臺灣博碩士論文加值系統

本研究以溶劑熱法製備Bi2WO6奈米光觸媒，並加入二氧化錫(SnO2)進行改質，形成SnO2/Bi2WO6複合材料，以C.I. Reactive Red 2 (RR2)為有機污染物進行光催化降解實驗。
將合成的SnO2/Bi2WO6複合材料由X光繞射儀 (X-ray diffraction, XRD) 鑑定晶相、比表面積分析儀 (BET) 測量比表面積、描式電子顯微鏡 (Scanning electron microscope, SEM) 與穿透式電子顯微鏡 (Transmission electron microscope, TEM) 觀察觸媒表面形貌、傅立葉轉換紅外光譜 (Fourier transform infrared spectroscopy, FTIR)及電子能譜儀 (X-ray photoelectron spectrometer, XPS) 進行觸媒化學鍵結之分析與測定元素組成、紫外-可見光光譜儀(UV-Vis spectrophotometer)分析臨界吸收波長並計算觸媒能隙值、光激螢光分光光譜儀(Photoluminescence, PL)鑑定電子電洞重組率，最後以界達電位 (Zeta-potential) 測定觸媒表面電位。
XRD結果可知，改質前後之Bi2WO6，皆符合Bi2WO6標準圖譜晶相，且隨著SnO2比例增加，SnO2特徵峰越明顯，由BET測量發現隨SnO2含量增加，比表面積隨之下降，並以UV-Vis分析得知SnO2含量增加導致能隙由2.85 eV增加至2.97 eV，產生藍移現象，由PL測定經由SnO2改質Bi2WO6後，皆可有效抑制電子及電洞發生重組反應，以界達電位測量得知改質前Bi2WO6等電位點 (Zero point charge, ZPC)為pH = 2.2，經由SnO2改質後之ZPC皆有效提升，此時觸媒表面具有較多正電荷，染料容易被觸媒吸附，進而提高反應效率。
本研究在400 W 氙燈 (Xe lamp)照射下進行光催化反應，改質前其Bi2WO6反應60分鐘之RR2去除率為82.9%，由擬一階反應方程式計算，其反應常數為0.0258 min-1，經由SnO2改質之Bi2WO6，其最佳化為錫鎢莫耳比0.5 (Sn/W = 0.5)，RR2去除率為94.6%，反應常數提升至0.0463 min-1，且從自由基實驗得知在光催化實驗中，電洞 (h+)為主要的反應物種，超氧自由基 (O2-•)為其次，而氫氧自由基 (HO•)在反應中含量最少。最後測試觸媒的再利用性，由實驗得知改質前Bi2WO6之第一次循環實驗效率為82.9%，第三次循環實驗效率為63.9%，效率下降了19.0%，而經由SnO2改質後之Bi2WO6觸媒，其第一次循環實驗效率為94.6%下降至第三次循環實驗效率為89.3%，僅下降5.3%，故改質後可以大幅提升其再利用性及穩定性。

This study prepared Bi2WO6 via the solvothermal method and modified Bi2WO6 by tin oxide (SnO2) doping to from SnO2/Bi2WO6. The photocatalytic activity of Bi2WO6 and SnO2/Bi2WO6 was determined by the photodegradation of C.I. Reactive Red 2 (RR2) under a 400 W Xe lamp irradiation.
The surface characteristics of prepared photocatalysts were determined by X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET) surface area analysis, scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), UV-vis spectroscopy (UV-vis), zeta potential meter, Fourier-transform infrared spectrometer (FTIR), and photoluminescence spectrometer (PL). The results of XRD indicated that all of the diffraction peaks of prepared photocatalysts match the standard data of Bi2WO6. After the SnO2 doping, the intensity of SnO2 diffraction peak gradually increases with the increasing of SnO2 content. The specific surface area of Bi2WO6 decreased with the increase of added SnO2 does in solvothermal method. The UV-Vis spectra of SnO2/Bi2WO6 displayed a blue shift in the band gap transition. The results of PL indicated that SnO2 doping to form SnO2/Bi2WO6 decreased the recombination of photogenerated electrons and holes in Bi2WO6. The zero point charge (ZPC) of Bi2WO6 and SnO2/Bi2WO6 (at Sn/W = 0.5) was 2.2 and 3.4, respectively.
After 60 min reaction, the RR2 photodegradation efficiency of Bi2WO6 and SnO2/Bi2WO6 (at Sn/W = 0.5) was 82.9% and 94.6%, respectively; moreover, the RR2 photodegradation rate constants of Bi2WO6 and SnO2/Bi2WO6 (at Sn/W = 0.5) were 0.0258 and 0.0463 min-1, respectively. The results of active species trapping experiments revealed that photogenerated hole (h+) was the major active species in the photocatalytic process of Bi2WO6 and SnO2/Bi2WO6. The recycling runs of RR2 photodegradation over Bi2WO6 and SnO2/Bi2WO6 were performed to evaluate their photocatalytic stability. The RR2 photodegradation in Bi2WO6 and SnO2/Bi2WO6 (at Sn/W = 0.5) systems decreased from 82.9% to 63.9% and 94.6% to 89.3% after three recycling runs. The reusability and stability of SnO2/Bi2WO6 exceeded that of Bi2WO6.

摘要 I
ABSTRACT III
致謝 V
目錄 VI
表目錄 VIII
圖目錄 X
第一章緒論 1
1-1 研究動機 1
1-2研究目的與內容 2
第二章文獻回顧 3
2-1高級氧化程序 3
2-1-1光觸媒催化 4
2-2偶氮染料 5
2-3 Bi2WO6 8
2-4 Bi2WO6金屬氧化物改質 11
第三章實驗方法 14
3-1藥品及儀器 14
3-2實驗流程及操作變因 15
3-2-1 Bi2WO6摻雜SnO2改質 16
3-3光催化活性實驗 18
3-4樣品表面物性分析 23
第四章結果與討論 28
4-1實驗樣品圖 28
4-2表面特性分析 29
4-2-1晶相分析 (XRD) 29
4-2-3掃描式電子顯微鏡 (SEM) 32
4-2-4穿透式電子顯微鏡 (TEM) 39
4-2-5官能基鑑定分析 (FTIR) 42
4-2-6元素組成分析 (XPS) 44
4-2-7固相紫外-可見光譜儀 (UV-Vis Spectrophotometer) 50
4-2-8 PL光激發螢光光譜 (Photoluminescence Spectra) 51
4-2-9表面電性分析 (Zeta Potential) 52
4-3光催化反應探討 54
4-3-1直接光解 54
4-3-2 Bi2WO6及改質後之光降解比較 54
4-3-3觸媒劑量效應 57
4-3-4 RR2濃度效應 59
4-3-5 RR2之pH效應 60
4-3-6自由基捕捉實驗 62
4-3-7觸媒再利用實驗 64
4-3-8動力學模擬 66
4-3-9實際應用:太陽光降解實驗 69
第五章 結論與建議 72
5-1結論 72
5-2建議 73
參考文獻 74

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