CN102403446A - Thermoelectric material with aluminum element added in PbTe or PbSe - Google Patents
Thermoelectric material with aluminum element added in PbTe or PbSe Download PDFInfo
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- CN102403446A CN102403446A CN2011103489092A CN201110348909A CN102403446A CN 102403446 A CN102403446 A CN 102403446A CN 2011103489092 A CN2011103489092 A CN 2011103489092A CN 201110348909 A CN201110348909 A CN 201110348909A CN 102403446 A CN102403446 A CN 102403446A
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- pbte
- pbse
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- OCGWQDWYSQAFTO-UHFFFAOYSA-N tellanylidenelead Chemical compound [Pb]=[Te] OCGWQDWYSQAFTO-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 239000000463 material Substances 0.000 title claims abstract description 21
- 229910002665 PbTe Inorganic materials 0.000 title claims abstract description 19
- YBNMDCCMCLUHBL-UHFFFAOYSA-N (2,5-dioxopyrrolidin-1-yl) 4-pyren-1-ylbutanoate Chemical compound C=1C=C(C2=C34)C=CC3=CC=CC4=CC=C2C=1CCCC(=O)ON1C(=O)CCC1=O YBNMDCCMCLUHBL-UHFFFAOYSA-N 0.000 title claims abstract description 18
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 title abstract description 9
- 229910052782 aluminium Inorganic materials 0.000 claims abstract description 12
- 239000011159 matrix material Substances 0.000 claims abstract description 4
- 229910052738 indium Inorganic materials 0.000 claims description 2
- 239000004411 aluminium Substances 0.000 claims 1
- GGYFMLJDMAMTAB-UHFFFAOYSA-N selanylidenelead Chemical compound [Pb]=[Se] GGYFMLJDMAMTAB-UHFFFAOYSA-N 0.000 abstract description 7
- 239000011573 trace mineral Substances 0.000 abstract description 5
- 235000013619 trace mineral Nutrition 0.000 abstract description 5
- 238000005551 mechanical alloying Methods 0.000 abstract description 3
- 238000002844 melting Methods 0.000 abstract description 3
- 230000008018 melting Effects 0.000 abstract description 3
- 238000000034 method Methods 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 abstract description 3
- 238000010248 power generation Methods 0.000 abstract description 3
- 238000005057 refrigeration Methods 0.000 abstract description 3
- 239000007787 solid Substances 0.000 abstract description 3
- 239000000758 substrate Substances 0.000 abstract description 3
- AZDRQVAHHNSJOQ-UHFFFAOYSA-N alumane Chemical group [AlH3] AZDRQVAHHNSJOQ-UHFFFAOYSA-N 0.000 abstract description 2
- 229910021654 trace metal Inorganic materials 0.000 abstract 1
- 238000007731 hot pressing Methods 0.000 description 4
- 238000003825 pressing Methods 0.000 description 4
- ZCYVEMRRCGMTRW-UHFFFAOYSA-N 7553-56-2 Chemical compound [I] ZCYVEMRRCGMTRW-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 238000000498 ball milling Methods 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 239000011630 iodine Substances 0.000 description 2
- 229910052740 iodine Inorganic materials 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229910052714 tellurium Inorganic materials 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000009529 body temperature measurement Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 125000001309 chloro group Chemical group Cl* 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 238000000713 high-energy ball milling Methods 0.000 description 1
- 229910052745 lead Inorganic materials 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 description 1
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- Powder Metallurgy (AREA)
Abstract
本发明公开了一种在PbTe或PbSe中添加微量元素铝的热电材料，在PbTe或PbSe基体上添加微量金属Al，其组成配方为(摩尔比)：Pb∶Te∶Al＝1∶1∶(0.001-0.05)；Pb∶Se∶Al＝1∶1∶(0.001-0.05)。采用熔融法或机械合金法制备的“在PbTe或PbSe中添加元素铝的热电材料”，是在PbTe(碲化铅)或PbSe(硒化铅)基体上添加元素铝。元素铝在PbTe(碲化铅)或PbSe(硒化铅)中形成共振能级，提高了材料Seebeck系数，从而提高了材料热电优值ZT，在温差发电、固体制冷上将具有潜在的应用价值。The invention discloses a thermoelectric material in which a trace element aluminum is added to PbTe or PbSe, and a trace metal Al is added to a PbTe or PbSe substrate, and its composition formula is (molar ratio): Pb:Te:Al=1:1:( 0.001-0.05); Pb:Se:Al=1:1:(0.001-0.05). The "thermoelectric material with elemental aluminum added to PbTe or PbSe" prepared by melting method or mechanical alloying method is to add elemental aluminum on the PbTe (lead telluride) or PbSe (lead selenide) matrix. Elemental aluminum forms a resonance energy level in PbTe (lead telluride) or PbSe (lead selenide), which improves the Seebeck coefficient of the material, thereby improving the thermoelectric figure of merit ZT of the material, and will have potential application value in thermoelectric power generation and solid refrigeration .
Description
技术领域 technical field
本发明涉及一种在PbTe(碲化铅)或PbSe(硒化铅)中添加元素铝的热电材料，采用熔融或机械合金法制造一种热电材料，属于热电材料技术领域。The invention relates to a thermoelectric material in which elemental aluminum is added to PbTe (lead telluride) or PbSe (lead selenide). The thermoelectric material is manufactured by melting or mechanical alloying, and belongs to the technical field of thermoelectric materials.
背景技术 Background technique
热电材料在温差发电、固体制冷等方面应用前景广阔。热电材料综合性能用其热电优值ZT来衡量，ZT越高，则能量的转换效率越高。PbTe(碲化铅)是著名的中温热电材料，一般通过添加微量元素I(碘)等氯族元素以形成n型导电，其ZT一般在1以下。由于PbTe(碲化铅)中含有昂贵且易挥发的元素Te(碲)，为了降低成本、提高材料化学稳定性，PbSe(硒化铅)越来越受到重视，添加微量元素I(碘)等氯族元素后，其ZT一般在0.8左右。Thermoelectric materials have broad application prospects in thermoelectric power generation and solid refrigeration. The comprehensive performance of thermoelectric materials is measured by its thermoelectric figure of merit ZT, the higher the ZT, the higher the energy conversion efficiency. PbTe (lead telluride) is a well-known medium-temperature thermoelectric material. Generally, trace elements such as I (iodine) and other chlorine elements are added to form n-type conductivity, and its ZT is generally below 1. Since PbTe (lead telluride) contains the expensive and volatile element Te (tellurium), in order to reduce the cost and improve the chemical stability of the material, PbSe (lead selenide) has been paid more and more attention, adding trace elements such as I (iodine) After the chlorine group elements, its ZT is generally around 0.8.
发明内容 Contents of the invention
本发明的目的是提出一种在PbTe(碲化铅)或PbSe(硒化铅)中添加微量元素铝的热电材料。The object of the present invention is to propose a thermoelectric material in which trace element aluminum is added to PbTe (lead telluride) or PbSe (lead selenide).
一种在PbTe或PbSe中添加微量元素铝的热电材料，在PbTe或PbSe基体上添加微量金属Al，其组成配方为(以下为摩尔比)：A thermoelectric material in which a trace element of aluminum is added to PbTe or PbSe, and a trace amount of metal Al is added to a PbTe or PbSe substrate, and its composition formula is (the following is the molar ratio):
Pb∶Te∶Al＝1∶1∶(0.001-0.05)Pb:Te:Al=1:1:(0.001-0.05)
Pb∶Se∶Al＝1∶1∶(0.001-0.05)。Pb:Se:Al=1:1:(0.001-0.05).
所述的热电材料，在PbTe或PbSe基体上添加微量金属Al和In，其组成配方为(以下为摩尔比)：In the thermoelectric material, trace metals Al and In are added on the PbTe or PbSe substrate, and its composition formula is (the following is the molar ratio):
Pb∶Te∶Al∶In＝1∶1∶(0.001-0.05)∶(0.001-0.02)Pb:Te:Al:In=1:1:(0.001-0.05):(0.001-0.02)
Pb∶Se∶Al∶In＝1∶1∶∶(0.001-0.05)∶(0.001-0.02)。Pb:Se:Al:In=1:1::(0.001-0.05):(0.001-0.02).
采用熔融法或机械合金法制备的“在PbTe或PbSe中添加元素铝的热电材料”，是在PbTe(碲化铅)或PbSe(硒化铅)基体上添加元素铝。元素铝在PbTe(碲化铅)或PbSe(硒化铅)中形成共振能级，提高了材料Seebeck系数，从而提高了材料热电优值ZT，在温差发电、固体制冷上将具有潜在的应用价值。The "thermoelectric material with elemental aluminum added to PbTe or PbSe" prepared by melting method or mechanical alloying method is to add elemental aluminum on the PbTe (lead telluride) or PbSe (lead selenide) matrix. Elemental aluminum forms a resonance energy level in PbTe (lead telluride) or PbSe (lead selenide), which improves the Seebeck coefficient of the material, thereby improving the thermoelectric figure of merit ZT of the material, and will have potential application value in thermoelectric power generation and solid refrigeration .
具体实施方式 Detailed ways
以下结合具体实施例，对本发明进行详细说明。The present invention will be described in detail below in conjunction with specific embodiments.
实施例1Example 1
Pb∶Te∶Al＝1∶1∶0.02上述配比为摩尔比，即原子数比。Pb:Te:Al=1:1:0.02 The above ratio is molar ratio, that is, atomic number ratio.
制备方法：高能球磨+快速热压。Preparation method: high-energy ball milling + rapid hot pressing.
原材料为单质Pb，Te和Al，纯度不低于99.99％。球磨机为SPEX 8000M型。在氩气保护的手套箱中，将按上述化学配方配好的原材料与不锈钢磨球按1∶5(质量比)的比例一起放入上述球磨机配套的不锈钢球磨罐中，旋紧罐盖以防止氧气进入球磨罐，球磨时间5小时。快速热压可在直流快速热压机上进行。热压模具由石墨制造而成。模具为圆柱型，外径φ35mm，内径φ12.7mm，高40mm。距模具一端15mm处，从圆柱外表面向柱心钻一直径φ1.5mm、深10mm的盲孔，用于插入测温热电偶。称此端为下端，另一端为上端。上下两个压杆由石墨圆棒构成，直径均为12.7mm，其中一个14mm长，一个30mm长。模具及压杆放入手套箱中。将长14mm的压杆从下端放入模具并直立放置。在手套箱中打开球磨罐，将球磨了5小时的粉末约3克从上端装入模具，并且将另一个长度为30mm的压杆从上端放入模具。将装好粉末的模具取出手套箱，放入直流快速热压机。将测温热电偶从上述小孔插入模具，设置热压机压力为55MPa，热压温度500℃，到温后保温时间1分钟。开启热压机热压样品。热压结束后，待模具温度降至室温后，卸掉压力，取出模具。用顶杆将压杆顶出，即可取出压制好的材料。The raw materials are elemental Pb, Te and Al, and the purity is not less than 99.99%. The ball mill is SPEX 8000M type. In the argon-protected glove box, put the raw materials prepared according to the above chemical formula and the stainless steel grinding balls in the ratio of 1:5 (mass ratio) into the stainless steel ball milling tank supporting the above ball mill, and tighten the tank cover to prevent Oxygen enters the ball mill jar, and the ball milling time is 5 hours. Rapid heat pressing can be carried out on a DC rapid heat press. The hot pressing die is made of graphite. The mold is cylindrical, with an outer diameter of φ35mm, an inner diameter of φ12.7mm, and a height of 40mm. At 15mm from one end of the mold, drill a blind hole with a diameter of φ1.5mm and a depth of 10mm from the outer surface of the cylinder to the center of the cylinder, for inserting a thermocouple for temperature measurement. Call this end the lower end and the other end the upper end. The upper and lower compression rods are made of graphite round rods with a diameter of 12.7mm, one of which is 14mm long and the other 30mm long. The mold and pressure rod are put into the glove box. Put the 14mm long pressing rod into the mold from the lower end and place it upright. Open the ball mill jar in the glove box, put about 3 grams of powder that has been ball-milled for 5 hours into the mold from the upper end, and put another 30mm long pressing rod into the mold from the upper end. Take the powder-loaded mold out of the glove box and put it into a DC rapid hot press. Insert the temperature-measuring thermocouple into the mold from the above-mentioned small hole, set the pressure of the hot press to 55MPa, the hot pressing temperature to 500°C, and hold the temperature for 1 minute after reaching the temperature. Turn on the heat press to heat press the sample. After the hot pressing, after the temperature of the mold drops to room temperature, the pressure is released and the mold is taken out. Use the push rod to push out the pressing rod, and then the pressed material can be taken out.
电阻率和Seebeck系数测试在ULVAC ZEM-3上进行，热导率在NETZSCH LFA-457上进行。ZT＝α2T/(ρκ)。其中，α为Seebeck系数，ρ为电阻率，κ为热导率，T为绝对温度。Resistivity and Seebeck coefficient tests were performed on ULVAC ZEM-3 and thermal conductivity on NETZSCH LFA-457. ZT = α2T/(ρκ). Among them, α is the Seebeck coefficient, ρ is the resistivity, κ is the thermal conductivity, and T is the absolute temperature.
500℃时主要性能如下：The main properties at 500°C are as follows:
电阻率：2.9E-5ΩmResistivity: 2.9E-5Ωm
Seebeck系数：-200μV/KSeebeck coefficient: -200μV/K
热导率：1.36W/mKThermal conductivity: 1.36W/mK
ZT＝1.1ZT=1.1
实施例2Example 2
Pb∶Se∶Al＝1∶1∶0.01，其余同实施例1。Pb:Se:Al=1:1:0.01, and the rest are the same as in Example 1.
575℃时主要性能如下：The main properties at 575°C are as follows:
电阻率：4.27E-5ΩmResistivity: 4.27E-5Ωm
Seebeck系数：-241μV/KSeebeck coefficient: -241μV/K
热导率：0.9W/mKThermal conductivity: 0.9W/mK
ZT＝1.3ZT=1.3
实施例3Example 3
Pb∶Te∶Al∶In＝1∶1∶0.01∶0.005，其余同实施例1。Pb:Te:Al:In=1:1:0.01:0.005, and the rest are the same as in Example 1.
500℃时主要性能如下：The main properties at 500°C are as follows:
电阻率：2.51E-5ΩmResistivity: 2.51E-5Ωm
Seebeck系数：-208μV/KSeebeck coefficient: -208μV/K
热导率：1.12W/mKThermal conductivity: 1.12W/mK
ZT＝1.2ZT=1.2
实施例4Example 4
Pb∶Te∶Al∶In＝1∶1∶0.01∶0.005，其余同实施例1。Pb:Te:Al:In=1:1:0.01:0.005, and the rest are the same as in Example 1.
500℃时主要性能如下：The main properties at 500°C are as follows:
电阻率：2.51E-5ΩmResistivity: 2.51E-5Ωm
Seebeck系数：-208μV/KSeebeck coefficient: -208μV/K
热导率：1.12W/mKThermal conductivity: 1.12W/mK
ZT＝1.2ZT=1.2
实施例4Example 4
Pb∶Se∶Al∶In＝1∶1∶0.01∶0.005，其余同实施例1。Pb:Se:Al:In=1:1:0.01:0.005, and the rest are the same as in Example 1.
575℃时主要性能如下：The main properties at 575°C are as follows:
电阻率：4.76E-5ΩmResistivity: 4.76E-5Ωm
Seebeck系数：-261μV/KSeebeck coefficient: -261μV/K
热导率：0.95W/mKThermal conductivity: 0.95W/mK
ZT＝1.3ZT=1.3
应当理解的是，对本领域普通技术人员来说，可以根据上述说明加以改进或变换，而所有这些改进和变换都应属于本发明所附权利要求的保护范围。It should be understood that those skilled in the art can make improvements or changes based on the above description, and all these improvements and changes should belong to the protection scope of the appended claims of the present invention.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111517292A (en) * | 2020-04-30 | 2020-08-11 | 西华大学 | Tin telluride-based thermoelectric material and preparation method thereof |
| CN121341958A (en) * | 2025-12-16 | 2026-01-16 | 山东海化集团有限公司 | An n-type lead selenide thermoelectric material, its preparation method and application |
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| US20090084422A1 (en) * | 2006-03-16 | 2009-04-02 | Basf Se | Doped lead tellurides for thermoelectric applications |
| CN101656291A (en) * | 2009-09-21 | 2010-02-24 | 吉林大学 | Functional grade thermoelectric material n-PbTe and preparation method thereof |
| CN101965312A (en) * | 2008-01-14 | 2011-02-02 | 俄亥俄州立大学研究基金会 | Improve by the thermoelectric figure of merit that improves density of electronic states |
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- 2011-11-08 CN CN2011103489092A patent/CN102403446A/en active Pending
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| US20090084422A1 (en) * | 2006-03-16 | 2009-04-02 | Basf Se | Doped lead tellurides for thermoelectric applications |
| CN101106092A (en) * | 2007-04-13 | 2008-01-16 | 浙江大学 | Preparation method of IV-VI semiconductor single crystal thin film and its heterostructure |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN111517292A (en) * | 2020-04-30 | 2020-08-11 | 西华大学 | Tin telluride-based thermoelectric material and preparation method thereof |
| CN121341958A (en) * | 2025-12-16 | 2026-01-16 | 山东海化集团有限公司 | An n-type lead selenide thermoelectric material, its preparation method and application |
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Application publication date: 20120404 |