WO2023054416A1 - 熱電変換素子及びセンサ - Google Patents
熱電変換素子及びセンサ Download PDFInfo
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- WO2023054416A1 WO2023054416A1 PCT/JP2022/036045 JP2022036045W WO2023054416A1 WO 2023054416 A1 WO2023054416 A1 WO 2023054416A1 JP 2022036045 W JP2022036045 W JP 2022036045W WO 2023054416 A1 WO2023054416 A1 WO 2023054416A1
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- H—ELECTRICITY
- H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
- H02N—ELECTRIC MACHINES NOT OTHERWISE PROVIDED FOR
- H02N11/00—Generators or motors not provided for elsewhere; Alleged perpetua mobilia obtained by electric or magnetic means
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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
- H10N15/00—Thermoelectric devices without a junction of dissimilar materials; Thermomagnetic devices, e.g. using the Nernst-Ettingshausen effect
- H10N15/20—Thermomagnetic devices using thermal change of the magnetic permeability, e.g. working above and below the Curie point
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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
- H10N50/00—Galvanomagnetic devices
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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
- H10N59/00—Integrated devices, or assemblies of multiple devices, comprising at least one galvanomagnetic or Hall-effect element covered by groups H10N50/00 - H10N52/00
Definitions
- the present invention relates to thermoelectric conversion elements and sensors.
- Patent Document 1 describes a thermoelectric power generation device that utilizes the anomalous Nernst effect.
- the anomalous Nernst effect is a phenomenon in which a voltage is generated in a direction orthogonal to both the magnetization direction and the temperature gradient when a heat flow is applied to a magnetic material and a temperature difference is generated.
- thermoelectric power generation device has a substrate, a power generation body, and a connection body.
- the power generating body consists of a plurality of thin wires arranged parallel to each other along the surface of the substrate.
- the power generator is configured to generate power with a temperature difference in the direction perpendicular to the magnetization direction due to the anomalous Nernst effect.
- the connector consists of a plurality of thin wires arranged parallel to and between the thin wires of the power generator along the surface of the substrate. Each thin wire of the connector electrically connects one end of each thin wire of the power generating body and the other end of the adjacent thin wire on one side of each thin wire.
- the connection body electrically connects each thin wire of the power generation body in series.
- the connector is made of, for example, non-magnetic Cr.
- thermoelectric conversion elements for heat sensing.
- thermoelectric conversion elements using magnetic thermoelectric conversion such as the thermoelectric conversion device described in Patent Document 1
- thermoelectric power generation devices using the Seebeck effect thermoelectric conversion elements using the Seebeck effect
- thermoelectric conversion device In the thermoelectric conversion device described in Patent Document 1, the power generator is configured to generate power by the temperature difference in the direction perpendicular to the direction of magnetization.
- a thermoelectric conversion element using magnetic thermoelectric conversion it is assumed that an electromotive force is generated by a mechanism different from that of magnetic thermoelectric conversion.
- the thermoelectric conversion device described in Patent Document 1 if a temperature gradient occurs in the longitudinal direction of the thin wire of the power generator made of the FePt thin film and the thin wire of the connecting member made of non-magnetic Cr, the Seebeck coefficient of FePt and the Cr Due to the difference from the Seebeck coefficient, a thermoelectromotive force associated with the Seebeck effect may occur in the longitudinal direction.
- thermoelectromotive force is advantageous from the viewpoint of the accuracy of heat sensing. This is because the electromotive force due to the Seebeck effect is superimposed on the electromotive force due to magneto-thermoelectric conversion.
- a connection body made up of a plurality of fine wires is electrically connected in series with a power generation body made up of a plurality of fine wires. ing. In such a configuration, the electromotive force associated with the Seebeck effect tends to increase, which may greatly affect the accuracy of heat sensing.
- the present invention provides a thermoelectric conversion element that is advantageous from the viewpoint of improving the accuracy of heat sensing while using magnetic thermoelectric conversion.
- the present invention a linearly extending magnetic thermoelectric conversion body; and a wiring electrically connected to the magnetic thermoelectric conversion body,
- the absolute value of the difference between the Seebeck coefficient Sm in the longitudinal direction of the magnetic thermoelectric converter and the Seebeck coefficient Sc in the longitudinal direction of the wiring is 10 ⁇ V/K or less.
- a thermoelectric conversion element is provided.
- thermoelectric conversion element is advantageous from the viewpoint of improving the accuracy of heat sensing while using magnetic thermoelectric conversion.
- FIG. 1 is a perspective view showing an example of an embodiment of a thermoelectric conversion element.
- FIG. 2 is a cross-sectional view of the thermoelectric conversion element taken along plane II shown in FIG.
- FIG. 3 is a cross-sectional view showing another example of the thermoelectric conversion element.
- FIG. 4 is a cross-sectional view showing still another example of the thermoelectric conversion element.
- the thermoelectric conversion element 1 a includes a magnetic thermoelectric conversion body 11 and wiring 12 .
- the magnetic thermoelectric converter 11 extends linearly.
- the wiring 12 is electrically connected to the magneto-thermoelectric converter 11 .
- of the difference between the Seebeck coefficient Sm in the longitudinal direction of the magnetic thermoelectric converter 11 and the Seebeck coefficient Sc in the longitudinal direction of the wiring 12 is 10 ⁇ V/K or less.
- the Seebeck coefficient Sm and the Seebeck coefficient Sc are, for example, values at 25 to 40° C., and can be measured according to the method described in Examples.
- the X, Y and Z axes are orthogonal to each other.
- the magneto-thermoelectric converters 11 and the wirings 12 are arranged, for example, along a plane parallel to the XY plane.
- thermoelectric conversion element 1a when a temperature gradient occurs in the longitudinal direction (Y-axis direction) of the magnetic thermoelectric conversion body 11, the difference between the Seebeck coefficient Sm and the Seebeck coefficient Sc results in a thermoelectric rise due to the Seebeck effect in the longitudinal direction. Electricity can be generated.
- is 10 ⁇ V/K or less. tends to be small. Therefore, in sensing using the thermoelectric conversion element 1a, the electromotive force due to the Seebeck effect superimposed on the electromotive force due to magnetic thermoelectric conversion tends to be small. As a result, the thermoelectric conversion element 1a is advantageous from the viewpoint of realizing highly accurate heat sensing using magnetic thermoelectric conversion.
- may be 9.5 ⁇ V/K or less, 9.0 ⁇ V/K or less, 8.5 ⁇ V/K or less, or 8.0 ⁇ V/K or less. It may be less than or equal to 7.5 ⁇ V/K, or less than or equal to 7.0 ⁇ V/K.
- may be 6.5 ⁇ V/K or less, 6.0 ⁇ V/K or less, 5.5 ⁇ V/K or less, or 5.0 ⁇ V/K or less. There may be.
- may be 4.5 ⁇ V/K or less, 4.0 ⁇ V/K or less, 3.5 ⁇ V/K or less, or 3.0 ⁇ V/K or less.
- may be 1.5 ⁇ V/K or less, 1.0 ⁇ V/K or less, 0.8 ⁇ V/K or less, or 0.5 ⁇ V/K or less. 0.3 ⁇ V/K or less, or 0.2 ⁇ V/K or less.
- is not limited to a specific value.
- is, for example, 0.01 ⁇ V/K or more, may be 0.05 ⁇ V/K or more, may be 0.1 ⁇ V/K or more, or may be 0.2 ⁇ V/K or more may be 0.5 ⁇ V/K or more, or 1.0 ⁇ V/K or more.
- the relationship between the signs of the Seebeck coefficient Sm and the Seebeck coefficient Sc is not limited to a specific relationship as long as the absolute value
- the Seebeck coefficient Sm and the Seebeck coefficient Sc for example, have values of the same sign. This tends to reduce the absolute value
- the Seebeck coefficient Sm and the Seebeck coefficient Sc may have values of different signs.
- the Seebeck coefficient Sc is not limited to a specific value.
- the Seebeck coefficient Sc has a value of 0 or less, for example.
- the Seebeck coefficient Sc is, for example, 0 ⁇ V/K or less, may be ⁇ 5 ⁇ V/K or less, may be ⁇ 10 ⁇ V/K or less, may be ⁇ 15 ⁇ V/K or less, may be ⁇ 20 ⁇ V/K or less. It may be K or less.
- the Seebeck coefficient Sc is, for example, -50 ⁇ V/K or more.
- the Seebeck coefficient Sc may be a positive value, for example, 1 ⁇ V/K or more, 3 ⁇ V/K or more, 5 ⁇ V/K or more, or 10 ⁇ V/K or more. There may be.
- the Seebeck coefficient Sm is not limited to a specific value.
- the Seebeck coefficient Sm is, for example, 0 ⁇ V/K or less, may be ⁇ 5 ⁇ V/K or less, may be ⁇ 10 ⁇ V/K or less, or may be ⁇ 15 ⁇ V/K or less.
- the Seebeck coefficient Sm is -50 ⁇ V/K or more, for example.
- the Seebeck coefficient Sm may be a positive value, for example, 1 ⁇ V/K or more, 3 ⁇ V/K or more, 5 ⁇ V/K or more, or 10 ⁇ V/K or more. There may be.
- of the Seebeck coefficient Sm is desirably 10 ⁇ V or more.
- the magnetic thermoelectric coefficient tends to increase, and the thermoelectric conversion performance of the thermoelectric conversion element 1a tends to increase.
- may be 15 ⁇ V or more, or may be 20 ⁇ V or more.
- the resistivity of the wiring 12 is not limited to a specific value.
- the wiring 12 has a specific resistance of 8 to 200 ⁇ cm, for example. This facilitates adjustment of the Seebeck coefficient Sc to a desired range. In addition, even if the wiring 12 is made thin, it is easy to reduce the resistance.
- the specific resistance of the wiring 12 may be 10 ⁇ cm or more, 15 ⁇ cm or more, 20 ⁇ cm or more, 25 ⁇ cm or more, or 30 ⁇ cm. or more.
- the specific resistance of the wiring 12 may be 180 ⁇ -cm or less, 150 ⁇ -cm or less, 140 ⁇ -cm or less, 130 ⁇ -cm or less, or 120 ⁇ -cm. or less, 110 ⁇ cm or less, or 100 ⁇ cm or less.
- the material forming the wiring 12 is not limited to a specific material.
- the wiring 12 contains at least one metal selected from the group consisting of Cu, Ag, Au, Al, Ni, and Co, for example.
- the content of these metals in the wiring 12 is 50% or more based on the number of atoms.
- the total content of Cu, Ag, Au, Al, Ni, and Co in the wiring 12 is 50% or more based on the number of atoms.
- the wiring 12 may be made of a single metal, or may be made of an alloy.
- the wiring 12 is composed of at least one metal selected from the group consisting of Cu, Ag, Au, and Al, and at least one metal selected from the group consisting of Group 8 elements, Group 9 elements, and Group 10 elements. element.
- the Seebeck coefficient Sc of the alloy tends to fluctuate over a wide range from positive values to negative values depending on the composition, and the Seebeck coefficient Sc is easily adjusted to a desired value.
- the Group 8 element is, for example, Fe.
- a group 9 element is Co, for example.
- Group 10 elements are, for example, Ni or Pt.
- the content of at least one element selected from the group consisting of Group 8 elements, Group 9 elements, and Group 10 elements in the wiring 12 is not limited to a specific value. The content may be 1% or more, 3% or more, 5% or more, 10% or more, or 20% or more based on the number of atoms. may be 30% or more, 40% or more, or 50% or more.
- the magnetic thermoelectric converter 11 is not limited to a specific material.
- the magneto-thermoelectric converter 11 generates an electromotive force by the magneto-thermoelectric effect.
- the magneto-thermoelectric effect is, for example, the anomalous Nernst effect or the spin Seebeck effect.
- the magneto-thermoelectric converter 11 contains, for example, a material exhibiting the anomalous Nernst effect. Substances exhibiting the anomalous Nernst effect are not limited to specific substances. A material exhibiting the anomalous Nernst effect is, for example, a magnetic material having a saturation magnetic susceptibility of 5 ⁇ 10 ⁇ 3 T or more or a material having a band structure having a Weyl point near the Fermi energy.
- the magneto-thermoelectric converter 11 includes at least one substance selected from the group consisting of the following (i), (ii), (iii), (iv), and (v) as the substance exhibiting the anomalous Nernst effect. contains.
- a stoichiometric substance having a composition represented by Fe 3 X (ii) an off-stoichiometric substance in which the composition ratio of Fe and X deviates from the substance (i) above (iii) the above ( A substance (iv) Fe 3 M1 1-x M2 x (iv) in which a part of the Fe site of the substance i) or part of the Fe site of the substance (ii) is replaced with a typical metal element other than X or a transition element (v) a substance having a composition represented by 0 ⁇ x ⁇ 1), wherein M1 and M2 are different representative elements; , a substance in which a part of the X site of the substance (i) above is replaced with a main group metal element other than X
- X is a typical element or a transition element.
- X is, for example, Al, Ga, Ge, Sn, Si, Ti, Zr, Hf, V, Nb, Ta, Cr, Mo, W, Sc, Ni, Mn, or Co.
- the combination of M1 and M2 is not limited to a specific combination as long as M1 and M2 are representative elements different from each other.
- the combination of M1 and M2 is Ga and Al, Si and Al, or Ga and B, for example.
- the magneto-thermoelectric converter 11 may contain Co 2 MnGa as a substance exhibiting the anomalous Nernst effect, and may contain Mn 3 Sn, which is an antiferromagnetic substance.
- the magneto-thermoelectric converter 11 may be an alloy containing Fe and having a body-centered cubic crystal structure. In this case, the magneto-thermoelectric converter 11 tends to generate a large electromotive force based on the anomalous Nernst effect.
- the magneto-thermoelectric converter 11 is an alloy containing Fe and having a body-centered cubic lattice crystal structure
- the content of Fe and the content of elements other than Fe in the alloy are not limited to specific values.
- the content of Fe in the alloy is, for example, 50% or more based on the number of atoms
- the content of elements other than Fe in the alloy is, for example, 10% or more based on the number of atoms.
- the magneto-thermoelectric converter 11 tends to generate a large electromotive force based on the anomalous Nernst effect.
- the content of Fe in the above alloy may be 55% or more, 60% or more, 65% or more, or 70% or more, based on the number of atoms. .
- the content of Fe in the above alloy is 90% or less, may be 85% or less, or may be 80% or less, based on the number of atoms.
- the content of elements other than Fe in the above alloy may be 15% or more, or 20% or more, based on the number of atoms.
- the content of elements other than Fe in the above alloy is 50% or less, may be 40% or less, or may be 30% or less, based on the number of atoms.
- the magnetic thermoelectric coefficient S NE of the magnetic thermoelectric converter 11 is not limited to a specific value.
- the absolute value of the magnetic thermoelectric coefficient S NE of the magnetic thermoelectric converter 11 is, for example, 0.5 ⁇ V/K or more. As a result, a large electromotive force is likely to be generated by the magnetic thermoelectric conversion in the magnetic thermoelectric converter 11, and the accuracy of sensing using the thermoelectric conversion element 1a is likely to be improved. Therefore, minute heat is easily detected.
- the absolute value of the magnetic thermoelectric coefficient S NE of the magnetic thermoelectric converter 11 is preferably 1.0 ⁇ V/K or more, more preferably 1.5 ⁇ V/K or more, and still more preferably 2.0 ⁇ V/K or more. .
- the absolute value of the magnetic thermoelectric coefficient S NE of the magnetic thermoelectric converter 11 may be 3.0 ⁇ V/K or more, 4.0 ⁇ V/K or more, or 5.0 ⁇ V/K or more. It may be 6.0 ⁇ V/K or more, 7.0 ⁇ V/K or more, or 8.0 ⁇ V/K or more.
- the magnetic thermoelectric converter 11 has a plurality of first thin wires 11a.
- the wiring 12 has a plurality of second thin wires 12a.
- the thermoelectric conversion element 1a the plurality of first fine wires 11a and the plurality of second fine wires 12a are electrically connected in series. According to such a configuration, the electromotive forces accompanying the magnetic thermoelectric conversion generated in the plurality of first fine wires 11a are synthesized, and a large output can be easily obtained from the thermoelectric conversion element 1a.
- thermoelectric conversion element 1a the plurality of first thin wires 11a and the plurality of second thin wires 12a form, for example, a plurality of thin wire pairs 15.
- Each thin line pair 15 consists of a first thin line 11a and a second thin line 12a.
- each thin wire pair 15 consists of one first thin wire 11a and one second thin wire 12a.
- the number of thin wire pairs 15 in thermoelectric conversion element 1a is not limited to a specific value.
- the plurality of first fine wires 11a and the plurality of second fine wires 12a form 50 or more fine wire pairs 15, for example.
- the electromotive force due to the Seebeck effect increases as the number of pairs of joined dissimilar materials increases.
- thermoelectric conversion element 1a the absolute value
- the plurality of first fine lines 11a and the plurality of second fine lines 12a form a meander pattern. According to such a configuration, even if the area of the plane on which the plurality of first fine wires 11a and the plurality of second fine wires 12a are arranged is small, it is easy to obtain a large output from the thermoelectric conversion element 1a.
- the plurality of first thin wires 11a are, for example, separated at predetermined intervals in the X-axis direction and arranged parallel to each other.
- the plurality of first thin wires 11a are arranged at regular intervals in the X-axis direction.
- the plurality of second thin wires 12a electrically connect, for example, first thin wires 11a adjacent to each other in the X-axis direction.
- the second thin line 12a electrically connects, for example, one end of the first thin line 11a in the Y-axis direction and the other end in the Y-axis direction of another first thin line 11a adjacent to the first thin line 11a. ing.
- One end of the plurality of first fine lines 11a in the Y-axis direction is located at the end of the first fine line 11a on the same side in the Y-axis direction, and the other end of the plurality of first fine lines 11a in the Y-axis direction is located at , at the end opposite to the one end in the Y-axis direction of the first thin wire 11a.
- the thickness of the first fine wire 11a is not limited to a specific value.
- the first thin wire 11a has a thickness of 1000 nm or less, for example. This makes it possible to reduce the amount of material used for forming the magnetic thermoelectric converter in the thermoelectric conversion element 1a, thereby easily reducing the manufacturing cost of the thermoelectric conversion element 1a. In addition, disconnection of the conductive paths formed by the plurality of first fine wires 11a and the plurality of second fine wires 12a in the thermoelectric conversion element 1a is less likely to occur.
- the thickness of the first fine wire 11a may be 750 nm or less, 500 nm or less, 400 nm or less, 300 nm or less, or 200 nm or less.
- the thickness of the first thin wire 11a is, for example, 5 nm or more. This makes it easy for the thermoelectric conversion element 1a to exhibit high durability.
- the thickness of the first thin wire 11a may be 10 nm or more, 20 nm or more, 30 nm or more, or 50 nm or more.
- the width which is the dimension of the first thin wire 11a in the X-axis direction, is not limited to a specific value.
- the width of the first thin wire 11a is, for example, 500 ⁇ m or less. This makes it possible to reduce the amount of material used for forming the magnetic thermoelectric converter in the thermoelectric conversion element 1a, thereby easily reducing the manufacturing cost of the thermoelectric conversion element 1a. In addition, it is easy to arrange a large number of first thin wires 11a in the X-axis direction, and the electromotive force generated by magneto-thermoelectric conversion in the thermoelectric conversion element 1a tends to increase.
- the width of the first thin wire 11a may be 400 ⁇ m or less, 300 ⁇ m or less, 200 ⁇ m or less, 100 ⁇ m or less, or 50 ⁇ m or less.
- the width of the first thin wire 11a is, for example, 0.1 ⁇ m or more.
- the width of the first fine line 11a may be 0.5 ⁇ m or more, 1 ⁇ m or more, 2 ⁇ m or more, 5 ⁇ m or more, or 10 ⁇ m or more, It may be 20 ⁇ m or more, or may be 30 ⁇ m or more.
- the thickness of the second fine wire 12a is not limited to a specific value.
- the thickness of the second thin wire 12a is, for example, 1000 nm or less.
- the thickness of the second thin wire 12a may be 750 nm or less, 500 nm or less, 400 nm or less, 300 nm or less, 200 nm or less, or 100 nm or less. may be
- the thickness of the second fine wire 12a is, for example, 5 nm or more. This makes it easy for the thermoelectric conversion element 1a to exhibit high durability.
- the thickness of the second thin wire 12a may be 10 nm or more, 20 nm or more, 30 nm or more, or 50 nm or more.
- the width which is the maximum dimension in the X-axis direction of the second thin wire 12a, is not limited to a specific value.
- the width of the second fine line 12a is, for example, 500 ⁇ m or less.
- the amount of material used for forming the wiring 12 in the thermoelectric conversion element 1a can be reduced, and the manufacturing cost of the thermoelectric conversion element 1a can be easily reduced.
- the width of the second thin wire 12a may be 400 ⁇ m or less, 300 ⁇ m or less, 200 ⁇ m or less, 100 ⁇ m or less, or 50 ⁇ m or less.
- the width of the second fine line 12a is, for example, 0.1 ⁇ m or more. As a result, disconnection of the conductive path is less likely to occur in the thermoelectric conversion element 1a, and the thermoelectric conversion element 1a tends to exhibit high durability.
- the width of the second fine line 12a may be 0.5 ⁇ m or more, 1 ⁇ m or more, 2 ⁇ m or more, 5 ⁇ m or more, or 10 ⁇ m or more, It may be 20 ⁇ m or more, or may be 30 ⁇ m or more.
- thermoelectric conversion element 1a further includes a substrate 20 as shown in FIG.
- the magneto-thermoelectric converter 11 and the wiring 12 are arranged on the substrate 20 .
- the material forming the base material 20 is not limited to a specific material.
- the base material 20 does not contain MgO in the surface layer, for example. As a result, it is not necessary to add MgO to the surface layer of the base material 20, so the production of the thermoelectric conversion element 1a is less complicated, and acid resistance is easily obtained.
- the base material 20 has flexibility, for example. In this case, the shape of the object to which the thermoelectric conversion element 1a can be attached is less likely to be restricted.
- the substrate 20 contains at least an organic polymer, for example. Thereby, it is easy to reduce the manufacturing cost of the thermoelectric conversion element 1a.
- organic polymers are polyethylene terephthalate (PET), polyethylene naphthalate (PEN), acrylic resin (PMMA), polycarbonate (PC), polyimide (PI) or cycloolefin polymer (COP).
- Substrate 20 may be ultra-thin glass.
- An example of ultra-thin glass is G-Leaf (registered trademark) manufactured by Nippon Electric Glass Co., Ltd.
- thermoelectric conversion element 1a An example of a method for manufacturing the thermoelectric conversion element 1a will be described.
- a precursor of the magnetic thermoelectric converter 11 is applied to one main surface of the base material 20 by a method such as sputtering, chemical vapor deposition (CVD), pulsed laser deposition (PLD), ion plating, and plating.
- CVD chemical vapor deposition
- PLD pulsed laser deposition
- ion plating ion plating
- a thin film of a precursor of the wiring 12 is formed on one main surface of the substrate 20 by sputtering, CVD, PLD, ion plating, plating, or the like.
- a photoresist is applied on the thin film of the precursor of the wiring 12, a photomask is placed on the thin film of the precursor of the wiring 12, exposure is performed, and then wet etching is performed.
- the wiring 12 is obtained, and the linear patterns of the precursor of the magnetic thermoelectric converter 11 are electrically connected to each other.
- the magnetic thermoelectric converter 11 is formed by magnetizing the precursor of the magnetic thermoelectric converter 11 .
- the thermoelectric conversion element 1a is obtained.
- the precursor of wiring 12 may be magnetized to form wiring 12 .
- the thermoelectric conversion element 1a may be provided with, for example, an adhesive layer.
- the substrate 20 is arranged between the magnetic thermoelectric converter 11 and the adhesive layer in the thickness direction of the substrate 20 .
- the thermoelectric conversion element 1a can be attached to the article by pressing the adhesive layer against the article.
- the adhesive layer contains, for example, a rubber-based adhesive, an acrylic adhesive, a silicone-based adhesive, or a urethane-based adhesive.
- Thermoelectric conversion element 1a may be provided with an adhesive layer and a release liner.
- the release liner covers the adhesive layer.
- a release liner is typically a film that can retain the adhesive strength of the adhesive layer when covering the adhesive layer and that can be easily peeled from the adhesive layer.
- the release liner is, for example, a film made of polyester resin such as PET. By peeling off the release liner, the adhesive layer is exposed, and the thermoelectric conversion element 1a can be attached to the article.
- thermoelectric conversion element 1a A sensor equipped with the thermoelectric conversion element 1a can be provided.
- this sensor for example, when a temperature gradient occurs in the thickness direction of the base material 20, an electromotive force is generated in the longitudinal direction of the magneto-thermoelectric converter 11 due to the magneto-thermoelectric effect.
- the sensor can sense heat by processing the electric signal output to the outside of the thermoelectric conversion element 1a based on this electromotive force.
- thermoelectric conversion element 1a can be changed from various points of view.
- the thermoelectric conversion element 1a may be changed, for example, into a thermoelectric conversion element 1b shown in FIG. 3 or a thermoelectric conversion element 1c shown in FIG.
- the thermoelectric conversion elements 1b and 1c are constructed in the same manner as the thermoelectric conversion element 1a, except for the parts that are particularly described.
- Components of the thermoelectric conversion elements 1b and 1c that are the same as or correspond to the components of the thermoelectric conversion element 1a are denoted by the same reference numerals, and detailed description thereof will be omitted.
- the description regarding the thermoelectric conversion element 1a also applies to the thermoelectric conversion elements 1b and 1c unless technically contradictory.
- the magnetic thermoelectric conversion body 11 extends continuously on the same plane, for example.
- the wiring 12 is arranged on part of the magneto-thermoelectric converter 11 .
- the plurality of second fine wires 12a are arranged on the magnetic thermoelectric converter 11 at predetermined intervals.
- the magnetic thermoelectric conversion body 11 has, for example, a meander pattern.
- the thermoelectric conversion element 1b is configured such that a single layer of the magnetic thermoelectric conversion body 11 and a laminated body including the magnetic thermoelectric conversion body 11 and the second fine wire 12a appear alternately in the X-axis direction.
- the wiring 12 extends continuously on the same plane, for example.
- the magneto-thermoelectric converter 11 is arranged on part of the wiring 12 .
- the plurality of first thin wires 11a are arranged on the wiring 12 at predetermined intervals from each other. With such a configuration, the thermoelectromotive force associated with the Seebeck effect tends to be small. Moreover, it is easy to reduce the manufacturing cost.
- the wiring 12 forms, for example, a meander pattern.
- the thermoelectric conversion element 1c is configured such that a single layer of the wiring 12 and a laminated body including the wiring 12 and the first thin wires 11a appear alternately in the X-axis direction.
- thermoelectric conversion element A thermoelectric conversion element according to each example and each comparative example was fixed between a pair of Cu plates having dimensions of 30 mm, 30 mm, and 5 mm using Shin-Etsu Chemical Co., Ltd.'s silicone grease KS609, and the thermoelectric properties were measured. A sample for evaluation was produced. The sample was placed on the cooling plate SCP-125 from AS ONE. A film heater manufactured by Shinwa Kiseki Co., Ltd. was fixed on the upper Cu plate with double-sided tape No. 5000NS manufactured by Nitto Denko. The heater had dimensions of 30 mm square and an electrical resistance of 20 ohms.
- thermoelectric conversion element In the plane of the thermoelectric conversion element according to each example and each comparative example, one longitudinal end of the thermoelectric conversion thin wire and wiring was heated by a heater, and the temperature between both ends of the thermoelectric conversion thin wire and wiring in the longitudinal direction was 1°C. of temperature difference. In this state, the electromotive force Vs associated with the Seebeck effect was measured. In this measurement, the temperature of both surfaces of the thermoelectric conversion element was kept constant so as not to generate a temperature gradient in the thickness direction of the thermoelectric conversion element except at one end in the longitudinal direction of the thermoelectric conversion fine wire and wiring. Table 1 shows the results.
- PET polyethylene terephthalate
- a CuNi thin film having a thickness of 100 nm was formed by DC magnetron sputtering using a target material containing Cu and Ni.
- the atomic ratio of Cu content:Ni content was 95:5.
- a photoresist was applied on the CuNi thin film, a photomask was placed on the CuNi thin film, exposure was performed, and then wet etching was performed. Thereby, a wiring having a width of 40 ⁇ m was formed.
- a plurality of thin wires for magnetic thermoelectric conversion were electrically connected in series.
- the plurality of thin wires for magneto-thermoelectric conversion and this wiring formed a meander pattern.
- thermoelectric conversion element according to Example 1 was obtained by magnetizing the thin wire for magnetic thermoelectric conversion in a direction parallel to the plane of the PET film and perpendicular to the longitudinal direction of the thin wire for magnetic thermoelectric conversion. This thermoelectric conversion element generated an electromotive force based on the anomalous Nernst effect.
- thermoelectric conversion element according to Example 5 was produced in the same manner as in Example 1, except that the wiring was formed using Ni as a target material.
- a thermoelectric conversion element according to Example 12 was produced in the same manner as in Example 1 except for the above.
- a thermoelectric conversion element according to Example 13 was produced in the same manner as in Example 1 except for the above.
- thermoelectric conversion element according to Comparative Example 1 was produced in the same manner as in Example 1, except that the wiring was formed using Cu as a target material.
- thermoelectric conversion element according to Comparative Example 2 was produced in the same manner as in Example 1, except that a thin wire for thermoelectric conversion was formed using a target material containing Fe and Pt, and wiring was formed using Cr as a target material. .
- This thermoelectric conversion element generated an electromotive force based on the anomalous Nernst effect.
- thermoelectric conversion element according to Comparative Example 3 was produced in the same manner as in Example 1, except that the wiring was formed using Au as a target material.
- thermoelectric conversion element according to Comparative Example 4 was fabricated in the same manner as in Example 1, except that a Co 2 MnGa target was used instead of the target material containing Fe and Ga, and the wiring was formed using Au as the target material. made.
- the Seebeck electromotive force Vs in the thermoelectric conversion element according to each example was lower than the Seebeck electromotive force Vs in the thermoelectric conversion element according to each comparative example. Since the absolute value of the difference between the Seebeck coefficient Sm in the longitudinal direction of the thin wire for magnetic thermoelectric conversion and the Seebeck coefficient Sc in the longitudinal direction of the wiring is 10 ⁇ V/K or less, the Seebeck electromotive force Vs can be reduced, and the thickness direction of the thermoelectric conversion element can be reduced. It is understood to be advantageous from the point of view of increasing the accuracy of the measurement of the temperature difference in .
- a first aspect of the present invention is a linearly extending magnetic thermoelectric conversion body; and a wiring electrically connected to the magnetic thermoelectric conversion body,
- the absolute value of the difference between the Seebeck coefficient Sm in the longitudinal direction of the magnetic thermoelectric converter and the Seebeck coefficient Sc in the longitudinal direction of the wiring is 10 ⁇ V/K or less.
- a thermoelectric conversion element is provided.
- a second aspect of the present invention is The absolute value of the Seebeck coefficient Sm is 10 ⁇ V / K or more, A thermoelectric conversion element according to the first aspect is provided.
- a third aspect of the present invention is The Seebeck coefficient Sm and the Seebeck coefficient Sc have values of the same sign, A thermoelectric conversion element according to the first aspect or the second aspect is provided.
- a fourth aspect of the present invention is The Seebeck coefficient Sc has a value of 0 or less, A thermoelectric conversion element according to any one of the first side to the third side is provided.
- a fifth aspect of the present invention is The wiring has a specific resistance of 8 to 200 ⁇ cm, A thermoelectric conversion element according to any one of the first side to the fourth side is provided.
- a sixth aspect of the present invention is the wiring contains at least one metal selected from the group consisting of Cu, Ag, Au, Al, Ni, and Co;
- the content of the metal in the wiring is 50% or more based on the number of atoms,
- a thermoelectric conversion element according to any one of the first side to the fifth side is provided.
- a seventh aspect of the present invention is The wiring includes at least one metal selected from the group consisting of Cu, Ag, Au, and Al, and at least one metal selected from the group consisting of Group 8 elements, Group 9 elements, and Group 10 elements. including elements and A thermoelectric conversion element according to any one of the first side to the sixth side is provided.
- the eighth aspect of the present invention is
- the magneto-thermoelectric converter is an alloy containing Fe and having a body-centered cubic lattice crystal structure, A thermoelectric conversion element according to any one of the first side to the seventh side is provided.
- a ninth aspect of the present invention is The content of Fe in the alloy is 50% or more based on the number of atoms, The content of elements other than Fe in the alloy is 10% or more based on the number of atoms.
- a thermoelectric conversion element according to the eighth aspect is provided.
- a tenth aspect of the present invention is
- the magnetic thermoelectric conversion body has a plurality of first thin wires
- the wiring has a plurality of second thin wires
- the plurality of first thin wires and the plurality of second thin wires are electrically connected in series
- a thermoelectric conversion element according to any one of the first side to the ninth side is provided.
- the eleventh aspect of the present invention is The plurality of first thin wires and the plurality of second thin wires form 50 or more thin wire pairs, Each of the 50 or more thin wire pairs consists of the first thin wire and the second thin wire, A thermoelectric conversion element according to the tenth aspect is provided.
- a twelfth aspect of the present invention is The plurality of first fine lines and the plurality of second fine lines form a meander pattern, A thermoelectric conversion element according to the tenth or eleventh aspect is provided.
- thermoelectric conversion element according to any one of the first to twelfth sides.
Landscapes
- Measuring Temperature Or Quantity Of Heat (AREA)
Abstract
Description
線状に延びる磁気熱電変換体と、
前記磁気熱電変換体に電気的に接続された配線と、を備え、
前記磁気熱電変換体の長手方向におけるゼーベック係数Smと前記配線の長手方向におけるゼーベック係数Scとの差の絶対値は、10μV/K以下である、
熱電変換素子を提供する。
(i)Fe3Xで表される組成を有するストイキオメトリックな物質
(ii)上記(i)の物質からFeとXとの組成比がずれたオフ・ストイキオメトリックな物質
(iii)上記(i)の物質のFeサイトの一部又は上記(ii)の物質のFeサイトの一部がX以外の典型金属元素又は遷移元素で置換された物質
(iv)Fe3M11-xM2x(0<x<1)で表される組成を有し、M1及びM2が互いに異なる典型元素である物質
(v)上記(i)の物質のFeサイトの一部がX以外の遷移元素で置換され、上記(i)の物質のXサイトの一部がX以外の典型金属元素で置換された物質
Quantum Design社製の小型無冷媒型物理特性測定システムPPMS VersaLabを用いて、各実施例及び各比較例に係る熱電変換素子における磁気熱電変換用細線の長手方向における27~37℃のゼーベック係数Smと、配線の長手方向における27~37℃のゼーベック係数Scとを測定し、それらの差の絶対値|ΔS|を決定した。結果を表1に示す。ゼーベック係数Sm及びゼーベック係数Scのそれぞれは、試料の一端に取り付けたヒータによって熱流を発生させたときの試料に取り付けた2つの温度計の間に誘起された起電力及び温度差に基づいて決定した。
Quantum Design社製の小型無冷媒型物理特性測定システムPPMS VersaLabを用いて、各実施例及び各比較例に係る熱電変換素子における磁気熱電変換用細線の27~37℃の磁気熱電係数(ネルンスト係数)を測定した。結果を表1に示す。
30mm、30mm、及び5mmの寸法を有する一対のCu製のプレートの間に、信越化学工業社製のシリコーングリースKS609を用いて各実施例及び各比較例に係る熱電変換素子を固定し、熱電特性評価用のサンプルを作製した。このサンプルを、アズワン社の冷却プレートSCP-125の上に置いた。上方のCu製のプレートの上に、シンワ測定社製のフィルムヒーターを日東電工社製の両面テープNo.5000NSで固定した。このヒータは、30mm平方の寸法及び20Ωの電気抵抗値を有していた。冷却プレートの温度を25℃に保った状態で、フィルムヒーターを10Vの定電圧制御で発熱させ、フィルムヒーターから出力される熱量を0.52W/cm2に調整した。このとき、デジタルマルチメーターを用いて、熱電変換素子において発生する起電力VNを計測し、定常状態における起電力の値を読み取った。結果を表1に示す。
ナプソン社製の非接触式抵抗測定装置 NC-80MAPを用いて日本産業規格JIS Z 2316-1:2014に準拠して、渦電流測定法に従って、各実施例及び各比較例に関し、配線のための薄膜のシート抵抗を測定した。このようにして測定した配線のための薄膜のシート抵抗と配線の厚みとの積を求め、配線の比抵抗を決定した。結果を表1に示す。
各実施例及び各比較例に係る熱電変換素子の面内において熱電変換用細線及び配線の長手方向の一端をヒータで加熱して、熱電変換用細線及び配線の長手方向の両端の間に1℃の温度差を生じさせた。この状態でゼーベック効果に伴う起電力Vsを測定した。この測定において、熱電変換用細線及び配線の長手方向の一端以外において、熱電変換素子の厚み方向に温度勾配が生じないように熱電変換素子の両面の温度を一定に保った。結果を表1に示す。
50μmの厚みを有するポリエチレンテレフタレート(PET)フィルム上に、Fe及びGaを含むターゲット材を用いてDCマグネトロンスパッタリングによって100nmの厚みを有する薄膜を形成した。このターゲット材において、原子数比で、Feの含有量:Gaの含有量=3:1の関係にあった。フォトレジストを薄膜上に塗布し、フォトマスクを薄膜の上に配置して露光を行い、その後ウェットエッチングを行った。これにより、所定の間隔で互いに平行に配置された94本の磁気熱電変換用細線が形成された。各磁気熱電変換用細線の幅は100μmであり、各磁気熱電変換用細線の長さは15mmであった。その後、Cu及びNiを含むターゲット材を用いてDCマグネトロンスパッタリングによって100nmの厚みを有するCuNi薄膜を形成した。このターゲット材において、原子数比で、Cuの含有量:Niの含有量=95:5の関係にあった。フォトレジストをCuNi薄膜上に塗布し、フォトマスクをCuNi薄膜の上に配置して露光を行い、その後ウェットエッチングを行った。これにより、40μmの幅を有する配線が形成された。この配線によって、複数の磁気熱電変換用細線が電気的に直列に接続されていた。また、複数の磁気熱電変換用細線及びこの配線は、メアンダパターンをなしていた。PETフィルムの平面に平行であり、かつ、磁気熱電変換用細線の長手方向と直交する方向に磁気熱電変換用細線を磁化させ、実施例1に係る熱電変換素子を得た。この熱電変換素子は、異常ネルンスト効果に基づいて起電力を発生した。
原子数比でCuの含有量:Niの含有量=93:7の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例2に係る熱電変換素子を作製した。
原子数比でCuの含有量:Niの含有量=87:13の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例3に係る熱電変換素子を作製した。
原子数比でCuの含有量:Niの含有量=79:21の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例4に係る熱電変換素子を作製した。
Niをターゲット材として用いて配線を形成したこと以外は実施例1と同様にして実施例5に係る熱電変換素子を作製した。
原子数比でCuの含有量:Coの含有量=77:23の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例6に係る熱電変換素子を作製した。
原子数比でCuの含有量:Feの含有量=41:59の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例7に係る熱電変換素子を作製した。
原子数比でCuの含有量:Niの含有量=88:12の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例8に係る熱電変換素子を作製した。
原子数比でCuの含有量:Coの含有量=68:32の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例9に係る熱電変換素子を作製した。
原子数比でCuの含有量:Coの含有量=63:37の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例10に係る熱電変換素子を作製した。
原子数比でCuの含有量:Coの含有量=22:78の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例11に係る熱電変換素子を作製した。
Fe及びGaを含むターゲット材の代わりにCo2MnGaのターゲットを用い、かつ、原子数比でCuの含有量:Niの含有量=79:21の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例12に係る熱電変換素子を作製した。
Fe及びGaを含むターゲット材の代わりにMn3Snのターゲットを用い、かつ、原子数比でCuの含有量:Agの含有量=50:50の関係を有するターゲット材を用いて配線を形成したこと以外は実施例1と同様にして実施例13に係る熱電変換素子を作製した。
Cuをターゲット材として用いて配線を形成したこと以外は実施例1と同様にして比較例1に係る熱電変換素子を作製した。
Fe及びPtを含むターゲット材を用いて熱電変換用細線を形成し、Crをターゲット材として用いて配線を形成したこと以外は実施例1と同様にして比較例2に係る熱電変換素子を作製した。この熱電変換素子は、異常ネルンスト効果に基づいて起電力を発生した。
Auをターゲット材として用いて配線を形成したこと以外は実施例1と同様にして比較例3に係る熱電変換素子を作製した。
Fe及びGaを含むターゲット材の代わりにCo2MnGaのターゲットを用い、かつ、Auをターゲット材として用いて配線を形成したこと以外は実施例1と同様にして比較例4に係る熱電変換素子を作製した。
線状に延びる磁気熱電変換体と、
前記磁気熱電変換体に電気的に接続された配線と、を備え、
前記磁気熱電変換体の長手方向におけるゼーベック係数Smと前記配線の長手方向におけるゼーベック係数Scとの差の絶対値は、10μV/K以下である、
熱電変換素子を提供する。
前記ゼーベック係数Smの絶対値は、10μV/K以上である、
第1側面に係る熱電変換素子を提供する。
前記ゼーベック係数Sm及び前記ゼーベック係数Scは、同符号の値を有する、
第1側面又は第2側面に係る熱電変換素子を提供する。
前記ゼーベック係数Scは、0以下の値を有する、
第1側面から第3側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記配線は、8~200μΩ・cmの比抵抗を有する、
第1側面から第4側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記配線は、Cu、Ag、Au、Al、Ni、及びCoからなる群より選択される少なくとも1つの金属を含み、
前記配線における前記金属の含有量は、原子数基準で50%以上である、
第1側面から第5側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記配線は、Cu、Ag、Au、及びAlからなる群より選択される少なくとも1つの金属と、第8族元素、第9族元素、及び第10族元素からなる群より選択される少なくとも1つの元素とを含む、
第1側面から第6側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記磁気熱電変換体は、Feを含有し、かつ、体心立方格子の結晶構造を有する合金である、
第1側面から第7側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記合金におけるFeの含有量は、原子数基準で50%以上であり、
前記合金におけるFe以外の元素の含有量は、原子数基準で10%以上である、
第8側面に係る熱電変換素子を提供する。
前記磁気熱電変換体は、複数の第一細線を有し、
前記配線は、複数の第二細線を有し、
前記複数の第一細線及び前記複数の第二細線は、電気的に直列に接続されている、
第1側面から第9側面のいずれか1つの側面に係る熱電変換素子を提供する。
前記複数の第一細線及び前記複数の第二細線は、50対以上の細線対をなしており、
前記50対以上の細線対のそれぞれは、前記第一細線及び前記第二細線からなる、
第10側面に係る熱電変換素子を提供する。
前記複数の第一細線及び前記複数の第二細線は、メアンダパターンをなしている、
第10側面又は第11側面に係る熱電変換素子を提供する。
第1側面から第12側面のいずれか1つの側面に係る熱電変換素子を備えた、センサを提供する。
Claims (13)
- 線状に延びる磁気熱電変換体と、
前記磁気熱電変換体に電気的に接続された配線と、を備え、
前記磁気熱電変換体の長手方向におけるゼーベック係数Smと前記配線の長手方向におけるゼーベック係数Scとの差の絶対値は、10μV/K以下である、
熱電変換素子。 - 前記ゼーベック係数Smの絶対値は、10μV/K以上である、
請求項1に記載の熱電変換素子。 - 前記ゼーベック係数Sm及び前記ゼーベック係数Scは、同符号の値を有する、
請求項1に記載の熱電変換素子。 - 前記ゼーベック係数Scは、0以下の値を有する、
請求項1に記載の熱電変換素子。 - 前記配線は、8~200μΩ・cmの比抵抗を有する、
請求項1に記載の熱電変換素子。 - 前記配線は、Cu、Ag、Au、Al、Ni、及びCoからなる群より選択される少なくとも1つの金属を含み、
前記配線における前記金属の含有量は、原子数基準で50%以上である、
請求項1に記載の熱電変換素子。 - 前記配線は、Cu、Ag、Au、及びAlからなる群より選択される少なくとも1つの金属と、第8族元素、第9族元素、及び第10族元素からなる群より選択される少なくとも1つの元素とを含む、
請求項1に記載の熱電変換素子。 - 前記磁気熱電変換体は、Feを含有し、かつ、体心立方格子の結晶構造を有する合金である、
請求項1に記載の熱電変換素子。 - 前記合金におけるFeの含有量は、原子数基準で50%以上であり、
前記合金におけるFe以外の元素の含有量は、原子数基準で10%以上である、
請求項8に記載の熱電変換素子。 - 前記磁気熱電変換体は、複数の第一細線を有し、
前記配線は、複数の第二細線を有し、
前記複数の第一細線及び前記複数の第二細線は、電気的に直列に接続されている、
請求項1に記載の熱電変換素子。 - 前記複数の第一細線及び前記複数の第二細線は、50対以上の細線対をなしており、
前記50対以上の細線対のそれぞれは、前記第一細線及び前記第二細線からなる、
請求項10に記載の熱電変換素子。 - 前記複数の第一細線及び前記複数の第二細線は、メアンダパターンをなしている、
請求項10に記載の熱電変換素子。 - 請求項1~12のいずれか1項に記載の熱電変換素子を備えた、センサ。
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