CN109687006B - Low-temperature solid oxide fuel cell based on cerium oxide/nickel oxide composite material - Google Patents
Low-temperature solid oxide fuel cell based on cerium oxide/nickel oxide composite material Download PDFInfo
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- CN109687006B CN109687006B CN201811631918.0A CN201811631918A CN109687006B CN 109687006 B CN109687006 B CN 109687006B CN 201811631918 A CN201811631918 A CN 201811631918A CN 109687006 B CN109687006 B CN 109687006B
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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
- H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
- H01M8/124—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte
- H01M8/1246—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides
- H01M8/126—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte characterised by the process of manufacturing or by the material of the electrolyte the electrolyte consisting of oxides the electrolyte containing cerium oxide
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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
- 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
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- 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
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Abstract
The invention discloses a low-temperature solid oxide fuel cell based on a cerium oxide/nickel oxide composite material, wherein a cathode and an anode of the fuel cell are foamed nickel with NCAL (nickel carbide) coated on the surfaces, and an electrolyte layer of the fuel cell is CeO (CeO)2/NiO composite materialAnd (5) feeding. Namely, the fuel cell of the present invention has the structure: foamed nickel// NCAL// CeO2/NiO// NCAL// nickel foam. The low-temperature solid oxide fuel cell adopts CeO2the/NiO 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/nickel 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 800 ℃, completes the electrochemical reaction of the fuel cell and outputs electric power. The material (YSZ) has good oxygen ion transport capability only at high temperature, and has little oxygen ion transport capability when the temperature is reduced to below 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/nickel 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 conductivity 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 (300-.
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/nickel 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 CeO2the/NiO composite material.
The fuel cell of the present invention has the structure: foamed nickel// NCAL// CeO2/NiO// 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 CeO2the/NiO composite material is prepared by mixing CeO2And the NiO is synthesized by adopting a chemical wet method in one step and is obtained by cleaning, filtering, drying, sintering and fully grinding.
CeO as defined above2The preparation method of the/NiO composite material comprises the following steps: adding CeO2Mixing with NiO 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, slowly dropwise adding concentrated nitric acid until the NiO powder completely disappears (the NiO powder is fully dissolved), dropwise adding a proper amount of sodium carbonate solution, after full reaction, cleaning and filtering for 4 times, then drying and sintering, fully grinding after sintering to obtain CeO2a/NiO 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 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 13mm2The two sides of/NiO are in a symmetrical structure, namely foamed nickel// NCAL// CCeO2The structure of NiONCAL/foam nickel is prepared by placing a piece of foam nickel/NCAL at the bottom of a tabletting mold, with the surface coated with NCAL facing upwards, and collecting 0.35g of CeO2Putting the/NiO composite material into a tabletting mold, putting another piece of foamed nickel// NCAL into the tabletting mold, and putting the piece of foamed nickel// NCAL into the CeO2Above the/NiO composite, TableAnd (3) facing the surface coated with the NCAL downwards, putting a tabletting mould 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 synthesis2The composite electrolyte material CeO of the invention is obtained after fully grinding the/NiO composite material2The 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 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 species2Composite NiO/NiO 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 CeO2The preparation process of/NiO adopts NaCO3When in precipitation, the maximum output power reaches 530mW/cm2；
FIG. 3 shows CeO2the/NiO composite material adopts NaCO3An alternating current impedance characteristic curve in a hydrogen-oxygen atmosphere during a precipitation process;
FIG. 4 shows CeO2NaCO-free/NiO composite material3An 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 CeO2XRD pattern of/NiO composite material.
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 CeO2the/NiO composite material, therefore, the structure of the fuel cell is as follows: foamed nickel// NCAL// CeO2/NiO// NCAL// nickel foam; wherein NCAL is purchased nickel cobalt aluminum lithium-Ni0.8Co0.15Al0.05LiO2-δMaterial, CeO2the/NiO is the composite material 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 CeO2the/NiO composite (as an electrolyte layer-power generation element of a fuel cell):
adding CeO2Mixing with NiO at a 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)2Dissolving NiO in water, wherein the NiO is not dissolved in the water), stirring at constant temperature for 4 hours, slowly dropwise adding concentrated nitric acid until the NiO powder completely disappears (namely the NiO powder is completely dissolved), 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; 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 CeO2the/NiO composite material.
CeO2In the/NiO composite material, CeO2Besides NiO, the NiO 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 13mm2The two sides of/NiO are in a symmetrical structure, namely foamed nickel// NCAL// CeO2The structure of/NiO// NCAL// nickel foam is prepared by placing a piece of nickel foam// NCAL into the bottom of a tabletting mold, placing the surface coated with NCAL upward, and taking 0.35g of CeO2Putting the/NiO composite material into a tabletting mold, and finally putting another piece of foamed nickel// NCAL into the tabletting mold, wherein the piece of foamed nickel// NCAL is placed on the CeO2And (3) placing a tabletting mold on the/NiO composite material with the surface coated with the NCAL facing downwards, pressurizing to 8Mpa by using a tabletting mold, maintaining 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/NiO composite material prepared by mixing NiO with CeO2Compounding to prepare a nanocomposite, i.e., CeO2The electrochemical output performance of the/NiO composite material is from 72mW/cm2Rising to 237mW/cm2When NaCO is dripped in the one-step synthesis process3The output performance of the solution is obviously improved to 530mW/cm2。
In FIG. 3, CeO2NaCO is adopted in the synthesis process of the/NiO 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 0.17. omega. cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is about 0.48. omega. cm2。
In FIG. 4, CeO2No NaCO is generated in the synthesis process of the/NiO composite material3Settling toolThe first intersection point of the AC impedance characteristic curve and the imaginary axis in hydrogen-oxygen atmosphere represents ohmic loss, and its value is about 0.27 Ω cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is up to about 0.78. omega. cm2。
In FIG. 5, pure CeO2The first intersection point of the AC impedance characteristic curve with the imaginary axis of (A) represents an ohmic loss having a value of about 0.39. omega. cm2The second intersection of the AC impedance characteristic curve 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 of CeO prepared by a chemical wet method2The ohmic loss and the grain boundary loss of the/NiO composite material are greatly reduced, so that the performance of the doped composite material is greatly improved.
NiO is a P-type semiconductor material, the NiO prepared by a chemical wet method is not strict with the atomic ratio of 1-1, and has a plurality of defects to cause an intrinsic P-type; with an ionic conductor CeO2Recombination, i.e., doping of an electronic phase in an ionic phase, to form a heterostructure, i.e., a semiconductor-ion heterostructure; from CeO2The electrolyte layer of the ion conductor becomes an electrolyte layer having a semiconductor-ion heterostructure, and the electrolyte material having the semiconductor-ion heterostructure can enhance the transport ability for oxygen ions, so that the electrolyte composite material also has good output power in a low temperature section (300-.
The material prepared by the invention is a nano material, namely the nano ionic material and the nano semiconductor material are compounded, and then the nano compound of the ionic 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 ionic 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 ionic phase, so that the output power of the fuel cell is obviously increased.
As shown in FIG. 6, blue CeO was compared2Standard spectrum, it can be seen that pure CeO2Also in the mixed powder, pairCompared with the red NiO standard spectrum, it can be seen that pure NiO is also present in the mixed powder, and thus, CeO2The NiO is compounded with two phases, no reaction occurs, and no new phase appears; a peak was found at the 30 degree position and this peak corresponded to the peak of the Na standard PDF card by analytical comparison.
From XRD analysis, CeO2Is a two-phase composite nano material with NiO, does not generate chemical reaction per se, and is CeO2Belongs to ion conductor materials, but the ion conductivity is not very high, NiO is doped into CeO2Secondly, firstly, NiO is a material with a catalytic effect, so that the ionic conductivity of the composite material is further improved, and meanwhile, carriers cannot flow due to the entanglement of the internal structure of nickel oxide, so that the nickel oxide is an insulator and is not conductive; in the composite material, a small amount of Na ions appear in the composite material, so that the catalytic activity of the composite material is further improved, because Na has higher catalytic activity.
In the structure of the fuel cell, the foamed nickel is respectively used for the anode and the cathode to promote the oxidation-reduction reaction process of the two electrodes and play a role in collecting electrons. The invention is in pure CeO2The NiO material is doped by a chemical wet method, and the composite material has high oxygen ion conductivity when running at a low temperature, so that the running efficiency of the fuel cell at the low temperature is effectively improved.
Claims (3)
1. A low-temperature solid oxide fuel cell based on a cerium oxide/nickel oxide composite material is characterized in that: the electrolyte layer of the fuel cell is CeO2a/NiO composite material;
the CeO2The preparation method of the/NiO composite material comprises the following steps: adding CeO2Mixing the powder with NiO 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, slowly dropwise adding concentrated nitric acid until NiO powder completely disappears, dropwise adding a proper amount of sodium carbonate solution, and stopping dropwise adding the sodium carbonate solution when new precipitates are not generated in the reaction solution; repeatedly cleaning and filtering the reaction solution for 4 times, and drying the obtained filtrate in a drying oven at 120 deg.C for 12 hrThen placing the mixture into a muffle furnace to be sintered for 4 hours at 700 ℃, naturally cooling the mixture to room temperature, and fully grinding the mixture to obtain CeO2a/NiO composite material; CeO (CeO)2In the/NiO composite material, CeO2Besides NiO, the NiO is also doped with trace sodium ions.
2. The low-temperature solid oxide fuel cell based on the ceria/nickel oxide composite according to claim 1, characterized in that: the cathode and the anode of the fuel cell are coated with Ni on the surfaces0.8Co0.15Al0.05LiO2-δThe nickel foam of (1).
3. The low-temperature solid oxide fuel cell based on the ceria/nickel oxide composite according to claim 2, characterized in that: surface coated with Ni0.8Co0.15Al0.05LiO2-δThe foamed nickel is prepared by the following method: adding required amount of Ni0.8Co0.15Al0.05LiO2-δAdding the powder into terpineol to obtain pasty mixture, uniformly coating the pasty mixture on foamed nickel, and oven drying to obtain the final product with Ni coated on the surface0.8Co0.15Al0.05LiO2-δThe nickel foam of (1).
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Effective date of registration: 20211028 Address after: A213, Kechuang building, National Science and Technology Park, Southeast University, 271 Heyan Road, Qixia District, Nanjing, Jiangsu 210028 Patentee after: NANJING SUOLEYOU ENERGY SAVING TECHNOLOGY Co.,Ltd. Address before: No. 3601 Jiangning Road, Nanjing District hirokage 211171 cities in Jiangsu Province Patentee before: NANJING XIAOZHUANG University |