WO2010066444A1 - Anode material for high-temperature fuel cells - Google Patents

Anode material for high-temperature fuel cells Download PDF

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Publication number
WO2010066444A1
WO2010066444A1 PCT/EP2009/008884 EP2009008884W WO2010066444A1 WO 2010066444 A1 WO2010066444 A1 WO 2010066444A1 EP 2009008884 W EP2009008884 W EP 2009008884W WO 2010066444 A1 WO2010066444 A1 WO 2010066444A1
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WO
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Prior art keywords
anode material
vol
material according
anode
further metal
Prior art date
Application number
PCT/EP2009/008884
Other languages
French (fr)
Inventor
Sascha Kuehn
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Ezelleron 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 Ezelleron Gmbh filed Critical Ezelleron Gmbh
Priority to DE112009003518T priority Critical patent/DE112009003518T5/en
Publication of WO2010066444A1 publication Critical patent/WO2010066444A1/en

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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
    • H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
    • H01M4/8652—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites as mixture
    • 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
    • H01M4/92—Metals of platinum group
    • 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
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide 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

Definitions

  • the invention relates to an anode material for high- temperature fuel cells (SOFCs) , especially tubular high temperature solid oxide fuel cells .
  • SOFCs high- temperature fuel cells
  • This invention besides mechanical and thermal stability, also improved chemical and/or catalytic stability against contamination by fuel pollutants such as sulphur and hydrocarbons can be achieved.
  • the commonly used anodes used consist of a mixture of metallic nickel and Yttrium-stabilized zirconium oxide (YSZ) . They possess some positive properties such as high electrical and thermal conductivity, a coefficient of expansion well adapted at the one of the electrolyte (mostly YSZ) , chemical stability at anode conditions and a high degree of electrochemical activity as regards hydrogen oxidation. With these anodes their sensitivity to small sulphur pollutions in the ppm range is a disadvantage. In addition they have a tendency to carbon deposition especially in the utilization of higher hydrocarbons and/or with lower water or oxygen to carbon ratio which also leads to loss of performance.
  • YSZ Yttrium-stabilized zirconium oxide
  • cerium oxide also prevents the sooting of the cells and increases the power density.
  • a further possibility is the partial replacement of the Ni by selected elements or oxides, e.g. Cu/CeO2/YSZ for higher sulphur- tolerance and good electrochemical performance, although Cu can only be used at temperatures below 700 0 C and has a poor catalytic activity for hydrogen oxidation. With combinations of Ni-Cu or Ni-Cu alloys the performance of these anodes could not be increased to the level of the anodes with Ni as the only metallic component.
  • the problem addressed by this invention is to improve the chemical stability of a high- temperature fuel cell and at the same time not to reduce the achievable performance compared to the common anode materi- als, or at least not substantially ( ⁇ 10%) .
  • the anode material according to the invention is nickel and copper, also as a Ni-Cu alloy, and formed with at least one further metal.
  • the further metal can be a transition metal. It can be selected from Co, V, Cr, Pt, Rh, Ag, Au, Mo, W, Ru and Pd.
  • the further metal can be an alkaline earth metal or alkaline metal, especially Mg or Li.
  • Iron is preferred as the further metal .
  • the content of the further metal should be in the range of 0.5 vol.-% to 95 vol.-%, preferably from 0.5 vol.-% to 10 vol. -%
  • the anode material can also contain at least one ce- ramie material.
  • this can be a cerium oxide compound and/or a zirconium oxide compound.
  • ceramics with an ionic conductivity, preferably oxygen conductivity and specially preferred with a mixed conductivity (ion and electronic conduction) can also be made of a gallate or a bismuth oxide compound. In this one or more of these compounds can be included. Beneficial is the use of the compounds in doped form.
  • the content of ceramic material in the anode material according to the invention should be 5 vol.-% to 70 vol.-%, preferably 25 vol.-% to 50 vol.-% and especially preferred 30 vol.-% to 40 vol-%.
  • the doping with further materials such as the alkaline earth metals and alkali metals as well as the addition of titanates and vanadates further improve the stability of the anodes against hydrocarbon deposition and/or the tolerance towards pollutants such as sulphur or chlorine compounds.
  • the contents of the before mentioned materials should be in the range of 0.1 vol.-% to 50 vol.-%.
  • the anode material can contain one or also at least two of these chemical compounds .
  • the anode material should advantageously partly or in regions possess a face-centered cubic lattice.
  • a further metal/transition metal to a Ni-Cu-cermet anode, an anode with an increased sulphur tolerance (greater than 10 ppm sulphur- compound in the fuel) can be manufactured that at the same time possesses a high power density and with the use of cerium oxide the sooting of the anodes can be prevented or at least reduced.
  • Anodes made with the anode material according to the invention can be manufactured for example by injection moulding or also extrusion and subsequent de- binding and thermal treatment.
  • a possibility for the manufacture of a material according to the invention consists of producing a mixture of oxides that can, at least partially, be converted to metallic phases by means of subsequent re- duction.
  • Ni-Cu-Co mixture as the metallic phase in combination with GDC - Gd stabilized cerium oxide - as the ceramic phase.
  • first nickel oxide, copper oxide, cobalt oxide and GDC are mixed in forms of fine powders such that the metal phases achieved by reduction are at least 30 vol.-% of the final anode material.
  • the content of Ni, Cu and Co in the metallic phase should be 70 vol.-%, 25 vol.-% and 5 vol . - % .
  • a binder system is added to make a feedstock that has a viscosity suitable for injection moulding or extrusion.
  • anodes for high- temperature fuel cells can be formed by extrusion and then subjected to a thermal treatment in air at a temperature of 115O 0 C.
  • the organic binder components can be burnt out and sintering can be carried out until a material strength for further processing is reached.
  • it can be reduced at 800 0 C in a hydrogen atmosphere and in this way the metallic phases of Ni, Cu and Co can be maintained.
  • Ni-Cu-Fe-Co-GDC anode materials powdered nickel oxide, copper oxide, iron oxide and GDC are mixed such that after the reduction, the metal phases in the material are at least 30 vol.-% and the contents in the metal phase of the Ni are 70 vol.-%, Cu is 25 vol.-%, Fe is 3 vol.-% and Co is 2 vol. -%.
  • a binder system is added to make a feedstock that has a viscosity suitable for injection moulding or extrusion.
  • anodes for high- temperature fuel cells can be formed by extrusion and then subjected to a thermal treatment in air at a temperature of 1250 0 C.
  • the organic binder components can be burnt out and sintering can be carried out until a material strength for further processing is reached.
  • it can be reduced at 1200 0 C in a hydrogen atmosphere and in this way the metallic phases of Ni, Cu, Fe and Co can be maintained.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Composite Materials (AREA)
  • Inert Electrodes (AREA)

Abstract

The invention concerns an anode material for high temperature fuel cells. In this way the chemical stability of a high- temperature fuel cell is improved and at the same time the achievable performance compared to the known anode materials, is not made worse, or at least not substantially (<10%). The anode material according to the invention is nickel and copper also as a Ni-Cu alloy and formed with at least one further metal. The anode material can contain at least one ceramic material.

Description

Anode material for high- temperature fuel cells
The invention relates to an anode material for high- temperature fuel cells (SOFCs) , especially tubular high temperature solid oxide fuel cells . With this invention, besides mechanical and thermal stability, also improved chemical and/or catalytic stability against contamination by fuel pollutants such as sulphur and hydrocarbons can be achieved.
The ability also to use conventional fossil fuels is an important advantage of the high- temperature solid oxide fuel cell. However, these fuels also contain a not inconsiderable amount of pollutants such as hy- drogen sulphide and other sulphur compounds. In the currently common anodes these cause losses in performance due to poisoning of the anode. However, de- pending on the particular case, also the use of carbon containing fuels (e.g. hydrocarbons) can lead to unstable behaviour of the solid oxide fuel cells. Basically, the following processes can be responsible: (1) Physical adsorption/chemisorption of pollutants (e.g. of H2S) on the active surface of the anode, which reduces the usable active surface (reactive centres) for the electrochemical reactions, and/or
(2) undesired reactions of the pollutant and/or fuel components (e.g. hydrocarbons) with the respective anode material (e.g. formation of sulphides due to reaction between sulphur and the anode material which can lead to a loss of catalytic activity, conductivity and stability and/or a formation of whiskers due to soot and nickel) and/or
(3) blocking of the anode's pores due to deposition especially of soot and causing impairment of the gas transport in the anode .
The commonly used anodes used consist of a mixture of metallic nickel and Yttrium-stabilized zirconium oxide (YSZ) . They possess some positive properties such as high electrical and thermal conductivity, a coefficient of expansion well adapted at the one of the electrolyte (mostly YSZ) , chemical stability at anode conditions and a high degree of electrochemical activity as regards hydrogen oxidation. With these anodes their sensitivity to small sulphur pollutions in the ppm range is a disadvantage. In addition they have a tendency to carbon deposition especially in the utilization of higher hydrocarbons and/or with lower water or oxygen to carbon ratio which also leads to loss of performance.
In order to prevent these disadvantages, investigations have been carried out for some time in the use of different materials for the manufacture of sulphur-tolerant anodes for the SOFC, in which in most cases the increased sulphur tolerance brings with it a reduced power density of the SOFC. Thus, the application of lanthanum strontium titanates and lanthanum strontium vanadates as sulphur- tolerant anode material has been thought of. These chemical compounds, however, do not possess the catalytic activities for hydrogen oxidation that the Ni-YSZ anodes possess.
Besides the perovskites, like the above mentioned titanates and vanadates, investigations have also been carried out especially on improved cermets as sulphur-tolerant materials. With the replacement of YSZ by scandium- stabilised zirconium oxide (SSZ) the sul- phur- tolerance can be increased and with the higher conductivity in comparison with YSZ, the losses of performance are small or non-existing. However, scandium is too expensive for general use. Besides this, investigations have also been carried out with combi- nations of nickel or other metals with cerium oxide or stabilised cerium oxides. Thus the cerium oxide prevents the coarsening of the metallic particles that would lead to a loss of performance. The use of cerium oxide also prevents the sooting of the cells and increases the power density. A further possibility is the partial replacement of the Ni by selected elements or oxides, e.g. Cu/CeO2/YSZ for higher sulphur- tolerance and good electrochemical performance, although Cu can only be used at temperatures below 7000C and has a poor catalytic activity for hydrogen oxidation. With combinations of Ni-Cu or Ni-Cu alloys the performance of these anodes could not be increased to the level of the anodes with Ni as the only metallic component.
The problem addressed by this invention is to improve the chemical stability of a high- temperature fuel cell and at the same time not to reduce the achievable performance compared to the common anode materi- als, or at least not substantially (<10%) .
According to the invention this task is achieved by an anode material possessing the properties of claim 1. An advantageous design and further development of the invention can be achieved with the claims mentioned in the dependend claims.
The anode material according to the invention is nickel and copper, also as a Ni-Cu alloy, and formed with at least one further metal. The further metal can be a transition metal. It can be selected from Co, V, Cr, Pt, Rh, Ag, Au, Mo, W, Ru and Pd. Just as advantageously the further metal can be an alkaline earth metal or alkaline metal, especially Mg or Li.
Iron is preferred as the further metal . The content of the further metal should be in the range of 0.5 vol.-% to 95 vol.-%, preferably from 0.5 vol.-% to 10 vol. -%
The anode material can also contain at least one ce- ramie material. Preferably this can be a cerium oxide compound and/or a zirconium oxide compound. Preferred are ceramics with an ionic conductivity, preferably oxygen conductivity and specially preferred with a mixed conductivity (ion and electronic conduction) . Use can also be made of a gallate or a bismuth oxide compound. In this one or more of these compounds can be included. Beneficial is the use of the compounds in doped form.
The content of ceramic material in the anode material according to the invention should be 5 vol.-% to 70 vol.-%, preferably 25 vol.-% to 50 vol.-% and especially preferred 30 vol.-% to 40 vol-%.
The doping with further materials such as the alkaline earth metals and alkali metals as well as the addition of titanates and vanadates further improve the stability of the anodes against hydrocarbon deposition and/or the tolerance towards pollutants such as sulphur or chlorine compounds. The contents of the before mentioned materials should be in the range of 0.1 vol.-% to 50 vol.-%. In this the anode material can contain one or also at least two of these chemical compounds .
The anode material should advantageously partly or in regions possess a face-centered cubic lattice. With the addition of a further metal/transition metal to a Ni-Cu-cermet anode, an anode with an increased sulphur tolerance (greater than 10 ppm sulphur- compound in the fuel) can be manufactured that at the same time possesses a high power density and with the use of cerium oxide the sooting of the anodes can be prevented or at least reduced.
Anodes made with the anode material according to the invention can be manufactured for example by injection moulding or also extrusion and subsequent de- binding and thermal treatment.
In the following, concrete information of examples of the anode materials and their manufacture according to the invention are given.
A possibility for the manufacture of a material according to the invention consists of producing a mixture of oxides that can, at least partially, be converted to metallic phases by means of subsequent re- duction.
Example 1
For the manufacture of an anode for high- temperature fuel cells it is proposed to use as the material a
Ni-Cu-Co mixture as the metallic phase in combination with GDC - Gd stabilized cerium oxide - as the ceramic phase. For this purpose first nickel oxide, copper oxide, cobalt oxide and GDC are mixed in forms of fine powders such that the metal phases achieved by reduction are at least 30 vol.-% of the final anode material. The content of Ni, Cu and Co in the metallic phase should be 70 vol.-%, 25 vol.-% and 5 vol . - % .
After a homogenous mixing of the oxide powders, a binder system is added to make a feedstock that has a viscosity suitable for injection moulding or extrusion. In this way anodes for high- temperature fuel cells can be formed by extrusion and then subjected to a thermal treatment in air at a temperature of 115O0C. In this the organic binder components can be burnt out and sintering can be carried out until a material strength for further processing is reached. In a subsequent processing step it can be reduced at 8000C in a hydrogen atmosphere and in this way the metallic phases of Ni, Cu and Co can be maintained.
Example 2
For the manufacture of Ni-Cu-Fe-Co-GDC anode materials powdered nickel oxide, copper oxide, iron oxide and GDC are mixed such that after the reduction, the metal phases in the material are at least 30 vol.-% and the contents in the metal phase of the Ni are 70 vol.-%, Cu is 25 vol.-%, Fe is 3 vol.-% and Co is 2 vol. -%.
After a homogenous mixing of the oxide powders a binder system is added to make a feedstock that has a viscosity suitable for injection moulding or extrusion. In this way anodes for high- temperature fuel cells can be formed by extrusion and then subjected to a thermal treatment in air at a temperature of 12500C. In this the organic binder components can be burnt out and sintering can be carried out until a material strength for further processing is reached. In a subsequent processing step it can be reduced at 12000C in a hydrogen atmosphere and in this way the metallic phases of Ni, Cu, Fe and Co can be maintained.

Claims

Claims
1. Anode material for high- temperature fuel cells that is formed of nickel, copper and at least one further metal.
2. Anode material according to claim 1 characterised in that the further metal is a transition metal .
3. Anode material according to claim 1 characteri- sed in that the further metal is an alkaline- or alkaline earth metal.
4. Anode material according to claim 1 characterised in that the further metal is iron.
5. Anode material according to one of the previous claims characterised in that the further metal is selected from Co, V, Cr, Pt, Rh, Ag, Au, Mo, W, Pd, Ru, Mg and Li.
6. Anode material according to one of the previous claims characterised in that the content of the further metal is in the range between 0.5 vol.-% to 95 vol. -%.
7. Anode material according to claim 6 characterised in that the content of the further metal is in the range between 0.5 vol.-% and 10 vol.-%.
8. Anode material according to one of the previous claims characterised in that additionally it contains a ceramic material .
9. Anode material according to claim 8 character- ised in that the ceramic material is an ion conductor, especially an oxygen ion conductor and/or a mixed conductor.
10. Anode material according to claim 8 or 9 characterised in that the ceramic material is selected from a cerium oxide compound, a gallate, a bismuth oxide compound and a zirconium oxide compound .
11. Anode material according to one of the claims 8 to 10 characterised in that the content of the ceramic material possesses is in the range between 5 vol.-% to 70 vol.-%.
12. Anode material according claim 11 characterised in that the content of the ceramic material is in the range between 25 vol.-% and 50 vol.-%.
13. Anode material according claim 11 characterised in that the content of the ceramic material is in the range between 30 vol.-% and 40 vol.-%.
14. Anode material according to one of the previous claims characterised in that it contains as a dopant and/or additive at least one oxide of an alkaline- or alkaline earth metal, a titanate and/or a vanadate with a volume ratio in the range between 0.1 vol.-% to 50 vol.-%.
15. Anode material according to one of the previous claims characterised in that the material has at least partly and/or in some sections a face- centered cubic lattice.
PCT/EP2009/008884 2008-12-11 2009-12-11 Anode material for high-temperature fuel cells WO2010066444A1 (en)

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DE102008062615.5 2008-12-11

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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2517928A (en) * 2013-09-04 2015-03-11 Ceres Ip Co Ltd Metal supported solid oxide fuel cell
US9793551B2 (en) 2013-05-17 2017-10-17 Universiti Brunei Darussalam Cu-based cermet materials for solid oxide fuel cells
US10003080B2 (en) 2013-09-04 2018-06-19 Ceres Intellectual Property Company Limited Process for forming a metal supported solid oxide fuel cell
CN113363543A (en) * 2021-06-01 2021-09-07 中国科学技术大学 Solid oxide cell fuel electrode material, preparation method thereof and solid oxide cell

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20060257718A1 (en) * 2005-05-12 2006-11-16 Kazunori Sato Electrode material and fuel cell
US20080070084A1 (en) * 2006-09-19 2008-03-20 Tatsumi Ishihara Fuel electrode precursor of low shrinkage rate in an electric power generation cell for a solid oxide fuel cell
US20080124613A1 (en) * 2006-10-16 2008-05-29 Gur Turgut M Multi-functional cermet anodes for high temperature fuel cells
EP1939967A1 (en) * 2006-12-01 2008-07-02 Atomic Energy Council - Institute of Nuclear Energy Research Nanostructured composite anode with nano gas channels and atmosphere plasma spray manufacturing method thereof

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20060257718A1 (en) * 2005-05-12 2006-11-16 Kazunori Sato Electrode material and fuel cell
US20080070084A1 (en) * 2006-09-19 2008-03-20 Tatsumi Ishihara Fuel electrode precursor of low shrinkage rate in an electric power generation cell for a solid oxide fuel cell
US20080124613A1 (en) * 2006-10-16 2008-05-29 Gur Turgut M Multi-functional cermet anodes for high temperature fuel cells
EP1939967A1 (en) * 2006-12-01 2008-07-02 Atomic Energy Council - Institute of Nuclear Energy Research Nanostructured composite anode with nano gas channels and atmosphere plasma spray manufacturing method thereof

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9793551B2 (en) 2013-05-17 2017-10-17 Universiti Brunei Darussalam Cu-based cermet materials for solid oxide fuel cells
GB2517928A (en) * 2013-09-04 2015-03-11 Ceres Ip Co Ltd Metal supported solid oxide fuel cell
WO2015033104A1 (en) * 2013-09-04 2015-03-12 Ceres Intellectual Property Company Limited Metal supported solid oxide fuel cell
US9236614B2 (en) 2013-09-04 2016-01-12 Ceres Intellectual Property Company Limited Metal supported solid oxide fuel cell
GB2517928B (en) * 2013-09-04 2018-02-28 Ceres Ip Co Ltd Metal supported solid oxide fuel cell
US10003080B2 (en) 2013-09-04 2018-06-19 Ceres Intellectual Property Company Limited Process for forming a metal supported solid oxide fuel cell
US10008726B2 (en) 2013-09-04 2018-06-26 Ceres Intellectual Property Company Limited Metal supported solid oxide fuel cell
CN113363543A (en) * 2021-06-01 2021-09-07 中国科学技术大学 Solid oxide cell fuel electrode material, preparation method thereof and solid oxide cell

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