# US 2019/0375654 A1 · Chalcogen-containing compound, its preparation method and thermoelectric element comprising the same

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- Number: US 2019/0375654 A1
- Document ID: US20190375654A1
- Status: Published application
- Kind: A1
- Application number: 16/463,300
- Filed: 2018-05-11
- Published: 2019-12-12
- Earliest claimed: 2017-06-27
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Min Kyoung KIM; Yu Ho MIN; Cheol Hee PARK; Kyung Moon KO; Chee Sung PARK; Jae Hyun KIM; Myung Jin JUNG
- Web page: https://patentgrep.com/patent/US20190375654A1

## CPC

- C01G 29/006: {Compounds containing bismuth, with or without oxygen or hydrogen, and containing two or more other elements}
- C01B 19/00: Selenium; Tellurium; Compounds thereof (phosphorus compounds C01B25/14)
- H10N 10/851: comprising inorganic compositions
- C01P 2002/30: Three-dimensional structures
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2006/32: Thermal properties
- C01P 2006/40: Electric properties
- C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- 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

## Abstract

A chalcogen-containing compound of the following Chemical Formula 1 which exhibits excellent phase stability at a temperature corresponding to the driving temperature of a thermoelectric element, and also exhibits an excellent thermoelectric performance index (ZT) through an increase in a power factor and a decrease in thermal conductivity, a method for preparing the same, and a thermoelectric element including the same: V1-xMxSn4-yPbyBi2Se7-zTez [Chemical Formula 1] In the above Formula 1, V is a vacancy, M is an alkali metal, x is greater than 0 and less than 1, y is greater than 0 and less than 4, and z is greater than 0 and less than or equal to 1.

## Claims

### Claim 1

A chalcogen-containing compound represented by the following Chemical Formula 1:
V1-xMxSn4-yPbyBi2Se7-zTez [Chemical Formula 1]
wherein, in the above Formula 1, V is a vacancy, M is an alkali metal, x is greater than 0 and less than 1, y is greater than 0 and less than 4, and z is greater than 0 and less than or equal to 1.

### Claim 2 (depends on 1)

The chalcogen-containing compound of claim 1, wherein the M is at least one alkali metal selected from the group consisting of Li, Na, and K.

### Claim 3 (depends on 1)

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

### Claim 4 (depends on 3)

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

### Claim 5 (depends on 3)

The chalcogen-containing compound of claim 3, wherein the Se is filled in an anion site of the face-centered cubic lattice structure, the Sn, Pb, and Bi are filled in a cation site of the face-centered cubic lattice structure, the Pb is substituted by replacing a part of the Sn, the V is a vacant site of the remaining cationic sites excluding the sites filled with Sn, Pb, and Bi, the M is filled in at least a part of the V, and the Te is substituted by replacing a part of the Se.

### Claim 6 (depends on 1)

The chalcogen-containing compound of claim 1, wherein the V, M, Sn, Pb, and Bi are randomly distributed at the site of (x, y, z)=(0, 0, 0), and Se and Te are randomly distributed at the site of (x, y, z)=(0.5, 0.5, 0.5).

### Claim 7 (depends on 1)

The chalcogen-containing compound of claim 1, wherein the x+y+z is greater than 0 and less than or equal to 5.

### Claim 8 (depends on 1)

The chalcogen-containing compound of claim 1, wherein the compound is selected from the group consisting of V0.8Na0.2Sn3.2Pb0.8Bi2Se6.95Te0.05, V0.8Na0.2Sn3.2Pb0.8Bi2Se6.6Te0.4, and V0.8Na0.2Sn3.2Pb0.8Bi2Se6.2Te0.8.

### Claim 9 (depends on 1)

A method for preparing the chalcogen-containing compound of claim 1 comprising the steps of:
mixing raw materials of Sn, Pb, Bi, Se, Te, and an alkali metal (M) and subjecting the mixture to a melting reaction;
heat-treating the resultant product obtained through the melting reaction;
pulverizing the resultant product obtained through the heat treatment; and
sintering the pulverized product.

### Claim 10 (depends on 9)

The method for preparing the chalcogen-containing compound of claim 9, wherein the melting is carried out at a temperature of 700° C. to 800° C.

### Claim 11 (depends on 9)

The method for preparing the chalcogen-containing compound of claim 9, wherein the heat treatment is carried out at a temperature of 550° C. to 640° C.

### Claim 12 (depends on 9)

The method for preparing the chalcogen-containing compound of claim 9, further comprising a step of cooling the result of the heat treatment step to form an ingot between the heat treatment step and the pulverization step.

### Claim 13 (depends on 9)

The method for preparing the chalcogen-containing compound of claim 9, wherein the sintering step is carried out by a spark plasma sintering method.

### Claim 14 (depends on 9)

The method for preparing the chalcogen-containing compound of claim 9, wherein the sintering step is carried out at a temperature of 550° C. to 700° C. under a pressure of 10 MPa to 100 MPa.

### Claim 15 (depends on 1)

A thermoelectric element comprising the chalcogen-containing compound according to claim 1.