CN109802162B - Low-temperature solid oxide fuel cell based on zinc oxide-stannous oxide composite material - Google Patents
Low-temperature solid oxide fuel cell based on zinc oxide-stannous oxide composite material Download PDFInfo
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Abstract
The invention discloses a low-temperature solid oxide fuel cell based on a zinc oxide-stannous oxide composite material, wherein a cathode and an anode of the fuel cell are both foamed nickel with NCAL coated on the surfaces, and an electrolyte layer of the fuel cell is made of a SnO/ZnO/NCAL composite material. Namely, the fuel cell of the present invention has the structure: nickel foam// NCAL// SnO/ZnO/NCAL// NCAL// nickel foam. The low-temperature solid oxide fuel cell adopts the nickel-cobalt-aluminum-lithium and the SnO/ZnO composite material synthesized by the wet method as the electrolyte layer of the oxide fuel cell, thereby greatly reducing the electrode polarization loss in the electrochemical reaction process of the fuel cell; the electrolyte material has good output power 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 zinc oxide-stannous oxide composite material, belonging 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. Nickel-cobalt-aluminum-lithium (NCAL) is well known and has been used only as an electrode material in a solid oxide fuel cell, and there is no report on its use as an electrolyte material.
At present, 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 conductivity 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. If a semiconductor material is used as an electrolyte material of a fuel cell, it is easy to conceive of occurrence of a short-circuit phenomenon, and as such, a material having semiconductor properties has not been used in the fuel cell so far. A large number of experimental researches show that the semiconductor material is compositely applied to the electrolyte material of the fuel cell, no short circuit phenomenon occurs, and the electrolyte composite material has good output power at a low-temperature section.
Disclosure of Invention
The invention aims to solve the technical problem of providing a low-temperature solid oxide fuel cell based on a zinc oxide-stannous oxide composite material, wherein an electrolyte material in the fuel cell has higher oxygen ion conduction capability at a low-temperature section, so that the solid oxide fuel cell adopting the electrolyte material can efficiently operate at the low-temperature section (300-600 ℃).
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 a zinc oxide-stannous oxide composite material is characterized in that a cathode and an anode of the fuel cell are nickel foam coated with NCAL on the surface, and an electrolyte layer of the fuel cell is a SnO/ZnO/NCAL composite material.
The fuel cell of the present invention has the structure: nickel foam// NCAL// SnO/ZnO/NCAL// 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.
The SnO/ZnO/NCAL composite material is prepared by mixing and grinding SnO/ZnO powder prepared by a wet method and NCAL powder by a dry method.
The preparation method of the SnO/ZnO/NCAL composite material specifically comprises the following steps:
step 1, preparing SnO/ZnO powder:
SnCl2.2H2O and C4H6O4Zn is mixed according to the mol ratio of 1:1 to obtain a mixed material A; dissolving the mixed material A in a proper amount of deionized water, stirring for 4 hours at a constant temperature of 80 ℃, and slowly adding citric acid (SnCl) into the mixed material A during stirring2.2H2O∶C4H6O4Zn and citric acid are 1: 3 in a molar ratio), obtaining a mixed material B, carrying out suction filtration and drying on the mixed material B, then carrying out sintering treatment, and fully grinding a sintered substance after sintering is finished to obtain SnO/ZnO powder;
step 2, preparing the SnO/ZnO + NCAL composite material:
mixing the SnO/ZnO powder prepared in the step 1 with NCAL powder according to the mass ratio of 1:4, and fully grinding to obtain the SnO/ZnO/NCAL composite material; doping NCAL substance into SnO/ZnO by dry grinding.
Wherein, in the step 1, the sintering is carried out at the heating rate of 8 ℃/min, the temperature is raised from the drying temperature to 700 ℃, the sintering is carried out for 2 hours, and then the sintering is naturally cooled to the room temperature.
Wherein in the step 1, in the mixed material B, SnCl2∶C4H6O4The mixing molar ratio of Zn to citric acid is 1: 3.
The preparation of the low-temperature solid oxide fuel cell of the invention comprises the following steps:
the nickel foam coated with NCAL on the surface is made into an electrode, the size of the electrode is circular, the diameter D is 13mm, the electrode is in a symmetrical structure at two sides of the composite material SnO/ZnO/NCAL, namely, the structure of the fuel cell of the invention is as follows: the nickel foam// NCAL// SnO/ZnO/NCAL// NCAL// nickel foam structure is characterized in that one piece of nickel foam// NCAL is placed at the bottom of a tabletting mold, the surface coated with NCAL faces upwards, 0.35g of SnO/ZnO/NCAL composite material is placed in the tabletting mold, the other piece of nickel foam// NCAL is placed in the tabletting mold, the SnO/ZnO/NCAL composite material is placed on the surface, the surface coated with NCAL faces downwards, the tabletting mold is placed in a tabletting machine, the pressure is increased to 8MPa, the pressure is maintained for 5 seconds, and then a cell piece is taken out, so that the low-temperature solid oxide fuel cell is prepared.
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 wet synthesis technology to prepare a SnO/ZnO composite material, then the SnO/ZnO composite material and NCAL are ground and mixed in a dry method, the composite electrolyte material SnO/ZnO/NCAL is obtained after full grinding, and the obtained electrolyte composite material not only can prevent the transmission of electrons, but also has high oxygen ion conduction capacity, so that the electrolyte composite material has good output power in a low-temperature section, and meanwhile, the electrode polarization loss in the electrochemical reaction process of the fuel cell is greatly reduced by the composite material; therefore, the solid oxide fuel cell adopting the electrolyte composite 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 is a graph showing the I-V and I-P characteristics of fuel cells of different mass ratios of SnO/ZnO to NCAL at a test temperature of 550 degrees, respectively; under the operation condition of 550 ℃, when the mass ratio of SnO/ZnO to NCAL is 1:4, the maximum output power reaches 583mW/cm2；
FIG. 3 is a graph showing the I-V and I-P characteristics of a fuel cell at a mass ratio of SnO/ZnO to NCAL of 1:4 at test temperatures of 550, 500 and 450 degrees, respectively; the maximum output power is 583mW/cm respectively2，481 mW/cm2，415mW/cm2；
FIG. 4 is a graph of the I-V and I-P characteristics of a fuel cell having a mass ratio of SnO/ZnO to NCAL of 1:4 versus a fuel cell of pure SnO/ZnO at a test temperature of 550 ℃; the maximum output power of the pure SnO/ZnO fuel cell is 247mW/cm under the operation condition of 550 DEG2；
FIG. 5 is an AC impedance characteristic curve of pure SnO/ZnO in a hydrogen-oxygen atmosphere;
FIG. 6 is an AC impedance characteristic curve in a hydrogen-oxygen atmosphere at a mass ratio of SnO/ZnO to NCAL of 1: 4.
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 fig. 1, the nickel foam coated with the NCAL on the surface constitutes a symmetrical electrode, the cathode and the anode of the fuel cell of the present invention both use the nickel foam coated with the NCAL on the surface, and the core electrolyte layer is a composite material of SnO/ZnO and NCAL, so the fuel cell has the structure: nickel foam// NCAL// SnO/ZnO/NCAL// NCAL// nickel foam; wherein NCAL is Ni0.8Co0.15Al0.05LiO2-δSnO/ZnO is a composite material prepared by wet synthesis; the nickel foam is a commercially available nickel material in the form of a foam, and the NCAL powder is a commercially available nickel-cobalt-aluminum-lithium powder.
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;
and preparing a SnO/ZnO/NCAL composite material (serving as an electrolyte layer-power generation element of the fuel cell):
step 1, preparing SnO/ZnO powder:
SnCl2·2H2O and C4H6O4Zn is mixed according to the mol ratio of 1:1 to obtain a mixed material A; dissolving the mixed material A in a proper amount of deionized water, stirring for 4 hours at a constant temperature of 80 ℃, and slowly adding citric acid (SnCl) into the mixed material A during stirring2·2H2O∶C4H6O4Zn and citric acid are in a molar ratio of 1: 3) to obtain a mixed material B, the mixed material B is subjected to suction filtration and drying and then is subjected to sintering treatment, and after sintering is finished, a sintered product is fully ground to obtain SnO/ZnO powder;
step 2, preparing the SnO/ZnO/NCAL composite material:
and (3) mixing the SnO/ZnO powder prepared in the step (1) with the NCAL powder according to the mass ratio of 1:4, and fully grinding to obtain the SnO/ZnO/NCAL composite material.
Finally, the prepared electrode material is combined with an electrolyte material to obtain the low-temperature solid oxide fuel cell of the invention:
the nickel foam coated with the NCAL on the surface is made into an electrode, the size of the electrode is circular, the diameter D is 13mm, the electrode is in a symmetrical structure on two sides of the composite material SnO/ZnO/NCAL, namely the nickel foam// NCAL// SnO/ZnO/NCAL// NCAL// nickel foam structure, one piece of nickel foam// NCAL is placed at the bottom of a tabletting mold, the side coated with the NCAL on the surface faces upwards, then 0.35g of the SnO/ZnO/NCAL composite material is placed in the tabletting mold, finally the other piece of nickel foam// NCAL is placed in the tabletting mold, the side coated with the NCAL on the surface faces downwards, the tabletting mold is placed in the tabletting machine, the pressure is increased to 8MPa, the pressure is maintained for 5 seconds, and then the cell piece is taken out, thus the low-temperature solid oxide fuel cell is prepared.
As can be seen from FIGS. 2 to 4, pure SnO/ZnO can be used as the electrolyte of the fuel cell, and the maximum output power is 247mW/cm under the condition of 550 DEG2After SnO/ZnO material is compounded with NCAL according to different mass ratios, when the mass ratio of SnO/ZnO to NCAL is 1:4, the electrochemical performance reaches 583mW/cm2The mass ratio of SnO/ZnO to NCAL is changed, and the battery performance is obviously changed. When the mass ratio of SnO/ZnO to NCAL is 1:1, the maximum output power of the fuel cell is 223mW/cm2When the mass ratio of SnO/ZnO to NCAL is 1: 2, the maximum output power of the fuel cell is 353mW/cm2When the mass ratio of SnO/ZnO to NCAL is 1: 3, the maximum output power of the fuel cell is 506mW/cm2Compared with the output power when the mass ratio of SnO/ZnO to NCAL is 1:4, the output power is slightly reduced, if the mass ratio of NCAL in the composite material is further increased, the performance of the composite material is gradually close to the pure NCAL, and the output performance of the battery is almost disappeared at the moment. When the mass ratio of SnO/ZnO in the composite material is further increased, the performance of the composite material gradually tends to the output performance of pure SnO/ZnO. In conclusion, the research results show that doping NCAL in a pure SnO/ZnO material is beneficial to improving the catalytic activity of electrolyte, and experimental researches show that the optimal ratio of the NCAL to the SnO ZnO material is 1:4 by mass. Pure NCAL is used as electrolyte of the fuel cell, and the output power is 0mW/cm under the condition of 550 DEG2I.e., it does not have oxygen ion transport capability.
Both ZnO and NCAL are materials having semiconducting properties, and if SnO is not present in the composite electrolyte material, the material exhibits semiconducting properties, having only an electron-conducting function and not an ion-conducting function, if only ZnO and NCAL are compounded. When SnO and ZnO are compounded, the SnO/ZnO nano composite material has an ion transmission function, and oxygen ions are conducted to the hydrogen ion side, so that water is generated in a combined manner, and electrons are released, thereby realizing conversion to generate electric energy and realizing the electrochemical reaction of a fuel cell.
Experiments show that: the SnO/ZnO nano composite material can be used as an electrolyte of a fuel cell, the open-circuit voltage exceeds 1V, the phenomenon of short circuit is not generated after the SnO and the ZnO are compounded, but the output power is low because the current is small although the open-circuit voltage is high, and the oxygen ion conduction capability is insufficient because of the small current. When a certain amount of NCAL material is added into the SnO/ZnO nano composite material, the oxygen ion conduction capability of the electrolyte material can be obviously improved, and the current and the power are improved.
In FIG. 5, the first intersection of the AC impedance characteristic curve of pure SnO/ZnO with the imaginary axis represents the ohmic loss, which is about 0.35. omega. cm2The second intersection of the second AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is up to about 0.78. omega. cm2. In FIG. 6, the first intersection of the AC impedance characteristic curve of SnO/ZnO doped with NCAL (SnO/ZnO to NCAL mass ratio of 1: 4) and the imaginary axis represents the ohmic loss, and its value is about 0.12. omega. cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is about 0.27. omega. cm2. As can be seen by comparing fig. 5 and 6, compared with the impedance characteristic of pure SnO/ZnO, the ohmic loss and the grain boundary loss of the SnO/ZnO and NCAL composite are greatly reduced, so that the performance of the doped composite electrolyte material is greatly improved.
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. According to the invention, the NCAL material is doped in the pure SnO/ZnO composite material, and when the composite electrolyte material operates at a low temperature (300-600 ℃), the composite electrolyte material has good oxygen ion conduction capability, so that the operating efficiency of the fuel cell at the low temperature is effectively improved.
Claims (5)
1. A low-temperature solid oxide fuel cell based on a zinc oxide-stannous oxide composite material is characterized in that: the electrolyte layer of the fuel cell is made of SnO/ZnO/NCAL composite material;
the SnO/ZnO/NCAL composite material is prepared by mixing SnO/ZnO powder and NCAL powder and then fully grinding the mixture; the method specifically comprises the following steps:
step 1, preparing SnO/ZnO powder:
SnCl2﹒2H2O and C4H6O4Zn is mixed according to the molar ratio of 1:1 to obtain a mixed material A; dissolving the mixed material A in a proper amount of deionized water, stirring for 4 hours at a constant temperature of 80 ℃, slowly adding citric acid into the mixed material A in the stirring process to obtain a mixed material B, carrying out suction filtration and drying on the mixed material B, then carrying out sintering treatment, and fully grinding a sintered product after sintering to obtain SnO/ZnO powder;
step 2, preparing the SnO/ZnO/NCAL composite material:
and (3) mixing the SnO/ZnO powder prepared in the step (1) with the NCAL powder according to the mass ratio of 1:4, and fully grinding to obtain the SnO/ZnO/NCAL composite material.
2. The zinc oxide-stannous oxide composite based low temperature solid oxide fuel cell of claim 1, wherein: the cathode and the anode of the fuel cell are foamed nickel with NCAL coated on the surface.
3. The zinc oxide-stannous oxide composite based low temperature solid oxide fuel cell of claim 2, wherein: 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 zinc oxide-stannous oxide composite based low temperature solid oxide fuel cell of claim 1, wherein: in the step 1, the temperature of sintering is raised from the drying temperature to 700 ℃ at the heating rate of 8 ℃/min, the sintering is carried out for 2 hours, and then the sintering is naturally cooled to the room temperature.
5. The low temperature solid oxide fuel cell of claim 1, wherein: in step 1, in the mixed material B, SnCl2：C4H6O4Zn: the mixing molar ratio of the citric acid is 1: 1: 3.
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