臺灣博碩士論文加值系統

近年來，大陸地區經濟及工業快速發展，石化燃料消耗量及人為污染物的排放量均大幅增加，導致環境污染問題日益嚴重。馬祖地區緊鄰閩江口，與大陸福州僅一水之隔，島上並無大型經濟開發及人為污染，現今仍保有純淨的生態環境，然而其空氣品質卻不若台灣本島鄉村地區佳，甚至較部分都市空氣品質污染更為嚴重。基於此區域之獨特地理環境，本研究乃將閩江口週邊之馬祖地區及福州地區視為相同空品區，並針對該空品區之懸浮微粒污染來源加以探討。
本研究於2012年7月至2013年5月期間在閩江口海域(馬祖)及陸域(福州)地區設置6處採樣點，分別於不同季節進行PM10懸浮微粒採樣，並針對所採集之懸浮微粒進行化學成份分析，藉以瞭解閩江口海域及陸域之大氣懸浮微粒特性。此外，為釐清該區域之污染來源種類及貢獻率，本研究亦利用主成份分析、化學質量平衡受體模式配合逆軌跡模擬等不同方法，進行懸浮微粒污染來源種類及貢獻量之解析，並探討不同季節之差異性。
由PM10濃度季節變化得知，除夏季期間閩江口海陸域之PM10濃度較其他季節為低，而秋、冬、春等東北季風吹襲期間，PM10濃度亦普遍較高。就PM10濃度空間分佈而言，則主要呈現西邊(陸域)較高且東邊(海域)較低的情形，其中梅花中學於不同季節之PM10濃度均普遍高於其他測站，然而此濃度高低分佈情形與季風風向遞減效應並不一致，顯示閩江口海陸域除受到長程傳輸影響外，亦與福州地區背景濃度及大氣擴散條件有密切關係。
由化學成份分析結果顯示，各季節水溶性離子均以二次無機性氣膠(SIA)為主，約佔水溶性離子成份70%左右，其中又以SO42-及NO3-居多，導致閩江口海陸域懸浮微粒中和比值(NR)均小於1。此結果顯示境外傳輸將上風區酸性污染物吹送至閩江口，使得懸浮微粒呈現偏酸性。金屬元素則以Al、Ca、Fe、K、Mg為主要物種，而其他微量金屬元素(如：Cd、As、Ni及Cr)濃度在東北季風盛行期間均呈上升趨勢。不論在何種季節碳成份均以有機碳(OC)為主，OC/EC值普遍高於2.2，且金屬元素成份及碳成份濃度均呈現陸域高於海域之情形。
就懸浮微粒污染源種類及貢獻量而言，閩江口海陸域主要以逸散性揚塵、二次衍生性氣膠、交通污染源、海鹽飛沫、農廢燃燒為主；而秋季過後及空氣品質劣化期間，傳輸路徑以北方傳輸型及高壓迴流型為主，污染源種類較多且貢獻率較高，其中工業污染源貢獻量約成長8倍左右，與夏季背景貢獻量差異甚大，顯示受到境外長程傳輸污染物移入之影響嚴重。

In recent years, due to rapid economic and industrial development of mainland China, significant increases in fossil fuel consumption and anthropogenic emissions of air pollutants cause increasing environmental pollution problems. Matsu Islands located at the Minjiang Estuary faces Fuzhou in mainland. The islands have no large-scale industries and pollution sources, which conserve the islands as an ecological environment. However, the ambient air quality is worse than the rural areas of Taiwan, and even more serious than urban air quality. Due to the unique meteorological and geographical environment, Matsu and Fuzhou areas surrounding the Minjiang Estuary are treated at the same air quality zone for investigating their sources of suspended particles.
In this study, six sites were selected to collect PM10 samples from July 2012 to April 2013, respectively located at offshore (Matsu) and inland (Fuzhou) region for different seasons. The chemical composition of PM10 was then analyzed to characterize the PM10 sampled at inland and offshore regions. Additionally, in order to clarify the region''s pollution sources and their contributions, this study applied principal component analysis (PCA), chemical mass balance (CMB) receptor model, and backward trajectory simulation methods to understand the source apportionment of suspended particles, and to explore their variation for different seasons.
The results showed lower average PM10 concentration in summer, and higher concentration in the northeast monsoon period. From the perspective of spatial distribution, PM10 concentration increased from the west to the east. The PM10 concentrations observed at MH site were generally higher than other sites for all seasons. However, the spatial distribution of PM10 was inconsistent with the seasonal prevailing wind direction, showing that ambient PM10 at Minjiang Estuary was not only influenced by long-range transportation, but also by local emissions from Fuzhou.
Chemical composition analysis showed that most abundant water-soluble ionic species of PM10 were secondary inorganic aerosols (SO42-, NO3-, and NH4+) which accounted for 70% of total ions, resulting in NR of suspended particles less than unity at Minjiang Estuary. These results indicated that the upwind acidic pollutants transferred to the Minjiang Estuary, making rendered acidic aerosols. For all seasons, the major metallic elements of suspended particles were Al, Ca, Fe, K, Mg, other trace metals (eg: Cd, As, Ni and Cr) concentration increased during the northeast monsoon period. Organic carbons (OC) was the main species of carbon for all seasons, thus OC/EC ratio was generally higher than 2.2. The spatial distribution showed that metallic elements and carbon components had relatively higher concentrations at inland than those at offshore.
Results from PCA and CMB receptor model showed that major sources of ambient PM10 at Minjiang Estuary were soil dusts, secondary inorganic aerosols, transportation emissions, sea salts, and biomass burning. During the northeast monsoon and poor air quality periods, the contribution of industrial pollution grew eight times, and cross-boundary transportation accounted for 55~77% of total PM concentrations, showing that ambient air quality was significantly affected by cross-boundary transport at Minjiang Estuary.

中文摘要 I
英文摘要 III
目錄 V
表目錄 VIII
圖目錄 X
第一章 前言 1-1
1-1 研究緣起 1-1
1-2 研究目的 1-2
1-3 研究範圍與架構 1-2
第二章 文獻回顧 2-1
2-1 馬祖地區環境概況 2-1
2-1-1 地理位置及人口 2-1
2-1-2 氣候概況 2-2
2-1-3 馬祖地區空氣品質概況 2-4
2-2 懸浮微粒物化特性 2-6
2-3 懸浮微粒化學成份 2-8
2-3-1 水溶性離子成份 2-8
2-3-2 金屬元素成份 2-13
2-3-3 碳成份 2-15
2-4 海域氣膠特性 2-17
2-5 逆軌跡模式之應用 2-20
2-6 富集因子分析 2-22
2-7 主成份分析 2-23
2-8 CMB模式推估懸浮微粒來源 2-25
第三章 研究方法 3-1
3-1 懸浮微粒採樣規劃 3-1
3-1-1 採樣地點 3-1
3-1-2 採樣時間 3-2
3-2 懸浮微粒採樣方法與原理 3-2
3-3 懸浮微粒質量濃度與化學成份分析方法 3-3
3-3-1 質量濃度量測方法 3-4
3-3-2 水溶性離子成份分析方法 3-4
3-3-3 金屬元素成份分析方法 3-5
3-3-4 碳成份分析方法 3-6
3-4 品保與品管 3-7
3-4-1 採樣方法之品保品管 3-7
3-4-2 分析方法之品保品管 3-8
3-5 大氣懸浮微粒之污染源解析法 3-10
3-5-1 等濃度空間分佈 3-10
3-5-2 逆軌跡模式模擬 3-10
3-5-3 富集因子分析法 3-10
3-5-4 主成份分析法 3-11
3-5-5 化學質量平衡受體模式 3-12
第四章 結果與討論 4-1
4-1 例行性採樣期間馬祖地區氣象條件分析 4-1
4-1-1 風速及風向 4-1
4-1-2 相對溼度 4-3
4-2 懸浮微粒濃度季節變化趨勢分析 4-5
4-3 懸浮微粒化學成份分析 4-12
4-3-1 水溶性離子成份季節變化趨勢分析 4-12
4-3-2 金屬元素成份季節變化趨勢分析 4-25
4-3-3 碳成份季節變化趨勢分析 4-26
4-4 密集採樣期間懸浮微粒物化特性變化趨勢 4-36
4-5 懸浮微粒傳輸路徑分析 4-52
4-6 富集因子分析法 4-59
4-7 主成份分析 4-61
4-8 化學質量平衡受體模式解析 4-70
第五章 結論與建議 5-1
5-1 結論 5-1
5-2 建議 5-3
參考文獻…………………………………………………………………R-1
附錄A 分析儀器之品保品管…………………………………..……A-1
附錄B 分析儀器之檢量線……………………………..……………B-1
 
表目錄
頁次
表 2.1馬祖地區人口統計表 2-2
表 2.2馬祖地區現有車輛、船舶及航空運輸數量統計 2-2
表 2.3馬祖地區氣候資料彙整表 2-3
表 2.4連江縣歷年空氣品質彙整表 2-4
表 2.5大氣懸浮微粒粒徑分佈 2-7
表 2.6各污染源排放懸浮微粒主要成份一覽表 2-26
表 2.7 PM10及PM2.5污染源貢獻量分析 2-29
表 3.1採樣位置一覽表 3-2
表 3.2元素分析儀操作參數一覽表 3-7
表 4.1例行性採樣期間盛行風向一覽表 4-1
表 4.2例行性採樣期間相對濕度彙整表 4-4
表 4.3採樣期間海陸域懸浮微粒濃度之季節變化一覽表 4-5
表 4.4夏季採樣期間海陸域及各採樣點之水溶性離子濃度彙整表 ..4-13
表 4.5秋季採樣期間海陸域及各採樣點之水溶性離子濃度彙整表 ..4-14
表 4.6冬季採樣期間海陸域及各採樣點之水溶性離子濃度彙整表 ..4-15
表 4.7春季採樣期間海陸域及各採樣點之水溶性離子濃度彙整表 ..4-16
表 4.8採樣期間海陸域懸浮微粒之氯損失彙整表 4-18
表 4.9不同季節之二次無機性氣膠(SIA)彙整表 4-19
表 4.10採樣期間南竿鄉懸浮微粒硫氧化率及氮氧化率表 4-23
表 4.11夏季採樣期間海陸域金屬元素濃度彙整表 4-27
表 4.12秋季採樣期間海陸域金屬元素濃度彙整表 4-27
表 4.13冬季採樣期間海陸域金屬元素濃度彙整表 4-28
表 4.14春季採樣期間海陸域金屬元素濃度彙整表 4-28
表 4.15閩江口海陸域地殼元素濃度彙整表 4-30
表 4.16採樣期間海陸域碳成份濃度一覽表 4-32
表 4.17水溶性離子、金屬元素及碳成份百分比彙整表 4-34
表 4.18密集採樣期間SIA濃度及所佔離子百分比 4-44
表 4.19密集採樣期間海陸域氯損失及[Cl-]/[Na+]一覽表 4-44
表 4.20密集採樣期間海陸域碳成份濃度彙整表 4-50
表 4.21密集採樣期間懸浮微粒化學成份分佈百分比 4-51
表 4.22採樣期間懸浮微粒傳輸路徑彙整表 4-55
表 4.23夏季採樣期間主成份分析彙整表 4-63
表 4.24秋季採樣期間主成份分析彙整表 4-63
表 4.25冬季採樣期間主成份分析彙整表 4-67
表 4.26春季採樣期間主成份分析彙整表 4-67
表 4.27密集採樣期間主成份因子負荷矩陣表 4-68
表 4.28受體模式解析之指紋資料庫彙整表 4-71
表 4.29閩江口海陸域夏季期間CMB模擬結果 4-72
表 4.30閩江口海陸域秋季期間CMB模擬結果 4-72
表 4.31閩江口海陸域冬季期間CMB模擬結果 4-74
表 4.32閩江口海陸域春季期間CMB模擬結果 4-74
 
圖目錄
頁次
圖 1.1研究架構流程圖 1-4
圖 2.1馬祖列島地理位置圖 2-1
圖 2.2 2011年馬祖地區四季風玫圖 2-4
圖 2.3 2006~2011年馬祖地區PM10濃度逐月變化趨勢圖 2-5
圖 2.4東引測站與台灣本島各測站懸浮微粒濃度時序圖 2-5
圖 2.5懸浮微粒粒徑分佈圖 2-8
圖 2.6水溶性離子中不同無機化合物在不同污染程度之分佈 2-11
圖 2.7北京PM10及PM2.5日平均濃度與地面輻射相關圖 2-11
圖 2.8世界各測站之AMS監測結果 2-12
圖 2.9逆軌跡模式模擬氣團傳輸路徑與其污染源貢獻量分佈 2-22
圖 2.10天津市PM10之污染源種類及貢獻率 2-28
圖 3.1本研究PM10採樣站位置圖 3-1
圖 3.2 PM10高量採樣器 3-3
圖 4.1夏季例行性採樣期間風玫圖 4-2
圖 4.2秋季例行性採樣期間風玫圖 4-2
圖 4.3冬季例行性採樣期間風玫圖 4-2
圖 4.4春季例行性採樣期間風玫圖 4-2
圖 4.5採樣期間風速逐時變化趨勢圖 4-3
圖 4.6採樣期間相對濕度逐時變化趨勢圖 4-4
圖 4.7夏季例行性採樣懸浮微粒濃度分佈圖 4-6
圖 4.8秋季例行性採樣懸浮微粒濃度分佈圖 4-7
圖 4.9冬季例行性採樣懸浮微粒濃度分佈圖 4-8
圖 4.10春季例行性採樣懸浮微粒濃度分佈圖 4-9
圖 4.11本研究採樣結果與環保署監測站PM10濃度測值比較圖 4-9
圖 4.12夏季採樣期間懸浮微粒等濃度分佈圖 4-10
圖 4.13秋季採樣期間懸浮微粒等濃度分佈圖 4-10
圖 4.14冬季採樣期間懸浮微粒等濃度分佈圖 4-11
圖 4.15春季採樣期間懸浮微粒等濃度分佈圖 4-11
圖 4.16例行性採樣期間不同季節水溶性離子濃度分佈圖 4-17
圖 4.17閩江口海陸域懸浮微粒氯損失及濾鈉比值分析圖 4-19
圖 4.18懸浮微粒中[NH4+]及[nss-SO42-]+[NO3-]關係圖 4-21
圖 4.19懸浮微粒中[NH4+]+[Na+]及[nss-SO42-]+[NO3-]關係圖 4-22
圖 4.20例行採樣期間不同季節硫氧化率 4-23
圖 4.21例行採樣期間不同季節氮氧化率 4-24
圖 4.22採樣期間陸域及鄰近海域之[NO3-]/[SO42-]比值 4-24
圖 4.23例行性採樣期間金屬元素濃度分佈圖 4-29
圖 4.24採樣期間海陸域懸浮微粒碳成份季節變化圖 4-30
圖 4.25海陸域懸浮微粒OC與EC相關趨勢及(OC/EC)min圖 4-33
圖 4.26懸浮微粒之水溶性離子、金屬元素及碳成份百分比圖 4-35
圖 4.27第一次密集採樣期間PM10懸浮微粒濃度分佈圖 4-37
圖 4.28第二次密集採樣期間PM10懸浮微粒濃度分佈圖 4-37
圖 4.29第一次密集採樣期間PM10等濃度圖(11月6日) 4-38
圖 4.30第一次密集採樣期間PM10等濃度圖(11月7日) 4-38
圖 4.31第一次密集採樣期間PM10等濃度圖(11月8日) 4-38
圖 4.32第一次密集採樣期間PM10等濃度圖(11月9日) 4-38
圖 4.33第一次密集採樣期間PM10等濃度圖(11月10日) 4-38
圖 4.34第二次密集採樣期間PM10等濃度圖(12月3日) 4-39
圖 4.35第二次密集採樣期間PM10等濃度圖(12月4日) 4-39
圖 4.36第二次密集採樣期間PM10等濃度圖(12月5日) 4-39
圖 4.37第二次密集採樣期間PM10等濃度圖(12月6日) 4-39
圖 4.38第二次密集採樣期間PM10等濃度圖(12月7日) 4-39
圖 4.39密集採樣期間[NO3-]/[SO42-]相關圖 4-42
圖 4.40密集採樣期間[NO3-]/[SO42-]比值分佈圖 4-42
圖 4.41密集採樣期間[NH4+]及[nss-SO42-]+[NO3-]關係圖 4-43
圖 4.42密集採樣期間[NH4+]+[Na+]及[nss-SO42-]+[NO3-]關係圖 4-43
圖 4.43第一次密集性採樣期間水溶性離子濃度分佈圖 4-45
圖 4.44第二次密集性採樣期間水溶性離子濃度分佈圖 4-46
圖 4.45第一次密集性採樣期間金屬元素濃度分佈圖 4-47
圖 4.46第二次密集性採樣期間金屬元素濃度分佈圖 4-48
圖 4.47密集採樣期間碳成份濃度比較圖(上：第一次密集採樣；
下：第二次密集採樣) 4-49
圖 4.48本研究污染氣團傳輸路徑類型彙整圖 4-54
圖 4.49不同傳輸路徑與PM10濃度相關圖 4-56
圖 4.50不同傳輸路徑與海域水溶性離子濃度相關圖 4-57
圖 4.51不同傳輸路徑與陸域水溶性離子濃度相關圖 4-57
圖 4.52不同傳輸路徑與海域金屬元素濃度相關圖 4-58
圖 4.53不同傳輸路徑與陸域金屬元素濃度相關圖 4-58
圖 4.54不同傳輸路徑與海陸域碳成份濃度相關圖 4-58
圖 4.55夏季期間閩江口海陸域以Al為參考元素之富集因子分析
圖 4-59
圖 4.56秋季期間閩江口海陸域以Al為參考元素之富集因子分析
圖 4-60
圖 4.57冬季期間閩江口海陸域以Al為參考元素之富集因子分析
圖 4-60
圖 4.58春季期間閩江口海陸域以Al為參考元素之富集因子分析
圖 4-60
圖 4.59第一次密集性採樣主成份分析因子負荷圖 4-69
圖 4.60第二次密集性採樣主成份分析因子負荷圖 4-69
圖 4.61閩江口海陸域例行性採樣懸浮微粒污染源種類及貢獻率 4-75
圖 4.62閩江口海陸域不同季節污染源貢獻量差異圖 4-76

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