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博碩士論文 etd-0705116-170621 詳細資訊
Title page for etd-0705116-170621
論文名稱
Title
藥品及個人保健用品經加氯氧化程序生成新興消毒副產物亞硝胺之研究
Formation of N-nitrosamines from pharmaceuticals and personal care products during chlor(am)ination disinfection
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
104
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2016-07-11
繳交日期
Date of Submission
2016-08-16
關鍵字
Keywords
額外氮源、藥品及個人保健用品、新興污染物、亞硝胺、加氯消毒、消毒副產物
Chlorination, Additional nitrogen, Chloramination, Emerging contaminants, Nitrosamines, Pharmaceuticals and personal care products, Disinfection byproducts
統計
Statistics
本論文已被瀏覽 5677 次,被下載 100
The thesis/dissertation has been browsed 5677 times, has been downloaded 100 times.
中文摘要
亞硝胺類化合物為新興含氮消毒副產物(Nitrogenous disinfection byproducts,N­DBPs),近年來陸續在世界各國多處飲用水中,發現其高濃度存在而廣泛受到注意,且比目前許多已受法規規範的消毒副產物(Disinfection byproducts,DBPs)擁有更高的人體健康危害風險。過去研究發現特定的藥品及個人保健用品(Pharmaceuticals and personal care products,PPCPs)在消毒(尤其是氯胺消毒)過程中可生成高致癌性的N-二甲基亞硝胺(N-Nitrosodimethylamine,NDMA)。為明確瞭解PPCPs被釋放至環境後,經由加氯消毒氧化過程對N­DBPs亞硝胺生成之影響,本研究選定四種藥品作為前驅物包含胃酸抑制劑雷尼替丁(Ranitidine)、尼唑替丁(Nizatidine)、抑制過敏症狀的氯苯那敏(Chlorpheniramine)、具有鎮定及催眠效果的多西拉明(Doxylamine),模擬水處理程序中的加氯消毒程序,並分析八種亞硝胺包括N­Nitrosodimethylamine(NDMA)、N-Nitrosomethylethylamine(NMEA)、N-nitrosopyrrolidine(NPyr)、N-nitrosodiethylamine(NDEA)、N-nitrosopiperidine(NPip)、N-Nitrosomorpholine(NMor)、N-nitroso-di-n-propylamine(NDPA)及N-Nitrosodi-n-butylamine(NDBA)之生成潛勢。
結果顯示,研究選定之四種藥品模擬加氯及氯胺氧化程序,NDMA為主要生成物種,另發現有NMEA、NDEA、NMor及NPip生成,且一氯胺為藥品較有效生成NDMA的氧化劑。Ranitidine無論經加氯氧化或氯胺氧化,皆呈現最高的NDMA生成潛勢,其經由加氯氧化程序後亦可生成第二種亞硝胺NPip,顯示本身結構特徵具有較高亞硝胺生成潛勢的前驅物,經由單純的加氯氧化,即有可能生成兩種以上的亞硝胺。當水體中存在不同額外氮化物時,會增加亞硝胺生成潛勢與物種,其中影響最顯著的為Ranitidine和亞硝酸鹽共存之情況,其經次氯酸氧化程序後,NDMA生成轉換率增加將近一個數量級。氯/氮莫耳比率對NDMA生成之影響結果顯示,NDMA之莫耳轉換率與氯/氮莫耳比率成反比,此結果在實務上若欲控制亞硝胺生成,在加氯量固定的情況下(考量飲用水水質標準對自由有效餘氯須有一定的濃度要求),藉由減少加氯量抑制亞硝胺生成之策略可行性有限,去除前驅物仍為有效控制飲用水消毒過程中NDMA生成之主要策略。
Abstract
Nitrosamines are a group of emerging nitrogenous disinfection by-products (N-DBPs) in drinking water, and have recently caused significant public concerns because of their carcinogenic potentials higher than those of currently regulated DBPs. Some amine-based pharmaceuticals have been demonstrated to form NDMA during chloramination in previsou studies. The objective of this study was to investigate the formation of different nitrosamines during chlorination or chloramination of four pharmaceuticals including ranitidine, nizatidine, chlorpheniramine, and doxylamine, with the effects of different disinfection approaches and additional inorganic nitrogen being studied. The formation of eight nitrosamines including N-nitrosodimethylamine (NDMA), N-nitrosomethylethylamine (NMEA), N-nitrosopyrrolidine (NPyr), N-nitrosodiethylamine (NDEA), N-nitrosopiperidine(NPip), N-nitrosomorpholine (NMor), N-nitrosodi-n-propylamine (NDPA) and N-nitrosodi-n-butylamine (NDBA)during chlorination or chloramination of selected phazrmaceuticals were investigated in this study.
The results showed that NDMA was the main species formed from four pharmaceuticals during chlorination or chloramination, as the presences of few other nitorsamines such as NMEA、NDEA、NMor and NPip were sometimes observed. During chlorination or chloramination, NDMA formation increased in the order OCl- < NHCl2 < NH2Cl. Ranitidine was the species that possessed the strongest NDMA formation potential. Interestingly, NPip formation during chlorination of ranitidine was found, indicating that pharmaceuticals with complex chemical structures may feature potentials to form multiple nitrosamines during chlorination or chloramination. The presence of excess inorganic nitrogen enhnaced the formation of NDMA and other nitrosamines during chlorination or chloramination of pharmaceutcials. The most potent NDMA formation occurred when ranitidine coexisted with nitrite, in which NDMA conversions increased nearly an order of magnitude compared to the result when nitrite was added. By changing the Cl/N molar ratio in the solution, the NDMA conversion rate increased as the Cl/N molar ratio elevated/ Considered the minimum chlorine residual requird by compliance with the drinking water standard in Taiwan, which limits the feasibility of minimizing the nitrosamine formation by reducing the chlorine dosage, efficiently removing potential precursors would still be the more possible approach to effectively control NDMA or other nitrosamine formation during disinfection of pharmaceuticals.
目次 Table of Contents
目錄
論文審定書 i
摘要 ii
Abstract iv
目錄 vi
圖目錄 ix
表目錄 xi
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 4
1.3 研究架構 5
第二章 文獻回顧 8
2.1 新興含氮消毒副產物 9
2.2 亞硝胺類化合物 11
2.2.1 亞硝胺類化合物之物化特性 12
2.2.2 亞硝胺類化合物的危害與規範 14
2.2.3 亞硝胺類化合物之生成機制 17
2.2.3.1 氯胺氧化 19
2.2.3.2 加氯氧化 21
2.2.3.3 臭氧氧化 22
2.2.4 亞硝胺類化合物之前驅物 24
2.2.4.1 胺類化合物 24
2.2.4.2 藥品及個人保健用品 26
2.2.4.3 苯脲系除草劑 27
2.3 藥品及個人保健用品簡介 29
2.3.1 環境中藥品及個人保健用品之來源 29
2.3.2 水體中藥品及個人保健用品之流佈 30
2.3.3 藥品及個人保健用品之去除 31
2.3.4 藥品生成亞硝胺之機制介紹 32
第三章 材料與方法 35
3.1 實驗藥品與儀器設備 35
3.1.1 實驗藥品 35
3.1.2 實驗器材與儀器設備 37
3.2 實驗方法 38
3.2.1 完全混合消毒程序模擬系統 38
3.2.2 氧化劑(氯、氯胺)的製備及分析 41
3.2.3 亞硝胺類化合物樣品前處理 42
3.2.4 亞硝胺類化合物樣品分析 43
3.3 實驗室品質保證與品質管理 44
3.4 不同藥品前驅物生成亞硝胺之莫耳轉換率計算 46
第四章 結果與討論 47
4.1 Nizatidine與Doxylamine經兩種化學(氯、氯胺)氧化程序生成NDMA 47
4.2 四種藥品經氯與氯胺氧化程序生成亞硝胺類化合物 52
4.3 水體中存在額外氮化物對亞硝胺類化合物生成的影響 60
4.3.1 次氯酸氧化 60
4.3.2 一氯胺氧化 65
4.3.3 二氯胺氧化 70
4.4 四種藥品經氯與氯胺氧化並考量額外氮化物共存對NDMA生成之影響 75
4.5 Cl/N莫耳比率對NDMA生成之影響 79
第五章 結論與建議 81
5.1 結論 81
5.2 建議 83
參考文獻 84
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