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研究生: 朱昱璋
YU-CHANG CHU
論文名稱: 二氧化鈦奈米管擔載金、鉑觸媒進行紫
指導教授: 楊思明
Sze-Ming Yang
口試委員:
學位類別: 碩士
Master
系所名稱: 工學院 - 化學工程與材料工程學系
Department of Chemical & Materials Engineering
畢業學年度: 94
語文別: 中文
論文頁數: 77
中文關鍵詞: 金觸媒甲醇奈米管二氧化鈦
外文關鍵詞: TiO2, hydrogen, methanol, gold
相關次數: 點閱:8下載:0
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  • 本研究利用化學法(Chemical Method)將二氧化鈦製備成二氧化
    鈦奈米管,比較不同鍛燒溫度對奈米管的成型與表面積的影響,並利
    用沉澱固著法(Deposition Precipitation)和初濕含浸法將二氧化鈦擔載
    金觸媒;利用光化學沉積法和沉澱固著法製備鉑觸媒,以不同晶相及
    不同表面積的二氧化鈦擔載金屬觸媒在紫外光照射下進行甲醇重組
    反應產生氫氣。利用XRD、TEM、BET 等不同鑑定方法分析所合成
    的二氧化鈦奈米管之結構與表面積,並探討擔載金、鉑觸媒的反應特
    性及觸媒活性。
    結果顯示,化學法製備的二氧化鈦奈米管管外徑約12 奈米,內
    徑8 奈米,長約數百奈米。沉澱固著法製備的二氧化鈦擔載金觸媒,
    金顆粒呈半圓球型,顆粒大小約4~7 奈米,沉積於擔體表面或奈米管
    中,而初濕含浸法製備的金觸媒其金顆粒大小分佈較為不均。比較光
    化學沉積法與沉澱固著法製備的白金觸媒,發現光化學沉積法製備的
    鉑觸媒,其擔體上的白金顆粒較沉澱固著法小。活性測試顯示,金觸
    媒活性隨鍛燒溫度升高而降低,其中以200℃鍛燒後的金觸媒活性最
    佳。而沉澱固著法製備的觸媒反應活性較初濕含浸法製備的觸媒好。
    白金觸媒對甲醇重組產氫也有與金觸媒相同的效果,金屬顆粒越小將
    會有越好的反應活性。


    Titanium nanotubes were prepared from titanium powers by
    treating with 10 M NaOH at 110~130℃ for 24 hours(Chemical method).
    Excess NaOH was then neutralized with distilled water and HCl(aq). The
    TiO2 nanotubes were characterized by X-ray diffraction (XRD), specific
    surface area (BET), and transmission election microscope (TEM). Then
    we prepare Au/TiO2, Pt/TiO2 by deposition precipitation and incipient
    wetness methods. And we prepare Pt/TiO2 by photochemical deposition
    method. We can evaluate the activities of these catalysts by hydrogen
    production of methanol reforming under ultraviolet light (350nm)
    irradiation. We use XRD, BET, and TEM to analyze various catalysts.
    The TiO2 nanotubes were prepared by chemical method with inner
    diameters of approximately 8 nm and outer diameters 12nm and 100 nm
    lengths. The gold on the surface of TiO2 by deposition precipitation
    method is hemisphere and the Au particles size is 4~7 nm. And we use
    photochemical deposition method to prepare Pt/TiO2, the Pt particles size
    is about 1nm. When Au/TiO2 and Pt/TiO2 were calcined at higher
    temperature the particles size gets bigger. The catalytic activity is
    strongly dependent on the gold and platinum particles size, the smaller
    particles produces higher amount of hydrogen.

    誌謝............................................................................................................. I 摘要............................................................................................................II Abstract .....................................................................................................III 目錄.......................................................................................................... IV 圖目錄..................................................................................................... VII 表目錄...................................................................................................... XI 第一章 緒論...........................................................................................1 第二章 文獻回顧......................................................................................2 2.1 金觸媒的性質................................................................................2 2.2 金觸媒的製備................................................................................3 2.3 鉑觸媒的性質................................................................................5 2.4 二氧化鈦簡介................................................................................5 2.5 二氧化鈦奈米管............................................................................9 2.6 氫氣的製備..................................................................................14 2.6.1 甲醇氧化蒸氣重組反應(Oxidative steam reforming of methanol).....................................................................................16 2.6.2 甲醇直接分解反應(Methanol decomposition).................17 2.6.3 甲醇部分氧化反應(Partial oxidation of methanol)..........17 V 2.6.4 甲醇光催化重組產氫反應................................................17 2.7 實驗目的......................................................................................22 第三章 實驗方法....................................................................................23 3.1 實驗藥品......................................................................................23 3.2 儀器設備......................................................................................24 3.3 實驗方法.....................................................................................25 3.3.1 二氧化鈦奈米管製備........................................................25 3.3.2 以沉澱固著法製備金觸媒................................................27 3.3.3 以初濕含浸法製備二氧化鈦奈米管金觸媒...................29 3.3.4 白金、銀觸媒製備............................................................29 3.4 鑑定分析.....................................................................................31 3.4.1 粉末X 光繞射(XRD).......................................................31 3.4.2 穿透式電子顯微鏡............................................................32 3.4.3BET 法測量比表面積........................................................32 3.4.4 感應耦合電漿原子發射光譜儀(ICP-AES)......................33 3.4.5 甲醇重組反應活性測試...................................................34 3.5 二氧化鈦奈米金、鉑觸媒總表.................................................37 第四章 結果與討論................................................................................38 4.1 觸媒鑑定......................................................................................38 VI 4.1.1 XRD 分析..........................................................................38 4.1.2 TEM 影像分析..................................................................48 4.1.3 觸媒比表面積分析............................................................55 4.1.4 元素分析............................................................................57 4.2 甲醇光催化重組反應..................................................................59 4.2.1 鍛燒溫度、不同擔體對觸媒活性的影響.......................59 4.2.2 不同金屬對觸媒活性的影響............................................62 4.2.3 金屬擔載量對觸媒活性的影響........................................63 4.2.4 不同製備方法對觸媒活性的影響...................................66 4.3 與文獻上利用UV 光進行甲醇轉化的銅、鈀,金、鉑觸媒比較 氫氣產生量........................................................................................68 第五章 結論.............................................................................................71 參考文獻...................................................................................................72

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