CN111403752A - Low-temperature solid oxide fuel cell composite cathode material and preparation method of single fuel cell thereof - Google Patents
Low-temperature solid oxide fuel cell composite cathode material and preparation method of single fuel cell thereof Download PDFInfo
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- H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
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Abstract
A low-temperature solid oxide fuel cell composite cathode material and a preparation method of a single fuel cell thereof belong to the field of chemical power source solid oxide fuel cell materials. It solves the problems of low electrocatalytic activity and poor high-temperature chemical stability of the existing cathode material. Materials: from Bi0.5Sr0.5Fe0.9Sb0.1O3‑Cathode and L a0.8Sr0.2O3‑An electron conductor. The method comprises the following steps: firstly, mixing a cathode and an electronic conductor, and then adding terpineol to obtain mixed slurry; secondly, brushing the mixed slurry on the surface of the GDC buffer layer, drying and sintering to obtain the composite cathode which is Bi0.5Sr0.5Fe0.9Sb0.1O3‑‑La0.8Sr0.2O3‑The unit fuel cell of (1). The invention effectively increases the output power of the single fuel cell, improves the electrocatalysis performance of the fuel cell, and has good high-temperature chemical stability. The invention is suitable for the composite cathode material of the low-temperature solid oxide fuel cell.
Description
Technical Field
The invention belongs to the field of chemical power source solid oxide fuel cell materials.
Background
A solid oxide fuel cell is an all-solid-state energy conversion device that can directly convert chemical energy of fuel into electrical energy, and is known as a green energy source in the 21 st century because of its advantages of high energy conversion efficiency, low pollutant emission, fuel flexibility, and the like. However, the conventional solid oxide fuel cell has problems of poor high-temperature chemical stability and loss of activation polarization of the cathode material due to high operation temperature (1000 ℃). Therefore, the search for low temperature (400-600 ℃) solid oxide fuel cells has become a hot spot of research. But the catalytic activity of the electrode rapidly decreases with a decrease in operating temperature and the ohmic polarization resistance of the electrolyte also increases. The conventional solid oxide battery cathode material has limited its practical application range due to low ion-electron conductivity and catalytic activity below 800 ℃. Therefore, the development of new cathode materials with high electrocatalytic properties is an important task for the development of low temperature solid oxide fuel cells.
Disclosure of Invention
The invention aims to solve the problems of low electrocatalytic activity and poor high-temperature chemical stability of the conventional cathode material, and provides a low-temperature solid oxide fuel cell composite cathode material and a preparation method of a single fuel cell thereof.
The composite cathode material for low temperature solid oxide fuel cell consists of Bi in 60-90 wt%0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-An electron conductor.
The method for preparing the single fuel cell by adopting the low-temperature solid oxide fuel cell composite cathode material is realized by the following steps:
firstly, 60 to 90 weight percent of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-Mixing the electronic conductors, adding terpineol, and uniformly mixing to obtain mixed slurry;
secondly, brush-coating the mixed slurry on the surface of a half-cell GDC buffer layer with NiO-YSZ/YSZ/GDC anode support, drying for 4h at 120 ℃ in a drying oven, and sintering for 4h at 900 ℃ in a muffle furnace to obtain a composite cathode which is Bi0.5Sr0.5Fe0.9Sb0.1O3--La0.8Sr0.2O3-The single fuel cell is prepared by the low-temperature solid oxide fuel cell composite cathode material.
The invention has the advantages that:
the composite cathode material of the low-temperature solid oxide fuel cell has the advantage that L a is added into the cathode material0.8Sr0.2O3-The electronic conductor can improve the ion-electron mixed conductivity of the electrode, and can prolong the reaction active area of the air-electrode-electrolyte three-phase interface, so that the active interface is expanded to the whole cathode layer, thereby effectively increasing the output power of the single fuel cell and improving the electrocatalysis performance of the fuel cell.
The composite cathode has good high-temperature chemical stability within the temperature range of 400-600 ℃; the single fuel cell prepared by adopting the low-temperature solid oxide fuel cell composite cathode material has the cell output power of 1.05Wcm at 600 DEG C-2And with Bi0.5Sr0.5Fe0.9Sb0.1O3-The output power of the single fuel cell as the cathode is 0.57Wcm-2The prepared composite cathode of the solid oxide fuel cell effectively increases the output power of the single fuel cell and improves the electrocatalytic performance of the fuel cell.
The invention has the advantages of easily obtained raw materials, simple preparation method and convenient operation.
The invention is suitable for the composite cathode material of the low-temperature solid oxide fuel cell.
Drawings
FIG. 1 shows Bi in example0.5Sr0.5Fe0.9Sb0.1O3-Cathode and L a0.8Sr0.2O3-X-ray diffraction spectrum of the electronic conductor mixture powder, wherein o is represented by Bi0.5Sr0.5Fe0.9Sb0.1O3-Diffraction peak of cathode, indicated as L a0.8Sr0.2O3-Diffraction peaks of the electron conductor;
FIG. 2 shows a composite cathode 70Bi prepared in the examples0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-A surface topography map after sintering for 4h at 900 ℃;
FIG. 3 shows example 70Bi0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-Is a composite cathode and Bi0.5Sr0.5Fe0.9Sb0.1O3-Current-power density and current-voltage curves at 600 ℃ for a fuel cell unit as cathode, where- ● -represents 70Bi0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-Current-Power Density Curve of a Fuel cell Unit as composite cathode, - ▲ -expressed in Bi0.5Sr0.5Fe0.9Sb0.1O3-Current-power density curve of the fuel cell unit as cathode, - ○ -expressed as 70Bi0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-Current-voltage curve of single fuel cell as composite cathode, - △ -expressed in Bi0.5Sr0.5Fe0.9Sb0.1O3-Current-voltage curve of the unit fuel cell as cathode.
Detailed Description
The technical solution of the present invention is not limited to the following specific embodiments, but includes any combination of the specific embodiments.
The first embodiment is as follows: the embodiment of the invention relates to a low-temperature solid oxide fuel cell composite cathode material which is prepared by weightBi accounting for 60 to 90 percent of the weight percentage0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-An electron conductor.
The second embodiment is as follows: the difference between the present embodiment and the first embodiment is that it is composed of 70-80 wt% of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 20% -30% of L a0.8Sr0.2O3-An electron conductor. The rest is the same as the first embodiment.
The third concrete implementation mode: this embodiment differs from the first embodiment in that it consists of 75% by weight of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 25% L a0.8Sr0.2O3-An electron conductor. The rest is the same as the first embodiment.
The fourth concrete implementation mode: the method for preparing the single fuel cell by adopting the low-temperature solid oxide fuel cell composite cathode material is realized by the following steps:
firstly, 60 to 90 weight percent of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-Mixing the electronic conductors, adding terpineol, and uniformly mixing to obtain mixed slurry;
secondly, brush-coating the mixed slurry on the surface of a half-cell GDC buffer layer with NiO-YSZ/YSZ/GDC anode support, drying for 4h at 120 ℃ in a drying oven, and sintering for 4h at 900 ℃ in a muffle furnace to obtain a composite cathode which is Bi0.5Sr0.5Fe0.9Sb0.1O3--La0.8Sr0.2O3-The single fuel cell is prepared by the low-temperature solid oxide fuel cell composite cathode material.
In the second step of the present embodiment, the NiO-YSZ/GDC anode support half cell, where NiO-YSZ is the anode, YSZ is the electrolyte, and GDC is the buffer layer; purchased from Ningbosufu energy Co.
The fifth concrete implementation mode: the difference between the fourth embodiment and the fourth embodiment is that in the first step, 70% by weight of Bi is added0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 30% L a0.8Sr0.2O3-The electron conductors are mixed. Other steps and parameters are the same as those in the fourth embodiment.
The sixth specific implementation mode: the difference between this embodiment and the embodiment in four or five is that in the step one, Bi is0.5Sr0.5Fe0.9Sb0.1O3-Preparing a cathode: according to the chemical formula Bi0.5Sr0.5Fe0.9Sb0.1O3-Weighing raw material Bi according to stoichiometric ratio2O3、SrCO3、Fe2O3And Sb2O3Uniformly mixing, then placing the mixture in a planetary ball mill for grinding for 12-24 h, and sintering at 900-1100 ℃ for 12-24 h to obtain Bi0.5Sr0.5Fe0.9Sb0.1O3-And a cathode. The other steps and parameters are the same as those in the fourth or fifth embodiment.
The seventh embodiment: sixth embodiment is different from the sixth embodiment in that Bi is as described above2O3、SrCO3、Fe2O3And Sb2O3The purities of the compounds are all more than 99.99 percent. Other steps and parameters are the same as those in the sixth embodiment.
The specific implementation mode is eight: the sixth difference from the sixth embodiment is that the rotation speed of the planetary ball mill is 800r/min, the ball-material ratio is 15: 1. other steps and parameters are the same as those in the sixth embodiment.
Ninth embodiment, the difference between the fourth and fifth embodiments is that L a is used in the first step0.8Sr0.2O3-Preparation of an electronic conductor 6g of L a (NO)3)3·6H2O and 0.74g Sr (NO)3)3Dissolving in 200ml of deionized water, and then dissolving in 40-60 ml of deionized waterHeating and stirring at the temperature of below 6.72 ℃ to form a mixed solution, adding 6.72g of citric acid, continuously heating and stirring until the solution is transparent, heating at the temperature of 120 ℃ to evaporate and remove water to obtain a mixed sol, drying at the temperature of 180 ℃ for 6 hours to obtain a gel, and sintering the gel in a muffle furnace at the temperature of 800 ℃ for 10 hours to obtain L a0.8Sr0.2O3-An electron conductor. The other steps and parameters are the same as those in the fourth or fifth embodiment.
The detailed implementation mode is ten: the difference between this embodiment and the embodiment in four or five is that in the step one, Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and L a0.8Sr0.2O3-The volume ratio of the total mass of the electronic conductor to the terpineol is 0.1g:0.2 ml. The other steps and parameters are the same as those in the fourth or fifth embodiment.
The concrete implementation mode eleven: the fourth or fifth embodiment is different from the fourth or fifth embodiment in that the thickness of the mixed slurry coated in the second step is 0.15-0.30 mm. The other steps and parameters are the same as those in the fourth or fifth embodiment.
The beneficial effects of the present invention are demonstrated by the following examples:
example (b):
the method for preparing the single fuel cell by adopting the low-temperature solid oxide fuel cell composite cathode material is realized by the following steps:
firstly, 70 percent of Bi by weight percentage0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 30% L a0.8Sr0.2O3-Mixing the electronic conductors, adding terpineol, and uniformly mixing to obtain mixed slurry;
secondly, brush-coating the mixed slurry on the surface of a half cell GDC buffer layer with NiO-YSZ/YSZ/GDC anode support, drying for 4h at 120 ℃ in a drying oven, and sintering for 4h at 900 ℃ in a muffle furnace to obtain a composite cathode of 70Bi0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-Namely, the low-temperature solid oxide fuel cell composite cathode is completedThe electrode material is used for preparing a single fuel cell.
In the first step of this example, Bi0.5Sr0.5Fe0.9Sb0.1O3-Preparing a cathode: 5.00 g of Bi are weighed2O31.90 g SrCO31.85 g Fe2O3And 0.75 g Sb2O3Uniformly mixing, then placing the mixture into a planetary ball mill for grinding for 20 hours, and sintering the mixture for 20 hours at 1000 ℃ to obtain Bi0.5Sr0.5Fe0.9Sb0.1O3-And a cathode.
L a in the first step of this embodiment0.8Sr0.2O3-Preparation of an electronic conductor 6g of L a (NO)3)3·6H2O and 0.74g Sr (NO)3)3Dissolving in 200ml deionized water, heating and stirring at 50 ℃ to form a mixed solution, adding 6.72g of citric acid, continuously heating and stirring until the solution is transparent, heating at 120 ℃ to evaporate and remove water to obtain a mixed sol, drying at 180 ℃ for 6 hours to obtain a gel, and sintering the gel in a muffle furnace at 800 ℃ for 10 hours to obtain L a0.8Sr0.2O3-An electron conductor.
(1) Research on high-temperature chemical stability and micro-morphology of low-temperature solid oxide fuel cell composite cathode material
Bi prepared by the above method0.5Sr0.5Fe0.9Sb0.1O3-Cathode and L a0.8Sr0.2O3-The electronic conductors are uniformly mixed according to the mass ratio of 1:1, and are ground for 12 hours in a planetary ball mill by taking zirconia microspheres as a grinding medium and absolute ethyl alcohol as a dispersing agent to obtain a uniform mixture. Sintering at 1100 deg.C in air for 24h, grinding for the second time to obtain powder, and performing phase detection on the composite cathode with powder X-ray diffractometer;
the results demonstrate that Bi is sintered at 1100 ℃ for 24h0.5Sr0.5Fe0.9Sb0.1O3-Cathode and L a0.8Sr0.2O3-The electron conductor does not undergo chemical reaction (see fig. 1), which indicates that the two have good high-temperature chemical compatibility.
Scanning electron microscope is used for observing 70Bi with the electron conductor composite mass ratio of 30%0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-The micro-morphology of the composite cathode;
the results show that the composite cathode prepared according to the above process conditions has a certain porous structure and a certain sintering connection among particles, which is beneficial to the transmission and diffusion of gas (see fig. 2).
(2) Research on electrochemical performance of composite cathode material
Tested at 700 ℃ with 70Bi0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-Is a composite cathode and Bi0.5Sr0.5Fe0.9Sb0.1O3-The I-P and I-V curves for a single fuel cell with the cathode; the results show that 70Bi is present at 600 DEG C0.5Sr0.5Fe0.9Sb0.1O3--30La0.8Sr0.2O3-The output power of the single fuel cell as the composite cathode is 1.05Wcm-2And with Bi0.5Sr0.5Fe0.9Sb0.1O3-The output power of the single fuel cell as the cathode is 0.57Wcm-2(see FIG. 3). The composite cathode of the solid oxide fuel cell prepared by the embodiment effectively increases the output power of the single fuel cell and improves the electrocatalytic performance of the fuel cell.
Claims (10)
1. The composite cathode material for low temperature solid oxide fuel cell features that it contains Bi in 60-90 wt%0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-An electron conductor.
2. The low-temperature solid oxide fuel cell composite cathode material as claimed in claim 1, wherein the low-temperature solid oxide fuel cell composite cathode material is prepared by mixing the following components in percentage by weightFrom 70% to 80% of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 20% -30% of L a0.8Sr0.2O3-An electron conductor.
3. The low-temperature solid oxide fuel cell composite cathode material as claimed in claim 1, wherein the low-temperature solid oxide fuel cell composite cathode material comprises 75 wt% of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 25% L a0.8Sr0.2O3-An electron conductor.
4. The method for preparing the single fuel cell by adopting the low-temperature solid oxide fuel cell composite cathode material as claimed in claim 1 is characterized by comprising the following steps:
firstly, 60 to 90 weight percent of Bi0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 10% -40% of L a0.8Sr0.2O3-Mixing the electronic conductors, adding terpineol, and uniformly mixing to obtain mixed slurry;
secondly, brush-coating the mixed slurry on the surface of a half-cell GDC buffer layer with NiO-YSZ/YSZ/GDC anode support, drying for 4h at 120 ℃ in a drying oven, and sintering for 4h at 900 ℃ in a muffle furnace to obtain a composite cathode which is Bi0.5Sr0.5Fe0.9Sb0.1O3--La0.8Sr0.2O3-The single fuel cell is prepared by the low-temperature solid oxide fuel cell composite cathode material.
5. The method for preparing single fuel cell by using low-temperature solid oxide fuel cell composite cathode material according to claim 4, wherein 70% of Bi by weight percentage is added in the step one0.5Sr0.5Fe0.9Sb0.1O3-Cathode and 30% L a0.8Sr0.2O3-The electron conductors are mixed.
6. The method of claim 4, wherein the Bi is selected from the group consisting of Bi, Bi0.5Sr0.5Fe0.9Sb0.1O3-Preparing a cathode: according to the chemical formula Bi0.5Sr0.5Fe0.9Sb0.1O3-Weighing raw material Bi according to stoichiometric ratio2O3、SrCO3、Fe2O3And Sb2O3Uniformly mixing, then placing the mixture in a planetary ball mill for grinding for 12-24 h, and sintering at 900-1100 ℃ for 12-24 h to obtain Bi0.5Sr0.5Fe0.9Sb0.1O3-And a cathode.
7. The method for preparing single fuel cell by using low-temperature solid oxide fuel cell composite cathode material according to claim 6, wherein the Bi is2O3、SrCO3、Fe2O3And Sb2O3The purities of the compounds are all more than 99.99 percent.
8. The method for preparing single fuel cell by using low-temperature solid oxide fuel cell composite cathode material according to claim 4, wherein L a is obtained in step one0.8Sr0.2O3-Preparation of an electronic conductor 6g of L a (NO)3)3·6H2O and 0.74g Sr (NO)3)3Dissolving the mixture in 200ml of deionized water, heating and stirring the mixture at 40-60 ℃ to form a mixed solution, adding 6.72g of citric acid, continuously heating and stirring the solution until the solution is transparent, heating the solution at 120 ℃ to evaporate and remove water to obtain a mixed sol, drying the mixed sol at 180 ℃ for 6 hours to obtain a gel, and sintering the gel in a muffle furnace at 800 ℃ for 10 hours to obtain L a0.8Sr0.2O3-An electron conductor.
9. The method of claim 4 using low temperature solid oxide fuelThe method for preparing the single fuel cell by using the composite cathode material of the cell is characterized in that Bi is used in the step one0.5Sr0.5Fe0.9Sb0.1O3-Cathode and L a0.8Sr0.2O3-The volume ratio of the total mass of the electronic conductor to the terpineol is 0.1g:0.2 ml.
10. The method for preparing the single fuel cell by adopting the low-temperature solid oxide fuel cell composite cathode material as claimed in claim 4, wherein the thickness of the mixed slurry brush-coated in the step two is 0.15-0.30 mm.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| CN114349059A (en) * | 2021-12-22 | 2022-04-15 | 南华大学 | Preparation and application of novel uranium-fixed solid oxide fuel cell cathode material |
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| CN103441294A (en) * | 2013-09-13 | 2013-12-11 | 哈尔滨工业大学 | Method and device for generating power by using carbon-containing garbage as fuel of solid oxide fuel cell (SOFC) |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| 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 |
| CN114349059A (en) * | 2021-12-22 | 2022-04-15 | 南华大学 | Preparation and application of novel uranium-fixed solid oxide fuel cell cathode material |
| CN114349059B (en) * | 2021-12-22 | 2023-10-20 | 南华大学 | Preparation and application of novel uranium-fixed solid oxide fuel cell cathode material |
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Application publication date: 20200710 |