臺灣博碩士論文加值系統

近年來奈米材料之異質複合工程已然成為開發高熱電性能材料最具潛力的策略。異質相摻雜除了可以選擇性彌補母材熱電特性外，其衍生之異質功能性介面，更可突破材料熱電性質之物理耦合關係，進一步有效提升整體熱電優值(Thermoelectric figure of merit, ZT)。碲化鉍銻(Bi0.5Sb1.5Te3)屬於V-VI族p型半導體材料，在室溫下具有極佳之熱電性質，是目前商用化發展最為成熟的熱電材料之一。有鑑於此，本研究利用Bi0.5Sb1.5Te3 (BST)良好之導電性能，選擇具有低導電導熱特性之類鑽碳(Diamond-like carbon; DLC)進行異質混摻，期待透過降低材料導熱率，及產生之各式DLC/BST異質介面引發載子濾能效應，提升整體熱電效能。
本研究利用雙光束脈衝雷射沉積系統，於SiO2/Si絕緣基板上成功製備一系列新穎DLC/BST異質奈米複合薄膜(Hetero-nanocomposite films)。首先透過分光鏡調控主副靶材雷射功率，製備所得之薄膜DLC摻雜比例約在0~19.3 wt%之間。DLC混摻薄膜(4.3 wt% DLC)之Seebeck係數最高達652 µVK-1約3倍於本質BST。從Pisarenko plot分析可知，此增幅情形來自於異質介面引發之載子濾能效應。透過熱擴散度及拉曼光譜分析可證明DLC摻雜確實能有效降低薄膜之熱傳導。為了進一步調控優選方向及介面結構，選用熱電特性最佳化之分光比，基板沉積溫度從400 oC調升至450 oC及500 oC，結果發現優選方向從(015)逐漸轉變至(00Ɩ)。此外，從TEM分析發現高密度、高方向性之雙晶介面貫穿BST片狀結構，推測能在不影響載子傳輸的前提下，達到散射聲子降低熱導率之效果，其中沉積溫度450oC之薄膜(3.8 wt% DLC) Seebeck及功率因子分別為616 µVK-1及37 µWcm-1K-2，普遍優於文獻報導BST之值。

In recent years, heterogeneous nanostructuring has become one of the most promising strategies for modifying thermoelectric materials. The introduction of heterogeneous dopants could not only selectively improve intrinsically-poor specific properties of the base materials, but potentially break the physically coupled thermoelectric properties due to the created various heterogeneous functional interfaces for further enhancing the overall thermoelectric figure of merit (ZT). Bismuth-antimony-tellurium (BST), one of the most mature thermoelectric composites in commercialization, is a p-type V-VI semiconductor material exhibiting a high thermoelectric performance around room temperature. In this work, from the view point of lowering the thermal conductivity, diamond-like carbon (DLC), a representative
branch in the family of less-conductive amorphous carbons was specially introduced as the heterogeneous component to cooperate with BST, and expected to provide various DLC/BST hetero-interfaces for activating the known energy filtering effect for enhancing the thermoelectric properties.
In this dissertation, a series of novel DLC/BST heterogeneous nanocomposite films were successfully deposited on SiO2/Si substrates using dual beam pulse laser deposition system. Beam splitters were applied to regulate laser energy for individually ablating BST and pyrolytic carbon targets for fabricating the DLC/BST films with different DLC contents (0~19.3 wt%). The highest Seebeck coefficient of the DLC/BST film (4.3 wt% DLC) was found to approach 652 µVK-1 which is over three times higher than that for intrinsic BST. According to Pisarenko plot, the significantly enhanced Seebeck coefficient evidently originated from the DLC/BST hetero-interfaces induced energy filtering effect. Besides, the greatly suppressed thermal transport as evidenced by micro-Raman and thermal diffusivity characterizations reasonably came from the effects of grain fining of BST and the intrinsically low thermal conductivity of DLC. To further adjust preferential orientation and interfacial structure, the laser energy ratio for providing the highest Seebeck coefficient was maintained for film preparation with a higher deposition temperature of 450 oC and 500 oC. It was found that preferential orientation gradually shifted from (015) to (00Ɩ) with temperature increasing. In addition, the TEM images attested high-density and strongly oriented twin bands almost across the whole BST flake-like structure, indicated the potential for scattering multi-wavelength phonons and further decreasing the thermal conductivity, without greatly interfering the carrier transportation. An enhanced Seebeck coefficient of 616 μVK-1 and the corresponding power factor of 37 µWcm-1K-2 obtained from the DLC/BST film prepared at 450 oC (3.8 wt% DLC) are comparable to or higher than previous reported values of BST or BiSbTe-based nanocomposites.

摘要 I
Abstract III
誌謝 V
目錄 VI
圖目錄 VIII
表目錄 XI
第一章 前言 1
第二章 文獻回顧 3
2.1 熱電材料的原理與簡介 3
2.1.1 熱電效應 4
2.1.2 熱電優值(ZT) 7
2.1.3 熱電材料類型簡介 8
2.2 奈米化熱電材料簡介 10
2.2.1 奈米化對熱電性質之影響 10
2.2.2 異質奈米複合結構熱電材料 13
2.3 Bi0.5Sb1.5Te3的背景與簡介 15
2.4 碳混摻之熱電材料研究現況 19
2.4.1石墨烯(Graphene) 19
2.4.2奈米碳管(Carbon nanotube; CNT) 20
2.4.3 C60 (Fullerene) 21
2.5 研究動機 22
第三章 研究方法與步驟 24
3.1 鍍膜前置作業 25
3.1.1 靶材製備 25
3.1.2 試片預備與清洗 25
3.2 雙脈衝雷射沉積 25
3.2.1 靶材裝置及雷射設定 25
3.2.2 DLC/BST薄膜沉積 27
3.3 微結構分析 27
3.3.1 掃描式電子顯微鏡 28
3.3.2 X光繞射分析儀 28
3.3.3 X光光電子能譜儀 28
3.3.4 聚焦離子束顯微鏡 28
3.3.5 穿透式電子顯微鏡 28
3.3.6 拉曼光譜儀 29
3.4 熱電性質量測 29
3.4.1 霍爾量測系統 29
3.4.2 Seebeck量測系統 30
3.4.3 熱擴散量測系統 31
第四章 結果與討論 33
4.1 雙靶共沉積混摻結構：DLC摻雜比例 33
4.1.1 成分及形貌分析 33
4.1.2 熱電性質分析 40
4.1.3 熱傳導分析 43
4.2 雙靶共沉積混摻結構：沉積溫度 45
4.2.1 成分及形貌分析 45
4.2.2 熱電性質分析 50
第五章 結論 52
參考文獻 53

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