本研究於高雄地區(楠梓站及小港空品測站)量測四季大氣中醛酮類化合物(Carbonyls)之濃度特徵，並探討醛酮類化合物濃度四季變化及日變化，最後利用因子分析及絕對主成份分析推估高雄地區境內之可能污染來源及其貢獻量。

楠梓及小港站四季之總Carbonyls濃度分布以夏季明顯高於冬季。兩站四季均以甲醛濃度最高，其次為乙醛。推測夏季光化學反應強烈，導致Carbonyls濃度為最高，而冬季光化反應較弱，造成濃度較低。

日變化方面，楠梓及小港站四時段濃度最高均為甲醛，其次為乙醛，總Carbonyls及甲、乙醛濃度均為上、中午時段出現高值，下午時段濃度較低，至夜間時段濃度則略為提高，推測發生此一差距主要為移動污染源及光化學反應造成。

根據C1-C3比值，顯示高雄地區污染型態屬都市型態，以人為污染為主，季節之C1/C2以夏季最高，冬季最低。時段之C1/C2以中午最高，夜間最低，且夏季中午明顯高於其他時段，造成C1/C2差異主要為光化學反應影響，尤其夏季中午，造成C1大量增加。

本研究繼以受體模式解析高雄地區(楠梓與小港站)造成大氣Carbonyls可能之污染族群及貢獻量，結果顯示楠梓站以移動源(柴油車)及固定源(石化與食品工業)對大氣中醛酮類化合物貢獻百分比為55.9 ±1 7.7 %最高，移動源(汽油車)排放貢獻百分比為28.0 ± 8.8 % 與餐飲源排放貢獻百分比為17.2 ± 5.4 % 次之。小港站以移動源(汽油車)排放對大氣中醛酮類化合物貢獻百分比為32.4 ± 10.2 %最高，其次為固定源(鋼鐵工業)及其他污染排放貢獻百分比為28.2 ± 8.9 %，移動源(柴油車)及固定源(石化工業)排放貢獻百分比為24.4 ± 7.7 %，餐飲源排放貢獻百分比為18.9 ± 6.0 %。

The seasonal and diurnal concentrations of atmospheric carbonyls were measured by the LpDNPH-Cartridge and the microcomputer air sampling device at Nan-Chie and Hsiung-Kong sites in Kaohsiung area. Then, factor analysis and absolute principal component analysis were also used to determine the source apportionment in Kaohsiung area.

Total concentrations of carbonyls were higher in Summer than in winter at Nan-Chie and Hsiung-Kong sites. Measurements showed that the highest carbonyls were formaldehyde and acetaldehyde, due to the fact that photochemical activities are stronger in summer than in winter.

The concentrations of total carbonyls, formaldehyde, acetaldehyde were showed similar diurnal variations, that highest concentrations were found in the morning and noon, then drop down at afternoon and increased at night. Due to the fact that photochemical activities and vehicle exhausts.

C1-C3 ratio indicated the local participation of anthropogenic hydrocarbons was important in the production of carbonyls in the Kaohsiung area. C1/C2 was highest in the summer than in the winter, that photochemical activities cause highest concentrations of formaldehyde, especially in the summer noon.

The results of factor analysis and absolute principal component analysis showed that the primary pollution sources at Nan-Chie were traffic exhausts (diesel and gasoline vehicle) and stationary sources (petrochemical and food industry) and restaurant emissions, and the primary pollution sources at Hsiung-Kong were traffic exhausts (diesel and gasoline vehicle), stationary emissions (metal assembly and petrochemical industry) and restaurant emissions.

謝誌 i
摘要 ii
Abstract iv
目錄 v
圖次 vii
表次 viii
附圖目錄 x

第一章 前言 1
1.1 研究緣起 1
1.2 研究目標 2

第二章 相關研究及文獻回顧…3
2.1 高雄地區近年空氣及氣象背景資料概述…3
2.1.1 空氣品質PSI變化趨勢…3
2.1.2 各空氣污染物濃度變化趨勢…5
2.1.3 高雄地區空氣污染物排放量概估…11
2.1.4高雄地區氣象概述…23
2.2 醛酮類化合物…26
2.2.1 醛酮類化合物之物化特性…26
2.2.2大氣中醛酮類化合物來源及排放特徵…28
2.2.3醛酮類化合物在大氣環境中之形成機制…34
2.2.4醛酮類化合物在大氣環境中之轉化…37
2.2.5醛酮類化合物及其前驅物致臭氧生成特性…39
2.2.6醛酮類化合物之健康危害及毒性特徵…40
2.2.7醛酮類化合物之濃度分布…45
2.3 空氣品質相關受體模式…46
2.3.1 化學質量平衡法 (CMB)…46
2.3.2 因子分析 (FA)/絕對主成分分析 (APCA)…47
第三章 研究方法與步驟…50
3.1 研究架構與流程…50
3.2醛酮類化合物採樣地點及時程規劃…51
3.2.1 醛酮類化合物採樣地點…51
3.2.2 醛酮類化合物採樣時程…53
3.3 採樣方法與設備…54
3.3.1空氣採樣器…54
3.3.2吸附管…54
3.4採樣程序…56
3.5樣品分析…56
3.6分析設備及程序…57
3.7 Carbonyls分析之品質保證與品質控制…58
3.7.1空白試驗…58
3.7.2方法偵測極限…59
3.7.3檢量線之配置…59
3.7.4準確度…60
3.7.5精密度(RSD)…61
3.8 因子分析與絕對主成份分析之理論基礎…65
3.8.1因子分析…65
3.8.2絕對主成分分析…68

第四章 結果與討論…74
4.1採樣時間之氣象資料…74
4.2大氣中醛酮類化合物濃度…76
4.2.1大氣中醛酮類化合物之特性…76
4.2.2大氣中醛酮類化合物季節變化…84
4.2.3大氣中醛酮類化合物日變化…90
4.3大氣中醛酮類化合物 (C1−C3)相關性解析 ... 97
4.4 高雄地區大氣中醛酮類化合物污染來源分析 ... 102
4.4.1 大氣中醛酮類化合物指紋建立 ... 102
4.4.2 醛酮類化合物夏季污染來源分析 ... 108
4.4.3 醛酮類化合物冬季污染來源分析 ... 115
4.4.4 楠梓站與小港站醛酮類平均濃度因子分析結果 ... 121
第五章 結論與建議 ... 128
5.1 結論 ... 128
5.2 建議 ... 130
參考文獻 ... 131
附錄A 空氣中氣態之醛類化合物檢驗方法 ... 142
附錄B 高雄地區(楠梓站及小港站)四季採樣時程之各時段風花圖 ... 152
附錄C 個人簡歷 ... 169

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