孔徑尺寸與銀擔載量對於二氧化鈦奈米管在0.5 M硫酸中之氧還原催化之影響

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姓名

黎修甫(Hsiu-Fu Li) 查詢紙本館藏

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機械工程學系

論文名稱

孔徑尺寸與銀擔載量對於二氧化鈦奈米管在0.5 M硫酸中之氧還原催化之影響
(The effect of diameter and Ag loading on the Self-organized TiO2 nanotube for oxygen reduction reaction catalytic performance in 0.5 M H2SO4)

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摘要(中)

在本研究中，採用兩極式陽極氧化電化學法在含氟蝕刻液中，藉由改變工作偏壓(5V~30V)、電解液氟離子濃度(0.1M~0.7M)、蝕刻液pH值(pH1~pH7)、蝕刻液溫度(20~80℃)、蝕刻液添加甘油量(0~10M)，來探討製程參數對二氧化鈦奈米管管徑之影響。結果顯示：二氧化鈦奈米管之管徑會隨工作偏壓(5V~20V)、蝕刻液中氟離子濃度(0.1M~0.7M)及蝕刻液溫度(20~40℃) 增加而增大，其直徑範圍在65~134 nm。但直徑會隨蝕刻液中之pH值(pH1~pH7)及甘油添加濃度(0M~10M)增加而減小。
陽極氧化所得之二氧化鈦奈米管經為非晶態，經480℃、3小時熱處理後成為銳鈦礦(anatase)為主和金紅石(rutile)為副晶體之混合，經浸泡於0.2M硝酸銀溶液中15、30、45與60分鐘用以擔載不同濃度之銀，或浸泡0.5g SnCl2+0.56M HCl 浸泡5分鐘，接著再以0.05M PdCl2+0.5M HCl 浸泡1分鐘，以擔載鈀，分別於0.5 M硫酸溶液中進行氧還原(oxygen reduction reaction ,ORR)催化反應，藉以比較其ORR催化反應之活性。結果顯示：非晶質二氧化鈦奈米管不具活性，經480℃、3小時熱處理後，結晶性二氧化鈦奈米管開始具有活性，其活隨奈米管孔徑由100縮小至65nm而增加活性。若奈米管擔載銀，其ORR之起始電位(Eonset)上升至較正值，表示催化活性增大，還原電流隨銀含量之增多而增大，表示增加銀擔載量，有增進催化速率之結果，管徑在65nm之奈米管經1小時之紫外光(λ=254nm)還原銀觸媒可得最高之催化反應電流(242μA/cm2)。在相同中擔載量下，鈀擔載於二氧化鈦奈米管中比擔載銀的活性更高、催化速率更快。

摘要(英)

Self-organized titanium dioxide nanotube was fabricated on titanium foils by electrochemical anodization in fluoride solution at room temperature. The effect of voltage employed, fluoride concentration, pH of the bath and the temperature of the bath on the diameter of the nanotubes was of interest. The result revealed that the diameter of nano tubes increases (from 30 to 100 nm) with increasing the voltage from 5 to 20 V. It also increases (from 70 to 134 nm) with an increase of the fluoride concentration from 0.1 to 0.7 M. The diameter of the nano tubes increases with increasing the bath temperature (from 20 to 80℃), whereas it decreases (from 100 to 45 nm) with increasing the pH value of the bath (from 1 to 7). The addition of glycerol causes a decrease in the diameter of the nano tubes, with increasing glycerol from 0 to 5.0 M, the diameter of the tubes decreases from 100 nm to 87 nm. The anodized nanotubes were amorphous and they turned out to be a mixture of anatase and rutile after exerting a heat-treatment at 480 ℃ for 3 h. The heat-treated nano tubes were immersed in 0.2M silver nitrate for 15、30、45 and 60 minutes to be loaded with various silver contents. And they were immersed in a mixture of 0.5M SnCl2+0.05M PdCl2 for 5 minutes to be loaded with Pd. All kinds of nano tubes were put in 0.5 M sulfuric acid solution to conduct oxygen reduction reaction (ORR) and compare their onset potential (Eonset) and cathodic current density. The results revealed that amorphous TiO2 is inactive to ORR, heat-treated at 480℃ for 3 h turning the amorphous nano tubes into crystalline to become active. The reactivity of the nano tubes increases with decreasing the diameter from 100 to 65nm. In the presence of Ag loading, the onset potential (Eonset) of ORR becomes more positive so that the catalytic activity is higher, and the cathodic current density increases with increasing the Ag-loading. Obviously, Ag-load on the crystal TiO2 nano tubes enhances the catalytic activity. For instance, For nano tubes with diameter at 65nm illuminated by UV-light(λ=254nm) for 1 h to be loaded with silver leads to highest cathodic current density (242μA/cm2) for ORR。At the same loading level, Pd-loaded nano tubes are better than Ag-loaded nano tubes to reveal higher catalytic activity.

關鍵字(中)

★ 氧還原反應
★ 電化學陽極氧化
★ 奈米管
★ 二氧化鈦

關鍵字(英)

★ oxygen reduction reaction
★ Titanium dioxide
★ nanotube
★ andization

論文目次

中文摘要 Ι
Abstract Ⅲ
圖目錄 Ⅸ
表目錄 XIV
第一章前言 1
1-1研究背景 1
1-2研究動機與目的 2
第二章文獻回顧 3
2-1奈米材料簡介 3
2-2二氧化鈦奈米管簡介 3
2-3二氧化鈦晶體結構 4
2-4二氧化鈦製作方式 5
2-5二氧化鈦奈米管蝕孔機制 7
2-6氧氣還原反應(Oxygen Reduction Reaction，ORR) 9
第三章研究方法 11
3-1試片準備 11
3-2陽極處理實驗參數 11
3-3陽極處理實驗裝置 12
3-4 擔載銀與鈀試片製備 12
3-4-1 擔載銀試片之製備 12
3-4-2 擔載鈀試片之製備 13
3-5循環伏安法(CV) 13
3-6本實驗所使用之儀器 13
第四章　研究結果 15
4-1 蝕刻液特性 15
4-1-1不同氟離子含量實驗前蝕刻液之導電度與黏度量測 15
4-1-2不同蝕刻液pH值實驗前導電度與黏度量測 15
4-1-3不同蝕刻液溫度實驗前蝕刻液之導電度與黏度量測 15
4-1-4不同甘油含量實驗前之導電度與黏度量測 16
4-2 偏壓對於二氧化鈦奈米管結構之結果 16
4-3 氟離子濃度對於二氧化鈦奈米管結構之結果 17
4-4蝕刻液的pH值對於二氧化鈦奈米管結構之結果 18
4-5蝕刻液溫度對於二氧化鈦奈米管結構之結果 19
4-6不同甘油含量對於二氧化鈦奈米管結構之結果 20
4-7在甘油含氟溶液中不同偏壓對於二氧化鈦奈米管形貌之影響 21
4-8熱處理後擔載銀、鈀試片分析 22
4-9 循環伏安法(CV)結果 23
4-9-1 熱處理試片對氧還原催化能力之循環伏安之結果 23
4-9-2 不同孔徑試片擔載銀之循環伏安結果 23
4-9-3不同孔徑試片擔載相同濃度鈀之循環伏安結果 24
4-9-4擔載不同銀含量試片之循環伏安結果 24
第五章　討論 25
5-1 陽極氧化參數對於二氧化鈦奈米管結構之影響 25
5-1-1偏壓對於二氧化鈦奈米管結構之影響 25
5-1-2 氟離子濃度對於二氧化鈦奈米管結構之影響 25
5-1-3蝕刻液pH值對於二氧化鈦奈米管結構之影響 26
5-1-4 溫度對於二氧化鈦奈米管結構之影響 27
5-1-5不同甘油含量與純甘油對於二氧化鈦奈米管結構之影響 28
5-2擔載銀、鈀於不同孔徑二氧化鈦奈米管後對其在0.5M H2SO4 之氧還原催化活性之影響 30
第六章結論與未來展望 32
6-1結論 32
6-2 未來展望 33
第七章參考文獻 34

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指導教授

林景崎(Jing-Chie Lin)

審核日期

2010-8-27

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