KR20170056853A - Flexible thermoeletric element and the manufacturing method of it - Google Patents

Flexible thermoeletric element and the manufacturing method of it Download PDF

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KR20170056853A
KR20170056853A KR1020150160186A KR20150160186A KR20170056853A KR 20170056853 A KR20170056853 A KR 20170056853A KR 1020150160186 A KR1020150160186 A KR 1020150160186A KR 20150160186 A KR20150160186 A KR 20150160186A KR 20170056853 A KR20170056853 A KR 20170056853A
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South Korea
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thermoelectric material
thermoelectric
type thermoelectric
type
insulating polymer
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KR1020150160186A
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Korean (ko)
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고종수
정경국
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부산대학교 산학협력단
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Publication of KR20170056853A publication Critical patent/KR20170056853A/en

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Abstract

The present invention relates to a flexible thermoelectric device and a method of manufacturing the same, and more particularly, to a flexible thermoelectric device capable of flexing not only a base material substrate but also all thermoelectric materials, and a method of manufacturing the same.
A flexible thermoelectric device according to the present invention comprises a base substrate, a thermoelectric material including a p-type thermoelectric material and an n-type thermoelectric material, and an electrode for connecting the n-type thermoelectric material and the p-type thermoelectric material. Here, the base substrate is formed with a flexible insulating polymer material. The p-type thermoelectric material and the n-type thermoelectric material may be carbon nanotubes (CNT), graphene, or nano / micro conductive particles on the surface of a thermoelectric material such as bismuth telluride (BiTe) or lead telluride A combined thermoelectric material powder is formed by incorporation into the flexible insulating polymer material.
According to the present invention, since the thermoelectric material and the base substrate can be bent flexibly, the whole area of the thermoelectric element can be bent equally when the thermoelectric element is bent. Thus, the bending can be prevented from being concentrated at a specific point of the thermoelectric element.

Description

TECHNICAL FIELD [0001] The present invention relates to a flexible thermoelectric element and a manufacturing method thereof,

The present invention relates to a flexible thermoelectric device and a method of manufacturing the same, and more particularly, to a flexible thermoelectric device capable of flexing not only a base material substrate but also all thermoelectric materials, and a method of manufacturing the same.

In recent years, interest and demand for smart watches such as Fibit, Apple watch and Gear S2 have increased significantly. However, smart watches can measure various information related to the human body such as real time heart rate, calorie consumption measurement, walking posture, sleep pattern only when worn by the user. All current smart watches are operated by battery When charging, the function will not be performed.

Therefore, each manufacturer has chosen to minimize the charging cycle by minimizing the consumption power of the smart clock and increasing the performance of the battery, but it is difficult to use it continuously. For this reason, the need for a battery that can be continuously used without charging is emphasized. To solve this problem, researches on thermoelectric elements capable of continuously generating electricity using heat generated in the human body are being conducted in various ways.

As shown in Fig. 1, the thermoelectric element connects the thermoelectric material 1 made of the p-type thermoelectric material 1a and the n-type thermoelectric material 1b with the p-type thermoelectric material 1a and the n-type thermoelectric material 1b (3). Of course, the thermoelectric material 1 is formed on a base material substrate (not shown). Since the p-type thermoelectric material 1a has many holes at a higher temperature, the holes move from a higher temperature to a lower temperature due to the difference in density between the lower temperature and the lower one. The n-type thermoelectric material 1b Since a lot of electrons are generated at a higher temperature side, electrons move from a higher temperature to a lower temperature due to the difference in density between the lower temperature side and the lower one. Thus, a thermoelectric device is a device that generates electricity using the temperature difference between both ends, and has a higher power generation efficiency as the heat loss when heat is transferred from the heat source to the thermoelectric device is smaller. Therefore, when manufacturing a thermoelectric device applicable to a human body, consideration should be given to the curvature of the human body and suitability for movement. Since all portions of the human body have curvature and the muscles of all parts move according to the movement, the thermoelectric elements using the conventional ceramic substrate as the substrate are not flexible because the contact surfaces are not so close to the human body. In order to solve such a problem, studies have been actively made on a flexible thermoelectric element which can be operated in close contact with a human body.

The method of making a flexible thermoelectric element is classified into a method using a mineral material as a thermoelectric element and a method using a flexible polymer material. Both of these methods use a flexible material as the base substrate.

When a flexible material is used as an inorganic material or a base material substrate as a thermoelectric material, bending is concentrated on the base material substrate because the thermoelectric material is a rigid material when bending the thermoelectric device. As a result, intensive bending occurs in the electrode formed on the surface of the base material substrate, so that the bending degree is limited.

When a flexible polymer material and a base material substrate are used as a flexible material by a thermoelectric material, the entire area is bent when the thermoelectric device is bent, so that the bending property is better than when using an inorganic material. However, There is a drawback that the resistance is large.

A common limitation of the above two methods is that the adhesion between the different materials is not good because the materials of the thermoelectric material and the substrate are different. As a result, there is a possibility that the thermoelectric element material and the substrate substrate are separated during use, which means that the thermoelectric element can not achieve the desired performance.

Registration No. 10-1249292 (Registration date March 26, 2013) Published Patent No. 10-2010-0119184 (Published date June 5, 2012)

The present invention is intended to solve the above problems. An object of the present invention is to provide a flexible thermoelectric element which can be bent flexibly both on a thermoelectric material and a base substrate and can be prevented from being separated during use, and a method for manufacturing the same.

A flexible thermoelectric device according to the present invention comprises a base substrate, a thermoelectric material including a p-type thermoelectric material and an n-type thermoelectric material, and an electrode for connecting the n-type thermoelectric material and the p-type thermoelectric material. Here, the base substrate is formed with a flexible insulating polymer material. The p-type thermoelectric material and the n-type thermoelectric material may be carbon nanotubes (CNT), graphene, or nano / micro conductive particles on the surface of a thermoelectric material such as bismuth telluride (BiTe) or lead telluride A combined thermoelectric material powder is formed by incorporation into the flexible insulating polymer material.

In addition, in the flexible thermoelectric device, the flexible insulating polymer may be a silicone-based elastic rubber including PDMS (polydimethyl siloxane) or a polymer material such as nylon, polyvinyl, Kapton, Various carbon based polymer materials are preferred.

In the flexible thermoelectric device, the electrode may be formed of a metal material including aluminum, copper, gold, and silver, one end of which is bonded to the p-type thermoelectric material on one side of the base material substrate, Or a composite material thereof, and a conductive polymer.

The method of manufacturing a flexible thermoelectric device according to the present invention includes the steps of preparing a thermoelectric material powder, preparing a thermoelectric material mixture, forming a thermoelectric material column, arranging a thermoelectric material column, fabricating a substrate substrate, do. In the step of manufacturing the thermoelectric material powder, a p-type thermoelectric material and a thermoelectric material powder of an n-type thermoelectric material having conductive particles bonded to the surface of the thermoelectric material are prepared. In the thermoelectric material mixture manufacturing step, the thermoelectric material powder is mixed with the insulating polymer to form a thermoelectric material mixture. The thermoelectric material manufacturing step inserts the thermoelectric material mixture into a hole of a perforated plate to produce a thermoelectric material. The thermoelectric material column arranging step removes the perforated plate so that the thermoelectric material is arranged on a flat plate so that the p-type thermoelectric material and the n-type thermoelectric material are paired. In the step of fabricating the base material substrate, a base material substrate is manufactured using an insulating polymer so that the thermoelectric materials arranged on the flat plate are bonded. The electrode connection step connects electrodes to both the n-type thermoelectric material and the p-type thermoelectric material on both surfaces of the base substrate.

In the flexible thermoelectric device manufacturing method, it is preferable that the thermoelectric material powder manufacturing step includes a thermoelectric material solution manufacturing step, a stirring step, and an organic solvent evaporation step. The thermoelectric material solution preparation step may include adding a thermoelectric material and conductive particles to an organic solvent such as ethanol, methanol, acetone, alcohol, benzene, and toluene to prepare a thermoelectric material solution. The stirring step stirs the thermoelectric material solution. The organic solvent evaporation step evaporates the organic solvent in the stirred thermoelectric material solution.

In the flexible thermoelectric device manufacturing method, it is preferable that the thermoelectric material mixture manufacturing step includes a stirring step and a degassing step. In the stirring step, the thermoelectric material powder is added to a liquid insulating polymer material and stirred. The thermoelectric material powders can be more effectively dispersed in the liquid insulating polymer by using ultrasonic waves during or after the stirring. The degassing step is a vacuum degassing step after the stirring step.

In the flexible thermoelectric device manufacturing method, it is preferable that the thermoelectric material manufacturing step includes a coating step and a first curing step. The applying step applies the thermoelectric material mixture to the top of the perforated plate. And a step of combing with the blade so that the thermoelectric material mixture is embedded in the hole of the perforated plate may be added. In the first curing step, the thermoelectric material is cured by heating, infrared / ultraviolet irradiation, or the like.

Further, in the flexible thermoelectric device manufacturing method, it is preferable that the base material substrate manufacturing step includes a pressing step, a penetration step, and a secondary curing step. The pressing step presses the thermoelectric material arranged on the flat plate by using the upper flat plate. The infiltrating step infiltrates a liquid insulating polymer between the upper plate and the flat plate. In the second curing step, the base material substrate is cured by heating the infiltrated liquid insulating polymer, using an infrared / ultraviolet irradiation method or the like. The base material substrate manufacturing step may be performed by first applying a liquid insulating polymer, followed by a pressing step and a secondary curing step.

In the flexible thermoelectric device manufacturing method, it is preferable that the electrode connecting step includes an etching step and a deposition step. The etching step etches both surfaces of the base substrate. Through this etching, the insulating polymer film covering the surface of the n-type thermoelectric material column and the p-type thermoelectric material column is etched. By etching this film, the conductive particles covered with the insulating polymer film are exposed to the surface. The exposed conductive particles directly contact the electrode to be deposited thereafter, thereby greatly reducing the contact resistance. In the deposition step, a metal such as aluminum, copper, gold, or silver or a composite material thereof and a conductive polymer material are deposited and electrically connected so that the n-type thermoelectric material column and the p-type thermoelectric material column are selectively connected.

According to the present invention, since the thermoelectric material and the base substrate can be bent flexibly, the whole area of the thermoelectric element can be bent equally when the thermoelectric element is bent. Thus, the bending can be prevented from being concentrated at a specific point of the thermoelectric element.

1 is a conceptual view of a conventional thermoelectric element,
2 is a conceptual diagram of an embodiment of a flexible thermoelectric device according to the present invention,
Fig. 3 is a conceptual view of the thermoelectric material and the electrode of Fig. 2,
Figs. 4 to 8 are conceptual views of a manufacturing method of the embodiment of Fig. 2,
Fig. 9 is a scanning electron microscope (SEM) photograph of the thermoelectric material of the embodiment of Fig. 2,
FIG. 10 is a photograph of the embodiment of FIG. 2,
Fig. 11 is a photograph showing a bent image of Fig. 10,
12 is a flowchart of a manufacturing method of the embodiment of FIG.

An embodiment of a flexible thermoelectric device according to the present invention will be described with reference to FIGS. 2 to 12. FIG.

A flexible thermoelectric device according to the present invention comprises a thermoelectric material (10), a substrate substrate (20) and an electrode (30).

The thermoelectric material (10) has a p-type thermoelectric material (11) and an n-type thermoelectric material (13). The p-type thermoelectric material 11 and the n-type thermoelectric material 13 are formed by mixing a thermoelectric material powder having conductive particles bonded to a p-type or n-type thermoelectric material in a liquid insulating polymer.

The base substrate 20 is formed of an insulating polymer. The thermoelectric material (10) is inserted through the base substrate (20). Here, the thermoelectric material 10 is embedded in the matrix substrate 20 as a pair of p-type thermoelectric material 11 and n-type thermoelectric material 13 in the form of a column.

The electrode 30 is selectively attached to both surfaces of the base substrate 20 so that one end is coupled to the p-type thermoelectric material 11 so that the p-type thermoelectric material 11 and the n-type thermoelectric material 13 are electrically connected to each other, Is coupled to the n-type thermoelectric material (13). In the present embodiment, the electrode 20 is formed of a conductive thin film such as a metal such as aluminum, copper, gold, silver, or a composite material thereof and a conductive polymer.

In this embodiment, a scanning electron microscope (SEM) photograph of the thermoelectric material 10 is shown in Fig. It is found that the thermoelectric material (Bi / Te) is located at the center, the conductive particles (CNT) and the insulating polymer (PDMS) are distributed around the center, and the CNT is bonded to the surface of Bi / Te. PDMS is originally a nonconductive material, but due to the network structure composed of Bi / Te and CNTs, electrons and holes generated from thermoelectric materials can move. This makes it possible to use PDMS, which is a very flexible material with low thermal conductivity, as a thermoelectric material base. In addition, CNTs with strong tensile stress are randomly distributed in the network structure within the PDMS, and thus have excellent characteristics in terms of rigidity and flexibility.

Therefore, in this embodiment, not only the thermoelectric material 10 is flexed flexibly, but also the base material substrate 20 can be flexibly bent.

The manufacturing process of this embodiment includes a thermoelectric material powder manufacturing step S11, a thermoelectric material mixture manufacturing step S13, a thermoelectric material column manufacturing step S15, a thermoelectric material column arranging step S17, (S19) and an electrode connecting step (S21).

In the thermoelectric material powder production step (S11), the thermoelectric material powder of the p-type thermoelectric material (11) and the n-type thermoelectric material (13) having conductive particles bonded to the surface of the thermoelectric material is produced.

More specifically, the thermoelectric material powder manufacturing step S11 includes a thermoelectric material solution manufacturing step, a stirring step, and an ethanol evaporation step.

The thermoelectric material solution preparation step may include adding a thermoelectric material and conductive particles to an organic solvent such as ethanol, methanol, acetone, alcohol, benzene, and toluene to prepare a thermoelectric material solution.

The stirring step stirs by applying a forcing force such as magnetic stirring.

In the ethanol evaporation step, the stirred thermoelectric material solution is heated or allowed to stand at room temperature to evaporate the organic solvent. Then a thermoelectric material powder in which the conductive particles are bonded to the surface of the thermoelectric material is produced.

In the thermoelectric material mixture preparation step (S13), the thermoelectric material powder is mixed with a liquid insulating polymer to form a thermoelectric material mixture.

More specifically, the thermoelectric material mixture preparation step (S13) includes a stirring step and a degassing step.

The thermoelectric material powder can be more effectively dispersed in the liquid insulating polymer by using ultrasonic waves during stirring or stirring in the stirring step.

The degassing step is then degassed under vacuum conditions. This creates a thermoelectric material mixture in which the thermoelectric material powder is incorporated into the insulating polymer.

In the thermoelectric material column manufacturing step S15, the thermoelectric material 10 is formed by inserting the thermoelectric material mixture into the holes of the perforated plate 41. [

In more detail, the thermoelectric material column manufacturing step S51 includes an application step and a primary curing step. The application step is applied to the top of the perforated plate 41 (see FIG. 4). The step of combing the upper portion of the perforated plate 41 by using the blades 43 so that the thermoelectric material mixture is embedded in the holes of the perforated plate may be added (see FIG. 4). The first curing step is performed by heating, infrared / ultraviolet irradiation or curing for a long time. Then, the punched thermoelectric material 11 and the thermoelectric material 10 of the n-type thermoelectric material 13 are formed as shown in FIG. At this time, the p-type thermoelectric material 11 and the n-type thermoelectric material 13 may be separately manufactured, or a pair of the p-type thermoelectric material 11 and the n-type thermoelectric material 13 may be disposed on one perforated plate 41 It is possible.

For example, when the thermoelectric material mixture of the p-type thermoelectric material 11 or the n-type thermoelectric material 13 is applied on the upper surface of the punched plate 41, The material 10 is produced. In this case, the p-type thermoelectric material 11 and the n-type thermoelectric material 13 are separately manufactured. However, in the application step, the thermoelectric material mixture of the p-type thermoelectric material 11 is selectively applied only to the holes of the perforated plate 41 corresponding to the positions where the p-type thermoelectric materials are to be arranged. Next, The thermoelectric material mixture of the material (11) is applied. Then, the thermoelectric material 10 in which the p-type thermoelectric material 11 and the n-type thermoelectric material 13 are arranged in a pair is manufactured in the perforated plate 41. In this state, after the first curing step is performed and the pier plate 41 is removed, the shape as shown in FIG. 6 can be obtained immediately. Therefore, by using this method, the step of forming the p-type thermoelectric material 11 and the n-type thermoelectric material 13 in a columnar shape and arranging them in the lower flat plate 45 is omitted.

The columnar thermoelectric material 10 as shown in FIG. 5 can be manufactured by making a thermoelectric material mixture into a cylindrical shape using a method such as extrusion or casting, and then cutting the thermoelectric material into a desired thickness. The columnar thermoelectric material 10 as shown in FIG. 5 can be manufactured by casting a thermoelectric material mixture to a mold having a cavity such as a thermoelectric material and then discharging the mixture.

In the thermoelectric material column arrangement step S17, the thermoelectric material 10 produced in the thermoelectric material column manufacturing step S15 is arranged on the lower flat plate 45 (see Fig. 6). At this time, the p-type thermoelectric material and the n-type thermoelectric material are arranged on the lower plate 45 in a pair.

If the thermoelectric material 10 in which the p-type thermoelectric material 11 and the n-type thermoelectric material 13 are arranged in pairs is manufactured in the thermoelectric material column manufacturing step S15, (S17), the perforated plate 41 may be removed.

In the base material substrate manufacturing step S19, the base material substrate 20 is formed using the insulating polymer so that the thermoelectric materials 10 arranged on the lower flat plate 45 are bonded.

More specifically, the base material substrate manufacturing step S19 includes a pressing step, a penetration step, and a secondary curing step.

In the pressing step, the thermoelectric material 10 arranged on the lower flat plate 45 is pressed using the upper flat plate 47 (see FIG. 7). The penetration step penetrates the liquid insulating polymer 49 into the void space between the upper plate 47 and the lower plate 45 in this state (see FIG. 7). In the second curing step, the curing process is performed by sufficiently infiltrating the liquid insulating polymer 49 between the upper flat plate 47 and the lower flat plate 45, heating or leaving the liquid insulating polymer 49 intact. When the lower flat plate 45 and the upper flat plate 47 are removed, the base substrate 20 to which the thermoelectric material 10 is bonded is formed as shown in FIG.

The base material substrate manufacturing step (S19) may be performed by first applying a liquid insulating polymer, followed by a pressing step and a secondary curing step.

The electrode connection step S21 connects the electrodes 30 to both the n-type thermoelectric material 11 and the p-type thermoelectric material 13 on both sides of the base substrate 20. [

In more detail, the electrode connection step S21 includes an etching step and a deposition step. In the etching step, both surfaces of the base substrate 20 are etched by dry etching or wet etching to deposit the electrode 30. [ In the deposition step, a metal such as aluminum, copper, gold, or silver or a composite material thereof and a conductive polymer material are deposited and electrically connected so that the n-type thermoelectric material column and the p-type thermoelectric material column are selectively connected. As the electrode deposition method, a dry deposition method such as sputtering, electron beam deposition, thermal evaporation deposition, or a wet deposition method such as screen printing or electroplating may be used. Then, the thermoelectric element as shown in FIG. 10 is completed. Since the thermoelectric element illustrated in FIG. 10 uses PDMS as the material of the mother substrate 20, the region of the mother substrate is transparent due to the property of the material, and is bent very flexibly when bent by hand as shown in FIG.

10: thermoelectric material 11: p-type thermoelectric material
13: n-type thermoelectric material 20: base material substrate
30: Electrode 41: Perforated plate
43: blade 45: lower plate
47: upper plate 49: liquid insulating polymer

Claims (11)

A thermoelectric element comprising a base substrate, a thermoelectric material including a p-type thermoelectric material and an n-type thermoelectric material, and an electrode for connecting the n-type thermoelectric material and the p-type thermoelectric material,
The base substrate is formed with a flexible insulating polymer material,
Wherein the p-type thermoelectric material and the n-type thermoelectric material are formed by mixing a thermoelectric material powder in which conductive particles are bonded to the surface of a thermoelectric material particle, into the flexible insulating polymer material. The method according to claim 1,
Wherein the flexible insulating polymer is a silicone-based polymer material including polydimethyl siloxane (PDMS), a composite material thereof, or a carbon-based polymer material. 3. The method of claim 2,
The electrode is formed of a thin film made of a metal material including aluminum, copper, gold, and silver, or a composite material of which one end is bonded to the p-type thermoelectric material and the other end is bonded to the n-type thermoelectric material, Wherein the thermoelectric element is a thin film. A thermoelectric material powder production step of producing a thermoelectric material powder of a p-type thermoelectric material and an n-type thermoelectric material having conductive particles bonded to the surfaces of the thermoelectric particles,
A thermoelectric material mixture production step of mixing the thermoelectric material powder with a liquid insulating polymer to form a thermoelectric material mixture,
A thermoelectric material column manufacturing step of inserting the thermoelectric material mixture into a hole of a perforated plate and then removing a perforated plate or forming a thermoelectric material by a molding process such as extrusion, casting or die casting of the thermoelectric material mixture;
A thermoelectric material column arranging step of arranging the thermoelectric material on a flat plate such that the p-type thermoelectric material and the n-type thermoelectric material are paired,
A base material substrate manufacturing step of forming a base material substrate using an insulating polymer so that the thermoelectric materials arranged on the flat plate are bonded,
And an electrode connecting step of connecting an electrode to the n-type thermoelectric material and the p-type thermoelectric material on both surfaces of the base substrate. The method according to claim 4, wherein the thermoelectric material powder manufacturing step
A thermoelectric material solution manufacturing step of forming a thermoelectric material solution by adding a thermoelectric material and conductive particles to an organic solvent,
A stirring step of stirring the thermoelectric material solution,
And an organic solvent evaporation step of evaporating the organic solvent in the stirred thermoelectric material solution. The method according to claim 5, wherein the thermoelectric material mixture manufacturing step
A stirring step of adding the thermoelectric material powder to a liquid insulating polymer and stirring the mixture,
And a degassing step of performing a vacuum degassing treatment after the stirring. The method according to claim 6, wherein the thermoelectric material manufacturing step
Applying the thermoelectric material mixture to an upper portion of the perforated plate;
And a first curing step of curing the thermoelectric material. The method according to claim 6, wherein the thermoelectric material manufacturing step
Wherein the thermoelectric material mixture is extruded or casted, or a thermoelectric material is formed by a molding process of die casting. The method as claimed in claim 7,
A pressing step of pressing the thermoelectric material arranged on the lower flat plate at the upper part by using the upper flat plate,
An infiltrating step of infiltrating a liquid insulating polymer between the upper flat plate and the lower flat plate,
And a second curing step of curing the infiltrated liquid-phase insulating polymer. The method as claimed in claim 7,
Applying a liquid insulating polymer on the thermoelectric material arranged on the lower flat plate;
A pressing step of pressing the upper plate using the upper plate,
And a second curing step of curing the liquid insulating polymer. 11. The method according to claim 9 or 10, wherein the electrode connection step
An etching step of etching both surfaces of the base substrate,
And a deposition step of depositing a thin film made of a metal material including aluminum, copper, gold, silver or a composite material thereof and a conductive polymer thin film so that the n-type thermoelectric material and the p-type thermoelectric material are connected to each other, / RTI >
KR1020150160186A 2015-11-16 2015-11-16 Flexible thermoeletric element and the manufacturing method of it KR20170056853A (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20200069735A (en) 2018-12-07 2020-06-17 서울대학교산학협력단 Bidirectional stretchable and flexible wearable thermoelectric cooler and heater
CN114242880A (en) * 2021-12-10 2022-03-25 武汉大学 Flexible self-healing thermoelectric power generation device and preparation method thereof

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20200069735A (en) 2018-12-07 2020-06-17 서울대학교산학협력단 Bidirectional stretchable and flexible wearable thermoelectric cooler and heater
CN114242880A (en) * 2021-12-10 2022-03-25 武汉大学 Flexible self-healing thermoelectric power generation device and preparation method thereof
CN114242880B (en) * 2021-12-10 2022-11-15 武汉大学 Flexible self-healing thermoelectric power generation device and preparation method thereof

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