臺灣博碩士論文加值系統

本研究以超音波輔助Hummers法製備氧化石墨烯，以循環伏安法進行氧化石墨烯的電沉積，並還原於二氧化鈦奈米管陣列膜上，製備出石墨烯複合二氧化鈦奈米管陣列膜。用不同光源作比較，以光電催化進行染料溶液去除效率之影響研究，並且以開路電壓，閉路電流，交流阻抗進行電化學分析。本研究結果顯示石墨烯複合二氧化鈦奈米管陣列膜在紫外光照射下，其染料降解效率比二氧化鈦奈米管陣列膜效果佳；外加偏壓1 V下，加入0.1 M的氯化鉀溶液，有最佳的光電催化降解效率；在甲基橙溶液濃度提高至30 mg/L下仍有良好的降解效率。相對於二氧化鈦奈米管陣列膜，石墨烯複合二氧化鈦奈米管陣列膜之光電流有提升，與染料降解效率之提升相呼應，証實石墨稀複合之二氧化鈦奈米管陣列膜可提升整體反應效率。同樣地，甲基橙溶液的可見光光催化與光電催化反應顯示，石墨烯複合二氧化鈦奈米管陣列膜，比二氧化鈦奈米管陣列膜的催化能力強。

The ultrasonic and Hummers method were used in this study to prepare graphene oxide. The cyclic voltammetry was used for reduction of graphene oxide to graphene and deposition of graphene on the TiO2 nanotube array film. Thus, the graphene composited TiO2 nanotube array film was prepared. The photoelectrocatalysis of dye solution and its degradation efficiency was implemented with visible light and UV. The open-circuit voltage, closed circuit current and AC impedance of electrochemical analysis were implemented. The results showed that the dye degradation efficiency of the graphene composite TiO2 nanotube array film in UV-irradiation is better than that of TiO2 nanotube array film. With bias of 1 V, the addition of 0.1 M potassium chloride resulted in the optimum photoelectrocatalytic degradation efficiency. The degradation efficiency is still good when the methyl orange solution concentration is increased to 30 mg/L. The photocurrent of graphene composite TiO2 nanotube array film was increased compared with TiO2 nanotube array film. The results proving that the graphene composite TiO2 nanotube array film can increase the overall photoelectrocatalytic efficiency. In the same way, photocatalysis and photoelectrocatalysis of methyl orange solution with the visible light showed that the graphene composite TiO2 nanotube array film also has better catalytic efficiency than TiO2 nanotube array film.

總目錄
摘要..........I
Abstract..........II
總目錄..........IV
表目錄..........VI
圖目錄..........VII
第一章 前言..........1
第二章 文獻回顧..........3
2.1二氧化鈦晶體結構與特性..........3
2.2二氧化鈦奈米管陣列膜製備..........7
2.3光催化與光電催化..........9
2.4光催化之光電效應..........17
2.5二氧化鈦電極平帶電位..........22
2.6石墨烯複合二氧化鈦奈米管陣列膜..........25
2.7交流阻抗譜之應用..........32
第三章 材料與方法..........34
3.1實驗架構圖..........34
3.2實驗儀器設備..........38
3.3實驗材料及藥劑..........39
3.4二氧化鈦奈米管陣列膜製備..........41
3.5石墨烯製備..........42
3.6石墨烯以循環伏安法電解複合二氧化鈦奈米管陣列膜..........43
3.7光電催化反應系統..........44
3.8電化學量測..........47
第四章 結果與討論..........48
4.1不同光源降解染料之影響..........49
4.2外加偏壓以紫外光照射降解染料之影響..........52
4.3外加偏壓以可見光照射降解染料之影響..........56
4.4 TNT/G以紫外光照射降解染料之染料濃度變化..........60
4.5 TNT/G以可見光照射降解染料之染料濃度變化..........63
4.6 TNT/G以紫外光照射降解染料之電解質濃度變化..........66
4.7 TNT/G以可見光照射降解染料之電解質濃度變化..........69
4.8不同光源照射之閉路光電流..........72
4.9不同光源照射之開路光電壓..........74
4.10不同電極之交流阻抗..........77
第五章 結論..........81
參考文獻..........82
表目錄
表2.1不同二氧化鈦晶型之物化特性比較表..........6
表2.2光電催化程序之相關文獻整理..........14
表2.1碳材料複合二氧化鈦合成光觸媒之文獻整理..........26
表2.2國外應用石墨烯作為複合觸媒之文獻整理..........30
表3.1實驗儀器設備..........38
表3.2實驗材料-1..........39
表3.3實驗材料-2..........40
表3.4實驗藥劑..........40
圖目錄
圖2.1二氧化鈦三種主要的晶相結構..........5
圖2.2陽極氧化製備奈米管之結構成長示意圖..........8
圖2.3二氧化鈦催化反應機制..........9
圖2.4液相光伏特電池示意圖..........12
圖2.5在受光及外加偏壓下電子-電洞在TiO2/電極行徑圖..........17
圖2.6 n型半導體與溶液物種接觸前後能帶分佈示意圖..........19
圖3.1實驗架構..........34
圖3.2二氧化鈦奈米管陣列膜製備流程..........35
圖3.3超音波輔助Hummers法合成氧化石墨烯製備流程..........36
圖3.4石墨烯以循環伏安法電解製備流程..........37
圖3.5陽極氧化電解裝置..........42
圖3.6循環伏安電解裝置..........44
圖3.7光電催化反應裝置..........46
圖4.1不同光源照射降解染料之降解率變化..........50
圖4.2不同光源照射降解染料之反應速率常數..........51
圖4.3 TNT-UV降解染料之降解率變化..........53
圖4.4 TNT/G-UV降解染料之降解率變化..........54
圖4.5外加偏壓以紫外光照射降解染料之反應速率常數..........55
圖4.6 TNT-W降解染料之降解率變化..........57
圖4.7 TNT/G-W降解染料之降解率變化..........58
圖4.8外加偏壓以可見光照射降解染料之反應速率常數..........59
圖4.9 TNT/G-UV之染料濃度降解率效應..........61
圖4.10 TNT/G-UV之染料濃度反應速率常數..........62
圖4.11 TNT/G-W之染料濃度降解率效應..........64
圖4.12 TNT/G-W之染料濃度反應速率常數..........65
圖4.13 TNT/G-UV之電解質濃度降解率效應..........67
圖4.14 TNT/G-UV之電解質濃度反應速率常數..........68
圖4.15 TNT/G-W之電解質濃度降解率效應..........70
圖4.16 TNT/G-W之電解質濃度反應速率常數..........71
圖4.17石墨烯複合二氧化鈦之閉路電流比較..........73
圖4.18石墨烯複合二氧化鈦之開路電壓..........75
圖4.19石墨烯複合二氧化鈦之開路電壓比較..........76
圖4.20不同電極未照光之交流阻抗..........78
圖4.21不同電極以紫外光照射之交流阻抗..........79
圖4.22不同電極以可見光射之交流阻抗..........80

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