A thermoelectric interface material and a preparation method thereof, and a thermoelectric device

By preparing thermoelectric interface materials with the chemical composition MgaAgbXc and thermoelectric conversion materials with the chemical composition MgxAgySbz, the problems of rare earth element scarcity and electrode contact fragility in Bi2Te3 thermoelectric devices were solved, and the performance improvement of efficient and reliable thermoelectric devices was achieved.

CN117535575BActive Publication Date: 2026-03-17SOUTHERN UNIVERSITY OF SCIENCE AND TECHNOLOGY
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Filing Date
2023-11-20
Publication Date
2026-03-17

AI Technical Summary

Technical Problem

The widespread application of existing Bi2Te3 thermoelectric devices is limited by the scarcity of the rare earth element Te and the fragility of the electrode contact interface.

Method used

A thermoelectric interface material with the chemical composition MgaAgbXc, where X is a transition metal, is used to prepare thermoelectric devices through ball milling and plasma sintering. Combined with the thermoelectric conversion material MgxAgySbz, a contact interface with high bonding strength and low contact resistivity is formed.

Benefits of technology

It improves the output power and conversion efficiency of thermoelectric devices, has excellent welding and thermal shock resistance stability, and provides a high-performance and low-cost alternative.

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Abstract

The application discloses a thermoelectric interface material and a preparation method thereof, and a thermoelectric device. a Ag b X c , X is a transition metal, a, b, c are atomic ratios, a = 0-2.5; b = 0-1.5; c = 0-1.5, and a, b, c are not zero at the same time. The thermoelectric device comprises the thermoelectric interface material. The thermoelectric interface material has a contact interface with high bonding strength and low contact resistivity of MgAgSb TEcM, and has excellent welding and thermal shock resistance in the phase transition temperature range. The thermoelectric device shows a maximum power density of 0.8 W cm ‑2 and a maximum conversion efficiency of 9.1% at a temperature difference of 325 DEG C, which is a breakthrough value of the full Mg-based Te-free thermoelectric device in the low temperature range. The application provides an ecological, high-performance and low-cost alternative solution to replace the traditional Bi2Te3-based thermoelectric device for low-grade waste heat recovery.
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Description

TECHNICAL FIELD

[0001] The present application relates to the field of inorganic bulk thermoelectric technology, and in particular to a thermoelectric interface material, a preparation method thereof and a thermoelectric device. BACKGROUND

[0002] Thermoelectric materials are a class of functional materials that can directly convert low-quality heat energy into high-quality electric energy (Seebeck effect) or directly generate refrigeration and heating effects (Peltier effect) from electric energy. The materials have the advantages of reliable performance, no noise, no wear and tear, easy miniaturization, and flexible movement. They can be used to prepare thermoelectric devices. At present, Bi2Te3 thermoelectric devices are mature thermoelectric technology products on the market, which have high hot spot figure of merit (ZT), but also have problems such as scarcity of rare earth element Te and fragility of electrode contact interface, which limit their wide application.

[0003] Therefore, the existing thermoelectric device preparation technology still needs to be further improved and promoted. SUMMARY

[0004] In view of the deficiencies of the prior art, the present application provides a thermoelectric interface material, a preparation method thereof and a thermoelectric device, aiming to provide an ecological friendly, high performance and low cost solution to replace traditional Bi2Te3-based thermoelectric devices.

[0005] The technical scheme adopted by the present application to solve the above technical problems is as follows:

[0006] In a first aspect, a thermoelectric interface material is provided, wherein the chemical composition of the thermoelectric interface material is represented as Mg a Ag b X c , X is a transition metal, a, b, c are atomic ratios, a = 0-2.5; b = 0-2.5; c = 0-2.5, a, b, c are not zero at the same time. For example, Mg 0.5 Ag 0.5 X 0.1 , MgAgX 0.1 , Mg 1.5 Ag 2.5 X, Mg 2.5 Ag 2.5 X 0.1 , MgAg, Mg 0.5 X 0.1 , Ag 0.5 X 0.1 , etc.

[0007] The following is a preferred technical scheme of the present application, but is not a limitation on the technical scheme provided by the present application. Through the following preferred technical scheme, the purpose and beneficial effects of the present application can be better achieved and realized.

[0008] As a preferred technical solution, the thermoelectric interface material, wherein the transition metal is selected from any one of manganese, iron, cobalt, nickel, copper, chromium, zinc, vanadium and titanium.

[0009] In a second aspect, a preparation method of the thermoelectric interface material is provided, comprising: weighing each elemental raw material according to the stoichiometric ratio of Mg a Ag b X c , mixing and ball milling to obtain the thermoelectric interface material.

[0010] As a preferred technical solution, the preparation method, wherein the ball milling is carried out under inert gas protection; the inert gas is at least one of nitrogen, helium, neon, argon, krypton and xenon.

[0011] In a third aspect, a thermoelectric device is provided, comprising the thermoelectric interface material.

[0012] As a preferred technical solution, the thermoelectric device, wherein the thermoelectric device further comprises a thermoelectric conversion material compounded on the surface of the thermoelectric interface material; the chemical composition of the thermoelectric conversion material is represented as Mg x Ag y Sb z , wherein x, y and z are atomic ratios, x = 0.5-2.0, y = 0.5-2.0, and z = 0.5-2.0. For example, Mg 0.5 Ag 0.5 Sb 0.5 , MgAgSb, Mg 2.5 Ag 2.5 Sb 2.5 , MgAgSb 0.5 , etc.

[0013] In a fourth aspect, a preparation method of the thermoelectric device is provided, comprising: placing an electrode material, the thermoelectric interface material and the thermoelectric conversion material in a mold, and sintering to obtain the thermoelectric device.

[0014] As a preferred technical solution, the preparation method of the thermoelectric device, wherein the sintering is plasma sintering, which is carried out at 200-500℃ and 30-60MPa axial pressure. The sintering temperature can be 200℃-250℃, 250℃-300℃, 300℃-350℃, 350℃-400℃, 400℃-450℃, 450℃-500℃; the pressure can be 30MPa, 40MPa, 50MPa or 60MPa.

[0015] In a fifth aspect, a wearable device comprising the thermoelectric interface material or the thermoelectric device described above.

[0016] In a sixth aspect, a sensor comprising the thermoelectric interface material or the thermoelectric device described above.

[0017] Beneficial effects: Compared with the prior art, the thermoelectric interface material provided by the application has a high bonding strength and a low contact resistance with the MgAgSb thermoelectric conversion material, effectively improving the output power and conversion efficiency of the thermoelectric device. The microstructure evolution of the contact interface in the phase transition temperature range is observed by in-situ transmission electron microscopy technology, which proves that the contact interface has excellent welding and thermal shock resistance, ensuring the reliability and durability of the thermoelectric device in practical application. BRIEF DESCRIPTION OF DRAWINGS

[0018] Figure 1 Preparation flowchart for the thermoelectric device.

[0019] Figure 2 Performance comparison chart of the thermoelectric device provided by the application and the same type of thermoelectric device in the prior art.

[0020] Figure 3 Comparison chart of shear strength and contact resistance of the thermoelectric device provided by the embodiment of the application and the thermoelectric device provided by the comparative example.

[0021] Figure 4 Comparison chart of maximum conversion efficiency and maximum power density of the thermoelectric device provided by the embodiment of the application and the existing thermoelectric device under different temperature difference conditions. DETAILED DESCRIPTION

[0022] The application provides a thermoelectric interface material and a preparation method thereof, and a thermoelectric device. To make the purpose, technical solutions and effects of the application more clear and explicit, the application is further described in detail below. It should be understood that the specific embodiments described herein are only used to explain the application and do not limit the application.

[0023] In addition, features described in the specification, operations or characteristics can be combined in any appropriate manner to form various embodiments. Meanwhile, the steps or actions in the method description can also be sequentially changed or adjusted in a manner apparent to those skilled in the art. Therefore, the various sequences in the specification and drawings are only for the purpose of clearly describing a certain embodiment, and do not mean that the sequence is necessary. Unless otherwise stated, the sequence of some steps is necessarily followed. The numbers used in this paper for components, such as "first", "second", etc., are only used to distinguish the described objects, and have no order or technical meaning. The instruments and reagents used are commercially available. For example: the particle size of the raw materials used is 100-300 mesh, and the purity is greater than 98%. The raw material composition is as follows: Mn powder, 200 mesh, purity 99.9%, manufacturer Macklin; Mg scrap, purity greater than 99.9%, manufacturer Acros Organics; Cu powder, 200 mesh, purity 99.9%, manufacturer Macklin Sb powder, 200 mesh, purity 99.9%, manufacturer Alfa, Ag powder, 200 mesh, purity 99.5%, manufacturer Alfa.

[0024] The inventor found that the Bi2Te3 thermoelectric device in the mature thermoelectric technology product on the market needs to rely on Te, and the electrode contact interface is weak, which makes the application range narrow, and is not conducive to the popularization and application of thermoelectric devices.

[0025] In order to solve the above problems, the present application provides the following technical scheme, that is, a new type of thermoelectric interface material without Te is designed first, which can be represented by chemical composition Mg a Ag b X c , such as Mg 0.5 Ag 0.5 Mn 0.5 , MgAgMn 0.5 , MgAgMn, MgAgMn 1.5 . The thermoelectric interface material has a high bonding strength and a low contact resistance with MgAgSb, and has excellent welding and thermal shock resistance in the phase transition temperature range.

[0026] Based on the thermoelectric interface material, the present application provides a thermoelectric device, which comprises a thermoelectric conversion material and a thermoelectric interface material and a ceramic copper-clad plate. The thermoelectric interface material (TEiM) is a material connecting the thermoelectric conversion material (TEcM) and the external circuit. The thermoelectric device shows 0.8 W cm -2The maximum power density and maximum conversion efficiency of 9.1% represent breakthrough values ​​for all-Mg-based, Te-free thermoelectric devices in the low-temperature range. This invention provides an eco-friendly, high-performance, and low-cost alternative to traditional Bi2Te3-based thermoelectric devices for low-grade waste heat recovery.

[0027] Based on the same inventive concept, the present invention also provides a method for preparing the above-mentioned thermoelectric device, comprising: placing an electrode material, the thermoelectric interface material and the thermoelectric conversion material in a mold, and subjecting them to sintering treatment to obtain the thermoelectric device.

[0028] The following specific preparation examples will further explain and illustrate the thermoelectric interface material, its preparation method, and the thermoelectric device provided by the present invention.

[0029] Example 1

[0030] Preparation of thermoelectric conversion material (p-type TEcM): MgAg was prepared according to the designed ratio. 0.97 Sb 0.92 Weigh the raw materials and then ball mill them for 10 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0031] Preparation of thermoelectric conversion material (n-type TEcM): Mg was prepared according to the designed ratio. 3.2 Sb 1.5 Bi 0.49 Te 0.01 Ti 0.01 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0032] Preparation of thermoelectric interface material (TEiM): MgAgMn according to the designed ratio 0.5 The raw materials were weighed and then subjected to high-energy ball milling for 10 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0033] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 200℃ for 5 min under an axial pressure of 30 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 50℃ / min. -1 .

[0034] Example 2

[0035] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0036] Preparation of thermoelectric conversion material (n-type TEcM): Mg was prepared according to the designed ratio. 3.2 Sb 1.5 Bi 0.49 Te 0.01 Ti 0.01 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0037] Preparation of thermoelectric interface material (TEiM): Mg was prepared according to the designed ratio. 0.5 Ag 0.5 Mn 0.5 The raw materials were weighed and then subjected to high-energy ball milling for 20 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0038] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 600℃ for 10 min under an axial pressure of 60 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0039] Example 3

[0040] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials were weighed according to the designed ratio of Mg2Ag2Sb2, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0041] Preparation of thermoelectric conversion material (n-type TEcM): Mg was prepared according to the designed ratio. 3.2 Sb 1.5 Bi 0.49 Te 0.01 Ti 0.01 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0042] Preparation of thermoelectric interface material (TEiM): Mg was prepared according to the designed ratio. 2.5 Ag 1.5 Mn 1.5 The raw materials were weighed and then subjected to high-energy ball milling for 20 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0043] Fabrication of thermoelectric devices: Combining Figure 1Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 600℃ for 10 min under an axial pressure of 60 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0044] Example 4

[0045] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0046] Preparation of thermoelectric conversion material (n-type TEcM): Mg3Sb according to the designed ratio 1.5 Bi 0.5 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0047] Preparation of thermoelectric interface material (TEiM): Mg was prepared according to the designed ratio. 2.5 Ag 1.5 Mn 1.5 The raw materials were weighed and then subjected to high-energy ball milling for 20 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0048] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 600℃ for 10 min under an axial pressure of 60 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0049] Example 5

[0050] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0051] Preparation of thermoelectric conversion material (n-type TEcM): Mg3Sb according to the designed ratio 1.5 Bi 0.5 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0052] Preparation of thermoelectric interface material (TEiM): MgAgMn according to the designed ratio 0.1The raw materials were weighed and then subjected to high-energy ball milling for 10 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0053] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 500℃ for 5 min under an axial pressure of 60 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0054] Example 6

[0055] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 12 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0056] Preparation of thermoelectric conversion material (n-type TEcM): Mg3Sb according to the designed ratio 1.5 Bi 0.5 Weigh the raw materials and then ball mill them for 15 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0057] Preparation of thermoelectric interface material (TEiM): According to the designed ratio of MgAg, the raw materials were weighed and obtained by high-energy ball milling for 10 hours under argon protection through mechanical alloying. The powder obtained after ball milling was placed in a glove box for later use.

[0058] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 400℃ for 5 min under an axial pressure of 50 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0059] Example 7

[0060] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0061] Preparation of thermoelectric conversion material (n-type TEcM): Mg3Sb according to the designed ratio 1.5 Bi 0.5 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0062] Preparation of thermoelectric interface material (TEiM): MgMn according to the designed ratio 0.5 The raw materials were weighed and then subjected to high-energy ball milling for 10 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0063] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 500℃ for 5 min under an axial pressure of 40 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0064] Example 8

[0065] Preparation of thermoelectric conversion material (p-type TEcM): The raw materials MgAgSb were weighed according to the design ratio, and then ball-milled for 10 hours under argon protection. The powder obtained after ball milling was placed in a glove box for later use.

[0066] Preparation of thermoelectric conversion material (n-type TEcM): Mg3Sb according to the designed ratio 1.5 Bi 0.5 Weigh the raw materials and then ball mill them for 18 hours under argon protection. The powder obtained after ball milling is placed in a glove box for later use.

[0067] Preparation of thermoelectric interface material (TEiM): Ag according to the designed ratio 0.1 Mn 0.1 The raw materials were weighed and then subjected to high-energy ball milling for 10 hours under argon protection using a mechanical alloying method to obtain alloy powder. The powder obtained after ball milling was placed in a glove box for later use.

[0068] Fabrication of thermoelectric devices: Combining Figure 1 Electrode material powder, TEiM powder, and TEcM powder were sintered by spark plasma at 500℃ for 5 min under an axial pressure of 60 MPa. Thermoelectric devices were then fabricated using wire cutting and welding processes. The heating rate during sintering was 100℃ / min. -1 .

[0069] Comparative Example 1

[0070] Thermoelectric conversion material TEcM: Commercial pn Bi2Te3 (bulk units purchased from Guangdong Fuxin Technology Co.),

[0071] Thermoelectric interface material TEiM: Ni (the company provides its own electroplated Ni electrode). The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM are loaded into a mold and sintered to prepare the Bi2Te3 thermoelectric device. The sintering conditions for this part are 500℃, 5min, 50MPa.

[0072] Comparative Example 2

[0073] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0074] Thermoelectric interface material TEiM:Mg

[0075] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0076] Comparative Example 3

[0077] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0078] Thermoelectric interface material TEiM:Ag

[0079] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0080] Comparative Example 4

[0081] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0082] Thermoelectric interface material TEiM: Ni

[0083] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0084] Comparative Example 5

[0085] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0086] Thermoelectric interface material TEiM: Al

[0087] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0088] Comparative Example 6

[0089] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0090] Thermoelectric interface material TEiM: Zn

[0091] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0092] Comparative Example 7

[0093] Thermoelectric conversion material TEcM:MgAg 0.97 Sb 0.92 Powder was obtained by high-energy ball milling for 8 hours under argon protection;

[0094] Thermoelectric interface material TEiM: Cu

[0095] Fabrication of the thermoelectric device: The thermoelectric conversion material TEcM and the thermoelectric interface material TEiM were loaded into a mold and sintered to prepare a tellurium-free (Te) thermoelectric device. The sintering conditions for this part were 300℃, 20min, and 50MPa.

[0096] Depend on Figure 2 It can be seen that the thermoelectric device provided by the present invention has better performance in terms of maximum conversion efficiency and maximum power density.

[0097] Depend on Figure 3 It can be seen that the thermoelectric device provided by this invention has the highest shear strength of 35.0 MPa and the lowest contact resistivity of 4.5 μΩcm. 2 .

[0098] Depend on Figure 4 It can be seen that the Te-free thermoelectric device based on MgAgSb / Mg3Sb2 proposed in this invention exhibits a power of 0.8 W / cm² at a temperature difference of 325°C. -2The maximum power density and maximum conversion efficiency of 9.1% represent a breakthrough for all-Mg-based Te-free thermoelectric devices in the low-temperature range (previous Te-free thermoelectric devices had efficiencies of less than 9.0% at a temperature difference of 300°C, and commercial Bi2Te3-based thermoelectric devices had efficiencies of less than 6.0% at a temperature difference of 300°C).

[0099] In summary, this invention provides a thermoelectric interface material, its preparation method, and a thermoelectric device. The chemical composition of the thermoelectric interface material is represented as Mg. a Ag b X c X is a transition metal, a, b, and c are atomic ratios, where a = 0-2.5, b = 0-1.5, and c = 0-1.5, and a, b, and c are not simultaneously zero. The thermoelectric device includes this thermoelectric interface material. The thermoelectric interface material has a high bonding strength and low contact resistivity with MgAgSbTEcM, and exhibits excellent welding and thermal shock resistance stability within the phase transition temperature range. The thermoelectric device shows a thermal conductivity of 0.8 W / cm² at a temperature difference of 325°C. -2 The maximum power density and maximum conversion efficiency of 9.1% represent breakthrough values ​​for all-Mg-based, Te-free thermoelectric devices in the low-temperature range. This invention provides an eco-friendly, high-performance, and low-cost alternative to traditional Bi2Te3-based thermoelectric devices for low-grade waste heat recovery.

[0100] It should be understood that the application of the present invention is not limited to the examples above. Those skilled in the art can make improvements or modifications based on the above description, and all such improvements and modifications should fall within the protection scope of the appended claims.

Claims

1. A thermoelectric interface material, characterized by, The chemical composition of the thermoelectric interface material is represented as Mg a Ag b X c , X is a transition metal, a, b, c are atomic ratios, and the transition metal is manganese; wherein, when being a ternary material, a = 1-2.5; b = 0.5-1.5; c = 1-1.5; when being a binary material, a = 0; b = 0.5-1.5; c = 0.1-1.5; when being a binary material, a = 0.5-2.5; b = 0; c = 0.1-1.5; when being a binary material, a = 1-2.5; b = 1-1.5; c = 0.

2. A method of producing the thermoelectric interface material according to claim 1, characterized by, comprising: Mg a Ag b X c The raw materials are weighed according to the stoichiometric ratio of the chemical composition Mg a Ag b X c , mixed, and ball milled to obtain the thermoelectric interface material.

3. The preparation method according to claim 2, characterized in that, the ball milling is carried out under protection of inert gas; the inert gas is at least one selected from nitrogen, helium, neon, argon, krypton and xenon.

4. A thermoelectric device, characterized by, The thermoelectric interface material of claim 1.

5. The thermoelectric device of claim 4, wherein, The thermoelectric device further comprises a thermoelectric conversion material complexed on the surface of the thermoelectric interface material; the chemical composition of the thermoelectric conversion material is represented as Mg x Ag y Sb z , wherein; x, y, z are atomic ratios, x = 0.5-2.0; y = 0.5-2.0; z = 0.5-2.

0.

6. A method of producing a thermoelectric device as claimed in claim 4 or 5, characterized in that comprising: placing the electrode material, the thermoelectric interface material and the thermoelectric conversion material into a mold, and subjecting to a sintering treatment to obtain the thermoelectric device.

7. The method of producing a thermoelectric device according to claim 6, wherein The sintering is plasma sintering, which is carried out at 200-500℃ under axial pressure of 30-60MPa.

8. A wearable device, comprising: The thermoelectric interface material of claim 1, or the thermoelectric device of claim 4 or 5.

9. A sensor, characterized by The thermoelectric interface material of claim 1, or the thermoelectric device of claim 4 or 5.

Citation Information

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