臺灣博碩士論文加值系統

本研究是以高壓水熱法合成碘氧化鉍複合石墨相氮化碳(graphitic carbon nitride, g-C3N4)及氧化石墨烯 (Graphene Oxide, GO)，g-C3N4是以三聚氰胺在馬弗爐(Muffle Furnace)內鍛燒540℃合成，GO則是使用修改後Hummer 法來進行合成，g-C3N4及石墨烯皆具有單層sp2結構，能增加電子電洞轉移的面積，能降低光觸媒的重組率。碘氧化鉍在不同pH值會有不同的晶形，如BiOI、Bi4O5I2、Bi7O9I3、Bi5O7I等，藉由在不同pH值下跟g-C3N4及GO複合，合成出不同晶形的複合光觸媒，觸媒樣品以X射線粉末繞射圖(XRD)、場發掃描式電子顯微鏡(FE-SEM )、場發穿透式電子顯微鏡(FE-TEM)、X射線光電子能譜圖(XPS )、光激發螢光光譜(PL)、紫外光-可見光漫反射光譜(DRS)、氮氣吸脫附曲線圖及比表面積測定(BET)、傅立葉轉換紅外線光譜(FT -IR)、電子順磁共振圖譜（EPR）等儀器分析產物的組成，並探討不同晶形碘氧化鉍複合g-C3N4及石墨烯對於光催化效率的影響。結晶紫(Crystal Violet, CV)及水楊酸(Salicylic Acid, SA)為常見環境有機汙染物，本研究利用光催化反應降解有機物，再利用HPLC-PDA- MS技術分離、鑑定其降解中間物，研究在未來可將此複合觸媒用於環境中有機汙染物處理和控制。

In this study, a series of the bismuth oxyiodide composite graphene oxide (GO) or graphitic carbon nitride (g-C3N4) are prepared using autoclave hydrothermal methods. In the preparation procedure, g-C3N4 is synthesized by calcinations at 540℃ in muffle furnace , and graphene oxide is synthesized by Hummer method modified. Graphene and g-C3N4 are the two-dimensional atomic crystal available for enhancing electron-hole transfer surface and reduce the recombination rate of photocatalyst. Bismuth oxyiodide, with different crystalline in different pH vm alue, can synthesize different bismuth oxyiodide composite graphene or g-C3N4 photocatalysts. The structures and morphologies of BiOxIy/g-C3N4 or graphene oxide photocatalysts are characterized by XRD, FE-TEM, SEM-EDS, HR-XPS, DR-UV, BET, EPR and PL. Discuss different crystalline bismuth oxyiodide composite graphene or g-C3N4 affect the photocatalytic efficiency. Crystal Violet and Salicylic acid is a common organic pollutants in the environment. The study is useful for photocatalytic degradation of organic samples and use HPLC-PDA-MS for separation and identification of degradation intermediates. The study is useful for degrading the organic compounds in the future applications of environmental pollution and control.

摘要 ......................................................................................................... I
英文摘要 ................................................................................................... II
第一章 緒論 ............................................................................................ 1
1.1 研究動機 ...................................................................................... 1
1.2 研究目的 ...................................................................................... 2
第二章 文獻回顧 ..................................................................................... 3
2.1 染料及染整廢水之特性與危害 .................................................. 3
2.1.1染料之特性及三苯甲烷類染料 ............................................ 3
2.1.2染整廢水之特性與危害 ........................................................ 4
2.2染料廢水處理技術 ......................................................................... 5
2.2.1 高級氧化程序 ...................................................................... 6
2.2.2 光催化氧化法 ........................................................................ 7
2.3水楊酸工業應用及汙染 ................................................................. 7
2.4碘氧化鉍 ....................................................................................... 8
2.5石墨烯及氧化石墨烯 ..................................................................... 9
2.6石墨相碳氮化合物(g-C3N4) ......................................................... 10
第三章 實驗材料與方法 ........................................................................ 12
3.1實驗材料與設備 ............................................................................. 13
3.1.1 有機物 ...................................................................................... 13
3.1.2 實驗藥品 ................................................................................ 14
3.1.2.1碘氧化鉍的製備藥品 ........................................................ 14
3.1.2.2氧化石墨烯和g-C3N4的製備藥品 ................................. 14
3.1.2.3測試染料廢水藥品 ............................................................ 14
3.1.2.4高效能液相層析電灑質譜儀(HPLC-ESI-MS)分析藥
品 ...................................................................................... 15
3.1.3 實驗設備 .................................................................................. 15
3.2實驗步驟 ....................................................................................... 16
3.2.1氧化石墨烯的製備 ................................................................ 16
3.2.2複合石墨烯光觸媒的製備 ...................................................... 17
3.2.3石墨相氮化碳的製備 .............................................................. 17
3.2.2複合g-C3N4光觸媒的製備 ..................................................... 18
IV
3.2.3 照光程序 ................................................................................ 19
3.3儀器與分析方法 ............................................................................. 20
3.3.1材料特性分析 ........................................................................... 20
3.3.2分離與鑑定 ............................................................................... 21
第四章 結果與討論 ................................................................................ 22
4.1 BiOxIy/ GO之表面特性分析 ......................................................... 22
4.1.1 BiOxIy/GO改變不同GO克數 (pH值=1) ............................ 23
4.1.1.1 X射線粉末繞射圖 ........................................................ 23
4.1.1.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 24
4.1.1.3紫外光-可見光漫反射光譜 ............................................. 26
4.1.1.4傅立葉轉換紅外線光譜 .................................................. 27
4.1.1.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 29
4.1.1.6光激發螢光光譜 .............................................................. 31
4.1.1.7光降解效率圖 .................................................................. 32
4.1.2 BiOxIy/GO改變不同GO克數 (pH值=4) ............................ 35
4.1.2.1 X射線粉末繞射圖 ........................................................ 35
4.1.2.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 36
4.1.2.3紫外光-可見光漫反射光譜 ............................................. 38
4.1.2.4傅立葉轉換紅外線光譜 .................................................. 39
4.1.2.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 41
4.1.2.6光激發螢光光譜 .............................................................. 43
4.1.2.7光降解效率圖 .................................................................. 44
4.1.3 BiOxIy/GO改變不同GO克數 (pH值=7) ............................ 48
4.1.3.1 X射線粉末繞射圖 ........................................................ 48
4.1.3.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 49
4.1.3.3紫外光-可見光漫反射光譜 ............................................. 51
4.1.3.4傅立葉轉換紅外線光譜 .................................................. 52
4.1.3.5 X射線光電子能譜圖 ....................................................... 54
4.1.3.6氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 59
4.1.3.7光激發螢光光譜 .............................................................. 61
4.1.3.8光降解效率圖 .................................................................. 62
4.1.4 BiOxIy/GO改變不同GO克數 (pH值=10) .......................... 66
4.1.4.1 X射線粉末繞射圖 ........................................................ 66
V
4.1.4.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 67
4.1.4.3紫外光-可見光漫反射光譜 ............................................. 69
4.1.4.4傅立葉轉換紅外線光譜 .................................................. 70
4.1.4.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 72
4.1.4.6光激發螢光光譜 .............................................................. 74
4.1.4.7光降解效率圖 .................................................................. 75
4.1.5 BiOxIy/GO改變不同GO克數 (pH值=13) ........................ 79
4.1.5.1 X射線粉末繞射圖 ........................................................ 79
4.1.5.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 80
4.1.5.3紫外光-可見光漫反射光譜 ............................................. 82
4.1.5.4傅立葉轉換紅外線光譜 .................................................. 83
4.1.5.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 85
4.1.5.6光激發螢光光譜 .............................................................. 87
4.1.5.7光降解效率圖 .................................................................. 88
4.2 BiOxIy/ g-C3N4之表面特性分析 92
4.2.1 BiOxIy/ g-C3N4改變重量比(pH值=1) .................................... 92
4.2.1.1 X射線粉末繞射圖 ........................................................ 92
4.2.1.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 93
4.2.1.3紫外光-可見光漫反射光譜 ............................................. 96
4.2.1.4傅立葉轉換紅外線光譜 .................................................. 98
4.2.1.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 99
4.2.1.6光激發螢光光譜 .............................................................. 101
4.2.1.7光降解效率圖 .................................................................. 102
4.2.2 BiOxIy/ g-C3N4改變重量比(pH值=4) .................................... 104
4.2.2.1 X射線粉末繞射圖 ........................................................ 104
4.2.2.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 105
4.2.2.3紫外光-可見光漫反射光譜 ............................................. 107
4.2.2.4傅立葉轉換紅外線光譜 .................................................. 109
4.2.2.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 110
4.2.2.6光激發螢光光譜 .............................................................. 112
4.2.2.7光降解效率圖 .................................................................. 113
4.2.3 BiOxIy/ g-C3N4改變不同g-C3N4克數 (pH值=7) ................. 115
4.2.3.1 X射線粉末繞射圖 ........................................................ 115
VI
4.2.3.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 116
4.2.3.3紫外光-可見光漫反射光譜 ............................................. 118
4.2.3.4傅立葉轉換紅外線光譜 .................................................. 119
4.2.3.5 X射線光電子能譜圖 ....................................................... 120
4.2.3.6氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 125
4.2.3.7光激發螢光光譜 .............................................................. 126
4.2.3.8光降解效率圖 .................................................................. 128
4.2.4 BiOxIy/ g-C3N4改變重量比(pH值=10) .................................. 132
4.2.4.1 X射線粉末繞射圖 ........................................................ 132
4.2.4.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 133
4.2.4.3紫外光-可見光漫反射光譜 ............................................. 135
4.2.4.4傅立葉轉換紅外線光譜 .................................................. 137
4.2.4.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 138
4.2.4.6光激發螢光光譜 .............................................................. 140
4.2.4.7光降解效率圖 .................................................................. 141
4.2.5 BiOxIy/ g-C3N4改變重量比(pH值=13) .................................. 143
4.2.5.1 X射線粉末繞射圖 ........................................................ 143
4.2.5.2 場發穿透式電子顯微鏡及場發掃描式電子顯微鏡 ..... 144
4.2.5.3紫外光-可見光漫反射光譜 ............................................. 146
4.2.5.4傅立葉轉換紅外線光譜 .................................................. 148
4.2.5.5氮氣吸脫附曲線圖及比表面積、孔隙測定 .................. 149
4.2.5.6光激發螢光光譜 .............................................................. 151
4.2.5.7光降解效率圖 .................................................................. 152
4.3 光催化實驗 ................................................................................. 155
4.3.1回收觸媒降解效率變化 ......................................................... 155
4.3.1.1 BiOxIy/GO回收降解效率 ................................................ 155
4.3.1.2 BiOxIy/ g-C3N4回收降解效率 .......................................... 157
4.3.2光催化反應之活性物種測定 ................................................. 158
4.3.3電子順磁共振圖譜 ................................................................. 161
4.3.4光催化過程中結晶紫溶液的UV-Vis PDA光譜 ................. 164
4.3.5光催化過程中改變結晶紫溶液的pH 值 ............................. 165
4.3.6光催化反應機制圖 ................................................................. 166
4.3.7結晶紫染料光催化過程中間產物之分析 ............................. 167
VII
4.4 實驗分析總整理 ........................................................................... 172
4.4.1 BiOxIy/GO材料分析及降解速率比較 ................................... 172
4.4.2 BiOxIy/ g-C3N4 材料分析及降解速率比較 ............................ 173
第五章 結論與建議 .............................................................................. 175
5.1 結論.............................................................................................. 175
5.2 未來方向與建議 ......................................................................... 176
參考文獻 ................................................................................................... 177

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