IP Library Granted Patent US 9,231,180
Granted Patent B2
US 9,231,180 · App. 14/050,184 · Granted Jan 5, 2016

Nanostructured silicide composites for thermoelectric applications

Inventors: Jean-Pierre Fleurial (Altadena, CA); Sabah K. Bux (Chino Hills, CA)
Assignee: California Institute of Technology
H01L35/22C01B33/06H01L35/26H01L35/34
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Quick Facts
Patent No.
US 9,231,180
App. No.
14/050,184
Granted
Jan 5, 2016
Kind
B2
Abstract

The present invention provides a method of preparing a nanocomposite thermoelectric material. The method includes heating a reaction mixture of a semiconductor material and a metal complex to a temperature greater than the decomposition temperature of the metal complex. The heating forms metallic inclusions having a size less than about 100 nm that are substantially evenly distributed throughout the semiconductor material forming the nanocomposite thermoelectric material. The present invention also provides a nanocomposite thermoelectric material prepared by this method.

Claims (35)

1. A method of preparing a nanocomposite thermoelectric material comprising:

heating a reaction mixture comprising a semiconductor material and a metal complex to a temperature greater than the decomposition temperature of the metal complex, wherein the semiconductor material comprises Si, wherein the metal complex comprises a transition metal, wherein the heating initiates a reaction between the transition metal and the semiconductor material that forms metallic inclusions having a size less than about 100 nm that are substantially evenly distributed throughout the semiconductor material, and wherein the metallic inclusions comprise a silicide of the formula

M x-1 Si x

wherein

M is the transition metal, and

subscript x is greater than 1,

thereby preparing the nanocomposite thermoelectric material.

2. The method of claim 1 , wherein the semiconductor material is selected from the group consisting of Si, Mg 2 Si and Si 1-y Ge y , wherein subscript y is greater than 0 and less than 1.

3. The method of claim 1 , wherein the metal complex is an organometallic compound.

4. The method of claim 3 , wherein the organometallic compound is selected from the group consisting of ferrocene and tungstencene.

5. The method of claim 1 , wherein subscript x is 2.

6. The method of claim 1 , wherein M is selected from the group consisting of Fe and W.

7. The method of claim 1 , wherein the silicide is selected from the group consisting of FeSi 2 and WSi 2 .

8. The method of claim 1 , wherein the metal complex comprises about 0.1 to 10% (v/v) of the reaction mixture prior to heating.

9. The method of claim 1 , wherein the semiconductor material is in powder form prior to heating, and wherein the temperature is sufficient to sinter the semiconductor material.

10. The method of claim 1 , wherein the method comprises:

preparing the reaction mixture by mixing the semiconductor material comprising Si and the metal complex using a ball milling device for about 1 to 4 hours, wherein the metal complex is selected from the group consisting of ferrocene and tungstencene, wherein the semiconductor material is in powder form, and wherein the metal complex comprises about 0.1 to 10% (v/v) of the reaction mixture; and

heating the reaction mixture using a hot pressing device to a temperature of at least about 1160° C. and at a pressure of at least about 150 MPa, wherein the heating forms the metallic inclusions comprising the silicide having a size less than about 100 nm that are substantially evenly distributed throughout the semiconductor material, wherein the temperature is sufficient to sinter the semiconductor material, wherein if the metal complex is ferrocene, the silicide is FeSi 2 , and wherein if the metal complex is tungstencene, the silicide is WSi 2 , thereby preparing the nanocomposite thermoelectric material.

11. A nanocomposite thermoelectric material comprising:

a semiconductor material comprising Si; and

silicide inclusions of the formula

M x-1 Si x

wherein

M is a transition metal, and

subscript x is greater than 1,

wherein the silicide inclusions have a size less than about 100 nm, wherein the silicide inclusions are substantially evenly distributed within grains of the semiconductor material, and wherein the nanocomposite thermoelectric material has a lattice thermal conductivity of less than about 120 W/mK at a temperature of about 300-1275 K.

12. The nanocomposite thermoelectric material of claim 11 , wherein the semiconductor material is selected from the group consisting of Si, Mg 2 Si and Si 1-y Ge y , wherein subscript y is greater than 0 and less than 1.

13. The nanocomposite thermoelectric material of claim 11 , wherein subscript x is 2.

14. The nanocomposite thermoelectric material of claim 11 , wherein M is selected from the group consisting of Fe and W.

15. The nanocomposite thermoelectric material of claim 11 , wherein the silicide is selected from the group consisting of FeSi 2 and WSi 2 .

16. The nanocomposite thermoelectric material of claim 11 , wherein the silicide inclusions are substantially not located in grain boundaries of the semiconductor material.

17. The nanocomposite thermoelectric material of claim 11 , wherein at least a portion of the silicide inclusions have a size less than about 2 nm.

18. The nanocomposite thermoelectric material of claim 11 , wherein the nanocomposite thermoelectric material comprises:

the semiconductor material comprising Si; and

the silicide inclusions, wherein the silicide inclusions are selected from the group consisting of FeSi 2 and WSi 2 , wherein the silicide inclusions have a size less than about 100 nm, wherein the silicide inclusions are substantially evenly distributed within grains of the semiconductor material, and wherein the nanocomposite thermoelectric material has the lattice thermal conductivity of less than about 120 W/mK at a temperature of about 300-1275 K.

Assignments (2)
CONFIRMATORY LICENSE Recorded Oct 23, 2013
From: CALIFORNIA INSTITUTE OF TECHNOLOGY
To: NASA
Reel/Frame 031541/0736 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded Oct 17, 2013
From: FLEURIAL, JEAN-PIERRE; BUX, SABAH K.
To: CALIFORNIA INSTITUTE OF TECHNOLOGY
Reel/Frame 031429/0562 →
Continuity (2)
Provisional Application 61711387 · Oct 9, 2012
Related Publication 20140097391A1 · Apr 10, 2014