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研究生:洪瑋佐
研究生(外文):Wei-Tso Hung
論文名稱:製備Bi0.5Sb1.5Te3熱電材料與熱電特性之研究
論文名稱(外文):Study on the Preparation and Characterization of Bi0.5Sb1.5Te3 Thermoelectrical Material
指導教授:唐自標王錫福
指導教授(外文):Tze-Piao TangSea-Fue Wang
口試委員:張世賢邱六合
口試日期:2012-07-10
學位類別:碩士
校院名稱:國立臺北科技大學
系所名稱:材料科學與工程研究所
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2012
畢業學年度:100
語文別:中文
論文頁數:88
中文關鍵詞:熱電材料Seebeck係數熱傳導導電率球磨優值
外文關鍵詞:Thermoelectric materialsSeebeck coefficientThermal conductivityelectrical conductivitymillingfigure of merit
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本實驗研究的方向為Bi0.5Sb1.5Te3,隸屬於室溫使用範圍的熱電材料。該熱電材料在室溫下操作會有較好的熱電優值。材料是利用區熔法(Zone melting)所製備而成,成形為塊材後,再利用不?袗?研缽將其搗碎。
實驗初期,先將搗碎且過篩後之熱電粉末,直接利用萬能試驗機進行冷壓,並逐漸提高持加壓力,觀察其熱電性質,但由於熱傳導係數較高,導致熱電優值偏低。而後,為了降低熱傳導係數,將粉末進行球磨,以增加載子散射的機率。比較後發現,粉末球磨3小時可得到較高之熱電優值。但因球磨時產生之熱能會使溫度提高,粉末產生氧化現象,因而使導電率降低。為防止此氧化現象,將粉末進行還原,但效果不如預期。若在球磨前先將球磨罐內通入氮氣作為保護性氣體,則可防止粉末氧化。經實驗證實,導電率確實有回復的趨勢,ZT值亦隨之提高。進一步改變持壓溫度,將粉末進行熱壓,並且在燒結前將試片利用石墨紙包覆以防止試片氧化。最後數據結果顯示,通氮氣球磨3小時,持壓250 MPa,溫度350oC,10分鐘,燒結400oC,2小時之樣品,計算後可得到本實驗最高之ZT值為0.51。


This research focus on Bi0.5Sb1.5Te3 which is a room-temperature use thermoelectrical material. Higher ZT value can be achieved when used in room temperature. The material was prepared by using Zone melting process.
In the beginning of the experiment, the smashed and screened powder was then conducted by cold pressing with omnipotent material experiment machine. During the cold pressing stage, observing the thermal-electrical properties by gradually increasing the pressure. The figure of merit was low due to the higher thermal conductivity. Therefore, in order to decrease the thermal conductivity, the powder was milled so that the carrier scattering possibility was increased. A higher ZT value was obtained from the 3-hour milling powder. However, the heat was generated accordingly during the milling which resulted in the decrease of electrical conductivity due to the oxidation of powder. To prevent the powder from oxidation, the de-oxidation process of powder was adopted but the result was not as good as expected. In another way to avoid the oxidation of powder, the N2 gas was introduced before milling. The conductivity and the ZT value were increased as a result. Furthermore, changing the compression temperature, applying hot pressing onto powder and wrapping the sample with graphite paper before sintering were considered. According to the final result, sample with milling for 3 hours under N2 atmosphere, pressing under 250 Mpa at 350oC for 10 minutes and sintering at 400oC for 2 hours can obtain the highest ZT value 0.51.


摘要 I
ABSTRACT II
誌謝 IV
目錄 V
圖目錄 VIII
表目錄 XIII
第一章 簡介 1
1.1前言 1
1.2 研究目的 2
1.3熱電材料之發展與介紹 3
1.3.1熱電材料之發展史 3
1.3.2熱電材料之簡介 5
1.3.2.1改善熱電優值(Thermoelectric figure of merit)的方法 6
1.3.2.2熱電元件之優缺點[13] 10
1.3.2.3熱電材料分類 11
1.3.2.4碲化鉍系統熱電材料簡介 12
1.3.2.5熱電材料的製備 14
第二章 基礎理論與文獻回顧 16
2.1 熱電現象 16
2.1.1Seebeck效應[21] 16
2.1.2Peltier效應 19
2.1.3Thomson效應 22
第三章實驗流程及量測方法 23
3.1實驗規劃與步驟 23
3.2實驗儀器與設備 26
3.2.1不?袗?研缽 26
3.2.2篩網 26
3.2.3行星式球磨機 27
3.2.4萬能試驗機 27
3.2.5分離式加熱器 28
3.2.6全自動真空抽取機 29
3.2.7真空燒結爐 29
3.2.8 X-ray繞射儀 30
3.2.9真空乾燥罐 31
3.2.10場發射式電子顯微鏡(FE-SEM) 31
3.2.11熱游離式電子顯微鏡(TE-SEM) 32
3.2.12氣氛還原爐 33
3.2.13光學顯微鏡 34
3.2.14熱電量測系統 35
3.3 熱電性質量測 36
3.3.1熱傳導係數量測 36
3.3.2 Seebeck係數量測 40
3.3.3導電率量測 41
第四章 結果與討論 42
4.1 晶體結構分析 42
4.1.1 X光繞射分析 44
4.1.2 DTA/TGA分析結果 46
4.1.3 SEM分析 49
4.2 熱電性質之分析 53
4.2.1持加壓力 53
4.2.2球磨時間 57
4.2.3還原 66
4.2.4球磨罐通入保護氣體 71
4.2.5冷壓與熱壓 75
4.2.6燒結包覆石墨紙 79
第五章 結論 83
參考文獻 85


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