Decolorization of dye compounds in aqueous solution by VUV-based advanced oxidation processes
Nguyen Thi Hang、申永順
E-mail: [email protected]
ABSTRACT
The purpose of this study is to investigate the reaction behaviors of the decomposition of dye-containing wastewaters by VUV-based advanced oxidation processes (AOPs). The effects of pH value, VUV intensity, initial dye concentration, initial H2O2 concentration, and TiO2 loading dose on the degradation of three azo dyes: acid Orange 8, acid Blue 29, and acid Blue 113 were studied to explore and compare the treatment efficiencies among the adopted AOPs. The degradation of three azo dyes was observed during VUV irradiation, while they were not oxidized by H2O2 alone and TiO2 alone. It was found that pH represented as an important role which affected strongly on the degradation of three dyes. For VUV/H2O2, VUV/TiO2, and VUV/TiO2/H2O2 processes, the decoloration rates of three azo dyes were always decomposed more efficiently at acidic condition than those at alkaline condition except VUV only process. Especially, three azo dyes were considered to disappear in a short time at acidic condition by VUV/TiO2 and VUV/TiO2/H2O2 process because of their absorption on positively charged TiO2 surface. The effect of VUV intensity on the degradation efficiency of dyes was negligible. On the other hand, the degradation rates of dyes increased with increasing of H2O2 concentration, but the reaction rates would be retarded while H2O2 concentration was too high because it acted as a scavenger of hydroxyl radical. The results also indicated that the degradation rate decrease with increasing of azo dye concentration. The optimal concentration of TiO2 applied in this study was 0.5 g/L, some degradation rates of dyes would decrease if exceeding this optimal dose because of the blocking effect on VUV of TiO2. The decomposition rates of mono-azo dye (i.e. acid Orange 8) were found to be larger than those of di-azo dye (i.e. acid Blue 29), and amino-azo benzene of diazo dye (i.e. acid Blue 113). The experimental results were explained based on the differences among their molecular structure. The effect of VUV direct photolysis among the VUV-based AOPs can not be negligible because three azo dyes can be decomposed efficiently by VUV irradiation. The treatment efficiency of dyes by VUV/TiO2/H2O2 process was the worst one possibly due to the excess effects of TiO2 and H2O2 dose to retard the generation of hydroxyl radicals. A pseudo-first order kinetic was established for the four VUV-base AOPs. However, kinetic for direct photolysis reaction acted as zero-order that was better well fitted than the first order reaction. The K absorption behaviors of three azo dyes on TiO2 surface were determined based on the Langmui-Hinshelwood kinetic model. In addition, a kinetic model with pseudo-steady state assumption (PSSA) was established according to the generally accepted elementary reaction in VUV/H2O2 process. The rate constant for the reaction between dyes and hydroxyl radicals was found by fitting the experimental data to the PSSA kinetic model.
Keywords : advanced oxidation processes ; VUV irradiation ; azo dyes ; wastewater treatment ; VUV/TiO2 ; VUV/H2O2 ; VUV/TiO2/H2O2
Table of Contents
博碩士論文暨電子檔案上網授權書iii ABSTRACTiv 中文摘要vi ACKNOWLEDGMENTSviii CONTENTSix LIST OF TABLESxiii LIST OF FIGURESxv LIST OF SYMBOLSxxii Chapter I. INTRODUCTION1 1.1 Background1 1.2 Motivation2 1.3 Objective and scope3 Chapter II. LITERATURE REVIEW5 2.1 Dye wastewater5 2.2 Advanced Oxidation Processes6 2.3 VUV only process7 2.3.1 UV radiation7 2.3.2 VUV only process8 2.4 VUV/H2O2 process11 2.5 VUV/ TiO2 process13 2.5.1 Titanium and Titanium dioxide13 2.5.2 VUV/ TiO2 process15 2.6 VUV/TiO2/H2O2 system18 2.7 Reaction kinetics20 2.7.1 Homogeneous reactions20 2.7.2 Heterogeneous reactions23 2.8 Influence of process parameters24 2.8.1 Effect of UV intensity24 2.8.2 Effect of pH solution25 2.8.3 Effect of H2O2 concentration on decolorization of azo dye 28 2.8.4 Effect of TiO2 dosage30 Chapter III. EXPERIMENTAL PROCEDURE AND ANALYSIS36 3.1 Materials36 3.1.1 Azo dye compounds36 3.1.2 Other chemicals38 3.2 Apparatus39 3.3 Experimental setup40 Chapter IV. RESULTS AND DISCUSSION47 4.1 The acid dissociation constant (Ka) of azo dye solutions47 4.2 The degradation of azo dye compounds by VUV only process51 4.2.1 The effect of pH on the degradation of azo dyes in aqueous solution by VUV only process52 4.2.2 The effect of VUV intensity on the degradation of azo dye compounds in aqueous solution by VUV only process56 4.3 The degradation of azo dyes in aqueous solution by VUV/H2O2 process59 4.3.1 The degradation of three dyes in aqueous solution by H2O2 oxidation process59 4.3.2 The determination of absorption coefficient of three dyes and hydrogen peroxide61 4.3.3 The effect of pH on the degradation of three azo dyes in aqueous
solution by VUV/H2O2 process64 4.3.4 The effect of VUV intensity on the degradation of azo dyes in aqueous solution by VUV/H2O2 process72 4.3.5 The effect of initial H2O2 concentration on the degradation of azo dyes by VUV/H2O2 process75 4.3.6 The effect of initial concentration of three azo dye solutions on their degradation80 4.3.7 Kinetic model development83 4.4 The degradation of azo dyes by VUV/TiO2 process88 4.4.1 The degradation of azo dyes in aqueous solution by TiO2 only89 4.4.2 The kinetic for VUV/TiO2 photo-oxidation of three azo dyes and the effect of dye concentration91 4.4.3 The effect of pH on the degradation of azo dye solutions by VUV/TiO2 process98 4.4.4 The effect of TiO2 dose on the degradation of three azo dyes in aqueous solution by VUV/TiO2 process105 4.4.5 Discussion of the Intermediates and Reaction Pathways108 4.5 The degradation of three azo dyes in aqueous solution by VUV/TiO2/H2O2 process113 4.5.1 The effect of pH on the degradation of three azo dyes in aqueous solution by VUV/TiO2/H2O2 process114 4.5.2 The effect of TiO2 dose on the degradation of three azo dyes in aqueous solution by VUV/TiO2/H2O2 process119 4.5.3 The effect of H2O2 concentration on the degradation of three azo dyes in aqueous solution by VUV/TiO2/H2O2 process123 4.6 Comparison treatment efficiency among azo dyes by different Advanced Oxidation Processes127 4.6.1 The comparison of these four processes at acidic condition127 4.6.2 The comparison of these four processes at neutral condition130 4.6.3 The comparison of these four processes at alkaline condition132 4.6.4 The comparison of oxidation efficiency per mmole of oxidants136 Chapter V. CONLUSION AND RECOMENDATION138 5.1 Conclusion138 5.2 Recommendation139 REFERENCES141 APPENDIX149
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