CN109964349A - Method for the anode of fuel cell and for manufacturing anode - Google Patents
Method for the anode of fuel cell and for manufacturing anode Download PDFInfo
- Publication number
- CN109964349A CN109964349A CN201780072550.6A CN201780072550A CN109964349A CN 109964349 A CN109964349 A CN 109964349A CN 201780072550 A CN201780072550 A CN 201780072550A CN 109964349 A CN109964349 A CN 109964349A
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- China
- Prior art keywords
- additive
- anode
- composite material
- fuel cell
- oxide
- 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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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
- H01M4/9041—Metals or alloys
- H01M4/905—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC
- H01M4/9066—Metals or alloys specially used in fuel cell operating at high temperature, e.g. SOFC of metal-ceramic composites or mixtures, e.g. cermets
-
- 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
- H01M4/8605—Porous 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
- 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
- H01M4/8885—Sintering or firing
-
- 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
- H01M4/8885—Sintering or firing
- H01M4/8889—Cosintering or cofiring of a catalytic active layer with another type of layer
-
- 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
-
- 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
Abstract
The present invention is based on a kind of for fuel cell, particularly for the anode (10) of solid oxide fuel cell, and the anode is at least substantially formed by the composite material of ceramet (12), and the composite material is doped at least one additive (14).It proposes, additive (14) has at least 20m2The specific surface area of/g.
Description
Background technique
Itd is proposed it is a kind of for fuel cell, particularly for the anode of solid oxide fuel cell, the anode is extremely
Few substantially to be formed by the composite material of ceramet, the composite material is doped at least one additive.
Summary of the invention
The present invention is based on a kind of for fuel cell, particularly for the anode of solid oxide fuel cell, the anode
It is at least substantially formed by the composite material of ceramet, the composite material is doped with additive.
It proposes, additive has at least 20m2The specific surface area of/g.
" anode " should be especially understood as to the burning gases electrode of fuel cell herein.It herein should be by " fuel
Battery " is especially appreciated that for following equipment, the equipment is arranged for, at least by least one combustion gas being especially continuously conveyed
The chemical reaction of body, especially hydrogen and/or carbon monoxide and at least one cathode gas, especially oxygen can especially be converted into electric energy
And/or thermal energy." composite material of ceramet " is herein it should be particularly understood that by least one of metal matrix ceramics
The composite material that material is constituted, especially cermet." ceramic material " is herein it should be particularly understood that inorganic, nonmetallic
Material.In particular, ceramic material can be at least partly crystallization and/or polycrystalline." nonmetallic " especially answers herein
It being understood as, ceramics do not have the metallic character for being particularly based on metallic bond at least as much as possible, however may include metallic compound,
Such as metal oxide and/or silicide.In particular, ceramics are engineering ceramics.In particular, ceramic material is zirconium oxide, especially
It is yttrium stable zirconium oxide.Metal matrix is especially formed by metal material, preferably nickel.In particular, anode by processing straticulation, especially
The mixture manufacture of printing layer and/or casting film being made of nickel oxide and yttrium stable zirconium oxide.It in particular, can be for by oxygen
Change mixture addition pore former, organic bond and/or other additives that nickel and yttrium stable zirconium oxide are constituted.In particular, positive
Sinter fuel electricity in the case that pole and at least one other functional layer of fuel cell, such as cathode and/or electrolyte are compound into
Pond or half-cell.In particular, anode has the structure of the frame structure interlaced with each other with there are two after the sintering, one of them
It is formed by yttrium stable zirconium oxide, and second is formed by nickel oxide.Suitable pore structure within composite material can deposit
It is being generated by suitable sintering parameter and/or by addition pore former.After sintered anode, nickel oxide is at high temperature, especially
It is converted into nickel in reduction atmosphere at a temperature of between 600 DEG C and 1000 DEG C.
" additive " especially should be understood to following substance herein, and the substance is added to composite material particularly for shadow
Ring material property.In particular, additive is arranged for, during manufacturing anode, especially before sintering process and/or period
It is added to composite material.In particular, additive is arranged for, and influences the sintering character of composite material.Additive is especially set
It sets and is used for, the sintering character of the composite material of anode is made at least substantially to be matched with the sintering character of fuel cell functional layer, sun
Pole is sintered together during fabrication with the fuel cell functional layer.In particular, additive has at least 20m2/ g, advantageously extremely
Few 50m2/ g, especially preferably at least 100m2The specific surface area of/g.
By this design scheme, it is capable of providing and is sintered about manufacture, especially with respect to the other function layer of fuel cell
There is the anode for improving characteristic together.In particular, by the big specific surface area of additive, it can be realized in additive and answer
Advantageously good and/or uniform contact between the component of condensation material, especially nickel oxide and yttrium stable zirconium oxide.Thus, it is possible to
It realizes, acting under advantageously small concentration levels for additive has already appeared.
Moreover, it is proposed that the content of additive in the composite is highest 1000ppm, advantageously highest 750ppm and outstanding
Its advantageously highest 500ppm.In particular, the content of additive relative to composite material basic component and up to
1000ppm.The content of additive especially with respect to nickel oxide and yttrium stable zirconium oxide in composite material quality and highest
For 1000ppm.By the small content of additive, the out-phase that advantageously can be at least avoided as much as within composite material
And advantageously by the negative effect of the characteristic of this different opposite anode, such as conductive reduction minimizes.
Moreover, it is proposed that additive is at least substantially nanometer powder." nanometer powder " herein especially should be understood to as
Lower powder, the powder have maximum 100nm, preferably at most 80nm, advantageously maximum 50nm and especially preferably maximum 20nm
Particle size.By small particle size, advantageously big specific surface area can be realized.
Moreover, it is proposed that additive is at least one metal oxide." metal oxide " especially should be understood to herein
Metal, rare earth metal and/or alkaline-earth metal oxide.Preferably, additive is aluminium oxide.Thereby, it is possible to advantageously
Influence the sintering character of composite material, especially sintering shrinkage.
In addition, proposing that a kind of composite material for by ceramet is manufactured for fuel cell, especially by means of being sintered
The method of its anode for being used for solid oxide fuel cell, wherein by the basic component of composite material before sintering with addition
Agent mixing, the additive is arranged for the sintering character of adjustment composite material and the additive has at least 20m2/g
Specific surface area.In particular, additive is added to composite material before sintered combined material.In at least one method and step
In, the basic component of composite material, especially nickel oxide powder and powdered yttrium stable zirconium oxide are mixed with each other.In particular,
Other additives can be inserted for the mixture of basic component, for example, pore former, organic bond, solvent, softening agent and/or its
His Organic additives.It is that additive is added in the mixture of basic component in another method step.It preferably, is composite material
Basic component add a certain amount of additive before sintering, the amount relative to basic material and correspond to maximum
1000ppm.The basic component and additive of composite material are preferably mixed into before sintering and/or are uniformly melted into cream and/or soft
Mud.In another method step, the mixture being made of the basic component of composite material and additive is processed into anode layer, and
And it is especially sintered under conditions of compound at least one other functional layer of fuel cell.It is advantageously simple thus, it is possible to realize
Single ground and/or reliably manufacture are used for the anode of fuel cell.
In addition, proposing a kind of fuel cell at least one anode according to the present invention.Fuel cell especially constructs
For solid oxide fuel cell (SOFC).Other than anode, fuel cell has at least one cathode and at least one cloth
Set electrolyte between the anode and cathode.Electrolyte is more particularly at least substantially by yttrium stable zirconium oxide, the oxygen of scandium doping
The cerium oxide for changing zirconium, the lanthanum gallate of doping and/or Gd2 O3 is constituted.Anode is more particularly at least substantially by cermet, outstanding
It is by nickeliferous cermet, such as Ni-ZrO2Cermet is constituted.Cathode is more particularly at least substantially by doping alkaline earth gold
The manganate of category, such as LSM, the cobaltatess of adulterated alkaline-earth metal, such as LSC and/or the material, such as similar to perovskite
LSCF is constituted.Thereby, it is possible to provide fuel cell, the fuel cell does not have out-phase at least substantially within anode.
Anode according to the present invention and/or the method according to the present invention for manufacture should not necessarily be limited by hereinbefore retouch herein
The application and embodiment stated.In particular, anode according to the present invention and/or method are in order to meet in the function side wherein described
Formula can have the quantity different in the quantity wherein mentioned from each element, component and unit.
Detailed description of the invention
Other advantages are obtained from following attached drawing description.One embodiment of the present of invention is shown in the accompanying drawings.Attached drawing is said
Bright book and claim include the combination of big measure feature.Those skilled in the art reasonably also individually consider these features and will
A combination thereof is at other significant combinations.
Wherein:
Fig. 1 shows the schematic diagram of the functional layer packet of the fuel cell with the anode being made of composite material, the composite material
Added with additive,
Fig. 2 shows the flow charts of the method for manufacturing anode, and
Fig. 3 shows the comparison of the sintering curre of the anode without additive and the anode with additive.
Specific embodiment
Fig. 1 shows the schematic diagram of the functional layer packet 16 for the fuel cell not being shown specifically.Functional layer packet 16 is applied to especially
On the load-carrying unit 18 of ceramics.Load-carrying unit 18 constructs especially porously.Functional layer packet 16 has anode 10, cathode 20 and arrangement
Electrolyte 38 between anode 10 and cathode 20.Functional layer packet 16 is directly arranged on load-carrying unit 18 with cathode 20.Electrolysis
Zirconium oxide, the lanthanum gallate of doping and/or the oxidation of Gd2 O3 that matter 38 is especially at least substantially adulterated by yttrium stable zirconium oxide, scandium
Cerium is constituted.Cathode 20 is especially at least substantially by the manganate of adulterated alkaline-earth metal, the cobalt acid of such as LSM, adulterated alkaline-earth metal
Salt, such as LSC and/or similar to the material of perovskite, such as LSCF constitute.Anode 10 by ceramet composite material 12,
Especially at least substantially by cermet, preferably by nickeliferous cermet, such as Ni-ZrO2Cermet is constituted.Anode 10
Composite material 12 doped with additive 14.Additive 14 has at least 20m2The specific surface area of/g.Additive 14 is in composite wood
Content in material 12 is up to 1000ppm.Preferably, additive 14 is at least substantially nanometer powder, and the nanometer powder exists
The composite material 12 of anode 10 is added to during manufacture anode 10.Additive 14 is metal oxide, preferably aluminium oxide.
Fig. 2 shows the flow charts of the method for manufacturing anode 10.In first method step 22, by composite material 12
Basic component weighing and mixing.The basic component of composite material 12 is yttrium stable zirconium oxide and nickel oxide.In particular, basic component
It is powdered respectively.Nickel oxide especially has in 4m2/ g and 8m2Specific surface area between/g.As an alternative, nickel oxide can have
Have in 0.5m2/ g and 20m2Specific surface area between/g.Yttrium stable zirconium oxide especially has in 8m2/ g and 12m2Ratio between/g
Surface area.As an alternative, yttrium stable zirconium oxide can have in 0.5m2/ g and 30m2Specific surface area between/g.Yttrium stable zirconium oxide
Especially by with the Y of 8 moles of %2O3Stable zirconium oxide is constituted.As an alternative, zirconium oxide can have 3 moles of % to 12 moles of %.In oxygen
Change the quantity ratio between nickel and yttrium stable zirconium oxide preferably between 65/35 Mol% and 80/20 Mol%.It can be basic component
(nickel oxide and yttrium stable zirconium oxide) mixes other additives.Other additives more particularly to be pore former, for example flame black and/or
PMMA ball, organic bond, such as polyvinyl butyral, ethyl cellulose, methylcellulose and/or acrylate, solvent,
Such as water, ethyl alcohol and/or terpinol, softening agent and/or other organic additives, such as defrother and/or crosslinking agent.Another
In method and step 24, a certain amount of additive 14 is added before sintering for the basic component of composite material 12, the amount is opposite
In basic material and correspond to maximum 1000ppm.Additive 14 adds for example in the form of nanometer powder.As an alternative, it adds
Agent 14 can be added in dissolved form.Additive 14 is preferably alumina powder.Alternatively or additionally, other can be added
Additive, especially other metal oxides, rare-earth oxide and/or alkaline earth oxide.In particular, additive 14 has
There is at least 20m2The specific surface area of/g.As an alternative, additive 14 can have in 20m2/ g and 1000m2Specific surface between/g
Product.
The basic component of composite material 12 and the additive 14 of addition mix before sintering in another method step 26
At and/or uniform chemical conversion cream and/or ooze.For example, first can be by the additive of the basic component of composite material 12 and addition
14 homogenize in advance in epicyclic mixer or by stirring tool and are then processed into three roller tools cream, and the cream is suitble to
In silk-screen printing, pouring technology or other techniques for being used to manufacture thin layer.As an alternative, other mixing apparatus, example are also able to use
Such as dissolvers and/or blender.In another method step 28, it will be made of the basic component of composite material 12 and additive 14
Mixture be poured in particular by means of silk-screen printing, film and/or proportion is processed into anode layer and is being greater than 500 DEG C of temperature
Lower sintering.The nickel oxide of composite material 12 is reduced into nickel in reduction atmosphere and in another method step 30 or can be built into
It is carried out after fuel cell pack.
Fig. 3 indicates graphically the burning of the not sintering curre 32 of the anode by additive doping and anode according to the present invention 10
Tie the comparison of curve 34.Sintering curre 32,34 shows the length variation 36 of percentage respectively about the time 40 of sintering process.It burns
Knot curve 32,34 is shown, and the sum of the basic component of the composite material 12 relative to anode 10 of additive 14 is less than 1000ppm
Doping be enough, it will be apparent that change sintering character, obviously particularly improve sintering shrinkage.
Claims (10)
1. it is a kind of for fuel cell, particularly for the anode of solid oxide fuel cell, the anode at least substantially by
Composite material (12) formation of ceramet, the composite material doped at least one additive (14),
It is characterized in that,
The additive (14) has at least 20m2The specific surface area of/g.
2. anode according to claim 1,
It is characterized in that,
Content of the additive (14) in the composite material (12) is up to 1000ppm.
3. anode according to claim 1 or 2,
It is characterized in that,
The additive (14) is at least substantially nanometer powder.
4. anode according to any one of the preceding claims,
It is characterized in that,
The additive (14) is at least one metal oxide.
5. anode according to any one of the preceding claims,
It is characterized in that,
The additive (14) is aluminium oxide.
6. a kind of composite material (12) for by ceramet is manufactured by means of being sintered for fuel cell, particularly for solid
The method in particular according to anode described in any one of the claims (10) of oxide body fuel cell,
It is characterized in that,
The basic component of the composite material (12) is mixed with additive (14) before sintering, use is set in the additive
In the sintering character for adjusting the composite material (120), and the additive has at least 20m2The specific surface area of/g.
7. according to the method described in claim 6,
It is characterized in that,
Added before sintering a certain amount of additive (14) for the basic component of the composite material (12), the amount relative to
Basic material and correspond to maximum 1000ppm.
8. method according to claim 6 or 7,
It is characterized in that,
The basic component of the composite material (12) and the additive (14) are at least mixed into/uniformly chemical conversion before sintering
Cream and/or ooze.
9. the method according to any one of claim 6 to 8,
It is characterized in that,
Sun is processed and sintered into the mixture being made of the basic component of the composite material (12) and the additive (14)
Pole layer.
10. a kind of fuel cell, the fuel cell has at least one sun according to any one of claim 1 to 5
Pole (10).
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE102016223293.2A DE102016223293A1 (en) | 2016-11-24 | 2016-11-24 | Anode for a fuel cell and method of making the anode |
| DE102016223293.2 | 2016-11-24 | ||
| PCT/EP2017/075198 WO2018095631A1 (en) | 2016-11-24 | 2017-10-04 | Anode for a fuel cell, and method for manufacturing said anode |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| CN109964349A true CN109964349A (en) | 2019-07-02 |
Family
ID=60080775
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201780072550.6A Pending CN109964349A (en) | 2016-11-24 | 2017-10-04 | Method for the anode of fuel cell and for manufacturing anode |
Country Status (5)
| Country | Link |
|---|---|
| EP (1) | EP3545578A1 (en) |
| JP (1) | JP7105772B2 (en) |
| CN (1) | CN109964349A (en) |
| DE (1) | DE102016223293A1 (en) |
| WO (1) | WO2018095631A1 (en) |
Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101112683A (en) * | 2007-06-27 | 2008-01-30 | 山东齐鲁华信实业有限公司 | Cerium zirconium aluminum composite oxides sosoloid with a mesopore structure and method for preparing the same |
| JP2009016350A (en) * | 2007-07-04 | 2009-01-22 | Korea Inst Of Science & Technology | Electrode/electrolyte composite powder for fuel cell, and its preparation method |
| JP2011198758A (en) * | 2010-02-26 | 2011-10-06 | Nippon Telegr & Teleph Corp <Ntt> | Fuel electrode material for solid oxide fuel cell, fuel electrode, solid oxide fuel cell, and manufacturing method of fuel electrode material |
| US20130280638A1 (en) * | 2010-11-29 | 2013-10-24 | Saint-Gobain Centre De Recherches Et D'etudes Europeen | Fused powder of yttria-stabilised zirconia |
| CN104103838A (en) * | 2014-07-08 | 2014-10-15 | 华中科技大学 | Anode protection layer for solid oxide fuel cell, and preparation method and application of anode protection layer |
Family Cites Families (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2006046624A1 (en) * | 2004-10-29 | 2006-05-04 | The Tokyo Electric Power Company, Incorporated | Powdery metal oxide mother particles, powdery metal oxide child particles, process for producing powdery metal oxide particles, powdery composite particles, and electrode for solid oxide fuel cell |
| CA2595854C (en) | 2005-01-31 | 2015-04-14 | Technical University Of Denmark | Redox stable anode |
| DE102005039442A1 (en) * | 2005-08-18 | 2007-02-22 | Forschungszentrum Jülich GmbH | Protection of anode-supported high-temperature fuel cells against reoxidation of the anode |
| JP2007335193A (en) | 2006-06-14 | 2007-12-27 | Nippon Telegr & Teleph Corp <Ntt> | Ceria layer for air electrode of solid oxide fuel cell, and its manufacturing method |
| ES2375407T3 (en) * | 2007-08-31 | 2012-02-29 | Technical University Of Denmark | SEPARATION OF IMPURITY PHASES OF ELECTROCHEMICAL DEVICES. |
| US20120251922A1 (en) | 2011-03-28 | 2012-10-04 | WATT Fuel Cell Corp | Electrode for a solid oxide fuel cell and method for its manufacture |
-
2016
- 2016-11-24 DE DE102016223293.2A patent/DE102016223293A1/en active Pending
-
2017
- 2017-10-04 WO PCT/EP2017/075198 patent/WO2018095631A1/en unknown
- 2017-10-04 CN CN201780072550.6A patent/CN109964349A/en active Pending
- 2017-10-04 EP EP17783435.5A patent/EP3545578A1/en not_active Withdrawn
- 2017-10-04 JP JP2019527890A patent/JP7105772B2/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101112683A (en) * | 2007-06-27 | 2008-01-30 | 山东齐鲁华信实业有限公司 | Cerium zirconium aluminum composite oxides sosoloid with a mesopore structure and method for preparing the same |
| JP2009016350A (en) * | 2007-07-04 | 2009-01-22 | Korea Inst Of Science & Technology | Electrode/electrolyte composite powder for fuel cell, and its preparation method |
| JP2011198758A (en) * | 2010-02-26 | 2011-10-06 | Nippon Telegr & Teleph Corp <Ntt> | Fuel electrode material for solid oxide fuel cell, fuel electrode, solid oxide fuel cell, and manufacturing method of fuel electrode material |
| US20130280638A1 (en) * | 2010-11-29 | 2013-10-24 | Saint-Gobain Centre De Recherches Et D'etudes Europeen | Fused powder of yttria-stabilised zirconia |
| CN104103838A (en) * | 2014-07-08 | 2014-10-15 | 华中科技大学 | Anode protection layer for solid oxide fuel cell, and preparation method and application of anode protection layer |
Also Published As
| Publication number | Publication date |
|---|---|
| WO2018095631A1 (en) | 2018-05-31 |
| JP2019536237A (en) | 2019-12-12 |
| DE102016223293A1 (en) | 2018-05-24 |
| EP3545578A1 (en) | 2019-10-02 |
| JP7105772B2 (en) | 2022-07-25 |
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Application publication date: 20190702 |