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研究生:石珮琦
研究生(外文):Pei-chi Shih
論文名稱:高雄地區大氣顆粒態多環芳香烴-污染來源及濃度影響因子
論文名稱(外文):Source identification of atmospheric particulate polycyclic aromatic hydrocarbons in Kaohsiung
指導教授:李宗霖李宗霖引用關係
指導教授(外文):Chon-Lin Lee
學位類別:碩士
校院名稱:國立中山大學
系所名稱:海洋環境及工程學系研究所
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:2015
畢業學年度:104
語文別:中文
論文頁數:156
中文關鍵詞:多環芳香烴PM2.5資料群集處理技術正矩陣分解因子來源分析
外文關鍵詞:PM2.5source analysisPMFGMDHPAHs
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為了瞭解高雄地區懸浮微粒以及多環芳香烴之汙染情形,本研究於2014年1月至2014年12月期間,依照區域型態,分別於海岸地區(NSYSU)、高雄工業區(SG)、交通區(AG)以及住宅區(FS)設置採樣點,藉由採集大氣懸浮微粒(PM2.5、PM2.5-10),並分析其多環芳香烴化合物(PAHs),來探討高雄地區不同區域之污染濃度,進而分析主要污染來源以及濃度影響因子。研究結果顯示四個測站之懸浮微粒年平均濃度(PM2.5、PM2.5-10)皆以SG最高,FS最低,其PM2.5年平均濃度分別為 43.3 ng m-3 (NSYSU)、50.8 ng m-3 (SG)、45.6 ng m-3 (AG)、39.0 μg〖 m〗^(-3) (FS),PM2.5-10年平均濃度分別為16.7 ng m-3 (NSYSU)、18.0 ng m-3 (SG)、16.1 ng m-3 (AG)、15.3 μg〖 m〗^(-3) (FS)。採樣期間大部份之PM2.5濃度皆超過我國空氣品質之日平均規範值,PM10則大都符合規範標準。在PAHs分佈方面,大氣懸浮微粒中之多環芳香烴主要是分佈在PM2.5上,且以高環數的PAH為主,其平均濃度以SG最高、NSYSU最低,濃度分別為 0.91 ng m-3 (NSYSU)、2.36 ng m-3 (SG)、1.87 ng m-3 (AG)、1.27 ng m-3 (FS)。
多環芳香烴來源之綜合分析結果顯示,各測站PM2.5上的多環芳香烴主要來自汽柴油燃燒之交通來源。此外,在SG測站則有比較強的燃煤訊號,FS地區則有天然氣燃燒來源之訊號。不同於PM2.5,PM2.5-10 上NSYSU、AG、FS 是以汽油為主的交通排放來源,SG則是汽油排放及燃煤混和來源。此外,PMF分析結果顯示NSYSU測站PM2.5之主要來源為其柴油混和之交通來源(占61%),SG則是汽柴油來源為主(46%),AG測站主要污染來源為交通排放(46%),FS則是柴油及天然氣混和燃燒來源(51%)。
在模式預測部分,本研究將過去2013年之監測數據利用GMDH模式建模,來驗證及預測採樣期間(2014年)之多環芳香烴濃度,模式效能解析出之大氣中多環芳香烴濃度主要影響因子為PM2.5、PM10、氮氧化物以及雨量,模式效能屬於高準度的預測以及合理的預測,且預測出之季節變化趨勢跟實驗結果相符。
Polycyclic aromatic hydrocarbons (PAHs) were analyzed from ambient air particulate matter (PM2.5 and PM2.5–10) at four sampling sites in Kaohsiung city to characterize the spatiotemporal distribution and source identification. Air samples were collected at NSYSU site (coastal area), SG (industrial area), AG (urban area) and FS (residential area) from January to December 2014.
The annual mean concentrations of atmospheric PM2.5 (PM2.5-10) at NSYSU, SG, AG, and FS were 43.3 (16.7), 50.8 (18.0), 45.6 (16.1), and 39.0 (15.3) μg m-3, respectively. The highest concentration of PM2.5 and PM2.5-10 was found at SG, followed by AG, while the lowest one was found at FS. Most samples exceeded the 24-hr air quality standards of PM2.5; while only a few PM10 did not meet the standards. The particle size distribution of PAHs shows that PM2.5 had higher PAHs concentrations than PM2.5–10, and high molecular weight (HMW) PAHs prefer partitioning in PM2.5 as compared to low molecular weight (LMW) PAHs. The annual mean concentration of PM2.5-PAHs at NSYSU, SG, AG, and FS were 0.91, 2.36, 1.87, and 1.27 ng m-3, respectively. It was found that SG had the highest concentration of PM2.5-PAHs, followed by AG, FS, and NSYSU
The results of diagnostic ratios, HCA/PCA and Positive Matrix Factor (PMF) suggested that the major sources of PM2.5-PAHs at four sites were traffic emission from gasoline and diesel engines. In addition, SG site had strong signal from coal combustion and FS site also had signal from natural gas combustion. Unlike PM2.5-PAHs, the main source of PAHs on PM2.5-10 was traffic emission from gasoline engine exhausts in NSYSU, AG and FS sites; gasoline emission and coal combustion mixed sources for SG site.
The PMF results also indicated that the PM2.5-PAH contribution of traffic emission was 61% from gasoline and diesel at NSYSU site, diesel and gasoline burning contributed 46% at SG site, traffic emission accounted for 46% at AG site, and the source mixed with diesel and natural gas combustion was estimated to contribute approximately 51% at FS site.
According to the results of Group Method of Data Handling (GMDH), the PM2.5-PAHs concentration variation was associated with PM2.5, PM10, NOx and rainfall. Model prediction of PM2.5-PAH showed seasonal variation in 2014 was good agreement with measured data.
目錄
論文審定書 i
論文公開授權書 ii
誌謝 iii
摘要 iv
Abstract v
圖目錄 x
表目錄 xiii
第一章 前言 1
1-1研究動機 1
1-2研究目的 3
第二章 文獻回顧 4
2-1多環芳香烴介紹 4
2-1-1多環芳香烴特性介紹 4
2-1-2多環芳香烴的來源 7
2-1-3多環芳香烴毒性 8
2-1-4多環芳香烴指紋特徵 10
2-2 正矩陣分解因子 11
2-2-1 PMF基本概述 11
2-2-2 PMF之運算原理 12
2-2-3 EPA PMF v5.0軟體操作介紹 13
2-3 資料群及處理技術 17
2-3-1 資料群集處理技術(GMDH)概述 17
2-3-2 GMDH演算法之基本參數設定與說明 19
第三章 研究方法 21
3-1研究流程 21
3-2材料與儀器 22
3-2-1 材料 22
3-2-2試藥及器具前處理 22
3-3-2設備與分析儀器 23
3-3採樣與保存 22
3-3-1採樣時間與地點 25
3-3-3採樣方法 26
3-4樣品分析 27
3-5品保及品管(QA/QC) 29
3-5-1空白實驗 29
3-5-2方法偵測極限 29
3-5-3擬似標準品回收率 29
3-6資料分析 31
3-6-1主成分分析法(Principal Component analysis, PCA) 31
3-6-2階層群集方法(Hierarchical Cluster Analysis, HCA) 31
3-6-3正矩陣分解因子 (Positive Matrix Factor) 31
3-6-4資料群集處理技術 (Group Method of Data Handling, GMDH) 32
第四章 結果與討論 33
4-1大氣中懸浮微粒濃度 33
4-1-1懸浮微粒濃度空間分布 33
4-1-2懸浮微粒濃度時間分布 38
4-2大氣中多環芳香烴濃度 44
4-2-1多環芳香烴時空濃度變化 44
4-2-2 PM2.5及PM2.5-10上多環芳香烴濃度分布 47
4-2-3懸浮微粒與PAHs之關係 59
4-3來源分析 60
4-3-1化學指紋特徵 60
4-3-2主成分分析 (Principal Component Analysis, PCA) 67
4-3-3階層群集分析 (Hierarchical Cluster Analysis, HCA) 76
4-3-4正矩陣分解因子(Positive Matrix Factor) 87
4-4大氣中多環芳香烴毒性當量因子及健康風險評估 94
4-4-1大氣中BaP濃度之時空變化 94
4-4-2大氣中BaPeq濃度之時空變化 97
4-5 資料群集處理技術(Group Method of Data Handling, GMDH) 109
4-5-1多環芳香烴預測結果分析 109
4-5-2實際案例預測結果 112
第五章 結論與建議 115
5-1 結論 115
5-2 建議 116
參考文獻 118
附錄 123
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