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研究生:陳柏嘉
研究生(外文):Chen, Bo-Chia
論文名稱:泡棉盤被動式空氣採樣器之定量改善與擴散梯度薄膜之監測效能評估
指導教授:凌永健凌永健引用關係
學位類別:博士
校院名稱:國立清華大學
系所名稱:化學系
學門:自然科學學門
學類:化學學類
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:202
中文關鍵詞:泡棉盤被動式空氣採樣器擴散梯度薄膜被動式空氣
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國際現行的採樣標準方法,多用需外加能源及人為控制的主動式採樣方法,然而主動式採集樣品分析結果只代表特定時間內之污染物組成和濃度,為瞬時濃度值,無法呈現出一般的污染情形,必須提高採樣的時間長度和頻率才有可能釐清,對於超微量污染物則需加長採樣時間至採集儀器足以偵測的濃度,導致工作量大且花費不貲,而被動式採樣裝置(PAD)不需用外加能源及人為控制,可以進行大地區長時間採樣,採樣之時間和空間解析度佳,檢測結果與生物毒性關聯性佳,國際間相關研究及應用與日俱增。
本研究開發新的風速統計方式,用以定量風速影響,得到風速校正因子,成功校正泡棉盤(PUF disk)被動式空氣採樣器(PAS)採樣速率,在高風速時(> 4 m/s)使用PAS測得之類戴奧辛化合物(DCLs)濃度及趨勢與主動式空氣採樣器(AAS)類似,同時使用階層式集群分析法(HCA)顯示PUF disk PAS得到之周界空氣DCLs同源物組成特性與AAS相似,並成功用於實際監測與釐清可能污染來源,結果顯示台灣的代表高污染潛勢地區主要汙染來源類別為小型焚化爐、輔助燃料(木削為主)和二次銅/鐵冶煉製程;東南亞的代表地區主要為交通廢氣和火耕行為貢獻,且其濃度較低,屬於背景值範圍。
擴散梯度薄膜(DGT),使用擴散膠將吸附樹脂與溶液分隔,擴散膠可作質傳的擴散控制,可藉採樣天數和擴散係數獲得金屬物種的估算濃度。本研究的模擬實驗建立Mn、Ni、Cu、In、Cd、Ga、Ba和Pb等之擴散速率,DGT用於實際監測河川水和湖水等自然水體,歸納出DGT能測得Mn、Ni和Cu與主動式方法類似的濃度結果;In、Cd、Ga、Ba、Pb、Cr、Fe、Mo、Ag、As、Se和Sb會因形成物種使濃度有差異,但能反映濃度級數和趨勢。

The standard sampling methods usually require external power and controller. The methods usually collected a small amount of discrete samples which were subsequently analyzed using standard methods. If the data meet the requirements of quality control and quality assurance, we can identify law-violating contaminating source in due time. However, the data can’t represent the normal pollution situation. For contaminant concentration varying with time, we need to prolong sampling time and increase sampling frequency to assist identifying the contaminating source at the price of heavier workload and higher expense. Similar problems are encountered when analyzing ultratrace contaminants, bioaccumulating and bioavailable toxic substances. Passive accumulation devices (PAD) are free of external power and human intervention.
Polyurethane foam (PUF) disk passive air sampler (PAS) has been successfully applied to persistent organic pollutants (POPs) in air. This study we successfully quantified the wind effect by monitoring and classifying wind speeds into ranges. Our calculated concentrations of dioxin-like compounds for PUF disk PAS samples approach those determined by active air sampling (AAS) methods. The hierarchical cluster analysis (HCA) indicated the PUF disk PAS can determine congener profiles of PCDD/Fs in ambient air. We also clarified the kind of dioxin pollution sources in monitoring area: They are small incinerator, auxiliary fuel (wood shavings) and secondary copper/iron smelters at industrial area in Taiwan; traffic exhaust gas and outdoor burning at Southeast Asia with background level concentration.
Diffusion Gradients in Thin-film (DGT) use diffusive gel to separate the resin layer from bulk solution. The metal ions diffusing through the diffusive gel, the diffusion coefficient in the gel and sampling tine could calculate labile metal ion concentration. We established diffusion coefficient of metal like Mn, Ni, Cu, In, Cd, Ga, Ba and Pb. About application to natural water like river and lake, DGT could calculate the labile Mn, Ni and Cu concentration approach those determined by active methods; the concentration grade and trend of Cd, Ga, Ba, Pb, Cr, Fe, Mo, Ag, As, Se and Sb.

第一章 前言
1-1
1.1 被動式採樣技術的崛起 1-1
1.2 研究主題 1-8
第二章 修正高風速對PUF disk PAS的影響並定量空氣中類戴奧辛化合物
2.1 導論 2-1
2.1.1 持久性污染物 2-1
2.1.2 被動式空氣採樣器(passive air sampler, PAS)研究概況 2-5
2.1.3 PAS採樣理論 2-6
2.1.4 研究目的 2-9
2.2 實驗規劃 2-10
2.2.1 PUF disk PAS製作 2-10
2.2.2 模擬實驗 2-12
2.2.3 PUF disk PAS應用於偶發高風速地區的實際採樣 2-14
2.2.4 風速校正PAS數據方法 2-16
2.3 採樣與分析方法 2-19
2.3.1 採樣流程 2-19
2.3.2 前處理流程 2-20
2.3.3 HRGC/HRMS分析 2-29
2.4 結果與討論 2-39
2.4.1 品保/品管 2-39
2.4.2 模擬實驗高流量AAS和PUF disk PAS分析結果 2-41
2.4.3 建立飽和曲線 2-49
2.4.4 PUF disk PAS的採樣速率建立結果 2-52
2.4.5 階層式集群分析法(hierarchical cluster analysis, HCA)分析結果 2-56
2.4.6 採樣速率的風速影響校正 2-66
2.4.7 比較高流量AAS和PUF disk PAS的定量結果 2-68
2.5 結論 2-74
第三章 PUF disk PAS實際應用
3.1 高戴奧辛污染潛勢地區空氣中類戴奧辛化合物濃度與污染來源類別調查 3-1
3.1.1 研究動機 3-1
3.1.2 研究規劃 3-1
3.1.3 結果與討論 3-3
3.2 東南亞區域空氣中類戴奧辛化合物濃度與來源類別調查 3-31
3.2.1 研究動機 3-31
3.2.2 研究規劃 3-32
3.2.3 結果與討論 3-34
3.3 結論 3-48
第四章 DGT針對自然水體中金屬採樣方法開發
4.1 導論 4-1
4.1.1 微量金屬來源與簡介 4-1
4.1.2 擴散梯度薄膜(Diffusion Gradients in Thin-film, DGT)研究現況 4-5
4.1.3 DGT採樣理論 4-8
4.1.4 研究目的 4-11
4.2 實驗規劃 4-12
4.2.1 模擬實驗 4-12
4.2.2 實際採樣 4-15
4.3 採樣與分析方法 4-18
4.3.1 採樣流程 4-18
4.3.2 前處理流程 4-20
4.3.3感應耦合電漿質譜儀(Inductively Coupled Plasma Mass Spectrometer,
ICP-MS)分析 4-20
4.4 結果與討論 4-23
4.4.1 模擬實驗 4-23
4.4.2主動式採樣的濃度分析結果 4-31
4.4.3 DGT估算濃度與主動式分析濃度比較 4-43
4.5 結論 4-58
第五章 未來展望與總結
5.1未來展望 5-1
5.1.1泡棉盤被動式空氣採樣器(Polyurethane foam disk passive air sampler, PUF
disk PAS) 5-1
5.1.2擴散梯度薄膜(Diffusion Gradients in Thin-film, DGT) 5-1
5.2總結 5-2
參考文獻

表 目 錄
表1-1 PAD的研發時程表 1-3
表1-2 被動式採樣與生物監測及主動式採樣的優、缺點比較 1-6
表2-1 17種戴奧辛同源物的毒性當量因子 2-3
表2-2 12種共平面型多氯聯苯世界衛生組織毒性當量因子 2-4
表2-3 PUF disk PAS及使用器具規格 2-11
表2-4 PUF disk PAS監測空氣中PCDD/Fs和DL-PCBs的模擬實驗內容 2-13
表2-5 不同風速範圍影響程度(Wc)的校正倍數假設 2-18
表2-6 PUF disk和氣相樣品使用的13C及37Cl-同位素標幟標準品溶液(PCDD/Fs) 2-22
表2-7 固相樣品使用的13C及37Cl-同位素標幟標準品溶液(PCDD/Fs) 2-23
表2-8 樣品使用的13C同位素標幟標準品溶液(DL-PCBs) 2-24
表2-9 HRGC/HRMS層析儀及質譜儀操作條件參數 2-31
表2-10 PCDD/Fs待測物和13C-及37Cl-同位素標幟物監測離子 2-32
表2-11 PUF disk和氣相樣品用的PCDD/Fs起始檢量校正標準溶液 2-33
表2-12 固相樣品用的PCDD/Fs起始檢量校正標準溶液 2-34
表2-13 樣品用的DL-PCBs起始檢量校正標準溶液 2-35
表2-14 樣品用的PCDD/Fs和DL-PCBs檢量校正相對感應因子品管限值 2-36
表2-15 樣品之PCDD/Fs和PCBs離子強度比之品管範圍 2-37
表2-16 模擬實驗和實際採樣分析PCDD/Fs和DL-PCBs數據的品保/品管結果 2-40
表2-17 模擬實驗高流量AAS的氣相PCDD/Fs同源物濃度 2-42
表2-18 模擬實驗高流量AAS的固相PCDD/Fs同源物濃度 2-43
表2-19 模擬實驗PUF disk PAS的PCDD/Fs同源物截存量 2-44
表2-20 模擬實驗高流量AAS的氣相DL-PCBs同源物濃度 2-45
表2-21 模擬實驗高流量AAS的固相DL-PCBs同源物濃度 2-46
表2-22 模擬實驗PUF disk PAS的DL-PCBs同源物截存量 2-47
表2-23 模擬實驗PUF disk PAS監測空氣中PCDD/Fs和DL-PCBs同源物的採樣速率(RStotal和RSg) 2-55
表2-24 實際採樣高流量AAS樣品中氣相(Cp)和固相(Cg)PCDD/F濃度 2-58
表2-25 實際採樣PUF disk PAS樣品中PCDD/F同源物截存量 2-59
表2-26 實際採樣高流量AAS樣品中氣相(Cp)和固相(Cg)DL-PCBs濃度 2-60
表2-27 實際採樣PUF disk PAS樣品中DL-PCBs同源物截存量 2-61
表2-28 模擬實驗和實際採樣PUF disk PAS架設期間的風速影響定量結果(M)和修正倍數(N) 2-67
表2-29 實際採樣高流量AAS和PUF disk PAS監測空氣中的PCDD/F和DL-PCB毒性當量濃度 2-70
表2-30 各方法計算實際採樣PUF disk PAS與高流量AAS毒性當量濃度的相對差異百分比(RPD, %) 2-71
表3-1 PUF disk PAS監測工業區的風速影響定量結果(M)和修正倍數(N) 3-4
表3-2 高污染潛勢地區之採集樣品的品保/品管結果 3-7
表3-3 PUF disk PAS和高流量AAS監測工業區空氣中PCDD/Fs毒性當量濃度 3-8
表3-4 PUF disk PAS監測工業區空氣中DL-PCBs毒性當量濃度 3-9
表3-5 PUF disk PAS監測工業區空氣中PCDD/Fs同源物截存量(I) 3-14
表3-6 PUF disk PAS監測工業區空氣中PCDD/Fs同源物截存量(II) 3-15
表3-7 PUF disk PAS監測工業區空氣中PCDD/Fs同源物截存量(III) 3-16
表3-8 PUF disk PAS監測工業區空氣中PCDD/Fs同源物截存量(IV) 3-17
表3-9 高流量AAS監測工業區空氣中PCDD/Fs同源物濃度(I) 3-18
表3-10 高流量AAS監測工業區空氣中PCDD/Fs同源物濃度(II) 3-19
表3-11 高流量AAS監測工業區空氣中PCDD/Fs同源物濃度(III) 3-20
表3-12 PUF disk PAS監測工業區空氣中DL-PCBs同源物截存量(I) 3-21
表3-13 PUF disk PAS監測工業區空氣中DL-PCBs同源物截存量(II) 3-22
表3-14 PUF disk PAS監測工業區空氣中DL-PCBs同源物截存量(III) 3-23
表3-15 PUF disk PAS監測工業區空氣中DL-PCBs同源物截存量(IV) 3-24
表3-16 PUF disk PAS在東南亞採樣時間和地區 3-32
表3-17 東南亞地區之採集樣品的品保/品管結果 3-34
表3-18 PUF disk PAS監測東南亞空氣中PCDD/Fs同源物截存量結果(第1次) 3-35
表3-19 PUF disk PAS監測東南亞空氣中PCDD/Fs同源物截存量結果(第2次) 3-36
表3-20 PUF disk PAS監測東南亞空氣中DL-PCBs同源物截存量結果(第1次) 3-37
表3-21 PUF disk PAS監測東南亞空氣中DL-PCBs同源物截存量結果(第2次) 3-38
表3-22 PUF disk PAS監測東南亞空氣中PCDD/Fs同源物定量濃度結果(第1次) 3-39
表3-23 PUF disk PAS監測東南亞空氣中PCDD/Fs同源物定量濃度結果(第2次) 3-40
表3-24 PUF disk PAS監測東南亞空氣中DL-PCBs同源物定量濃度結果(第1次) 3-41
表3-25 PUF disk PAS監測東南亞空氣中DL-PCBs同源物定量濃度結果(第2次) 3-42
表3-26 PUF disk PAS監測東南亞空氣中PCDD/Fs和DL-PCBs
毒性當量濃度結果 3-43
表4-1 不同模擬實驗水質條件 4-13
表4-2 ICP-MS儀器參數之參考值 4-22
表4-3 模擬實驗結果(偏酸性) 4-25
表4-4 不同濃度級數和流速的模擬實驗(偏鹼性)結果 4-26
表4-5 模擬實驗(偏酸性)截存量(ng) 4-27
表4-6 不同濃度級數和流速的模擬實驗(偏鹼性)截存量(ng) 4-28
表4-7 模擬實驗(偏酸性)重覆實驗結果 4-29
表4-8 不同濃度級數和流速的模擬實驗(偏鹼性)重覆實驗結果 4-30
表4-9 實際採樣日期和水質條件(A檢驗單位) 4-32
表4-10 實際採樣日期和水質條件(牛稠坑溪) 4-33
表4-11 實際採樣日期和水質條件(霄裡溪-第一次) 4-34
表4-12 實際採樣日期和水質條件(霄裡溪-第二次) 4-35
表4-13 實際採樣日期和水質條件(清華大學) 4-36
表4-14 實際主動式採樣濃度分析結果(ppb)-A檢驗單位 4-37
表4-15 實際主動式採樣濃度分析結果(ppb)-牛稠坑溪 4-38
表4-16 實際主動式採樣濃度分析結果(ppb)-霄裡溪(第一次) 4-39
表4-17 實際主動式採樣濃度分析結果(ppb)-霄裡溪(第二次) 4-40
表4-18 實際主動式採樣濃度分析結果(ppb)-清華大學 4-42
表4-19 第一次實際採樣DGT截存量(ng) -A檢驗單位 4-45
表4-20 實際採樣DGT截存量(ng)-牛稠坑溪和霄裡溪(第一次) 4-46
表4-21 實際採樣DGT截存量(ng)-霄裡溪(第二次) 4-47
表4-22 實際採樣DGT截存量(ng)-清華大學 4-48
表4-23 實際採樣DGT估算濃度(ppb)- A檢驗單位 4-49
表4-24 實際採樣DGT估算濃度(ppb)-牛稠坑溪和霄裡溪(第一次) 4-50
表4-25 實際採樣DGT估算濃度(ppb)-霄裡溪(第二次) 4-51
表4-26 實際採樣DGT估算濃度(ppb)-清華大學 4-52
表4-27 真實採樣主動式分析與DGT估算濃度倍率比較- A檢驗單位 4-53
表4-28 真實採樣主動式分析與DGT估算濃度倍率比較-牛稠坑溪和霄裡溪(第一次) 4-54
表4-29 真實採樣主動式分析與DGT估算濃度倍率比較-霄裡溪(第二次) 4-55
表4-30 真實採樣主動式分析與DGT估算濃度倍率比較-清華大學 4-56
表4-31 DGT實際採樣的適用環境條件和金屬物種 4-57

圖 目 錄
圖1-1 被動式採樣器應用於環境品質監測應用之論文 1-8
圖2-1 被動式空氣採樣器的平衡飽和曲線圖 2-8
圖2-2 PUF disk PAS裝置內部圖 2-11
圖2-3 模擬實驗PUF disk PAS架設照片 2-13
圖2-4 實際採樣地點和氣象站分布圖 2-15
圖2-5 酸性矽膠淨化管柱示意圖 2-27
圖2-6 酸性氧化鋁淨化管柱示意圖 2-27
圖2-7 活性碳淨化管柱示意圖 2-28
圖2-8 2,3,7,8-TeCDD在DB-5MS層析管柱之解析度 2-38
圖2-9 模擬實驗高流量AAS和PUF disk PAS的(a)PCDD/Fs和(b)DL-PCBs同源物組成分布比較 2-48
圖2-10 模擬實驗PUF disk PAS的PCDD/Fs截存量與採樣天數趨勢圖 2-50
圖2-11 模擬實驗PUF disk PAS的DL-PCBs截存量與採樣天數趨勢圖 2-51
圖2-12 模擬實驗高流量AAS樣品中(a)PCDD/Fs和(b)DL-PCBs同源物的氣固百分比 2-54
圖2-13 實際採樣高流量AAS樣品中PCDD/Fs同源物的氣固相百分比 2-62
圖2-14 實際採樣高流量AAS樣品中DL-PCBs同源物的氣固相百分比 2-63
圖2-15 實際採樣PUF disk PAS和高流量AAS樣品與美國各種空氣污染排放的PCDD/Fs同源物組成的HCA分析結果 2-64
圖2-16 實際採樣PUF disk PAS和高流量AAS樣品的DL-PCBs同源物組成的HCA分析結果 2-65
圖2-17 實際採樣高流量AAS和PUF disk PAS監測空氣中的PCDD/F的毒性當量濃度比較圖 2-72
圖2-18 實際採樣高流量AAS和PUF disk PAS監測空氣中的DL-PCB的毒性當量濃度比較圖 2-73
圖3-1 工業區採樣點分布圖 3-2
圖3-2 PUF disk PAS和高流量AAS監測工業區空氣中PCDD/s毒性當量濃度比較圖 3-10
圖3-3 PUF disk PAS監測工業區空氣中DL-PCBs毒性當量濃度比較圖 3-11
圖3-4 PUF disk PAS和高流量AAS樣品與列管工廠煙囪排放的PCDD/Fs同源物組成的HCA分析結果-A工業區 3-25
圖3-5 PUF disk PAS和高流量AAS樣品與列管工廠煙囪排放的PCDD/Fs同源物組成的HCA分析結果-B工業區 3-26
圖3-6 PUF disk PAS和高流量AAS樣品與列管工廠煙囪排放的PCDD/Fs同源物組成的HCA分析結果-C工業區 3-27
圖3-7 PUF disk PAS和高流量AAS樣品與美國各種空氣污染排放的PCDD/Fs同源物組成的HCA分析結果 3-28
圖3-8 PUF disk PAS樣品的DL-PCBs同源物組成的HCA分析結果-A、B和C工業區 3-29
圖3-9 PUF disk PAS監測東南亞地區空氣中PCDD/Fs和DL-PCBs的總毒性當量濃度分布圖 3-44
圖3-10 PUF disk PAS樣品與美國各種空氣污染排放的PCDD/Fs同源物組成的HCA分析結果 3-46
圖3-11 PUF disk PAS樣品的DL-PCBs同源物組成的HCA分析結果-東南亞地區 3-47
圖4-1 DGT的功能示意圖和對應之實際照片 4-7
圖4-2 DGT截存水中活性金屬離子示意圖 4-10
圖4-3 模擬系統設計圖(上)與實體圖(下) 4-14
圖4-4 牛稠坑溪採樣點分布圖 4-16
圖4-5 霄裡溪採樣點分布圖 4-16
圖4-6 清華大學景觀湖採樣點分布圖 4-17
圖4-7 實際採樣之DGT架設 4-19

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