# US 11,309,476 B2 · Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same

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- Number: US 11,309,476 B2
- Document ID: US11309476B2
- Status: Granted
- Kind: B2
- Application number: 16/310,554
- Filed: 2018-03-19
- Published: 2019-10-31
- Granted: 2022-04-19
- Earliest claimed: 2017-05-15
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Yu Ho Min; Min Kyoung Kim; Cheol Hee Park; Kyung Moon Ko; Chee Sung Park; Myung Jin Jung
- Web page: https://patentgrep.com/patent/US11309476B2

## CPC

- H10N 10/852: comprising tellurium, selenium or sulfur
- 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
- C01P 2006/32: Thermal properties
- C01P 2006/40: Electric properties
- H10N: ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS

## Abstract

The present invention relates to a novel chalcogen-containing compound that exhibits excellent phase stability even at a temperature corresponding to the driving temperature of a thermoelectric element, and has a high output factor and thermoelectric figure of merit, a method for preparing the same, and a thermoelectric element including the same.

## Claims

### Claim 1

A chalcogen-containing compound represented by the following Chemical Formula 1:
VxMyPbzSn4-zBi2Se7 [Chemical Formula 1]
wherein, in Chemical Formula 1, V is a vacancy, M is an alkali metal,
x, y, z, and 4−z are mole ratios of V, M, Pb, and, Sn, respectively, x is greater than 0 and less than 1, y is greater than 0 and less than 1, x+y is greater than 0 and equal to or less than 1, z is greater than 0 and equal to or less than 4, and x+y+z is greater than 0 and equal to or less than 5.

### Claim 2 (depends on 1)

The chalcogen-containing compound according to claim 1, wherein M is one or more alkali metals selected from the group consisting of Li, Na, and K.

### Claim 3 (depends on 1)

The chalcogen-containing compound according to claim 1, wherein the compound has a crystal structure of a face-centered cubic lattice structure.

### Claim 4 (depends on 3)

The chalcogen-containing compound according to claim 3, wherein the vacancy (V) is a vacant site excluding the sites filled with Se, Sn, Pb and Bi in the face-centered cubic lattice structure, and M is filled in a part of the vacancy (V).

### Claim 5 (depends on 3)

The chalcogen-containing compound according to claim 3, wherein
the Se fills anion sites of the face-centered cubic lattice structure,
the Sn, the Pb and the Bi fill cation sites of the face-centered cubic lattice structure,
the vacancy (V) is a vacant site of remaining cation sites, excluding the sites filled with Sn, Pb, and Bi, and
the M is filled in a part of the vacancy (V).

### Claim 6 (depends on 3)

The chalcogen-containing compound according to claim 3, wherein the Pb is substituted at the Sn site, in the face-centered cubic lattice structure.

### Claim 7 (depends on 1)

The chalcogen-containing compound according to claim 1, wherein the compound is used as thermoelectric conversion material.

### Claim 8

A method for preparing the chalcogen-containing compound of claim comprising the steps of:
melting a mixture comprising raw materials of Sn, Pb, Bi, Se, and an alkali metal (M);
heat treating the molten mixture;
grinding the heat treated product; and
sintering the ground product.

### Claim 9 (depends on 8)

The method for preparing a chalcogen-containing compound according to claim 8, wherein the melting is performed at a temperature of 750 to 900° C.

### Claim 10 (depends on 8)

The method for preparing a chalcogen-containing compound according to claim 8, wherein the heat treatment is performed at a temperature of 500 to 650° C.

### Claim 11 (depends on 8)

The method for preparing a chalcogen-containing compound according to claim 8, further comprising a step of cooling the product of the heat treatment step to form an ingot, between the heat treatment step and the grinding step.

### Claim 12 (depends on 8)

The method for preparing a chalcogen-containing compound according to claim 8, wherein the sintering step is performed by a spark plasma sintering method.

### Claim 13 (depends on 8)

The method for preparing a chalcogen-containing compound according to claim 8, wherein the sintering step is performed at a temperature of 550 to 700° C. and a pressure of 10 to 130 MPa.

### Claim 14 (depends on 1)

A thermoelectric element comprising the chalcogen-containing compound according to claim 1, as a thermoelectric conversion material.