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研究生:蘇奕綾
研究生(外文):Yi-ling Su
論文名稱:稻草燃燒期間大氣中多環芳香烴化合物來源與粒徑分佈研究
論文名稱(外文):Source identification and size distribution of atmospheric polycyclic aromatic hydrocarbons during rice straw burning period
指導教授:楊錫賢楊錫賢引用關係
指導教授(外文):Hsi-Hsien Yang
學位類別:碩士
校院名稱:朝陽科技大學
系所名稱:環境工程與管理系碩士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2006
畢業學年度:94
語文別:中文
論文頁數:133
中文關鍵詞:懸浮微粒特徵比燃燒稻草多環芳香烴化合物粒徑分佈
外文關鍵詞:Size distributionsPAHsRice straw burning
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本研究針對稻作收成季節,農民就地燃燒稻草期間大氣中多環芳香烴化合物 (Polycyclic Aromatic Hydrocarbons, PAHs) 粒徑分佈特性進行研究。採樣於2004 年6 月至12 月間,以高流量PS-1 空氣採樣器 (High volume air sampler) 及微孔均勻沉積衝擊器 (Mirco-Orifice Uniform Deposit Impactor, MOUDI) 進行周界大氣中懸浮微粒與PAHs 濃度及粒徑分析,採集之樣品經前處理後以氣相層析質譜儀 (Gas Chromatograph / Mass Spectrometer, GC/MS) 進行PAHs 分析。
研究結果顯示燃燒稻草期間大氣中TSP 平均濃度為254 μg/m3,遠高於非燃燒稻草期間之108 μg/m3,且PM10/TSP 為非燃燒期的1.2 倍,顯示燃燒期間所產生之懸浮微粒以PM10 為主。此外,燃燒稻草與非燃燒稻草期間總PAHs 濃度分別為1193 ng/m3 與593 ng/m3,即大氣中PAHs 濃度隨燃燒稻草而增加。在總PAHs 之粒徑方面,燃燒稻草期間大致呈三峰分佈,最大波峰出現在細微粒範圍;非燃燒期間則呈雙峰分佈,最大波峰亦分佈於細微粒範圍。整體而言,燃燒稻草期間各階PAHs 濃度皆大於非燃燒稻草期間。總懸浮微粒之MMD (Mass median diameter, MMD) 於燃燒稻草與非燃燒稻草期間分別為1.1 與0.9 μm;總PAHs 之MMD 值分別為0.7 與0.5 μm,顯示燃燒稻草期間之懸浮微粒相對較大。在燃燒稻草期間大氣懸浮微粒中的PAHs 有60%以上存在於粒徑小於1 μm 之微粒上。另外,本研究藉由特徵比的比對來辨識PAHs 之來源,Benzo[a]pyrene/benzo[ghi]rylene 比顯示,在採樣區域燃燒稻草為PAHs 之重大來源,研究結果亦顯示,燃燒稻草主要貢獻細微粒之PAHs。稻草燃燒產生之微粒和微粒相PAHs 粒徑較車輛尾氣排放粗,且大氣微粒中PAHs 含量燃燒稻草期間小於非燃燒稻草期間。另外,燃燒稻草期間稻草燃燒所產生的PAHs 總毒性當量濃度為非燃燒稻草期間之 2.69 倍,顯著提高罹患癌症之機率。而燃燒稻草期間總 PAHs 之致癌風險佔百萬分之 0.7;非燃燒稻草期間總 PAHs 之致癌風險佔百萬分之
0.07。
This study investigates the polycyclic aromatic hydrocarbons (PAHs) size
distributions during rice straw burning periods. Samplings were conducted from
June, 2004 to September, 2004. A semi-volatile sampling equipment (PS-1
sampler) and a micro-orifice uniform deposit impactor (MOUDI) were used to
measure the mass concentrations and size distributions of particulate and PAHs.
PAHs was analyzed by gas chromatograph/mass selective detector (GC/MSD).
The results showed that the average TSP concentration was 254 μg/m3
during rice straw burning period, which was much higher than that during
non-rice straw burning period. PM10/TSP during rice straw burning period was
1.2 times higher than that during rice straw burning period. PAH concentrations
were 1193 ng/m3 and 593 ng/m3 during rice straw burning and non-burning
period, respectively, indicating that rice burning could induce high atmospheric
PAH concentration. There were three peaks for atmospheric PAH size
distribution during rice burning period. Mode I located in fine particle size range.
There were two peaks for atmospheric PAH size distribution during non-rice
burning period. Mode I also located in fine particle size range. PAH
concentrations in all size ranges were higher for rice burning period. The values
of mass median diameters (MMDs) of particulate were 1.1 and 0.9 μm during
rice burning and non-burning periods, respectively. The values of mass median
diameters (MMDs) of PAHs were 0.7 and 0.5 μm during rice burning and
non-burning periods, respectively. More than 60% PAHs existed in particulate
less than 1 μm diameter. The characteristic ratios were used to identify PAH
emission sources. The value of benzo[a]pyrene/benzo[ghi]perylene showed that
rice burning was the major PAH emission source during rice burning period.
The results also suggested that the rice straw burning primarily contribute fine
particulate PAHs. The particulate and particulate phase PAHs from rice straw
burning are coarser than those from vehicle exhaust. The results suggested that the amounts of PAHs per unit mass of particulate were less for the burning of
rice straw than those of vehicle emissions. Moreover, the total toxic equivalent
was 2.69 times higher for straw burning period than that of non-straw burning
period. The carcinogenic risk was 0.7 parts per million for straw burning period
and 0.07 parts per million for non-straw burning period.
總目錄
摘要........................................................................................................................I
Abstract ............................................................................................................... III
總目錄.................................................................................................................VI
表目錄.................................................................................................................. X
圖目錄................................................................................................................XII
第一章 前言......................................................................................................... 1
1-1 研究緣起................................................................................................. 1
1-2 研究目的與範疇..................................................................................... 3
第二章 文獻回顧................................................................................................. 4
2-1 懸浮微粒................................................................................................. 4
2-1-1 懸浮微粒之定義.......................................................................... 4
2-1-2 懸浮微粒之來源.......................................................................... 5
2-1-3 懸浮微粒之生成機制.................................................................. 7
2-1-4 懸浮微粒之粒徑分佈.................................................................. 9
2-1-5 懸浮微粒之危害性.................................................................... 10
2-2 多環芳香烴化合物............................................................................... 14
2-2-1 多環芳香烴化合物研究緣起.................................................... 14
2-2-2 多環芳香烴化合物之定義........................................................ 15
2-2-3 多環芳香烴化合物之來源........................................................ 18
2-2-4 多環芳香烴化合物之生成機制................................................ 22
2-2-5 多環芳香烴化合物之物化特性................................................ 26
2-2-6 多環芳香烴化合物之危害性.................................................... 31
VII
2-3 露天燃燒............................................................................................... 37
2-3-1 露天燃燒..................................................................................... 37
2-3-2 露天燃燒產生之空氣污染........................................................ 38
2-3-3 稻草燃燒對空氣品質之影響.................................................... 40
2-4 健康風險............................................................................................... 43
2-4-1 風險評估方法與程序................................................................ 43
2-4-2 非致癌性風險分析.................................................................... 46
2-4-3 致癌性風險分析........................................................................ 47
三、實驗設備與方法......................................................................................... 48
3-1 採樣規劃............................................................................................... 48
3-1-1 採樣地點與時程......................................................................... 49
3-2 採樣設備與方法................................................................................... 50
3-2-1 高流量PS-1 空氣採樣器............................................................ 50
3-2-2 微孔均勻沉積衝擊器................................................................ 56
3-3 採樣流程................................................................................................ 62
3-4 樣品分析................................................................................................ 63
3-4-1 樣品前處理.................................................................................. 64
3-4-2 實驗試劑..................................................................................... 66
3-4-3 氣相層析質譜儀 (GC/MS) ....................................................... 67
第四章 PAHs 分析品質保證與品質控制....................................................... 69
4-1 空白試驗............................................................................................... 69
4-1-1 溶劑空白..................................................................................... 69
4-1-2 濾紙空白..................................................................................... 69
4-1-3 現場空白..................................................................................... 70
4-1-4 運送空白..................................................................................... 70
VIII
4-1-5 採樣設備空白............................................................................ 70
4-2 方法偵測極限....................................................................................... 71
4-3 PAHs 成分分析方法............................................................................. 73
4-3-1 檢量線......................................................................................... 73
4-3-2 PAHs 儲備溶液的配置............................................................... 74
4-3-3 內標準溶液.................................................................................. 74
4-3-4 檢量線配置方法......................................................................... 75
4-3-5 標準品檢量線之建立................................................................ 76
4-3-6 檢量線確認................................................................................. 77
4-4 標準品回收率之準確度 (Accuracy) 及精密度 (Precision)............. 85
4-5 PAHs 於分析儀器之滯留時間......................................................... 88
4-6 儲備標準品穩定性測試....................................................................... 91
第五章 結果與討論........................................................................................... 92
5-1 懸浮微粒............................................................................................... 92
5-2 懸浮微粒粒徑分析............................................................................... 93
5-2-1 燃燒與非燃燒稻草期間懸浮微粒粒徑分佈............................ 93
5-2-2 懸浮微粒之質量中位數粒徑與幾何標準偏差........................ 95
5-3 多環芳香烴化合物粒徑分析............................................................... 96
5-3-1 燃燒與非燃燒稻草期間 PAHs 粒徑分佈............................... 96
5-3-2 PAHs 之質量中位數粒徑與幾何標準偏差.............................. 98
5-3-3 總PAHs 之濃度累積分佈......................................................... 99
5-4 多環芳香烴化合物濃度..................................................................... 100
5-4-1 懸浮微粒中21 種 PAHs 的含量........................................... 100
5-4-2 不同粒徑範圍微粒中 PAHs 含量......................................... 102
5-5 多環芳香烴化合物來源分析............................................................. 103
IX
5-5-1 大氣中PAHs 圖譜................................................................... 103
5-5-2 燃燒源 PAHs 圖譜................................................................. 105
5-5-3 PAHs 特徵比 (Characteristic ratio)......................................... 106
5-6 健康風險分析..................................................................................... 109
5-6-1 BaP 毒性當量........................................................................... 109
5-6-2 致癌性風險評估...................................................................... 113
第六章 結論..................................................................................................... 115
參考文獻........................................................................................................... 117
表目錄
表2-1 不同粒徑大小微粒之形成機制............................................................... 7
表2-2 二十一種 PAHs 之分子量、結構式及物理特性............................... 16
表2-2 二十一種PAHs 之分子量、結構式及物理特性 (續)......................... 17
表2-3 PAHs 之蒸氣壓、於25°C 水中之溶解度與親電性反應 (Eπ)........... 27
表2-4 二十一種 PAHs 之毒理特性............................................................... 33
表2-5 二十一種PAHs 之致癌性...................................................................... 35
表2-6 稻草的主要成分..................................................................................... 40
表3-1 MOUDI 各階段之截取粒徑.................................................................. 58
表4-1 GC/MS 之方法偵測極限....................................................................... 72
表4-2 PAHs 標準品之成分及濃度 (Chem Service) ....................................... 81
表4-3 PAHs 標準品之成分及濃度 (Gravimetric Certificate) ........................ 82
表4-4 PAHs 標準品原液稀釋成 10 μg/ml GC/MS 圖譜積分面積............... 83
表4-5 PAHs 標準品原液稀釋成 10 μg/ml 之GC/MS 圖譜積分面積平均
值、標準偏差及相對標準偏差................................................................. 84
表4-6 標準品之回收率..................................................................................... 86
表4-7 PAHs 標準品回收率之精密度與準確度.............................................. 87
表4-8 二十一種 PAHs 於 GC/MS 之滯留時間 (min) ................................ 89
表4-9 二十一種 PAHs 於 GC/MS 滯留時間平均值及標準偏差............... 90
表4-10 二十一種 PAHs 標準品在質譜儀中掃描定量與次要離子............. 91
表5-1 總懸浮微粒與PM10 濃度....................................................................... 92
表5-2 PM 之質量中位數粒徑及幾何標準偏差............................................... 95
表5-3 PAHs 之質量中位數粒徑及幾何標準偏差.......................................... 98
表5-4 懸浮微粒中 21 種 PAHs 含量.......................................................... 101
表5-5 PAHs 特徵比之比較............................................................................. 108
XI
表5-6 燃燒稻草期間 21 種 PAHs 之毒性當量係數................................. 111
表5-7 非燃燒稻草期間 21 種 PAHs 之毒性當量係數............................. 112
表5-8 燃燒稻草與非燃燒稻草期間 21 種 PAHs 之致癌風險................. 114
附表1 稻草成分分析...................................................................................... 129
附表2 燃燒源 PAHs 濃度 (μg/m3)............................................................... 130
附表2 燃燒源 PAHs 濃度 (μg/m3) (續)....................................................... 131
附表3 燃燒源排放係數.................................................................................. 131
XII
圖目錄
圖2-1 大氣氣膠表面積粒徑分布圖.................................................................... 8
圖2-2 典型大氣懸浮微粒之粒徑分佈圖........................................................... 9
圖2-3 PAHs 生成之熱烈解反應........................................................................ 23
圖2-4 PAHs 生成之聚合反應............................................................................ 24
圖2-5 PAHs 在大氣中與氮氧化物之反應式.................................................. 25
圖3-1 採樣點位置圖......................................................................................... 49
圖3-2 PS-1 採樣器構造圖................................................................................ 51
圖3-3 玻璃套筒填充方式................................................................................. 52
圖3-4 PS-1 採樣器壓力表讀數與水柱高差關係圖........................................ 55
圖3-5 PS-1 採樣器壓力表讀數與流量關係圖................................................ 55
圖3-6 微孔均勻沉積衝擊................................................................................. 57
圖3-7 階段式衝擊............................................................................................. 57
圖3-8 MOUDI 採樣器流量校正圖................................................................... 61
圖3-9 採樣流程圖............................................................................................. 62
圖3-10 索氏萃取設備....................................................................................... 64
圖4-1 Nap, AcPy, Acp, Flu, PA, Ant, FL, Pyr 之檢量線.................................. 78
圖4-2 CYC, BaA, CHR, BbF, Bep, BaP, PER 之檢量線................................. 79
圖4-3 IND, DBA, BbC, Bghip, COR 之檢量線................................................ 80
圖5-1 MOUDI 採樣燃燒與非燃燒稻草期間 PM 之粒徑分佈.................... 94
圖5-2 MOUDI 採樣燃燒與非燃燒稻草期間 PAHs 之粒徑分佈................. 97
圖5-3 PAHs 累積分佈百分比 (%).................................................................... 99
圖5-4 不同粒徑範圍下 PAHs 之含量.......................................................... 102
圖5-5 燃燒稻草與非燃燒稻草期間 PAHs 之圖譜..................................... 104
圖5-6 燃燒源 PAHs 之圖譜.......................................................................... 105
XIII
附圖1 玫瑰風花圖.......................................................................................... 133
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4. 41.溫豐文,〈善意占有人之孳息收取權〉,《臺灣本土法學雜誌》,第33期(2002年4月)。
5. 40.溫豐文,〈論不動產登記─以探討民法物權編修正草案之規定為主〉,《月旦法學雜誌》,第68期(2001年1月)。
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