Thermoelectric devices and applications for the same

• US 7,851,691 B2
• Filed: 09/28/2007
• Issued: 12/14/2010
• Est. Priority Date: 12/02/2003
• Status: Active Grant

• Current Assignee: Battelle Memorial Institute
• Original Assignee: Battelle Memorial Institute
• Inventors: Olsen, Larry C., Martin, Peter M., DeSteese, John G.
• Primary Examiner(s): BARTON, JEFFREY THOMAS
• Application Number:
  US11/864,595
• Publication Number:
  US 20080173537A1
• Time in Patent Office: 1,173 Days
• Field of Search: 136200-242, 204/192.14, 204/192.15, 204/192.25
• US Class Current: 136/201
• CPC Class Codes: H10N 10/01 Manufacture or treatment
• CPC Class Codes: H10N 10/17 characterised by the structure or configuration of the cell or thermocouple forming the device
• CPC Class Codes: H10N 10/817 the junction being non-separable, e.g. being cemented, sintered or soldered
• CPC Class Codes: H10N 10/852 comprising tellurium, selenium or sulfur

Abstract

High performance thin film thermoelectric couples and methods of making the same are disclosed. Such couples allow fabrication of at least microwatt to watt-level power supply devices operating at voltages greater than one volt even when activated by only small temperature differences.

Claims

1. A method of making a thermoelectric power source comprising:

(a) providing a flexible substrate having an upper surface

(b) forming a thermocouple by

(i) sputter depositing a thin film of p-type material comprising Ge, Ag, Sb, and Te to form at least one thermoelement on the upper surface of the flexible substrate and

(ii) sputter depositing a thin film of an n-type material to form at least one thermoelement positioned on the upper surface of the flexible substrate adjacent the p-type thermoelement; and

(iii) forming an electrically conductive member electrically connecting the first end of the p-type thermoelement in electrical contact with the second end of the n-type thermoelement.

2. The method of claim 1 wherein the p-type thermoelements have L/A ratios greater than about 20 cm⁻

1.

3. The method of claim 1 wherein the sputter depositing of the p-type thermoelement further comprises forming the p-type material to comprise:

Ge from about 0.01 to about 25 atomic percent, Ag from about 0.01 to about 10 atomic percent, Sb from about 0.01 to about 20 atomic percent and Te from about 60 to about 90 atomic percent.

4. The method of claim 1 wherein the n-type thin film comprises (Ag_xPbTe/M)_n wherein M may comprise PbTe, SbTe, Sb₂Te₃, Bi₂Te₃, or mixtures thereof.

5. The method of claim 1 wherein the sputter depositing of the n-type thermoelement further comprises forming the n-type thin film thermoelement composition to comprise Ag from about 0.01 to about 10 atomic percent, Pb from about 35 to about 55 atomic percent and Te from about 40 to about 60 atomic percent.

6. The method of claim 1 wherein the sputter depositing of the n-type thermoelement further comprises forming the n-type material to form a thin film consisting essentially of Ag, Pb and Te.

7. The method of claim 6 further comprising sputter depositing the p-type thermoelements to have a thickness of less than about 0.01 cms.

8. The method of claim 1 wherein the sputter depositing of the p-type thermoelement further comprises forming the p-type material to comprise about 14 atomic percent Ge, about 2 atomic percent Ag, about 6 atomic percent Sb and about 78 atomic percent Te.

9. The method of claim 1 further comprising forming at least about 500 thermocouples on the flexible substrate such that the thermoelectric power source has a power output of at least about 10 μ

W with a voltage of at least about 0.1 volt.

10. The method of claim 1 further comprising sputter depositing the p-type thermoelements to have different widths as compared to the sputter deposited n-type thermoelements.

11. The method of claim 1 wherein two or more p-type thermoelements are positioned and electrically connected in parallel with one another and the parallel positioned p-type thermoelements are electrically connected in series to n-type thermoelements.

12. The method of claim 1 further forming including multiple thermocouples electrically connected in series on the upper surface of the flexible substrate and subsequently winding the flexible substrate into a coiled configuration.

13. The method of claim 1 wherein the thermoelectric power source is formed to have a volume of less than about 10 cm³ and has a power output of at least about 50 μ

W.

14. The method of claim 1 wherein the thermoelectric power source is formed to have a volume of less than about 10 cm³ and provide voltages of greater than about 1.0 volt.

15. The method of claim 1 wherein the thermoelectric power source is formed to produce power at temperature differences of about 20°

C. or less.

16. The method of claim 1 wherein the thermoelectric power source is formed to operate in an environment of from about 400 to about 600°

C.

17. The method of claim 1 further comprising spooling the flexible substrate with the thermoelements sputter deposited thereon to form the thermoelectric power source such that the device is in a coil configuration.

18. A method of forming a thermoelectric power source comprising:

forming at least about 500 thermocouples and electrically connecting the thermocouples to one another on an upper surface of a flexible substrate, the forming of the thermocouples comprising;

sputter depositing thin films of GAST p-type material comprising Ge, Ag, Sb, and Te, thereby forming p-type thermoelements;

sputter depositing thin films of n-type material forming n-type thermoelements alternatingly positioned adjacent the p-type thermoelements; and

forming the thermoelectric power source such that it occupies a volume of less than about 10 cm³ and has a power output of at least about 50 μ

W.

19. The method of claim 18 further comprising spooling the flexible substrate with the thermoelements formed thereon to form the thermoelectric power source.

20. The method of claim 18 wherein the p-type thermoelements have L/A ratios greater than about 20 cm⁻

1.

21. The method of claim 18 wherein the sputter depositing of the p-type thermoelement further comprises forming the p-type material to comprise Ge from about 10 to about 25 atomic percent, Ag from about 0.5 to about 10 atomic percent, Sb from about 1 to about 20 atomic percent and Te from about 60 to about 90 atomic percent.

22. The method of claim 18 wherein the sputter depositing of the n-type thermoelement further comprises forming the n-type thin film thermoelement composition to comprise Ag from about 0.01 to about 10 atomic percent, Pb from about 35 to about 55 atomic percent and Te from about 40 to about 60 atomic percent.

23. The method of claim 18 wherein the sputter depositing of the p-type thermoelement further comprises forming the p-type material to comprise about 14 atomic percent Ge, about 2 atomic percent Ag, about 6 atomic percent Sb and about 78 atomic percent Te.