WO2021187347A1 - 垂直型熱電変換素子、並びにこれを用いた熱電発電応用機器又は熱流センサー - Google Patents

垂直型熱電変換素子、並びにこれを用いた熱電発電応用機器又は熱流センサー Download PDF

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WO2021187347A1
WO2021187347A1 PCT/JP2021/009982 JP2021009982W WO2021187347A1 WO 2021187347 A1 WO2021187347 A1 WO 2021187347A1 JP 2021009982 W JP2021009982 W JP 2021009982W WO 2021187347 A1 WO2021187347 A1 WO 2021187347A1
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thermoelectric
layer
magnetic material
temperature side
conversion element
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French (fr)
Japanese (ja)
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裕弥 桜庭
偉男 周
健一 内田
山本　薫
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National Institute for Materials Science
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National Institute for Materials Science
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Priority to US17/801,061 priority Critical patent/US11889762B2/en
Priority to EP21770787.6A priority patent/EP4123897B1/en
Priority to JP2022508305A priority patent/JP7371980B2/ja
Publication of WO2021187347A1 publication Critical patent/WO2021187347A1/ja
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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
    • H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
    • H10N10/17—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device
    • 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
    • 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
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N52/00—Hall-effect devices
    • H10N52/80—Constructional details

Definitions

  • the present invention relates to a vertical thermoelectric conversion element, and a thermoelectric power generation application device or a heat flow sensor using the vertical thermoelectric conversion element.
  • the anomalous Nernst effect in a magnetic material is a phenomenon in which an electric field is generated in the outer product direction ( ⁇ T ⁇ M) of the magnetization M and the temperature gradient ⁇ T.
  • thermoelectric power (abnormal Nernst coefficient) of the anomalous Nernst effect reported so far for various magnetic materials is 6 ⁇ V / K (Non-Patent Document 1) for Co 2 MnGa Heusler alloy and 2 for FeGa alloy, even if it is large. .1 ⁇ V / K (Non-Patent Document 2), SmCo 5 permanent magnet 3.1 to 3.6 ⁇ V / K (Non-Patent Document 3), and the Seebeck effect thermoelectric power (Seebeck coefficient) of the material used for Seebeck thermoelectric power generation. ) Is about several hundred ⁇ V / K, which is about two orders of magnitude smaller. Regarding thermoelectric materials, for example, they are comprehensively listed in Non-Patent Documents 5 and 6.
  • Non-Patent Document 4 it is required to realize 20 ⁇ V / K.
  • thermoelectric power generation and heat flow sensors For the applications of thermoelectric power generation and heat flow sensors, it has been conventionally aimed to realize thermoelectric power due to a high anomalous Nernst effect as an essential characteristic of a magnetic material alone.
  • the thermoelectric power achieved at present is only about 6 ⁇ V / K at the maximum.
  • the present invention solves the above-mentioned problems, and is a vertical thermoelectric conversion having a novel structure capable of enhancing the thermoelectric ability showing the same symmetry as the anomalous Nernst effect while maintaining the thermoelectric conversion characteristics of the magnetic material. It is an object of the present invention to provide an element. Another object of the present invention is to provide a new thermoelectric power generation application device or a heat flow sensor using a vertical thermoelectric conversion element.
  • the present inventor has proposed a novel structure of a vertical thermoelectric conversion element capable of enhancing the thermoelectric ability showing the same symmetry as the above-mentioned anomalous Nernst effect without substantially improving the thermoelectric conversion characteristics of the magnetic material. To do.
  • the vertical thermoelectric conversion element of the present invention is, for example, as shown in FIGS. 1 and 2, a thermoelectric layer 10 made of a thermoelectric material exhibiting a Seebeck effect, and one end of the thermoelectric layer 10 is on the low temperature side.
  • the other end portion 14 facing the low temperature side end portion 12 is the thermoelectric layer 10 on the high temperature side; the magnetic material layer 20 laminated on the thermoelectric layer 10 in the thickness direction of the magnetic material layer 20.
  • a magnetic material layer 20 that is conductive when magnetized or an external magnetic field is applied and generates a potential in the temperature gradient direction of the magnetic material layer 20 and the outer product direction in the magnetization direction; with the low temperature side end portion 12 of the thermoelectric layer 10.
  • the low temperature side conductor portion 44 connecting the low temperature side end portion 22 of the magnetic material layer 20; the high temperature side conductor portion 42 connecting the high temperature side end portion 14 of the thermoelectric layer 10 and the high temperature side end portion 24 of the magnetic material layer 20; Further, potentials generated in the outer product direction provided at both ends of the magnetic material layer 20 in the outer product direction, which are the outer product directions of the temperature gradient direction ( ⁇ T) of the thermoelectric layer 10 and the magnetization direction (M) of the magnetic material layer 20. It is provided with output terminals (26a, 26b); for taking out.
  • an electrically insulating layer 30 having thermal conductivity which is provided between the thermoelectric layer 10 and the magnetic material layer 20 in the stacking direction, is preferably further provided. It is good to have.
  • the electrically insulating layer 30 having thermal conductivity is made of an oxide selected from SiO 2 and Al 2 O 3 or a nitride selected from Al N and BN. It is preferable to include one type or two or more types.
  • the thermoelectric layer 10 is a Bi 2 Te 3 , PbTe, Si, Ge, Fe—Si alloy, Cr—Si alloy, Mg—Si alloy, CoSb 3 alloy. , Fe 2 VAl-based Heusler alloy, and may consist of at least one thermoelectric material selected from the group of thermoelectric material consisting of SrTiO 3, etc..
  • the magnetic material layer 20 is a magnetic material having conductivity, has an abnormal hole angle of 1% or more, and spontaneously magnetizes up to 100 ° C. or more. It is preferable that it is made of a magnetic material having.
  • the magnetic material having an abnormal hole angle of 1% or more and spontaneous magnetization up to 100 ° C. or more is selected from the following groups (A) to (H). It may consist of at least one type of magnetic material.
  • thermoelectric power generation application device or heat flow sensor of the present invention may use the vertical thermoelectric conversion element according to any one of the above [1] to [6].
  • thermoelectric conversion element of the present invention in addition to the anomalous Nernst effect generated by the magnetic material alone, the anomalous Hall effect generated with respect to the Seebeck current is superimposed on the magnetic material forming the magnetic material layer, resulting in a net effect. Since the effect of increasing the abnormal Nernst thermoelectromotive force is generated, high thermoelectric power can be obtained. So to speak, by assisting the Seebeck effect and the abnormal Hall effect, a thermoelectromotive force showing the same symmetry as the abnormal Nernst effect is generated, and a vertical thermoelectric conversion element showing high thermoelectric power can be obtained.
  • thermoelectric conversion element which shows one Example of this invention. It is a model diagram of the Nernst voltage by the Seebeck assist effect. It is a calculation value figure of the Nernst thermoelectromotive force using Co 2 MnGa as an example. It is a block diagram explaining the vertical thermoelectric conversion element which shows one Example of this invention, (A) is the structural perspective view before connection, (B) is a photograph which shows the plane of the vertical thermoelectric conversion element, (C) is The cross-sectional view taken along the line CC of (B) shows a state in which the thermoelectric layer and the magnetic material layer are insulated by the insulating layer.
  • thermoelectric conversion element which shows one Example of this invention
  • A is the structural perspective view after connection
  • B is a photograph which shows the plane of the vertical thermoelectric conversion element
  • C is The cross-sectional view taken along the line CC of (B) shows a state in which the insulating layer is separated by a laser processing machine.
  • It is a structural perspective view which shows the basic structure of the thermoelectric power generation / heat flow sensor using the anomalous Nernst effect which shows one Example of this invention.
  • FIG. 1 is a configuration perspective view of a vertical thermoelectric conversion element showing an embodiment of the present invention.
  • the vertical thermoelectric conversion element of the present invention has a three-layer structure of a thermoelectric layer 10, a magnetic material layer 20, and an electrically insulating layer 30, and also has a high temperature side conductor portion 42, a low temperature side conductor portion 44, and an output terminal. It includes 26a and 26b.
  • E ANE indicates the anomalous Nernst effect voltage
  • E SE indicates the Seebeck effect voltage
  • M indicates the magnetization direction
  • ⁇ T indicates the direction of the temperature gradient from the low temperature side to the high temperature side.
  • the thermoelectric layer 10 is made of a thermoelectric material having a Seebeck effect, one end of the thermoelectric layer 10 is the low temperature side end portion 12, and the other end portion facing the low temperature side end portion 12 is the high temperature side end portion 14.
  • the thermoelectric material having the Seebeck effect for example, Bi 2 Te 3 , PbTe, Si, Ge, FeSi alloy, CrSi alloy, MgSi alloy, CoSb 3 alloy, Fe 2 VAL-based Whistler alloy, SrTIO 3 and the like can be used. can.
  • the known thermoelectric materials are comprehensively listed in Non-Patent Documents 5 and 6, and this description is incorporated as a list of thermoelectric materials.
  • the magnetic material layer 20 is a magnetic material layer 20 laminated on the thermoelectric layer 10, and is conductive while being magnetized or an external magnetic field is applied in the film thickness direction of the magnetic material layer 20, and the magnetic material layer 20. A potential is generated in the outer product direction of the temperature gradient direction ⁇ T and the magnetization direction M.
  • the magnetic material layer 20 is a magnetic material having conductivity, and is preferably made of a magnetic material having an abnormal hole angle of 1% or more. If it is a magnetic material, it exhibits both an abnormal Nernst effect and an abnormal Hall effect, but in order to obtain a large assist effect, it is preferable to select a magnetic material that exhibits a large abnormal Hall effect (abnormal Hall angle).
  • the abnormal hole angle is a parameter indicating how much the current is bent in the lateral direction when a current is passed through the magnetic material.
  • the abnormal hole angle is less than 1%, the potential generated by the outer product direction of the temperature gradient direction ⁇ T and the magnetization direction M of the magnetic material layer 20 is low, which is not preferable as a vertical thermoelectric conversion element.
  • L1 0 type ordered alloy such as FePt, CoPt, FePd, CoPd , FeNi, MnAl, and is MnGa like.
  • the Whisler alloy include Co 2 MnGa and Co 2 MnAl.
  • the D0 22 type ordered alloy include Mn 3 Ga, Mn 2 FeGa, Mn 2 CoGa, and Mn 2 RuGa.
  • Examples of the binary irregular alloy include FeCr, FeAl, FeGa, FeSi, FeTa, FeIr, FePt, FeSn, FeSm, FeTb, CoFeB, CoTb, and NiPt.
  • Examples of the permanent magnet material include SmCo 5 series magnets, Sm 2 Co 17 series magnets, and Nd 2 Fe 14 B series magnets.
  • Examples of the multilayer magnetic material include Co / Pt and Co / Pd.
  • Examples of perovskite-type nitride materials include Mn 4 N and Fe 4 N.
  • Examples of the D0 19 type ordered alloy include Mn 3 Ga, Mn 3 Ge, and Mn 3 Sn.
  • the output terminals 26a and 26b are provided at both ends of the magnetic material layer 20 in the outer product direction, which is the outer product direction of the temperature gradient direction ⁇ T of the thermoelectric layer 10 and the magnetization direction M of the magnetic material layer 20, in the outer product direction. It is an output terminal for taking out the generated potential.
  • the electrical insulating layer 30 is an electrically insulating layer having thermal conductivity between the thermoelectric layer 10 and the magnetic material layer 20 and provided in the stacking direction.
  • the electrically insulating layer for example, one containing one or more kinds of oxides such as SiO 2 , Al 2 O 3 or nitrides such as Al N and BN can be used.
  • the high-temperature side conductor portion 42 connects the high-temperature side end portion 14 of the thermoelectric layer 10 and the high-temperature side end portion 24 of the magnetic material layer 20, and is a metal conductor wire having low electrical resistance such as a copper wire. Can be used.
  • the low-temperature side conductor portion 44 connects the low-temperature side end portion 12 of the thermoelectric layer 10 and the low-temperature side end portion 22 of the magnetic material layer 20, and is a metal conductor wire having low electrical resistance such as a copper wire. Can be used.
  • the thermoelectric layer 10 has substantially the same conductivity as an insulator such as an oxide, the electrical insulating layer 30 may be omitted. In this case, in a structure in which the insulating layer 30 is not placed on the high temperature side and the low temperature side, the high temperature side conductor portion 42 and the low temperature side conductor portion 44 become unnecessary.
  • thermoelectric layer 10 and the magnetic material layer 20 are laminated via an electrically insulating layer 30, and form the thermoelectric layer 10 by the temperature gradient ⁇ T of the low temperature side end portion 12 and the high temperature side end portion 14 of the thermoelectric layer 10. Seebeck thermoelectromotive force E SE by thermoelectric material is generated. Since the magnetic material layer 20 is in thermal contact with the thermoelectric layer 10 via the electrically insulating layer 30, a temperature gradient ⁇ T of the low temperature side end portion 22 and the high temperature side end portion 24 of the magnetic material layer 20 is generated. ing.
  • the magnetic material layer 20 Since the magnetic material layer 20 is magnetized with the film thickness direction as the magnetization direction M due to the application of an external magnetic field in the film thickness direction or the magnetic anisotropy of the magnetic material 20 itself, the magnetic material layer 20 is magnetized by the anomalous Nerunst effect. A potential is generated in the outer product direction of the temperature gradient direction ⁇ T and the magnetization direction M of the layer 20. Further, in the thermoelectric layer 10 and the magnetic material layer 20, the high temperature side end portion 14 of the thermoelectric layer 10 and the high temperature side end portion 24 of the magnetic material layer 20 are connected by the high temperature side conductor portion 42, and the low temperature side conductor portion 44 connects the thermoelectric layer 10 and the magnetic material layer 20.
  • thermoelectric layer 10 Since the low temperature side end portion 12 of the thermoelectric layer 10 and the low temperature side end portion 22 of the magnetic material layer 20 are connected, an electrically closed circuit is formed. Under the temperature gradient, a Seebeck current flows through the magnetic material of the magnetic layer 20 due to the large thermoelectromotive force of the Seebeck thermoelectric material. As a result, in the magnetic layer 20, the Seebeck current drives the anomalous Hall effect.
  • the Seebeck thermoelectric material and the magnetic material that generate a large Seebeck thermoelectromotive force are thermally arranged in parallel, and the Seebeck thermoelectric material and the magnetic material are physically separated in order to be electrically insulated. Or, it has a structure with an insulator in between. From this state, when only the high temperature side and the low temperature side of the Zeebeck thermoelectric material and the magnetic material are electrically connected to form an electrically closed circuit, the magnetic material alone is contained in the magnetic material forming the magnetic material layer.
  • the anomalous Hall effect that occurs with respect to the Seebeck current is superimposed to generate a thermoelectromotive force in the same direction as the anomalous Nernst thermoelectromotive force. ..
  • FIG. 2 is a model diagram of the Nernst voltage due to the Seebeck assist effect.
  • the low temperature side end portion 12 ( TL ) and the high temperature side end portion 14 ( TH ) are located at both ends of the thermoelectric layer 10.
  • L x S is the length (width) of the Seebeck thermoelectric material S in the x-axis direction (width direction).
  • L z S is the length of the Seebeck thermoelectric material S in the z-axis direction (longitudinal direction / Seebeck effect voltage direction).
  • L y S is the length (thickness) of the Seebeck thermoelectric material S in the y-axis direction (film thickness direction).
  • the low temperature side end portion 22 (TL ) and the high temperature side end portion 24 ( TH ) are located at both ends of the member in the direction parallel to the thermoelectric layer 10 of the magnetic material layer 20.
  • l x N is the length (width) of the member in the direction parallel to the thermoelectric layer 10 of the magnetic material N in the x-axis direction (width direction).
  • L z N is the length of the member in the direction parallel to the thermoelectric layer 10 of the magnetic material N in the z-axis direction (longitudinal direction).
  • L y N is the length (thickness) of the magnetic material N in the y-axis direction (film thickness direction / magnetization direction).
  • Voltage output terminals 26a and 26b are located at both ends of the member in the direction orthogonal to the thermoelectric layer 10 of the magnetic material layer 20.
  • L x N is the length (width) of the member in the direction orthogonal to the thermoelectric layer 10 of the magnetic material N in the x-axis direction (width direction / abnormal Nernst effect voltage direction).
  • l z N is the length of the member in the direction orthogonal to the thermoelectric layer 10 of the magnetic material N in the z-axis direction (longitudinal direction).
  • thermoelectric power of the vertical thermoelectric conversion element of the present invention the following formula can be formulated corresponding to the model shown in FIG.
  • the anomalous Hall effect means that the Hall resistivity increases in proportion to the external magnetic field in the normal Hall effect, but a huge Hall resistivity appears in response to the change in magnetization in the ferromagnetic metal.
  • the Hall resistivity ⁇ is expressed by the following equation with respect to the external magnetic field H and the magnetization M.
  • RH is a normal Hall coefficient
  • R AHE is an abnormal Hall coefficient.
  • the abnormal Hall coefficient R AHE is about 10 to 1000 times larger than the normal Hall coefficient RH.
  • S S is the Seebeck coefficient of the Seebeck thermoelectric material S
  • S N is the Seebeck coefficient of the magnetic material N
  • S ANE abnormal Nernst coefficient [rho AHE is anomalous Hall effect factor
  • [rho S is the electrical resistivity of the Seebeck thermoelectric material S
  • ⁇ N is the electrical resistivity of the magnetic material N.
  • E x N is an electric field E in the x-axis direction (film thickness direction / magnetization direction) of the magnetic material N.
  • the second term on the right side of the above equation is the Nernst (Hall) voltage due to Seebeck assist, and the larger the absolute value of the second term on the right side, the greater the assist effect.
  • the abnormal hole resistivity ⁇ AHE in the second term on the right side indicates that the assist effect is large when the abnormal hole resistivity ⁇ AHE is large.
  • the denominator of the second term on the right side Indicates that the assist effect is large when the electric resistivity of the Seebeck thermoelectric material S is small and the film thickness ratio to the magnetic material N is large.
  • Right side S S in a second term the sign of the Seebeck coefficient S S Seebeck thermoelectric material S, if the sign is different signs of the Seebeck coefficient S N of magnetic material N, the assist effect as the absolute value of S S is large It shows that it is big. Also, if S S and S N are the same sign, when the absolute value of S S is greater than twice the absolute value of S N, it represents that assist effect is large and the absolute value of S S is large.
  • the conditions for increasing the assist effect of the Seebeck thermoelectric material S are that the film thickness ratio of the thermoelectric material to the magnetic material is small, the Seebeck electromotive force of the thermoelectric material is large, the electrical resistance is low, and the abnormal hole angle of the magnetic material is large. It turns out that it is a large case.
  • FIG. 3 shows the calculation results in which the physical property parameters when Co 2 MnGa was used as the magnetic material and the n-type Si substrate was used as the thermoelectric material were substituted into this model. Phenomenon calculations show that the smaller the film thickness ratio of Co 2 MnGa to Si, the greater the assist effect and the maximum Nernst electromotive force of 90 ⁇ V / K is realized.
  • a Whistler alloy magnetic thin film Co 2 MnGa was formed on three substrates of n-type doped, p-type doped, and non-doped, and a verification experiment was conducted.
  • a thermally oxidized SiO insulating film having a thickness of 100 nm was formed on the surfaces of all the substrates. Normally, the Co 2 MnGa thin film and the Si substrate are electrically insulated.
  • the next manufacturing process as shown in FIG.
  • the insulating film near the left and right ends of the Co 2 MnGa thin film is removed by a laser, a metal electrode is attached to that portion, and the Co 2 MnGa thin film and the Si substrate are electrically connected at both ends. It was connected to and formed a closed circuit.
  • the Seebeck effect was measured, it was confirmed that in the sample electrically connected to Si, the Seebeck voltage of the Co 2 MnGa thin film changed due to the influence of the Seebeck effect of the substrate.
  • the n-type Si substrate it was about -20 ⁇ V / K without removing the insulating film by a laser, but when a closed circuit was formed, a Seebeck effect of -160 ⁇ V / K appeared.
  • the anomalous Nernst effect is measured, in the sample using the n-type Si substrate, the thermoelectromotive force of the magnetic film alone is about +2.4 ⁇ V / K, but when it is electrically connected to the Si substrate, it is +7.9 ⁇ V / K. It was confirmed that the thermoelectromotive force increased more than 3 times. Although this increase in output is smaller than the prediction by the above model calculation +23.7 ⁇ V / K, it is an experimental result demonstrating the effect of the present invention.
  • FIG. 7 is a configuration perspective view showing an example of a thermoelectric power generation application using the vertical thermoelectric conversion element of the present invention and an application element for a heat flow sensor. As shown in FIG. 7, the series voltage can be amplified by a simple in-plane connection type thermocouple array structure.
  • thermoelectric layer a case where a Si substrate is laminated as a thermoelectric layer, a Co 2 MnGa thin film as a magnetic material layer, and a thermally oxidized SiO insulating film as an insulating layer is laminated, but the present invention is limited to this.
  • a thermoelectric material having a Seebeck effect can be used for the thermoelectric layer
  • a conductive ferromagnetic material can be used for the magnetic material layer
  • an electrically insulating material having thermal conductivity can be used for the insulating layer.
  • the vertical thermoelectric conversion element of the present invention can be used in thermoelectric power generation application equipment and heat flow sensors.

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PCT/JP2021/009982 2020-03-19 2021-03-12 垂直型熱電変換素子、並びにこれを用いた熱電発電応用機器又は熱流センサー Ceased WO2021187347A1 (ja)

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US17/801,061 US11889762B2 (en) 2020-03-19 2021-03-12 Vertical thermoelectric conversion element and device with thermoelectric power generation application or heat flow sensor using same
EP21770787.6A EP4123897B1 (en) 2020-03-19 2021-03-12 Vertical thermoelectric conversion element and device with thermoelectric power generation application or heat flow sensor using same
JP2022508305A JP7371980B2 (ja) 2020-03-19 2021-03-12 垂直型熱電変換素子、並びにこれを用いた熱電発電応用機器又は熱流センサー

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