CN109818021B - Low-temperature solid oxide fuel cell based on cerium oxide/ferroferric oxide composite material - Google Patents
Low-temperature solid oxide fuel cell based on cerium oxide/ferroferric oxide composite material Download PDFInfo
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- CN109818021B CN109818021B CN201811629494.4A CN201811629494A CN109818021B CN 109818021 B CN109818021 B CN 109818021B CN 201811629494 A CN201811629494 A CN 201811629494A CN 109818021 B CN109818021 B CN 109818021B
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Abstract
The invention discloses a low-temperature solid oxide fuel cell based on cerium oxide/ferroferric oxide composite material, wherein the surfaces of a cathode and an anode of the fuel cell are coated withNCAL nickel foam, the electrolyte layer of the fuel cell being CeO2/Fe3O4A composite material. Namely, the fuel cell of the present invention has the structure: foamed nickel// NCAL// CeO2/Fe3O4// NCAL// nickel foam. The low-temperature solid oxide fuel cell adopts CeO2/Fe3O4The nano composite material is used as an electrolyte layer of the fuel cell, so that the electrode polarization loss in the electrochemical reaction process of the fuel cell is greatly reduced; the electrolyte material has high oxygen ion conduction capability at a low-temperature section, so that the solid oxide fuel cell adopting the electrolyte material can efficiently and stably operate for a long time at the low-temperature section (300-600 ℃).
Description
Technical Field
The invention relates to a low-temperature solid oxide fuel cell based on a cerium oxide/ferroferric oxide composite material, and belongs to the technical field of new energy.
Background
Solid oxide fuel cells can efficiently convert chemical energy in a fuel (e.g., hydrogen, methane, etc.) to electrical energy. The conversion efficiency is not limited by the Carnot cycle, and the efficiency is far higher than that of a thermal generator set. Fuel cells are classified into proton exchange membrane fuel cells, solid oxide fuel cells, alkaline fuel cells, molten carbonate fuel cells, and phosphate fuel cells according to their electrolytes, and among them, solid oxide fuel cells have received much attention because they do not require a noble metal catalyst, have a wide range of material selection, and have high conversion efficiency. However, the current solid oxide fuel cell mainly uses Yttria Stabilized Zirconia (YSZ) as an electrolyte, and YSZ needs a high temperature (about 900 ℃) to obtain a high catalytic activity. Conventional solid oxide fuel cells generally operate at high temperatures. High temperature operation imposes harsh requirements on cell materials and connection materials, and in addition, high temperature operation imposes a challenge on long-term stability of the solid oxide fuel cell. Therefore, the research on the solid oxide fuel cell of the low temperature section (300-600 ℃) has attracted wide attention in recent years.
The electrolyte of the solid oxide fuel cell based on the cathode-electrolyte-anode structure is widely applied to YSZ (yttria stabilized zirconia), has high oxygen ion conduction capacity at about 900 ℃, completes the electrochemical reaction of the fuel cell and outputs electric power. However, this material (YSZ) has good oxygen ion transport capacity only at high temperature, and has little oxygen ion transport capacity when the temperature is lowered to 600 ℃. Therefore, in recent years, more and more technologies for reducing the solid oxide fuel cell mainly focus on two technical routes, one is to develop a thin film technology to reduce the thickness of the electrolyte YSZ so that it can have a high ion transport capability also in the middle temperature range, but subject to the technical limitations, the thickness cannot be infinitely reduced, and the yield of the thin film technology is not very high; and secondly, new materials are developed, and new materials capable of transmitting ions at a low-temperature section are searched.
A fuel cell is a typical electrochemical device, and the function of the intermediate electrolyte is to transport ions and to block the transport of electrons. Doping the ion conductor with a semiconductor is readily reminiscent of the occurrence of short-circuiting, and as such, materials with semiconductor properties have not been used in fuel cells to date. A large number of experimental researches show that materials with semiconductor properties, particularly semiconductor materials with perovskite structures or perovskite-like structures are properly doped in the ionic conductor materials, any short circuit phenomenon does not occur, an enhancement effect is generated, and the output power is obviously increased.
Disclosure of Invention
The technical problem to be solved by the invention is to provide a low-temperature solid oxide fuel cell based on a cerium oxide/ferroferric oxide composite material, wherein an electrolyte material in the fuel cell is a composite of a nano-ion material and a nano-semiconductor material, and a semiconductor-ion heterostructure is formed in the composite electrolyte material, and is favorable for promoting the transmission speed of ions, so that the composite electrolyte material has high conduction capacity to oxygen ions at a low-temperature section, and the solid oxide fuel cell adopting the electrolyte material can efficiently operate at the low-temperature section (600 ℃ C.).
In order to solve the technical problems, the technical scheme adopted by the invention is as follows:
a low-temperature solid oxide fuel cell based on cerium oxide/ferroferric oxide composite material is characterized in that a cathode and an anode of the fuel cell are foamed nickel with NCAL coated on the surfaces, and an electrolyte layer of the fuel cell is CeO2/Fe3O4A composite material.
The fuel cell of the present invention has the structure: foamed nickel// NCAL// CeO2/Fe3O4// NCAL// nickel foam.
Wherein, the nickel foam coated with NCAL on the surface is prepared by the following method: adding the required amount of NCAL (Ni)0.8Co0.15Al0.05LiO2-δ) Gradually adding the powder into terpineol until the mixture is pasty, uniformly coating the pasty mixture on the foamed nickel, and drying the coated foamed nickel in an oven at 200 ℃ for 2 hours to obtain the foamed nickel with NCAL coated on the surface.
Wherein the CeO2/Fe3O4The composite material is prepared by mixing CeO2With Fe3O4The material is synthesized by one step by adopting a chemical wet method, and is obtained by cleaning, filtering, drying, sintering and fully grinding.
CeO as defined above2/Fe3O4The preparation method of the composite material comprises the following specific steps: adding CeO2With Fe3O4Mixing according to the mass ratio of 3:1 to obtain 4g of mixed powder, putting the mixed powder into 20mL of deionized water, stirring for 4 hours at constant temperature, and slowly dropwise adding concentrated nitric acid until Fe3O4The powder completely disappears, then proper amount of sodium carbonate solution is dripped, after full reaction, cleaning and suction filtration are carried out for 4 times, then drying and sintering treatment are carried out, and after sintering, full grinding is carried out to obtain CeO2/Fe3O4And (3) powder.
Wherein the concentration of the sodium carbonate solution is 0.5 mol/L.
Wherein, the sintering is carried out at the heating rate of 10 ℃/min, the temperature is raised from the drying temperature to 700 ℃, the sintering is carried out for 4 hours, and then the natural cooling is carried out to the room temperature.
Wherein the drying temperature is 120 ℃, and the drying time is 12 hours.
The material prepared by the invention is a composite nano material, namely the nano ion material and the nano semiconductor material are compounded, and then the nano compound of the ion material and the semiconductor material is formed by grinding, and a semiconductor-ion heterostructure is formed in the two-phase composite material, namely, an interface of a nano electronic phase and a nano ion phase is formed in an electrolyte layer, and the transmission capability of the material to oxygen ions can be enhanced by the interface of the nano electronic phase and the nano ion phase, so that the output power of the fuel cell is obviously increased; in addition, the interconversion between ferrous and ferric iron can further improve the catalytic activity of the composite material.
The preparation of the low-temperature solid oxide fuel cell of the invention comprises the following steps:
preparing electrode from nickel foam coated with NCAL on its surface, wherein the electrode is circular and has diameter D of 13mm2/Fe3O4Symmetrical structure on both sides, i.e. nickel foam// NCAL// CeO2/Fe3O4A piece of nickel foam/NCAL was placed on the bottom of a tablet die with the NCAL coated side facing up and 0.35g of CeO was taken2/Fe3O4The composite material is placed in a tabletting mold, and another piece of foamed nickel// NCAL is placed in the tabletting mold and placed on the CeO2/Fe3O4And (3) facing downwards the surface of the composite material coated with the NCAL, putting a tabletting mold into a tabletting machine, pressurizing to 8Mpa, keeping the pressure for 5 seconds, and taking out the cell piece to obtain the low-temperature solid oxide fuel cell.
Compared with the prior art, the technical scheme of the invention has the beneficial effects that:
the low-temperature solid oxide fuel cell adopts a chemical wet method to prepare CeO by one-step synthesis2/Fe3O4Fully grinding the composite material to obtain the composite electrolyte material CeO2/Fe3O4The composite material can improve the transmission speed of oxygen ions, so that the composite material has good output power at a low-temperature section, and meanwhile, the composite electrolyte material can also reduce the electrode polarization loss in the electrochemical reaction process of the fuel cell; therefore, the solid oxide fuel cell adopting the electrolyte material can efficiently and stably operate for a long time at a low temperature (300-600 ℃).
Drawings
FIG. 1 is a schematic diagram of the structure of a low temperature solid oxide fuel cell of the present invention;
FIG. 2 shows two CeO species2/Fe3O4Synthetic composite material and pure CeO2I-V and I-P characteristic curves of the fuel cell with the electrolyte material at the test temperature of 550 ℃ respectively; at 550 deg.C, when CeO2/Fe3O4The preparation process adopts NaCO3When in precipitation, the maximum output power reaches 530mW/cm2；
FIG. 3 shows CeO2/Fe3O4The synthetic composite material adopts NaCO3An alternating current impedance characteristic curve in a hydrogen-oxygen atmosphere during a precipitation process;
FIG. 4 shows CeO2/Fe3O4Synthetic composite material without NaCO3An alternating current impedance characteristic curve in a hydrogen-oxygen atmosphere during a precipitation process;
FIG. 5 shows pure CeO2An alternating current impedance characteristic curve in a hydrogen-oxygen atmosphere;
FIG. 6 shows CeO2/Fe3O4XRD pattern of the composite.
Detailed Description
The invention will be better understood from the following examples. However, those skilled in the art will readily appreciate that the description of the embodiments is only for illustrating the present invention and should not be taken as limiting the invention as detailed in the claims.
As shown in figure 1, the nickel foam coated with NCAL on the surface forms a symmetrical electrode, the cathode and the anode of the fuel cell of the invention both adopt the nickel foam coated with NCAL on the surface, and the core electrolyte layer is CeO2/Fe3O4A composite material, whereby the fuel cell has the structure: foamed nickel// NCAL// CeO2/Fe3O4// NCAL// nickel foam; wherein NCAL is purchased nickel cobalt aluminum lithium-Ni0.8Co0.15Al0.05LiO2-δMaterial, CeO2/Fe3O4The composite material is prepared by wet synthesis; foamed nickel is a commercially available foamed nickel material.
The preparation method of the fuel cell comprises the following steps:
firstly, preparing nickel foam (used as a cathode and an anode of a fuel cell) coated with NCAL on the surface: adding NCAL (Ni)0.8Co0.15Al0.05LiO2-δ) Gradually adding the powder into terpineol until the mixture is pasty, uniformly coating the pasty mixture on the foamed nickel, and drying the coated foamed nickel in an oven at 200 ℃ for 2 hours to obtain foamed nickel with NCAL coated on the surface;
preparation of CeO2/Fe3O4Composite material (as electrolyte layer-power generation element of fuel cell):
adding CeO2With Fe3O4Mixing according to the mass ratio of 3:1 to obtain 4g of mixed powder, and adding the mixed powder into 20mL of deionized water (CeO at the moment)2Dissolved in water, Fe3O4Insoluble in water), stirring for 4 hours at constant temperature, slowly adding concentrated nitric acid dropwise until Fe3O4Complete disappearance of the powder (i.e. Fe)3O4Completely dissolving the powder), then dropwise adding a proper amount of sodium carbonate solution (the concentration is 0.5mol/L), and stopping dropwise adding the sodium carbonate solution when new precipitates are not generated in the reaction solution any more; repeatedly cleaning and filtering the reaction solution for 4 times, drying the obtained filtered substance in a drying box of 120 ℃ for 12 hours, then putting the dried substance into a muffle furnace to sinter the substance for 4 hours at 700 ℃, naturally cooling the substance to room temperature, and fully grinding the substance to obtain CeO2/Fe3O4Composite material, CeO2/Fe3O4In the composite material, CeO2Besides iron elements of various valence states, the iron element is also doped with trace sodium ions.
Finally, the prepared electrode material is combined with an electrolyte material to obtain the low-temperature solid oxide fuel cell of the invention:
preparing electrode from nickel foam coated with NCAL on its surface, wherein the electrode is circular and has diameter D of 13mm2/Fe3O4Symmetrical structure on both sides, i.e. nickel foam// NCAL// CeO2/Fe3O4The structure of nickel foam/NCAL is prepared by placing a piece of nickel foam/NCAL into the bottom of a tabletting mold with the NCAL-coated side facing upwards, and collecting 0.35g of the nickel foam/NCALCeO2/Fe3O4The composite material is placed in a tabletting mold, and finally another piece of nickel foam// NCAL is placed in the tabletting mold, which is placed on the CeO2/Fe3O4And (3) facing downwards the surface of the composite material coated with the NCAL, putting a tabletting mold into a tabletting machine, pressurizing to 8Mpa, keeping the pressure for 5 seconds, and taking out the cell piece to obtain the low-temperature solid oxide fuel cell.
As can be seen in FIG. 2, experimental studies have shown that pure CeO2Can also be used as electrolyte of fuel cell, but has poor output performance, and the maximum output power is only 72mW/cm at the test temperature of 550 DEG C2And is unstable; one-step synthesis of CeO by chemical wet method2/Fe3O4Composite material of Fe3O4With CeO2Compounding to prepare a nanocomposite, i.e., CeO2/Fe3O4The electrochemical output performance of the composite material is from 72mW/cm2Rising to 157mW/cm2When NaCO is dripped in the one-step synthesis process3The output performance of the solution is obviously improved to 259mW/cm2。
In FIG. 3, CeO2/Fe3O4NaCO is adopted in the composite material synthesis process3The first intersection point of the AC impedance characteristic curve and the imaginary axis in the hydrogen-oxygen atmosphere during the precipitation process represents ohmic loss, which is about 0.35. omega. cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is about 0.4. omega. cm2。
In FIG. 4, CeO2/Fe3O4No NaCO is generated in the process of synthesizing the composite material3The first intersection point of the AC impedance characteristic curve and the imaginary axis in the hydrogen-oxygen atmosphere during the precipitation process represents ohmic loss, which is about 0.5. omega. cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is about 1.8. omega. cm2。
In FIG. 5, pure CeO2The first intersection point of the AC impedance characteristic curve with the imaginary axis of (1) represents an ohmic loss having a value of about 0.392cm2Characteristic curve of AC impedanceThe second intersection of the line and the imaginary axis represents grain boundary loss, which is up to about 1.6. omega. cm2。
As can be seen by comparing FIGS. 3, 4 and 5, with pure CeO2Compared with the impedance characteristic, NaCO is adopted in the synthesis process3CeO prepared by precipitation process2/Fe3O4The ohmic loss and the grain boundary loss of the composite material are greatly reduced, so that the performance of the doped composite material is greatly improved.
Fe3O4Is a complex oxide in which 1/3 is Fe 2+2/3 is Fe3+The invention uses chemical wet method to react Fe3O4With CeO2Synthesizing, sintering at high temperature to prepare a composite material with a nano structure, grinding to form nano composition of an ionic material and a semiconductor material, and forming a semiconductor-ion heterostructure in the two-phase composite material, namely changing an electrolyte layer of a traditional ion conductor into an electrolyte layer with the semiconductor-ion heterostructure. The electrolyte material with the semiconductor-ion heterostructure can enhance the transmission capability to oxygen ions, so that the electrolyte composite material has good output power in a low-temperature section (300 DEG-600 ℃).
As shown in FIG. 6, blue CeO was compared2Standard spectrum, it can be seen that pure CeO2There is also a composite powder in which, secondly, around 36 degrees, a peak appears, which, by comparison with standard PDF cards, corresponds to that of the magnetite Fe +2Fe2+3O4 standard cards, so that, as can be seen from XRD pattern analysis, Fe is doped in CeO2In addition, valence state change occurs, and the valence state change of Fe strengthens the catalytic activity of the composite material. Analysis of this result revealed that CeO2/Fe3O4The electrochemical performance of the composite material is improved mainly due to the change of the valence state of Fe, Na element is not found in XRD, on one hand, the content of Na element is probably too small, and on the other hand, the Na element is probably reduced in the suction filtration process.
The fuel cell structure of the present invention has foamed nickel used separately in the anode and the cathode to promote the oxidation-reduction reaction of the two electrodes andand the function of collecting electrons is achieved. The invention is in pure CeO2In-situ chemical wet doping of Fe3O4The composite material has high oxygen ion conduction capability when operating at a low temperature, so that the operating efficiency of the fuel cell at the low temperature is effectively improved.
Claims (6)
1. A low-temperature solid oxide fuel cell based on a cerium oxide/ferroferric oxide composite material is characterized in that: the electrolyte layer of the fuel cell is CeO2/Fe3O4A composite material; the CeO2/Fe3O4The composite material is formed by compounding a nano ion material and a nano semiconductor material, and a semiconductor-ion heterostructure is formed in the composite material;
wherein the CeO2/Fe3O4The preparation method of the composite material comprises the following specific steps: adding CeO2With Fe3O4Mixing according to the mass ratio of 3:1 to obtain 4g of mixed powder, putting the mixed powder into 20mL of deionized water, stirring for 4 hours at constant temperature, and slowly dropwise adding concentrated nitric acid until Fe3O4The powder completely disappears, then proper amount of sodium carbonate solution is dripped, after full reaction, cleaning and suction filtration are carried out for 4 times, then drying and sintering treatment are carried out, and after sintering, full grinding is carried out to obtain CeO2/Fe3O4A composite material.
2. The low-temperature solid oxide fuel cell based on the cerium oxide/ferroferric oxide composite material according to claim 1, characterized in that: the cathode and the anode of the fuel cell are foamed nickel with NCAL coated on the surface.
3. The low-temperature solid oxide fuel cell based on the cerium oxide/ferroferric oxide composite material according to claim 2, characterized in that: the nickel foam coated with NCAL on the surface is prepared by the following method: adding required amount of NCAL powder into terpineol to obtain pasty mixture, uniformly coating the pasty mixture on the nickel foam, and drying to obtain the nickel foam coated with NCAL on the surface.
4. The low-temperature solid oxide fuel cell based on the cerium oxide/ferroferric oxide composite material according to claim 1, characterized in that: the concentration of the sodium carbonate solution is 0.5 mol/L.
5. The low-temperature solid oxide fuel cell based on the cerium oxide/ferroferric oxide composite material according to claim 1, characterized in that: the sintering is carried out at a heating rate of 10 ℃/min, the temperature is raised from the drying temperature to 700 ℃, the sintering is carried out for 4 hours, and then the sintering is naturally cooled to the room temperature.
6. The low-temperature solid oxide fuel cell based on the cerium oxide/ferroferric oxide composite material according to claim 1, characterized in that: the drying temperature was 120 ℃ and the drying time was 12 hours.
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| CN114068958B (en) * | 2021-11-16 | 2023-12-08 | 东南大学 | Method for preparing carbon nano tube by catalytic pyrolysis of waste plastics and applying carbon nano tube to low-temperature fuel cell |
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| JP2003048778A (en) * | 2001-08-02 | 2003-02-21 | Kansai Electric Power Co Inc:The | Oxide ion conductor and production method therefor |
| CN101320814A (en) * | 2008-06-25 | 2008-12-10 | 施秀英 | Electrolyte material of low temperature oxide fuel battery and preparation method thereof |
| CN108808047A (en) * | 2018-05-07 | 2018-11-13 | 湖北大学 | LSCF/Na2CO3Nanocomposite is the preparation method of fuel cell ion transport layer |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| JP2003048778A (en) * | 2001-08-02 | 2003-02-21 | Kansai Electric Power Co Inc:The | Oxide ion conductor and production method therefor |
| CN101320814A (en) * | 2008-06-25 | 2008-12-10 | 施秀英 | Electrolyte material of low temperature oxide fuel battery and preparation method thereof |
| CN108808047A (en) * | 2018-05-07 | 2018-11-13 | 湖北大学 | LSCF/Na2CO3Nanocomposite is the preparation method of fuel cell ion transport layer |
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