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研究生： 陳冠志
Chen, Guan-Chih
論文名稱： 電漿輔助化學氣相沉積法在低溫下成長氧化鉬/二碲化鉬異質結構用於電解析氫反應
Heterostructure MoOx/MoTe2 nanosheet growth in low temperature via Plasma-enhanced Chemical Vapor Deposition for Electrical Hydrogen Evolution Reaction
指導教授： 陳雨澤
Chen, Yu-Ze
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年： 2022
畢業學年度： 110
語文別： 中文
論文頁數： 85
中文關鍵詞： 二碲化鉬 、化學氣相沉積法 、異質結構 、電漿 、析氫反應
外文關鍵詞： Molybdenum Ditelluride, chemical vapor deposition, Heterostructure, plasma, HER
相關次數： 點閱：139  下載：0 
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    • 通過電化學水解的析氫反應（HER）被認為是最有效的製氫方式之一，而目前降低電催化劑的成本是實際應用中常被研究之主題。過渡金屬二硫化物（TMDCs）的相工程因其不同相的能帶而被作為電催化劑的研究。與 2H 相 TMDCs 不同，1T'相 TMDCs 由於
    其高導電性而提供更高的電荷轉移效率。本實驗中使用了電漿輔助化學氣相沉積法成功合成 1T'-MoTe2/MoOx 奈米結構。通過改變製程溫度、電將功率和氣體流量比，我們可以控制 1T'-MoTe2奈米結構的形貌。除此之外，電漿輔助沉積製成可以將製程溫度大幅降低至 300°C，且更進一步提高 1T'-MoTe2/MoOx 奈米結構在 HER 反應中的穩定性。且 1T'-MoTe2/MoOx的異質結構比純粹的氧化鉬基板提供了更多的活性位點，這也進一步提高了 HER 效率。本實驗藉由電漿的幫助下同時達成降低製程溫度、增強奈米結構穩定性與成長目標 1T'-MoTe2 等效果，也為未來層狀材料成長在金屬氧化物基板上帶來更多的發展性。

    Hydrogen evolution reaction (HER) via water splitting is considered as one of the most effective ways to generate hydrogen. Nowadays, lower cost of electrocatalyst is a mainstream research topic for practical application.Phase engineering of Transition metal dichalcogenides (TMDCs) are appealing in electrocatalysts because of their different electric bandgap in different phase. Instead of 2H-phase TMDCs, 1T’-phase of TMDCs provide more charge-transfer efficiency due to its high conductivity. In this work, 1T’-MoTe2/MoOx nanostructure was successfully synthesized by plasmaenhanced chemical vapor deposition method. By differing the processing temperature, plasma, and gas flow ratio we can control the morphology of 1T'-MoTe2 nanostructure. Besides, the plasma-assisted process can greatly decrease the processing temperature to 300°C and enhance the stability of
    1T’-MoTe2/MoOx nanostructure in HER. Moreover, the heterostructure of 1T’-MoTe2/MoOx provide more active sites than MoOx Substrate, which also improved the HER efficiency. In this work, plasma-enhanced method is used to reduce the synthesized temperature, growing targeted 1T’-MoTe2, and controlled the morphology in the meantime. This report shows us a promising way to the preparation of TMDCs in metal-oxide substrate for boosting hydrogen evolution reaction.

    致謝 I 摘要 II Extended abstract III 目錄 IX 表目錄 XI 圖目錄 XI Chapter 1 緒論 1 1.1 前言 1 1.2 研究動機 3 Chapter 2 文獻回顧 5 2.1 二維層狀材料 5 2.1.1 石墨烯 5 2.1.2 過渡金屬碳氮化物 (MXene) 6 2.1.3 過渡金屬硫屬化物 (TMDC) 8 2.2 二碲化鉬(MoTe2) 10 2.2.1 基本性質 10 2.2.2 製程方法 11 2.3 析氫反應 (Hydrogen Evolution Reaction) 17 2.3.1 酸性析氫反應 (HER in acidic solution) 18 2.3.2 鹼性析氫反應 (HER in alkaline solution) 19 2.3.3 析氫反應重要的參數 21 2.4 增加析氫反應的策略 26 2.4.1 增加導電度 26 2.4.2 摻雜離子 (Doping) 27 2.4.3 邊界工程與層狀結構 29 2.4.4 異質結構 30 Chapter 3 分析儀器與實驗手法 34 3.1 實驗藥品 34 3.2 MoOx/MoTe2 異質結構成長步驟 34 3.2.1 實驗流程圖 34 3.2.2 清洗基板與氧化鉬層形成 36 3.2.3 MoOx/MoTe2 異質結構 36 3.2.4 HER 反應測量 39 3.3 實驗儀器 39 3.3.1 真空碲化系統 39 3.3.2 場發射掃描式電子顯微鏡 (Field-emission scanning electron XIII microscope, FE-SEM) 40 3.3.3 拉曼光譜儀 (Raman spectrometer) 41 3.3.4 電化學工作站 41 Chapter 4 結果與討論 42 4.1 MoTe2/MoOx 基本性質討論 42 4.1.1 MoOx 基板與 Mo 基板碲化後形貌研究 42 4.1.2 Mo 基板與 MoOx 基板碲化後材料分析 45 4.2 電漿製程下對 MoTe2 -微結構與形貌探討 49 4.2.1 無電漿製程對氧化鉬基板碲化製程之影響 49 4.2.2 不同電漿功率對 MoTe2的表面形貌之影響 51 4.3 MoTe2 製程參數探討-製程氣流與壓力 53 4.3.1 不同製程氣流量的比例對 MoTe2 之微結構影響 53 4.3.2 不同製程壓力參數對 MoTe2 之微結構影響。 56 4.4 MoTe2 製程參數探討-製程溫度與時間 59 4.4.1 不同製程溫度對 MoTe2之微結構影響 59 4.4.2 不同製程時間對 MoTe2之微結構影響 61 4.5 MoTe2 之 HER 性能探討 64 4.5.1 探討不同電漿功率對 HER 的性能探討 64 4.5.2 探討不同製程氣流對 HER 的性能探討 66 4.5.3 探討不同製程溫度對 HER 的性能探討 68 4.5.4 探討不同成長時間對 HER 的性能探討 69 4.5.5 循環性能探討 70 Chapter 5 結論 75 Chapter 6 未來展望 77 參考資料 78

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