF

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Publication number
GB2095025A
GB2095025A GB8108253A GB8108253A GB2095025A GB 2095025 A GB2095025 A GB 2095025A GB 8108253 A GB8108253 A GB 8108253A GB 8108253 A GB8108253 A GB 8108253A GB 2095025 A GB2095025 A GB 2095025A
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United Kingdom
Prior art keywords
fuel cell
acid
acid electrolyte
platinum
heavy metal
Prior art date
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Granted
Application number
GB8108253A
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GB2095025B (en
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Hitachi Ltd
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Hitachi Ltd
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Publication date
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Priority to GB8108253A priority Critical patent/GB2095025B/en
Priority to DE3110792A priority patent/DE3110792C2/en
Publication of GB2095025A publication Critical patent/GB2095025A/en
Application granted granted Critical
Publication of GB2095025B publication Critical patent/GB2095025B/en
Expired legal-status Critical Current

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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
    • H01M4/92—Metals of platinum group
    • H01M4/928—Unsupported catalytic particles; loose particulate catalytic materials, e.g. in fluidised state
    • 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
    • H01M4/92—Metals of platinum group
    • H01M4/921—Alloys or mixtures with metallic elements
    • 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
    • H01M4/92—Metals of platinum group
    • H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
    • H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/08—Fuel cells with aqueous electrolytes
    • 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
    • H01M2300/00—Electrolytes
    • H01M2300/0002—Aqueous electrolytes
    • H01M2300/0005—Acid electrolytes
    • 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
    • H01M2300/0005—Acid electrolytes
    • H01M2300/0008—Phosphoric acid-based
    • 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
    • H01M2300/0005—Acid electrolytes
    • H01M2300/0011—Sulfuric acid-based
    • 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

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Inert Electrodes (AREA)
  • Catalysts (AREA)

Abstract

An acid electrolyte fuel cell characterized by using as a fuel electrode catalyst a ternary electro- deposited platinum-rutherium-heavy metal catalyst wherein the heavy metal is rhenium, tin molybdenum, antimony, osmium, iridium, lead, bismuth or titanium and using as a fuel a liquid low-molecular weight hydrocarbon containing oxygen such as methanol, formaldehyde, formic acid.

Description

SPECIFICATION Acid electrolyte fuel cell This invention relates to an acid electrolyte fuel cell, more particularly to an acid electrolyte fuel cell using as a fuel a liquid low-molecuiar weight hydrocarbon containing oxygen such as methanol, formaldehyde, formic acid, or the like and having a special fuel electrode catalyst.
Heretofore, platinum has widely been used as an electrode catalyst for such a kind of fuel cell.
When platinum is used, necessary performance may be attained to some extent, but not sufficient due to large polarization. In order to improve this, various proposals have been made. Among them, efficiency is acknowledged in platinum-ruthenium alloys, platinum-tin electro-codeposits, and platinum-rhenium electrocodeposits (e.g., Electrochemical Technology 5, No. 9-10, 441-445 (1967); Journal of the Electrochemical Society, 1 16, No. 11,1608-1611(1969)).
Platinum-ruthenium alloys show the best performance but have disadvantages in requiring high-temperature heating for the preparation and difficulty in preparing uniform alloys. On the other hand, electrodeposited catalysts are superior in preparation method to the alloy catalysts, although slightly inferior to the latter in performance. Platinum-tin electro-codeposited catalysts are slightly inferior to platinum-rhenium catalysts, but the latter has a problem in life because of great deterioration of performance with the lapse of time; consequently these have advantages on one hand but also have disadvantages on the other hand.
It is an object of this invention to provide an acid electrolyte fuel cell having high performance improving the disadvantages mentioned above.
This invention provides an acid electrolyte fuel cell comprising a fuel chamber, a fuel electrode, an oxidizer electrode, an acid electrolyte placed between the fuel electrode and the oxidizer electrode and an oxidizer chamber and using as a fuel a liquid low-molecular weight hydrocarbon containing oxygen, characterized in that as a catalyst for the fuel electrode there is used a ternary electrodeposited platinum-ruthenium-M catalyst, wherein M is a heavy metal.
In the attached drawings, Figure 1 is a crosssectional view of the acid electrolyte fuel cell, Figure 2 is a graph showing a relationship between current density and cell voltage, Figures 3 and 4 are graphs showing changes in discharge properties with the lapse of time.
This invention is explained more in detail referring to Figure 1. In Figure 1, numeral 1 denotes a fuel inlet, numeral 2 denotes a fuel chamber, numeral 3 denotes a fuel electrode, numeral 4 denotes an electrolyte chamber, numeral 5 denotes an ion exchange membrane, numeral 6 denotes an oxidizer electrode, numeral 7 denotes an inlet for an oxidizer, numeral 8 denotes an oxidizer chamber and numeral 9 denotes an outlet for off gas.
As the fuel, there can be used liquid lowmolecular weight hydrocarbons containing oxygen in their molecules such as methanol, ethanol, ethylene glycol, etc.; formaldehyde (usually in the form of formalin), acetaldehyde, etc.; formic acid, oxalic acid, etc. The fuel can be supplied to the fuel cell as an anolyte, for example, containing CH3OH 0.3-1.0 mole/l in H2SO4 1.5-3.5 mole/l.
The fuel electrode comprises an electrode substrate and a catalyst. As the electrode substrate, there can be used metallic nets of platinum, tantaium, niobium, zirconium or the like, or expanded metal, or carbonaceous porous materials.
As the catalyst for the fuel electrode, there is used a ternary platinum-ruthenium-heavy metal (M) electro-codeposit. As the heavy metal, there can be used one member selected from the group consisting of molybdenum, tin, antimony, rhenium, osmium, iridium, lead bismuth and titanium. The heavy metal functions as a cocatalyst when used together with platinum and ruthenium. Among these heavy metals, rhenium and tin are more preferable.
As to the composition of the fuel electrode catalyst, 20~40% by weight of ruthenium, 1~20% by weight of the heavy metal and the remainder being platinum is preferable from the viewpoint of catalytic activity. in the case of Pt Ru-Sn codeposit, a preferable composition is 30-35% by weight of ruthenium, 2~7% by weight of tin and the remainder being platinum. In the case of Pt-Ru-Re codeposit, a preferable composition is 28~33% by weight of ruthenium, 2-1 5% by weight of rhenium and the remainder being platinum.
The ternary platinum-ruthenium-heavy metal electro-codeposit can be obtained by using a conventional metal plating technique. For example, in a plating solution containing a platinum source material, a ruthenium source material, and a heavy metal source material, a metallic net such as platinum net or the like as the electrode substrate is placed and a current is passed therethrough at a current density of, e.g., 8-30 mA/cm2 at 100--450C. As the platinum source materials, there can be used, for example, H2PtCl6 .6H 20, [ Pt(NH3)4 ] (0H2), (NH4)2 [ PtCl6 ] t [ Pt(NH3)4 ] C14. H20, [ Pt(N02)2(NH3)2 ] , H2 [ Pt(OH)6 ] , etc.As the ruthenium source materials, there can be used, for example, RuCI3 ~ 3H20, [ Ru(NH3)6 ] CI3, K3 [ Ru2NCl6(H20)2j, Ru2(S04)3, etc. As the heavy metal source materials, there can be used, for example, Re2O7, NaRcO4, KReO4, NH4ReO4, etc., Snot4, Na2Sn (OH)6, Sn(S04)2.2H20, etc.
As the electrolyte, there is used an acid electrolyte such as an aqueous solution of sulfuric acid, phosphoric acid, trifluoromethane sulfonic acid or a mixture thereof.
As the ion exchange membrane, there can be used conventionally used ones such as cation exchange membranes.
The oxidizer electrode comprises an electrode substrate, a catalyst and a water proof film. As the electrode substrate, the same one as used in the fuel electrode can be used. As the catalyst, fine platinum black, carbon powder supporting fine platinum black, and the like conventional ones can be used. The catalyst can be mounted on the substrate mixed with a hydrophobic binder such as polytetrafluoroethylene powder, polyvinyl chloride powder, polystyrene powder, etc. As the waterproof film pressed onto the catalystmounted substrate, there can be used conventionally used ones such as polytetrafluoroethylene porous film, and the like.
As the oxidizer, there can be used oxygen or oxygen-containing gas such as air.
This invention is illustrated by way of the following Examples.
EXAMPLE 1 In a plating solution containing chloroplatinic acid (H2PtCl6.6H20) 21 g/l, ruthenium chloride (RuCl3.3H20) 10 g/l, and rhenium oxide (Re207) 10 g/l, a platinum net of 80 mesh was placed and electrodeposition was carried out at a current density of 12 mA/cm2 at room temperature until the electrodeposited amount became 15 mg/cm2.
The thus obtained electrode was used as the fuel electrode and a fuel cell as shown in Figure 1 was constructed. As the oxidizer, air was used. As the acid electrolyte, an aqueous solution of sulfuric acid in a concentration of 3 mole/l was used. As the fuel, methanol was used and supplied as an anolyte containing methanol in a concentration of 1.0 or 0.5 mol/l in an aqueous solution of sulfuric acid of 3 mole/l.
The relationship between current density and cell voltage of the resulting fuel cell measured at room temperature is shown as the curve C in Figure 2. The curve C in Figure 3 shows changes in discharge properties with the lapse of time of the resulting fuel cell in the case of using as anolyte 3M H2S04-1 M CH3OH at a discharge current density of 30 mA/cm2 and the curve C in Figure 4 shows the same discharge properties as mentioned above in the case of using as anolyte 3M H2S04-O.5M CH3OH at a discharge current density of 60 mA/cm2.
For comparison, the results obtained in the same manner as mentioned above in the case of using as a fuel electrode platinum-ruthenium (1:1) alloy coated on a platinum net in an amount of 15 mg/cm2 are shown as the curve A in Figures 2, 3 and 4 and in the case of using as a fuel electrode platinum-rhenium electrocodeposit (electrodeposited amount 15 mg/cm2; Pt 90% by weight) are shown as the curve B in Figures 2, 3 and 4.
The same results as obtained in Example 1 are obtained when the plating conditions and the amounts of metal source materials for giving the ternary electrodeposited Pt-Ru-Re catalyst are changed in the following ranges: H2PtCle 6H20 30-10 g/l RuCl3.3H20 15- 4 gel Rue207 10- 5 g/l Current density for electrodeposition 30-8 mA/cm2 Bath temperature for electrodeposition 45~20 C.
EXAMPLE 2 The procedure for giving a fuel electrode as described in Example 1 was repeated except for using the following plating solution: H2PtCl6.6H20 21 g/l RuCl3.3H2O 10 g/l SnCI4 8 g/l Using the resulting fuel electrode, a fuel cell as shown in Figure 1 was constructed in the same manner as described in Example 1 and the relationship between current density and cell voltage was measured in the same manner as described in Example 1. The results are shown as the curve D in Figure 2. Changes in discharge properties with the lapse of time were also measured in the same manner as described in Example 1 and shown as the curve D in Figures 3 and 4.
The same results as obtained in Example 2 mentioned above are obtained when the plating conditions and the amounts of metal source materials for giving the ternary electrodeposited Pt-Ru-Sn catalyst are changed in the following ranges: H2PtCl6 .6H20 30--10 g/l RuCl3.3H20 15- 4g/l SnCI4 10- 5 9/l Current density for electrodeposition 30-8 mA/cm2 Bath temperature for electrodeposition 30~1 0 C.
As shown in Figures 2, 3 and 4, the fuel electrode catalysts of this invention (curves C and D) show the same or better performance compared with the fuel electrode catalyst made of the Pt-Ru (1:1) alloy (curve A) and clearly better performance compared with the fuel electrode catalyst made of the Pt-Re codeposit (curve D).
But it should be noted that very complicated and elaborate technique should be employed for preparing the Pt-Ru alloy having uniform quality as mentioned above, which is disadvantageous from the viewpoint of industrial production. Further, as shown in Figure 4, in the case of discharge current density being as large as 60 mA/cm2, the fuel cell according to Example 2 (curve D) shows very stable voltage even after 2000 hours or longer, which is clearly more excellent than the curves A and B (known fuel cells).
As mentioned above, according to this invention, an acid electrolyte fuel cell having higher performance than conventional ones can be obtained by a more simple way (i.e., by an electrodeposition process).

Claims (7)

1. An acid electrolyte fuel cell comprising a fuel chamber, a fuel electrode, an oxidizer electrode, an acid electrolyte placed between the fuel electrode and the oxidizer electrode and an oxidizer chamber as using as a fuel a liquid low-molecular weight hydrocarbon containing oxygen, characterized in that as a catalyst for the fuel electrode there is used a ternary electrodeposited platinumruthenium-heavy metal catalyst.
2. An acid electrolyte fuel cell according to claim 1, wherein the heavy metal is molybdenum, tin, antimony, rhenium, osmium, iridium, lead, bismuth or titanium.
3. An acid electrolyte fuel cell according to either of claims 1 and 2, wherein the ternary electrodeposited platinum-ruthenium-heavy metal catalyst contains 20 to 40% by weight of ruthenium, 1 to 20% by weight of the heavy metal and the remainder being platinum.
4. An acid electrolyte fuel cell according to any one of claims 1 to 3, wherein the ternary electrodeposited platinum-ruthenium-heavy metal catalyst is an electrodeposited platinumruthenium-rhenium or platinum-ruthenium-tin catalyst.
5. An acid electrolyte fuel cell according to any one of claims 1 to 4, wherein the liquid lowmolecular weight hydrocarbon containing oxygen is methanol, ethanol, ethylene glycol, formaldehyde, acetaldehyde, formic acid or oxalic acid.
6. An acid electrolyte fuel cell according to any one of claims 1 to 5, wherein the acid electrolyte is an aqueous solution of sulfuric acid, phosphoric acid, trifluoromethane sulfonic acid or a mixture thereof.
7. An acid electrolyte fuel cell substantially as hereinbefore described with particular reference to the Examples.
GB8108253A 1981-03-17 1981-03-17 Acid electrolyte fuel cell Expired GB2095025B (en)

Priority Applications (2)

Application Number Priority Date Filing Date Title
GB8108253A GB2095025B (en) 1981-03-17 1981-03-17 Acid electrolyte fuel cell
DE3110792A DE3110792C2 (en) 1981-03-17 1981-03-19 Fuel cell with acidic electrolyte

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB8108253A GB2095025B (en) 1981-03-17 1981-03-17 Acid electrolyte fuel cell
DE3110792A DE3110792C2 (en) 1981-03-17 1981-03-19 Fuel cell with acidic electrolyte

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GB2095025A true GB2095025A (en) 1982-09-22
GB2095025B GB2095025B (en) 1984-11-21

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2187880A (en) * 1986-02-28 1987-09-16 Nat Res Dev Electrode for oxidising methanol
WO1998040161A1 (en) * 1997-03-11 1998-09-17 Illinois Institute Of Technology SINGLE PHASE TERNARY Pt-Ru-Os CATALYSTS FOR DIRECT OXIDATION FUEL CELLS
EP1184079A2 (en) * 2000-09-04 2002-03-06 DaimlerChrysler AG Electrochemical process for producing a catalyst
EP1290747A1 (en) * 2000-06-01 2003-03-12 IdaTech, LLC. Fuel cells and fuel cell systems containing non-aqueous electrolytes
WO2008080227A1 (en) * 2006-12-29 2008-07-10 Tekion, Inc. Electrochemical oxidation of formic acid using a noble metal based catalyst with admetals

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19548421B4 (en) † 1995-12-22 2004-06-03 Celanese Ventures Gmbh Process for the continuous production of membrane electrode assemblies
US5904740A (en) * 1997-06-03 1999-05-18 Motorola, Inc. Fuel for liquid feed fuel cells
CN103007935A (en) * 2012-12-13 2013-04-03 北京化工大学常州先进材料研究院 Preparation method of Pt/antimony-doped tin oxide-graphene catalyst

Family Cites Families (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
NL288862A (en) * 1962-02-13
GB1028325A (en) * 1963-02-07 1966-05-04 Leesona Corp Improvements in or relating to fuel cells
JPS4116745B1 (en) * 1963-07-17 1966-09-22
GB1409260A (en) * 1971-12-29 1975-10-08 Exxon Research Engineering Co Fuel cell having non-alloyed palladium-ruthenium anode catalyst

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2187880A (en) * 1986-02-28 1987-09-16 Nat Res Dev Electrode for oxidising methanol
WO1998040161A1 (en) * 1997-03-11 1998-09-17 Illinois Institute Of Technology SINGLE PHASE TERNARY Pt-Ru-Os CATALYSTS FOR DIRECT OXIDATION FUEL CELLS
EP1290747A1 (en) * 2000-06-01 2003-03-12 IdaTech, LLC. Fuel cells and fuel cell systems containing non-aqueous electrolytes
EP1290747A4 (en) * 2000-06-01 2006-12-06 Idatech Llc Fuel cells and fuel cell systems containing non-aqueous electrolytes
EP1184079A2 (en) * 2000-09-04 2002-03-06 DaimlerChrysler AG Electrochemical process for producing a catalyst
EP1184079A3 (en) * 2000-09-04 2003-12-10 DaimlerChrysler AG Electrochemical process for producing a catalyst
WO2008080227A1 (en) * 2006-12-29 2008-07-10 Tekion, Inc. Electrochemical oxidation of formic acid using a noble metal based catalyst with admetals

Also Published As

Publication number Publication date
GB2095025B (en) 1984-11-21
DE3110792A1 (en) 1982-09-30
DE3110792C2 (en) 1984-01-19

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PCNP Patent ceased through non-payment of renewal fee

Effective date: 19930317