P-type skutterudite material and preparation method thereof

A skutterudite and p-type technology, which is applied in the direction of thermoelectric device node lead-out materials, thermoelectric device manufacturing/processing, etc., can solve the problems of material electrical transmission performance deterioration, uniform dispersion of nanoparticles, lack of multi-filling materials, etc. Achieve the effects of theoretical thermoelectric conversion efficiency improvement, power factor improvement, and industrialization prospects

Active Publication Date: 2012-03-14
SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

This method cannot convert CoSb 3 Nanoparticles are uniformly dispersed in the material, but enriched on the grain boundary, which has a significant effect on the deterioration of the electrical transport performance of the material
[0015] According to Johnson et al. (US patent application 5,994,639, 1999-11-30), the thermoelectric properties of skutterudite materials with superlattice metastable structure can be improved, but this typical layered structure is usually only available in two-dimensional Realized in structural materials (such as thin films), it is difficult to prepare in three-dimensional bulk materials
[0016] In summary, so far, in the field of p-type skutterudite materials, not only an effective multi-filler material is lacking, but also a stable composite material is lacking, and materials combining the two and their preparation processes are currently not yet

Method used

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  • P-type skutterudite material and preparation method thereof
  • P-type skutterudite material and preparation method thereof
  • P-type skutterudite material and preparation method thereof

Examples

Experimental program
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Effect test

Embodiment 1

[0102] Example 1: CeFe 4 Sb 12 / 0.2GaSb composite material

[0103] The metal raw materials Ce, Fe, Sb, and Ga are mixed in the glove box according to the molar ratio of 1:4:12.2:0.2, and the raw materials are sealed in a quartz tube with a carbon film on the inner wall, and the vacuum is drawn while using argon plasma The flame is used for packaging, and the quartz tube is filled with a small amount of Ar gas for protection. The mixed raw materials were melted at 1000° C. for 12 hours. Quenching is carried out after melting, the quenching medium is brine, and the quenching speed is about 300°C / s. After quenching, the quartz tube was annealed at 700°C for 120 hours, and the obtained block was ground into fine powder and then subjected to spark plasma sintering. The sintering temperature was 600°C, the holding time was 5 minutes, and the pressure was 50MPa. The field emission SEM pictures show that the second phase (GaSb phase) is well distributed on or within the...

Embodiment 2

[0104] Example 2: Ce 0.45 Nd 0.45 Fe 3 CoSb 12 Material

[0105] The metal raw materials Ce, Nd, Fe, Co, Sb are mixed in the glove box according to the molar ratio of 0.45:0.45:3:1:12, and the raw materials are sealed into the quartz tube with the carbon film evaporated on the inner wall, and the vacuum is drawn It is packaged with an argon plasma flame, and a small amount of Ar gas is filled in the quartz tube for protection. The mixed raw materials were heated to 1100°C at a rate of 3°C per minute and melted for 12 hours. Quenching is carried out after melting, the quenching medium is brine, and the quenching speed is about 300°C / s. The quenched ingot and the quartz tube were annealed at 600°C for 200 hours. The block was ground into fine powder and then spark plasma sintered. The sintering temperature was 600°C, the holding time was 10 minutes, and the pressure was 60MPa. Tests showed that Ce 0.45 Nd 0.45 Fe 3 CoSb 12 Has a ratio of (single) fill...

Embodiment 3

[0106] Example 3: Ce y Fe x co 4-x Sb 12 / 0.1GaSb material

[0107] The metal raw materials Ce, Fe, Co, Sb, and Ga are mixed in the glove box according to the molar ratio of 0.6:0.4:3:1:12.1:0.1, and the raw materials are sealed in a quartz tube with a carbon film evaporated on the inner wall. The vacuum side is sealed with an argon plasma flame, and a small amount of Ar gas is filled in the quartz tube for protection. The mixed raw materials were heated to 1050°C at a rate of 1°C per minute and melted for 10 hours. Quenching is carried out after melting, and the quenching medium is brine. The ingot obtained by quenching was annealed at 650°C for 96 hours together with the quartz tube. The block was ground into fine powder and then spark plasma sintered. The sintering temperature was 550°C, the holding time was 20 minutes, and the pressure was 50MPa.

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Abstract

The invention relates to a p-type skutterudite material and a preparation method thereof. The invention provides the p-type skutterudite material which has a chemical formula as represented by IyFe4-xMxSb12 / z(phi), wherein, I is one kind or more kinds of filling atoms in a skutterudite phase, the filling amount y of the filling atoms is no less than 0.01 and no more than 1, M is one kind or more kinds of dopant atoms, the dopant amount x of the dopant atoms is no less than 0 and less than 4, phi is one kind or more kinds of second phases, the molar ratio z of phi is no less than 0 and no morethan 0.5, and second phase sediment disperses in the skutterudite phase. The invention also provides the preparation method for the p-type skutterudite material.

Description

technical field [0001] The invention belongs to the field of p-type skutterudite materials, and provides a p-type skutterudite material with high thermoelectric performance and a preparation method thereof. Background technique [0002] Thermoelectric conversion technology is a technology that uses the Seebeck effect of materials to directly convert heat energy into electrical energy, or uses the Peltier effect of materials for refrigeration. This technology has no moving parts, high reliability, and long life. It can be widely used in waste heat power generation, aerospace power supply, medical and sanitary refrigeration, household refrigeration appliances and other fields. The thermoelectric conversion efficiency mainly depends on the dimensionless thermoelectric performance factor ZT of the material (ZT=S 2 σT / κ, where S is the Seebeck coefficient, σ is the electrical conductivity, κ is the thermal conductivity, and T is the absolute temperature). The higher the ZT valu...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): C22C12/00H01L35/18H01L35/34
CPCC22C12/00C22C30/00H10N10/853B22F3/10
Inventor 陈立东刘睿恒仇鹏飞张文清黄向阳杨炯何琳莫尼卡·拜克浩斯
Owner SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI
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