臺灣博碩士論文加值系統

戴奧辛(PCDDs)和呋喃(PCDFs)為持久性有機汙染物，因其為脂溶性之有毒物質，容易經由大氣的乾濕沉降作用而進入生態系統中，造成生物放大效應及毒性累積。
本研究之目的為瞭解台灣北部之陽明山地區大氣中戴奧辛(PCDDs)和呋喃(PCDFs)之分佈特性，利用台灣北部空氣品質監測站之氣象資料、氣固相分佈模式及PM10與戴奧辛/呋喃濃度之相對濃度進行迴歸分析，配合乾沉降速度及濕沉降掃除係數，進行乾沉降模擬及濕沉降模擬，進一步得到陽明山地區周界大氣中戴奧辛/呋喃之氣固相分佈、乾沉降通量及濕沉降通量。研究結果顯示，乾沉降通量隨氣溫上升而下降，而濕沉降通量則是與雨量有高度正相關，由此可知氣象條件為影響乾濕沉降之重要因子。此外，戴奧辛/呋喃之含氯數多寡及粒狀物沉降特性等因素亦會對沉降通量造成顯著之影響。由乾濕沉降之毒性特徵剖面圖觀之，戴奧辛/呋喃之毒性主要由2,3,4,6,7,8-HxCDF、 2,3,4,7,8-PeCDF所占比例較高。
由模擬結果觀之，陽明山地區戴奧辛/呋喃於2014年所模擬出之戴奧辛/呋喃濃度，介於0.00725-0.0176 pg WHO2005-TEQ/Nm3之間，而2015年之模擬數值介於0.00761-0.0162 pg WHO2005-TEQ/Nm3之間。戴奧辛/呋喃濃度之比值在此兩年皆小於1(平均為 0.407)，顯示呋喃為主要存在之毒性物質。
陽明山地區戴奧辛/呋喃之月乾沉降通量在2014年時介於9.63-91.7 pg WHO2005-TEQ/m2 ∙month，在2015年則介於12.2-61.0 pg WHO2005-TEQ/m2 ∙month。在戴奧辛/呋喃之月濕沉降通量方面，陽明山地區於2014年介於6.29-138.3 pg WHO2005-TEQ/m2 ∙month之間，在2015年則介於4.95-79.3 pg WHO2005-TEQ/m2 ∙month之間。陽明山地區2014年及2015年之年戴奧辛/呋喃濕沉降通量為637.3及511.1 pg WHO2005-TEQ/m2 ∙year。
陽明山地區戴奧辛/呋喃之月總沉降(乾沉降與濕沉降總和)通量在2014年時介於34.4-178.0 pg WHO2005-TEQ/m2 ∙month，而在2015年數值移動為28.1-119.1 pg WHO2005-TEQ/m2 ∙month。陽明山地區2014年及2015年之年戴奧辛/呋喃總沉降通量為969.7及803.6 pg WHO2005-TEQ/m2 ∙year。
關於乾沉降所占總沉降之比率，陽明山地區在2014年介於10.9%- 81.7%，2015年則介於16.4%- 82.4%之間，年平均比率為35.7%及39.2%。在兩個模擬年分中，戴奧辛/呋喃之乾沉降通量在秋季具最低比率，可能肇因於降雨強度和降雨頻率的增加。
此研究所模擬出的乾濕沉降資料配合過去研究之相關結果，可提供戴奧辛/呋喃相關決策管理作為參考依據。由於臺灣缺乏戴奧辛/呋喃之乾沉降速度及掃除係數等實測數據，建議進行相關研究以建立更加完整及精確之乾濕沉降模擬。

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) are carcinogenic persistent organic pollutants (POPs) that can bioaccumulate in the ecosystem, cause endocrines disruption and undergo long range transport in the atmosphere. Atmospheric deposition including those of dry and wet is a primary pathway for the transfer of POPs to terrestrial and aquatic ecosystems.
In this study, the characteristics of PCDD/Fs in the ambient air at Mt. Yangming were simulated by the PM10 versus PCDD/Fs concentration regression analysis, gas-particle partition modeling, dry deposition, and wet deposition simulations. Dry and wet deposition fluxes were obtained from the combination of the PCDD/F concentrations, meteorological information, dry deposition velocities, and scavenging ratios. The dry deposition fluxes of PCDD/F-WHO2005-TEQ increase with decreasing temperature, while increase with higher degree of chlorine numbers on PCDD/F homologues. However, a wet deposition flux increase with stronger rainfall intensity. The congener profile of PCDD/F-WHO2005-TEQ indicates that total deposition fluxes, 2,3,4,6,7,8-HxCDF, 2,3,4,7,8-PeCDF dominate the deposition fluxes.
The simulated PCDD/F concentration during 2014, at Yangming, ranged between 0.00725 and 0.0176 pg WHO2005-TEQ /Nm3, while those during 2015 ranged between 0.00761 and 0.0162 pg WHO2005-TEQ /Nm3. WHO2005-TEQ ratios of PCDDs to PCDFs at both year are all less than 1 (averaged 0.407), indicating that PCDF dominate the total toxicity.

During 2014, at Yangming, the monthly dry deposition flux of total PCDD/Fs-WHO2005-TEQ ranged between 9.63 and 91.7 pg WHO2005-TEQ /m2 ∙month, while those during 2015 ranged between 12.2 and 61.0 pg WHO2005-TEQ /m2 ∙month. At the other hand, during 2014, at Yangming, the monthly wet deposition flux of total PCDD/Fs-WHO2005-TEQ ranged between 6.29 and 138.3 pg WHO2005-TEQ /m2 ∙month, while those during 2015 ranged between 4.95 and 79.3 pg WHO2005-TEQ /m2 ∙month. The annual total wet deposition flux of total PCDD/Fs- WHO2005-TEQ concentration at Yangming were 637.3 and 511.1 pg WHO2005-TEQ /m2 ∙year in 2014 and 2015, respectively.
During 2014, at Yangming, the monthly total deposition flux of total (dry + wet) PCDD/Fs-WHO2005-TEQ ranged between 34.4 and 178.0 pg WHO2005-TEQ /m2 ∙month, while those during 2015 ranged between 28.1 and 119.1 pg WHO2005-TEQ /m2 ∙month. The annual total deposition flux of total PCDD/Fs-WHO2005-TEQ at Yangming were 969.7 and 803.6 pg WHO2005-TEQ /m2 ∙year in 2014 and 2015, respectively.
At Yangming, during 2014, the fraction contribute by dry deposition ranged between 10.9% and 81.7%, while during 2015 ranged between 16.4% and 82.4%. Mean fraction contribute by dry deposition at Yangming were 35.7% and 39.2% in 2014 and 2015, respectively.
The lowest fraction of individual PCDD/Fs dry deposition in total (dry + wet) deposition fluxes was found in fall in both years. It may be due to high rainfall intensity occurred in fall and also the day with precipitation were more in fall.
The simulated results of this study combine with the previous measured data provided useful information for the future policy making and further studies. In Taiwan, more measured data associated with dry deposition velocity and wet scavenging is needed for a more precise and complete investigation in the future.

摘要 III
Abstract V
誌謝 VII
List of Contents VIII
List of Tables XI
List of Figures XII
List of Appendices XV
Chapter 1 Introduction 1
Chapter 2 Literature review 3
2.1 Chemical structures and physical properties of PCDD/Fs 3
2.2 Toxic equivalency factors and formation mechanism of PCDD/Fs 7
2.2.1 Toxic equivalency factors of PCDD/Fs 7
2.2.2 Formation of PCDD/Fs from precursor compound 8
2.2.3 De novo synthesis 8
2.3 Characteristics of Particulate Matter 10
2.3.1 Particle Size Distributions 10
2.4 Sources of PCDD/Fs 12
2.4.1 Sources of PCDD/Fs 12
2.4.2 Sources of Particulate Matter 17
2.5 Impact of PCDD/Fs and Particulate Matter on human health 19
2.5.1 Impact of PCDD/Fs on human health 19
2.5.2 Impact of Particulate Matter on human health 21
2.6 Dry deposition 25
2.6.1 Gas-particle partitioning simulation model 25
2.6.2 Dry deposition process 26
2.7 Wet deposition 28
2.7.1 Scavenging ratio 28
2.7.2 Wet deposition process 29
Chapter 3 Material and methods 30
3.1 Bacic information of ambient air sampling 30
3.2 Sampling and Analysis of PCDD/Fs 33
3.3 Regression analysis between PM10 and total PCDD/F concentration 38
Chapter 4 Results and Discussion 39
4.1 Meteorological information 39
4.2 Simulated concentrations of PCDD/Fs in the ambient air 43
4.3 Gas-particle partitioning 46
4.4 Dry deposition fluxes 52
4.4.1 Monthly dry deposition flux of total PCDD/Fs-WHO2005-TEQ concentration 52
4.4.2 Dry deposition fluxes of individual PCDD/Fs 55
4.5 Wet deposition fluxes 64
4.5.1 Monthly wet deposition flux of total PCDD/Fs-WHO2005-TEQ concentration 64
4.5.2 Wet deposition fluxes of individual PCDD/Fs 67
4.6 Total (dry+wet) deposition fluxes 76
4.6.1 Monthly total deposition fluxes of total PCDD/Fs-WHO2005-TEQ 76
4.6.2 Total deposition fluxes of individual PCDD/Fs 78
4.7 Fraction of dry deposition contribute in total deposition fluxes 87
4.7.1 Monthly fraction of dry deposition in total (dry + wet) deposition fluxes of total PCDD/Fs-WHO2005-TEQ 87
4.7.2 Fraction of individual PCDD/Fs dry deposition in total (dry + wet) deposition fluxes………………..……………………………………………89
Chapter 5 Conclusions and suggestions 94
5.1 Conclusions 94
5.2 Suggestions 98
Appendices 99
References 112
Resume 135

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