臺灣博碩士論文加值系統

隨著人們對於個人健康和生活品質要求的提高，藥品的生產和使用量與日俱增。與此同時，生活污水和製藥工業廢水中所包含的藥品，因其對自然環境和人體存在潛在的影響，已成為一項不可忽視的問題。由於廢水中的藥品成分複雜且濃度較低，傳統活性污泥法和物理處理程序在去除藥品時效果有限，因此臭氧降解等高級氧化程序更加受到關注。藥品及相關有機污染物在和臭氧反應時機制複雜，可能可以直接與臭氧反應，又可以在臭氧降解的自由基鍊式反應中扮演起始劑 (initiator)、促進劑 (promoter)以及抑製劑 (inhibitor)的角色。由於藥品在反應中的角色和動力學機制尚未得到充分闡明，因此本研究的目的為：(1) 選擇特定6種藥品，利用現有的臭氧自由基鍊式反應模型，測定藥品在臭氧處理程序中與臭氧直接反應、起始反應、促進反應以及抑制反應的速率常數；(2) 基於測得之反應速率常數，模擬藥品在臭氧降解過程中的濃度變化，並與實際情況進行比對分析。結果顯示，6種藥品的四個速率常數可以被實驗分別測得，但相較於文獻中藥品與臭氧或自由基反應之總速率常數，其結果在不同程度上偏大；模擬的結果表明，受到中間產物及水中痕量有機物等可能原因之影響，尚不能有效模擬降解過程，整體模擬之降解速率偏快。在後續的實驗中，減少中間產物和背景值的干擾，提升速率常數的精確度是需要關注的主要問題。

With the higher demand for personal health and better quality of life, the productions and usages of pharmaceuticals increased over the years. Because of the potential impacts on ecology and human health, the removal of pharmaceuticals from the aquatic environments is highly desirable. The effectiveness of removing pharmaceuticals from wastewater by conventional wastewater treatment processes has been found to be limited for some pharmaceuticals. Advanced oxidation processes such as ozonation have received more attentions to remove these compounds. With diverse functional groups in the structures, pharmaceuticals could potentially react directly with ozone, as well as react as the initiator, promoter and inhibitor in the OH radical chain reactions resulting from ozone decomposition, which have not been considered before. The purposes of this study are (1) to determine the rate constants of 6 selected pharmaceuticals in terms of direct ozone reaction, initiation, promotion and inhibition in ozonation; (2) to simulate the degradation of pharmaceuticals based on the determined rate constants. The results showed that the rate constants of 6 pharmaceuticals could be determined but the values are greater than the “lumped” rate constants reported in the literature. The model simulation predicted faster degradation than the experimental observations, which could be caused by the interferences causing by the intermediates formed during ozonation and background trace organics.

CONTENTS
摘要………………………………………………………………I
Abstract…………………………………………………………II
Contents…………………………………………………………III
Figures…………………………………………………………V
Tables……………………………………………………………IX
Chapter 1 Introduction………………………………………1
1.1 Research background……………………………………………1
1.2 Objectives……………………………………………………….2
Chapter 2 Literature review………………………………………………3
2.1 Basic properties of ozone……………………3
2.2 Direct ozone reaction and OH radical chain reactions…………3
2.3 Reaction kinetics and Rct concept of ozonation process………5
2.4 Ozonation of pharmaceuticals…………………………10
Chapter 3 Materials and methods………………………………………14
3.1 Chemicals and reagents…………………………………14
3.2 Stock solutions…………………………………………14
3.3 Analytical Methods………………………………………15
3.4 Ozonation experiments…………………………………17
Chapter 4 Results and discussion………………………………………18
4.1 The initiation, promotion, inhibition and direct ozone reaction rate constants of selected pharmaceuticals.……………………………18
4.2 Removal of pharmaceuticals and model simulations using determined rate constants……………………………………………39
4.3 Resimulations of pharmaceutical removal……….……………44
Chapter 5 Conclusions and recommendations………………………….49
5.1 Conclusions……………………………………………………49
5.2 Recommendations……………………………………………..50
References………………………………………………………………51

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