CN109786795B - Low-temperature solid oxide fuel cell based on strontium stannate/lanthanum strontium cobalt iron composite material - Google Patents
Low-temperature solid oxide fuel cell based on strontium stannate/lanthanum strontium cobalt iron composite material Download PDFInfo
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Abstract
The invention discloses a low-temperature solid oxide fuel cell based on a strontium stannate/lanthanum strontium cobalt iron composite material, wherein 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 an SSO/LSCF composite material. Namely, the fuel cell of the present invention has the structure: foam nickel// NCAL// SSO/LSCF// NCAL// foam nickel. The low-temperature solid oxide fuel cell adopts the composite material of strontium stannate with a perovskite structure and lanthanum strontium cobalt iron as the electrolyte layer, 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 strontium stannate/lanthanum strontium cobalt iron 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.
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 with the perovskite structure or the perovskite-like structure is compositely applied to the electrolyte material of the fuel cell, no short circuit phenomenon occurs, and the electrolyte composite material also 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 strontium stannate/lanthanum strontium cobalt iron composite material, wherein an electrolyte material in the fuel cell adopts an N-type semiconductor material strontium stannate (SrSnO) with a perovskite structure3) The obtained electrolyte composite material can not only prevent the transmission of electrons, but also has high ion conduction capability, so that the electrolyte composite material has good output power at a low temperature section, and a 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 strontium stannate/lanthanum strontium cobalt iron composite material is characterized in that a cathode and an anode of the fuel cell are foamed nickel coated with NCAL on the surface, and an electrolyte layer of the fuel cell is an SSO/LSCF composite material.
The fuel cell of the present invention has the structure: foam nickel// NCAL// SSO/LSCF// NCAL// foam nickel.
Wherein, the nickel foam coated with nickel-cobalt-aluminum-lithium (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 SSO/LSCF composite material is obtained by mixing SSO powder and nano LSCF powder according to a certain mass ratio and fully grinding.
The preparation method of the SSO/LSCF composite material specifically comprises the following steps:
dissolving 0.025mol of stannic chloride in 1mol of ethylene glycol to obtain a mixed solution A, adding 0.25mol of citric acid into the mixed solution A, stirring at 60 ℃ for 2 hours, fully dissolving to obtain a mixed solution B, adding 0.025mol of SrCO into the mixed solution B3Stirring for 6 hours at a constant temperature of 80 ℃ to obtain a mixed solution C, heating the mixed solution C to 135 ℃ for more than 12 hours to obtain a brown transparent gel, heating the gel at 350 ℃ for 3 hours to obtain a dry gel, putting the Sr-containing dry gel into a heating furnace, heating to 700 ℃, sintering for 4 hours, naturally cooling to room temperature, and fully grinding a sintered object after sintering to obtain SSO powder;
and (3) mixing the SSO powder prepared in the step (1) with the LSCF powder according to the mass ratio of 1:2, and fully grinding to obtain the SSO/LSCF composite material.
In step 1, the heating of the gel is divided into two processes: firstly, the temperature is raised from the room temperature to 350 ℃ at the temperature raising rate of 5 ℃/min, the sintering is carried out for 3 hours, then the temperature is raised from 350 ℃ to 700 ℃, the sintering is carried out for 4 hours, and the sintering is naturally cooled to the room temperature.
The preparation of the low-temperature solid oxide fuel cell of the invention comprises the following steps:
preparing an electrode from the nickel foam coated with the NCAL on the surface, wherein the electrode is circular, the diameter D is 13mm, the electrode is in a symmetrical structure at two sides of the nano composite material SSO/LSCF, namely the nickel foam// NCAL// SSO/LSCF/NCAL// nickel foam structure, putting one piece of nickel foam// NCAL into the bottom of a tabletting mold, the surface coated with the NCAL faces upwards, putting 0.35g of the SSO/LSCF composite material into the tabletting mold, putting the other piece of nickel foam// NCAL on the SSO/LSCF composite material, the surface coated with the NCAL faces downwards, putting the tabletting mold into a tabletting machine, pressurizing to 8MPa, and holding the pressure for 5 seconds, and taking out a 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 wet method to synthesize an SSO material with a perovskite structure, then the prepared SSO material is mixed with LSCF with the perovskite structure in a dry method, and the composite electrolyte material SSO/LSCF is obtained after full grinding, so that the obtained electrolyte composite material not only can prevent the transmission of electrons, but also has high ion conduction capability, therefore, the electrolyte composite material has good output power at a low-temperature section, and simultaneously, the composite material also greatly reduces the electrode polarization loss in the electrochemical reaction process of the fuel cell; 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 shows fuel power of different mass ratios of SSO and LSCFI-V and I-P characteristic curves of the cell at the test temperature of 550 ℃ respectively; under the operation condition of 550 ℃, when the mass ratio of the SSO to the LSCF is 1:2, the maximum output power reaches 656mW/cm2；
FIG. 3 is an I-V and I-P characteristic curves at test temperatures of 550, 525, and 500 degrees, respectively, for a fuel cell having a mass ratio of SSO to LSCF of 1: 2; the maximum output power is 656mW/cm respectively2，535mW/cm2，399mW/cm2；
FIG. 4 is an AC impedance characteristic curve in a hydrogen-oxygen atmosphere at a mass ratio of SSO to LSCF of 1: 2;
FIG. 5 is an AC impedance characteristic of pure SSO in a hydrogen-oxygen atmosphere;
fig. 6 is a space charge region formed after the electrolyte composite is combined.
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 SSO and LSCF, so the fuel cell has the structure: nickel foam// NCAL// SSO/LSCF// NCAL// nickel foam; wherein NCAL is Ni0.8Co0.15Al0.05LiO2-aMaterials (either commercially available or prepared using published methods), SSO commercially available or prepared using the methods of the invention, LSCF commercially available; 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 adding the coated foamed nickel into the mixtureDrying in an oven at 200 ℃ for 2 hours to obtain the foamed nickel with NCAL coated on the surface;
and preparing the SSO/LSCF composite material (as an electrolyte layer-power generation element of the fuel cell):
dissolving 0.025mol of stannic chloride in 1mol of ethylene glycol to obtain a mixed solution A, adding 0.25mol of citric acid into the mixed solution A, stirring at 60 ℃ for 2 hours, fully dissolving to obtain a mixed solution B, adding 0.025mol of SrCO into the mixed solution B3Stirring for 6 hours at a constant temperature of 80 ℃ to obtain a mixed solution C, heating the mixed solution C to 135 ℃ for more than 12 hours to obtain a brown transparent gel, heating the gel at 350 ℃ for 3 hours to obtain a dry gel, putting the Sr-containing dry gel into a heating furnace, heating to 700 ℃, sintering for 4 hours, naturally cooling to room temperature, and fully grinding a sintered object after sintering to obtain SSO powder; the SSO prepared by the sol-gel method has a perovskite structure;
mixing the SSO powder prepared in the step 1 with the purchased LSCF powder according to the mass ratio of 1:2, and fully grinding to obtain an SSO/LSCF 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 method comprises the steps of preparing an electrode from nickel foam coated with NCAL on the surface, wherein the size of the electrode is circular, the diameter D is 13mm, the electrode is in a symmetrical structure on two sides of a nano composite material SSO/LSCF, namely the nickel foam// NCAL// SSO/LSCF// NCAL/nickel foam structure, firstly putting one piece of nickel foam// NCAL into the bottom of a tabletting mold, enabling the side coated with NCAL on the surface to face upwards, then putting 0.35g of the SSO/LSCF composite material into the tabletting mold, finally putting the other piece of nickel foam// NCAL into the tabletting mold, putting the tabletting mold on the SSO/LSCF composite material, enabling the side coated with NCAL on the surface to face downwards, putting the tabletting mold into a tabletting machine, pressurizing to 8MPa, maintaining the pressure for 5 seconds, and then taking out a cell piece, thus obtaining the low-temperature solid oxide fuel cell.
Experimental research shows that pure SSO can be used as an electrolyte of a fuel cell, but the output performance is poor and unstable, and as can be seen from figures 2 and 3, after the SSO material is compounded with LSCF according to different mass ratios, when the mass ratio of the SSO to the LSCF is 1:2, the electrochemical performance reaches 656mW/cm2When the mass ratio of the SSO to the LSCF is 1: 1, the maximum output power of the fuel cell is 415mW/cm2When the mass ratio of the SSO to the LSCF is 1:2, the maximum output power of the fuel cell is 656mW/cm2When the mass ratio of the SSO to the LSCF is 1: 3, the maximum output power of the fuel cell is 146mW/cm2When the mass ratio of the SSO to the LSCF is 2: 1, the maximum output power of the fuel cell is 199mW/cm2. It can be found by experiments that if the mass ratio of the LSCF in the composite material is further increased, the performance of the composite material is close to that of the pure LSCF, and gradually decreases, and when the mass ratio of the LSCF is close to 1 (namely, the LSCF in the composite material is almost pure), the battery output performance almost disappears. When the mass fraction of the SSO in the composite material is further increased, the performance gradually tends to the output performance of pure SSO. In conclusion, the research results show that the SSO and the LSCF are compounded according to a certain proportion, the obtained composite material has high ion conductivity at a low-temperature section, and thus has high output power, and experimental researches show that the optimal mass ratio of the SSO to the LSCF is 1: 2.
In FIG. 4, the first intersection point of the imaginary axis and the AC impedance characteristic curve at a mass ratio of SSO to LSCF of 1:2 represents the ohmic loss, which 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 0.2. omega. cm2. In FIG. 5, the first intersection of the AC impedance characteristic of pure SSO with the imaginary axis represents the ohmic loss, which is about 0.52 Ω cm2The second intersection of the AC impedance characteristic curve and the imaginary axis represents grain boundary loss, which is up to about 1.7. omega. cm2。
As can be seen from comparing fig. 4 and 5, compared with the impedance characteristic of pure SSO, the ohmic loss and grain boundary loss of the composite material of SSO and LSCF are both greatly reduced, thereby proving that the performance of the composite 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, an N-type semiconductor material SSO with a perovskite structure and a P-type semiconductor material LSCF with a perovskite structure are compounded, as shown in fig. 6, a space charge region established by a P-type material with a nano structure and an N-type material is formed in an electrolyte layer, the space charge region can cause an energy band to bend to establish a strong built-in electric field at a (P-N) interface, and further the conduction speed of oxygen ions is accelerated (the ions are accelerated in the space charge region), and meanwhile, the space charge region can prevent the transmission of electrons; in the traditional electrolyte, ions are transmitted in the electrolyte due to concentration difference, namely, the concentration of oxygen ions on the left side is increased continuously, so that the concentration of oxygen ions on the surface of the electrolyte is increased continuously, the oxygen ions diffuse into the electrolyte at high temperature and gradually reach the other side to react with hydrogen ions, but the composite electrolyte material can realize quick conduction of the oxygen ions to the hydrogen ions without high temperature, so that the electrolyte composite material has good output power at a low temperature section.
Claims (3)
1. The utility model provides a low temperature solid oxide fuel cell based on strontium stannate/lanthanum strontium cobalt iron combined material which characterized in that: the electrolyte layer of the fuel cell is an SSO/LSCF composite material; the SSO/LSCF composite material is prepared by mixing SSO powder and LSCF powder prepared by a wet method and then fully grinding; the method specifically comprises the following steps:
step 1, preparation of SSO powder: dissolving 0.025mol of stannic chloride in 1mol of ethylene glycol to obtain a mixed solution A, adding 0.25mol of citric acid into the mixed solution A, stirring for 2 hours at 60 ℃, fully dissolving to obtain a mixed solution B, and adding 0.025mol of SrCO into the mixed solution B3Stirring for 6 hours at the constant temperature of 80 ℃ to obtain a mixed solution C, heating the mixed solution C to 135 ℃ for more than 12 hours to obtain a brown transparent gel, heating the gel at 350 ℃ for 3 hours to obtain a dry gel, then putting the dry gel containing Sr into a heating furnace to heat for 700 ℃,sintering for 4 hours, naturally cooling to room temperature, and fully grinding the sinter after sintering to obtain SSO powder; the heating of the gel is divided into two processes: firstly, increasing the temperature from room temperature to 350 ℃ at the heating rate of 5 ℃/min, sintering for 3 hours, then increasing the temperature from 350 ℃ to 700 ℃, sintering for 4 hours, and naturally cooling to room temperature;
step 2, preparing the SSO/LSCF composite material: and (3) mixing the SSO powder prepared in the step (1) with the LSCF powder according to the mass ratio of 1:2, and fully grinding to obtain the SSO/LSCF composite material.
2. The strontium stannate/lanthanum strontium cobalt iron 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 strontium stannate/lanthanum strontium cobalt iron 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.
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| CN113725468A (en) * | 2021-08-13 | 2021-11-30 | 南京晓庄学院 | Application of lithium lanthanum zirconium tantalum oxygen as solid oxide fuel cell electrolyte material |
| CN113782794B (en) * | 2021-08-30 | 2024-03-08 | 湖北大学 | Fuel cell based on metal ion battery material and manufacturing method thereof |
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| CN101320814A (en) * | 2008-06-25 | 2008-12-10 | 施秀英 | Electrolyte material of low temperature oxide fuel battery and preparation method thereof |
| WO2011100361A2 (en) * | 2010-02-10 | 2011-08-18 | C3 International. Llc | Low temperature electrolytes for solid oxide cells having high ionic conductivity |
| CN107221679A (en) * | 2017-05-27 | 2017-09-29 | 李俊娇 | Symmetrical electrode structure fuel cell prepared by a kind of nano composite material |
| CN107660318A (en) * | 2015-06-30 | 2018-02-02 | 株式会社Lg化学 | Manufacture method, electrolyte for solid oxide fuel cell film, SOFC and the fuel cell module of electrolyte for solid oxide fuel cell film |
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| CN101320814A (en) * | 2008-06-25 | 2008-12-10 | 施秀英 | Electrolyte material of low temperature oxide fuel battery and preparation method thereof |
| WO2011100361A2 (en) * | 2010-02-10 | 2011-08-18 | C3 International. Llc | Low temperature electrolytes for solid oxide cells having high ionic conductivity |
| CN107660318A (en) * | 2015-06-30 | 2018-02-02 | 株式会社Lg化学 | Manufacture method, electrolyte for solid oxide fuel cell film, SOFC and the fuel cell module of electrolyte for solid oxide fuel cell film |
| CN107221679A (en) * | 2017-05-27 | 2017-09-29 | 李俊娇 | Symmetrical electrode structure fuel cell prepared by a kind of nano composite material |
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