CN107946453B - Thermoelectric conversion method - Google Patents
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Abstract
The present application provides a thermoelectric conversion method including: providing a sample, wherein the material of the sample is a dielectric material; and applying acting force on the sample to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance in the material. The thermoelectric conversion method provided by the invention is based on the coupling of the flexoelectric effect and the conductance, and is not related to the change of the ambient temperature or the temperature gradient. Compared with the method based on the Seebeck effect or the pyroelectric effect in the prior art, the thermoelectric conversion method provided by the invention can generate thermoelectric current without depending on temperature gradient or temperature change, so that the thermoelectric conversion method can be suitable for more materials, has low requirement on the temperature environment of thermoelectric conversion, and can further expand the application range of thermoelectric conversion.
Description
Technical Field
The invention belongs to the field of functional material application, and mainly relates to a thermoelectric conversion method.
Background
With the advent of the world-wide energy crisis, research into energy recycling has been conducted for decades. Over 40% is lost in the form of heat energy dissipated during energy use. If this part of the dissipated heat energy is collected and converted into electric energy, recycling of the energy can be achieved to some extent. Thermoelectric conversion technology in the traditional sense is based on the Seebeck effect. The Seebeck effect is to realize the macroscopic directional diffusion of charged particles by the temperature difference between the two ends of the material, thereby realizing thermoelectric conversion. The material for realizing thermoelectric conversion based on the Seebeck effect is a thermoelectric material in the traditional sense, and an ideal thermoelectric material has the characteristics of phonon insulation-electronic conduction, but the material is difficult to obtain in practice. Controlling the electrical and thermal conductivity of the material is a matter that must be considered to achieve a greater thermoelectric figure of merit.
Another method for realizing thermoelectric conversion is based on the pyroelectric effect, and the temperature change causes the change of the polarization intensity of the pyroelectric material, thereby generating induction current in an external circuit
(P is electricity)Polarization intensity, T is temperature, T is time), thermoelectric conversion is achieved. This method requires the pyroelectric material to sense the temperature change, i.e. the environment in which the temperature change needs to be provided in practice. In addition, after the temperature exceeds the curie temperature of the ferroelectric pyroelectric material, the polarization intensity disappears, no pyroelectric current is generated any more, and the disappearance of the polarization intensity caused by the temperature exceeding the curie point is irreversible, so that the ferroelectric pyroelectric material needs to perform thermoelectric conversion below the curie point thereof.
In summary, in addition to the respective requirements for the materials themselves, the two methods for implementing thermoelectric conversion in the prior art need to provide a certain special temperature environment (temperature gradient or temperature-changing environment), 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 thermoelectric conversion method, comprising:
providing a sample, wherein the material of the sample is a dielectric material;
applying force to the sample to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance of the sample material.
Preferably, the sample is a high symmetry sample having at least two macroscopic axes of symmetry.
Preferably, the highly symmetrical sample is a disk-shaped sample or a flat plate-shaped sample with a rectangular cross section.
Preferably, the applying a force on the sample generates a strain gradient inside the sample, and generates a thermoelectric current based on a flexoelectric effect and an electrical conductance of the sample material, specifically including:
and applying acting force to the sample by adopting a three-point bending method or a cantilever beam method to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance of the sample material.
Preferably, the sample is a low profile symmetric sample or an asymmetric profile sample, the low profile symmetric sample being a sample having only one axis of symmetry.
Preferably, the low symmetry sample is an isosceles trapezoid frustum shaped sample or a truncated cone shaped sample.
Preferably, the material of the sample is ferroelectric material.
Preferably, the ferroelectric material comprises sodium bismuth titanate-based ferroelectric ceramic with a chemical composition general formula of (1-x) Na1/2Bi1/ 2TiO3-xBaTiO3Wherein x is 0,0.04,0.2, 0.5.
As can be seen from the above technical solutions, the thermoelectric conversion method provided by the present invention specifically includes, based on the flexoelectric effect: after the sample is provided, a force is applied to the sample to generate a strain gradient in the sample, thereby generating a thermoelectric current. Compared with the prior art based on the Seebeck effect or the pyroelectric method, the thermoelectric conversion method provided by the invention can generate thermoelectric current without depending on temperature gradient or temperature change, so that the thermoelectric conversion method can adapt to more materials, has lower requirement on the temperature environment of thermoelectric conversion, and can expand the application range of thermoelectric conversion.
Further, because the thermoelectric conversion method provided by the invention does not need to provide a stable temperature difference environment, an additional system for controlling the temperature difference is not needed in the practical application process, so that the thermoelectric conversion system can be simplified, and the complexity of the thermoelectric conversion system is reduced.
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 embodiments of the present invention, and for those skilled in the art, other drawings can be obtained according to the provided drawings without creative efforts.
FIG. 1 is a schematic flow diagram of a thermoelectric conversion process provided by the present invention;
FIG. 2 is a schematic diagram of a structure for applying a force to a flat sample according to an embodiment of the present invention;
3-6 provide thermal current-temperature profiles for different component materials according to embodiments of the present invention;
FIG. 7 is a schematic structural diagram of a sample with an equal waist trapezoid table for applying a force according to an embodiment of the present invention;
fig. 8 is a schematic structural diagram of applying a force to a truncated cone sample according to an embodiment of the present invention.
Detailed Description
As described in the background section, the thermoelectric conversion methods in the related art each limit the use scenarios of the thermoelectric conversion methods and the use of materials capable of realizing thermoelectric conversion.
The inventors have found that the above problems occur in the prior art because the thermoelectric conversion methods in the prior art depend on a special temperature environment, such as a temperature gradient or a temperature-changing environment, and the structural requirements of the material itself are high. In the actual production process, the thermoelectric conversion based on the Seebeck effect requires an additional system to obtain a temperature gradient, and the thermoelectric conversion based on the pyroelectric effect is limited in applicable materials, so that the application of the thermoelectric conversion is limited.
Based on this, the present invention provides a thermoelectric conversion method comprising:
providing a sample, wherein the material of the sample is a dielectric material;
applying force to the sample to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance of the sample material.
Compared with the prior art based on the Seebeck effect or the pyroelectric method, the thermoelectric conversion method provided by the invention can generate thermoelectric current without depending on temperature gradient or temperature change, so that the thermoelectric conversion method can be suitable for more materials, has lower requirement on the temperature environment of thermoelectric conversion, and can further expand the application range of thermoelectric conversion.
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.
As shown in fig. 1, a schematic flow chart of a thermoelectric conversion method according to an embodiment of the present invention is provided, where the thermoelectric conversion method includes:
s101: providing a sample, wherein the material of the sample is a dielectric material;
in this embodiment, the material composition of the sample and the shape of the sample are not limited, and any sample that can generate a strain gradient inside and further generate a thermoelectric current after applying a force can be used as the sample in this embodiment.
It should be noted that the flexoelectric coefficient of a material is in a positive correlation with the dielectric constant of the material, and a material with a larger dielectric constant can generate a larger flexoelectric response at the same strain gradient than a material with a smaller dielectric constant, so that, in this embodiment, the sample is an optional dielectric material, so as to generate a stronger thermoelectric current based on the flexoelectric effect.
S102: applying acting force on the sample to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance of the sample.
In this embodiment, under the unchangeable condition of temperature, exert the effort to the sample, produce the strain gradient in sample inside, and then produce thermoelectric current. The principle of generating thermoelectric current in this embodiment is based on the flexoelectric effect, which is an electromechanical coupling response in a material, describing the coupling between electric polarization and a strain gradient generated by the material under the action of an external force, and can be expressed by the following formula:
wherein P is the electric polarization strength caused by the strain gradient generated by the material under the action of external force, mu is the flexoelectric coefficient of the material (having positive correlation dependence on the dielectric constant of the material),
is the strain gradient in the z-direction in the material. It is a general effect, has no special requirements on the crystal symmetry of the material, and is present in all dielectric materials.
Therefore, in the embodiment of the present application, after providing the sample, if a strain gradient can be generated inside the sample, the electric polarization can be induced, and then the flexural electric field can be generated, so that the electric conductance of the sample material can be induced, and the thermoelectric current can be generated.
In this embodiment, the type of force applied to the sample and the magnitude of the force are not limited, and optionally, the force and the shape of the sample act together to generate a strain gradient inside the sample, so as to generate thermoelectric current.
The mechanism of thermoelectric current generation in this example is: the material generates strain gradient (i.e. non-uniform deformation) under the action of external force, and an electric field can be generated in the material through the flexoelectric effect, i.e. a flexural electric field Eflexo。
Where Q is the charge due to the flexoelectric effect, C is the capacitance of the material, and h is the thickness of the sample. The electric field will leadThe electrical conductance of the material, and the resulting current density, may be expressed as i ═ σ Eflexo(where σ is the conductivity of the material), the carrier concentration in the material increases with increasing ambient temperature, and thus a stronger current can be generated.
Since the thermoelectric current is closely related to the flexoelectric coefficient of the material, and the ferroelectric material has a high flexoelectric coefficient, the material of the sample described in this embodiment is preferably a ferroelectric material.
The flexoelectric effect describes a phenomenon in which non-uniform strain (strain gradient) causes electrical polarization, whereas uniform strain cannot cause electrical polarization.
For dielectric materials, the existence of macroscopic potential difference indicates the existence of macroscopic electric polarization, and the relationship can be expressed by formula
(U is a potential difference, and S is a sample surface area). Therefore, a thermoelectric current can be formed by creating a macroscopic strain gradient inside the sample.
In the thermoelectric conversion method in the prior art, a stable temperature difference environment needs to be provided for the thermoelectric material, so that an additional system for controlling the temperature difference needs to be designed in the thermoelectric conversion system in the prior art; also, the limitations of the prior art thermoelectric conversion methods come from the limitations of the materials themselves: in the conventional thermoelectric material, the thermoelectric figure of merit ZT ═ S was evaluated for thermoelectric conversion performance2σ T/κ, where S is the Seebeck coefficient, σ is the electrical conductivity, and κ is the thermal conductivity. Therefore, besides the Seebeck coefficient, the electrical conductivity and the thermal conductivity of the material also reach a certain matching degree, and the electrical conductivity and the thermal conductivity have a certain positive correlation; in the pyroelectric material, the pyroelectric coefficient is a parameter which must be considered, and is an intrinsic characteristic of the corresponding component material, namely different components correspond to different pyroelectric coefficients. In addition, for thermoelectric conversion based on the pyroelectric effect, the range of the use temperature also limits the types of materials that can be used.
Compared with the thermoelectric conversion method in the prior art, the thermoelectric conversion method provided by the embodiment of the invention has the following advantages:
1. the method for bending the electric-heat conversion does not need the environment with temperature gradient or temperature change, and can be realized in a uniform environment, so that the environmental requirement of the electric-heat conversion is simplified;
2. because thermoelectric conversion can be realized in a uniform environment, an additional system for controlling stable temperature difference in the prior art is not needed, and the complexity of the corresponding thermoelectric conversion system is simplified;
3. can be applied to more materials, and is not limited to the traditional thermoelectric material.
In addition, it should be noted that the specific method employed when applying the force is not limited in this embodiment, and specific operation methods will be given in the following embodiments. The foregoing is a basic idea of an embodiment of the present invention, and a specific process of the thermoelectric conversion method provided in the embodiment is described below with a specific embodiment.
In one embodiment of the present invention, a thermoelectric conversion method includes:
providing a sample with high symmetry of the shape, wherein the sample with high symmetry of the shape is a sample with at least two symmetry axes;
in this embodiment, the specific shape of the highly symmetric sample is not limited, and alternatively, the highly symmetric sample may be a wafer-shaped sample, or may also be a flat-plate-shaped sample with a rectangular cross section, as shown in fig. 2, in this embodiment, a flat-plate-shaped sample 11 with a rectangular cross section is taken as an example for detailed description.
The method for realizing thermoelectric conversion is a method for driving carriers in a material to directionally move to form current through a flexural electric field generated by a flexoelectric effect so as to realize the thermoelectric conversion, and can be applied to ferroelectric materials. In the embodiment, the feasibility of the method is shown by taking sodium bismuth titanate-based ferroelectric ceramic as an example, and the general formula of the chemical component is (1-x) Na1/2Bi1/2TiO3-xBaTiO3(x ═ 0,0.04,0.2,0.5, abbreviated NBT, NBT4, NBT20, NBT 50).
Preparing ceramic sample by traditional solid phase synthesis method, and adding Bi in a certain proportion according to stoichiometric proportion2O3，Na2CO3，BaCO3，TiO2(analytical reagent)Mixing, adding alcohol, ball milling for 12 hr, stoving, and maintaining at 850 deg.c for 2 hr to synthesize powder of each component. Then adding the synthesized powder into alcohol, ball-milling for 12 hours again, drying, adding a proper binder, and pressing into a rectangular strip-shaped blank. Removing the binder in the green body at high temperature, and then putting the green body into a muffle furnace to be sintered for 2 to 4 hours at the temperature of 1140 to 1180 ℃. The sintered ceramic rectangular bar was cut into small pieces 4.5mm wide and 20mm long, then polished to about 0.6mm thick, then coated with silver paste at both ends, and sintered at 850 ℃ for 30min to form silver electrodes.
And applying force to the sample to generate a strain gradient inside the sample so as to generate thermoelectric current.
In this embodiment, since the sample is a highly symmetric sample, a certain method needs to be selected to apply an acting force on the sample to generate an internal strain gradient if a strain gradient, that is, a non-uniform deformation, is generated in the highly symmetric sample.
It should be noted that, in this embodiment, the method for applying the force capable of generating the strain gradient on the sample is not limited, and alternatively, a three-point bending method or a cantilever beam method may be used to bend the uniform sample, specifically, as shown in fig. 2, a three-point bending method is used to support two ends of the long strip of the dielectric material, and then a force is applied in the middle of the sample. Under the action of external force, the elongated dielectric material is bent (i.e., non-uniformly deformed).
It should be noted that, as the ambient temperature increases, the carrier concentration in the sample material increases, so that a stronger current can be generated, that is, the higher the ambient temperature is, the larger the thermoelectric current is, so as to obtain a larger thermoelectric current and facilitate the detection of the thermoelectric current. That is, the temperature raising, holding, and temperature lowering processes in this embodiment are only for obtaining thermoelectric current data at certain temperatures, and are not for creating an environment with temperature changes.
In this example, Na is added1/2Bi1/2TiO3-BaTiO3The ceramics were prepared into flat plate-shaped samples, and thermoelectric current could be measured at relatively high temperature using the thermoelectric conversion method provided by the present invention, as shown in fig. 3 to 6. Fig. 3 to 6 show the thermoelectric current versus temperature of flat plate samples having different compositions, wherein fig. 3 shows the thermoelectric current of the flat plate sample with NBT, fig. 4 shows the thermoelectric current of the flat plate sample with NBT4, fig. 5 shows the thermoelectric current of the flat plate sample with NBT20, fig. 6 shows the thermoelectric current of the flat plate sample with NBT50, and the horizontal axis and the vertical axis of the four images show the temperature and the thermoelectric current value, respectively. It can also be seen from fig. 3-6 that as the temperature increases, the sample material generates a greater thermoelectric current, and as the temperature decreases, the thermoelectric current within the sample material decreases.
In the testing process, the temperature is kept for 10min at the highest temperature of 600 ℃, the sample is in a uniform thermal environment in the heat preservation process, the corresponding testing current is not zero, the generation of the flexural electrothermal current is illustrated, and the temperature gradient or the changed temperature environment is not needed.
It should be noted that the solid lines in fig. 3-6 represent thermal current-temperature curves obtained by applying stress to the sample in the temperature raising process, the temperature keeping process, and the temperature reducing process after the sample is placed; and the dotted line represents a thermal current-temperature curve obtained by testing the sample under the conditions that the sample is only overturned and other parts of the test circuit are not changed and stress is applied to the sample in the processes of temperature rise, heat preservation and temperature reduction.
As can be seen from fig. 3 to 6, the bending electric field induces current, which realizes thermoelectric conversion; and no matter how the sample composition changes, thermoelectric current is generated, so that the thermoelectric conversion mode for realizing flexoelectricity can be applied to various materials, and the generated thermoelectric current is larger when the ambient temperature is higher.
In addition, after the sample placing direction is changed in the experiment (the sample end face placing modes corresponding to the two tests are opposite), the current directions in the obtained circuits are the same (both positive currents). That is, the thermoelectric current obtained by the test is independent of the sample placement direction and depends on the external stress gradient.
In this embodiment, a three-point bending acting force is applied to a sample with a highly symmetrical external shape, so that the sample is bent and deformed, and a strain gradient is generated in the sample, thereby generating a thermoelectric current. It has been demonstrated by experiments that thermoelectric currents are generated based on the flexoelectric effect in a uniform environment, independent of temperature changes, or temperature gradients.
In another embodiment of the present invention, a thermoelectric conversion method includes:
providing a sample having a low symmetry or a sample that is asymmetric in shape, the low symmetry sample being a sample having only one axis of symmetry;
in this embodiment, the specific shape of the low symmetry sample is not limited, and alternatively, the low symmetry sample may be an isosceles trapezoid frustum shaped sample or a truncated cone shaped sample, as shown in fig. 7 and 8, where fig. 7 is the isosceles trapezoid frustum shaped sample, and fig. 8 is the truncated cone shaped sample.
The difference from the previous embodiment is that the sample with a highly symmetrical shape is not uniformly deformed by bending, but only uniformly deformed due to uniform shape when positive compression is adopted.
In the embodiment, since the sample shape is provided to be low symmetrical or asymmetrical, a strain gradient can be generated in the sample by adopting a positive compression mode. As shown in fig. 7 and 8, the acting force is applied to the upper bottom surface of the isosceles trapezoid sample or the truncated cone sample, and the stress or strain generated on each section perpendicular to the acting force direction is different and is finally distributed in a gradient manner because the size of each section perpendicular to the acting force direction in the sample is different.
In this embodiment, applying a force to the sample to generate a strain gradient inside the sample and generate a thermoelectric current specifically includes: and applying positive compression acting force on the sample to generate a strain gradient in the sample so as to generate thermoelectric current.
And finally, putting the sample with the specific shape into an electric furnace to be heated, applying external force on the sample to generate non-uniform deformation, and generating thermoelectric current caused by flexoelectric effect and conductive coupling so as to realize thermoelectric conversion. The generation principle is the same as that in the previous embodiment, and detailed description thereof is omitted in this embodiment.
Compared with the prior art based on the Seebeck effect or the pyroelectric method, the thermoelectric conversion method provided by the invention can generate thermoelectric current without depending on temperature gradient or temperature change, so that the thermoelectric conversion method can be suitable for more materials, has lower requirement on the temperature environment of thermoelectric conversion, and can further expand the application range of thermoelectric conversion.
Further, because the thermoelectric conversion method provided by the invention does not need to provide a stable temperature difference environment, an additional system for controlling the temperature difference is not needed in the practical application process, so that the thermoelectric conversion system can be simplified, and the complexity of the thermoelectric conversion system is reduced.
It should be noted that, in the present specification, the embodiments are all described in a progressive manner, each embodiment focuses on differences from other embodiments, and the same and similar parts among the embodiments may be 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 (6)
1. A method of thermoelectric conversion, comprising:
providing a sample, wherein the material of the sample is a dielectric material;
applying acting force on the sample to generate a strain gradient inside the sample, and generating thermoelectric current based on a flexoelectric effect and the conductivity of the material;
the thermoelectric current generation mechanism is: the material generates strain gradient under the action of external force, and an electric field is generated in the material through the flexoelectric effect, namely a flexural electric field Eflexo(ii) a The flexural electric field drives the directional movement of carriers in the material to generate a current, and the current density generated thereby is expressed as i ═ σ EflexoWherein σ is the conductivity of the material;
wherein the sample is made of sodium bismuth titanate-based ferroelectric ceramic with a chemical component general formula of (1-x) Na1/2Bi1/2TiO3-xBaTiO3Wherein x is 0,0.04,0.2, 0.5.
2. The thermoelectric conversion method according to claim 1, wherein the sample is a high-symmetry sample having at least two macroscopic axes of symmetry.
3. The method according to claim 2, wherein the sample having a highly symmetrical outer shape is a disk-shaped sample or a flat plate-shaped sample having a rectangular cross section.
4. The method according to claim 3, wherein the applying a force on the sample generates a strain gradient inside the sample, and generates a thermoelectric current based on a flexoelectric effect and an electrical conductance of the sample material, and specifically comprises:
and applying acting force to the sample by adopting a three-point bending method or a cantilever beam method to generate a strain gradient inside the sample, and generating thermoelectric current based on the flexoelectric effect and the conductance of the sample material.
5. The thermoelectric conversion method according to claim 1, wherein the sample is a low profile symmetric sample or an asymmetric profile sample, and the low profile symmetric sample is a sample having only one axis of symmetry.
6. The method according to claim 5, wherein the low symmetry sample is an isosceles trapezoid frustum shaped sample or a truncated cone shaped sample.
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