||A Study on PCDD/Fs Scavenged by Cloud/Fog Water
||Department of Environmental Engineering
2019年主動式採樣器所採得雲霧水樣品之PCDD/F-WHO-TEQ濃度(平均值為1.35±1.80 pg WHO-TEQ L-1)高於被動式採樣器所採得樣品之PCDD/F-WHO-TEQ濃度(平均值為0.769±1.23 pg WHO-TEQ L-1)，其原因推測與被動式採樣器採樣過程中可能參雜些許雨水有關。接著將計算大氣中PCDD/Fs經由雲霧水之掃除效果，但由於2018並沒有採集大氣中PCDD/Fs，因此必須藉由雲霧水中之PCDD/Fs加以推估計算而得，為了證明氣固相推估的可行性，我們以2019年雲霧水和大氣中之PCDD/Fs做為參考，發現2019年由氣固相推估出的模擬數據(平均為0.128 pg m-3)確實和真實大氣中的PCDD/F濃度(平均為0.173 pg m-3)十分接近，因此我們將藉由2018年雲霧水中之PCDD/Fs加以推估計算而得到該年大氣中之總PCDD/F濃度(平均為0.0853 pg m-3)。
大氣中PCDD/Fs雲霧水之掃除效果可分成掃除係數(C-cloud/C-air)及掃除率(C-cloud/C-air *LWC)作探討，從掃除係數的比較可發現，被動式採樣器所得PCDD/Fs之毒性掃除係數(平均為2.24×105±2.96×105)相較於主動式採樣器(平均4.20×105±3.60×105)皆低了將近二分之一，由於被動式雲霧水採樣器所收集之雲霧水樣品亦包含雨水於其中，故雨水對PCDD/Fs之掃除率亦會有所貢獻；而2018年被動式採樣器所得PCDD/Fs之毒性掃除係數(平均為3.20×105±3.26×105)將高於2019年的數值，其原因則與2018年事件期間較豐富的雲霧水有關，此外也可觀察到雲霧水對於PCDD/Fs的掃除係數將隨著PCDD/F congeners的氯數增加而上升的現象。為了更加瞭解雲霧水對PCDD/F掃除係數的特性，比較發現雲霧水對於PCDD/F的掃除係數確實高於雨水的PCDD/F掃除係數(平均為1.9×105)，且與多環芳香烴(PAHs)在雲霧水中的掃除係數相比發現後者相對較低(介於103~105)。若從掃除率來看，被動式採樣器所得PCDD/Fs之毒性掃除率(平均則為0.063±0.065)將高於主動式採樣器所得之值(平均則為0.035±0.023)，其主要影響原因為被動式採樣器採集較多的雲霧水及雨水將更易捕集大氣中PCDD/Fs；而2018年被動式採樣器所得PCDD/Fs之毒性掃除率(平均為0.254±0.236)將高於2019年的數值，其原因則與2018年事件期間較豐富的雲霧水有關。接著，將其與微量元素在雲霧水中的掃除率相比，相比之下發現後者相對較高(約0.11-0.56)，二者之間掃除率的差別推測與溶解度有關，微量元素的水溶性遠大於PCDD/Fs，導致微量元素較容易被雲霧水所掃除。透過與雲霧水對其他汙染物掃除率的比較，可以得知雲霧水對於PCDD/Fs的掃除確實是一重要去除大氣中汙染物的機制。
Precipitation is one of the important sedimentation mechanisms of pollutants in the atmosphere, but the literature of Dibenzo-p-dioxin and Dibenzofuran (PCDD/Fs) deposition in cloud/fog water is still absent. However, droplets of cloud/fog water are much smaller and have a much higher surface-to-volume ratio compared to rain which might make it more efficiency in PCDD/F sedimentation. Therefore, we investigate PCDD/Fs scavenged by cloud/fog water in this study in order to figure it out.
Sequential cloud/fog water samples were collected for each cloud event during January 17th to February 24th, 2018 and January 15th to February 16th, 2019. The cloud water samples were combined into one to reach 20 L for PCDD/F measurement due to the low solubility of PCDD/Fs in water. There were 3 and 11 events happened during collecting period in 2018 and 2019, respectively, but only 8 events were analyzed in 2019 because of too short cloud/fog water event period or too low liquid water content. On the other hand, the ambient air sample were collected during January 14th and 28th, 2019, with 7 samples. Total PCDD/F-WHO-TEQ concentration collected by active fog collector in cloud/fog water samples in 2019 (mean: 1.35±1.80 pg WHO-TEQ L-1) averaged higher than the values of passive one (mean: 0.769±1.23 pg WHO-TEQ L-1). There might mix with a little bit rain in cloud/fog water sample collected by passive fog collector, which made liquid water content (LWC) for passive fog collector larger than LWC for active one.
Compared to scavenging coefficient of PCDD/F-WHO-TEQ of passive fog collector (mean: 2.24×105±2.96×105), scavenging coefficient (C-cloud/C-air) of PCDD/F-WHO-TEQ of active one was larger (mean: 4.20×105±3.60×105) in 2019. The cause of PCDD/F scavenging coefficient difference contributed to cloud/fog water sample mixing with rain which collected by passive fog collector. Besides, scavenging coefficient of PCDD/F-WHO-TEQ of passive fog collector in 2018 (mean: 3.20×105±3.26×105) averaged higher than the results of passive one in 2019 due to rich cloud and fog during collecting period in 2018. Then, compared to PCDD/F scavenging coefficient of precipitations (around 1.9×105), the scavenging coefficient of cloud/fog water in 2019 was larger. On the other hand, compared to scavenging ratio of PCDD/F-WHO-TEQ of passive fog collector (mean: 0.056±0.074), scavenging ratio (C-cloud/C-air *LWC) of PCDD/F-WHO-TEQ of active one was lower (mean: 0.033±0.029) in 2019. The reason might connect with higher LWC of passive fog collector where PCDD/Fs in the atmosphere could be scavenged by more cloud/fog water and rain. Besides, scavenging ratio of PCDD/F-WHO-TEQ of passive fog collector in 2018 (mean: 0.254±0.236) averaged higher than the results of passive one in 2019 due to higher LWC and rich cloud and fog during collecting period in 2018. Additionally, PCDD/F scavenging ratio of cloud/fog water was smaller than that of trace elements (ranged from 0.11- 0.56) since trace elements are easier to dissolve in water than PCDD/Fs. In conclusion, the obtained scavenging ratios of PCDD/Fs by cloud/fog water are crucial for clarifying the effect of cloud/fog water on the deposition of atmospheric PCDD/Fs.
List of Tables VIII
List of Figures X
Chapter 1 Introduction 1
Chapter 2 Literature Review 4
2.1 Cloud and Fog 4
2.1.1 Physical Characteristics of Cloud and Fog 4
2.1.2 Cloud Deposition 5
2.1.3 Cloud Formation in Northeast Monsoon in Taiwan 6
2.2 Composition of Cloud/Fog Water 7
2.2.1 Chemical Composition of Cloud/Fog Water 7
2.2.2 Organic Matter in Cloud/Fog Water 8
2.2.3 Toxic Pollutants Found in Cloud/Fog Water 9
2.3 Dry Deposition 11
2.3.1 Gas-particle partitioning 11
2.3.2 Dry Deposition Process 12
2.4 Wet Deposition 14
2.4.1 Liquid Water Content 14
2.4.2 Scavenging Ratio 14
2.4.3 Wet Deposition Process 15
2.5 PCDD/Fs 17
2.5.1 Chemical and Physical Characteristics of PCDD/Fs 17
2.5.2 Sources of PCDD/Fs 21
2.6 PCDD/Fs Impact on Human Health 23
2.6.1 Toxic Equivalency Factor of PCDD/Fs 23
2.6.2 Effects of PCDD/Fs on Human Health 25
Chapter3 Experimental Material and Method 26
3.1 Sampling Site 26
3.2 Sampling Method 27
3.2.1 Cloud/Fog Water Sampling 27
3.2.2 Ambient Air Sampling 30
3.2.3 Particulate and Gas Phase Organic Pollution Collection 34
3.3 Pretreatment and Analysis 36
3.3.1 Pretreatment before Sampling 36
3.3.2 Pretreatment before Analysis 36
Chapter 4 Results and Discussion 39
4.1 Meteorological Information 39
4.1.1 Cloud/Fog Water Events 39
4.1.2 Liquid Water Content 42
4.2 PCDD/F Concentration in Cloud/Fog Water 46
4.2.1 Total PCDD/F Concentration in Cloud/Fog Water 46
4.2.2 Phase Distribution of PCDD/Fs 48
4.2.3 Congener Profile of PCDD/Fs 51
4.2.4 Potential sources of PCDD/Fs 54
4.3 PCDD/F Concentration in the Ambient Air 57
4.3.1 Total PCDD/F Concentration in the Ambient Air in 2019 57
4.3.2 Comparison of Estimation and Analysis Data in 2019 58
4.3.3 Estimated atmospheric PCDD/F Concentration in 2018 63
4.4 PCDD/Fs Scavenged by Cloud/Fog Water 66
4.4.1 Scavenging Coefficient 66
4.4.2 Scavenging Ratio 73
Chapter 5 Conclusions and Suggestions 77
5.1 Conclusions 77
5.2 Suggestions 78
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國立中央大學 大氣物理研究所 碩士論文 北台灣冬季層狀雲化學特性分析 研究生： 簡瑋靚(2008), 14-15.