CN106450346A - Ca-doping medium-low-temperature solid oxide fuel battery cathode material - Google Patents
Ca-doping medium-low-temperature solid oxide fuel battery cathode material Download PDFInfo
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- CN106450346A CN106450346A CN201610910528.1A CN201610910528A CN106450346A CN 106450346 A CN106450346 A CN 106450346A CN 201610910528 A CN201610910528 A CN 201610910528A CN 106450346 A CN106450346 A CN 106450346A
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- cathode material
- oxide fuel
- solid oxide
- temperature solid
- fuel cell
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid 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
Abstract
The invention provides a Ca-doping medium-low-temperature solid oxide fuel battery cathode material, which has the composition general formula of yPrBa1-xCaxCoCuO5+delta-(1-y)M, wherein x is 0.001 to 1.0; delta is 0 to 1.0; y is 10 weight percent to 100 weight percent; M is one or the combination of more than one of Gd0.1Ce0.9O1.95, Gd0.2Ce0.8O1.9, Sm0.1Ce0.9O1.95, Sm0.2Ce0.9O1.9, Y0.16Zr0.92O2.08 and Sc0.2Ce0.01Zr0.89O2.1. The cathode material provided by the invention has the advantages that the Ca is doped into a site A of Pr BaCuCoO5+delta so as to improve the material electric conductivity and the electric chemical performance; meanwhile, the heat expansion coefficient of the material is reduced; the SOFC cathode material with excellent performance can be obtained, so that the cathode material has high oxygen catalytic reduction activity and electric conductivity in the medium-low temperature range; the polarization impedance at 700 DEG C is only 0.014 ohm cm<2>; the maximum output power of the corresponding single battery is as high as 1331 mW cm<-2> at 800 DEG C.
Description
Technical field
The invention belongs to battery cathode material preparation field, especially relate to be applicable to the middle low temperature of the calcium analysis of middle low temperature
The cathode material of SOFC.
Background technology
With the transition exploitation of fossil energy with inefficient use, environment goes from bad to worse, these problems seriously govern through
The sustainable development of Ji.SOFC (SOFC) as the energy conversion device of a kind of green owing to having energy concurrently
The features such as transformation efficiency is high, fuel is widely applicable are expected to make the problems referred to above be alleviated.During SOFC operating temperature is reduced to low
Temperature scope (500-800 DEG C) and to have preferable thermally matched performance be to realize its business-like key.But, with work temperature
The reduction of degree, the oxygen catalytic reduction activity of conventional cathode material is remarkably decreased, and then causes the notable of sofc cathode polarization impedance
Increase the deep fades with cell output.Cathode material and the mismatch of electrolyte heat make cathode material performance simultaneously
Deep fades occurs.Therefore develop and there is in middle low temperature range hyperoxia catalytic reduction activity and high thermally matched cathode material
Become one of practical the most key factor of restriction SOFC.
Reducing solid-oxide fuel cell operating temperature at present, exploitation medium and low temperature solid-oxide fuel cell is combustion
One of hot issue of material field of batteries research, lowers however as operating temperature, and the catalysis activity of cathode material significantly reduces.
Basic demand for middle low temperature solid-state oxide fuel battery cathode material is：Material have at the working temperature higher oxygen from
Son-Electronic Transport of Two Benzene, good chemical catalysis activity and heat endurance.Cobalt-based perovskite structure cathode material has higher
Oxonium ion-Electronic Transport of Two Benzene, and there is preferably catalysis activity, but its thermal coefficient of expansion differs bigger with electrolyte
(T.V.Aksenova,L.Yu.Gavrilova,A.A.Yaremchenko,V.A.Cherepanov,V.V.Kharton,
Oxygen nonstoichiometry,thermal expansion and high-temperature electrical
properties of layered NdBaCo2O5+δand SmBaCo2O5+δ), its negative electrode is with electrolyte thermal matching relatively
Difference, cobalt-based double-perovskite cathode material thermal coefficient of expansion is high main and Co 3+Content is relevant.Zhiwen Zhu et al. finds B position Cu
After doping, its thermal coefficient of expansion significantly reduces, but electrical conductivity and chemical property reduce (Zhiwen Zhu, Zetian simultaneously
Tao,Lei Bi,Wei Liu,Investigation of SmBaCuCoO5+ddouble-perovskite as cathode
for proton-conducting solid oxide fuel cells,Materials Research Bulletin
2010,45:1771).
Content of the invention
For Shortcomings in prior art, it is thus achieved that relatively low thermel expansion coefficient and preferable electrochemical Iy active cathode material,
The invention provides the intermediate temperature solid oxide fuel cell cathode material of a kind of calcium analysis, Ca is doped to Pr
BaCuCoO5+δBa position, to improve material electric conductivity, chemical property, simultaneously reduce material thermal coefficient of expansion, it is thus achieved that performance
Excellent sofc cathode material so that cathode material has hyperoxia catalytic reduction activity and electrical conductivity in middle low temperature range.
The intermediate temperature solid oxide fuel cell cathode material of a kind of calcium analysis, its composition formula is：yPrBa1- xCaxCoCuO5+δ-(1-y) M, wherein x=0.001-1.0, δ=0-1.0, y=10wt.%-100wt.%, M are electrolyte.
Preferably, x=0.1-1.0.
Preferably, x=0.3, the structural formula of described cathode material for solid-oxide fuel cell is：
yPrBa0.7Ca0.3CoCuO5+δ-(1-y)M.
Preferably, x=0.4, the structural formula of described cathode material for solid-oxide fuel cell is：
yPrBa0.6Ca0.4CoCuO5+δ-(1-y)M.
Preferably, x=0.5, the structural formula of described cathode material for solid-oxide fuel cell is：
yPrBa0.5Ca0.5CoCuO5+δ-(1-y)M.
Preferably, described M is Gd0.1Ce0.9O1.95,Gd0.2Ce0.8O1.9,Sm0.1Ce0.9O1.95,Sm0.2Ce0.9O1.9,
Y0.16Zr0.92O2.08,Sc0.2Ce0.01Zr0.89O2.1In one or more combination.
The material of the present invention can be prepared using the following method：
Dissolving ethylenediamine tetra-acetic acid (EDTA) in deionized water, dropping ammoniacal liquor regulation solution ph is 7, obtains mixed liquor
A；Dissolving citric acid in deionized water, dropping ammoniacal liquor regulation solution ph is 7, obtains mixed liquid B；By Pr (NO3)3·6H2O、
Ba(NO3)2、Ca(NO3)2·4H2O、Cu(NO3)2·4H2O and Co (NO3)2·6H2O is dissolved in deionized water, obtains slaine molten
Liquid C；Adding in mixed liquor A by metal salt solution C and mixed liquid B, in 80 DEG C of water-baths, heating stirring 12h, is coagulated after being evaporated
Glue；Described gel obtains the precursor powder of described battery cathode material through 350 DEG C of K cryogenic treatment；Described precursor powder is existed
High temperature sintering furnace i.e. can get described battery cathode material with 1000 DEG C of calcining 2h.
Beneficial effects of the present invention：
Cathode material of the present invention, by being doped to Pr BaCuCoO by Ca5+δBa position, to improve conductivity of material
Rate, chemical property, reduce the thermal coefficient of expansion of material, it is thus achieved that the sofc cathode material of excellent performance so that negative electrode material simultaneously
Material has hyperoxia catalytic reduction activity and electrical conductivity in middle low temperature range.As used component to be 80wt.%
PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95Symmetrical cells prepared by sample, negative electrode/Gd0.1Ce0.9O1.95/ cloudy
Pole, is only 0.014 Ω cm at the polarization impedances of 700 DEG C2, prepared anode-supported monocell, Ni-YSZ/YSZ/GDC/ is cloudy
Pole, is up to 1331mW cm at the maximum generation power of 800 DEG C-2.
Brief description
Fig. 1 is for 80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95Symmetrical cells for negative electrode exists
The specific surface polarization impedance value of 600-800 DEG C in air.
Fig. 2 is for 80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95For the monocell of negative electrode at sky
The electric discharge behavior curve of 600-800 DEG C in gas.
Detailed description of the invention
Below in conjunction with the accompanying drawings and specific embodiment the present invention is further illustrated, but protection scope of the present invention is simultaneously
It is not limited to this.
Embodiment 1：PrBa0.999Ca0.001CoCuO5+δPrepared by powder
Weighing EDTA (analyzing pure) 11.6869g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 6, obtains mixing
Liquid A；Weighing citric acid (analyzing pure) 16.8112g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 6, obtains mixed liquor
B；Weigh Pr (NO3)3·6H2O (analyzing pure) 4.3501g, Ba (NO3)2(analyzing pure) 2.6108g, Ca (NO3)2·4H2O (analyzes
Pure) 0.00024g, Co (NO3)2·6H2O (analyzing pure) 2.9103g and Cu (NO3)2·3H2O (analyzing pure) 2.416g be dissolved in from
In sub-water, obtain metal salt solution C；Add metal salt solution C and mixed liquid B in mixed liquor A, then add in 80 DEG C of water-baths
Heat simultaneously stirs 12h, is evaporated and obtains gel；The gel obtaining is obtained battery cathode material through 250 DEG C of K cryogenic treatment
PrBa0.999Ca0.001CoCuO5+δPrecursor powder；Precursor powder is calcined 2h with 1000 DEG C in high temperature sintering furnace,
Obtain described battery cathode material PrBa0.999Ca0.001CoCuO5+δPowder body material.
Embodiment 2：80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95Prepared by powder
Weighing EDTA (analyzing pure) 11.6869g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 6, obtains mixing
Liquid A；Weighing citric acid (analyzing pure) 16.8112g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 6, obtains mixed liquor
B；Weigh Pr (NO3)3·6H2O (analyzing pure) 4.3501g, Ba (NO3)2(analyzing pure) 1.4635g, Ca (NO3)2·4H2O (analyzes
Pure) 0.8502g, Co (NO3)2·6H2O (analyzing pure) 2.9103g and Cu (NO3)2·3H2O (analyzing pure) 2.4160g be dissolved in from
In sub-water, obtain metal salt solution C；Add metal salt solution C and mixed liquid B in mixed liquor A, then add in 80 DEG C of water-baths
Heat simultaneously stirs 12h, is evaporated and obtains gel；The gel obtaining is obtained battery cathode material through 250 DEG C of K cryogenic treatment
PrBa0.4Ca0.6CoCuO5+δPrecursor powder；Precursor powder is calcined 2h with 1000 DEG C in high temperature sintering furnace, i.e. available
Described battery cathode material PrBa0.4Ca0.6CoCuO5+δPowder body material.
By 4.8g PrBa0.4Ca0.6CoCuO5+δPowder and 1.2g Gd0.1Ce0.9O1.95Powder puts into the agate that volume is 50ml
In Nao ball grinder, and drip 15ml absolute ethyl alcohol and carry out ball mill mixing 5h as lubricant with the speed of 400 revs/min.Take out
Biased sample, in air dry oven, 100 DEG C of dry 4h i.e. obtain required 80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%
Gd0.1Ce0.9O1.95Powder.
By 80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95Powder and ethyl cellulose, α-pine tar
Alcohol in mass ratio 50：3：47 make cathode slurry, use silk screen print method to be uniformly coated on densification
Gd0.1Ce0.9O1.95Center, electrolyte disk two sides and monocell piece center, through calcining 2h at 950 DEG C, obtain with
80wt.%PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95For negative electrode, with Gd0.1Ce0.9O1.95Right for electrolyte
Claim battery and monocell.Carry out testing impedance with prepared Symmetrical cells, by Fig. 1 can obtain 80wt.%
PrBa0.4Ca0.6CoCuO5+δ-20wt.%Gd0.1Ce0.9O1.95Material is 0.014 Ω cm the polarization impedance value of 700 DEG C2, say
This material bright shows very excellent oxygen catalysed reductive energy in middle low temperature range, disclosure satisfy that SOFC for cathodic polarization
The requirement of impedance.Carry out electrochemical property test with prepared monocell, Fig. 2 can be obtained the effect that monocell is at 800 DEG C
Rate is up to 1331mW cm-2.
Embodiment 3 50wt.%PrCaCoCuO5+δ-50wt.%Sm0.2Ce0.8O1.9
Weighing EDTA (analyzing pure) 11.67g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 7, obtains mixed liquor
A；Weighing citric acid (analyzing pure) 16.8112g and adding in deionized water, dropping ammoniacal liquor regulation solution ph is 7, obtains mixed liquid B；
Weigh Pr (NO3)3·6H2O (analyzing pure) 4.3501g, Ca (NO3)2·4H2O (analyzing pure) 2.3616g, Co (NO3)2·6H2O
(analyzing pure) 2.9103g and Cu (NO3)2·3H2O (analyzing pure) 2.4160g is dissolved in deionized water, obtains metal salt solution C；
Add metal salt solution C and mixed liquid B in mixed liquor A, then heat in 80 DEG C of water-baths and stir 12h, being evaporated and coagulated
Glue；The gel obtaining is obtained battery cathode material PrCaCoCuO through 350 DEG C of K cryogenic treatment5+δPrecursor powder；By front
Drive body powder in high temperature sintering furnace with 950 DEG C of calcining 2h, i.e. can get described battery cathode material PrCaCoCuO5+δPowder
Material.
By 3g PrCaCoCuO5+δPowder and 3g Sm0.2Ce0.8O1.9Powder is put in the agate jar that volume is 50ml,
And drip 15ml absolute ethyl alcohol and carry out ball mill mixing 5h as lubricant with the speed of 400 revs/min.Take out biased sample,
In air dry oven, 100 DEG C of dry 4h i.e. obtain required 50wt.%PrCaCoCuO5+δ-50wt.%Sm0.2Ce0.8O1.9Powder.
Described embodiment be the present invention preferred embodiment, but the present invention is not limited to above-mentioned embodiment, not
In the case of deviating from the flesh and blood of the present invention, any conspicuously improved, replacement that those skilled in the art can make
Or modification belongs to protection scope of the present invention.
Claims (6)
1. the intermediate temperature solid oxide fuel cell cathode material of a calcium analysis, it is characterised in that its composition formula is：
yPrBa1-xCaxCoCuO5+δ-(1-y) M, wherein x=0.001-1.0, δ=0-1.0, y=10wt.%-100wt.%, M are electricity
Xie Zhi.
2. the intermediate temperature solid oxide fuel cell cathode material of calcium analysis according to claim 1, it is characterised in that
X=0.1-1.0.
3. the intermediate temperature solid oxide fuel cell cathode material of calcium analysis according to claim 1, it is characterised in that
X=0.3, the structural formula of described cathode material for solid-oxide fuel cell is：yPrBa0.7Ca0.3CoCuO5+δ-(1-y)M.
4. the intermediate temperature solid oxide fuel cell cathode material of calcium analysis according to claim 1, it is characterised in that
X=0.4, the structural formula of described cathode material for solid-oxide fuel cell is：yPrBa0.6Ca0.4CoCuO5+δ-(1-y)M.
5. the intermediate temperature solid oxide fuel cell cathode material of calcium analysis according to claim 1, it is characterised in that
X=0.5, the structural formula of described cathode material for solid-oxide fuel cell is：yPrBa0.5Ca0.5CoCuO5+δ-(1-y)M.
6. the intermediate temperature solid oxide fuel cell cathode material of the calcium analysis according to according to any one of claim 1-5,
It is characterized in that, described M is Gd0.1Ce0.9O1.95、Gd0.2Ce0.8O1.9、Sm0.1Ce0.9O1.95、Sm0.2Ce0.9O1.9、
Y0.16Zr0.92O2.08、Sc0.2Ce0.01Zr0.89O2.1In one or more combination.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107086310A (en) * | 2017-04-01 | 2017-08-22 | 江苏大学 | A kind of intermediate temperature solid oxide fuel cell cathode material |
| CN110729491A (en) * | 2019-10-29 | 2020-01-24 | 福州大学 | Method for refining cobalt-containing cathode powder |
| CN112186201A (en) * | 2020-10-22 | 2021-01-05 | 浙江氢邦科技有限公司 | Metal oxide cathode material, composite cathode material and battery |
| CN113178586A (en) * | 2021-04-29 | 2021-07-27 | 黑龙江大学 | Solid oxide fuel cell composite cathode catalyst and preparation method and application thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105932299A (en) * | 2016-04-20 | 2016-09-07 | 江苏大学 | Cathode material with composite phase structure of intermediate-low-temperature solid oxide fuel cell |
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2016
- 2016-10-19 CN CN201610910528.1A patent/CN106450346A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN105932299A (en) * | 2016-04-20 | 2016-09-07 | 江苏大学 | Cathode material with composite phase structure of intermediate-low-temperature solid oxide fuel cell |
Non-Patent Citations (2)
| Title |
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| BIAO WANG等: ""Layered perovskite PrBa0.5Sr0.5CoCuO5+d as a cathode for intermediate-temperature solid oxide fuel cells"", 《JOURNAL OF ALLOYS AND COMPOUNDS》 * |
| LING ZHAO等: ""Novel layered perovskite oxide PrBaCuCoO5+ı as a potential cathode"", 《JOURNAL OF POWER SOURCES》 * |
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107086310A (en) * | 2017-04-01 | 2017-08-22 | 江苏大学 | A kind of intermediate temperature solid oxide fuel cell cathode material |
| CN110729491A (en) * | 2019-10-29 | 2020-01-24 | 福州大学 | Method for refining cobalt-containing cathode powder |
| CN112186201A (en) * | 2020-10-22 | 2021-01-05 | 浙江氢邦科技有限公司 | Metal oxide cathode material, composite cathode material and battery |
| CN112186201B (en) * | 2020-10-22 | 2022-05-27 | 浙江氢邦科技有限公司 | Metal oxide cathode material, composite cathode material and battery |
| CN113178586A (en) * | 2021-04-29 | 2021-07-27 | 黑龙江大学 | Solid oxide fuel cell composite cathode catalyst and preparation method and application thereof |
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