本研究利用真空濺鍍法(sputtering)製備銦錫氧化薄膜 (indium-tin oxide, ITO)及氮摻雜改質之二氧化鈦光觸媒，進行改質光觸媒（TiO2/ITO、TiO2/N）與未改質光觸媒（TiO2）對丙酮之光催化分解效率之測試，並進一步探討光催化操作參數（光波長、相對濕度）對丙酮分解效率之影響。
本研究採用批次式光催化反應器進行光催化分解丙酮實驗，實驗探討之操作參數包括光波長 (350~400 nm、435~500 nm、506~600 nm)、觸媒種類（TiO2/ITO、TiO2/N、TiO2)及相對濕度(0％、50%、100%)。光催化反應器上方置放照射光源（4支20W近紫外光燈管、藍光LED、綠光LED），內部則置放披覆光觸媒薄膜之試片，丙酮則以氣密式注射針筒(gasket syringe)注入，進行光催化氧化反應實驗。反應物及產物分析係以氣相層析儀/火燄離子偵測器配合甲烷轉換器加以偵測並定量之。
本研究製備之改質光觸媒呈四角柱狀晶型，其寬度為100~200 nm、薄膜厚度約為4.0μm。光敏感度分析結果發現，TiO2/ITO之紅移效果比TiO2/N及TiO2明顯，而TiO2/N又略優於TiO2。異相光催化分解丙酮實驗結果得知，以TiO2/ITO之分解效率為最高，TiO2/N與TiO2次之，但TiO2/N分解丙酮之效率又略優於 TiO2。本研究結果發現以TiO2/ITO在照射UV光、相對濕度50%條件下，可達最佳丙酮分解效率。由本實驗分析結果得知，異相光催化分解丙酮為零階反應。ITO可有效改質光觸媒，在可見光照射下，對光催化分解丙酮之效率有一定程度之提昇，且與光敏感度分析結果一致。

This study investigated the decomposition efficiency of acetone using unmodified (pure TiO2) and modified TiO2 (TiO2/ITO、TiO2/N) prepared by sputtering technology. The influence of operating parameters including wavelength and relative humidity on the decomposition efficiency of acetone was further discussed. Operating parameters investigated included light wavelength (350~400, 435~500, and 506~600 nm), photocatalysts (TiO2/ITO, TiO2/N, and TiO2), and relative humidity (RH) (0%, 50%, and 100%).
In the experiments, acetone was degraded by photocatalysts in a self-designed batch photocatalytical reactor. Samples coated with TiO2 were placed in the batch reactor. The incident light with different wavelength was irradiated by a 20-watt lamp. Moreover, a low-pressure mercury lamp for UV light or LED lamps for blue and green lights were placed on the top of reactor. Acetone was injected into reactor by using a gasket syringe. Reactants and products were analyzed quantitatively by a gas chromatography with a flame ionization detector followed by a methaneizer (GC/FID-Methaneizer).
The structure of the photocatalyst film surface showed taper and the width of column ranged from 100 to 200 nm. The film structure showed crystallization cylindrical surface and the thickness of the photocatalyst film was in the range of 4.0-4.3 μm. The highest decomposition efficiency of acetone was observed by using TiO2/ITO under visible-light with 50% RH. The synthesis of TiO2 was mainly anatase for the tested photocatalysts. AFM images showed that the photocatalyst surface appeared rugged and the shape showed a mountain ridge distribution .

Keywords: sputtering technology, modified photocatalysts, photosensitive, acetone, photocatalytic oxidation, acetone decomposition

目錄
謝誌…………………………………………………………………. Ⅰ
中文摘要……………………………………………………………. Ⅱ
英文摘要……………………………………………………………. Ⅲ
目錄…………………………………………………………………. Ⅳ
表目錄………………………………………………………………. Ⅴ
圖目錄………………………………………………………………. Ⅵ
第一章 前言….................….................….................….................... 1-1
1-1 研究緣起............….................….................….................... 1-1
1-2 研究目的............….................….................….................... 1-2
1-3 研究範圍............….................….................….................... 1-5
第二章 文獻回顧............….................….................…..................... 2-1
2-1 光觸煤之發展趨勢及應用...….................…...................... 2-1
2-2 二氧化鈦光觸煤….................….................….................... 2-3
2-2-1 二氧化鈦結構特性....….................…...................... 2-3
2-2-2 二氧化鈦之光催化反應............…........................... 2-6
2-3 二氧化鈦改質之製備方法................….............................. 2-8
2-3-1 真空濺度法………………………………………... 2-10
2-3-2 改質二氧化鈦製備可見光光觸媒………………... 2-11
2-3-3 銦錫氧化導電薄膜………………………… 2-14
2-4 揮發性有機物之光催化反應.......…................................... 2-15
2-4-1揮發性有機物之來源與性質.................................... 2-15
2-4-2 異相光催化反應....................................................... 2-19
2-4-3 光催化反應機制....................................................... 2-21
2-5 影響光催化反應效率之參數.............................................. 2-23
2-5-1 光波長之影響........................................................... 2-23
2-5-2 溫度之影響………................................................... 2-25
2-5-3 水氣含量之影響....................................................... 2-25
第三章 研究方法............................................................................... 3-1
3-1 實驗設備與材料.................................................................. 3-1
3-1-1濺鍍設備……………………………….................... 3-1
3-1-2真空濺鍍法製備二氧化鈦及ITO薄膜……............ 3-2
3-2 光催化氧化實驗設計.......................................................... 3-5
3-2-1 實驗材料................................................................... 3-5
3-2-2 批次式光催化氧化反應系統................................... 3-6
3-2-3 載體吸附測試……………………………………... 3-7
3-2-4 均相光反應測試…………………………………... 3-8
3-2-5 異相光反應測試…………………………………... 3-8
3-2-6 不同波長範圍之光源設計……………………… 3-8
3-2-7 操作參數及範圍..................................................... 3-11
3-2-8 採樣與分析系統...................................................... 3-11
3-2-9 品保與品管............................................................. 3-13
3-3 反應物及產物分析方法...................................................... 3-16
第四章 結果與討論.......................................................................... 4-1
4-1光觸媒基本特性分析結果................................................... 4-1
4-1-1 光敏感度分析…....................................................... 4-1
4-1-2表面粗糙度………….……………........................... 4-4
4-1-3 薄膜厚度分析……………..………………………. 4-4
4-1-4 晶相分析…………………………………………... 4-12
4-2 光催化氧化反應背景測試結果.......................................... 4-14
4-2-1系統測試結果............................................................ 4-14
4-2-2均相光解反應測試結果............................................ 4-15
4-2-3載體吸附測試結果.................................................... 4-16
4-3光催化氧化反應之影響探討……………………………... 4-18
4-3-1光觸媒種類對於光催化氧化反應之影響………… 4-18
4-3-2光波長對於光催化氧化反應之影響……………… 4-21
4-3-3水氣對於光催化氧化反應之影響............................ 4-23
4-4光催化分解丙酮……………………................................... 4-26
4-4-1光催化分解丙酮之反應速率………........................ 4-26
4-4-2光催化分解丙酮之反應階數……………………… 4-27
4-5光源能量對分解丙酮之影響…………………………….. 4-31
4-6分解丙酮之產物分析……………………………………... 4-36
第五章 結論與建議.......................................................................... 5-1
5-1 結論...................................................................................... 5-1
5-2 建議……………………………………………………….. 5-3
參考文獻…………………................................................................. 6-1
附錄………......................................................................................... A-1

表目錄
表1-1 主要半導體材料的能隙和化學安定性…................... 1-4
表2-1 銳鈦礦與金紅石之物理特性比較.................….................. 2-5
表2-2 不同觸媒製備方法之優缺點比較………………………... 2-10
表2-3 大氣中常見揮發性有機化合物之種類....................... 2-17
表2-4 室內空氣中典型的有機性溶劑........................................... 2-18
表2-5 丙酮之物理及化學特性…................................................... 2-19
表3-1 光催化分解實驗之操作參數及範圍…………………….. 3-12
表3-2 品保及品管查核結果一覽表………………………….… 3-15
表3-3 氣相層析儀GC HP 5890之操作條件……………............. 3-17
表3-4 氣相層析儀�火焰離子偵測器-HP6890甲烷轉化器之操作條件……………………................................................... 3-18
表4-1 金紅石(Rutile)與銳鈦礦(Anatase) TiO2之XRD繞射峰位置表………………………………………………………... 4-14
表4-2 不同觸媒種類在不同燈源及不同相對濕度下之反應速率常數彙整表……………………………………………... 4-27



圖目錄
圖1-1 照光下的半導體光觸媒............................................................... 1-3
圖1-2 氮摻雜改質TiO2光觸媒示意圖........................................….. 1-4
圖1-3 光催化氧化實驗流程圖…........................................................... 1-6
圖2-1 常用半導體之能隙……………………………………………... 2-4
圖2-2 二氧化鈦光觸媒之應用領域…………………….…………….. 2-4
圖2-3 銳鈦礦與金紅石之晶格結構………………............................... 2-6
圖2-4 觸媒受光激發生成電子與電洞之能階位置圖……………....... 2-7
圖2-5 N摻雜 TiO2之UV-VIS吸收光譜圖…....................................... 2-12
圖2-6 S摻雜TiO2與TiO2之UV圖譜.................................................. 2-13
圖2-7 二氧化鈦薄膜於ITO導電薄膜上受光激發後電子電洞分離傳導圖……………………………………………………………. 2-15
圖2-8 不同電子轉移型式圖…………………………………………... 2-21
圖2-9 波長與能量關係圖……………………………………………... 2-24
圖2-10 溫度影響丙酮之分解趨勢圖…………………………...……… 2-25
圖2-11 水氣濃度影響丙酮分解速率之趨勢圖………………………... 2-26
圖3-1 英國GENCOA公司TWINLAB型濺鍍系統…...……………. 3-2
圖3-2 封閉式非平衡磁控濺鍍設備構造示意圖…….……...………... 3-5
圖3-3 批次式光催化氧化反應系統示意圖…….…………...………... 3-9
圖3-4 紫外燈管之光波長分佈……………………………….……….. 3-9
圖3-5 藍、綠LED燈之光源實體圖…………………………………. 3-10
圖3-6 藍色LED燈之光波長分佈…………………………………….. 3-10
圖3-7 綠色LED燈之光波長分佈…………………………………….. 3-11
圖4-1 不同觸媒種類之UV-VIS吸收光譜……………………………. 4-3
圖4-2 不同觸媒種類之UV-VIS穿透率光譜…………………………. 4-3
圖4-3 TiO2/ITO之表面粗糙度3D型態……………………………….. 4-5
圖4-4 TiO2/N之表面粗糙度3D型態…………………………………. 4-5
圖4-5 TiO2之表面粗糙度3D型態……………………………………. 4-6
圖4-6 TiO2/ITO放大37,000倍之SEM圖…………………………….. 4-7
圖4-7 TiO2/N放大37,000倍之SEM圖……………………………….. 4-8
圖4-8 TiO2放大37,000倍之SEM圖………………………………….. 4-8
圖4-9 TiO2/ITO放大100,000倍之SEM圖…………………………… 4-9
圖4-10 TiO2/N放大100,000倍之SEM圖……………………………… 4-9
圖4-11 TiO2放大100,000倍之SEM圖………………………………… 4-10
圖4-12 TiO2/ITO放大15,000倍之剖面SEM圖……………………….. 4-10
圖4-13 TiO2/N放大20,000倍之剖面SEM圖………………………….. 4-11
圖4-14 TiO2放大40,000倍之剖面SEM圖…………………………….. 4-11
圖4-15 TiO2/ITO之XRD分析圖……………………………………….. 4-13
圖4-16 TiO2/N、TiO2之XRD分析圖…………………………………… 4-13
圖4-17 批次式光氧化反應器之壓力測試結…………………………... 4-16
圖4-18 均相光解反應測試結果………………………………………... 4-17
圖4-19 試片吸附反應測試結果………………………………………... 4-17
圖4-20 在UV光照射下不同光觸媒分解丙酮效率隨時間之變化趨勢圖………………………………………………………………... 4-19
圖4-21 在藍光照射下不同光觸媒分解丙酮效率隨時間之變化趨勢圖…………................................................................................... 4-20
圖4-22 在綠光照射下不同光觸媒分解丙酮效率隨時間之變化趨勢圖…………................................................................................... 4-20
圖4-23 TiO2/ITO在不同波長下分解丙酮濃度隨時間之變化趨勢圖... 4-22
圖4-24 TiO2/N在不同波長下分解丙酮濃度隨時間之變化趨勢圖…... 4-22
圖4-25 TiO2在不同波長下分解丙酮濃度隨時間之變化趨勢圖……... 4-23
圖4-26 TiO2/ITO在不同濕度下分解丙酮濃度隨時間之變化趨勢圖... 4-24
圖4-27 TiO2/N在不同濕度下分解丙酮濃度隨時間之變化趨勢圖…... 4-24
圖4-28 TiO2在不同濕度下分解丙酮濃度隨時間之變化趨勢圖……... 4-25
圖4-29 在UV光照射下不同光觸媒分解丙酮效率反應階數示意圖… 4-28
圖4-30 TiO2/ITO在不同濕度、不同燈源下分解丙酮之反應速率常數 4-28
圖4-31 TiO2/N在不同濕度、不同燈源下分解丙酮之反應速率常數…. 4-29
圖4-32 TiO2在不同濕度、不同燈源下分解丙酮之反應速率常數……. 4-30
圖4-33 TiO2/ITO之反應速率常數與波長之關係趨勢圖……………... 4-32
圖4-34 TiO2/N之反應速率常數與波長之關係趨勢圖………………... 4-32
圖4-35 TiO2之反應速率常數與波長之關係趨勢圖…………………... 4-33
圖4-36 反應速率常數與光能量之關係趨勢圖………………………... 4-35
圖4-37 產物隨時間之生成趨勢圖……………………………………... 4-36
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