US20100155675A1 - Filled Skutterudites for Advanced Thermoelectric Applications - Google Patents
Filled Skutterudites for Advanced Thermoelectric Applications Download PDFInfo
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- US20100155675A1 US20100155675A1 US12/643,130 US64313009A US2010155675A1 US 20100155675 A1 US20100155675 A1 US 20100155675A1 US 64313009 A US64313009 A US 64313009A US 2010155675 A1 US2010155675 A1 US 2010155675A1
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- filled skutterudite
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/80—Constructional details
- H10N10/85—Thermoelectric active materials
- H10N10/851—Thermoelectric active materials comprising inorganic compositions
- H10N10/853—Thermoelectric active materials comprising inorganic compositions comprising arsenic, antimony or bismuth
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- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C1/00—Making non-ferrous alloys
- C22C1/04—Making non-ferrous alloys by powder metallurgy
- C22C1/047—Making non-ferrous alloys by powder metallurgy comprising intermetallic compounds
-
- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/01—Manufacture or treatment
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B1/00—Preliminary treatment of ores or scrap
- C22B1/14—Agglomerating; Briquetting; Binding; Granulating
- C22B1/24—Binding; Briquetting ; Granulating
- C22B1/2413—Binding; Briquetting ; Granulating enduration of pellets
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22B—PRODUCTION AND REFINING OF METALS; PRETREATMENT OF RAW MATERIALS
- C22B59/00—Obtaining rare earth metals
Definitions
- the present invention relates to thermoelectric devices which utilize a thermal gradient to generate electrical power and can be used in heating and cooling applications. More particularly, the present invention relates to filled skutterudites as thermoelectric materials, the fabrication of which includes use of the low-cost mischmetal alloys and mischmetal-transition metal alloys as starting materials.
- thermoelectric (TE) materials Due to an increasing awareness of global energy needs and environmental pollution in recent years, much interest has been devoted to the development and use of thermoelectric (TE) materials for automotive and other applications.
- TE devices are capable of transforming heat directly into electrical energy and also acting as solid state coolers. Through their energy-generating capability, TE devices are capable of enhancing the ability of internal combustion engines to convert fuel into useful power.
- the cooling capability of TE devices can contribute to a resolution of the greenhouse concerns associated with refrigerant use, as well as enable new design concepts for heating and air conditioning and improve the reliability of batteries.
- TE-based waste heat recovery is also applicable to modes of transportation such as diesel-electric locomotives, locomotive diesel engines, automotive diesel engines, diesel-electric hybrid buses, fuel cells, etc.
- ZT dimensionless figure of merit
- S, T, ⁇ , ⁇ total , ⁇ L , and ⁇ e are the Seebeck coefficient, absolute temperature, electrical resistivity, total thermal conductivity, lattice thermal conductivity and electronic thermal conductivity, respectively.
- An effective thermoelectric material should possess a large Seebeck coefficient, a low electrical resistivity and a low total thermal conductivity.
- Binary skutterudites are semiconductors with small band gaps of 18 100 meV, high carrier mobilities, and modest Seebeck coefficients.
- Binary skutterudite compounds crystallize in a body-centered-cubic structure with space group Im3 and have the form MX 3 , where M is Co, Rh or Ir and X is P, As or Sb.
- M is Co, Rh or Ir
- X is P, As or Sb.
- thermal conductivities that are excessively high to compete with state-of-the-art thermoelectric materials. It was found that filled skutterudites have much lower thermal conductivities. Therefore, filled skutterudites are increasingly popular as a thermoelectric material due to their lower thermal conductivities.
- Filled skutterudites can be formed by inserting rare earth guest atoms interstitially into large voids in the crystal structure of binary skutterudites.
- the chemical composition for filled skutterudites can be expressed as G y M 4 X 12 , where G represents a guest atom, typically a rare earth atom, and y is its filling fraction.
- G represents a guest atom, typically a rare earth atom
- y is its filling fraction.
- the lattice thermal conductivities of the rare earth filled skutterudites are significantly reduced over a wide temperature range. This property of filled skutterudites is due to the scattering of heat-carrying low-frequency phonons by the heavy rare earth atoms, which rattle inside the interstitial voids in the skutterudite crystal structure.
- n- and p-type rare earth filled skutterudites have been reported to have superior thermoelectric figure of merit (ZT) values in excess of 1 for temperatures above ⁇ 500 degrees C.
- ZT thermoelectric figure of merit
- the best n-type materials are La—Fe—Co—Sb and Ce—Fe—Co—Sb skutterudites.
- the best p-type materials are Yb—Co—Sb and Ba—Ni—Co—Sb.
- FIG. 1 shows ZT values of recently-discovered filled skutterudites as compared to those of state-of-the-art thermoelectric materials.
- thermoelectric devices The relatively high cost of high-purity starting materials for rare earth filled skutterudites contributes to the overall cost of the fabricated thermoelectric devices. Therefore, filled skutterudites are needed which utilize low-cost starting materials to decrease the overall cost of thermoelectric devices.
- the present invention is generally directed to filled skutterudites which are low-cost and suitable for use as a thermoelectric material.
- mischmetal in addition to a transition metal alloy or both rare earth and transition metal alloys, is used as a starting material for the fabrication of both n-type and p-type filled skutterudites.
- Mischmetal is an alloy of both Ce ( ⁇ 50 wt. %) and La ( ⁇ 50 wt. %).
- the filled skutterudite has a composition of Mm y Co 4 Sb 12 (0 ⁇ y ⁇ 1).
- Use of mischmetal as a starting material for fabrication of the skutterudite provides a low-cost alternative to high-purity rare earth starting materials which characterize conventional skutterudite fabrication processes.
- FIG. 1 is a line graph which compares the thermoelectric figure of merit (ZT) for recently-discovered filled skutterudites with the thermoelectric figure of merit for state-of-the-art thermoelectric materials;
- FIG. 2 illustrates a body-centered cubic crystal structure of a filled skutterudite fabricated according to the present invention
- FIG. 3 is a flow diagram which illustrates sequential process steps carried out in a typical method of fabricating a filled skutterudite according to the present invention.
- a portion of a filled skutterudite according to the present invention is generally indicated by reference numeral 10 .
- the filled skutterudite 10 is shown in the form of a body-centered cubic crystal structure having the composition G y M 4 X 12 , where G represents guest (filling) atoms 12 ; y is the filling fraction of the guest atoms 12 ; M represents transition metal atoms 14 ; and X represents atoms from groups IVA-VIA of the periodic table 16 .
- G represents guest (filling) atoms 12
- y is the filling fraction of the guest atoms 12
- M represents transition metal atoms 14
- X represents atoms from groups IVA-VIA of the periodic table 16 .
- a transition metal atom 14 is enclosed in each X 6 tetrahedron formed by the X atoms 16 .
- the guest atoms 12 are enclosed in the irregular dodecahedral cages formed by the adjacent tetrahedra of
- the X atom sites 16 may be C, Si, Ge, Sn, Pb, N, P, As, Sb, Bi, O, S, Se, Te or Po, or combinations of these atoms.
- the X atoms 16 are P, As or Sb.
- the X atoms 16 are Sb.
- the transition metal atoms 14 may be Mn, Tc, Re, Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag or Au, or combinations of these atoms.
- the transition metal atoms 14 are Co, Rh or Ir.
- the transition metal atoms 14 are Co.
- the guest atoms 12 in the filled skutterudite 10 may be rare earth atoms, Na, K, Ca, Sr, Ba, and combinations of these atoms.
- a source or starting material of the guest atoms 12 is mischmetal (Mm) alloy, which is an alloy of mostly Ce (about 50 wt. %) and La (about 50 wt. %).
- Mm mischmetal
- the mischmetal may be used alone or in combination with a rare earth metal or metals, or with Na, K, Ca, Sr, Ba, and combinations of these metals, as the source or starting material for the guest atoms 12 .
- rare-earth metals include those from the lanthanide series, such as Ce, Pr, Nd, Sm, Eu and Gd, as well as those from the actinides series, such as Th and U.
- the composition of the filled skutterudite 10 is Mm y Co 4 Sb 12 (0 ⁇ y ⁇ 1).
- “rattling” of the guest atoms 12 in the irregular dodecahedral cages formed by the adjacent tetrahedra of X atoms 16 reduces the lattice thermal conductivity of the material while minimally affecting carrier mobility by scattering phonons.
- Use of mischmetal as a source or starting material for the guest atoms 12 reduces the overall cost of the filled skutterudite 10 , since mischmetal is relatively low in cost compared to high-purity rare earth elements which serve as the starting material for the filler or guest atoms in conventional filled skutterudites.
- step 1 An illustrative method of fabricating the filled skutterudite 10 according to the present invention is shown in the flow diagram of FIG. 3 .
- step 2 mischmetal, transition metal and X powders are provided. These powders are available from commercial vendors.
- step 2 a precursor pellet is prepared using the mischmetal and transition metal powders, or the mischmetal and other guest element powders in combination with the transition metal powder, using the proper stoichiometric ratios. This step may be carried out by using an induction furnace process or any other process which is capable of producing high temperatures (typically>1,200 degrees C.) followed by rapid cooling or quenching.
- step 3 the precursor pellet formed in step 2 is mixed with the X powder.
- step 4 the mixture containing the precursor pellet and X powder is sintered. This is followed by annealing of the mixture (step 5 ) at a temperature of typically about 500 ⁇ 1000 degrees C. for at least about 24 hours. Finally, the annealed mixture is hot-pressed into the filled skutterudite material at a pressure of typically at least about 57,200 psi.
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- Engineering & Computer Science (AREA)
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- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Manufacturing & Machinery (AREA)
- Powder Metallurgy (AREA)
Abstract
Description
- This application is a divisional of application Ser. No. 10/979,005, filed Nov. 1, 2004.
- The present invention relates to thermoelectric devices which utilize a thermal gradient to generate electrical power and can be used in heating and cooling applications. More particularly, the present invention relates to filled skutterudites as thermoelectric materials, the fabrication of which includes use of the low-cost mischmetal alloys and mischmetal-transition metal alloys as starting materials.
- Due to an increasing awareness of global energy needs and environmental pollution in recent years, much interest has been devoted to the development and use of thermoelectric (TE) materials for automotive and other applications. TE devices are capable of transforming heat directly into electrical energy and also acting as solid state coolers. Through their energy-generating capability, TE devices are capable of enhancing the ability of internal combustion engines to convert fuel into useful power. The cooling capability of TE devices can contribute to a resolution of the greenhouse concerns associated with refrigerant use, as well as enable new design concepts for heating and air conditioning and improve the reliability of batteries. TE-based waste heat recovery is also applicable to modes of transportation such as diesel-electric locomotives, locomotive diesel engines, automotive diesel engines, diesel-electric hybrid buses, fuel cells, etc.
- The energy conversion efficiency and cooling coefficient of performance (COP) of a TE device are determined by the dimensionless figure of merit, ZT, defined as ZT=S2 T/ρκtotal=S2T/ρ(κL+κe), where S, T, ρ, κtotal, κL, and κe are the Seebeck coefficient, absolute temperature, electrical resistivity, total thermal conductivity, lattice thermal conductivity and electronic thermal conductivity, respectively. The larger the ZT values, the higher the efficiency or the Coefficient of Performance (COP). An effective thermoelectric material should possess a large Seebeck coefficient, a low electrical resistivity and a low total thermal conductivity.
- Binary skutterudites are semiconductors with small band gaps of 18 100 meV, high carrier mobilities, and modest Seebeck coefficients. Binary skutterudite compounds crystallize in a body-centered-cubic structure with space group Im3 and have the form MX3, where M is Co, Rh or Ir and X is P, As or Sb. Despite their excellent electronic properties, binary skutterudites have thermal conductivities that are excessively high to compete with state-of-the-art thermoelectric materials. It was found that filled skutterudites have much lower thermal conductivities. Therefore, filled skutterudites are increasingly popular as a thermoelectric material due to their lower thermal conductivities.
- Filled skutterudites can be formed by inserting rare earth guest atoms interstitially into large voids in the crystal structure of binary skutterudites. The chemical composition for filled skutterudites can be expressed as GyM4X12, where G represents a guest atom, typically a rare earth atom, and y is its filling fraction. Compared to binary skutterudites, the lattice thermal conductivities of the rare earth filled skutterudites are significantly reduced over a wide temperature range. This property of filled skutterudites is due to the scattering of heat-carrying low-frequency phonons by the heavy rare earth atoms, which rattle inside the interstitial voids in the skutterudite crystal structure.
- In recent years, both n- and p-type rare earth filled skutterudites have been reported to have superior thermoelectric figure of merit (ZT) values in excess of 1 for temperatures above ˜500 degrees C. For rare earth filled skutterudites, the best n-type materials are La—Fe—Co—Sb and Ce—Fe—Co—Sb skutterudites. The best p-type materials are Yb—Co—Sb and Ba—Ni—Co—Sb.
FIG. 1 shows ZT values of recently-discovered filled skutterudites as compared to those of state-of-the-art thermoelectric materials. - The relatively high cost of high-purity starting materials for rare earth filled skutterudites contributes to the overall cost of the fabricated thermoelectric devices. Therefore, filled skutterudites are needed which utilize low-cost starting materials to decrease the overall cost of thermoelectric devices.
- The present invention is generally directed to filled skutterudites which are low-cost and suitable for use as a thermoelectric material. According to the invention, mischmetal (Mm), in addition to a transition metal alloy or both rare earth and transition metal alloys, is used as a starting material for the fabrication of both n-type and p-type filled skutterudites. Mischmetal is an alloy of both Ce (˜50 wt. %) and La (˜50 wt. %). In a typical embodiment, the filled skutterudite has a composition of MmyCo4Sb12(0<y≦1). Use of mischmetal as a starting material for fabrication of the skutterudite provides a low-cost alternative to high-purity rare earth starting materials which characterize conventional skutterudite fabrication processes.
- The invention will now be described, by way of example, with reference to the accompanying drawings, in which:
-
FIG. 1 is a line graph which compares the thermoelectric figure of merit (ZT) for recently-discovered filled skutterudites with the thermoelectric figure of merit for state-of-the-art thermoelectric materials; -
FIG. 2 illustrates a body-centered cubic crystal structure of a filled skutterudite fabricated according to the present invention; and -
FIG. 3 is a flow diagram which illustrates sequential process steps carried out in a typical method of fabricating a filled skutterudite according to the present invention. - Referring to
FIG. 2 , a portion of a filled skutterudite according to the present invention is generally indicated byreference numeral 10. The filledskutterudite 10 is shown in the form of a body-centered cubic crystal structure having the composition GyM4X12, where G represents guest (filling)atoms 12; y is the filling fraction of theguest atoms 12; M representstransition metal atoms 14; and X represents atoms from groups IVA-VIA of the periodic table 16. In the filledskutterudite 10, atransition metal atom 14 is enclosed in each X6 tetrahedron formed by theX atoms 16. Theguest atoms 12 are enclosed in the irregular dodecahedral cages formed by the adjacent tetrahedra ofX atoms 16. - In the filled skutterudite 10, the
X atom sites 16 may be C, Si, Ge, Sn, Pb, N, P, As, Sb, Bi, O, S, Se, Te or Po, or combinations of these atoms. Preferably, theX atoms 16 are P, As or Sb. Most preferably, theX atoms 16 are Sb. - The
transition metal atoms 14 may be Mn, Tc, Re, Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Pt, Cu, Ag or Au, or combinations of these atoms. Preferably, thetransition metal atoms 14 are Co, Rh or Ir. Most preferably, thetransition metal atoms 14 are Co. - The
guest atoms 12 in the filledskutterudite 10 may be rare earth atoms, Na, K, Ca, Sr, Ba, and combinations of these atoms. According to the present invention, a source or starting material of theguest atoms 12 is mischmetal (Mm) alloy, which is an alloy of mostly Ce (about 50 wt. %) and La (about 50 wt. %). The mischmetal may be used alone or in combination with a rare earth metal or metals, or with Na, K, Ca, Sr, Ba, and combinations of these metals, as the source or starting material for theguest atoms 12. These rare-earth metals include those from the lanthanide series, such as Ce, Pr, Nd, Sm, Eu and Gd, as well as those from the actinides series, such as Th and U. In a typical embodiment, the composition of the filledskutterudite 10 is MmyCo4Sb12 (0<y≦1). - In the filled skutterudite 10, “rattling” of the
guest atoms 12 in the irregular dodecahedral cages formed by the adjacent tetrahedra ofX atoms 16 reduces the lattice thermal conductivity of the material while minimally affecting carrier mobility by scattering phonons. Use of mischmetal as a source or starting material for theguest atoms 12 reduces the overall cost of the filledskutterudite 10, since mischmetal is relatively low in cost compared to high-purity rare earth elements which serve as the starting material for the filler or guest atoms in conventional filled skutterudites. - An illustrative method of fabricating the filled
skutterudite 10 according to the present invention is shown in the flow diagram ofFIG. 3 . In step 1, mischmetal, transition metal and X powders are provided. These powders are available from commercial vendors. In step 2, a precursor pellet is prepared using the mischmetal and transition metal powders, or the mischmetal and other guest element powders in combination with the transition metal powder, using the proper stoichiometric ratios. This step may be carried out by using an induction furnace process or any other process which is capable of producing high temperatures (typically>1,200 degrees C.) followed by rapid cooling or quenching. Instep 3, the precursor pellet formed in step 2 is mixed with the X powder. Instep 4, the mixture containing the precursor pellet and X powder is sintered. This is followed by annealing of the mixture (step 5) at a temperature of typically about 500˜1000 degrees C. for at least about 24 hours. Finally, the annealed mixture is hot-pressed into the filled skutterudite material at a pressure of typically at least about 57,200 psi. - While the preferred embodiments of the invention have been described above, it will be recognized and understood that various modifications can be made in the invention and the appended claims are intended to cover all such modifications which may fall within the spirit and scope of the invention.
Claims (16)
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US12/643,130 US20100155675A1 (en) | 2004-07-23 | 2009-12-21 | Filled Skutterudites for Advanced Thermoelectric Applications |
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US59087804P | 2004-07-23 | 2004-07-23 | |
US10/979,005 US7648552B2 (en) | 2004-07-23 | 2004-11-01 | Filled skutterudites for advanced thermoelectric applications |
US12/643,130 US20100155675A1 (en) | 2004-07-23 | 2009-12-21 | Filled Skutterudites for Advanced Thermoelectric Applications |
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Cited By (4)
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US8646261B2 (en) | 2010-09-29 | 2014-02-11 | GM Global Technology Operations LLC | Thermoelectric generators incorporating phase-change materials for waste heat recovery from engine exhaust |
US9896763B2 (en) | 2016-05-13 | 2018-02-20 | GM Global Technology Operations LLC | Particle reactor for atomic layer deposition (ALD) and chemical vapor deposition (CVD) processes |
WO2018124660A1 (en) * | 2016-12-28 | 2018-07-05 | 주식회사 엘지화학 | Novel compound semiconductor and use thereof |
US11072530B2 (en) | 2016-12-28 | 2021-07-27 | Lg Chem, Ltd. | Compound semiconductor and use thereof |
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US20100111754A1 (en) * | 2006-07-12 | 2010-05-06 | Gm Global Technology Operations, Inc. | Potassium and Sodium Filled Skutterudites |
GB0724752D0 (en) * | 2007-12-19 | 2008-01-30 | Bari Mazhar A | Method for producing a thermoelectric material |
US20100071741A1 (en) * | 2008-03-14 | 2010-03-25 | Gm Global Technology Operations, Inc. | Thermoelectric material including a filled skutterudite crystal structure |
US20090293930A1 (en) * | 2008-03-14 | 2009-12-03 | Gm Global Technology Operations, Inc.@@Shanghai Institute Of Ceramics, | High efficiency skutterudite type thermoelectric materials and devices |
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- 2004-11-01 US US10/979,005 patent/US7648552B2/en active Active
-
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- 2009-12-21 US US12/643,130 patent/US20100155675A1/en not_active Abandoned
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US5487819A (en) * | 1992-06-26 | 1996-01-30 | Intec Pty Ltd | Production of metals from minerals |
US6069312A (en) * | 1994-01-28 | 2000-05-30 | California Institute Of Technology | Thermoelectric materials with filled skutterudite structure for thermoelectric devices |
US5726381A (en) * | 1994-10-11 | 1998-03-10 | Yamaha Corporation | Amorphous thermoelectric alloys and thermoelectric couple using same |
US7705233B2 (en) * | 2002-08-13 | 2010-04-27 | Showa Denko K.K. | Filled skutterudite-based alloy, production method thereof and thermoelectric conversion device fabricated using the alloy |
Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
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US8646261B2 (en) | 2010-09-29 | 2014-02-11 | GM Global Technology Operations LLC | Thermoelectric generators incorporating phase-change materials for waste heat recovery from engine exhaust |
US9896763B2 (en) | 2016-05-13 | 2018-02-20 | GM Global Technology Operations LLC | Particle reactor for atomic layer deposition (ALD) and chemical vapor deposition (CVD) processes |
WO2018124660A1 (en) * | 2016-12-28 | 2018-07-05 | 주식회사 엘지화학 | Novel compound semiconductor and use thereof |
US11072530B2 (en) | 2016-12-28 | 2021-07-27 | Lg Chem, Ltd. | Compound semiconductor and use thereof |
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US7648552B2 (en) | 2010-01-19 |
US20060016470A1 (en) | 2006-01-26 |
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