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Composite material of skutterudite filling substrate and preparation method thereof

A technology for filling skutterudite and composite materials, which is applied in the direction of cobalt compounds, chemical instruments and methods, and thermoelectric device node lead-out materials, etc. melting point etc.

Inactive Publication Date: 2011-04-27
SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

This method can ensure that Sb with nanometer size is uniformly dispersed in the matrix, but because Sb has a low melting point (~631°C) and high vapor pressure (0.01kPa, 597°C), it is easy to volatilize during use.
And Sb is a metal phase, which will cause the carrier concentration of the composite material to be much higher than the carrier concentration that can make the material obtain the best thermoelectric performance and deteriorate the electrical transport performance of the composite material.
The in-situ composite process can ensure the uniform dispersion of nanoparticles in the matrix, but it is currently difficult to find a suitable component and process to generate a stable nano-second phase in situ
[0012] According to Johnson et al. (US patent application 5,994,639, November 30, 1999), 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 structure Realized in materials (such as thin films), it is difficult to prepare in three-dimensional bulk materials

Method used

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  • Composite material of skutterudite filling substrate and preparation method thereof
  • Composite material of skutterudite filling substrate and preparation method thereof
  • Composite material of skutterudite filling substrate and preparation method thereof

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preparation example Construction

[0116] The preparation method of composite material of the present invention comprises the steps:

[0117] Weighing and packaging I, Co, Sb and Ga, the weighing process is carried out according to the stoichiometric ratio, wherein I is at least one of Yb, Eu, Ce, La, Nd, Ba and Sr,

[0118] obtaining a molten mixture of I, Co, Sb and Ga, wherein I is at least one of Yb, Eu, Ce, La, Nd, Ba and Sr,

[0119] said molten mixture is quenched to form a solid bulk material;

[0120] The solid matrix material is annealed; the annealed solid matrix material is obtained

[0121] The annealed solid matrix material is made into powder;

[0122] The powder is consolidating to form the composite material.

[0123] Specifically, the melting temperature of the molten mixture is 1000-1200°C.

[0124] Specifically, a quenching medium selected from air, water, brine, oil or liquid nitrogen or other quenching methods are used for quenching. Other quenching methods include Melt spinning and t...

Embodiment 1

[0146] The high-purity metal raw materials Yb block, Co block, Sb block, and Ga block are mixed in the glove box according to the molar ratio of 0.26:4:12:0 and 0.26:4:12.2:0.2, respectively, and the raw materials are sealed in the inner wall for evaporation. The carbon-filmed quartz tube is sealed with an argon plasma flame while drawing a vacuum. The packaged quartz tube was heated to 1100°C at a heating rate of 2°C / min and held for 20 hours, then quenched in saturated brine. The quenched ingot and the quartz tube were annealed at 730°C for 240 hours to obtain the composition Yb 0.26 co 4 Sb 12 and Yb 0.26 co 4 Sb 12 / 1.2mol% GaSb bulk. After the block is ground into fine powder, discharge plasma sintering is carried out, the sintering temperature is 600°C, the holding time is 5 minutes, and the pressure is 50MPa. The phase analysis, microstructure and thermoelectric properties of the obtained materials are as follows: Figure 4-9 shown.

Embodiment 2

[0148] The high-purity raw materials Yb block, Co block, Sb block, and Ga block are mixed in a glove box at a molar ratio of 0.26:4:12.3:0.3, and the raw materials are sealed in a quartz tube with a built-in tantalum foil crucible. Encapsulation was performed with an argon plasma flame. The packaged quartz tube was heated to 1200°C at a heating rate of 3°C / min and held for 10 hours, then quenched in saturated brine. The quenched ingot and the quartz tube were annealed at 750°C for 300 hours to obtain a composition of Yb 0.26 co 4 Sb 12 / 1.8mol% GaSb bulk. After the block is ground into fine powder, discharge plasma sintering is carried out, the sintering temperature is 600°C, the holding time is 10 minutes, and the pressure is 60MPa. The maximum ZT value of the obtained composite thermoelectric material is 1.35 (850K).

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Abstract

The invention provides a composite material. The composite material comprises a skutterudite filling substrate shown as the following formula (I): IyCo4Sb12 (1), wherein I is at least one of Yb, Eu, Ce, La, Nd, Ba and Sr, and y is less than 1 and not more than 0.05. The composite material further comprises GaSb particles distributed in the skutterudite filling substrate, wherein the composite material contains 0.05-5 mol% GaSb particles. Compared with the thermoelectric material substrate without compounding a nanometer GaSb phase, the Seebeck coefficient of the composite material is improved to a large extent, the total heat conductivity is slightly reduced, the thermoelectric performance index ZT value is greatly increased in the whole high temperature and low temperature zone range, and the thermoelectric conversion efficiency of the material is greatly improved. The composite material has simple process and favorable industrialization prospect and is easy to control.

Description

technical field [0001] The invention belongs to the field of thermoelectric materials, and in particular relates to a filled skutterudite-based composite material with excellent thermoelectric properties 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 temper...

Claims

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Application Information

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IPC IPC(8): C22C12/00C22C1/04
CPCC01G51/006C01P2002/72H01L35/18C01P2004/80C01P2004/64C01P2006/40C01P2002/52B82Y30/00Y10S977/779Y10S977/784H10N10/853C01G51/00C01G15/00H10N10/854
Inventor 陈立东熊震陈喜红黄向阳张文清何琳
Owner SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI
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