A method for preparing a flexible special-shaped thick-film thermoelectric device

Abstract

The present invention discloses a method for preparing a flexible, special-shaped thick-film thermoelectric device. By changing the flexibility and special shape of the thermoelectric arms inside a semiconductor thermoelectric generator (TEG), the excellent mechanical properties of thermoelectric materials such as silver selenide can be utilized, while raw materials can be saved and the thermoelectric conversion performance can be improved, thereby increasing the output power of the device. A flexible, special-shaped thick-film device with high output power is obtained through a hot pressing welding process, thereby solving the problems of high thermal conductivity and high production cost of thermoelectric generators using rectangular thermoelectric arms in the prior art, low output power of thin-film flexible thermoelectric power generation devices, and difficulty in applying rigid devices to wearable devices.

Description

Technical field:

[0001] The present invention relates to the technical field of room-temperature semiconductor temperature difference power generation, and in particular to a flexible special-shaped thick-film thermoelectric device and a preparation method thereof. Background technology:

[0002] With the rapid development of global society, the efficient use of environmental heat continues to attract the attention of scientific researchers. Furthermore, wearable devices, a hot topic for future development and application, face challenges in achieving efficient, stable, and uninterrupted operation. Thermoelectric devices, as a new type of energy conversion material with compact size, quiet operation, and pollution-free properties, hold great promise as power sources for wearable electronic devices. Semiconductor thermoelectric generators (TEGs) utilize their internal semiconductor thermoelectric arms to convert thermal energy into electrical energy, using human body heat as a heat source to power wearable devices.

[0003] Currently, thermoelectric devices are mainly divided into two categories. One is the bulk rigid type, which often has a higher output power, such as Bi2Te3, PbTe, SiGe, etc. Although rigid thermoelectric devices have the advantages of high integration, mature processing technology and high open-circuit voltage, their poor mechanical properties make them unable to adapt to non-planar heat sources such as human skin and cannot be used in wearable electronic devices. The other type is the thin-film flexible type, which uses methods such as electroplating or thermal evaporation to coat thermoelectric materials on a flexible substrate. However, since most thin films have poor thermal insulation and the substrate has poor electrical conductivity, their output power is much lower than that of bulk rigid devices. There is an urgent need to improve the output power of thin-film flexible thermoelectric devices. Summary of the invention:

[0004] The purpose of the present invention is to provide a method for preparing a flexible, special-shaped thick-film thermoelectric device. By changing the flexibility and special shape of the thermoelectric arms inside a semiconductor thermoelectric power generation device (TEG), on the one hand, the excellent mechanical properties of thermoelectric materials such as silver selenide can be utilized, and on the other hand, raw materials can be saved and the thermoelectric conversion performance can be improved, thereby increasing the output power of the device. A flexible, special-shaped thick-film device with high output power is obtained through a hot pressing welding process, thereby solving the problems of the prior art of thermoelectric generators using rectangular thermoelectric arms having high thermal conductivity, high production cost, low output power of thin-film flexible thermoelectric power generation devices, and difficulty in applying rigid devices to wearable devices.

[0005] The present invention is achieved through the following technical solutions:

[0006] A method for preparing a flexible special-shaped thick-film thermoelectric device, the method comprising the following steps:

[0007] (1) preparing silver selenide n-type thermoelectric materials and silver copper telluride p-type thermoelectric materials;

[0008] (2) plasma discharge sintering the silver selenide n-type thermoelectric material and the silver copper tellurium p-type thermoelectric material obtained in step (1) to obtain high-performance n-type silver selenide and p-type silver copper tellurium polycrystalline bulk thermoelectric materials;

[0009] (3) processing the n-type silver selenide and p-type silver copper telluride polycrystalline bulk thermoelectric materials obtained in step (2) into flexible X-shaped, trapezoidal or I-shaped thick-film thermoelectric arms by shape processing and hot pressing;

[0010] (4) Apply solder paste with a thickness of 1 to 2 mm and a width of 1 to 2 mm to the upper and lower ends of the thermoelectric arm obtained in step (3); arrange the n-type silver selenide and p-type silver copper telluride thermoelectric arms in parallel with a spacing of 7 to 9 mm, and adhere them to the electrode coating with copper foil, place them on a hot press and perform hot pressing welding to obtain a special-shaped flexible thick-film thermoelectric device.

[0011] The preparation method specifically comprises the following steps:

[0012] (1) Preparation of silver selenide n-type thermoelectric material and silver copper tellurium p-type thermoelectric material: Ag powder and Se powder are added to a ball mill, and reacted at a speed of 500-600 r / min for 10-20 h to obtain silver selenide n-type thermoelectric material; Ag powder, Cu powder and Te powder are added to a ball mill, and reacted at a speed of 300-600 r / min for 5-20 h to obtain silver copper tellurium p-type thermoelectric material. The molar ratio of Ag to Se powder is n Ag :n Se =1.96:1~2:1, the molar ratio of Ag, Cu and Te powder is n Ag :n Cu :n Te =:0.95:1.05:1~1:1:1;

[0013] (2) plasma discharge sintering the silver selenide n-type thermoelectric material and the silver copper tellurium p-type thermoelectric material obtained in step (1) to obtain high-performance n-type silver selenide and p-type silver copper tellurium polycrystalline bulk thermoelectric materials, respectively, at a sintering temperature of 300-450° C., a pressure of 30-50 MPa, and a holding time of 5 min;

[0014] (3) Cutting the n-type silver selenide and p-type silver copper tellurium polycrystalline bulk thermoelectric materials obtained in step (2) to obtain thick film materials with a thickness of 0.3±0.05 mm and hot pressing them at a hot pressing temperature of 200-300° C. and a pressure of 30 MPa; then shaping the thick film into X-shaped, trapezoidal or I-shaped thermoelectric arms: wherein the processing dimensions are: X-shaped, the thermoelectric arm height is 8-12 mm, the upper and lower widths are 6-10 mm, the center width is 4-5 mm, and the thickness is 0.3 mm±0.05; trapezoidal, the thermoelectric arm height is 8-12 mm, the upper and lower bottom widths are 6-12 mm, and the thickness is 0.3 mm±0.05; I-shaped, the thermoelectric arm height is 8-12 mm, the upper and lower bottom widths are 8-12 mm, the center width is 2-6 mm, and the thickness is 0.3 mm±0.05;

[0015] (4) applying solder paste with a thickness of 1 to 2 mm and a width of 1 to 2 mm to the upper and lower ends of the thermoelectric arm obtained in step (3); arranging the n-type silver selenide and p-type silver copper telluride thermoelectric arms in parallel with a spacing of 7 to 9 mm, and laminating them with copper foil at the electrode coating, placing them on a hot press for hot pressing welding to obtain a special-shaped flexible thick-film thermoelectric device, wherein the copper foil has a thickness of 0.03 to 0.06 mm and a width of 1 to 2 mm, and the hot pressing welding temperature is 200 to 270° C., the pressure is 30 to 50 MPa, and the time is 10 to 30 seconds.

[0016] Preferably, the temperature of the hot pressing treatment is 240-270°C.

[0017] Preferably, the thermoelectric arm is in an X-shape, with a height of 9 to 11 mm, a top and bottom width of 7 to 9 mm, and a center width of 4 to 4.5 mm.

[0018] Preferably, the shape of the thermoelectric arm is trapezoidal, with a height of 9 to 11 mm and a width of the upper and lower bases of 7 to 11 mm.

[0019] Preferably, the thermoelectric arm is in an I-shape, with a height of 9 to 11 mm, upper and lower bottom widths of 9 to 11 mm, and a center width of 3 to 5 mm.

[0020] Preferably, the temperature of the hot pressing welding is 220-250° C., the pressure is 35-45 MPa, and the time is 15-25 seconds.

[0021] Preferably, the ball-to-material ratio in the ball mill is 10:1, and the rotation speed is 550-600 r / min.

[0022] The beneficial effects of the present invention are as follows:

[0023] (1) The present invention has low cost, complete preparation method and simple processing method.

[0024] (2) The PN junction formed by the special-shaped P-type and N-type connections can effectively reduce heat loss during energy transmission, thereby increasing the temperature difference between the hot and cold ends of the device and improving the output voltage of the device. The results show that under an ambient temperature of 23°C, the output power of the thermoelectric generator with special-shaped thermoelectric arms in actual testing can reach up to 1.2359μW, which is 30% to 60% higher than that of devices with rectangular thermoelectric arms of the same size. In addition, the thermoelectric arms are all processed by simple cutting, which is low-cost, convenient and fast, and has the potential for industrial mass production. This solves the problems of the existing thermoelectric generators using rectangular thermoelectric arms, such as high thermal conductivity, high production cost, low power density, and difficulty in applying rigid devices to wearable devices. Description of the drawings:

[0025] Figure 1 This is a structural design diagram of the thermoelectric arm in a flexible special-shaped thick-film thermoelectric device;

[0026] Figure 2 This is a physical picture of a flexible, special-shaped thick-film thermoelectric device. Specific implementation method:

[0027] The following is a further description of the present invention, but not a limitation of the present invention.

[0028] Example 1:

[0029] (1) Ag powder (7.281 g) and Se powder (2.729 g) were added to a ball mill jar, followed by the addition of 100 g of ball milling balls. The jar was then covered and the screws tightened. The entire process was performed in a glove box. The ball mill jar was then removed from the glove box and placed in a ball mill, where it was reacted at 550 r / min for 10 h.

[0030] Ag powder (3.453 g), Cu powder (2.248 g), and Te powder (4.299 g) were added to a ball mill jar, followed by 100 g of ball milling balls. The jar was then covered and the screws tightened. This entire process was performed in a glove box. The jar was then removed from the glove box and placed in a ball mill, where it was reacted at 600 rpm for 10 hours.

[0031] (2) Taking out the powder after the reaction in step (1) and performing spark plasma sintering treatment respectively:

[0032] N-type silver selenide powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 300°C and 30 MPa. P-type silver copper telluride powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 450°C and 30 MPa into cylinders with a diameter of 15 mm and a height of 3 mm. After natural cooling, the resulting n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials were obtained.

[0033] (3) The n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials obtained in step (2) are cut and processed to obtain a thick film with a thickness of 0.3±0.05 mm, which is then hot-pressed at 200°C and 30 MPa. The thick film is then processed into an I-shaped thermoelectric arm with a thickness of 0.3±0.05 mm, a height of 10 mm, an upper and lower bottom width of 10 mm, and a center width of 4 mm. The processing accuracy of height and width is ±0.5 mm.

[0034] (4) Prepare two pieces of copper foil with a width of 2mm, a length of 8mm and a thickness of 0.06mm, and apply 2mm wide and 2mm thick solder paste on the upper and lower ends of the processed thermoelectric arm. 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) are placed in parallel with a spacing of 8mm. The upper and lower copper foils are placed on the solder paste to make n-type silver selenide (Ag 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) bonded together. The device was then placed in a hot press for hot pressing at 270°C, 30 MPa, and 20 seconds to create a connected, custom-shaped flexible thick-film thermoelectric device. Actual testing showed that the output power of the custom-shaped thick-film device reached a maximum of 0.5 μW, a 30% increase compared to a rectangular device of the same size.

[0035] Example 2

[0036] (1) Ag powder (7.281 g) and Se powder (2.729 g) were added to a ball mill jar, followed by the addition of 100 g of ball milling balls. The jar was then covered and the screws tightened. The entire process was performed in a glove box. The ball mill jar was then removed from the glove box and placed in a ball mill, where it was reacted at 550 r / min for 10 h.

[0037] Ag powder (3.453 g), Cu powder (2.248 g), and Te powder (4.299 g) were added to a ball mill jar, followed by the addition of ball milling balls (100 g). The jar was then covered with a lid and tightened with screws. The entire process was carried out in a glove box. The jar was then removed from the glove box and placed in a ball mill, where it was reacted at 600 r / min for 10 h.

[0038] (2) Taking out the powder after the reaction in step (1) and performing spark plasma sintering treatment respectively:

[0039] N-type silver selenide powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 300°C and 30 MPa. P-type silver copper telluride powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 450°C and 30 MPa into cylinders with a diameter of 15 mm and a height of 3 mm. After natural cooling, the resulting n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials were obtained.

[0040] (3) The n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials obtained in step (2) are cut and processed into a thick film with a thickness of 0.3±0.05 mm, and then hot-pressed at 200°C and 30 MPa. The thick film is then processed into a trapezoidal thermoelectric arm with a height of 10 mm, an upper base width of 8 mm, and a lower base width of 12 mm. The processing accuracy of height and width is ±0.5 mm.

[0041] (4) Prepare two pieces of copper foil with a width of 2mm, a length of 8mm and a thickness of 0.06mm, and apply 2mm wide and 2mm thick solder paste on the upper and lower ends of the processed thermoelectric arm. 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) are placed in parallel with a spacing of 8mm. The upper and lower copper foils are placed on the solder paste to make n-type silver selenide (Ag 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) bonded together. The device was then placed in a hot press for hot pressing at 270°C, 30 MPa, and 20 seconds to create a connected, custom-shaped flexible thick-film thermoelectric device. Actual testing showed that the output power of the custom-shaped thick-film device reached a maximum of 0.8 μW, a 40% increase compared to a rectangular device of the same size.

[0042] Example 3

[0043] (1) Ag powder (7.281 g) and Se powder (2.729 g) were added to a ball mill jar, followed by the addition of 100 g of ball milling balls. The jar was then covered and the screws tightened. The entire process was performed in a glove box. The ball mill jar was then removed from the glove box and placed in a ball mill, where it was reacted at 550 r / min for 10 h.

[0044] Ag powder (3.453 g), Cu powder (2.248 g), and Te powder (4.299 g) were added to a ball mill jar, followed by 100 g of ball milling balls. The jar was then covered and the screws tightened. This entire process was performed in a glove box. The jar was then removed from the glove box and placed in a ball mill, where it was reacted at 600 rpm for 10 hours.

[0045] (2) Taking out the powder after the reaction in step (1) and performing spark plasma sintering treatment respectively:

[0046] N-type silver selenide powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 300°C and 30 MPa. P-type silver copper telluride powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 450°C and 30 MPa into cylinders with a diameter of 15 mm and a height of 3 mm. After natural cooling, the resulting n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials were obtained.

[0047] (3) The n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials obtained in step (2) are cut and processed into a thick film with a thickness of 0.3±0.05 mm, and then hot-pressed at 240°C and 30 MPa. The thick film is then processed into an X-shaped thermoelectric arm with a height of 10 mm, a top and bottom width of 8 mm, and a center width of 4 mm. The processing accuracy of height and width is ±0.5 mm.

[0048] (4) Prepare two pieces of copper foil with a width of 2mm, a length of 8mm and a thickness of 0.06mm, and apply 2mm wide and 2mm thick solder paste on the processed thermoelectric arms. 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) are placed in parallel with a spacing of 8mm. The upper and lower copper foils are placed on the solder paste to make n-type silver selenide (Ag 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) bonded together. The device was then placed in a hot press for hot pressing at 250°C, 30 MPa, and 20 seconds to create a connected, custom-shaped flexible thick-film thermoelectric device. Actual testing showed that the output power of the custom-shaped thick-film device reached a maximum of 1.2 μW, a 60% increase compared to a rectangular device of the same size.

[0049] Example 4

[0050] (1) Ag powder (7.281 g) and Se powder (2.729 g) were added to a ball mill jar, followed by the addition of 100 g of ball milling balls. The jar was then covered and the screws tightened. The entire process was performed in a glove box. The ball mill jar was then removed from the glove box and placed in a ball mill, where it was reacted at 550 r / min for 10 h.

[0051] Ag powder (3.453 g), Cu powder (2.248 g), and Te powder (4.299 g) were added to a ball mill jar, followed by 100 g of ball milling balls. The jar was then covered and the screws tightened. This entire process was performed in a glove box. The jar was then removed from the glove box and placed in a ball mill, where it was reacted at 600 rpm for 10 hours.

[0052] (2) Taking out the powder after the reaction in step (1) and performing spark plasma sintering treatment respectively:

[0053] N-type silver selenide powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 300°C and 30 MPa. P-type silver copper telluride powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 450°C and 30 MPa into cylinders with a diameter of 15 mm and a height of 3 mm. After natural cooling, the resulting n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials were obtained.

[0054] (3) The n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials obtained in step (2) are cut and processed into a thick film with a thickness of 0.3±0.05 mm, and then hot-pressed at 200°C and 30 MPa. The thick film is then processed into an X-shaped thermoelectric arm with a height of 10 mm, a top and bottom width of 8 mm, and a center width of 4 mm. The processing accuracy of height and width is ±0.5 mm.

[0055] (4) Prepare two pieces of copper foil with a width of 2mm, a length of 8mm and a thickness of 0.06mm, and apply 2mm wide and 2mm thick solder paste on the processed thermoelectric arms. 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) are placed in parallel with a spacing of 8mm. The upper and lower copper foils are placed on the solder paste to make n-type silver selenide (Ag 1.96 Se) and p-type silver copper telluride (Ag 0.95 Cu 1.05 Te) bonded together. The device was then placed in a hot press for hot pressing at 250°C, 30 MPa, and 20 seconds to create a connected, custom-shaped flexible thick-film thermoelectric device. Actual testing showed that the output power of the custom-shaped thick-film device reached up to 1 μW, a 50% increase compared to a rectangular device of the same size.

[0056] Example 5

[0057] (1) Ag powder (7.321 g) and Se powder (2.689 g) were added to a ball mill jar, followed by the addition of 100 g of ball milling balls. The jar was then covered and the screws tightened. The entire process was performed in a glove box. The ball mill jar was then removed from the glove box and placed in a ball mill, where it was reacted at 550 r / min for 10 h.

[0058] Ag powder (3.607 g), Cu powder (1.222 g), and Te powder (5.171 g) were added to a ball mill jar, followed by 100 g of ball milling balls. The jar was then covered and the screws tightened. This entire process was performed in a glove box. The jar was then removed from the glove box and placed in a ball mill, where it was reacted at 600 rpm for 10 hours.

[0059] (2) Taking out the powder after the reaction in step (1) and performing spark plasma sintering treatment respectively:

[0060] N-type silver selenide powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 300°C and 30 MPa. P-type silver copper telluride powder was added to a graphite mold and sintered in a spark plasma sintering (SPS) furnace at 450°C and 30 MPa into cylinders with a diameter of 15 mm and a height of 3 mm. After natural cooling, the resulting n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials were obtained.

[0061] (3) The n-type silver selenide and p-type silver copper telluride polycrystalline bulk materials obtained in step (2) are cut and processed into a thick film with a thickness of 0.3±0.05 mm, and then hot-pressed at 300°C and 30 MPa. The thick film is then processed into an X-shaped thermoelectric arm with a height of 10 mm, a top and bottom width of 8 mm, and a center width of 4 mm. The processing accuracy of height and width is ±0.5 mm.

[0062] (4) Prepare two pieces of copper foil with a width of 2mm, a length of 8mm and a thickness of 0.06mm, and apply a 2mm wide and 2mm thick solder paste on the processed thermoelectric arm. Arrange n-type silver selenide (Ag2Se) and p-type silver copper telluride (AgCuTe) in parallel with an interval of 8mm. Place the upper and lower copper foils on the solder paste to bond n-type silver selenide (Ag2Se) and p-type silver copper telluride (AgCuTe) together. Then place the device on a hot press for hot pressing welding at a temperature of 270℃, a pressure of 30Mpa, and a time of 20s to obtain a connected special-shaped flexible thick film thermoelectric device. In actual testing, the output power of the flexible special-shaped thick film device can reach up to 0.75μW, which is 35% higher than that of the rectangular device of the same size.

Claims

1. A method for preparing a flexible special-shaped thick-film thermoelectric device, characterized in that: The method comprises the following steps: (1) Preparation of silver selenide n-type thermoelectric material and silver copper tellurium p-type thermoelectric material: Ag powder and Se powder were added to a ball mill, and reacted at a speed of 500-600 r / min for 10-20 h to obtain silver selenide n-type thermoelectric material; Ag powder, Cu powder and Te powder were added to a ball mill, and reacted at a speed of 300-600 r / min for 5-20 h to obtain silver copper tellurium p-type thermoelectric material, wherein the molar ratio of Ag to Se powder was nAg:nSe=1.96:1-2:1, and the molar ratio of Ag, Cu and Te powder was nAg:nCu: nTe=0.95:1.05:1~1:1:1; (2) plasma discharge sintering the silver selenide n-type thermoelectric material and the silver copper tellurium p-type thermoelectric material obtained in step (1) to obtain high-performance n-type silver selenide and p-type silver copper tellurium polycrystalline bulk thermoelectric materials; (3) processing the n-type silver selenide and p-type silver copper telluride polycrystalline bulk thermoelectric materials obtained in step (2) into flexible X-shaped, trapezoidal or I-shaped thick-film thermoelectric arms by shape processing and hot pressing; (4) Apply solder paste with a thickness of 1 to 2 mm and a width of 1 to 2 mm to the upper and lower ends of the thermoelectric arm obtained in step (3); The n-type silver selenide and p-type silver copper telluride thermoelectric arms are arranged in parallel with a spacing of 7-9 mm, and copper foil is used to adhere to the electrode coating. They are placed on a hot press and hot-pressed to obtain a special-shaped flexible thick-film thermoelectric device.

2. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1, characterized in that: The preparation method specifically comprises the following steps: (1) Preparation of silver selenide n-type thermoelectric material and silver copper tellurium p-type thermoelectric material: Ag powder and Se powder were added to a ball mill, and reacted at a speed of 500-600 r / min for 10-20 h to obtain silver selenide n-type thermoelectric material; Ag powder, Cu powder and Te powder were added to a ball mill, and reacted at a speed of 300-600 r / min for 5-20 h to obtain silver copper tellurium p-type thermoelectric material, wherein the molar ratio of Ag to Se powder was nAg:nSe=1.96:1-2:1, and the molar ratio of Ag, Cu and Te powder was nAg:nCu: nTe=0.95:1.05:1~1:1:1; (2) plasma discharge sintering the silver selenide n-type silver selenide and silver copper telluride p-type thermoelectric materials obtained in step (1) to obtain high-performance n-type silver selenide and p-type silver copper telluride polycrystalline bulk thermoelectric materials, respectively, at a sintering temperature of 300-450° C., a pressure of 30-50 MPa, and a holding time of 5 min; (3) The n-type silver selenide and p-type silver copper tellurium polycrystalline bulk thermoelectric materials obtained in step (2) are cut to obtain thick film materials with a thickness of 0.3±0.05 mm and hot-pressed at a temperature of 200-300° C. and a pressure of 30Mpa; then the thick film is shaped and processed into X-shaped, trapezoidal or I-shaped thermoelectric arms: the processing dimensions are: X-shaped, thermoelectric arm height is 8-12mm, upper and lower width is 6-10mm, center width is 4-5mm, thickness is 0.3mm±0.05; trapezoidal, thermoelectric arm height is 8-12mm, upper and lower bottom width is 6-12mm, thickness is 0.3mm±0.05; I-shaped, thermoelectric arm height is 8-12mm, upper and lower bottom width is 8-12mm, center width is 2-6mm, thickness is 0.3mm±0.05; (4) applying solder paste with a thickness of 1 to 2 mm and a width of 1 to 2 mm to the upper and lower ends of the thermoelectric arm obtained in step (3); arranging the n-type silver selenide and p-type silver copper telluride thermoelectric arms in parallel with a spacing of 7 to 9 mm, and laminating them with copper foil at the electrode coating, placing them on a hot press for hot pressing welding to obtain a special-shaped flexible thick film thermoelectric device, wherein the copper foil has a thickness of 0.03 to 0.06 mm and a width of 1 to 2 mm, the hot pressing welding temperature is 200 to 270° C., and the pressure is 30 to 50 Mpa, time is 10 to 30s.

3. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1 or 2, characterized in that: The temperature of the hot pressing treatment in step (3) is 240-270°C.

4. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1 or 2, characterized in that: The shape of the thermoelectric arm is X-shaped, with a height of 9 to 11 mm, a width of 7 to 9 mm at the top and bottom, and a center width of 4 to 4.5 mm.

5. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1 or 2, characterized in that: The shape of the thermoelectric arm is trapezoidal, with a height of 9 to 11 mm and a width of 7 to 11 mm at the upper and lower bases.

6. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1 or 2, characterized in that: The thermoelectric arm is in an I-shape, with a height of 9 to 11 mm, upper and lower bottom widths of 9 to 11 mm, and a center width of 3 to 5 mm.

7. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 1 or 2, characterized in that: The temperature of the hot pressing welding in step (4) is 220-250° C., the pressure is 35-45 MPa, and the time is 15-25 seconds.

8. The method for preparing a flexible special-shaped thick-film thermoelectric device according to claim 2, characterized in that: The ball-to-material ratio in the ball mill is 10:1, and the rotation speed is 550-600 r / min.

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