臺灣博碩士論文加值系統

本研究於2005年3至2006年3月間，在環保署屏東空氣品質監測站（簡稱屏東站）以分道採樣器（Dichot）及泛用型採樣器（UAS）採集大氣粗（PM2.5-10）及細（PM2.5）懸浮微粒；採樣後濾紙上之微粒樣品以離子層析儀（Dionex DX-120）分析微粒上之水溶性離子，碳成分以總有機碳分析儀（TOC-500A）分析，金屬成分以感應耦合電漿質譜儀（ICP-MS）及感應耦合電漿原子發射光譜儀（ICP-AES）分析，而PAHs則以氣相層析質譜儀（GC/MS）進行分析。由本研究結果顯示：在本研究採樣期間，屏東站PM2.5、PM2.5-10及PM10濃度之平均值分別為57.2±27.9、19.3±10.5及76.4±36.8 μg/m3，大氣懸浮微粒主要由細微粒所貢獻（佔75.9%）；水溶性離子均為PM2.5及PM2.5-10微粒上之主要成分，其平均佔微粒之比例分別為45.8及36.9%。於冬季期間其大氣氣膠之濃度最高，其PM2.5或PM10在四季中濃度之大小依序均為冬季>秋季>春季>夏季；各微粒上NO3-、SO42-及NH4+等衍生性氣膠佔水溶性離子之比例為68~91%，衍生性氣膠為水溶性離子之主要貢獻物種。
加強因子分析之結果顯示：其微粒上之Cl-及Mg2+主要來自海水飛沫；而微粒上之SO42-、K+及Ca2+可能分別來自人為活動及地殼元素所貢獻。歷次採樣期間，其PM2.5上TC、EC及OC之濃度皆較PM2.5-10上之值高，微粒上之碳成分主要分佈在細微粒（PM2.5）上。PM2.5及PM2.5-10微粒上之金屬元素均以Na、Mg、Al、Si、S、K、Ca、Fe及Zn為主要物種(以S之濃度最高)；屬於地殼元素之Na、Mg、Al、Si、Ca、Fe及Ti等主要分佈於粗微粒上(PM2.5-10)上，而人為污染排放之S、Cr、Ni、Zn及Pb等則主要分佈於細微粒(PM2.5)上。
於本研究採樣期間，其PM2.5、PM2.5-10及PM10微粒上所分析之物種中均以水溶性離子（分別佔45.8、36.9及43.7%）佔之比例最高，碳成分（分別佔30.0、26.0及29.1%）次之，金屬元素佔之比例為最低，而未分析成分（others）佔之比例依序分別為14.0、19.8及15.3%。大氣微粒上PAHs之平均濃度以冬季時最高，無論於何季節其微粒上之PAHs均主要分佈於細微粒（PM2.5）上；微粒上所測之21種PAHs均以HMW-PAHs為主(佔48~66%)。PM2.5微粒上其LMW-、MMW-、HMW-及Total-PAHs毒性當量之平均值均約為其PM2.5-10值之4倍，因細微粒易進入人體肺部深處，其對人體健康之影響及危害值得加以重視。
與ADS來襲前後（即Non-ADS時）相比，於ADS來襲期間，雖其粗細微粒之濃度均有明顯增加，然其粗微粒（PM2.5-10）增加之濃度尤為顯著，且PM2.5-10/PM10比例（48.6%）均明顯地較ADS來襲前（33.8%）及ADS離開後（38.9%）之值高。於ADS來襲時其粗細微粒上水溶性離子之濃度與Non-ADS時之比值均以Ca2+（黃沙之代表性離子）最高，SO42-次之，NO3-再次之。當ADS來襲時，其粗細微粒上金屬元素之濃度均明顯地增加，其中以具地殼元素特性之Al、Si、Ca、Ti、Mn及Fe等六種金屬元素增加之濃度較多。

In this study, the atmospheric coarse (PM2.5-10) and fine (PM2.5) particulates around Pingtung area were collected using a Dichot sampler and a UAS sampler, respectively, from March 2005 to March 2006. These particles were analyzed by the instruments of IC (Dionex DX-120), TOC (TOC-500A), ICP-MS, ICP-AES, and GC/MS to determine the water-soluble ionic species, carbon contents, metal contents, and PAHs contents in the particles, respectively. The results show that the mean concentrations of PM2.5, PM2.5-10, and PM10 were 57.2 ± 27.9, 19.3 ± 10.5, and 76.4 ± 36.8 μg/m3, respectively, indicating that the atmospheric particulates (PM10) in Pingtung area were mainly contributed by the fine particles (75.9%). The seasonal concentrations of PM2.5, PM2.5-10, and PM10 all followed the order of winter > fall > spring > summer. Water-soluble ions were found to be the major species in PM2.5 and PM2.5-10, with the ratios of 45.8 and 36.9%, respectively. The major components of these sized particulates (particularly in the PM2.5) were water-soluble ionic species (~68–91%) that were mainly contributed by secondary aerosols such as NO3-, SO42-, and NH4+.
Enrich Factor (EF) analysis was used to explore the sources of particle-bound ions and the results show that Cl- and Mg2+ were chiefly from ocean sprays; further, SO42-, K+, and Ca2+ were probably from artificial activity and crustal element, respectively. The TC, EC, and OC contents were higher in PM2.5 than in PM2.5-10, indicating that most of the carbon in PM was contributed by the fine particles (PM2.5). The metals in PM2.5 and PM2.5-10 were mainly contributed by Na, Mg, Al, Si, S, K, Ca, Fe, and Zn. The Na, Mg, Al, Si, Ca, Fe, and Zn in PM were mainly retained by the PM2.5-10 whereas the S, Cr, Ni, Zn, and Pb in PM were chiefly retained by the PM2.5.
Water-soluble ions were the main components in PM2.5 and PM2.5-10, and PM10 (45.8, 36.9, and 43.7%, respectively). While carbon species were the second (30.0, 26.0, and 29.1%, respectively) and metallic elements were the least. The other undetermined components were 14.0, 19.8, and 15.3%, respectively. Particulate PAHs were distributed mainly in PM2.5 and had highest mean concentration in wintertime. The analyzed 21 PAHs were mainly HMW-PAHs (about 48~66%). The average toxic equivalency of LMW-, MMW-, HMW-, and Total-PAHs in PM2.5 all were 4 times of those in PM2.5-10. Since fine particles can reach deep part of human lung, the health impact and risk of particulate PAHs have to be paid attention.
Though the concentrations of fine and coarse particles increased during the Asia Dust Storm (ADS) period, the increase of PM2.5-10 was more significant. The ratio of PM2.5-10 to PM10 was 48.6% in ADS, much higher than that before ADS (33.8%) and after ADS (38.9%). The concentration ratio of Ca2+ (the representative ion of yellow sand) of ADS to non-ADS was found highest among all the water-soluble ions, while SO42- was the second and NO3- were the third. During ADS, the amount of metallic elements in both coarse and fine particles increased significantly, among which the concentrations of crustal elements such as Al, Si, Ca, Ti, Mn, and Fe increased comparatively more than others.

摘要 I
Abstract III
誌謝 V
目錄 VI
表目錄 XI
圖目錄 XIV
第1章 前言 1
1.1 研究緣起 1
1.2 研究目的 1
1.3 研究目標 3
第2章 文獻回顧 4
2.1 懸浮微粒特性 4
2.1.1 氣膠定義 4
2.1.2 懸浮微粒形成機制及來源 4
2.1.3 影響懸浮微粒濃度之因子 8
2.1.4 懸浮微粒上組成成分特性 9
2.2 懸浮微粒之物理特性 11
2.2.1 懸浮微粒之粒徑分佈範圍 11
2.2.2 不同粒徑懸浮微粒之研究 13
2.3 懸浮微粒之化學特性 14
2.3.1 微粒上水溶性離子成分 14
2.3.1.1 微粒上水溶性離子來源及特性 14
2.3.1.2 硫酸鹽與硝酸鹽轉化現象 17
2.3.2 微粒上碳成分 18
2.3.2.1 微粒上碳成份來源及特性 18
2.3.2.2 二次有機碳推估(OCsec) 21
2.3.3 微粒上金屬成分 22
2.3.3.1 微粒上金屬來源及特性 22
2.3.4 微粒上PAHs成分 25
2.3.4.1 微粒上PAHs之來源及特性 25
2.4 汙染源推估模式 30
2.4.1 加強因子分析法： 30
2.4.2 汙染模式之應用 30
2.5 懸浮微粒之影響 31
2.5.1 懸浮微粒對人體健康之影響 31
2.5.2 懸浮微粒對環境影響 33
第3章 研究方法 34
3.1 大氣微粒採樣規劃 34
3.1.1 採樣點之環境描述 34
3.1.2 採樣時間與頻率 37
3.1.3 採樣設備 37
3.2 懸浮微粒成分分析 43
3.3 品保與品管 48
3.3.1 採樣方法之品保與品管 48
3.3.2 分析方法之品保與品管 50
第4章 結果與討論 54
4.1 大氣微粒質量濃度 54
4.1.1 PM10實測值與監測站監測值之比較 54
4.1.2 大氣微粒濃度之時間變化 54
4.1.3 大氣微粒之季節變化 58
4.1.4 懸浮微粒日夜濃度之變化 61
4.2 大氣微粒上水溶性離子成分 65
4.2.1 不同季節微粒上水溶性離子之濃度及含量 65
4.2.2 不同季節微粒上衍生性氣膠及水溶性離子之關係 76
4.2.3 微粒上水溶性離子日、夜濃度及百分比之變化 77
4.2.4 加強因子分析法 81
4.2.5 各季之SOR及NOR值 83
4.3 大氣微粒上碳成分 85
4.3.1 各季微粒上碳成分之濃度及比例 85
4.3.2 各季微粒上二次有機碳(OCsec)濃度之推估 88
4.3.3 微粒上碳成分日夜及百分比之變化 92
4.4 大氣懸浮微粒上金屬成分 94
4.4.1 大氣懸浮微粒上金屬元素之濃度 94
4.4.2 不同粒徑微粒上日夜間之金屬濃度及含量 104
4.5 不同季節微粒上各成分之比例 107
4.6 大氣微粒上PAHs成分 109
4.6.1 大氣微粒上PAHs之濃度 109
4.6.2 大氣微粒上PAHs季節之變化 111
4.6.3 大氣微粒上PAHs之含量 113
4.6.4 大氣微粒上PAHs之毒性當量 115
4.7 亞洲沙塵暴襲台期間大氣微粒之變化 117
4.7.1 ADS來襲期間大氣微粒濃度之變化 117
4.7.2 ADS來襲期間大氣微粒上水溶性離子之變化 118
4.7.3 沙塵暴期間大氣微粒上碳成分之變化 119
4.7.4 ADS來襲期間大氣微粒上金屬元素之變化 123
第5章 結論與建議 127
5.1 結論 127
5.2 建議 128
參考文獻 129
附錄 145
作者簡介 161

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