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Novel germanium telluride based thermo-electric material with high thermo-electric performance and preparation method thereof
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A technology of thermoelectric properties and thermoelectric materials, which is applied in the directions of thermoelectric device junction lead-out materials, chemical instruments and methods, selenium/tellurium compounds, etc. production effect
Active Publication Date: 2021-04-16
TONGJI UNIV
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[0004] Chinese patent ZL201710827678.0 discloses an alloy thermoelectric semiconductor material whose chemical formula is (GeTe) 1-x (PbSe) x , where 0<x≤0.4, which forms a solid solution with the same main group material PbSe, increases cations, and reduces the average size of anions to optimize the carrier concentration, which improves thermoelectric properties such as thermoelectric figure of merit to a certain extent , however, there is still room for improvement in the thermoelectric performance of the material
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[0050] The second technical solution of the present invention provides a method for preparing a novel germanium telluride-based thermoelectric material with high thermoelectric performance as described above, comprising the following steps:
[0051] (1) Vacuum packaging:
[0052] Weigh the elemental raw materials Ge, Cu, Pb, Se and Te according to the stoichiometric ratio, put them into a quartz tube and vacuum seal;
[0056] Reheating the obtained molten ingot to raise the temperature, heat preservation and annealing at a temperature below the melting point, and then water quenching to obtain an annealed ingot;
[0057] (4) Hot pressed samples:
[0058] The obtained annealed ingot is ground into powder, and hot pressed to obtain a disc m...
Embodiment 1
[0071] A novel telluride thermoelectric material, which is expressed as (Ge 1-x Cu 2x Te) 1-y (PbSe) y Alloy (x=0.02, 0≤y≤0.25), its preparation method comprises the following steps:
[0072] (1) Ge, Cu, Pb, Se and Te are used as raw materials of elemental elements with a purity greater than 99.99% (Ge 1-x Cu 2x Te) 1-y (PbSe) y The stoichiometric ratio in the alloy is weighed for batching, and vacuum-packed in a quartz tube, where x=0.02, 0≤y≤0.25, and y is specifically selected as 0.05, 0.08, 0.1, 0.12, 0.15, 0.18, 0.2, 0.22, 0.25;
[0073] (2) Hang the quartz tube containing the raw materials in a vertical high-temperature furnace, slowly raise the temperature to 900-1000°C at a rate of 150-200°C per hour, keep it warm for 8-10 hours, and then quickly quench and cool to obtain the first ingot (i.e. melting ingot); in this step of this embodiment, the temperature is slowly raised to 950° C. at a rate of 200° C. per hour, and kept at 950° C. for 8 hours.
[0074] (3)...
Embodiment 2
[0099] Compared with Example 1, most of them are the same, except that in step (2) of this example, the temperature is slowly raised to 900° C. at a rate of 150° C. per hour and kept for 8 hours.
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Abstract
The invention relates to a novel germaniumtelluride based thermo-electric material with high thermo-electric performance and a preparation method thereof. The chemical expression of the novel germaniumtelluride based thermo-electric material is (Ge<1-x>Cu<2x>Te)<1-y>(PbSe)<y>, wherein x is equal to 0.02, and y is greater than or equal to 0 and less than or equal to 0.25. The preparation method comprises the following steps: taking a metal simple substance as a raw material, proportioning according to a stoichiometric ratio, carrying out vacuum packaging, high-temperature melting, annealing heat treatment and quenching to obtain a cast ingot, grinding the cast ingot into powder, and carrying out vacuum hot pressing to obtain a flaky material, namely the target component: the novel germaniumtelluride based thermo-electric material. Compared with the prior art, the thermo-electric material provided by the invention creates a new record of zT peak value and average zT (the peak value zT reaches 2.5 at 600-800K, and the average zT of the working temperature is greater than 1.5), and is a material with optimal thermo-electric performance in GeTe at present, which is higher than other known p-type thermo-electric materials; through defect regulation and control in GeTe, the optimization of carrier concentration and the reduction of lattice thermal conductivity are realized, and the high thermo-electric performance with record-ability is obtained.
Description
technical field [0001] The invention belongs to the technical field of thermoelectric materials, and relates to a novel germanium telluride-based thermoelectric material with high thermoelectric performance and a preparation method thereof. Background technique [0002] Thermoelectric semiconductor material is a new type of clean energy material based on the Seebeck effect that can directly convert industrial waste heat into electricity with zero emissions and no transmission parts. It is generally considered to be an eco-friendly, sustainable and effective solution to the energy crisis. The current relative conversion efficiency of thermoelectric semiconductor materials is low, which limits the large-scale application of thermoelectric devices. Usually, the intrinsic properties of materials, the dimensionless thermoelectric figure of merit zT, can be used to measure the conversion efficiency of thermoelectric materials, zT=S 2 T / ρκ, where: T is the absolute temperature, S i...
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