臺灣博碩士論文加值系統

本研究於光纖表面批覆TiO2光觸媒，並藉由光纖的光傳輸特性，可在有限的光反應器空間做有效的光強度分佈，提高光的利用率，減少能量損失。因此利用光纖運用於管狀連續反應器，以光觸媒程序來進行氣相異丙醇之氧化。藉由含浸法將TiO2均勻披覆於已撥離反射層之光纖上，在光觸媒反應部分，將利用光觸媒催化氧化異丙醇，分析光觸媒催化效率，探討有關紫外光強度、反應物濃度、反應物滯留時間、相對濕度等操作因素對反應物的轉化率之影響及反應動力行為。並藉由紫外光發光二極體(UV-LED)能夠提供週期性照射之特性，應用於光觸媒催化程序，分析週期性照射於處理污染物之影響。實驗結果發現：當提高空氣中之相對濕度，由於水分子與異丙醇對活性位置進行競爭吸附，因此光觸媒催化之活性因而降低，相較於連續照射，當操作於週期照射環境下能將光量子效率由0.78%提升至1.28%，另外，在相同之亮/暗週期比率下，提高頻率能夠同時提升去除效率以及光量子效率。
本研究亦開發光電觸媒催化反應器，將外加電位施加於氣相光觸媒催化反應程序中，以減少光觸媒電極表面之電子–電洞再結合，研究中探討有關外加偏壓強度、相對濕度、初始濃度以及紫外光強度等操作因素對反應物的轉化率之影響，由實驗結果得知，相較於光觸媒催化程序，光電觸媒催化程序於具有濕度之環境下仍有一定量之去除率；光陽極之電流密度受到外加偏壓強度、相對濕度、紫外光強度的影響較大，卻不受異丙醇初始濃度之變化而受影響；其中濕度對於整個光電觸媒催化程序具有顯著的效應；此外，相較於以提升光強度方式增加反應效率，外加電位可進而提高光子的利用率並減少50 %之能耗。

Photocatalytic decomposition of isopropanol presented in gas stream was investigated using a continuous, tubular photoreactor loaded with single TiO2-coated optical fiber under controlled UV periodic illumination. The effects of UV light intensity, initial concentration of target compound, retention time and humidity on the photocatalytic efficiency for the oxidation of isopropanol. The TiO2 particles were coated on optical fiber through dip-coating process. UV light emitting diodes (UV-LEDs) will be utilized as the light source to enhance the utilization of UV light by applying periodic illumination on the oxidation of isopropanol. The introduction of humidity retarded the decomposition of isopropanol because of the competition between water and isopropanol molecules for the active sites on TiO2 surface. Operated at retention time of less than one second, about 21% isopropanol was decomposed for experiments conducted with initial isopropanol concentration of 10 ppmv. The apparent quantum yield was increased from 0.78 to 1.28 for experiments conducted with UV-LED as the light source operated at duty cycle shifted from 1.0 to 0.1. At the operation of equivalent duty cycle, both removal efficiencies and quantum yield was also enhanced in the highly frequent periodic illumination by decreasing both light and dark periods.
Electrochemical enhancement for photocatalytic decomposition of isopropanol in gas phase was carried out in a photoelectrocatalytic reactor. The effects of bias potential, relative humidity, initial isopropanol concentration and UV light intensities were investigated for the photoelectrocatalytic process. Photoelectrocatalytic decomposition of isopropanol was observed to be less sensitive to humidity for experiments applied with bias potential higher than 2.5V. Electrical current densities of photoanode were highly corresponded to the variation of bias potentials, relative humidity levels and UV light intensities, however independent of inlet isopropanol concentrations. Humidity presented a controversial effect for photocatalytic decomposition rate of isopropanol within the application of bias potential. Experimental results also exhibited that the energy consumption of photoelectrocatalytic process was much less than photocatalytic process to achieve similar isopropanol decomposition.

Table of Content
Chinese Abstract I
English Abstract III
Acknowledgment V
Table of Content VI
List of Figures IX
List of Tables XIV
List of Symbols XV

Chapter
1 Introduction 1
1.1 Background 1
1.2 Objectives and scope 3
2 Literature Review 4
2.1 Photocatalysis 5
2.1.1 Fundamental of photocatalysis 5
2.1.2 Mechanism and kinetics of photocatalysis 7
2.1.3 Operating factors affecting photocatalysis 13
2.2 Photoelectrocatalysis 24
2.2.1 Fundamental of photoelectrocatalysis 25
2.2.2 Solid electrolyte 30
2.3 Development of Photoreactor 35
2.3.1 Photoreactor applied for periodic irradiation 37
2.3.2 Optical fiber reactor 48
2.3.3 Photoelectrochemical reactor 58
3 Materials and Experiments 69
3.1 Materials and apparatus 69
3.2 Photocatalytic and photoelectrocatalytic activity 70
3.3 Experimental procedures 76
3.3.1 Experimental framework 76
3.3.2 Coating procedure of TiO¬2 78
3.3.3 Background experiments 78
3.3.4 Photocatalysis under periodic illumination 87
3.3.5 Gas phase photoelectrocatalysis 91
4 Results and Discussion 93
4.1 Photocatalytic decomposition of gaseous isopropanol in a tubular optical fiber reactor under periodic UV-LED illumination 94
4.1.1 Characterizations of TiO2-coated optical fiber 95
4.1.2 Effect of inlet relative humidity 97
4.1.3 Effect of inlet isopropanol concentration 99
4.1.4 Effect of UV light intensity 101
4.1.5 Effect of duty cycle 103
4.1.6 Effect of irradiation frequency 106
4.2 Photoelectrocatalytic decomposition of gaseous isopropanol in a polymer electrolyte cell 108
4.2.1 Characterizations of TiO2-coated photoanode 109
4.2.2 Effect of applied bias 112
4.2.3 Effect of inlet relative humidity 116
4.2.4 Effect of inlet isopropanol concentration 123
4.2.5 Effect of UV light intensity 126
4.2.6 Reaction kinetic of photoelectrocatalytic decomposition of gaseous isopropanol in a polymer electrolyte cell 129
4.2.7 Energy consumption of photoelectrocatalytic process 131
5 Conclusions and Recommendations 132
Reference 137
Appendix 150
Vita 151

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