臺灣博碩士論文加值系統

　　本研究應用真空濺鍍法(sputtering) 製備銦錫氧化薄膜(indium-tin oxide, ITO)及二氧化鈦光觸媒薄膜，並進行複合改質光觸媒單層與多層製程TiO2/ITO對丙酮之光催化分解效率之測試，並進一步探討濺鍍製程參數(包括氧氬比、溫度、載體基材、濺鍍時間與濺鍍層數)及光催化操作參數（包括光波長、水氣含量、氧氣含量、丙酮初始濃度、光觸媒種類）對丙酮分解效率之影響。
　　本研究以自製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（單層厚度為355.3、396.6、437.5、487.5、637.5 nm TiO2/ITO、單層、雙層、三層TiO2/ITO)及水氣含量(0、50、100、200、300 ppm)。光催化反應器上方置放照射光源（3 支15 W近紫外光燈管、藍光LED、綠光LED），內部則置入TiO2/ITO光觸媒薄膜之試片，丙酮則以氣密式注射針筒(gasket syringe)注入，進行光催化氧化分解實驗。反應物分析係以氣相層析儀/火燄離子偵測器加以偵測並定量之。
　　本研究製備之TiO2/ITO光觸媒薄膜晶型主要屬銳鈦礦結構，僅有少部分的金紅石結構。其薄膜厚度單層約為473.5 nm，雙層約為506.0 nm。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/毛玻璃與TiO2//玻璃次之。本研究結果發現不論濺鍍150 min 單層或雙層TiO2/ITO在反應溫度50°C、氧氣濃度20%及水氣添加量 100 ppm條件下，可達最佳丙酮分解效率。由反應動力分析結果得知，異相光催化分解丙酮在單層TiO2/ITO為零階反應，而雙層TiO2/ITO則在高濃度為零階反應，低濃度為一階反應。ITO可有效提升TiO2之光催化效能改質光觸媒，在可見光照藍光的照射下，單層TiO2/ITO對丙酮之分解速率為2.353×10-5 μmole/cm2-s，而雙層TiO2/ITO對丙酮之分解速率為3.478×10-5 μmole/cm2-s。
　　此外， 本研究應用相互競爭且反應之雙分子Langmuir-Hinshelwood (L-H)反應動力模式，建立丙酮之光催化反應動力模式，模擬在不同反應溫度、丙酮初始濃度及水氣添加量下，光催化分解丙酮之反應情形。模式模擬結果顯示，實驗值與模擬值具高度相關性，亦能成功模擬光催化分解丙酮之反應速率。

This study applied sputtering technology to prepare composite film
photocatalyst TiO2/ITO for investigating the decomposition efficiency of
acetone using composite TiO2/ITO made by single- and multi-layer
processes. The influences of operating parameters, including sputtering
operating parameters and photocatalytic operating parameters, on the
decomposition efficiency of acetone were further investigated.
Operating parameters investigated for the sputtering process included
oxygen to argon ratio (O2/Ar), temperature, substrate, sputtering dutation,
and sputtering layers, while operating parameters investigated for the
photocatalytic decomposition of acetone included light wavelength, H2O
concentration, O2 concentration, initial acetone concentration, and the
type of photocatalysts.
In the experiments, acetone was degraded by the composite film
photocatalyst TiO2/ITO in a self-designed batch photocatalytic reactor.
Operating parameters included light wavelength (350~400 nm, 435~500
nm, 506~600 nm), the type of photocatalysts (single-layer film
photocatalyst TiO2/ITO with the thickness of 355.3, 396.6, 437.5, 487.5,
and 637.5 nm; double- and triple-layer TiO2/ITO), H2O concentration (0,
50, 100, 200, and 300 ppm). The incident light with different
wavelength irradiated with three 15-W lamps of near UV light or LED
lamps of blue and green lights placed on the top of the photocatalytic
reactor. Acetone was injected into the reactor by using a gasket syringe
and vaporized for further photocatalytic degradation on the film
photocatalyst TiO2/ITO placed at the bottom of the reactor. Air samples
were taken to analyze acetone concentration with a GC/FID.
The composite film photocatalyst TiO2/ITO was mainly composed
of anatase with a few rutile. The thicknesses of the single- and
IV
double-layer film photocatalyst with the thickness of 473.5 nm and 506.0
nm, respectively. Experimental results indicated that the highest
decomposition efficiency of acetone was obtained by using TiO2/ITO,
followed by TiO2/ground glass and TiO2/glass. The highest
decomposition efficiency of acetone was observed by using TiO2/ITO at
50°C, 20% O2, and 100 ppm H2O. In the kinetic model, the acetone
decomposition of single-layer TiO2/ITO was zero-order reaction. The
acetone decomposition of double-layer TiO2/ITO in high initial acetone
concentration was zero-order reaction, while that in low initial acetone
concentration was first-order reaction. Thus, the decomposition of
acetone exerted by TiO2 film photocatalyst can be enhanced efficiently by
ITO. Under the incidence of blue light, the reaction rate of acetone
decomposition were 2.353×10-5 and 3.478×10-5 μmole/cm2-s for using
single- and double-layer TiO2/ITO, respectively.
Finally, a bimolecular Langmuir-Hinshelwood (L-H) kinetic model
was applied to simulate the influences of initial acetone concentration,
temperature, and relative humidity on the promotion and inhibition for
the photocatalytic degradation of acetone. This study revealed that the
L-H kinetic model could successfully simulate the photocatalytic reaction
rate of acetone.

目錄
謝誌………………………………………………………………………….. Ⅰ
中文摘要…………………………………………………………………….. Ⅱ
英文摘要…………………………………………………………………….. Ⅳ
目錄………………………………………………………………………….. Ⅵ
表目錄……………………………………………………………………….. Ⅸ
圖目錄……………………………………………………………………….. Ⅹ
第一章 前言….................….................….................…................................. 1-1
1-1 研究緣起............….................….................…............................ 1-1
1-2 研究目的............….................….................…............................ 1-3
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….................….................…............................ 2-4
2-2-1 二氧化鈦化學結構特性..............…................................. 2-4
2-2-2 二氧化鈦光催化反應............…....................................... 2-6
2-3 二氧化鈦改質之製備方法................…...................................... 2-8
2-3-1 真空濺鍍法………………………………………........... 2-10
2-3-2 改質二氧化鈦製備可見光光觸媒………………........... 2-13
2-3-3 銦－錫氧化導電薄…………………………................... 2-16
2-4 影響光催化反應效率之參數.......….......................................... 2-19
2-4-1 光波長之影響…………….............................................. 2-19
2-4-2 反應溫度之影響............................................................... 2-20
2-4-3 水氣含量之影響…........................................................... 2-22
2-4-4 氧氣濃度之影響…………………………………........... 2-23
2-5 光催化反應動力分析.................................................................. 2-24
2-5-1 光催化反應步驟………………………………………... 2-24
V I
2-5-2 等溫吸附模式…………………………………………... 2-25
2-5-3 反應動力模式…………………………………………... 2-27
2-5-4 速率決定步驟…………………………………………... 2-31
2-5-5 反應速率常數和吸附平衡常數與反應溫度之關係…... 2-32
2-5-6 反應速率隨溫度變化之關係…………………………... 2-34
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 濺鍍前基材前處理………………………….................... 3-3
3-1-3 實驗濺鍍製程…………………………………………… 3-3
3-2 光催化分解實驗............................................................................... 3-10
3-2-1 實驗材料........................................................................... 3-10
3-2-2 批次式光催化反應系統.................................................. 3-11
3-2-3 載體吸附實驗測試………………………………........... 3-13
3-2-4 均相光催化反應測試…………………………….......... 3-13
3-2-5 異相光反應測試………………………………….......... 3-14
3-2-6 不同波長範圍之光源設計…………………………….. 3-14
3-2-7 操作參數及範圍.............................................................. 3-15
3-2-8 採樣與分析系統.............................................................. 3-17
3-2-9 品保與品管....................................................................... 3-17
第四章 結果與討論........................................................................................ 4-1
4-1 真空濺鍍系統製程參數對生成TiO2/ITO薄膜特性分析結果....... 4-1
4-1-1 表面形貌SEM 分析........................................................ 4-1
4-1-2 表面形貌AFM 分析….…………….............................. 4-6
4-1-3 結晶性Raman 光譜分析…….………………………… 4-20
4-1-4 XRD 光譜分析…………..…………..…………………. 4-23
4-2 光催化氧化反應背景測試結果....................................................... 4-27
V II
4-2-1 系統測試結果.................................................................... 4-27
4-2-2 均相光解反應測試結果.................................................... 4-27
4-2-3 載體吸附測試結果............................................................ 4-29
4-3 光催化氧化反應實驗操作參數之影響……..…………................. 4-30
4-3-1 載體基材種類對於光催化分解丙酮反應之影響..……. 4-30
4-3-2 光觸媒種類對於光催化氧化反應之影響…...………… 4-32
4-3-3 反應溫度對於光催化氧化反應之影響…........................ 4-36
4-3-4 水氣含量對於光催化氧化反應之影響………………… 4-38
4-3-5 氧氣含量對於光催化氧化反應之影響…………........... 4-40
4-3-6 光波長對於光催化氧化反應之影響……………........... 4-43
4-3-7 丙酮初始濃度對於光催化氧化反應之影響……........... 4-46
4-4 光源能量對分解丙酮之影響……………........................................ 4-47
4-5 光催化反應動力模式之解析……………………………………... 4-48
第五章 結論與建議........................................................................................ 5-1
5-1 結論.............................................................................................. 5-1
5-2 建議…………………………………………………………….. 5-2
參考文獻………………….............................................................................. R-1
附錄A 反應物及產物之分析圖………………………………...………….. A-1
附錄B 反應物丙酮之檢量線……..………………………………………... B-1

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