CN114068798A - High-performance thermoelectric thick film and method for rapidly preparing same - Google Patents

High-performance thermoelectric thick film and method for rapidly preparing same Download PDF

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CN114068798A
CN114068798A CN202111345897.8A CN202111345897A CN114068798A CN 114068798 A CN114068798 A CN 114068798A CN 202111345897 A CN202111345897 A CN 202111345897A CN 114068798 A CN114068798 A CN 114068798A
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thermoelectric
thick film
thermoelectric thick
pressure
powder
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邓元
严跃冬
张玮峰
华小社
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Hangzhou Innovation Research Institute of Beihang University
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Hangzhou Innovation Research Institute of Beihang University
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/01—Manufacture or treatment
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80—Constructional details
    • H10N10/85—Thermoelectric active materials
    • H10N10/851—Thermoelectric active materials comprising inorganic compositions
    • H10N10/852—Thermoelectric active materials comprising inorganic compositions comprising tellurium, selenium or sulfur

Abstract

The invention relates to a method for rapidly preparing a high-performance thermoelectric thick film, which realizes the preparation of the thermoelectric thick film in a powder metallurgy mode. The method can realize the preparation of the thermoelectric thick film with the thickness of less than 200 mu m, has very good compatibility, and can be used for preparing various thermoelectric material thick films in low, medium and high temperature areas. The method has simple process and low material and equipment cost, can realize large-scale industrialized rapid preparation of the high-performance thermoelectric thick film, and further constructs various high-performance micro thermoelectric power generation or refrigeration devices, including high-density or flexible thermoelectric devices, thereby laying a foundation for rapid development of the high-performance micro thick film thermoelectric devices.

Description

High-performance thermoelectric thick film and method for rapidly preparing same
Technical Field
The invention belongs to the technical field of thermoelectric materials, and particularly relates to a high-performance thermoelectric thick film and a method for rapidly preparing the high-performance thermoelectric thick film.
Background
Thermoelectric conversion technology based on thermoelectric materials can realize thermoelectric generation through a Seebeck effect or realize quick refrigeration through a Peltier effect, is a new energy technology capable of realizing direct interconversion between heat energy and electric energy, has the advantages of no moving parts, no noise, no pollution, portability, micromation, long-term stability and the like, and has wide application in the aspects of waste heat energy collection, precise temperature control and the like. The current commercial thermoelectric power generation or refrigeration devices are all constructed by adopting block thermoelectric materials, namely, the thickness of a thermoelectric arm is generally more than 500 mu m, which limits the further miniaturization of the thermoelectric devices, and the block refrigeration devices also have the defects of low refrigeration power density and slow response speed. The thermoelectric device constructed by the thermoelectric thin film with the thickness less than 10 μm can compensate the defects of the bulk device, but is difficult to generate large refrigeration temperature difference. The thermoelectric refrigerator constructed by the thermoelectric thick film with the thickness of 10-500 mu m has the comprehensive performance of high response speed and larger refrigerating temperature difference, and the thick film thermoelectric device has the advantages of easy flexibility, miniaturization and high density. In recent years, continuous miniaturization of electronic devices and development of wearable equipment have brought urgent demands on precise temperature control, rapid refrigeration and flexible micro self-power supply of micro devices, so that it is of great significance to develop a method for rapidly preparing high-performance thermoelectric thick films to develop thick film thermoelectric devices.
At present, the thermoelectric thick film is mainly prepared by cutting thinning or thermoelectric paste printing. The cutting thinning method is difficult to cut the thermoelectric block body to a thickness of 200 μm or less, and repeated machining may cause secondary damage to the material. The printing method of the thermoelectric slurry is to prepare thermoelectric powder, a binder, an organic solvent, a dispersant and the like into the thermoelectric slurry with proper viscosity, then print the thermoelectric slurry into a film, dry the solvent, and finally sinter the film to remove organic components to obtain the thermoelectric thick film. This method has the following disadvantages: 1. the process is complicated; 2. the formulated slurry is commonly usedToxic organic matter; 3. the surface of the prepared thermoelectric thick film is rough; 4. after sintering to remove organic components, defects such as holes and cracks can be left in the thick film, so that the thermoelectric thick film has poor compactness and low thermoelectric property, and the Bi prepared by the method2Te3The power factor of the base thermoelectric thick film is usually less than 20 μ W-cm-1·K-2. Therefore, it is urgently needed to develop a new simpler and environmental-friendly method for realizing the rapid preparation of the high-performance thermoelectric thick film.
Disclosure of Invention
In order to solve the above problems in the prior art, the present invention provides a high performance thermoelectric thick film and a method for rapidly preparing the high performance thermoelectric thick film. The method is a powder metallurgy method, particularly, thermoelectric powder is used as a raw material, and the high-performance thermoelectric thick film is prepared by direct tabletting and sintering with the aid of a prepressing die.
The technical scheme adopted by the invention is as follows:
a method for rapidly preparing a high-performance thermoelectric thick film adopts a powder metallurgy mode to rapidly prepare the high-performance thermoelectric thick film.
The method for preparing the high-performance thermoelectric thick film by powder metallurgy comprises the following steps:
(1) pre-pressing and forming: paving thermoelectric powder in a pre-pressing die, and then applying proper pressure to obtain a sheet-shaped thermoelectric thick film;
(2) carrying out high-pressure cold pressing on the sheet-shaped thermoelectric thick film in the step (1), and maintaining the pressure for a certain time to obtain a densified thermoelectric thick film;
(3) and (3) annealing and sintering the thermoelectric thick film densified in the step (2) to obtain the high-performance thermoelectric thick film.
In the step (1), the particle size of the thermoelectric powder is smaller than the thickness of the sheet-shaped thermoelectric thick film.
In the step (1), the thermoelectric powder is Bi2Te3A base thermoelectric powder.
The Bi2Te3Base thermoelectric powerThe powder is Bi2Te3Or Bi0.5Sb1.5Te3。
In the step (1), the applied pressure is 100-400MPa when the pressing is performed.
In the step (1), the prepressing die is made of a hard material.
In the step (2), the pressure of the cold pressing is 400-1200MPa, and the pressure maintaining time is 1-10 min.
In the step (3), sintering is carried out under the argon atmosphere of one atmosphere;
the annealing sintering temperature is 300-500 ℃, and the annealing time is 0.5-2 h.
The high-performance thermoelectric thick film prepared by the method.
The invention has the beneficial effects that:
according to the method for rapidly preparing the high-performance thermoelectric thick film, the thermoelectric powder is used as a raw material in a powder metallurgy mode, under the assistance of a prepressing die, the uniformity and the thickness of the thermoelectric thick film are effectively controlled by a prepressing forming method, then the thermoelectric thick film with high compactness is obtained through high-pressure cold pressing and annealing, and the finally prepared thermoelectric thick film not only has a smooth surface, but also has high thermoelectric performance. Experimental data show that the n-Bi prepared by the method of the invention2Te3The power factor of the thick film can reach 26 muW cm at room temperature-1·K-2，p-Bi0.5Sb1.5Te3The power factor of the thick film can reach 29 muW cm at room temperature-1·K-2. The method can realize the preparation of the thermoelectric thick film with the thickness of less than 200 mu m, has very good compatibility, and can be used for preparing various thermoelectric material thick films in low, medium and high temperature areas. The method has the advantages of simple process and low material and equipment cost, can realize large-scale industrialized rapid preparation of the high-performance thermoelectric thick film, and can construct various high-performance micro thermoelectric power generation or refrigeration devices including high-density or flexible thermoelectric devices by patterning the thermoelectric thick film into the micro thick film thermoelectric arm by utilizing laser cutting, micro mechanical cutting and other modes. Therefore, the method of the invention is to be a high performance micro thick film thermoelectric deviceLays a solid foundation for the rapid development of the method.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to the drawings without creative efforts.
FIG. 1 shows n-type Bi according to example 1 of the present invention2Te3A preparation process flow chart of the thermoelectric thick film;
FIG. 2A is a 150 μm thick n-type Bi as described in example 12Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change with the annealing temperature;
FIG. 2B is the 150 μm thick n-type Bi described in example 12Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change trend graph along with the annealing time;
FIG. 2C is the 150 μm thick n-type Bi described in example 12Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change trend graph along with the cold pressure;
FIG. 3A is a 150 μm thick p-type Bi as described in example 20.5Sb1.5Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change with the annealing temperature;
FIG. 3B is a 150 μm thick p-type Bi as described in example 20.5Sb1.5Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change trend graph along with the annealing time;
FIG. 3C is the 150 μm thick p-type Bi described in example 20.5Sb1.5Te3The electric conductivity, the Seebeck coefficient and the power factor of the thermoelectric thick film change trend graph along with the cold pressure;
FIG. 4 shows Bi of 29 μm thickness described in example 32Te3Scanning electron microscope image of thermoelectric thick film section morphology;
FIG. 5 shows Bi of 52 μm thickness described in example 42Te3Scanning electron microscope image of thermoelectric thick film section morphology;
FIG. 6 shows Bi of 106 μm thickness described in example 52Te3Scanning electron microscope image of thermoelectric thick film section morphology;
FIG. 7 shows Bi of 175 μm thickness described in example 62Te3Scanning electron microscope image of thermoelectric thick film profile.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the technical solutions of the present invention will be described in detail below. It is to be understood that the described embodiments are merely exemplary of the invention, and not restrictive of the full scope of the invention. All other embodiments, which can be derived by a person skilled in the art from the examples given herein without any inventive step, are within the scope of the present invention.
Example 1
This example provides a method for rapidly preparing a high performance thermoelectric thick film of n-type Bi of 150 μm thickness2Te3Thermoelectric thick films.
The n-type Bi2Te3The preparation process flow of the thermoelectric thick film is shown in figure 1, and specifically comprises the following steps:
(1) manufacturing a 250-micrometer-deep groove on a 400-micrometer-thick aluminum oxide flat plate to serve as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 70 mu m by using a screen mesh2Te3Weighing 656mg of thermoelectric powder, placing the thermoelectric powder in a groove of a prepressing die, and paving the thermoelectric powder in the groove with the depth of 250 mu m; applying 150MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm, and pressing to obtain a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel and capable of just placing the wafer with the diameter of 20mm, applying the pressure of 400-1200MPa by using a tabletting machine and maintaining the pressure for 1min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at the temperature of 300-500 ℃ for 0.5-2h to finally obtain the n-type Bi with the high thermoelectric property and the thickness of 150 mu m2Te3Thermoelectric thick films.
By fixing the cold pressing pressure of 800MPa and the annealing time of 1h, Bi is studied at different annealing temperatures within the range of 300-2Te3The electric conductivity, Seebeck coefficient and power factor of the thick film change with the annealing temperature, as shown in FIG. 2A, the power factor of the thermoelectric thick film is the largest when the annealing temperature is 450 ℃.
By fixing the cold pressing pressure of 800MPa and the annealing temperature of 450 ℃, Bi is researched under different annealing times of 0.5-2h2Te3The electric conductivity, Seebeck coefficient and power factor of the thick film change trend along with the annealing time, as shown in FIG. 2B, the power factor of the thermoelectric thick film prepared when the annealing time is 1h is the largest.
By fixing the annealing temperature at 450 ℃ and the annealing time at 1h, Bi under different cold-pressing pressures of 400-1200MPa is studied2Te3The electric conductivity, Seebeck coefficient and power factor of the thick film change with the cold pressing pressure, as shown in figure 2C, the annealing and sintering can greatly improve Bi2Te3The thermoelectric property of the thick film is in the range of the cold pressure of 400-1200MPa, the characteristics that the thermoelectric property is higher when the cold pressure is higher are generally presented, but the influence is smaller.
The data show that n-type Bi of 150 μm thickness at room temperature2Te3The power factor of the thermoelectric thick film can reach 26 muW cm-1·K-2。
Example 2
This example provides a method for rapidly preparing a high performance thermoelectric thick film of p-type Bi of 150 μm thickness0.5Sb1.5Te3Thermoelectric thick films.
The p-type Bi0.5Sb1.5Te3The preparation method specifically comprises the following steps:
(1) manufacturing a 250-micrometer-deep groove on a 400-micrometer-thick aluminum oxide flat plate to serve as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 70 mu m by using a screen mesh0.5Sb1.5Te3Weighing 544mg of thermoelectric powder, placing the thermoelectric powder in a groove of a pre-pressing die, and paving the thermoelectric powder in the groove with the depth of 250 microns; applying 150MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm, and pressing to obtain a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel and capable of just placing the wafer with the diameter of 20mm, applying the pressure of 400-1200MPa by using a tabletting machine and maintaining the pressure for 1min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at the temperature of 300-500 ℃ for 0.5-2h to finally obtain the p-type Bi with the high thermoelectric property and the thickness of 150 mu m0.5Sb1.5Te3Thermoelectric thick films.
By fixing the cold pressing pressure of 800MPa and the annealing time of 1h, Bi at different annealing temperatures of 300 ℃ and 500 ℃ is studied0.5Sb1.5Te3The conductivity, Seebeck coefficient and power factor of the thick film change with the annealing temperature, as shown in FIG. 3A, when the annealing temperature is 450 ℃, p-type Bi is prepared0.5Sb1.5Te3The power factor of the thermoelectric thick film is maximized.
By fixing the cold pressing pressure of 800MPa and the annealing temperature of 450 ℃, Bi is researched under different annealing times of 0.5-2h0.5Sb1.5Te3The electric conductivity, Seebeck coefficient and power factor of the thick film change with the annealing time, as shown in FIG. 3B, the power factor of the thermoelectric thick film is the largest when the annealing time is 1.5 h.
By setting the annealing temperature toThe annealing time is 1.5h at 450 ℃, and the study shows that Bi is present under different cold pressure intensities of 400-1200MPa0.5Sb1.5Te3The electric conductivity, Seebeck coefficient and power factor of the thick film change with the cold pressing pressure, as shown in FIG. 3C, the annealing and sintering can greatly improve Bi0.5Sb1.5Te3The thermoelectric property of the thick film is in the range of the cold pressure of 400-1200MPa, the characteristics that the thermoelectric property is higher when the cold pressure is higher are generally presented, but the influence is smaller.
The data show that p-type Bi of 150 μm thickness at room temperature0.5Sb1.5Te3The power factor of the thermoelectric thick film reaches 29 mu W cm-1·K-2。
Example 3
This example provides a method for rapidly preparing a high performance thermoelectric thick film of n-type Bi 29 μm thick2Te3Thermoelectric thick films.
The n-type Bi2Te3The preparation method of the thermoelectric thick film comprises the following steps:
(1) manufacturing a groove with the depth of 40 mu m on an alumina flat plate with the thickness of 400 mu m to be used as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 10 mu m by using a screen mesh2Te3Weighing 127mg of thermoelectric powder, placing the thermoelectric powder in a groove of a prepressing die, and paving the thermoelectric powder in the groove with the depth of 40 mu m; applying 400MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm to press a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel, wherein the wafer with the diameter of 20mm can be just placed in the high-pressure tabletting mold, applying 800MPa pressure by using a tabletting machine and maintaining the pressure for 10min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at the temperature of 450 ℃ for 1h to finally prepare the thermoelectric thick filmObtaining the n-type Bi with the thickness of 29 mu m and high thermoelectric property2Te3Thermoelectric thick films.
FIG. 4 shows Bi of 29 μm thickness prepared by the method of this example2Te3Scanning electron microscope image of the profile morphology of the thermoelectric thick film, from which it can be seen that the Bi2Te3The thickness of the thermoelectric thick film is uniform, and the structure is compact. Measuring the 29 μm-thick Bi2Te3The power factor of the thermoelectric thick film is 25.78 μ W cm-1·K-2。
Example 4
This example provides a method for rapidly preparing a high performance thermoelectric thick film of n-type Bi of 52 μm thickness2Te3Thermoelectric thick films.
The n-type Bi2Te3The preparation method of the thermoelectric thick film comprises the following steps:
(1) manufacturing a 70-micron deep groove on a 400-micron thick aluminum oxide flat plate to be used as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 30 mu m by using a screen mesh2Te3Weighing 228mg of thermoelectric powder, placing the thermoelectric powder in a groove of a pre-pressing die, and paving the thermoelectric powder in the groove with the depth of 70 mu m; applying 400MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm to press a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel, wherein the wafer with the diameter of 20mm can be just placed in the high-pressure tabletting mold, applying 800MPa pressure by using a tabletting machine and maintaining the pressure for 10min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at 450 ℃ for 1h to finally obtain the n-type Bi with the thickness of 52 mu m and high thermoelectric property2Te3Thermoelectric thick films.
This embodiment is shown in FIG. 5Examples 52 μm thick Bi prepared by the method2Te3Scanning electron microscope image of the profile morphology of the thermoelectric thick film, from which it can be seen that the Bi2Te3The thickness of the thermoelectric thick film is uniform, and the structure is compact. Measuring the Bi of 52 μm thickness2Te3The power factor of the thermoelectric thick film is 26.15 muW cm-1·K-2。
Example 5
This example provides a method for rapidly preparing a high performance thermoelectric thick film of n-type Bi of 106 μm thickness2Te3Thermoelectric thick films.
The n-type Bi2Te3The preparation method of the thermoelectric thick film comprises the following steps:
(1) manufacturing a groove with the depth of 150 mu m on an alumina flat plate with the thickness of 400 mu m to be used as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 70 mu m by using a screen mesh2Te3Weighing 464mg of thermoelectric powder, placing the thermoelectric powder in a groove of a prepressing die, and paving the thermoelectric powder in the groove with the depth of 150 microns; applying 100MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm, and pressing to obtain a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel, wherein the wafer with the diameter of 20mm can be just placed in the high-pressure tabletting mold, applying 800MPa pressure by using a tabletting machine and maintaining the pressure for 1min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at 450 ℃ for 1h to finally obtain the n-type Bi with the high thermoelectric property and the thickness of 106 mu m2Te3Thermoelectric thick films.
FIG. 6 shows Bi of 106 μm thickness prepared by the method of this example2Te3Scanning electron microscope image of the profile morphology of the thermoelectric thick film, from which it can be seen that the Bi2Te3The thickness of the thermoelectric thick film is uniform, and the structure is compact. Measuring the Bi thickness of 106 μm2Te3The power factor of the thermoelectric thick film is 26.23 muW cm-1·K-2。
Example 6
This example provides a method for rapidly preparing a high performance thermoelectric thick film of n-type Bi 175 μm thick2Te3Thermoelectric thick films.
The n-type Bi2Te3The preparation method of the thermoelectric thick film comprises the following steps:
(1) manufacturing a 250-micrometer-deep groove on a 400-micrometer-thick aluminum oxide flat plate to serve as a prepressing die of thermoelectric powder, and cleaning the prepressing die by using ethanol;
screening Bi with the particle size of less than 70 mu m by using a screen mesh2Te3765mg of thermoelectric powder is weighed and placed in a groove of a prepressing die, and the thermoelectric powder is exactly paved in the groove with the depth of 250 mu m; applying 150MPa pressure on the paved thermoelectric powder by using a pressure head with the diameter of 20mm, and pressing to obtain a thermoelectric film wafer with the diameter of 20 mm;
(2) transferring the thermoelectric film wafer in the step (1) into a high-pressure tabletting mold made of high-hardness chrome steel, wherein the wafer with the diameter of 20mm can be just placed in the high-pressure tabletting mold, applying 800MPa pressure by using a tabletting machine and maintaining the pressure for 1min to realize the densification of the thermoelectric thick film and obtain the densified thermoelectric thick film;
(3) transferring the thermoelectric thick film densified in the step (2) into a quartz tube furnace, vacuumizing, introducing Ar gas with the flow of 200sccm and the pressure of 1atm, heating, annealing and sintering at 450 ℃ for 1h to finally obtain the n-type Bi with the thickness of 175 mu m and high thermoelectric property2Te3Thermoelectric thick films.
FIG. 7 shows Bi of 175 μm thickness prepared by the method of this example2Te3Scanning electron microscope image of the profile morphology of the thermoelectric thick film, from which it can be seen that the Bi2Te3The thickness of the thermoelectric thick film is uniform, and the structure is compact. Measuring the 175 μm thick Bi2Te3The power factor of the thermoelectric thick film is 26.09μW·cm-1·K-2。
The above description is only for the specific embodiments of the present invention, but the scope of the present invention is not limited thereto, and any person skilled in the art can easily conceive of the changes or substitutions within the technical scope of the present invention, and all the changes or substitutions should be covered within the scope of the present invention. Therefore, the protection scope of the present invention shall be subject to the protection scope of the appended claims.

Claims (10)

1. A method for rapidly preparing a high-performance thermoelectric thick film is characterized in that the high-performance thermoelectric thick film is rapidly prepared by adopting a powder metallurgy mode.
2. The method of rapidly fabricating a high performance thermoelectric thick film according to claim 1, wherein the powder metallurgy fabricating a thermoelectric thick film comprises the steps of:
(1) pre-pressing and forming: paving thermoelectric powder in a pre-pressing die, and then applying proper pressure to press to obtain a sheet-shaped thermoelectric thick film;
(2) carrying out high-pressure cold pressing on the sheet-shaped thermoelectric thick film in the step (1), and maintaining the pressure for a certain time to obtain a densified thermoelectric thick film;
(3) and (3) annealing and sintering the thermoelectric thick film densified in the step (2) to obtain the high-performance thermoelectric thick film.
3. The method for rapidly manufacturing a high performance thermoelectric thick film according to claim 2, wherein in the step (1), the particle size of the thermoelectric powder is smaller than the thickness of the sheet-shaped thermoelectric thick film.
4. The method for rapidly preparing a high performance thermoelectric thick film according to claim 2, wherein in step (1), the thermoelectric powder is Bi2Te3A base thermoelectric powder.
5. The method of rapidly preparing a high performance thermoelectric thick film of claim 4, wherein said Bi is2Te3The base thermoelectric powder is Bi2Te3Or Bi0.5Sb1.5Te3。
6. The method for rapidly preparing a high performance thermoelectric thick film as claimed in claim 2, wherein in the step (1), the pressure applied during the pressing is 100-400 MPa.
7. The method for rapidly manufacturing a high performance thermoelectric thick film according to claim 2, wherein in step (1), the pre-press mold is a hard material.
8. The method for rapidly preparing a high performance thermoelectric thick film according to claim 2, wherein in the step (2), the pressure of the cold pressing is 400-1200MPa, and the dwell time is 1-10 min.
9. The method for rapidly manufacturing a high performance thermoelectric thick film according to claim 2, wherein in the step (3), the sintering is performed under argon atmosphere of one atmosphere;
the annealing sintering temperature is 300-500 ℃, and the annealing time is 0.5-2 h.
10. A high performance thermoelectric thick film prepared according to the method of any one of claims 1-9.
CN202111345897.8A 2021-11-15 2021-11-15 High-performance thermoelectric thick film and method for rapidly preparing same Pending CN114068798A (en)

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