博碩士論文 953206012 詳細資訊




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姓名 劉恭廷(Kung-ting Liu)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 北台灣大氣環境中戴奧辛之 北台灣大氣環境中戴奧辛之乾、濕沈降特性研究
(Evaluation of Dry/Wet Deposition of PCDD/Fs in Northern Taiwan via Automated and Traditional Samplers )
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摘要(中) 燃燒程序排放至大氣中的戴奧辛於大氣擴散過程中會落至水體或民眾生活環境中,造成對人體健康之直接或間接影響。戴奧辛屬高沸點物質於環境中大量存在固相上,因此大氣中的粒狀物即成為戴奧辛自煙囪排放後的主要傳輸介質,所以監測落塵亦可間接得知戴奧辛影響水體環境及民眾健康的程度。
本研究利用新型落塵採樣器(Automated sampler)以北台灣地區為採樣背景,同時搭配傳統型落塵採樣器(Traditional sampler)進行大氣落塵採樣,一方面可精確得知沈降通量,另一方面也可瞭解傳統採樣器所存在的採樣問題及影響因素,並且探討不同沈降方式對戴奧辛沈降通量變化的影響。同時求出採樣期間戴奧辛沈降速度與雨除係數,藉以得知北台灣地區戴奧辛落至受體表面之速率以及降雨對於懸浮於大氣中的戴奧辛去除量。
傳統型落塵採樣器所得結果顯示戴奧辛沈降量為54-220 pg/m2-day (2.0-9.9 pg TEQ/m2-day),而Automated sampler採樣所得之沈降量239-490 pg/m2-day (15.0-25.8 pg TEQ/m2-day)。有無即時收樣系統避免光解是兩種採樣器最大不同處,具有即時收樣系統的Automated sampler所得之沈降通量大於傳統沈降採樣器所得之沈降通量。將兩種採樣器所得之沈降通量做一差異百分比可得知,總差異百分比與大氣溫度變化成正相關性,物種差異則是PCDD/Fs鍵結氯數越低,差異百分比越大,由此可知新型落塵採樣器較傳統型落塵採樣器更能準確採集戴奧辛沈降通量。此外,本研究也進行乾、濕沈降對戴奧辛沈降通量變化之影響,將乾、濕沈降各別實際採樣時間、雨量與降雨時數加入探討時,每一月份濕沈降通量皆高於乾沈降通量,乾沈降通量約149-224 pg/m2-sunny day (11.1-16.5 pg I-TEQ/m2-sunny day),濕沈降通量約690-10100 pg/m2-rainy day (36.8-228 pg I-TEQ/m2-rainy day)。另外,將乾、濕沈降通量與週界戴奧辛濃度經交叉計算後得平均沈降速度約0.26 cm/s,雨除係數則為1.4×105。
摘要(英) PCDD/Fs emitted to atmosphere may eventually fall to water body or environment during atmospheric diffusion and impact human health. Dioxin is a substance of high boiling point and is adsorbed enormously on the solid phase in environment and the particles become its main transportation media. Therefore, monitoring the atmospheric deposition of particles may provide the information regarding the extent of its PCDD/F effects on water body and people’s health.
This study focuses on the understanding of the dry/wet deposition of PCDD/Fs in northern Taiwan via automated and traditional samplers. The main advantages of this method include: (1) obtaining more accurate data regarding deposition flux of PCDD/Fs from atmosphere to land; (2) the combination of two types of samplers can help to clarify the possible under-estimation of deposition flux achieved with the traditional samplers. In addition, the deposition velocity and scavenging ratio during sampling process are also calculated so that we may find out how efficient PCDD/Fs falls on to the surface receptor in northern Taiwan and the removal efficiency of PCDD/Fs while raining.
The deposition flux of PCDD/Fs collected by traditional sampler ranged from 54- 220 pg/m2-day (2.0-9.9 pg TEQ/m2-day), while the deposition flux of PCDD/Fs collected by automated sampler was much higher, ranging from 239-490 pg/m2-day (15.0-25.8 pg TEQ/m2-day). Furthermore, the relative difference of PCDD/F deposition flux between the measurement of automated and traditional samplers increased with increasing atmospheric temperature. It is also interesting to find the relative difference of lowly chlorinated PCDD/Fs were higher than that of highly chlorinated PCDD/Fs.
This study also investigates the influences of dry/wet deposition on sampling time and rainfall. The results indicate that wet deposition flux was higher than dry deposition flux. Dry deposition flux was measured as 149-224 pg/m2-sunny day (11.1-16.5 pg TEQ/m2-sunny day) while wet deposition flux was 690-10100 pg/m2-rainy day (36.8-228 pg TEQ/m2-rainy day). As indicated by this finding, wet deposition can remove PCDD/Fs in a more significant way than dry deposition. Furthermore, the average PCDD/Fs deposition velocity and scavenging ratio in northern Taiwan are calculated as 0.26 cm/s and is 1.4×105, respectively.
關鍵字(中) ★ 戴奧辛
★ 沈降
★ 沈降通量
★ 傳統型落塵採樣器
關鍵字(英) ★ PCDD/Fs
★ deposition
★ deposition flux
★ automated sampler
★ traditional sampler
論文目次 目錄
摘要 I
ABSTRACT III
目錄 V
圖目錄 VII
表目錄 IX
第一章 前 言 1
1.1研究緣起 1
1.2研究目的與範疇 2
第二章 文獻回顧 3
2.1戴奧辛特性 3
2.1.1戴奧辛特徵與性質 3
2.1.2戴奧辛的毒理特性 4
2.1.3大氣中戴奧辛之分佈 6
2.2戴奧辛來源 8
2.2.1大氣中戴奧辛之來源 8
2.2.2週界採樣之缺失 11
2.3大氣落塵之沈降特性 12
2.3.1採樣器差異 15
2.3.2影響沈降通量因素—光解 17
2.3.3採樣器差異-落塵收樣系統 22
2.4.4各國沈降通量趨勢變化比較 23
2.3.5季節性變化與因素探討 27
2.3.6粒狀物與乾、濕沈降間之關係 31
2.4沈降速度與雨除係數 36
2.4.1沈降速度 36
2.4.2雨除係數 38
第三章 研究方法 40
3.1研究流程設計 40
3.1.1採樣點的選擇 44
3.1.2採樣時間選擇 46
3.1.3 PS-1採樣方法 47
3.1.4 PS-1採樣之品保品管程序 49
3.1.5 High volume air sampler 採樣方法 51
3.1.6 High volume air sampler採樣之品保品管程序 52
3.1.7傳統落塵採樣方法 54
3.1.8 Automated sampler 採樣方法 58
3.2 PCDD/Fs 前處裡 62
3.2.1實驗藥品 62
3.2.2實驗溶劑 63
3.2.3實驗材料 64
3.2.4實驗設備 65
3.2.5樣品前處理 65
3.3上機分析 67
第四章 結果與討論 70
4.1採樣時氣象資料 70
4.2週界樣品分析結果 75
4.2.1大氣中戴奧辛濃度季節變化 75
4.2.2氣、固相戴奧辛分佈與大氣溫度之關係 80
4.3 大氣中戴奧辛沈降分析結果 83
4.3.1傳統落塵採樣器之採樣結果 83
4.3.2 Automated sampler之採樣結果 90
4.3.3不同沈降採樣器之沈降通量比較 94
4.3.4不同沉降方式對戴奧辛沈降通量變化之影響 98
4.3.5氣象條件對沈降通量之影響 108
4.3.6週界氣、固相戴奧辛與乾、濕沈降之相關性 110
4.3.7沈降速度與雨除係數 111
第五章 結論與建議 115
5.1結論 115
5.2建議 117
參考文獻 118
圖目錄
圖2-1 固相戴奧辛隨溫度之變化趨勢 8
圖2-2 台灣大氣中戴奧辛濃度逐年變化趨勢 10
圖2-3 日本焚化爐與大氣戴奧辛濃度逐年變化 11
圖2-4 邊界層傳輸之主要機制 13
圖2-5 濕沈降與污染物間之各種作用 15
圖2-6 常用於大氣沈降之採樣器 17
圖2-7 以300-400 nm波長之UV光照射1,2,3,6,7,8-HxCDD後
產物分佈 18
圖2-8 2,3,7,8-位置戴奧辛之濃度隨時間變化趨勢 18
圖2-9 利用220-300 nm之波長照射PCDDs所得之照射強度
與殘留百分比之關係 19
圖2-10 利用310-400 nm之波長照射PCDDs所得之照射強度
與殘留百分比之關係 20
圖2-11 傳統落塵桶之收樣系統 23
圖2-12 森林內、外大氣採樣點其戴奧辛沉降量之同源物分佈特性 26
圖2-13 韓國大氣戴奧辛沉降量與時間之變化趨勢 27
圖2-14 義大利大氣戴奧辛沉降量與時間之變化趨勢 28
圖2-15 日本大氣戴奧辛沉降量與時間之變化趨勢 28
圖2-16 南韓市區與郊區每個月沈降量與粒狀物沈降量變化趨勢 30
圖2-17 乾沈降期間不同粒徑之粒狀物所佔比例分析 33
圖2-18 濕沈降期間不同粒徑之粒狀物所佔比例分析 33
圖2-19 日本 Kanto region之沈降粒狀物與沈降量關係 33
圖2-20 廣州市區PCDD/Fs於乾濕沈降中物種變化 34
圖2-21 PCDD/Fs於乾沈降時之沈降通量變化 35
圖2-22 PCDD/Fs於濕沈降時之沈降通量變化 35
圖3-1 研究流程 41
圖3-2 Automated sampler 示意圖 42
圖3-3 Automated sampler實照 42
圖3-4 傳統型落塵採樣桶裝置圖 43
圖3-5 PS-1採樣器示意圖 43
圖3-6 High volume air sampler示意圖 44
圖3-7 採樣地點 45
圖3-8 PS-1採樣作業流程 48
圖3-9 High volume air sampler採樣流程 51
圖3-10 高量採樣器之校正器 54
圖3-11 傳統落塵桶採樣流程 56
圖3-12 傳統落塵收樣系統 57
圖3-13 Automated sampler 採樣流程 58
圖3-14 採樣桶中實際渦流狀態 60
圖3-15 感雨計示意圖 62
圖3-16 戴奧辛樣品前處理流程示意 69
圖4-1 各月份之玫瑰風花圖 71
圖4-2 周界戴奧辛TEQ濃度逐月之變化 79
圖4-3 氣、固相戴奧辛分佈與大氣溫度之關係 81
圖4-4 TEQ沈降通量逐月變化之趨勢 87
圖4-5 以傳統落塵採樣器採集之沈降通量 88
圖4-6 以 Automated sampler 採集落塵之沈降通量 93
圖4-7 Automated sampler所得各月之沈降通量 94
圖4-8 不同沈降器之沈降通量比較 95
圖4-9 兩種採樣器所得沈降通量差異百分比與大氣溫度之相關性 97
圖4-10 各月之17種PCDD/Fs同源物之差異百分比 98
圖4-11 各月之乾、濕沈降通量 104
圖4-12 乾、濕沈降通量(以天為單位) 104
圖4-13 乾、濕沈降之平均沈降通量 105
圖4-14 乾、濕沈降之平均沈降通量百分比 105
圖4-15 濕沈降毒性通量與各月總降雨時數之關係 109
圖4-16 以傳統型採樣器所得毒性沈降通量與月平均溫度之關係 110
表目錄
表2-1 PCDD/Fs毒性當量係數 6
表2-2 戴奧辛各物種氣(V)固(P)相分布受大氣溫度之影響 7
表2-3 亞洲國家大氣中戴奧辛的濃度分布情形 9
表2-4 台灣特定污染源鄰近地區大氣中戴奧辛檢測結果 10
表2-5 PCDD/Fs於不同介質中半衰期之變化 21
表2-6 歐美各國大氣中戴奧辛沉降通量 24
表2-7 亞洲國家大氣中戴奧辛沉降量 26
表2-8 各國城市之沈降速度 37
表2-9 不同粒徑大小間濕沈降之去除效率 38
表2-10 降雨與霧氣之雨除係數 39
表3-1 PUF貫穿實驗結果 59
表4-1 氣象資料彙整 71
表4-2 週界PCDD/Fs濃度及物種分佈 76
表4-3 戴奧辛各物種氣(V)固(P)相分布受大氣溫度之影響 82
表4-4 以傳統落塵採樣器進行採樣之天數 84
表4-5 以傳統落塵採樣器採樣所得之PCDD/Fs沈降通量 85
表4-6 亞洲各國PCDD/Fs沈降通量比較 89
表4-7 Automated sampler 採樣時間 90
表4-8 以Automated sampler 採樣所得之PCDD/Fs沈降通量 91
表4-9 不同沈降器所得沈降量之差異百分比 96
表4-10 以感雨計偵測之乾、濕沈降各別採樣時間 99
表4-11 以Automated sampler 採樣所得之乾、濕沈降通量 100
表4-12 濕沈降對比於乾沈降之差異百分比 107
表4-13 毒性沈降通量與氣象條件之相關性 109
表4-14 乾、濕沈降與週界戴奧辛之物種相關性 111
表4-15 各月份之沉降速度 113
表4-16 各國沈降速度比較 113
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指導教授 張木彬(Moo-been Chang) 審核日期 2008-7-23
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