CN109087988B - Thermoelectric conversion method - Google Patents

Thermoelectric conversion method Download PDF

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CN109087988B
CN109087988B CN201810915554.2A CN201810915554A CN109087988B CN 109087988 B CN109087988 B CN 109087988B CN 201810915554 A CN201810915554 A CN 201810915554A CN 109087988 B CN109087988 B CN 109087988B
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thermoelectric conversion
oxide dielectric
temperature
dielectric material
internal strain
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CN109087988A (en
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初宝进
陈攀
周万丰
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University of Science and Technology of China USTC
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/01—Manufacture or treatment
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80—Constructional details
    • H10N10/85—Thermoelectric active materials
    • H10N10/851—Thermoelectric active materials comprising inorganic compositions
    • H10N10/853—Thermoelectric active materials comprising inorganic compositions comprising arsenic, antimony or bismuth

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Abstract

The invention discloses a thermoelectric conversion method, which comprises the following steps: providing a material having a stable internal strain gradient; and placing the material with the stable internal strain gradient in a first set temperature environment with uniform temperature, wherein the potential difference between two ends of the material with the stable internal strain gradient drives the current carriers in the material to form current, so that thermoelectric conversion is realized. Because the two ends of the material with the stable internal strain gradient present the macroscopic potential difference caused by the flexoelectric effect, the material with the stable internal strain gradient does not need the thermal environment with temperature gradient or temperature change, the potential difference in the material can drive thermally activated carriers to form current only under the environment with uniform temperature, and the material with the stable internal strain gradient can independently perform thermoelectric conversion in the thermal environment with uniform and stable temperature.

Description

Thermoelectric conversion method
Technical Field
The invention relates to the technical field of thermoelectric conversion, in particular to a thermoelectric conversion method.
Background
With the emergence of energy crisis in the world, the focus of attention of people is to find new energy, improve the utilization efficiency of energy and the like. In actual life or production, about 60% of energy released when the energy source is used is directly dissipated in the form of heat energy. If the part of heat energy existing in the form of waste heat is collected and converted into electric energy, secondary utilization of energy can be realized, the utilization efficiency of the energy is also improved, and the pressure of energy crisis is relieved to a certain extent. The functional material used in the process of converting thermal energy into electric energy may be referred to as a thermoelectric conversion material, and the corresponding functional material may be referred to as a thermoelectric material or a pyroelectric material according to a difference in physical effect (seebeck effect or pyroelectric effect) involved in the process. The current research on the application materials of thermoelectric conversion mainly focuses on thermoelectric materials, and the thermoelectric materials are slightly involved.
Thermoelectric materials need to form a temperature difference inside the materials when performing thermoelectric conversion, and ideal thermoelectric materials should have the characteristics of phonon insulation-electronic conduction, and in practice, better thermoelectric output performance is often realized by controlling the electrical conductivity and the thermal conductivity of the materials. While the pyroelectric material needs to be in a thermal environment with temperature change when performing thermoelectric conversion, when the temperature is higher than the curie point, the pyroelectric material can not express the thermoelectric conversion capability due to irreversible polarity loss. In practical applications of thermoelectric conversion materials of conventional angle, the required temperature gradient or temperature change greatly limits their applicability.
In summary, the methods for implementing thermoelectric conversion in the prior art need to provide a certain special temperature environment (temperature gradient or temperature-changing environment) in addition to the respective requirements on the materials themselves, which is very inconvenient in practical application.
Disclosure of Invention
In view of the above, the present invention provides a thermoelectric conversion method to solve the problem that the thermoelectric conversion method in the prior art must depend on a special temperature environment and has use limitation.
In order to achieve the purpose, the invention provides the following technical scheme:
a method of thermoelectric conversion, comprising:
providing a material having a stable internal strain gradient;
and placing the material with the stable internal strain gradient in a first set temperature environment with uniform temperature, wherein the potential difference between two ends of the material with the stable internal strain gradient drives the current carriers in the material to form current, so that thermoelectric conversion is realized.
Preferably, in the thermoelectric conversion method, the material having a stable internal strain gradient is formed by asymmetrically chemically reducing both ends of the oxide dielectric material.
Preferably, in the thermoelectric conversion method, asymmetric chemical reduction is performed on both ends of the oxide dielectric material, specifically:
A) disposing a reducing agent at a first end of the oxide dielectric material;
B) and heating the oxide dielectric material at a second set temperature for a first set time so as to enable the first end of the oxide dielectric material to chemically react with the reducing agent.
Preferably, in the thermoelectric conversion method, the step a) and the step B) further include:
A1) an alumina plate is disposed at a second end of the oxide dielectric material.
Preferably, in the thermoelectric conversion method, the reducing agent is graphite block, hydrogen gas or carbon monoxide.
Preferably, in the thermoelectric conversion method, the oxide dielectric material is a ferroelectric ceramic material.
Preferably, in the thermoelectric conversion method, the ferroelectric ceramic material is a sodium bismuth titanate-based ferroelectric ceramic material.
Preferably, in the thermoelectric conversion method, the preparation method of the sodium bismuth titanate-based ferroelectric ceramic material comprises:
a) bi to be set in proportion2O3、Na2CO3、BaCO3And TiO2Mixing, adding alcohol into the mixture, and then ball-milling for a second set time;
b) drying the powder obtained by ball milling in the step a), and then keeping the temperature at a third set temperature for a third set time to form powder;
c) adding alcohol into the formed powder, ball-milling for a fourth set time, and drying;
d) adding a binder, pressing into a green body, standing the green body at a high temperature to remove the binder, and then keeping the green body at a fourth set temperature for a fifth set time to sinter.
The thermoelectric conversion method provided by the invention comprises the following steps:
s1) providing a material with a stable internal strain gradient;
any material with a stable internal strain gradient can be selected, and the material with the stable internal strain gradient has a first end and a second end, and a macroscopic potential difference caused by a flexoelectric effect is presented between the first end and the second end of the material with the stable internal strain gradient.
S2) placing the material with stable internal strain gradient in a first set temperature environment with uniform temperature, and driving the carriers inside the material with stable internal strain gradient to form current by the potential difference between the two ends of the material, thereby realizing thermoelectric conversion.
Because the two ends of the material with the stable internal strain gradient present the macroscopic potential difference caused by the flexoelectric effect, the material with the stable internal strain gradient does not need the thermal environment with temperature gradient or temperature change, and the potential difference inside the material can drive the thermally activated carriers to form current only under the environment with uniform temperature, so that the material with the stable internal strain gradient can independently perform thermoelectric conversion in the thermal environment with uniform and stable temperature, namely the thermoelectric conversion method provided by the embodiment of the invention can realize thermoelectric conversion only in the thermal environment with uniform and stable temperature, and has stronger applicability and less limitation of the use environment.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the embodiments or the prior art will be briefly described below, it is obvious that the drawings in the following description are only some embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to the drawings without creative efforts.
FIG. 1 is a flow chart of a method of thermoelectric conversion provided by an embodiment of the present invention;
FIG. 2 is a schematic view of a placement configuration of an oxide dielectric material being asymmetrically reduced according to an embodiment of the present invention;
FIG. 3a is 0.92Na after asymmetric reduction provided by embodiments of the present invention0.5Bi0.5TiO3-0.08BaTiO3(NBT8) open circuit voltage versus temperature profile of the test in ceramic wafers;
FIG. 3b shows asymmetrically reduced 0.92Na0.5Bi0.5TiO3-0.08BaTiO3(NBT8) graph of short circuit current versus temperature for the test in ceramic wafers;
FIG. 4 shows various groups provided by embodiments of the present inventionIs divided into (1-x) Na0.5Bi0.5TiO3-xBaTiO3(0<x<0.8, abbreviated as NBT100x) at 825 c for 2h asymmetric chemical reduction, and the short-circuit current as a function of temperature.
In fig. 2:
1-alumina plate, 2-oxide dielectric material and 3-graphite block.
Detailed Description
The invention provides a thermoelectric conversion method, which aims to solve the problem that the thermoelectric conversion method in the prior art has use limitation because the thermoelectric conversion must depend on a special temperature environment.
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
In the description of the present invention, it is to be understood that the terms "upper", "lower", "front", "rear", "left" and "right", etc., indicate orientations or positional relationships based on those shown in the drawings, and are only for convenience of description and simplification of description, but do not indicate or imply that the positions or elements referred to must have specific orientations, be constructed in specific orientations, and be operated, and thus are not to be construed as limitations of the present invention. Furthermore, the terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance.
The inventors have found that the flexoelectric effect describes the coupling effect between electrical polarization and strain gradient, or between stress and electric field gradient, in a material. Due to the unique electromechanical coupling characteristics, the material can be controlled indirectly in electrical behavior through mechanical means. Thus, a method that can independently perform thermoelectric conversion in a general thermal environment can be explored by means of the flexoelectric effect, or a valuable option can be provided for the realization of practical application of the thermoelectric conversion. Because the two ends of the material with the stable internal strain gradient present the macroscopic potential difference caused by the flexoelectric effect, the material with the stable internal strain gradient does not need the thermal environment with temperature gradient or temperature change, and the potential difference inside the material can drive the thermally activated carriers to form current only under the environment with uniform temperature, so that the material with the stable internal strain gradient can independently perform thermoelectric conversion in the thermal environment with uniform and stable temperature, namely the thermoelectric conversion method provided by the embodiment of the invention can realize thermoelectric conversion only in the thermal environment with uniform and stable temperature, and has stronger applicability and less limitation of the use environment.
Based on this, referring to fig. 1, a thermoelectric conversion method according to an embodiment of the present invention includes the steps of:
s1) providing a material with a stable internal strain gradient;
any material with a stable internal strain gradient can be selected, and the material with the stable internal strain gradient has a first end and a second end, and a macroscopic potential difference caused by a flexoelectric effect is presented between the first end and the second end of the material with the stable internal strain gradient.
S2) placing the material with stable internal strain gradient in a first set temperature environment with uniform temperature, and driving the carriers inside the material with stable internal strain gradient to form current by the potential difference between the two ends of the material, thereby realizing thermoelectric conversion.
Preferably, the material having a stable internal strain gradient is formed by asymmetrically chemically reducing both ends of the oxide dielectric material 2. That is, the asymmetric chemical reduction means that the degree of reduction of the first end of the oxide dielectric material 2 is different from the degree of reduction of the second end, and the first end and the second end of the oxide dielectric material 2 are asymmetrically reduced. Wherein the oxide dielectric material 2 belongs to both dielectric and oxide. Of course, the material having a stable internal strain gradient may be other materials, and is not limited herein.
In the above embodiment, asymmetric chemical reduction reactions are performed at two ends of the oxide dielectric material 2, so that the reduction degrees of the first end and the second end of the oxide dielectric material 2 are different, the conductivity of the oxide dielectric material 2 is greatly improved, and meanwhile, the component nonuniformity and the internal strain gradient are generated in the oxide dielectric material 2, thereby presenting a macroscopic potential difference due to the flexoelectric effect. Under the thermal environment condition that the temperatures of the oxide dielectric materials 2 asymmetrically reduced at two ends are uniform and stable, the potential difference of the oxide dielectric materials 2 asymmetrically reduced at two ends can drive thermally activated carriers to form current, so that thermoelectric conversion is realized.
Further, the two ends of the oxide dielectric material 2 are asymmetrically chemically reduced, specifically:
A) disposing a reducing agent at a first end of the oxide dielectric material 2;
i.e., the oxide dielectric material 2 has a first end and a second end, the first end of the oxide dielectric material 2 may be directly contacted with the reducing agent, or the reducing agent may be located on the lower side of the oxide dielectric material 2, and the first end of the oxide dielectric material 2 may be directly placed on the reducing agent having a flat surface.
B) And heating the oxide dielectric material 2 at a second set temperature for a first set time so as to enable the first end of the oxide dielectric material 2 to chemically react with the reducing agent.
The oxide dielectric material 2 and the reducing agent are heated together at a second set temperature for a first set time. The first end of the oxide dielectric material 2 and the reducing agent are subjected to a reduction reaction at a high temperature, and the two ends of the oxide dielectric material 2 are subjected to asymmetric reduction.
Further, between step A) and step B), the method also comprises the following steps: A1) an alumina plate 1 is provided at a second end of the oxide dielectric material 2. The second end of the oxide dielectric material 2 does not chemically react with the alumina plate 1, when the oxide dielectric material 2 is heated at the second set temperature for the first set time, the oxide dielectric material 2 protects the second end of the oxide dielectric material 2 from being reduced by the graphite block 3, and simultaneously the alumina plate 1 presses on the oxide dielectric material 2 so that the first end of the oxide dielectric material 2 is always in contact with the graphite block 3.
In the step B), the second set temperature is 750-. The oxide dielectric material 2 is placed at the temperature of 750-850 ℃ for reaction for 1.5-2.5h, and can also be reacted for 2 h.
Specifically, the reducing agent may be graphite block 3, carbon monoxide, hydrogen, or the like, and is not limited thereto.
In one embodiment, the oxide dielectric material 2 is a ferroelectric ceramic material. Further, the oxide dielectric material 2 may be a sodium bismuth titanate-based ferroelectric ceramic having a chemical composition of general formula (1-x) Na0.5Bi0.5TiO3-xBaTiO3(0<x<0.7, abbreviated NBT100 x). Of course, the oxide dielectric material 2 may also be BaTiO3Ferroelectric material based on SrTiO3Ferroelectric material based on LiNbO3The ferroelectric material is not limited herein.
In another embodiment, step B) is followed by: C) cooling the oxide dielectric material 2 reacted with the reducing agent in the step B) to room temperature in air, and arranging gold electrodes at the first end and the second end of the oxide dielectric material 2. Specifically, gold electrodes may be provided at the first and second ends of the oxide dielectric material 2 by means of ion sputtering.
The oxide dielectric material 2 is cylindrical in its entirety and the thickness of the cylindrical oxide dielectric material 2 is 0.4-0.6mm, preferably 0.5 mm. The thickness of the cylindrical oxide dielectric material 2 is defined as the distance extending along the axis thereof.
When preparing the asymmetrically reduced oxide dielectric material 2, the first end of the oxide dielectric material 2 is placed on the flat graphite block 3, and the second end of the oxide dielectric material 2 is covered with an alumina plate 1 (aluminum sesquioxide plate) to ensure that the oxide dielectric material 2 is tightly attached to the graphite block 3. Then the oxide dielectric material 2, the graphite block 3 and the alumina plate 1 are placed in a resistance furnace together and placed for 2 hours at the temperature of 750-850 ℃ to realize the high-temperature chemical reduction reaction of the first end of the oxide dielectric material 2. The oxide dielectric material 2 after the high-temperature reduction is taken out of the resistance furnace, cooled to room temperature in the air, and then gold electrodes are plated on both ends of the sample by using an ion sputtering method.
In a high-temperature environment, both ends of the oxide dielectric material 2 are asymmetrically reduced, and electrodes are prepared at both ends of the oxide dielectric material 2 when cooled to room temperature. The oxide dielectric material 2 can form asymmetric component gradient after asymmetric chemical reduction under high temperature condition, and the conductivity is greatly improved. Since the oxide dielectric material 2 is normally at a lower temperature than that during reduction, there is a macroscopic strain gradient in the material due to uneven shrinkage. Due to the universality of the flexoelectric effect, a certain stable internal potential difference U is presented in the asymmetrically reduced oxide dielectric material 2int. The asymmetrically reduced oxide dielectric material 2 is connected to a closed external circuit, and the existence of the internal potential difference can cause the directional movement of self carriers to form current. As the ambient temperature increases, the conductivity of the oxide dielectric material 2 increases, resulting in a greater current. Since the thermoelectric current described above is closely related to the internal potential and the electrical conductivity existing within the thermoelectric conversion element, selection of an appropriate material and reduction conditions (reduction temperature, reduction time) are issues that must be considered. Since the ferroelectric oxide material generally has a relatively high flexoelectric coefficient, a relatively high thermoelectric conversion effect can be obtained in the ferroelectric oxide.
In another embodiment, the method for manufacturing the sodium bismuth titanate-based ferroelectric ceramic material comprises the following steps:
a) bi to be set in proportion2O3、Na2CO3、BaCO3And TiO2Mixing, adding alcohol into the mixture, and then ball-milling for a second set time;
i.e. Bi in the stoichiometrically to be set2O3、Na2CO3、BaCO3And TiO2Mixing, adding alcohol into the mixture, and performing ball milling, wherein the second set time can be 12 hours or 11-13 hours, which is not limited herein.
b) Drying the powder obtained by ball milling in the step a), and then keeping the temperature at a third set temperature for a third set time to form powder;
drying the powder obtained after ball milling in the step a) to remove alcohol, and then keeping the temperature at a second set temperature for a third set time to form powder. The third set temperature is 850 ℃ and the third set time is 2-4 h.
c) Adding alcohol into the formed powder, ball-milling for a fourth set time, and drying;
the fourth setting time is 12h, and the drying aims at removing alcohol and volatilizing the alcohol.
d) Adding a binder, pressing into a green body, standing the green body at a high temperature to remove the binder, and then keeping the green body at a fourth set temperature for a fifth set time to sinter. The fourth setting temperature is 1140-1180 ℃, and the fifth setting time is 2-4 h.
In addition, the inventors have also conducted various tests on materials having a stable internal strain gradient. After the sodium bismuth titanate-based ferroelectric ceramic is subjected to asymmetric chemical reduction for 2 hours at 825 ℃, although the measured short-circuit current changes with different components, the short-circuit current with similar behaviors is measured in each component of the ceramic sheet, and the test result is shown in fig. 3-4.
FIG. 3a is 0.92Na after asymmetric reduction0.5Bi0.5TiO3-0.08BaTiO3(NBT8) ceramic wafer, test open circuit voltage vs. temperature curve, FIG. 3b asymmetric reduced 0.92Na0.5Bi0.5TiO3-0.08BaTiO3(NBT8) ceramic wafer, short circuit current was measured as a function of temperature, with the dotted line representing the results of the measurement after flipping the sample end face.
FIG. 4 shows the different components (1-x) Na0.5Bi0.5TiO3-xBaTiO3(0<x<0.8, abbreviated as NBT100x) at 825 ℃ for 2h, and the constant temperature current at 350 ℃ after asymmetric reduction of different components NBT100x ceramic sheets.
The embodiments in the present description are described in a progressive manner, each embodiment focuses on differences from other embodiments, and the same and similar parts among the embodiments are referred to each other.
The previous description of the disclosed embodiments is provided to enable any person skilled in the art to make or use the present invention. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to other embodiments without departing from the spirit or scope of the invention. Thus, the present invention is not intended to be limited to the embodiments shown herein but is to be accorded the widest scope consistent with the principles and novel features disclosed herein.

Claims (8)

1. A method of thermoelectric conversion, comprising:
providing a material having a stable internal strain gradient;
and placing the material with the stable internal strain gradient in a first set temperature environment with uniform temperature, driving current carriers in the material with the stable internal strain gradient to form current by the potential difference between two ends of the material, and realizing thermoelectric conversion, wherein the first set temperature is more than or equal to 50 ℃ and less than or equal to 350 ℃.
2. The method according to claim 1, wherein the material having a stable internal strain gradient is formed by asymmetric chemical reduction of both ends of an oxide dielectric material (2).
3. A thermoelectric conversion method according to claim 2, characterized in that the oxide dielectric material (2) is subjected to asymmetric chemical reduction at both ends, specifically:
A) disposing a reducing agent at a first end of the oxide dielectric material (2);
B) heating the oxide dielectric material (2) at a second set temperature for a first set time to chemically react a first end of the oxide dielectric material (2) with the reducing agent.
4. The method of thermoelectric conversion according to claim 3, further comprising, between step A) and step B):
A1) an alumina plate (1) is arranged at the second end of the oxide dielectric material (2).
5. A method of thermoelectric conversion according to claim 3, characterized in that the reducing agent is graphite block (3), hydrogen or carbon monoxide.
6. A method of thermoelectric conversion according to claim 2, characterized in that the oxide dielectric material (2) is a ferroelectric ceramic material.
7. The thermoelectric conversion method according to claim 6, wherein the ferroelectric ceramic material is a bismuth sodium titanate-based ferroelectric ceramic material.
8. The thermoelectric conversion method according to claim 7, wherein the sodium bismuth titanate-based ferroelectric ceramic material is prepared by:
a) bi to be set in proportion2O3、Na2CO3、BaCO3And TiO2Mixing, adding alcohol into the mixture, and then ball-milling for a second set time;
b) drying the powder obtained by ball milling in the step a), and then keeping the temperature at a third set temperature for a third set time to form powder;
c) adding alcohol into the formed powder, ball-milling for a fourth set time, and drying;
d) adding a binder, pressing into a green body, standing the green body at a high temperature to remove the binder, and then keeping the green body at a fourth set temperature for a fifth set time to sinter.
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Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104529534A (en) * 2014-12-29 2015-04-22 中国科学技术大学 Method for improving flexoelectric effect of ferroelectric oxide material
CN107946453A (en) * 2017-12-01 2018-04-20 中国科学技术大学 A kind of thermoelectric conversion method

Patent Citations (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104529534A (en) * 2014-12-29 2015-04-22 中国科学技术大学 Method for improving flexoelectric effect of ferroelectric oxide material
CN107946453A (en) * 2017-12-01 2018-04-20 中国科学技术大学 A kind of thermoelectric conversion method

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