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研究生:張育婷
研究生(外文):Yu Ting Chang
論文名稱:台灣大氣細懸浮微粒戴奧辛採樣方法建立與相對健康潛勢評析
論文名稱(外文):Evaluation of Atmospheric PCDD/Fs and DL-PCBs Compounds in TSP and PM2.5 : Measurement and the Relative Health Risk in Taiwan
指導教授:紀凱獻
指導教授(外文):Kai Hsien Chi
學位類別:碩士
校院名稱:國立陽明大學
系所名稱:環境與職業衛生研究所
學門:醫藥衛生學門
學類:公共衛生學類
論文種類:學術論文
論文出版年:2014
畢業學年度:102
語文別:中文
論文頁數:191
中文關鍵詞:戴奧辛細懸浮微粒周界採樣相對危險比
外文關鍵詞:PCDD/FsPM2.5Environmental SamplingRelative Risk
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分布於大氣中的細懸浮微粒 (PM2.5) 可作為毒性有機化合物的載體進而導致協同效應的產生,而持久性有機污染物 (Persistent Organic Pollutants, POPs) 即為最可能附著於細懸浮微粒中的毒性污染物之一,但細懸浮微粒在戴奧辛毒理特性研究方面,目前仍無任何實際檢測數據可供參考,本研究根據台灣環保署現行公告之大氣戴奧辛及TSP採樣方法 (NIEA A809.11B) 、PM2.5TW採樣方法 (NIEA A205.11C) 以及歐盟EN-14907 PM2.5EU標準方法,進行同步採樣並進而釐清不同國家標準方法之差異性,並估算總懸浮微粒中細懸浮微粒PM2.5毒性當量及質量分布比例,選擇北部地區(都會測站、郊區測站、交通測站)、中部地區(中部工業測站、西部工業測站)進行監測,而後將所採集結果結合台灣死亡登記檔,分析細懸浮微粒戴奧辛與疾病死亡之相關性,進而維護民眾健康及生活環境品質。
PM2.5採樣結果指出,以台灣NIEA A205.11C (24.6 ± 4.01 μg/m3)與歐盟EN-14907 (25.0 ± 4.42 μg/m3) 所同步採集之PM2.5質量濃度值相當接近其差異性小於5%,故使用歐盟EN-14907採集細懸浮微粒可行性相當高。另外,戴奧辛同步分析結果亦顯示台北市以都會測站大氣戴奧辛毒性當量濃度 (28.2 ± 3.51 fg WHO-TEQ/m3) 最高,其中PM2.5EU戴奧辛濃度佔TSP約65%。郊區測站大氣戴奧辛濃度為12.4 ± 7.22 fg WHO-TEQ/m3,PM2.5EU戴奧辛濃度佔TSP約58%。交通測站所測得濃度 (10.9 ± 8.11 fg WHO-TEQ/m3) 最低,PM2.5EU戴奧辛濃度佔TSP約74%。工業區以西部工業測站戴奧辛毒性當量濃度 (321 ± 108 fg WHO-TEQ/m3) 最高,PM2.5EU戴奧辛濃度佔TSP約68%。中部工業測站大氣戴奧辛毒性當量濃度為57.6 ± 45.4 fg WHO-TEQ/m3,PM2.5EU戴奧辛濃度佔TSP約59%。各測站PCDD/Fs同源物以高氯數物種為主,且以固相方式存於大氣中,但部分測站如工業測站其氣相低氯數物種濃度較高,此外,由於氣相污染物易經由大氣化學反應機制形成二次氣膠,故細懸浮微粒與氣相之戴奧辛物種分布相當一致。
高戴奧辛濃度地區不分性別族群之全死因 (Relative risk = 1.200,CI = 1.118-1.289,P < 0.0001) 與肝和肝內膽管癌 (Relative risk = 1.567,CI = 1.162-2.113,P = 0.0032) 之相對死亡風險皆顯著高於低濃度地區。細懸浮微粒相關之疾病如腦血管疾病、肺炎,並無統計上顯著差異,初步推論若探討細懸浮微粒對人體健康影響,不應僅考慮其質量濃度之變化,其化學組成成分(如戴奧辛)也應當納入考量。另外,本研究以PMF模式針對台北都會區進行戴奧辛污染排放溯源解析,初步推估台北都會區PM2.5EU戴奧辛主要貢獻源為固體廢棄物焚化廠、火葬場、長程傳輸事件及交通源,但本研究以總懸浮微粒戴奧辛污染源指紋圖譜與本研究所量測之細懸浮微粒戴奧辛指紋圖譜進行污染源解析,可能會導致誤差,故應建立細懸浮微粒戴奧辛指紋圖譜資料庫,以供後續詳細調查台灣各戴奧辛污染來源的貢獻判斷。

Epidemiological and toxicological studies have demonstrated that the cardiovascular mortality and morbidity increased with increasing particulate matter (PM). In addition, the toxicity of PM generally increased as the decreasing of particle size. Particularly, the contents of Persistent Organic Pollutants exist in suspended particles. In this study, the PM2.5 samples were collected according to the main guidelines of the Taiwan-EPA NIEA A809.11B, NIEA A205.11C PM2.5TW, and European Union EN-14907 PM2.5EU in the mean time. Ambient air samples were collected for the analysis of PCDD/Fs from five locations over duration of 24-48 h, using both TSP and PM2.5 samplers. Locations with diverse characteristic such as urban, suburban, traffic-affected zones, western industrial area, and central industrial area were selected.
The measurements indicated that the PM2.5 mass concentration followed by Taiwan NIEA A205.11C PM2.5TW was 24.6 ± 4.01 μg/m3, and European Union EN-14907 PM2.5EU was 25.0 ± 4.42 μg/m3. According to the methods of EN-14907 and Taiwan NIEA A205.11C, The difference between those two PM2.5 sampling methods was around 5%, hence, we consider those two PM2.5 sampling methods were comparable. Our measurements indicated that the PCDD/F concentrations of TSP samples were 28.2 ± 3.51, 12.4 ± 7.22, 10.9 ± 8.11, 321 ± 108, and 57.6 ± 45.4 fg WHO‐TEQ/m3 at urban, suburban, traffic-affected zone, western industrial area, and central industrial area, respectively. Comparing the results for the PM2.5EU and TSP samples, the total TEQs PCDD/Fs concentrations in the PM2.5EU samples were around 58%-74% of the TSP samples. Therefore, the fine particles contained with higher levels of PCDD/Fs than coarse particles. On the other hand, high chlorinated- PCDD/Fs tend to be the most abundant PCDD/Fs in solid phase at all sites. The pollutants in vapor phase were easy to form secondary aerosol by the atmosphere, so the distribution of PCDD/Fs congeners in vapor and solid phase of PM2.5EU were similar.
The health relative risk of the all cause (Relative risk = 1.200, CI = 1.118-1.289, P < 0.0001) and liver cancer (Relative risk = 1.567, CI = 1.162-2.113, P = 0.0032) in high dioxin exposure group were significant higher than low dioxin exposure group. To further evaluate the health relative risk of PM2.5, not only the mass concentration but also the chemical component including PCDD/Fs of PM2.5 should be seriously investigated. According to the statistical results of PMF analysis, the major contributors of atmospheric PCDD/Fs for PM2.5EU samples observed at urban in Taipei were MSWI, crematorium, long-range transport, and traffic source. However, the PCDD/F emission inventory of stationary sources established in Taiwan was focus on PM, that may result on the miss identification of atmospheric PCDD/F distribution in PM2.5. Therefore, the database of PM2.5 including characteristics of dioxin content in Taiwan should be established in the near future.

目錄
致謝 I
摘要 II
Abstract IV
縮寫對照表 (Abbreviation) VI
目錄 VII
圖目錄 X
表目錄 XIV
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 2
第二章 文獻回顧 3
2.1 戴奧辛特性 3
2.1.1 戴奧辛之基本特性 3
2.1.2 戴奧辛來源 9
2.1.3 戴奧辛之流行病學研究 13
2.1.4 戴奧辛吸入暴露之探討 17
2.2 PM2.5細懸浮微粒特性 21
2.2.1 PM2.5細懸浮微粒來源 21
2.2.2 PM2.5細懸浮微粒之流行病學研究 24
2.3 PM2.5細懸浮微粒之戴奧辛污染物研究 27
2.3.1 煙道分階粒徑之戴奧辛濃度探討 27
2.3.2 大氣PM2.5與分階粒徑之戴奧辛濃度解析 30
2.4 台灣地區大氣戴奧辛濃度分布特性 43
2.5 台灣地區PM2.5細懸浮微粒之管制與濃度分布 56
2.5.1 台灣PM2.5細懸浮微粒管制規範 56
2.5.2 台灣地區大氣PM2.5細懸浮微粒濃度分布特性 58
第三章 研究方法 61
3.1 研究流程 61
3.2 採樣點之選擇 63
3.2.1 台北都會區 63
3.2.2 中、西部工業區 65
3.3懸浮微粒與戴奧辛空氣採樣方法 68
3.3.1 歐盟PM2.5EU EN-14907 72
3.3.2 台灣PM 2.5TW NIEA A205.11C 75
3.3.3 台灣TSP NIEA A809.11B 76
3.4 戴奧辛樣品前處理方法 79
3.4.1 實驗藥品 79
3.4.2 實驗溶劑 80
3.4.3 實驗材料 81
3.4.4 實驗設備 82
3.4.5 樣品前處理 83
3.5 戴奧辛樣品上機分析程序 91
3.6 戴奧辛之統計分析 93
3.6.1 研究資料概述 93
3.6.2 統計方法概述 94
3.6.3 污染來源解析-PMF正矩陣因子法 95
第四章 結果與討論 98
4.1 各採樣地點之氣象條件 98
4.1.1 各測站之氣象條件 98
4.1.2 各測站細懸浮微粒 (PM2.5) 自動監測濃度值 101
4.2 細懸浮微粒與總懸浮微粒質量濃度採樣方法比對 109
4.2.1 都會區細懸浮微粒與戴奧辛濃度比對 109
4.2.2 各測站不同採樣方法之PM2.5、TSP質量濃度比對 112
4.3 各測站大氣戴奧辛採樣結果 115
4.3.1 各測站PM2.5EU、TSP戴奧辛濃度探討 115
4.3.2 PM2.5EU與TSP中戴奧辛毒性當量質量數 123
4.3.3 PM2.5EU與TSP中戴奧辛指紋圖譜探討 126
4.4 細懸浮微粒戴奧辛與疾病之統計結果 137
4.4.1 細懸浮微粒與總懸浮微粒戴奧辛吸入暴露評估之探討 137
4.4.2 各測站大氣細懸浮微粒戴奧辛濃度歷年變化 140
4.4.3 高濃度與低濃度暴露地區疾病死亡探討 143
4.5 台北都會地區大氣戴奧辛來源解析 152
第五章 結論與建議 161
5.1 結論 161
5.2 建議 165
參考文獻 166
附錄 183

圖目錄
圖2-1 戴奧辛類化學結構式 6
圖2-2 環境中戴奧辛來源 11
圖2-3 2011年美國戴奧辛類同源物排放行業別 11
圖2-4 2010年歐盟戴奧辛排放行業 12
圖2-5 2010年歐盟多氯聯苯排放行業 12
圖2-6 戴奧辛在細胞中活動示意圖 16
圖2-7 PM2.5生成機制圖 22
圖2-8 懸浮微粒主要沉積部位 23
圖2-9 大氣中懸浮微粒尺寸與相對濃度分布圖 23
圖2-10 細懸浮微粒之全身性健康影響示意圖 25
圖2-11 飛灰中相對微粒粒徑之戴奧辛濃度分布 28
圖2-12 煙道粒徑分階樣品中戴奧辛同源物分布情形 29
圖2-13 大氣微粒粒徑與戴奧辛濃度分布情形 31
圖2-14 微粒濃度與戴奧辛濃度比 33
圖2-15 戴奧辛同源物濃度與粒徑分布關係 33
圖2-16 各微粒之戴奧辛濃度含量 35
圖2-17 戴奧辛與微粒質量濃度百分比 36
圖2-18持久性有機污染物與微粒濃度之相對關係 39
圖2-19 PM10與PM2.5戴奧辛與多氯聯苯濃度分布 40
圖2-20台灣各縣市大氣戴奧辛濃度值變化 46
圖2-21台灣各空品區之大氣戴奧辛濃度趨勢 46
圖2-22台灣大氣戴奧辛濃度年變化趨勢 47
圖2-23北部空品區之大氣戴奧辛濃度年變化趨勢 47
圖2-24 宜蘭空品區之大氣戴奧辛濃度年變化趨勢 48
圖2-25 竹苗空品區之大氣戴奧辛濃度年變化趨勢 48
圖2-26 中部空品區之大氣戴奧辛濃度年變化趨勢 49
圖2-27 雲嘉南空品區之大氣戴奧辛濃度年變化趨勢 49
圖2-28 高屏空品區之大氣戴奧辛濃度年變化趨勢 50
圖2-29 花東空品區之大氣戴奧辛濃度年變化趨勢 50
圖2-30 各國歷年大氣戴奧辛濃度 54
圖2-31 歷年英國大氣戴奧辛濃度趨勢 55
圖2-32 2013年台灣各空品區PM2.5質量濃度年平均值 59
圖3-1 研究方法流程圖 62
圖3-2 台北都會區採樣地點與鄰近污染源之相對位置 64
圖3-3 西部工業區採樣地點與鄰近污染源之相對位置 66
圖3-4 中部工業區採樣地點與鄰近污染源之相對位置 67
圖3-5 大氣TSP與PM2.5採樣方法流程 71
圖3-6 高流量PM2.5EU採樣圖 73
圖3-7 PM2.5EU分離器剖面圖 73
圖3-8 PM2.5EU採樣頭-分徑器(左)與濾紙匣(右)分解圖 73
圖3-9 PM2.5EU PUF採樣單元組裝圖 74
圖3-10 PM 2.5TW (PQ-200) NIEA A205.11C 75
圖3-11 PM2.5TW採樣器組合示意圖 75
圖3-12大氣TSP戴奧辛採樣器 (Shibata, HV-700) 77
圖3-13 Tisch TE-230 五階粒徑衝擊板 78
圖3-14大氣TSP戴奧辛採樣頭組裝圖 78
圖3-15 戴奧辛樣品前處理流程圖 83
圖3-16 酸洗程序 85
圖3-17酸性矽膠與酸性氧化鋁管柱淨化程序 87
圖3-18活性碳管柱淨化程序 89
圖3-19樣品轉移程序 90
圖4-1 各測站採樣期間之風花圖 100
圖4-2 都會測站2001年至2013年PM2.5自動監測質量濃度 103
圖4-3 郊區測站2005年至2013年PM2.5自動監測質量濃度 104
圖4-4 交通測站2010年至2013年PM2.5自動監測質量濃度 105
圖4-5 中部工業測站2005年至2013年PM2.5自動監測質量濃度 106
圖4-6 西部工業測站2005年至2013年PM2.5自動監測質量濃度 107
圖4-7 各測站2005年至2013年PM2.5自動監測月、年平均質量濃度 108
圖4-8 台北地區不同粒徑範圍之戴奧辛濃度比 122
圖4-9 工業地區不同粒徑範圍之戴奧辛濃度比 122
圖4-10 各測站粒徑範圍之戴奧辛毒性當量質量數 125
圖4-11 都會測站戴奧辛指紋圖譜 130
圖4-12 都會測站多氯聯苯指紋圖譜 131
圖4-13 郊區測站戴奧辛指紋圖譜 131
圖4-14 交通測站戴奧辛指紋圖譜 132
圖4-15 西部工業測站戴奧辛指紋圖譜 132
圖4-16 中部工業測站戴奧辛指紋圖譜 133
圖4-17 都會測站戴奧辛氣固相比例 134
圖4-18 郊區測站戴奧辛氣固相比例 134
圖4-19 交通測站戴奧辛氣固相比例 135
圖4-20 西部工業測站戴奧辛氣固相比例 135
圖4-21 中部工業測站戴奧辛氣固相比例 136
圖4-22 各測站大氣細懸浮微粒戴奧辛估算濃度年變化 142
圖4-23 長程傳輸事件戴奧辛指紋圖譜 155
圖4-24 固體 (MSWI) 與事業 (IWI) 廢棄物焚化廠戴奧辛指紋圖譜 156
圖4-25 火葬場之戴奧辛指紋圖譜 157
圖4-26 交通源之戴奧辛指紋圖譜 157
圖4-27 電弧爐之戴奧辛指紋圖譜 158
圖4-28 燒結廠之戴奧辛指紋圖譜 158
圖4-29 二次金屬冶煉之戴奧辛指紋圖譜 159
圖4-30 以PMF解析北台灣總懸浮微粒戴奧辛指紋圖譜 160
圖4-31 以PMF解析北台灣細懸浮微粒戴奧辛指紋圖譜 160

表目錄
表2-1 Typical physico-chemical properties of PCDD/Fs 5
表2-2 Homologues of PCDD/Fs, PCBs, PBDD/Fs, PxDD/Fs 6
表2-3 環境PCDD/Fs與PCBs半衰期 7
表2-4 戴奧辛、多氯聯苯之毒性當量因子 8
表2-5 各國戴奧辛吸入暴露值 20
表2-6 PM2.5之流行病學研究調查 26
表2-7戴奧辛毒性當量濃度與粒徑分布比例 32
表2-8 PM2.5之戴奧辛濃度物種分布(以FRM方法) 38
表2-9亞洲地區PM2.5與TSP中戴奧辛、多氯聯苯濃度比對 41
表2-10 歐美地區PM2.5與TSP中戴奧辛、多氯聯苯濃度比對 42
表2-11台灣各空品區與各縣市戴奧辛濃度值 45
表2-12各國細懸浮微粒管制標準 57
表2-13 各空品區測站類型與名稱 59
表2-14 各空品區四季、全年PM2.5質量濃度 60
表3-1 採樣方法比對 69
表4-1 各測站採樣期間之氣象條件彙整 99
表4-2 不同採樣方法之PM2.5質量濃度與戴奧辛濃度比對 111
表4-3 各測站不同採樣方法之PM2.5、TSP質量濃度比對 114
表4-4 各測站不同採樣方法之PM2.5質量濃度差異比例 114
表4-5 Atmospheric Dioxin concentration in vapor phase and solid phase (TSP) 118
表4-6 Atmospheric Dioxin concentration in vapor phase and solid phase (PM2.5EU) 119
表4-7 TSP中戴奧辛各物種之濃度分布特性 120
表4-8 PM2.5EU中戴奧辛各物種之濃度分布特性 121
表4-9 各測站戴奧辛毒性當量質量數 124
表4-10 各採樣地區戴奧辛吸入暴露值 139
表4-11 PM2.5高濃度組(沙鹿工業測站)與低濃度組(士林郊區測站)之標準化死亡比 146
表4-12 PM2.5高濃度組(沙鹿工業測站)與低濃度組(士林郊區測站)之疾病死亡相對危險比 148
表4-13 戴奧辛高濃度組(線西工業測站)與低濃度組(士林郊區測站)之標準化死亡比 149
表4-14 戴奧辛高濃度組(線西工業測站)與低濃度組(士林郊區測站)之疾病死亡相對危險比 151


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