臺灣博碩士論文加值系統

近年來，全球面對日益嚴重的環境污染與污染物處理問題，積極尋求合適的解決方法，加上能源緊縮，以至於科學家無不找尋再生能源期望為世界帶來一道曙光。此時由光驅動的光催化劑則被視為切合之技術，能在污染物降解與太陽能轉化中引起重要的作用。
本研究合成一系列溴氧化鉍/碘氧化鉍/石墨相氮化碳（BiOxBry / BiOmIn / g-C3N4）作為光催化反應的複合半導體材料。合成出的觸媒樣品透過X射線粉末繞射儀(XRD)、紫外光-可見光漫反射光譜儀(UV-vis DRS)、場發式掃描電子顯微鏡附能量散射光譜儀(FE-SEM-EDS)、場發式穿透電子顯微鏡附能量散射光譜儀(FE-TEM-EDS)、傅立葉轉換紅外線光譜儀(FT-IR)、高解析電子能譜儀(HR-XPS)、光激發螢光光譜儀(PL)、比表面積分析儀(BET)、電子順磁共振光譜儀(EPR)、紫外光光電子能譜儀(UPS)等儀器鑑定產物的組成和特性。實驗表明在一系列BiOxBry / BiOmIn / g-C3N4 合成觸媒實現了太陽能驅動的光催化降解結晶紫染料（Crystal Violet, CV）和水楊酸（Salicylic Acid, 2-HBA），以及將光催化還原CO2為CH4的成果，在研究中提出並討論光催化機制。
研究結果顯示，複合的BiOxBry / BiOmIn 系列樣品中降解結晶紫染料最高速率k值原本只有0.1967h-1，但複合的BiOxBry / BiOmIn / g-C3N4最高降解效率變為0.2888h-1有提高的效果，顯示這些觸媒具有光催化能力。另外將最佳觸媒進行五次回收使用，效率仍維持在94%，表示這些觸媒具有重複使用的價值。而在光催化還原 CO2反應時，BB2I1-200-7與BB2I1-200-7-C3N4-10的CH4的產量最高分別達63.81 ppm與 49.82 ppm，進而達成綠色化學之目標。

In face of worsening environmental pollution and pollutant treatment problems in past years, suitable solutions are positive searched globally. Moreover, energy crunch has scientists search renewable energy for a light at the end of the tunnel. In this case, light-driven photocatalysts are regarded as a suitable technology to induce important function in pollutant degradation and solar energy conversion.
A series of bismuth bromide oxide/bismuth oxyiodide/graphitic carbon nitride (BiOxBry / BiOmIn / g-C3N4) are synthesized as the compound semiconductor material for photocatalytic reaction. The synthesized catalyst samples are tested the composition and characteristics with X-ray powder diffractometer (XRD), ultraviolet-visible diffusion reflectance spectrophotometer (UV-vis DRS), field emission scanning electron microscope: energy dispersive spectrometer (FE-SEM-EDS), Fourier transform infrared spectrometer (FT-IR), high resolution X-ray photoelectron spectroscopy (HR-XPS), photoluminescence spectrometer (PL), surface area and porosimetry analyzer (BET), electron paramagnetic resonance spectrometer (EPR), and ultraviolet photoelectron spectroscopy (UPS). The experiment reveals that the series of BiOxBry / BiOmIn / g-C3N4 synthesized catalysts realize solar energy driven photocatalysis degrading crystal violet dye (CV) and salicylic acid (2-HBA) as well as photocatalytic reduction of CO2 to CH4. The photocatalysis mechanism is proposed and discussed in the research.
The research results show that the maximum speed k for degrading crystal violet dye among the compound BiOxBry / BiOmIn samples is merely 0.1967h-1, but the maximal degradation efficiency in the compound BiOxBry / BiOmIn / g-C3N4 appears 0.2888h-1. The increase reveals the photocatalytic analysis of such catalysts. Furthermore, the optimal catalysts are reused for 5 times, and the efficiency remains 94%, showing the value of such catalysts being repeatedly used. During the photocatalytic reduction of CO2, BB2I1-200-7 and BB2I1-200-7-C3N4-10 appear the highest CH4 production 63.81 ppm and 49.82 ppm, respectively, to further achieve the goal of green chemistry.

摘要 I
Abstract II
第一章 緒論 1
1-1研究動機 1
1-2研究目的 2
第二章 文獻探討 3
2-1結晶紫 3
2-2水楊酸 4
2-3染料廢水處理技術 5
2-4高級氧化程序 6
2-5光催化氧化法 6
2-6光催化還原二氧化碳 7
2-7光觸媒 8
2-8石墨相氮化碳(g-C3N4) 10
第三章 實驗材料與方法 11
3-1研究架構 11
3-2實驗藥品 12
3-2-1三元鹵氧化鉍製備藥品 12
3-2-2異質複合材料 12
3-2-3光催化活性實驗藥品 12
3-2-4活性物種試劑 12
3-3觸媒合成方法 13
3-3-1觸媒合成器材與設備 13
3-3-2石墨相氮化碳(g-C3N4)之製備 13
3-3-3溴氧化鉍/碘氧化鉍之製備 14
3-3-4溴氧化鉍/碘氧化鉍/石墨相氮化碳之製備 15
3-4複合光觸媒樣品代碼表 16
3-5觸媒成分鑑定及特性分析儀器 17
3-5-1儀器規格 17
3-5-2儀器對觸媒特性分析 18
3-6光觸媒降解汙染物實驗方法 19
3-6-1降解實驗器材與設備 19
3-6-2照光位置測驗 20
3-6-3暗室時間確認 21
3-6-4照光程序 22
3-7測定活性物種 23
3-8 光催化還原二氧化碳實驗方法 24
3-8-1 實驗器材與設備 24
3-8-2 實驗程序 25
第四章 結果與討論 26
4-1分析BiOxBry / BiOmIn之表面特性 26
4-1-1 X射線粉末繞射儀(XRD) 27
4-1-1-1 BB1I2在100 °C改變pH值 28
4-1-1-2 BB1I2在150 °C改變pH值 30
4-1-1-3 BB1I2在200 °C改變pH值 32
4-1-1-4 BB1I2在250 °C改變pH值 34
4-1-1-5 BB2I1在100 °C改變pH值 37
4-1-1-6 BB2I1在150 °C改變pH值 39
4-1-1-7 BB2I1在200 °C改變pH值 41
4-1-1-8 BB2I1在250 °C改變pH值 43
4-1-2紫外光-可見光漫反射光譜儀(UV-vis DRS) 46
4-1-2-1 BB1I2在100 °C改變pH值 47
4-1-2-2 BB1I2在150 °C改變pH值 48
4-1-2-3 BB1I2在200 °C改變pH值 49
4-1-2-4 BB1I2在250 °C改變pH值 50
4-1-2-5 BB2I1在100 °C改變pH值 51
4-1-2-6 BB2I1在150 °C改變pH值 52
4-1-2-7 BB2I1在200 °C改變pH值 53
4-1-2-8 BB2I1在250 °C改變pH值 54
4-1-3場發式掃描電子顯微鏡附能量散射光譜儀(FE-SEM-EDS) 57
4-1-4比表面積分析儀(BET) 60
4-2 BiOxBry / BiOmIn之光催化活性探討 61
4-2-1光降解效率圖 61
4-2-1-1 BB1I2在100 °C改變pH值 62
4-2-1-2 BB1I2在150 °C改變pH值 63
4-2-1-3 BB1I2在200 °C改變pH值 64
4-2-1-4 BB1I2在250 °C改變pH值 65
4-2-1-5 BB2I1在100 °C改變pH值 66
4-2-1-6 BB2I1在150 °C改變pH值 67
4-2-1-7 BB2I1在200 °C改變pH值 68
4-2-1-8 BB2I1在250 °C改變pH值 69
4-3 分析BiOxBry / BiOmIn / g-C3N4之表面特性 71
4-3-1 X射線粉末繞射儀(XRD) 71
4-3-2傅立葉轉換紅外線光譜儀(FT-IR) 73
4-3-3紫外光-可見光漫反射光譜儀(UV-vis DRS) 74
4-3-4場發式掃描電子顯微鏡附能量散射光譜儀(FE-SEM-EDS) 77
4-3-5場發式穿透電子顯微鏡附能量散射光譜儀(FE-TEM-EDS) 78
4-3-6高解析電子能譜儀(HR-XPS) 81
4-3-7比表面機分析儀(BET) 87
4-3-8光激發螢光光譜儀(PL) 89
4-4 BiOxBry/BiOmIn/g-C3N4之光催化活性探討 90
4-4-1光降解效率圖 90
4-4-2活性物種確認 97
4-4-3電子順磁共振光譜儀(EPR) 98
4-4-4光催化反應機制圖 100
4-4-5回收再利用 102
4-5 光催化還原二氧化碳之探討 103
第五章 結論與建議 106
5-1結論 106
5-2建議 107
參考文獻 108

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