TWI792310B - High-efficiency thermoelectric materials - Google Patents
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- TWI792310B TWI792310B TW110117320A TW110117320A TWI792310B TW I792310 B TWI792310 B TW I792310B TW 110117320 A TW110117320 A TW 110117320A TW 110117320 A TW110117320 A TW 110117320A TW I792310 B TWI792310 B TW I792310B
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- 239000000463 material Substances 0.000 title claims abstract description 63
- ZTERWYZERRBKHF-UHFFFAOYSA-N magnesium iron(2+) oxygen(2-) Chemical compound [Mg+2].[O-2].[Fe+2].[O-2] ZTERWYZERRBKHF-UHFFFAOYSA-N 0.000 claims abstract description 41
- 229910001245 Sb alloy Inorganic materials 0.000 claims abstract description 15
- JLLLMXTZJXZSJZ-UHFFFAOYSA-N [Sb].[Si].[Sn].[Mg] Chemical compound [Sb].[Si].[Sn].[Mg] JLLLMXTZJXZSJZ-UHFFFAOYSA-N 0.000 claims abstract description 15
- 239000002140 antimony alloy Substances 0.000 claims abstract description 15
- 239000000843 powder Substances 0.000 claims abstract description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 claims description 4
- MHKWSJBPFXBFMX-UHFFFAOYSA-N iron magnesium Chemical compound [Mg].[Fe] MHKWSJBPFXBFMX-UHFFFAOYSA-N 0.000 claims description 3
- 229910019021 Mg 2 Sn Inorganic materials 0.000 claims description 2
- 238000010438 heat treatment Methods 0.000 claims description 2
- 239000008187 granular material Substances 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 abstract description 6
- 238000010586 diagram Methods 0.000 description 5
- 239000002994 raw material Substances 0.000 description 5
- 238000001354 calcination Methods 0.000 description 3
- 239000011777 magnesium Substances 0.000 description 3
- 238000005245 sintering Methods 0.000 description 3
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 2
- NPVASHFELHRKPC-UHFFFAOYSA-N [Mg].[Si].[Sn] Chemical compound [Mg].[Si].[Sn] NPVASHFELHRKPC-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000001965 increasing effect Effects 0.000 description 2
- 229910052749 magnesium Inorganic materials 0.000 description 2
- -1 magnesium-iron-oxide compound Chemical class 0.000 description 2
- 239000002918 waste heat Substances 0.000 description 2
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 1
- 238000003723 Smelting Methods 0.000 description 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 229960005191 ferric oxide Drugs 0.000 description 1
- 239000002803 fossil fuel Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000011812 mixed powder Substances 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 231100000252 nontoxic Toxicity 0.000 description 1
- 230000003000 nontoxic effect Effects 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 229910052710 silicon Inorganic materials 0.000 description 1
- 239000010703 silicon Substances 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
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- Inorganic Compounds Of Heavy Metals (AREA)
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Abstract
本發明係一種高效能熱電材料，包含有一鎂錫矽銻合金與一鎂鐵氧化物，該高效能熱電材料係由該鎂錫矽銻合金之粉末與該鎂鐵氧化物之粉末混合後燒結在一起，藉此，該高效能熱電材料具有較高的熱電優質，可有效提升熱電轉換之效率。The present invention is a high-performance thermoelectric material, which includes a magnesium-tin-silicon-antimony alloy and a magnesium-iron oxide. The high-performance thermoelectric material is sintered after mixing the powder of the magnesium-tin-silicon-antimony alloy and the powder of the magnesium-iron oxide. At the same time, by this, the high-performance thermoelectric material has high thermoelectric quality, which can effectively improve the efficiency of thermoelectric conversion.
Description
本發明係關於一種熱電材料，特別是指一種具備高效能的熱電材料。The invention relates to a thermoelectric material, in particular to a thermoelectric material with high performance.
隨著全球經濟快速發展、人口數量增加，人類對於化石燃料的需求與日俱增，且人類活動伴隨著大量的廢氣排放導致環境污染更是日益嚴重，根據文獻指出，近年來石化能源的使用率約達34%，有近66%的能源白白浪費，其中大部分係以廢熱的形式逸散至大氣中，又以汽機車與工業所產生之廢熱為主，因此若是能將廢熱有效的利用如轉換成電能，不僅能提高能源的使用效率，還能延緩能源的消耗，達到節能之效果。With the rapid development of the global economy and the increase in population, human demand for fossil fuels is increasing day by day, and human activities are accompanied by a large amount of waste gas emissions, which lead to increasingly serious environmental pollution. According to literature, the utilization rate of fossil energy has reached about 34% in recent years. %, nearly 66% of the energy is wasted in vain, most of which are dissipated into the atmosphere in the form of waste heat, and the waste heat generated by automobiles, motorcycles and industries is the main one. , not only can improve the efficiency of energy use, but also delay the consumption of energy to achieve the effect of energy saving.
而熱電材料係一種能將熱能與電能相互轉換之材料，其熱電優值越高，代表所具備的熱電轉換效率越佳，目前熱電材料依據不同最佳熱電優值的溫度範圍可分為低溫型(低於200℃)、中溫型(200℃~600℃)、以及高溫型(高於600℃)，就以中溫型熱電材料來說，鎂錫矽熱電材料的組成元素皆為地球富含原料，且價格便宜、無毒性，熱電優值可達1以上，為極具發展潛力之熱電材料，但是如何進一步增加鎂錫矽熱電材料的熱電優值，讓熱電轉換性更為提升，是所屬領域業者共同研究的目標。Thermoelectric materials are materials that can convert thermal energy and electrical energy. The higher the thermoelectric figure of merit, the better the thermoelectric conversion efficiency. Currently, thermoelectric materials can be divided into low-temperature types according to the temperature range of the best thermoelectric figure of merit. (less than 200°C), medium-temperature type (200°C~600°C), and high-temperature type (above 600°C). As far as medium-temperature type thermoelectric materials are concerned, the constituent elements of magnesium-tin-silicon thermoelectric materials are all earth-rich It contains raw materials, is cheap, non-toxic, and has a thermoelectric figure of merit of more than 1. It is a thermoelectric material with great development potential. However, how to further increase the thermoelectric figure of merit of magnesium-tin-silicon thermoelectric materials and improve the thermoelectric conversion performance is a must. The goal of common research by the industry in the field.
有鑑於此，本發明目的之一在於提供一種高效能熱電材料，其具有較高的熱電優質，可有效提升熱電轉換之效率。In view of this, one of the objectives of the present invention is to provide a high-performance thermoelectric material, which has high thermoelectric quality and can effectively improve the efficiency of thermoelectric conversion.
為達上述目的，本發明揭露一種高效能熱電材料，其包含有鎂錫矽銻合金與鎂鐵氧化物，該高效能熱電材料係由該鎂錫矽銻合金之粉末與該鎂鐵氧化物之粉末混合後燒結在一起。To achieve the above purpose, the present invention discloses a high-performance thermoelectric material, which includes magnesium-tin-silicon-antimony alloy and magnesium-iron oxide. The high-performance thermoelectric material is composed of the powder of the magnesium-tin-silicon-antimony alloy and the magnesium-iron oxide The powders are mixed and sintered together.
藉此，該高效能熱電材料具有較高的熱電優質，可有效提升熱電轉換之效率。Thus, the high-performance thermoelectric material has high thermoelectric quality, which can effectively improve the efficiency of thermoelectric conversion.
以下藉由一較佳實施例配合圖式，詳細說明本發明的技術內容及特徵，本發明一較佳實施例所提供之高效能熱電材料包含有一鎂錫矽銻合金與一鎂鐵氧化物，更進一步說明，該高效能熱電材料係由該鎂錫矽銻合金之粉末與該鎂鐵氧化物之粉末混合後燒結而成，其中，該鎂錫矽銻合金為Mg 2Sn 0.7Si 0.285Sb 0.015，該鎂錫矽銻合金係將鎂原料、錫原料、矽原料、以及銻原料依照配比進行熔煉所得，該鎂鐵氧化物為MgFe 2O 4，該鎂鐵氧化物為鎂鐵層狀雙氫氧化物經過熱處理鍛燒所得，於本實施例中，該鎂鐵層狀雙氫氧化物的鍛燒溫度為600 ℃至900 ℃，鍛燒時間為至少1小時，但該鎂鐵氧化物的製作條件並不以上述為限，該鎂鐵氧化物為片狀或粒狀晶體，圖1所示為該鎂鐵氧化物呈片狀之態樣。於其他可能的實施例中，該鎂錫矽銻合金的成分比例可有其他變化，例如Mg的比例範圍可為1.5~2.3，Sn的比例範圍可為0.5~0.9，Si的比例範圍可為0.24~0.30，Sb的比例範圍可為大於0並小於0.02。 The technical content and features of the present invention will be described in detail below by referring to a preferred embodiment with drawings. The high-performance thermoelectric material provided by a preferred embodiment of the present invention includes a magnesium-tin-silicon-antimony alloy and a magnesium-iron oxide. To further explain, the high-performance thermoelectric material is sintered by mixing the powder of the magnesium-tin-silicon-antimony alloy and the powder of the magnesium-iron oxide, wherein the magnesium-tin-silicon-antimony alloy is Mg 2 Sn 0.7 Si 0.285 Sb 0.015 The magnesium-tin-silicon-antimony alloy is obtained by smelting magnesium raw materials, tin raw materials, silicon raw materials, and antimony raw materials according to the ratio. The magnesium-iron oxide is MgFe 2 O 4 . The hydroxide is obtained by heat treatment and calcining. In this embodiment, the calcining temperature of the magnesium-iron layered double hydroxide is 600°C to 900°C, and the calcining time is at least 1 hour, but the magnesium-iron oxide The production conditions are not limited to the above. The magnesium-iron oxide is in the form of flakes or granular crystals. FIG. 1 shows that the magnesium-iron oxide is in the form of flakes. In other possible embodiments, the composition ratio of the magnesium-tin-silicon-antimony alloy may have other changes, for example, the ratio of Mg may range from 1.5 to 2.3, the ratio of Sn may range from 0.5 to 0.9, and the ratio of Si may range from 0.24 ~0.30, the ratio range of Sb can be greater than 0 and less than 0.02.
實務上可先將該鎂錫矽銻合金破脆成顆粒狀，再將成為顆粒狀的該鎂錫矽銻合金與粉末狀的該鎂鐵氧化合物一起置於一球磨機中，藉由該球磨機將該鎂錫矽銻合金磨成粉末並與該鎂鐵氧化合物混合在一起，接著再將混合後的粉末裝入模具中進行燒結，燒結溫度為500 ℃至675 ℃，壓力為50 MPa，燒結時間至少1小時，以此獲得該高效能熱電材料。該鎂鐵氧化物分布於該高效能熱電材料中，該鎂鐵氧化物之含量可等於或小於2 wt%、等於或小於0.5 wt%、等於或小於0.1 wt%，例如可為0.05 wt %、0.1 wt %、0.5 wt %、0.7 wt %、1 wt %、1.5 wt %、或2 wt %。於其他可能的實施例中，該鎂鐵氧化物之含量可視情況變化，不以上述為限。In practice, the magnesium-tin-silicon-antimony alloy can be broken into brittle particles first, and then the granular magnesium-tin-silicon-antimony alloy and the powdered magnesium-iron-oxide compound can be placed in a ball mill. The magnesium-tin-silicon-antimony alloy is ground into powder and mixed with the magnesium-iron oxide compound, and then the mixed powder is put into a mold for sintering. The sintering temperature is 500°C to 675°C and the pressure is 50 MPa. The sintering time is At least 1 hour to obtain the high-efficiency thermoelectric material. The magnesium-iron oxide is distributed in the high-performance thermoelectric material, and the content of the magnesium-iron oxide can be equal to or less than 2 wt%, equal to or less than 0.5 wt%, equal to or less than 0.1 wt%, for example, can be 0.05 wt%, 0.1 wt%, 0.5 wt%, 0.7 wt%, 1 wt%, 1.5 wt%, or 2 wt%. In other possible embodiments, the content of the magnesium-iron oxide may vary depending on the situation and is not limited to the above.
實務上判斷熱電材料的熱電性能最重要的指標為熱電優值(ZT)，根據公式ZT=σS 2T/κ，要獲得ZT值必須量測電導率(σ)、Seebeck係數(S)、熱導率(κ)隨溫度變化之結果，再由上述公式計算獲得熱電材料的熱電性能，其中σS 2的結果即為功率因數(power factor)。因此接下來說明添加不同鎂鐵氧化物含量之高效能熱電材料，與不添加該鎂鐵氧化物之一般熱電材料之間的比較。 In practice, the most important indicator for judging the thermoelectric performance of thermoelectric materials is the thermoelectric figure of merit (ZT). According to the formula ZT=σS 2 T/κ, to obtain the ZT value, it is necessary to measure the electrical conductivity (σ), Seebeck coefficient (S), thermal The result of the change of conductivity (κ) with temperature, and then calculate the thermoelectric performance of the thermoelectric material by the above formula, where the result of σS 2 is the power factor (power factor). Therefore, the comparison between the high-efficiency thermoelectric materials with different contents of magnesium-iron oxides and the general thermoelectric materials without the addition of the magnesium-iron oxides will be described next.
如圖2所示，無論該高效能熱電材料所添加的該鎂鐵氧化物含量為多少，該高效能熱電材料的電導率(electrical conductivity, σ)均較一般熱電材料為高，尤其是該鎂鐵氧化物含量為0.1 wt%時，其電導率為1200至2000 S.cm -1，而一般熱電材料的電導率為900至1600 S.cm -1；由圖3可得知，無論是否添加該鎂鐵氧化物，該高效能熱電材料與該一般熱電材料的塞貝克係數(Seebeck coefficient, S)均為負值，但整體而言添加該鎂鐵氧化物的該高效能熱電材料之塞貝克係數較一般熱電材料為高；就功率因數(power factor)而言，如圖4所示，於300 ℃時，該鎂鐵氧化物含量為0.05 wt%的高效能熱電材料具有最高的功率因數，約5.00 × 10 -3W.m -1.K -2；就熱導率(thermal conductivity, κ)而言，如圖5所示，尤其該鎂鐵氧化物含量為0.1 wt%時，該高效能熱電材料在所有測量溫度下都顯示出最低的熱導率(thermal conductivity)，約為1.9 W.m -1.K -1；根據上述參數所計算出的ZT值如圖6所示，由此可得知當溫度為400 ℃時，該高效能熱電材料具有較高的ZT值，為1.39(該鎂鐵氧化物含量1 wt%)至1.72(該鎂鐵氧化物含量0.1 wt%)，而不添加該鎂鐵氧化物的一般熱電材料在400 ℃時的ZT值則為1.19，由此可見該高效能熱電材料的ZT值可有效提升17 %至45 %。需特別說明的是，當該鎂鐵氧化物之含量較2%為大時，該高效能熱電材料的ZT值或其他上述參數的結果未優於該鎂鐵氧化物之含量等於或小於2%時，因此本實施例僅呈現該鎂鐵氧化物之含量等於或小於2%時該高效能熱電材料的ZT值以及其他上述參數的結果。 As shown in Figure 2, regardless of the content of the magnesium iron oxide added to the high-performance thermoelectric material, the electrical conductivity (electrical conductivity, σ) of the high-performance thermoelectric material is higher than that of general thermoelectric materials, especially the magnesium When the iron oxide content is 0.1 wt%, its electrical conductivity is 1200 to 2000 S.cm -1 , while the electrical conductivity of general thermoelectric materials is 900 to 1600 S.cm -1 ; it can be seen from Figure 3 that no matter whether it is added The magnesium-iron oxide, the high-performance thermoelectric material and the general thermoelectric material have negative Seebeck coefficients (Seebeck coefficient, S), but overall the Seebeck coefficient of the high-performance thermoelectric material added with the magnesium-iron oxide The coefficient is higher than that of general thermoelectric materials; in terms of power factor (power factor), as shown in Figure 4, at 300 °C, the high-efficiency thermoelectric material with a magnesium-iron oxide content of 0.05 wt% has the highest power factor, About 5.00 × 10 -3 Wm -1 .K -2 ; in terms of thermal conductivity (thermal conductivity, κ), as shown in Figure 5, especially when the content of magnesium iron oxide is 0.1 wt%, the high-efficiency thermoelectric The material shows the lowest thermal conductivity (thermal conductivity) at all measured temperatures, which is about 1.9 Wm -1 .K -1 ; the ZT value calculated according to the above parameters is shown in Figure 6, from which it can be known that When the temperature is 400 °C, the high-performance thermoelectric material has a relatively high ZT value, ranging from 1.39 (the content of the magnesium-iron oxide is 1 wt%) to 1.72 (the content of the magnesium-iron oxide is 0.1 wt%), without adding the The general thermoelectric material of magnesium iron oxide has a ZT value of 1.19 at 400 °C, which shows that the ZT value of this high-efficiency thermoelectric material can be effectively increased by 17% to 45%. It should be noted that when the content of the magnesium-iron oxide is greater than 2%, the ZT value of the high-efficiency thermoelectric material or the results of other above-mentioned parameters are not better than that of the magnesium-iron oxide content equal to or less than 2%. Therefore, this embodiment only presents the results of the ZT value of the high-efficiency thermoelectric material and other parameters mentioned above when the content of the magnesium-iron oxide is equal to or less than 2%.
本發明所提供之該高效能熱電材料具有該鎂鐵氧化物，故能有效提升功率因數，並同時降低熱傳導率，從而增強該高效能熱電材料的熱電優值，達到提升熱電轉換效率之目的。The high-efficiency thermoelectric material provided by the present invention has the magnesium-iron oxide, so it can effectively increase the power factor and reduce the thermal conductivity at the same time, thereby enhancing the thermoelectric figure of merit of the high-efficiency thermoelectric material and achieving the purpose of improving the thermoelectric conversion efficiency.
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圖1為本發明一較佳實施例之高效能熱電材料的鎂鐵氧化物之掃瞄式電子顯微鏡(SEM)的影像； 圖2為本發明一較佳實施例之添加不同含量鎂鐵氧化物的高效能熱電材料與一般熱電材料於不同溫度的電導率示意圖； 圖3為本發明一較佳實施例之添加不同含量鎂鐵氧化物的高效能熱電材料與一般熱電材料於不同溫度的塞貝克係數示意圖； 圖4為本發明一較佳實施例之添加不同含量鎂鐵氧化物的高效能熱電材料與一般熱電材料於不同溫度的功率因數示意圖； 圖5為本發明一較佳實施例之添加不同含量鎂鐵氧化物的高效能熱電材料與一般熱電材料於不同溫度的熱導率示意圖； 圖6為本發明一較佳實施例之添加不同含量鎂鐵氧化物的高效能熱電材料與一般熱電材料於不同溫度的熱電優值示意圖。 Fig. 1 is the scanning electron microscope (SEM) image of the magnesium iron oxide of the high-performance thermoelectric material of a preferred embodiment of the present invention; Figure 2 is a schematic diagram of the electrical conductivity of high-performance thermoelectric materials and general thermoelectric materials at different temperatures with different contents of magnesium-iron oxide added in a preferred embodiment of the present invention; 3 is a schematic diagram of the Seebeck coefficients of high-performance thermoelectric materials with different contents of magnesium-iron oxides and general thermoelectric materials at different temperatures according to a preferred embodiment of the present invention; Fig. 4 is a schematic diagram of the power factor of a high-efficiency thermoelectric material added with different contents of magnesium iron oxide and a general thermoelectric material at different temperatures according to a preferred embodiment of the present invention; Fig. 5 is a schematic diagram of the thermal conductivity of high-performance thermoelectric materials and general thermoelectric materials at different temperatures with different contents of magnesium-iron oxide added according to a preferred embodiment of the present invention; FIG. 6 is a schematic diagram of thermoelectric figure of merit at different temperatures of high-performance thermoelectric materials added with different contents of magnesium-iron oxides and general thermoelectric materials according to a preferred embodiment of the present invention.
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| TW200702305A (en) * | 2005-04-13 | 2007-01-16 | Sumitomo Chemical Co | Thermoelectrical conversion material, manufacturing method thereof and thermoelectrical conversion element |
| TW200832768A (en) * | 2006-11-28 | 2008-08-01 | Sumitomo Chemical Co | Thermoelectric conversion material and thermoelectric conversion element |
| TW200950165A (en) * | 2008-02-07 | 2009-12-01 | Basf Se | Doped tin tellurides for thermoelectric applications |
| CN107516709A (en) * | 2017-07-14 | 2017-12-26 | 贵研铂业股份有限公司 | A kind of rhodium base thermoelectricity material and preparation method thereof |
| CN107710429A (en) * | 2015-11-11 | 2018-02-16 | 株式会社Lg化学 | P-type skutterudite thermoelectric material, its preparation method and thermoelectric device comprising it |
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2021
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Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| TW200702305A (en) * | 2005-04-13 | 2007-01-16 | Sumitomo Chemical Co | Thermoelectrical conversion material, manufacturing method thereof and thermoelectrical conversion element |
| TW200832768A (en) * | 2006-11-28 | 2008-08-01 | Sumitomo Chemical Co | Thermoelectric conversion material and thermoelectric conversion element |
| TW200950165A (en) * | 2008-02-07 | 2009-12-01 | Basf Se | Doped tin tellurides for thermoelectric applications |
| CN107710429A (en) * | 2015-11-11 | 2018-02-16 | 株式会社Lg化学 | P-type skutterudite thermoelectric material, its preparation method and thermoelectric device comprising it |
| CN107710429B (en) | 2015-11-11 | 2021-01-05 | 株式会社Lg化学 | P-type skutterudite thermoelectric material, method for preparing same, and thermoelectric device comprising same |
| CN107516709A (en) * | 2017-07-14 | 2017-12-26 | 贵研铂业股份有限公司 | A kind of rhodium base thermoelectricity material and preparation method thereof |
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