CN111834656B - Optimized single-phase doped lanthanum gallate electrolyte preparation device and method - Google Patents
Optimized single-phase doped lanthanum gallate electrolyte preparation device and method Download PDFInfo
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- H01M8/00—Fuel cells; Manufacture thereof
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- 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
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Abstract
The invention provides an optimized single-phase doped lanthanum gallate (La)0.9Sr0.1Ga0.8Mg0.2O3‑δLSGM) electrolyte preparation apparatus and method including a generant canister, a base, and controlsThe top parts of the two sides of the base are fixedly provided with supporting rods, the generating tank is fixedly arranged on the top parts of the supporting rods, a first electric push rod is fixedly arranged at the center position of the top part of the base, a supporting frame is fixedly arranged on the top part of the first electric push rod, and a fixed seat is fixedly arranged on the top part of the supporting frame; the method indicates that the combustion process for preparing the precursor powder is an important step for influencing whether the subsequent sintering can form a phase, and the heating power of a proper solution is 22 g/W.dm2‑30g/W·dm2The optimized single-phase lanthanum gallate-doped electrolyte preparation device and the method have reasonable design, the prepared LSGM electrolyte is basically single-phase, and SrLaGaO is eliminated4、SrLaGa3O7The negative effect brought by the relative conductivity of the impurities can effectively improve the power of the battery, enhance the anti-attenuation performance of the battery and prolong the service life of the battery.
Description
Technical Field
The invention belongs to the technical field of fuel cells, and particularly relates to an optimized single-phase doped lanthanum gallate electrolyte preparation device and method.
Background
The traditional Solid Oxide Fuel Cell (SOFC) has higher operation temperature (800-. One of the important reasons is that the conductivity of the electrolyte decreases significantly with decreasing temperature. Therefore, finding an electrolyte material having high conductivity and high stability at a medium temperature is an important way to break through the above-mentioned problems. Research finds that La0.9Sr0.1Ga0.8Mg0.2O3-δThe (LSGM) electrolyte shows higher oxygen ion conductivity at medium and low temperature, has lower working temperature (600 ℃ F. and 800 ℃ C.), and is an ideal electrolyte material for medium and low temperature solid oxide fuel cells. However, since the LSGM perovskite phase has a narrow range of stable components and Ga is easily volatilized at high temperature, it is locally deviated from stoichiometry and thus a hetero-phase is easily formed, thereby deteriorating electrical and mechanical properties of the material. Although the glycine combustion method is a common method for preparing LSGM at present, the prepared sample often contains SrLaGaO4、SrLaGa3O7The conductivity of the LSGM is obviously reduced due to the equal impurity phase (both high resistance phases); at the same time, the presence of the impurity phase will also result in a decrease in the compactness of the sample, further impairing the performance of LSGM as an electrolyte. Therefore, the single-phase LSGM preparation process still needs to be optimized.
The main process for preparing LSGM by glycine combustion method comprises two steps: firstly, preparing precursor powder by a combustion method; secondly, pressing the precursor powder into a compact, and sintering at high temperature until the final phase is formed. Among them, the combustion process of the precursor powder greatly affects the activation energy of the powder, which becomes an important cause for the generation of a heterogeneous phase in the post-sintering. In addition, the existing process does not have special equipment for preparing the LSGM, each link needs to be separately carried out, and the preparation efficiency is low, so that the invention provides an optimized single-phase doped lanthanum gallate electrolyte preparation device and method.
Disclosure of Invention
In order to solve the problems in the prior art, the invention provides an optimized single-phase doped lanthanum gallate electrolyte preparation device and a method, the optimized single-phase doped lanthanum gallate electrolyte preparation device is reasonable in design, the LSGM electrolyte prepared by the optimized device and the method is basically single-phase, and SrLaGaO is eliminated4、SrLaGa3O7The negative effect brought by the relative conductivity of the impurities can effectively improve the power of the battery, enhance the anti-attenuation performance of the battery and prolong the service life of the battery.
In order to achieve the purpose, the invention is realized by the following technical scheme: an optimized single-phase doped lanthanum gallate electrolyte preparation device comprises a generating tank, a base and a control box, wherein supporting rods are fixedly installed at the tops of two sides of the base, the generating tank is fixedly installed at the tops of the supporting rods, a first electric push rod is fixedly installed at the central position of the top of the base, a supporting frame is fixedly installed at the top of the first electric push rod, a fixed seat is fixedly installed at the top of the supporting frame, a stepping motor is fixedly installed between the fixed seat and the supporting frame, a convex sliding ring is fixedly installed at the bottom of a placing seat, an annular sliding groove is formed in the top of the fixed seat, the convex sliding ring is installed in the annular sliding groove, a through hole is formed in the bottom of the generating tank, the top of the placing seat penetrates through the through hole and extends into the generating tank, the placing seat is fixedly connected with an output shaft of the stepping motor, and a placing groove is formed in the top of the placing seat, the device comprises a generating tank, a grinding pressure sheet seat is fixedly arranged at the position corresponding to a placing seat on the inner side wall of the top of the generating tank, a movable groove is formed in the top of the grinding pressure sheet seat, a movable seat is arranged in the movable groove, a plurality of blocking rods are fixedly arranged at the bottom of the movable seat, an electric push rod II is arranged at the top of the generating tank through bolts, an air channel and a gas fuel channel are respectively arranged in two sides of the grinding pressure sheet seat, a mixing cavity is formed in the grinding pressure sheet seat, the air channel and the gas fuel channel are both communicated with the mixing cavity, an igniter is fixedly embedded in the inner side wall of the top of the mixing cavity, a spray hole is formed at the position corresponding to the blocking rod at the bottom of the grinding pressure sheet seat, an air pipe and a gas fuel pipe are fixedly connected with the top of the generating tank, and the air pipe and the gas fuel pipe are respectively communicated with the air channel and the gas fuel channel, all install electronic flow valve on air hose and the gas fuel pipe, control box fixed mounting is at the top of generating tank, install display screen and operation button on the control box, install the treater in the control box, it has temperature sensor to fix to inlay on the inside wall of generating tank one side, one side fixedly connected with power cord of generating tank.
In a preferred embodiment of the present invention, an exhaust pipe is fixedly connected to one side of the canister.
In a preferred embodiment of the present invention, a plug is connected to one end of the power cord.
As a preferred embodiment of the present invention, the power line is electrically connected to the processor, the display screen, the operation button, the first electric push rod, the second electric push rod, the stepping motor, the electric flow valve, the igniter, and the temperature sensor through the power supply circuit.
As a preferred embodiment of the present invention, the processor is electrically connected to the display screen, the operation button, the first electric push rod, the second electric push rod, the stepping motor, the electric flow valve, the igniter, and the temperature sensor, respectively.
In a preferred embodiment of the present invention, the material of the placing seat is high-temperature ceramic.
An optimized preparation method of a single-phase doped lanthanum gallate electrolyte comprises the following steps:
the method comprises the following steps: dissolving raw materials; appropriate amount of analytically pure La (NO) or more3)3·XH2O、Sr(NO3)2、Ga(NO3)3·XH2O, MgO is weighed according to stoichiometric ratio and placed in a beaker, deionized water is added to dissolve the raw materials, and then HNO is added3Reacting with MgO, adding glycine as complexing agent at a molar ratio of 1:1 to metal ions in the raw material, preferably HNO3The concentration is 45-80%;
step two: preparing precursor powder; and (3) placing the solution obtained in the step one on a magnetic stirrer, heating and stirring until the solution becomes colorless viscous colloid, and finally burning to generate LSGM precursor powder. The activation energy of the precursor powder is influenced to a great extent by the combustion process, which is an important step for judging whether a single-phase perovskite structure can be formed by subsequent high-temperature sintering. Here we regulate the combustion process by means of regulating the heating power of the stirrer, we are at 18W/g dm2-40W/g·dm2The heating power of the solution is changed within the range, and the heating power is found to be lower than 20W/g dm2When the solution is heated to 20W/g.dm, the colloid does not reach the ignition point of glycine, and even if the colorless viscous colloid is dried, the colloid does not burn, and the required precursor powder can not be formed, and when the solution is heated to 20W/g.dm2-22W/g·dm2When the solution is evaporated to form colorless transparent liquid, the liquid will spontaneously combust under the action of glycine to generate the required precursor powder, but the impurity phase (such as SrLaGaO) is easily generated during the subsequent sintering4) However, when the solution is heated to a power higher than 30W/g dm2In this case, the finally sintered sample also tends to contain a hetero-phase (e.g., SrLaGa)3O7Etc.), through a large amount of experiments, only when the heating power of the solution is 22W/g dm2-30W/g·dm2When the heating power of the solution deviates from the interval, the compound generated by high-temperature sintering contains SrLaGaO4Or SrLaGa3O7Hetero phase of which willThe conductivity of the LSGM is reduced, thereby reducing fuel cell performance.
In summary, the preferred heating power here is 22W/g dm2-30W/g·dm2；
Step three: preparing single-phase LSGM; connecting a power line of a single-phase lanthanum gallate electrolyte preparation device to an external power supply through a plug, connecting an exhaust pipe to a proper discharge position, connecting an air pipe and a gas fuel pipe to an air source and a gas fuel source with certain pressure, inputting a preparation instruction through an operation key, controlling a first electric push rod to shrink by a processor, driving a fixed seat and a placing seat to move downwards by the electric push rod, discharging the top of the placing seat from a generation tank, placing precursor powder in the step two in a placing groove of the placing seat, inputting a grinding instruction through the operation key, controlling a second electric push rod to extend by the processor, driving a movable seat to move downwards by the second electric push rod, driving a blocking rod to block a spray hole by the movable seat, then controlling the first electric push rod to continue to extend by the processor, enabling a grinding tablet seat to enter the placing groove and press a raw material, driving the placing seat to rotate by a stepping motor, thereby fully grinding the precursor powder, inputting a starting instruction through an operation key, controlling the first electric push rod to reset by the processor, controlling the electric flow valve to release air and gas fuel at a certain flow rate and simultaneously controlling the igniter to ignite, respectively enabling the air and the gas fuel to enter the mixing cavity through the air channel and the gas fuel channel to be mixed, and spraying flame from the spray hole after being ignited, monitoring the temperature by the temperature sensor, controlling the temperature of the spraying flame by the processor through controlling the flow rate of the electric flow valve to enable precursor powder to be pre-burnt for 3 hours at 700 ℃ so as to remove residual nitride, carbonate and the like, inputting a grinding instruction through the operation key, controlling the electric flow valve to close by the processor, stopping spraying flame, simultaneously controlling the second electric push rod to extend, driving the second electric push rod to move downwards, driving the blocking rod to block the spray hole by the movable seat, and then controlling the first electric push rod to continue to extend by the processor, make and grind preforming seat and get into the standing groove and push down the raw materials, step motor drives and places the seat and rotate, thereby realize the purpose of grinding, the grinding in-process, treater timing control electric putter two extends partly, make the shutoff pole outstanding, thereby make by the raw materials of compaction not hard up, then withdraw, then treater control electric putter one extends, place the seat and go upward, place the seat and grind the preforming of preforming with the raw materials seat, through abundant grinding, behind the preforming, treater control each part resets, the continuation control flame is sintered to the raw materials of preforming, last high temperature sintering generates single-phase LSGM.
In a preferred embodiment of the present invention, in the second step, the heat power of the solution is preferably 22W/g dm2-30W/g·dm2(ii) a The preferable sintering conditions in the third step are as follows: air atmosphere, 1430-1500 deg.c, 6 hr.
The invention has the beneficial effects that: the invention discloses an optimized single-phase doped lanthanum gallate electrolyte preparation device which comprises a generating tank, a base, a control box, a first electric push rod, a support frame, a fixed seat, a stepping motor, a placing seat, a convex slip ring, an annular sliding groove, a placing groove, a grinding and pressing seat, a movable groove, a movable seat, a blocking rod, a second electric push rod, an air channel, a mixing cavity, a spray hole, an air pipe, a gas fuel pipe, an electric flow valve, a display screen, an operation key, a support rod, a temperature sensor, a gas fuel channel, an exhaust pipe, a power line and an igniter.
1. The LSGM electrolyte prepared by the optimized preparation method of the single-phase lanthanum gallate-doped electrolyte is basically single-phase, and SrLaGaO is eliminated4、SrLaGa3O7The negative effect brought by the relative conductivity of the impurities can effectively improve the power of the battery, enhance the anti-attenuation performance of the battery and prolong the service life of the battery.
2. This single-phase doping lanthanum gallate electrolyte preparation facilities's of optimizing grinding preforming seat can grind, preforming and flame projecting to can accomplish a plurality of links integration of preparation process, thereby can effectual efficiency and the security that improves the preparation, can avoid polluting simultaneously, the practicality is strong.
3. This single-phase doping lanthanum gallate electrolyte preparation facilities's of optimizing grinding pressure piece seat is when grinding precursor powder, can get up the orifice shutoff of flame projecting through the shutoff pole to avoid blockking up, simultaneously, at the in-process of grinding, the shutoff pole can be with the not hard up turning up of compacted precursor powder, thereby improves the efficiency and the effect of grinding.
4. The mixing cavity is formed in the grinding tabletting seat of the optimized single-phase lanthanum gallate electrolyte preparation device, so that air and gas fuel can be uniformly mixed and then sprayed out from a plurality of uniformly distributed spray holes, and the uniformity of heating of precursor powder is improved.
Drawings
FIG. 1 is a schematic structural diagram of an optimized single-phase lanthanum gallate-doped electrolyte preparation device;
FIG. 2 is a schematic cross-sectional view of an optimized single-phase lanthanum gallate-doped electrolyte preparation device;
FIG. 3 is a schematic partial cross-sectional view of a generant canister of an optimized single-phase lanthanum gallate electrolyte preparation device;
FIG. 4 is a flow chart of the steps of an optimized single-phase lanthanum gallate-doped electrolyte preparation method;
FIG. 5 is an X-ray diffraction pattern of a single phase LSGM electrolyte;
FIG. 6 is a single phase LSGM electrolyte morphology map;
in the figure: 1. a generating tank; 2. a base; 3. a control box; 4. an electric push rod I; 5. a support frame; 6. a fixed seat; 7. a stepping motor; 8. a placing seat; 9. a male slip ring; 10. an annular chute; 11. a placement groove; 12. grinding the pressing sheet seat; 13. a movable groove; 14. a movable seat; 15. a plugging rod; 16. a second electric push rod; 17. an air passage; 18. a mixing chamber; 19. spraying a hole; 20. an air tube; 21. a gas fuel pipe; 22. an electrically operated flow valve; 23. a display screen; 24. operating a key; 25. a support bar; 26. a temperature sensor; 27. a gaseous fuel passage; 28. an exhaust pipe; 29. a power line; 30. an igniter.
Detailed Description
In order to make the technical means, the creation characteristics, the achievement purposes and the effects of the invention easy to understand, the invention is further described with the specific embodiments.
Referring to fig. 1 to 6, the present invention provides a technical solution: an optimized single-phase doped lanthanum gallate electrolyte preparation device comprises a generation tank 1, a base 2 and a control box 3, wherein support rods 25 are fixedly installed at the tops of two sides of the base 2, the generation tank 1 is fixedly installed at the tops of the support rods 25, an electric push rod I4 is fixedly installed at the central position of the top of the base 2, a support frame 5 is fixedly installed at the top of the electric push rod I4, a fixed seat 6 is fixedly installed at the top of the support frame 5, a stepping motor 7 is fixedly installed between the fixed seat 6 and the support frame 5, a convex sliding ring 9 is fixedly installed at the bottom of a placement seat 8, an annular sliding groove 10 is formed in the top of the fixed seat 6, the convex sliding ring 9 is installed in the annular sliding groove 10, a through hole is formed in the bottom of the generation tank 1, the top of the placement seat 8 penetrates through the through hole and extends into the generation tank 1, and the placement seat 8 is fixedly connected with an output shaft of the stepping motor 7, the top of the placing seat 8 is provided with a placing groove 11, a grinding pressure plate seat 12 is fixedly installed at a position corresponding to the placing seat 8 on the inner side wall of the top of the generating tank 1, a movable groove 13 is opened at the top of the grinding pressure plate seat 12, a movable seat 14 is installed in the movable groove 13, a plurality of blocking rods 15 are fixedly installed at the bottom of the movable seat 14, an electric push rod II 16 is installed at the top of the generating tank 1 through bolts, an air channel 17 and a gas fuel channel 27 are respectively arranged in two sides of the grinding pressure plate seat 12, a mixing cavity 18 is arranged in the grinding pressure plate seat 12, the air channel 17 and the gas fuel channel 27 are both communicated with the mixing cavity 18, an igniter 30 is fixedly embedded on the inner side wall of the top of the mixing cavity 18, a spray hole 19 is arranged at a position corresponding to the blocking rod 15 at the bottom of the grinding pressure plate seat 12, an air pipe 20 and a gas fuel pipe 21 are fixedly connected to the top of the generating tank 1, air hose 20 and gas fuel pipe 21 communicate with air channel 17 and gas fuel channel 27 respectively, all install electric flow valve 22 on air hose 20 and the gas fuel pipe 21, control box 3 fixed mounting is at the top of generating tank 1, install display screen 23 and operation button 24 on the control box 3, install the treater in the control box 3, fixed the inlaying has temperature sensor 26 on the inside wall of generating tank 1 one side, one side fixedly connected with power cord 29 of generating tank 1.
In a preferred embodiment of the present invention, an exhaust pipe 28 is fixedly connected to one side of the generator tank 1.
In a preferred embodiment of the present invention, a plug is connected to one end of the power cord 29.
In a preferred embodiment of the present invention, the power line 29 is electrically connected to the processor, the display 23, the operation buttons 24, the first electric push rod 4, the second electric push rod 16, the stepping motor 7, the electric flow valve 22, the igniter 30 and the temperature sensor 26 through the power supply circuit.
In a preferred embodiment of the present invention, the processor is electrically connected to the display screen 23, the operation buttons 24, the first electric push rod 4, the second electric push rod 16, the stepping motor 7, the electric flow valve 22, the igniter 30 and the temperature sensor 26, respectively.
In a preferred embodiment of the present invention, the material of the placing base 8 is high temperature ceramic.
An optimized preparation method of a single-phase doped lanthanum gallate electrolyte comprises the following steps:
the method comprises the following steps: dissolving raw materials; appropriate amount of analytically pure La (NO) or more3)3·XH2O、Sr(NO3)2、Ga(NO3)3·XH2O, MgO is weighed according to stoichiometric ratio and placed in a beaker, deionized water is added to dissolve the raw materials, and then HNO is added3Reacting with MgO, adding glycine as complexing agent at a molar ratio of 1:1 to metal ions in the raw material, preferably HNO3The concentration is 45-80%;
step two: preparing precursor powder; putting the solution obtained in the step one on a magnetic stirrer, heating and stirring until the solution is changed into colorless viscous colloid, finally burning to generate LSGM precursor powder, wherein the burning process influences the activation energy of the precursor powder to a great extent, which is an important step for judging whether a single-phase perovskite structure can be formed by subsequent high-temperature sintering, and the burning process is regulated by regulating the heating power of the stirrer, namely the burning process is regulated at 18W/g dm2-40W/g·dm2The heating power of the solution is changed within the range, and the heating power is found to be lower than 20W/g dm2When the colloid does not reach the glycine fuelEven if the colorless viscous colloid is dried, the colloid is not burnt, the required precursor powder can not be formed, and when the heating power of the solution is 20W/g dm2-22W/g·dm2When the solution is evaporated to form colorless transparent liquid, the liquid will spontaneously combust under the action of glycine to generate the required precursor powder, but the impurity phase (such as SrLaGaO) is easily generated during the subsequent sintering4) However, when the solution is heated to a power higher than 30W/g dm2In this case, the finally sintered sample also tends to contain a hetero-phase (e.g., SrLaGa)3O7Etc.), through a large amount of experiments, only when the heating power of the solution is 22W/g dm2-30W/g·dm2When the heating power of the solution deviates from the interval, the compound generated by high-temperature sintering contains SrLaGaO4Or SrLaGa3O7Hetero-phase, which will reduce the conductivity of the LSGM, thereby reducing fuel cell performance.
In summary, the preferred heating power here is 22W/g dm2-30W/g·dm2；
Step three: preparing single-phase LSGM; connecting a power line 29 of a single-phase lanthanum gallate-doped electrolyte preparation device to an external power supply through a plug, connecting an exhaust pipe 28 to a proper discharge position, connecting an air pipe 20 and a gas fuel pipe 21 to an air source and a gas fuel source with certain pressure, inputting a preparation instruction through an operation key 24, controlling a first electric push rod 4 to shrink by a processor, driving a fixed seat 6 and a placing seat 8 to move downwards by the first electric push rod 4, discharging the top of the placing seat 8 from a generating tank 1, placing the precursor powder in the second step into a placing groove 11 of the placing seat 8, inputting a grinding instruction through the operation key 24, controlling a second electric push rod 16 to extend by the processor, driving a movable seat 14 to move downwards by the second electric push rod 16, driving a blocking rod 15 by the movable seat 14 to block a spray hole 19, then controlling the first electric push rod 4 to extend continuously by the processor, enabling a grinding tablet pressing seat 12 to enter the placing groove 11 and press raw materials, the stepping motor 7 drives the placing seat 8 to rotate, so that precursor powder is fully ground, a start instruction is input through the operation key 24, the processor controls the first electric push rod 4 to reset, the processor controls the electric flow valve 22 to release air and gas fuel at a certain flow rate and simultaneously controls the igniter 30 to ignite, the air and the gas fuel respectively enter the mixing cavity 18 through the air channel 17 and the gas fuel channel 27 to be mixed and then spray flame from the spray hole 19 after being ignited, the temperature sensor 26 monitors the temperature, the processor controls the temperature of the spray flame through controlling the flow rate of the electric flow valve 22 to pre-burn the precursor powder at 700 ℃ for 3 hours to remove residual nitride, carbonate and the like, the grinding instruction is input through the operation key 24, the processor controls the electric flow valve 22 to close, the spray flame is stopped, the second electric push rod 16 is controlled to extend, the second electric push rod 16 drives the movable seat 14 to go down, the sliding seat 14 drives the plugging rod 15 to plug the orifice 19, then the processor controls the electric push rod 4 to continue to extend, the grinding pressure piece seat 12 enters the placing groove 11 and presses the raw material, the stepping motor 7 drives the placing seat 8 to rotate, thereby realizing the grinding purpose, in the grinding process, the processor controls the electric push rod 16 to extend partially, the plugging rod 15 protrudes, thereby the compacted raw material is loosened, then the raw material is withdrawn, then the processor controls the electric push rod 4 to extend, the placing seat 8 goes upward, the placing seat 8 and the grinding pressure piece seat 12 press the raw material into pieces, after full grinding and pressing, each part is reset by the processor control, the raw material of the pressing piece is sintered by continuously controlling flame spraying, and finally, single-phase LSGM is generated by high-temperature sintering.
In a preferred embodiment of the present invention, in the second step, the heat power of the solution is preferably 22W/g dm2-30W/g·dm2(ii) a The preferable sintering conditions in the third step are as follows: air atmosphere, 1430-1500 deg.c, 6 hr.
As a preferred embodiment of the present invention, the grinding and tablet-pressing base 12 can perform grinding, tablet pressing and fire spraying, so that multiple steps of the preparation process can be integrally completed, thereby effectively improving the efficiency and safety of the preparation, and simultaneously avoiding pollution, the practicability is strong, when the grinding and tablet-pressing base 12 grinds the precursor powder, the spray holes 19 of the fire spraying can be blocked by the blocking rod 15, thereby avoiding blockage, and simultaneously, during the grinding process,the plugging rod 15 can loosen and turn up the compacted precursor powder, so that the grinding efficiency and effect are improved, the mixing cavity 18 is formed in the grinding pressing sheet seat 12, air and gas fuel can be uniformly mixed and then sprayed out from a plurality of uniformly distributed spray holes 19, the heating uniformity of the precursor powder is improved, the LSGM electrolyte prepared by the optimized single-phase lanthanum gallate electrolyte preparation method is basically single-phase, and SrLaGaO is eliminated4、SrLaGa3O7The negative effect brought by the relative conductivity of the impurities can effectively improve the power of the battery, enhance the anti-attenuation performance of the battery and prolong the service life of the battery.
Comparative example 1:
preparing LSGM by a solid phase reaction technology: la203And MgO are respectively presintered for 10 hours at 980 ℃ to remove carbonate and moisture in the La and the La which are dried203MgO and SrCO3、Ga2O3Weighing according to the stoichiometric ratio, fully grinding, presintering at 1000 ℃ for 20 hours, then regrinding, tabletting, sintering at 1200 ℃ for 20 hours in an air atmosphere, then continuously grinding, tabletting and sintering at 1550 ℃ for 20 hours to generate the LSGM electrolyte.
The LSGM prepared in comparative example 1 has a monoclinic structure, a lattice symbol of I2/a, and an electrical conductivity of about 9.72X 10 at 700 deg.C- 3S·cm-1The sample easily contains SrLaGaO4、SrLaGa3O7The mixed phase is obtained by comparing the embodiment with the comparative example 1, the embodiment prepares precursor powder by regulating the heating power of the solution and utilizing a glycine combustion method, and meanwhile, the electrolyte LSGM prepared by the device is basically single-phase and belongs to an orthogonal structure, the lattice symbol is Imma, and the crystal symmetry is higher than that of the comparative example 1; the conductivity of the LSGM prepared in the example was about 3.82X 10 at 700 deg.C-2S·cm-1Higher than in comparative example 1; meanwhile, the embodiment has low sintering temperature, short sintering time and simple preparation process.
Comparative example 2:
the procedure for preparing LSGM as an electrolyte was the same as in example 1 except that the solution was heated at a power of 19W/g dm in the second step2。
The LSGM prepared by this comparative example contains a heterophase SrLaGaO4The main phase is an orthogonal structure, the lattice symbol is Imma, and the conductivity at 700 ℃ is about 8.75 multiplied by 10-3S·cm-1。
As can be seen from the comparison of examples and comparative example 2, the heat power of the solution was less than 22W/g dm2In this case, the prepared LSGM is liable to contain a hetero phase, resulting in a decrease in conductivity.
Comparative example 3:
the procedure for preparing LSGM as an electrolyte was the same as in example 1 except that the solution was heated at 35W/g dm in the second step2。
The LSGM prepared by this comparative example contains a heterophase SrLaGaO4The main phase is still in an orthogonal structure, the lattice symbol is Imma, and the conductivity at 700 ℃ is about 5.43 multiplied by 10-3S·cm-1。
As can be seen from the comparison of examples and comparative example 2, the heating power of the solution was higher than 30W/g dm2In this case, the prepared LSGM is liable to contain a hetero phase, resulting in a decrease in conductivity.
While there have been shown and described what are at present considered the fundamental principles and essential features of the invention and its advantages, it will be apparent to those skilled in the art that the invention is not limited to the details of the foregoing exemplary embodiments, but is capable of other specific forms without departing from the spirit or essential characteristics thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein. Any reference sign in a claim should not be construed as limiting the claim concerned.
Furthermore, it should be understood that although the present description refers to embodiments, not every embodiment may contain only a single embodiment, and such description is for clarity only, and those skilled in the art should integrate the description, and the embodiments may be combined as appropriate to form other embodiments understood by those skilled in the art.
Claims (8)
1. The optimized single-phase doped lanthanum gallate electrolyte preparation device comprises a generation tank (1), a base (2) and a control box (3), and is characterized in that supporting rods (25) are fixedly installed at the tops of two sides of the base (2), the generation tank (1) is fixedly installed at the tops of the supporting rods (25), a first electric push rod (4) is fixedly installed at the center position of the top of the base (2), a supporting frame (5) is fixedly installed at the top of the first electric push rod (4), a fixed seat (6) is fixedly installed at the top of the supporting frame (5), a stepping motor (7) is fixedly installed between the fixed seat (6) and the supporting frame (5), a convex sliding ring (9) is fixedly installed at the bottom of a placing seat (8), an annular sliding groove (10) is formed in the top of the fixed seat (6), and the convex sliding ring (9) is installed in the annular sliding groove (10), the bottom of the generating tank (1) is provided with a through hole, the top of the placing seat (8) penetrates through the through hole and extends into the generating tank (1), the placing seat (8) is fixedly connected with an output shaft of the stepping motor (7), the top of the placing seat (8) is provided with a placing groove (11), a grinding pressure sheet seat (12) is fixedly installed at a position corresponding to the placing seat (8) on the inner side wall of the top of the generating tank (1), the top of the grinding pressure sheet seat (12) is provided with a movable groove (13), a movable seat (14) is installed in the movable groove (13), the bottom of the movable seat (14) is fixedly provided with a plurality of blocking rods (15), the top of the generating tank (1) is provided with a second electric push rod (16) through bolts, and air channels (17) and gas fuel channels (27) are respectively arranged in two sides of the grinding pressure sheet seat (12), offer hybrid chamber (18) in grinding pressure plate seat (12), air passage (17) and gas fuel passageway (27) all communicate with hybrid chamber (18), fixed the inlaying has some firearm (30) on the inside wall at hybrid chamber (18) top, the bottom of grinding pressure plate seat (12) has seted up orifice (19) with the position department that shutoff pole (15) correspond, the top fixedly connected with air hose (20) and gas fuel pipe (21) of generating tank (1), air hose (20) and gas fuel pipe (21) communicate with air passage (17) and gas fuel passageway (27) respectively, all install electronic flow valve (22) on air hose (20) and gas fuel pipe (21), control box (3) fixed mounting is at the top of generating tank (1), install display screen (23) and operation button (24) on control box (3), install the treater in control box (3), it has temperature sensor (26) to fix to inlay on the inside wall of generating tank (1) one side, one side fixedly connected with power cord (29) of generating tank (1).
2. The optimized single-phase doped lanthanum gallate electrolyte preparation device according to claim 1, wherein: and an exhaust pipe (28) is fixedly connected to one side of the generating tank (1).
3. The optimized single-phase doped lanthanum gallate electrolyte preparation device according to claim 1, wherein: one end of the power line (29) is connected with a plug.
4. The optimized single-phase doped lanthanum gallate electrolyte preparation device according to claim 1, wherein: the power line (29) is electrically connected with the processor, the display screen (23), the operation key (24), the electric push rod I (4), the electric push rod II (16), the stepping motor (7), the electric flow valve (22), the igniter (30) and the temperature sensor (26) through the power supply circuit respectively.
5. The optimized single-phase doped lanthanum gallate electrolyte preparation device according to claim 1, wherein: the processor is respectively and electrically connected with the display screen (23), the operation key (24), the electric push rod I (4), the electric push rod II (16), the stepping motor (7), the electric flow valve (22), the igniter (30) and the temperature sensor (26).
6. The optimized single-phase doped lanthanum gallate electrolyte preparation device according to claim 1, wherein: the placing seat (8) is made of high-temperature ceramics.
7. An optimized preparation method of a single-phase doped lanthanum gallate electrolyte is characterized by comprising the following steps:
step (ii) ofFirstly, the method comprises the following steps: dissolving raw materials; appropriate amount of analytically pure La (NO) or more3)3·XH2O、Sr(NO3)2、Ga(NO3)3·XH2O, MgO is weighed according to stoichiometric ratio and placed in a beaker, deionized water is added to dissolve the raw materials, and then HNO is added3Reacting with MgO, adding glycine as complexing agent at a molar ratio of 1:1 to metal ions in the raw material, and HNO3The concentration is 45-80%;
step two: preparing precursor powder; putting the solution obtained in the step one on a magnetic stirrer, heating and stirring until the solution becomes colorless viscous colloid, and finally burning to generate LSGM precursor powder with the heating power of 22W/g dm2-30W/g·dm2；
Step three: preparing single-phase LSGM; connecting a power line (29) of a single-phase doped lanthanum gallate electrolyte preparation device to an external power supply through a plug, connecting an exhaust pipe (28) to a proper discharge position, connecting an air pipe (20) and a gas fuel pipe (21) to an air source and a gas fuel source with certain pressure, inputting a preparation instruction through an operation key (24), controlling a first electric push rod (4) to contract by a processor, driving a fixing seat (6) and a placing seat (8) to move downwards by the first electric push rod (4), enabling the top of the placing seat (8) to come out of a generating tank (1), placing precursor powder in the second step into a placing groove (11) of the placing seat (8), inputting a grinding instruction through the operation key (24), controlling a second electric push rod (16) to extend by the processor, driving a movable seat (14) to move downwards by the second electric push rod (16), driving a blocking rod (15) to block a spray hole (19) by the movable seat (14), then the processor controls the electric push rod I (4) to extend continuously, the grinding and pressing sheet seat (12) enters the placing groove (11) and presses the raw materials, the stepping motor (7) drives the placing seat (8) to rotate, so that the precursor powder is fully ground, a start instruction is input through an operation key (24), the processor controls the electric push rod I (4) to reset, the processor controls the electric flow valve (22) to release air and gas fuel at a certain flow rate and simultaneously controls the igniter (30) to ignite, the air and the gas fuel respectively enter the mixing cavity (18) through the air channel (17) and the gas fuel channel (27) to be mixed, after being ignited, the flame is sprayed out from the spray hole (19), the temperature sensor (26) monitors the temperature, the processor controls the temperature of the spray flame through controlling the flow rate of the electric flow valve (22), so that the precursor powder is presintered for 3 hours at 700 ℃, to remove the residual nitride and carbonate, a grinding instruction is input through an operation key (24), a processor controls an electric flow valve (22) to close, the flame spraying is stopped, meanwhile, an electric push rod II (16) is controlled to extend, the electric push rod II (16) drives a movable seat (14) to move downwards, the movable seat (14) drives a blocking rod (15) to block a spray hole (19), then, the processor controls an electric push rod I (4) to continue to extend, a grinding pressure sheet seat (12) enters a placing groove (11) and presses a raw material, a stepping motor (7) drives the placing seat (8) to rotate, so that the grinding purpose is realized, in the grinding process, the processor controls a part of the electric push rod II (16) to extend in a timing mode, the blocking rod (15) protrudes, so that the compacted raw material is loosened and then is retracted, then, the processor controls the electric push rod I (4) to extend, the placing seat (8) moves upwards, the placing seat (8) and the grinding and tabletting seat (12) are used for tabletting the raw materials, after full grinding and tabletting, the processor controls all the components to reset, the flame throwing is continuously controlled to sinter the tabletted raw materials, and finally, the single-phase LSGM is generated through high-temperature sintering.
8. The optimized preparation method of the single-phase doped lanthanum gallate electrolyte according to claim 7, wherein the method comprises the following steps: in the second step, the heating power of the solution is 22W/g.dm2-30W/g·dm2(ii) a In the third step, the sintering conditions are as follows: air atmosphere, 1430-1500 deg.c, 6 hr.
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