KR101760834B1 - Chalcogenide thermoelectric material and thermoelectric device comprised same - Google Patents
Chalcogenide thermoelectric material and thermoelectric device comprised same Download PDFInfo
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Abstract
The present invention can be applied to any one selected from Ge and Sn; P, As, Sb and Bi and one selected from S, Se and Te, and any one selected from the group consisting of P, As, Sb and Bi has a relative content of at least one selected from the group consisting of Ge and Sn And at least one selected from the group consisting of P, As, Sb and Bi is relatively less than any one selected from the group consisting of S, Se and Te, or any one selected from Ge and Sn; P, As, Sb and Bi; S, Se and Te; And at least one selected from the group consisting of P, As, Sb and Bi is selected from the group consisting of F, Cl, Br and I, Bi is relatively less in content than any one selected from among S, Se and Te, and any one selected from the group consisting of F, Cl, Br and I has a content relative to the selected one of Ge and Sn And one selected from the group consisting of F, Cl, Br and I has a lower content than any one selected from among S, Se and Te, and a thermoelectric device including the same. .
Description
TECHNICAL FIELD The present invention relates to a chalcogen compound thermoelectric material and a thermoelectric device including the chalcogen compound thermoelectric material, and more particularly, to a chalcogen compound thermoelectric material having an n-type semiconductor property by a composition design of a chalcogen compound and a thermoelectric device including the same. will be.
Thermoelectric conversion means reversible, direct energy conversion between heat and electricity. Heat transfer is a phenomenon in which heat is moved by the movement of electrons and holes in the material, or the movement of electrons or holes is caused by the movement of heat, that is, a current is generated. The peltier effect applied to the cooling field by using the temperature difference at both ends formed by the externally applied current and the seebeck effect applied to the power generation field by using the electromotive force generated from the temperature difference between the both ends of the material Both of these effects are reversible phenomena.
These thermoelectric elements are called thermoelectric modules, Peltier elements, thermoelectric coolers, and thermoelectric modules. These thermoelectric elements are small heat pump devices that absorb heat from a low temperature heat source and heat it to a high temperature heat source , And it is possible to generate electric power by the temperature difference generated at both ends of the material, and it is attracting attention as one of the renewable energy sources.
Generally, thermoelectric cooling and thermoelectric generation are related to the direct conversion of heat and electricity. The success of this technology is closely related to the thermoelectric performance of thermoelectric devices or thermoelectric materials that make up thermoelectric modules. The thermoelectric module should consist of an n-type thermo leg and a p-type thermo leg. It is very advantageous to form each thermoelectric leg with the same material base in the configuration of the thermoelectric device and the setting of the operating temperature range. Therefore, it is necessary to secure both the n-type thermoelectric material and the p-type thermoelectric material in order to commercialize and commercialize the thermoelectric module.
These thermoelectric materials are in the form of n-type and p-type semiconductor devices. Recently, the thermoelectric performance index ZT in a specific crystallographic direction of a SnSe single crystal, which is one of p-type semiconductor materials, , There is a growing interest of academia and industry in the MQ thermoelectric materials to which SnSe belongs, and many studies are underway to manufacture and characterize polycrystalline samples of MQ based materials for commercialization and commercialization.
However, SnSe chalcogen compounds are thermodynamically stable in the formation of Sn vacancies, and thus most of the compounds exhibit p-type semiconductor characteristics, which are difficult to realize as n-type semiconductor characteristics. Therefore, thermal stability and mechanical stability of the thermoelectric module using such a thermoelectric material can not be guaranteed.
SUMMARY OF THE INVENTION The present invention has been made to solve the above-mentioned problems, and it is an object of the present invention to provide a high performance chalcogen compound thermoelectric material and a thermoelectric device including the thermoelectric device. However, these problems are exemplary and do not limit the scope of the present invention.
According to one aspect of the present invention, a chalcogen compound thermoelectric material is provided. Wherein the chalcogen compound thermoelectric material is selected from the group consisting of Ge and Sn; P, As, Sb and Bi and one selected from S, Se and Te, and any one selected from the group consisting of P, As, Sb and Bi has a relative content of at least one selected from the group consisting of Ge and Sn And any one selected from the group consisting of P, As, Sb and Bi may have a relatively smaller content than any one selected from among S, Se and Te.
In the chalcogen compound thermoelectric material, the thermoelectric material may have a composition represented by the following formula (1).
[Chemical Formula 1]
M 1 ± δ- x A x Q
(Where M is any one selected from Ge and Sn, A is any one selected from P, As, Sb and Bi, Q is any one selected from S, Se and Te, and 0 < Real number, real number 0 <x? 0.1)
According to another aspect of the present invention, a chalcogen compound thermoelectric material is provided. Wherein the chalcogen compound thermoelectric material is selected from the group consisting of Ge and Sn; P, As, Sb and Bi; S, Se and Te; And at least one selected from the group consisting of P, As, Sb and Bi is selected from the group consisting of F, Cl, Br and I, Bi is relatively less in content than any one selected from among S, Se and Te, and any one selected from the group consisting of F, Cl, Br and I has a content relative to the selected one of Ge and Sn And any one selected from the group consisting of F, Cl, Br and I may have a relatively smaller content than any one selected from among S, Se and Te.
In the chalcogen compound thermoelectric material, the thermoelectric material may have a composition represented by the following formula (2).
(2)
M 1 ± δ- x A x Q 1 - y Z y
(Where M is any one selected from Ge and Sn, A is any one selected from P, As, Sb and Bi, Q is any one selected from S, Se and Te, Z is F, Cl, Br, and I, and is a real number satisfying 0 < / = 0. 1, and a real number satisfying 0 < x &
In the chalcogen compound thermoelectric material, the thermoelectric material may have n-type characteristics.
In the chalcogenide thermoelectric material, the thermoelectric material may be a cation substitution method of adding any one selected from P, As, Sb and Bi to a compound containing any one of Ge and Sn having a p-type semiconductor property And the self-doping method in which any one selected from the group consisting of Ge and Sn is added as an excess element may be used so that the compound is converted to have an n-type semiconductor property.
In the chalcogenide thermoelectric material, the thermoelectric material may be any one selected from among P, As, Sb and Bi, and one selected from among F, Cl, Br and I, selected from Ge and Sn having p- By using a cation and / or anion substitution method to add to a compound containing any one and a self-doping method in which any selected one of Ge and Sn is added as an excess element, and may be converted to have n-type semiconductor characteristics.
According to another aspect of the present invention, a thermoelectric element is provided. The thermoelectric element may comprise the chalcogen compound thermoelectric material described above.
According to one embodiment of the present invention as described above, it is possible to effectively convert a Sn chalcogen compound-based semiconductor characteristic, which has been known to be difficult in the prior art, to n-type and to increase the possibility of commercialization and commercialization of the thermoelectric module. A compound thermoelectric material and a thermoelectric device including the thermoelectric material can be realized. Of course, the scope of the present invention is not limited by these effects.
1 is a graph of a semiconductor characteristic of a chalcogenide thermoelectric material exhibiting a temperature dependence of a Jacobin coefficient and a temperature according to an embodiment of the present invention.
Hereinafter, embodiments of the present invention will be described in detail with reference to the accompanying drawings. It should be understood, however, that the invention is not limited to the disclosed embodiments, but may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided so that this disclosure will be thorough and complete, Is provided to fully inform the user. Also, for convenience of explanation, the components may be exaggerated or reduced in size.
Hereinafter, embodiments of the present invention will be described with reference to the drawings schematically showing ideal embodiments of the present invention. In the figures, for example, variations in the shape shown may be expected, depending on manufacturing techniques and / or tolerances. Accordingly, the embodiments of the present invention should not be construed as limited to the particular shapes of the regions shown herein, but should include, for example, changes in shape resulting from manufacturing.
Generally, thermoelectric cooling and thermoelectric generation are related to the direct conversion of heat and electricity. The success of this technology is closely related to the thermoelectric performance of thermoelectric devices or thermoelectric materials that make up thermoelectric modules. The thermoelectric module should consist of an n-type thermo leg and a p-type thermo leg. It is very advantageous to form each thermoelectric leg with the same material base in the configuration of the thermoelectric device and the setting of the operating temperature range. Therefore, it is necessary to secure both the n-type thermoelectric material and the p-type thermoelectric material in order to commercialize and commercialize the thermoelectric module.
Recently, studies on MQ-based thermoelectric materials showing p-type semiconductor characteristics have been carried out. However, since most of MQ-based compounds are thermodynamically stable, they have to show p-type semiconductor characteristics. This is known to be difficult.
In order to solve this problem, the present invention provides a chalcogen compound thermoelectric material having an n-type semiconductor property by suppressing the spontaneous generation of cation vacancies of an MQ system compound and a thermoelectric device including the same. More specifically, a method and composition of a compound capable of effectively inhibiting the spontaneous generation of vacancies in a chalcogen compound will be described below.
The chalcogen compound thermoelectric material according to an embodiment of the present invention may include any one selected from Ge and Sn; P, As, Sb and Bi, and one selected from S, Se and Te. At this time, any one selected from among P, As, Sb and Bi is relatively less than any one selected from Ge and Sn, and any one selected from among P, As, Sb and Bi is selected from among S, Se and Te The content is relatively smaller than that of any one selected from the group consisting of < RTI ID = 0.0 >
Meanwhile, the chalcogen compound thermoelectric material according to another embodiment of the present invention may include any one selected from Ge and Sn, one selected from P, As, Sb and Bi, one selected from S, Se and Te, Br and < RTI ID = 0.0 > I. < / RTI > At this time, any one selected from among P, As, Sb and Bi is relatively less than any one selected from Ge and Sn, and any one selected from among P, As, Sb and Bi is selected from among S, Se and Te And at least one selected from the group consisting of F, Cl, Br and I is less than any one selected from the group consisting of Ge and Sn, And one of them is characterized in that the content thereof is smaller than that of any one selected from among S, Se and Te. A detailed description thereof will be given below, for example.
For example, SnSe-based materials are attracting attention as high-performance thermoelectric materials composed of non-toxic and non-conductive elements compared to PbTe-based materials, which are typical thermoelectric materials for middle temperature. The SnSe-based material is an MQ-based thermoelectric material exhibiting intrinsic p-type semiconductor characteristics, in general, in which cation vacancies are thermally generated spontaneously. Here, M is, for example, a chalcogen element such as Ge and Sn, and Q is, for example, an element of S, Se and Te.
On the other hand, in order to realize the desired semiconductor characteristics of the MQ-based material thermoelectric material, the electronic band structure of the MQ-based thermoelectric material can be controlled by changing the composition design of the MQ-based thermoelectric material.
Methods to control this include MQ-based thermoelectric materials such as cation / anion substitution and self-doping. That is, the thermoelectric material may be prepared by a cation substitution method in which any one selected from P, As, Sb and Bi is added to a compound containing any one of Ge and Sn having p-type semiconductor properties, By using a self-doping method in which either is added as an excess element, the compound can be converted to have n-type semiconductor properties.
The thermoelectric material may be any one selected from P, As, Sb and Bi, and any one selected from among F, Cl, Br and I as a compound containing any one selected from Ge and Sn having p- Doping method in which any one selected from the group consisting of Ge and Sn is added as an excess element is used to convert the compound into an n-type semiconductor property, .
Hereinafter, for convenience of description, an embodiment of the present invention will be described in which the above method is applied to SnSe chalcogen compounds.
First, according to one embodiment of the present invention, the SnSe chalcogen compound thermoelectric material can be represented by the following formula (1).
[Chemical Formula 1]
M 1 ± δ- x A x Q
(Where M is any one selected from Ge and Sn, A is any one selected from P, As, Sb and Bi, Q is any one selected from S, Se and Te, and 0 < Real number, real number 0 <x? 0.1)
That is, SnSe chalcogen compounds spontaneously generate Sn vacancies. Therefore, by substituting SnSe chalcogen compounds for any one element selected from Group 15 elements, for example, N, P, As, Sb and Bi, SnSe chalcogen The electron density in the compound is increased and the generation of Sn vacancies can be suppressed.
Further, according to another embodiment of the present invention, the SnSe chalcogenide thermoelectric material can be represented by the following formula (2).
(2)
M 1 ± δ- x A x Q 1 - y Z y
(Where M is any one selected from Ge and Sn, A is any one selected from P, As, Sb and Bi, Q is any one selected from S, Se and Te, Z is F, Cl, Br, and I, and is a real number satisfying 0 < / = 0. 1, and a real number satisfying 0 < x &
That is, any one element selected from among Group 15 elements such as N, P, As, Sb and Bi and a Group 17 element such as F, Cl, Br, Substitution with a cogen compound enables n-type characterization through electron generation of SnSe chalcogen compounds. The detailed description thereof is omitted because it is the same as the above description with reference to the formula (1).
Further, according to another embodiment of the present invention, by adding excess Sn to the SnSe chalcogen compound at the same time as the cation and anion substitution, the compound The Sn spontaneously generated in the compound can be suppressed by generating a dopant spontaneously in itself.
On the other hand, the Jeckeck coefficient, which is related to the properties of thermoelectric materials, varies depending on the composition of the compound. At least one of the Group 15 element and the Group 17 element added to the thermoelectric material of the chalcogen compound having the composition of the above Chemical Formula 1 and Chemical Formula 2 is designed to have a relatively smaller content than the M element or the Q element, , The chalcogen compound thermoelectric material has a positive shear coefficient value or a negative shear coefficient value.
As described above, the chalcogenide thermoelectric material according to the embodiments of the present invention has n-type characteristics by using a cation / anion substitution and a self-doping method for a semiconductor material having p-type characteristics The branch may be converted to a semiconductor material.
Thus, chalcogenide thermoelectric materials have the advantage that their properties do not change over a wide operating temperature range (300 K to 800 K). In addition, conventional MQ-based materials can be used at room temperature as a conventional thermoelectric material for middle temperature. If it can be used at room temperature, it can be directly applied to thermoelectric devices because it is inexpensive, simple to manufacture, low in thermal energy loss, and high in energy conversion efficiency. In addition, it can be applied to various substrates such as a rigid ceramic substrate or a flexible polymer film. Therefore, it can be applied not only to wearable electronic devices but also to various sensors based on solar cells, IR / UV detectors, It can be applied to various places where waste heat such as factories, airplanes and ships is generated.
Hereinafter, in order to facilitate the understanding of the present invention, experimental examples of n-type characteristic thermoelectric conversion by cation substitution are provided. It should be understood, however, that the following examples are for the purpose of promoting understanding of the present invention and are not intended to limit the scope of the present invention.
As a sample according to the experimental example of the present invention, SnSe chalcogen compound was added with a predetermined amount of one of Group 15 elements to prepare a SnSe chalcogen compound thermoelectric material sample. Here, the predetermined amount is calculated by adding the number of moles of each element so that 0 < x < = 0.1 in the formula (1).
On the other hand, for comparison, the same materials as those used in the above Experimental Example were used, and nothing was added thereto.
1 is a graph of a semiconductor characteristic of a chalcogenide thermoelectric material exhibiting a temperature dependence of a Jacobin coefficient and a temperature according to an embodiment of the present invention.
Referring to FIG. 1, the temperature dependency of the whitening coefficient is shown. The samples of the comparative example exhibit typical p-type semiconductor properties since they have a positive shear coefficient value, while samples of the present invention have negative shear coefficient values, indicating that n-type semiconductor characteristics are successfully implemented have.
As described above, by changing the composition of the chalcogen compound simply by changing the composition of the chalcogen compound at a low cost to a thermodynamically stable chalcogen compound as in the embodiment of the present invention, it is possible to change the structure and the band gap of the chalcogen compound, Can be controlled.
Further, the thermoelectric device according to another embodiment of the present invention may include the chalcogen compound thermoelectric material described above. For example, the thermoelectric element may comprise the chalcogenide thermoelectric material and at least two electrodes. Here, the chalcogen compound thermoelectric material may include both an n-type thermoelectric material and a p-type thermoelectric material, and may be electrically connected by being in contact with the at least two electrodes. The thermoelectric element can be understood as a thermoelectric module. The thermoelectric module may be included in a thermoelectric device including a thermoelectric generator, a thermoelectric cooler, and a thermoelectric sensor, but is not limited thereto, and any device capable of directly converting heat and electricity is possible. The construction and the manufacturing method of the thermoelectric element are already known, and a detailed description thereof will be omitted herein.
While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it is evident that many alternatives, modifications and variations will be apparent to those skilled in the art. Accordingly, the true scope of the present invention should be determined by the technical idea of the appended claims.
Claims (8)
Wherein at least one selected from the group consisting of P, As, Sb, and Bi has a relatively smaller content than either Ge or Sn,
Wherein any one selected from the group consisting of P, As, Sb and Bi has a relatively smaller content than any one selected from the group consisting of S, Se and Te,
Wherein at least one selected from the group consisting of F, Cl, Br and I has a smaller content than either Ge or Sn,
Wherein one selected from the group consisting of F, Cl, Br and I has a lower content than any one selected from the group consisting of S, Se and Te.
Chalcogen compound thermoelectric material.
Wherein the thermoelectric material has an n-type characteristic,
Chalcogen compound thermoelectric material.
Wherein the thermoelectric material is one selected from the group consisting of P, As, Sb and Bi and one selected from the group consisting of F, Cl, Br and I to a compound containing any one selected from the group consisting of Ge and Sn having p- Doping method in which at least one selected from the group consisting of Ge and Sn is added as an excess element is used so that the compound has an n-type semiconductor property , ≪ / RTI >
Chalcogen compound thermoelectric material.
Wherein the thermoelectric material has a composition represented by the following formula (2).
(2)
M 1 ± δ-x A x Q 1 -y Z y
(Where M is any one selected from Ge and Sn, A is any one selected from P, As, Sb and Bi, Q is any one selected from S, Se and Te, Z is F, Cl, Br, and I, and is a real number satisfying 0 < / = 0. 1, and a real number satisfying 0 < x &
Wherein the thermoelectric material has an n-type characteristic,
Chalcogen compound thermoelectric material.
Wherein the thermoelectric material is one selected from the group consisting of P, As, Sb and Bi and one selected from the group consisting of F, Cl, Br and I to a compound containing any one selected from the group consisting of Ge and Sn having p- Doping method in which at least one selected from the group consisting of Ge and Sn is added as an excess element is used so that the compound has an n-type semiconductor property , ≪ / RTI >
Chalcogen compound thermoelectric material.
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| KR102121434B1 (en) * | 2017-05-15 | 2020-06-10 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| KR102123041B1 (en) * | 2017-06-07 | 2020-06-15 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| KR102121436B1 (en) * | 2017-06-27 | 2020-06-10 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| KR102121435B1 (en) * | 2017-06-30 | 2020-06-10 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| WO2019066580A2 (en) * | 2017-09-29 | 2019-04-04 | 주식회사 엘지화학 | Chalcogen compound, method for preparing same, and thermoelectric element comprising same |
| KR102138937B1 (en) * | 2017-09-29 | 2020-07-28 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| KR102573731B1 (en) * | 2018-08-24 | 2023-08-31 | 주식회사 엘지화학 | Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same |
| CN111244257B (en) * | 2020-01-20 | 2022-08-05 | 昆明理工大学 | Bi-Sb-Te-Se-S quinary high-entropy alloy and preparation method thereof |
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| US8772622B2 (en) | 2008-02-07 | 2014-07-08 | Basf Se | Doped tin tellurides for thermoelectric applications |
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| US8772622B2 (en) | 2008-02-07 | 2014-07-08 | Basf Se | Doped tin tellurides for thermoelectric applications |
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| Tobias Rosenthal 외, "Enhancing the Thermoelectric Properties of Germanium Antimony Tellurides by Substitution with Selenium in Compounds GenSb2(Te1-xSex)n+3 (0 ≤ x ≤ 0.5; n ≥ 7)," Chem. Mater., 26 (8)* |
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