# US 8,785,762 B2 · Self-organising thermoelectric materials

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- Number: US 8,785,762 B2
- Document ID: US8785762B2
- Status: Granted
- Kind: B2
- Application number: 13/259,454
- Filed: 2010-03-23
- Published: 2012-01-05
- Granted: 2014-07-22
- Earliest claimed: 2009-03-24
- Assignees: BASF SE
- Applicants: Frank Haaβ; Jan Dieter König
- Inventors: Frank Haaβ; Jan Dieter König
- Web page: https://patentgrep.com/patent/US8785762B2

## CPC

- C01B 19/007: {Tellurides or selenides of metals (C01B19/002 takes precedence)}
- C01B 17/20: Methods for preparing sulfides or polysulfides, in general (ammonium sulfides or polysulfides C01C; sulfides or polysulfides of metals, other than alkali metals, magnesium, calcium, strontium and barium, see the relevant groups of subclasses C01F or C01G, according to the metal)
- C01B 19/002: {Compounds containing, besides selenium or tellurium, more than one other element, with -O- and -OH not being considered as anions}
- H10N 10/01: Manufacture or treatment
- H10N 10/852: comprising tellurium, selenium or sulfur
- H10N 10/857: comprising compositions changing continuously or discontinuously inside the material
- C01P 2004/80: Particles consisting of a mixture of two or more inorganic phases
- C01P 2006/40: Electric properties
- Y02P 20/129: Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- H10N: ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

In a process for producing thermoelectric materials with a polyphasic structure, in which particles of a first phase with a characteristic length of not more than 10 μm are present in homogeneous dispersion in a second phase, by self-assembly, an a least binary thermoelectric material is melted together with a metal which is not a component of the at least binary thermoelectric material, or a chalcogenide of said metal, and, after mixing, is cooled or bonded by reactive grinding.

## Claims

### Claim 1

A process for producing thermoelectric materials with a polyphasic structure, in which particles of a first phase with a characteristic length, a measure of the mean geometric dimension of the particles within the matrix, of not more than 10 μm are present in homogeneous dispersion in a second phase, so that particles of the first phase are present distributed in the second phase such that the particles of the first phase are not in contact and, in macroscopic terms, there is homogeneous distribution over the entire matrix material, by self-assembly, which comprises melting an at least binary thermoelectric material together with a metal which is not a component of the at least binary thermoelectric material, or a chalcogenide of said metal, and, after mixing, cooling or bonding by means of reactive grinding, and wherein the thermoelectric material and the metal have the general formula (I):
(AIVBVI)1−xMex (I)
where
AIVis Si, Ge, Sn, Pb or a combination thereof,
BVIis S, Se, Te or a combination thereof,
Me is Ta, Nb, Mo, W, Ni, Pd, Pt, Ti, Zr, Hf, Fe, Co or a combination thereof,
1 ppm <x<0.8,
or wherein the thermoelectric material and the metal have the general formula (II)
(CV2BVI3)1−xMex (II)
where
CV is P, As, Sb, Bi or a combination thereof,
BVI is S, Se, Te or a combination thereof,
Me is Ta, Nb, Mo, W, Ni, Pd, Pt, Au, Ag, Cu, Ti, Zr, Hf, V, Cr, Mn, Fe, Ru, Os, Co, Rh, Ir, In, Ga, Al, Zn, Cd, Tl or a combination thereof,
1 ppm<x<0.8,
or wherein the thermoelectric material and the metal chalcogenide have the general formula (III)
(AIVBVI)1−x(MeBVIb)x (III)
where
AIV is Si, Ge, Sn, Pb or a combination thereof,
BVI is S, Se, Te or a combination thereof,
Me is Ta, Nb, Mo, W, Ni, Pd, Pt, Ti, Zr, Hf, Fe, Co or a combination thereof,
1 ppm<x<0.8 and
0<b<3,
or wherein the thermoelectric material and the metal chalcogenide have the general formula (IV)
(CV2BVI3)1−x(MeBVIb)x (IV)
where
CV is P, As, Sb, Bi or a combination thereof,
BVI is S, Se, Te or a combination thereof,
Me is Ta, Nb, Mo, W, Ni, Pd, Pt, Au, Ag, Cu, Ti, Zr, Hf, V, Cr, Mn, Fe, Ru, Os, Co, Rh, Ir, In, Ga, Al, Zn, Cd, Tl or a combination thereof,
1 ppm<x<0.8 and
0<b<3.

### Claim 2 (depends on 1)

The process according to claim 1, wherein the particles of the first phase have a characteristic length of not more than 1 μm.

### Claim 3 (depends on 2)

The process according to claim 2, wherein the particles of the first phase have a characteristic length of not more than 0.1 μm.

### Claim 4 (depends on 1)

The process according to claim 1, wherein the proportion of the metals or metal chalcogenides of the first phase is 5 to 60 atom%, based on the overall thermoelectric material.

### Claim 5 (depends on 1)

The process according to claim 1, wherein the entire thermoelectric material is free of silver.

### Claim 6 (depends on 1)

A thermoelectric material obtainable by a process according to claim 1.

### Claim 7 (depends on 6)

A thermoelectric generator or Peltier arrangement comprising a thermoelectric material according to claim 6.

### Claim 8 (depends on 7)

A heat pump, cooler, refrigerator, (laundry) dryer, generator for utilizing heat sources, generator for converting thermal energy to electrical energy, comprising at least one thermoelectric generator or a Peltier arrangement according to claim 7.