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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 林招松 | |
| dc.contributor.author | Wei-Chen Chou | en |
| dc.contributor.author | 周韋辰 | zh_TW |
| dc.date.accessioned | 2021-05-13T08:35:59Z | - |
| dc.date.available | 2017-08-30 | |
| dc.date.available | 2021-05-13T08:35:59Z | - |
| dc.date.copyright | 2016-08-30 | |
| dc.date.issued | 2016 | |
| dc.date.submitted | 2016-08-17 | |
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Analysis of selenium species using cathodic stripping voltammetry. Jurnal Teknologi, 44(1), 55-66. [52] Ham, S., Jeon, S., Park, M., Choi, S., Paeng, K. J., Myung, N., & Rajeshwar, K. (2010). Electrodeposition and stripping analysis of bismuth selenide thin films using combined electrochemical quartz crystal microgravimetry and stripping voltammetry. Journal of Electroanalytical Chemistry, 638(2), 195-203. | |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/3691 | - |
| dc.description.abstract | 在中低溫範圍，碲化鉍合金系統是效率最好的熱電材料。透過添加第三元素硒，可以形成三元n型熱電材料，其中以Bi2Te2.7Se0.3化學組成熱電轉換效率最高。面對微型化時代，傳統塊材尺寸有其限制，而薄膜材料受限於製程昂貴及前驅物毒性，較為困難工業化；厚膜製備提供了可能的前景，其中電鍍製程具有成膜速率快、不需真空設備、與微機電元件整合等優點。三元n型電鍍製程中，相對於硝酸系統，鹽酸系統較少被討論。本研究將探討不同電鍍參數對鍍層之影響，並量測熱電性質，且於微機電元件上進行電鍍。
由循環伏安掃描結果可知氯離子對於三種離子之影響，分別使鉍離子及硒離子還原峰值電位向負偏，使碲離子還原峰值向正偏。不論在硝酸或鹽酸系統中，均可發現添加Se造成還原峰值電位提前，表示有pure underpotential deposition發生。 板材電鍍部分，在鹽酸系統下，經三小時與六小時定電位電鍍後，可分別獲得27與43 μm平坦緻密的三元n-type鍍層，成分分別為Bi1.88Te2.80Se0.32及Bi1.89Te2.82Se0.29。XRD結果顯示三元鍍層結晶性優於二元系統，TEM影像顯示由奈米等級顆粒堆疊，且具有特殊層狀結構。因導電底材會影響電阻率量測，故鍍層先經由冷鑲埋樹脂翻模後，再進行熱電材性質之量測。本研究之電阻率及載子遷移率優於文獻，但鍍層成分稍微偏離計量比，造成Seebeck係數不足；比較緻密與鬆散鍍層，可發現緻密鍍層之電阻、載子遷移率、Seebeck係數均優於鬆散鍍層。 由於微機電元件幾何形狀與板材不同，影響電鍍過電位，使鍍層形貌與成分皆不同於板材電鍍所設計之結果。經調控電鍍液之配比，成分可符合計量比，定電位電鍍三小時可獲得20 μm三元n型緻密鍍層。 | zh_TW |
| dc.description.abstract | Thermoelectric materials can convert heat into electricity, and vice versa. Bi2Te2.7Se0.3 is considered to be one of the most efficient n-type thermoelectric materials near room temperature. The current tendency to miniaturization has provoked interest in thick film thermoelectric devices. Among the methods to deposit thick films, electrochemical deposition is a promising method due to its vacuum-free system, higher deposition rate, and complete integration with MEMS. In fact, nitric acid system was studied well, so further investigation of hydrochloric acid system has to be conducted.
In this research, electrodeposition of n-type Bi2Te2.7Se0.3 was studied, followed by the measurement of thermoelectric properties and the preparation of MEMS devices. Firstly, in order to understand the differences between the nitric acid and the hydrochloric acid system, cyclic voltammetry was conducted. According to the results, with the introduction of chloride ions, reduction potential for BiIII and SeIV would shift toward negative direction; a positive shift of reduction potential for TeIV was observed. Furthermore, by adding selenium ions in the binary system, the reduction peaks shifted toward positive direction. Secondly, compact deposits of Bi1.88Te2.80Se0.32 with 27 μm and Bi1.89Te2.82Se0.29 with 43 μm were obtained, respectively, after potentiostatic deposition for 3 and 6 hours. Thirdly, deposits were flipped from substrates by epoxy resin prior to the measurement of thermoelectric properties. The resistivity and mobility of the deposits were better than other researches, but slight deviation of composition may lead to low Seebeck coefficient. Last but not least, compact and stoichiometric n-type deposits with 20 μm were successfully produced on MEMS. | en |
| dc.description.provenance | Made available in DSpace on 2021-05-13T08:35:59Z (GMT). No. of bitstreams: 1 ntu-105-R03527002-1.pdf: 8069785 bytes, checksum: f8057a9f17202068ef3bb0ace315028b (MD5) Previous issue date: 2016 | en |
| dc.description.tableofcontents | 總目錄
口試委員審定書 i 致謝 ii 中文摘要 iii Abstract iv 總目錄 v 圖目錄 viii 表目錄 xi 第1章 緒論 1 第2章 文獻回顧 2 2.1熱電效應 2 2.1.1 Seebeck效應 2 2.1.2 Peltier效應 3 2.1.3 Thomson效應 4 2.1.4熱電材料重要物理量 5 2.2熱電材料製備方式 8 2.3電化學 9 2.3.1電鍍基本原理 9 2.3.2過電位 10 2.3.3二元化合物電鍍機制 10 2.3.4循環伏安法 11 2.3.5 Pourbaix Diagram簡介 14 2.4 Bi2Te3 15 2.4.1晶體結構 16 2.4.2 Bi2Te3相圖 17 2.4.3 Bi2Te3電鍍製程 17 2.4.4 硝酸與鹽酸系統之差異 18 2.5 Bi0.5Sb1.5Te3 20 2.6 Bi2Te2.7Se0.3 22 2.6.1 鉍碲硒Pourbaix Diagram 23 2.6.2 電鍍Bi2Te2.7Se0.3之發展 26 2.6.3 Bi2Te2.7Se0.3之熱電性質 29 2.7熱電元件 31 第3章 實驗方法 33 3.1實驗流程 33 3.2溶液配製 33 3.3電化學 34 3.3.1電鍍製程 34 3.3.2循環伏安掃描 35 3.4微結構及成分分析 36 3.4.1掃描式電子顯微鏡 36 3.4.2能量散佈光譜儀 36 3.4.3 電子探測微分析儀 37 3.4.4 X射線繞射分析 37 3.4.5穿透式電子顯微鏡 38 3.5板材性質量測 38 第4章 結果與討論 39 4.1循環伏安掃描 39 4.2板材電鍍 47 4.2.1電鍍參數(電位、時間、溫度)與鍍層之關係 47 4.2.2結晶性與晶粒觀察 54 4.3性質量測 57 4.4微機電元件電鍍 59 第5章 結論 63 參考文獻 64 圖目錄 圖2.1 Seebeck及Peltier效應實驗裝置圖[1] 3 圖2.2 串聯失敗示意圖 4 圖2.3 有效串聯示意圖 4 圖2.4 Thomson實驗裝置圖[2] 5 圖2.5載子濃度(n)與導電率(σ)、Seebeck係數(α)、功率因子(α2σ)以及熱導率(λ) 的關係[3] 7 圖2.6 載子與聲子於奈米微米複合材料中行進路線示意圖[5] 7 圖2.7 不同維度ZT隨量子井與量子線之寬度變化[7] 8 圖2.8 電極表面不同電鍍階段區域示意圖[17] 10 圖2.9 循環伏安法輸入電壓與時間之關係圖[19] 12 圖2.10 循環伏安法電位-電流關係圖[19] 13 圖2.11 循環伏安掃瞄過程中離子濃度分佈[19] 13 圖2.12 水之Pourbaix diagram [20] 15 圖2.13 不同材料ZT值隨溫度變化[21] 15 圖2.14 Bi2Te3晶體結構[22] 16 圖2.15 Bi-Te二元平衡相圖[24] 17 圖2.16 鉍於不同酸中CV掃描結果比較[26] 19 圖2.17 碲於不同酸中CV掃描結果比較[26] 19 圖2.18 鉍、碲及其混合溶液在鹽酸中CV掃描結果比較[27] 20 圖2.19 三元p-type電鍍(a)不同電鍍電位下相對應之鍍層成分，以及電位在(b)區間I (c)區間II (d)區間III電鍍之表面形貌[29] 21 圖2.20 加入Sb前後循環伏安掃描比較[30] 21 圖2.21 三元、二元熱電材料Z值隨導電率變化[28] 22 圖2.22 鉍之Pourbaix diagram [20] 23 圖2.23 碲之Pourbaix diagram [20] 24 圖2.24 BiTe二元Pourbaix diagram [16] 25 圖2.25 硒之Pourbaix diagram [20] 26 圖2.26 三元Bi1.97Te2.66Se0.36鬆散鍍層[34] 28 圖2.27 三元n-type鍍層於(a)較高沉積速率與(b)較低沉積速率之橫截面形貌[35] 28 圖2.28 三元n-type鍍層於(a)不鏽鋼底材與(b)金底材上電鍍之表面形貌[36] 29 圖2.29 於不銹鋼底材上之較緻密表面形貌[38] 29 圖2.30 文獻中鍍層形貌[32] 30 圖2.31 熱電元件示意圖[48] 32 圖2.32 微型化效應對單位面積冷卻功率之影響[43] 32 圖3.1 實驗流程圖 33 圖4.1 鉍離子於不同種類酸中循環伏安掃描結果 41 圖4.2 碲離子於不同種類酸中循環伏安掃描結果 41 圖4.3 硒離子於不同種類酸中循環伏安掃描結果 42 圖4.4 硒離子於不同濃度鹽酸中循環伏安掃描結果 42 圖4.5 三元BiTeSe (a)循環伏安掃描結果(b)陰極部分 43 圖4.6 鍍液在1 M硝酸中循環伏安陰極部分綜合比較 44 圖4.7 鍍液在0.35 M鹽酸中循環伏安陰極部分綜合比較 45 圖4.8 金底材與三元鍍層底材於硝酸系統循環伏安掃描結果 46 圖4.9 金底材與三元鍍層底材於鹽酸系統循環伏安掃描結果 46 圖4.10 不同電鍍電位鍍層形貌(a)0mV (b)-20 mV (c)-40 mV (d)-60 mV (e)-80 mV (f)-100 mV (g)-120 mV (h)-140 mV 49 圖4.11 不同電鍍電位鍍層形貌(a)-160 mV (b)-180 mV (c)-200 mV 50 圖4.12 於電鍍電位0 mV至-200 mV區間鍍層成分隨電位變化之關係 50 圖4.13 三元鍍液於-20 mV定電位電鍍15分鐘(a)表面形貌(b)橫截面 51 圖4.14 三元鍍液於-20 mV下定電位電鍍三小時之(a)表面形貌與(b)橫截面形貌 52 圖4.15 三元鍍液於-20 mV下定電位電鍍三小時橫截面成分分析 52 圖4.16 三元鍍液於-20 mV下定電位電鍍六小時之(a)表面形貌與(b)橫截面形貌 53 圖4.17 三元鍍液於-20 mV下定電位電鍍六小時橫截面成分分析 53 圖4.18 二元鍍層於-20 mV定電位電鍍XRD結果 55 圖4.19 三元鍍層於-20 mV定電位電鍍XRD結果 55 圖4.20 三元鍍層於-20 mV定電位電鍍20分鐘TEM橫截面形貌 56 圖4.21 三元鍍層於-20 mV定電位電鍍20分鐘TEM橫截面暗場影像 56 圖4.22 S2鍍液於-140 mV定電位電鍍1小時鬆散鍍層橫截面 58 圖4.23 S2溶液於(a)0 mV (b)-10 mV (c)-20 mV (d)-30 mV定電位電鍍表面形貌 60 圖4.24 以S2溶液於-20 mV下定電位電鍍元件覆蓋情形 60 圖4.25 以(a)S3 (b)S4 (c)S5 (d)S6 (e)S7電鍍液於-20 mV定電位電鍍30分鐘之表面形貌 61 圖4.26 以S7鍍液於-20 mV定電位電鍍三小時(a)元件之表面形貌(b)元件邊緣(c)邊緣橫截面(d)橫截面影像 62 表目錄 表2.1 Bi2Te2.7Se0.3塊材熱電性質隨溫度變化[33] 22 表2.2 文獻三元n-type熱電性質比較(*表示沒翻模) 30 表3.1 鍍液成分 34 表3.2 鹽酸系統循環伏安掃描溶液配方 35 表3.3 硝酸系統循環伏安掃描溶液配方 36 表4.1 鍍液在1 M硝酸中循環伏安峰值統整 44 表4.2 鍍液在0.35 M鹽酸中循環伏安峰值統整 45 表4.3 三元鍍液於峰值及接近峰值電位下定電位電鍍20分鐘鍍層成分分析結果 45 表4.4 板材性質量測結果(a)三組25 μm之Bi1.88Te2.80Se0.32鍍層 (b)20 μm之Bi2.08Te2.54Se0.34鬆散鍍層 58 表4.5 使用S2鍍液配方於不同電位下電鍍鍍層成分比較 60 表4.6 使用不同鍍液配方於-20 mV定電位電鍍之板材及元件成分比較 61 | |
| dc.language.iso | zh-TW | |
| dc.subject | 熱電材料 | zh_TW |
| dc.subject | 循環伏安 | zh_TW |
| dc.subject | Bi2Te2.7Se0.3 | zh_TW |
| dc.subject | 微機電元件 | zh_TW |
| dc.subject | 厚膜 | zh_TW |
| dc.subject | thick film | en |
| dc.subject | MEMS device | en |
| dc.subject | cyclic voltammetry | en |
| dc.subject | thermoelectric material | en |
| dc.subject | Bi2Te2.7Se0.3 | en |
| dc.title | Bi-Te-Se三元熱電厚膜製備及性質研究 | zh_TW |
| dc.title | Electrodeposition and Characterization of Bi-Te-Se Thermoelectric Thick Films | en |
| dc.type | Thesis | |
| dc.date.schoolyear | 104-2 | |
| dc.description.degree | 碩士 | |
| dc.contributor.oralexamcommittee | 李文錦,莊東漢,廖建能,黃憲中 | |
| dc.subject.keyword | Bi2Te2.7Se0.3,熱電材料,循環伏安,厚膜,微機電元件, | zh_TW |
| dc.subject.keyword | Bi2Te2.7Se0.3,thermoelectric material,cyclic voltammetry,thick film,MEMS device, | en |
| dc.relation.page | 70 | |
| dc.identifier.doi | 10.6342/NTU201603178 | |
| dc.rights.note | 同意授權(全球公開) | |
| dc.date.accepted | 2016-08-19 | |
| dc.contributor.author-college | 工學院 | zh_TW |
| dc.contributor.author-dept | 材料科學與工程學研究所 | zh_TW |
| 顯示於系所單位： | 材料科學與工程學系 | |
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