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研究生： 陳思妤
Chen, Shih-Yu
論文名稱： 三維二氧化錫奈米結構陣列之成長與其應用於光電化學分解 水之研究
Growth of Three-Dimensional SnO2 Nanostructured Array Scaffold for Use in Heterojunction Photoanodes of Photoelectrochemical Water Splitting
指導教授： 吳季珍
Wu, Jih-Jen
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2017
畢業學年度： 105
語文別： 中文
論文頁數： 86
中文關鍵詞： 二氧化錫 、四氧化釩鉍 、三維奈米結構 、異質奈米結構 、光陽極 、光電化學分解水
外文關鍵詞： SnO2, BiVO4, 3-D nanostructure, heterojunction photoanode, PEC water splitting
相關次數： 點閱：71  下載：1 
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    • 本研究使用溶劑熱法於導電玻璃基板上成長出具有高方向性與高間隙度之二氧化錫一維奈米柱陣列。接著以化學浴沉積法成長樹芽狀奈米顆粒，做為後續成長三維樹枝狀結構之晶種層，最後再次使用溶劑熱法可於樹芽狀顆粒處成長出側枝結構，形成三維二氧化錫樹枝狀奈米結構陣列。穿透式電子顯微鏡分析結果顯示，此二氧化錫奈米柱陣列與三維樹枝狀結構皆為單晶的二氧化錫金紅石結構，具有良好的結晶性。本研究繼以800 奈米長的二氧化錫奈米柱與奈米樹枝結構陣列作為傳輸電子的支架，於其上以金屬-有機物熱裂解法，沉積四氧化釩鉍奈米顆粒薄膜作為吸光層，形成異質介面結構，應用於光電化學分解水之光陽極材料。相較於一維二氧化錫奈米柱狀結構，三維奈米樹枝狀結構能更有效地提升四氧化釩鉍-二氧化錫異質介面光電極的載子分離效率。在噬電洞劑存在電解液的情況下，四氧化釩鉍-二氧化錫奈米樹枝陣列異質介面光電極在施加1.23V vs. RHE時，可得2.02 mA/cm2，與其吸收圖譜換算之完全轉換光電流值2.24 mA/cm2相較計算得知，載子分離效率可達到87%。

    In this work, high directional tin oxide nanodendrite array (SnO2 ND) was derived from the solvothermal-grown nanorod (NR) array. The synthesis of the branches on the surface of the SnO2 NR was carried out using chemical batch deposition (CBD) followed by another solvothermal process. Bismuth vanadate (BiVO4) thin film were then deposited on the surface of SnO2 NR and SnO2 ND by metal organic decomposition method to form heterojunction photoanodes for use in photoelectrochemical (PEC) water splitting cell. Under AM 1.5G solar simulator illumination, the photocurrent density of SnO2 ND/BiVO4 photoanode is optimized to be 2.02mA/cm2 at 1.23 V versus reversible hydrogen electrode (RHE) with sodium sulfite (Na¬2SO¬¬3) in the electrolyte as hole scavenger. The three-dimensional nanostructured heterojunction photoanode demonstrates a charge separation efficiency as high as 87% at 1.2 V vs. RHE.

    摘要 I 目錄 X 表目錄 XIII 圖目錄 XIV 第一章 緒論 1 1-1 前言 1 1-2 光觸媒產氫 3 1-3 研究動機 4 第二章 文獻回顧 6 2-1 二氧化錫性質與應用 6 2-2 奈米尺度二氧化錫之應用 9 2-2.1 零維奈米結構 9 2-2.2 一維奈米結構 12 2-2.3 二維奈米結構 17 2-2.4 三維奈米結構 18 2-3光觸媒分解水 20 2-3.1光觸媒分解水工作原理 20 2-3.2奈米結構對光觸媒分解水之效應 23 2-3.3異質結構對光觸媒分解水之效應 26 2-3.4 共觸媒對光觸媒分解水之效應 30 第三章 實驗步驟與方法 31 3-1 實驗材料 31 3-2 實驗流程 33 3-2.1 基板清洗 34 3-2.2 旋轉塗佈二氧化錫晶種層 34 3-2.3 溶劑熱法成長二氧化錫奈米柱陣列 34 3-2.4 化學浴沉積法成長樹芽狀奈米結構於二氧化錫奈米柱陣列 35 3-2.5 溶劑熱法成長三維樹枝狀二氧化錫奈米結構陣列 35 3-2.6 金屬有機物分解法成長四氧化釩鉍薄膜 36 3-2.7 沉積共觸媒氫氧化鐵(FeOOH) 37 3-2.8 光電化學分解水電極製備及量測 37 3-2.9 載子分離效率與注入效率之量測 38 3-3 分析儀器 39 3-3.1 掃描式電子顯微鏡（Scanning Electron Microscope，SEM） 39 3-3.2 穿透式電子顯微鏡（Transmission Electron Microscope，TEM） 40 3-3.3 X光繞射（Xray Diffraction，XRD） 41 3-3.4 拉曼光譜分析（Raman spectroscopy） 42 3-3.6 太陽光模擬器（Solar Simulator） 44 3-3.7 恆電位儀（Potentiostat） 45 第四章 結果與討論 45 4-1 成長一維二氧化錫奈米柱結構 45 4-1.1 晶種層熱處理溫度對表面形貌之影響 45 4-1.2 四氯化錫濃度對反應速率之影響 46 4-1.3 溶劑比例對反應速率之影響 48 4-1.4 溴化鈉濃度對反應速率之影響 50 4-1.5 最佳化成長二氧化錫奈米柱陣列製程 52 4-1.6 二氧化錫奈米柱之結構分析 55 4-2 成長三維二氧化錫奈米樹枝狀陣列 58 4-2.1 鹽酸濃度對成長樹枝狀結構之影響 58 4-2.2 溶劑比例對水熱法成長樹枝狀結構之影響 60 4-2.3 四氯化錫濃度對水熱法成長樹枝狀結構之影響 62 4-2.4 溴化鈉濃度對水熱法成長樹枝狀結構之影響 63 4-2.5 三維二氧化錫奈米結構分析 65 4-3 成長四氧化釩鉍－二氧化錫異質介面奈米結構陣列於光電化學分解水之應用 69 4-3.1 四氧化釩鉍－二氧化錫異質介面奈米結構陣列表面型態與結構分析 69 4-3.2 四氧化釩鉍-二氧化錫異質介面結構於光電化學分解水之特性 71 4-3.3 三維二氧化錫奈米異質結構對於光電化學分解水之效應 73 4-4 表面沉積共觸媒之效應 76 第五章 結論 78 參考文獻 81

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