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Copper-sulfur-based high-performance thermoelectric material and preparation method thereof

A technology of thermoelectricity and raw materials, which is applied in the direction of thermoelectric device node lead-out materials, thermoelectric device manufacturing/processing, etc., can solve the problems of low thermal conductivity value and inability to have thermoelectric performance, and achieve low thermal conductivity and good thermoelectric application prospects , good controllability and repeatability

Active Publication Date: 2014-06-18
SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

[0009] Experimental studies found that the intrinsic Cu 2 S has an extremely low thermal conductivity value, only 0.3-0.4Wm in the test temperature range of 300-800K -1 K -1 , but due to its low carrier concentration, its conductivity value is less than 100Sm when it is close to 650K -1 , that is, because the power factor (PF) is too small, it cannot have excellent thermoelectric performance

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  • Copper-sulfur-based high-performance thermoelectric material and preparation method thereof
  • Copper-sulfur-based high-performance thermoelectric material and preparation method thereof
  • Copper-sulfur-based high-performance thermoelectric material and preparation method thereof

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preparation example Construction

[0049] ●The preparation process of the present invention is realized through vacuum packaging, melting, quenching and annealing processes, figure 1 A process flow diagram for the preparation of this material is shown.

[0050] ●The preparation method of the present invention uses pure elements as initial raw materials, which are respectively simple copper, sublimed sulfur and simple Se / Te. The starting materials were weighed in the stoichiometric ratio (2-x):1-y:y and sealed in quartz tubes.

[0051] ●Vacuum packaging is carried out in an argon atmosphere glove box, using plasma or flame gun packaging, the quartz tube is vacuumed during packaging, and the internal pressure is 1-10000Pa.

[0052] ●The melting process is carried out in a vertical melting furnace. Heat up to 1150°C at a heating rate of 4.5°C / min, melt at a constant temperature for 20 hours, and then quench in an ice-water mixture.

[0053] ●The annealing process is carried out in a tubular annealing furnace. ...

Embodiment 1

[0056] Cu 1.88 S (x=0.02,y=0)

[0057] The elemental raw materials Cu and S were weighed at a molar ratio of 1.98:1, and then packaged in a quartz tube. The temperature was raised to 1150°C at a heating rate of 4.5°C / min, and the raw material was melted at 1150°C for 20 hours, and then quenched in a mixture of ice and water. The block obtained after quenching was ground into powder in an agate mortar, the powder was cold-pressed into a block, packaged in a quartz tube again, and finally put into a tube furnace and annealed at 580°C for 7 days, and then followed Furnace cool to room temperature.

[0058] The product obtained after annealing is ground into powder and subjected to spark plasma sintering (SPS sintering). The sintering temperature is 390-420°C, the pressure is 50 or 65MPa, and the sintering time is 5-10 minutes, and finally a dense bulk material is obtained.

[0059] Such as figure 2 As shown, the resulting Cu 1.98 The measurement of thermoelectric properties...

Embodiment 2

[0061] Cu 1.95 S(x=005,y=0)

[0062] The elemental raw materials Cu and S were weighed at a molar ratio of 1.95:1, and then packaged in a quartz tube. The temperature was raised to 1150°C at a heating rate of 4.5°C / min, and the raw material was melted at 1150°C for 20 hours, and then quenched in a mixture of ice and water. The block obtained after quenching was ground into powder in an agate mortar, the powder was cold-pressed into a block, packaged in a quartz tube again, and finally put into a tube furnace and annealed at 580°C for 7 days, and then followed Furnace cool to room temperature.

[0063] The product obtained after annealing is ground into powder, and subjected to spark plasma sintering at a sintering temperature of 390-420° C., a pressure of 65 MPa, and a sintering time of 5-10 minutes to obtain a dense bulk material.

[0064] Such as image 3 As shown, the resulting Cu 1.95 Measurements of the thermoelectric properties of S bulk materials show that the Seeb...

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Abstract

The invention relates to a copper-sulfur-based high-performance thermoelectric material and a preparation method thereof, and particularly provides a novel p-type thermoelectric compound Cu(2-x)S or Cu2S(1-y)Ay (A is Se or Te) and a preparation method thereof. The compound is composed of Cu-S-(Se / Te), x equals 0.02-0.05, and y equals 0.2-0.4. The material is a semiconductor. Compared with traditional thermoelectric materials, the compound is simple, low in cost of raw materials, high in Seebeck coefficient, low in thermal conductivity, and excellent in thermal property, the thermoelectric figures of merit ZT of some components can reach 1 and above at 800K, and the compound has good thermoelectric application prospects.

Description

technical field [0001] The present invention relates to a copper-sulfur-based high-performance thermoelectric material and a preparation method thereof, specifically, the present invention relates to a novel p-type thermoelectric compound Cu 2-x S 1-y A y (for example, Cu 2-x S and Cu 2 S 1-y A y , where A is Se or Te) and its preparation method, the composition of the p-type thermoelectric compound is Cu 2-x S 1-y (Se / Te) y , where the value of x is 0.02-0.05, and the value of y is 0.2-0.4. [0002] The copper-sulfur-based high-performance thermoelectric material of the present invention is a semiconductor. Compared with traditional thermoelectric materials, this compound has simple composition, low raw material price, high Seebeck coefficient and extremely low thermal conductivity. Excellent performance, some thermoelectric figures of merit ZT can reach 1.0 or above at 800K, which has a good prospect for thermoelectric applications. technical background [0003] ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01L35/16H01L35/34H10N10/852H10N10/01
Inventor 史迅陈立东何颖
Owner SHANGHAI INST OF CERAMIC CHEM & TECH CHINESE ACAD OF SCI
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