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研究生:林倚楨
研究生(外文):Yi-Chen Lin
論文名稱:天然有機物於臭氧降解程序中氫氧自由基之生成與消耗及其去除新興污染物之影響
論文名稱(外文):Effect of natural organic matter on the formation and consumption of OH radical and removal of emerging contaminants in ozonation
指導教授:林逸彬
指導教授(外文):Yi-Pin Lin
口試委員:蔣本基侯嘉洪
口試委員(外文):Pen-Chi ChiangChia-Hung Hou
口試日期:2015-07-13
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:環境工程學研究所
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2015
畢業學年度:103
語文別:英文
論文頁數:44
中文關鍵詞:臭氧天然有機物(NOM)起始劑促進劑抑制劑活化能和新興污染物
外文關鍵詞:ozoneNatural organic matter (NOM)initiatorpromoter and inhibitoractivation energy and emerging contaminants
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臭氧被廣泛應用於去除自來水和廢水中的有機污染物,近幾年來更是運用於降解地表水及地下水中之新興污染物。由於天然有機物(NOM)與臭氧及氫氧自由基的反應相當複雜,所以天然有機物在臭氧處理程序中之影響尚未被闡明。故本研究的目的為:(1)測定天然有機物於臭氧處理程序中起始反應(initiation)、促進反應(promotion)、抑制反應(inhibition)以及與臭氧直接反應之速率常數。(2) 探討pH值及溫度對起始反應、促進反應、抑制反應以及與臭氧直接反應速率常數之影響。(3) 測定及模擬天然有機物於臭氧處理程序中對新興污染物去除之影響。本研究所使用之四種自然水體為:新店溪(新北市)、宜蘭河(宜蘭市)、金沙水庫(金門縣)及台中地下水(台中縣)。結果顯示起始反應、抑制反應及與臭氧的直接反應之速率常數會隨著pH值升高而增加,但促進反應之速率常數則明顯的趨勢。在溫度影響的部分,所有的速率常數皆是隨著溫度的升高而增加。在天然有機物於臭氧處理程序下對新興污染物降解影響的部分,從結果顯示都可利用所測得之速率常數得到良好的預測結果。

Ozonation has been widely used for removing organic contaminants in water treatment. The effect of natural organic matter (NOM) on this process, however, is not well understood due to the complex reactions of NOM with ozone and •OH generated from ozone decomposition. The objectives of this study are to determine the rate constants of NOM from different sources in terms of initiation, promotion, inhibition and direct ozone reactions in the ozonation process and to investigate the influences of NOM on the removal of emerging contaminants. The rate constants of NOM in four natural waters including Hsintien river (New Taipei City), Yilan river (Yilan City), Jinsha reservoir (Kinmen County) and Taichung groundwater (Taichung County) were determined using a recently developed approach that integrates the pseudo first order ozone decomposition kinetics, transient steady state •OH concentration and the Rct concept. The effects of pH value and temperature on the rate constants were also determined. With these rate constants, the influences of NOM on the degradation of three emerging contaminants including ibuprofen, acetylsulfamethoxazole and metoprolol can be fairly well predicted.

TABLE OF CONTENT
摘要 i
SUMMARY ii
TABLE OF CONTENT iii
LIST OF FIGURES v
LIST OF TABLES vi
ABBREVIATIONS vii
Chapter 1 INTRODUCTION 1
1.1. Research background 1
1.2. Objectives 2
Chapter 2 LITERATURE REVIEW 4
2.1. Basic properties of ozone 4
2.2. Ozonation of organic compounds 5
2.3. The Rct concept and modified Rct model 8
2.4. Ozonation of emerging contaminants 12
CHAPTER 3 MATERIALS AND METHODS 15
3.1. Chemicals 15
3.2. Stock Solutions 15
3.3. Natural waters 16
3.4. Ozonation experiments 17
3.5. Analytical method 18
Chapter 4 RESULTS AND DISCUSSION 21
4.1. Determination of the initiation, promotion, inhibition and direct ozone reaction rate constants of NOM in surface water and groundwater 21
4.2. Effect of pH value on NOM rate constants 30
4.3. Effect of temperature on NOM rate constants 31
4.4. Quantify and model the effects of NOM on the degradation of ibuprofen, acetylsulfamethoxazole and metoprolol 35
Chapter 5 CONCLUSIONS AND RECOMMENDATIONS 39
5.1. Conclusions 39
5.2. Recommendations for future study 40
REFERENCES 42


LIST OF FIGURES
Figure 1.1. Reactions of ozone with the presence of foreign compounds acting as the initiator, promoter and inhibitor 5
Figure 4.1. Ozone decomposition for natural waters in the presence of 0-0.3 mM tert-butanol 22
Figure 4.2. The Rct plots for natural waters in the presence of 0-0.3 mM tert-butanol 23
Figure 4.3. The plots of 1/Rct vs kSS[S] for four natural waters 27
Figure 4.4. The plots of kobs vs. Rct for four natural waters 28
Figure 4.5. The Arrhenius plot for different reaction modes of Yilan river NOM 34
Figure. 4.6 Effect of pH value on the degradation of ibuprofen, acetylsulfamethoxazole and metoprolol in Yilan river water 37
Figure. 4.7 Effect of temperature on the degradation of ibuprofen, acetylsulfamethoxazole and metoprolol in Yilan river water 38




LIST OF TABLES
Table 2.1 Physical properties of ozone 4
Table 3.1. Characteristics of natural waters used in this study 17
Table 4.1. The second stage Rct values determined for the four natural waters in the presence of 0-0.3 mM tert-butanol 24
Table 4.2. The second-order rate constants of initiation (kI), promotion (kP), inhibition (kS) and direct reaction (kD) for NOM in four natural waters 29
Table 4.3. The relative contributions of direction reaction (kD) vs. initiation (kI) in the reaction between ozone and NOM and the relative contributions of promotion (kP) vs. inhibition (kS) in the reaction between •OH and NOM for the four natural waters 29
Table. 4.4 The initiation (kI), promotion (kP), inhibition (kS) and direct reaction (kD) rate constants for Yilan river NOM at pH 6.0-8.0 31
Table 4.5. The initiation (kI), promotion (kP), inhibition (kS) and direct reaction (kD) rate constants for Yilan river NOM at 10-30 0C 33
Table. 4.6 The rate constants with •OH are similar and those with ozone differ substantially as show below water 35


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