鄰近北高雄人口密集地區之石化及石油煉製業工廠，主要位於中油公司高雄煉油廠、仁武工業區及大社工業區。近年來，雖有不少學者曾於上述區域進行相關研究，但仍受限於缺少相關資料(如：異味物質鑑定及VOCs指紋資料庫)加以佐證，致無法明確判斷導致空氣污染之具體原因。藉由空氣污染物採樣規劃及完整分析，將可瞭解北高雄地區石化工業區之主要污染源種類及其貢獻率，俾提供環保相關單位擬定環境空氣品質管理及管制對策之參考。
本研究針對中油公司高雄煉油廠、仁武工業區及大社工業區之主要石化產區及鄰近區域，執行工業區周界揮發性有機物及含硫異味物質採樣，與製程排放管道進行同步採樣，乾、濕兩季期間採樣時間規劃於2011年1月7日、14日、19日(乾季)與2011年5月6日、13日、23日(濕季)進行採樣，建置製程管道排放污染源排放資料庫，瞭解VOCs指紋特徵，並推估各排放管道之排放係數，期能藉以瞭解此區域內空氣污染物時空分佈特性及主要污染源種類及貢獻率。
中油公司高雄煉油廠製程排放管道檢測出之VOCs物種均以甲苯及丙酮為主，顯示石油煉製製程具有相似之指紋特徵；而仁武及大社工業區之排放管道，其主要污染物物種則隨著不同製程而有明顯差異。含硫異味物質方面，各工業區皆以硫化氫為主，而仁武工業區製程排放管道含有物種較多且濃度較高的含硫異味物質。
由石化廠區周界之VOCs檢測結果顯示，以異丁烷、正丁烷、異戊烷、正戊烷、丙烷等烷類化合物，丙烯等烯類化合物，甲苯、乙苯、二甲苯、苯乙烯等苯環類化合物，2-丁酮、丙酮等醛酮類化合物為主要VOCs物種。另外，乙烯+乙炔+乙烷(C2)、1,2-二氯乙烷、氯甲烷、二氯甲烷、甲基三級丁基醚(MTBE)等其他類化合物，亦為偶而發現的污染物。含硫異味物質檢測結果顯示，主要異味污染物包括硫化氫、甲硫醇、一甲基硫、二硫化碳等，並以硫化氫的濃度較高，其可檢測出的硫化氫濃度最高可達5.5 ppbv。
本研究將工業區污染物種類分為烷類、烯類、苯環類、醛酮類與其他類等，探討各類污染物之時空分佈特性，主要隨近地面之盛行風向所推送，往污染源下風處擴散傳送，以烷類、苯環類、醛酮類之污染物傳輸最為明顯，不過普遍在風速不高的情形下，各類污染物的顯著影響範圍仍以鄰近石化廠區周界附近為主要影響區域，顯示製程管道排放污染源與逸散污染源對鄰近區域空品優劣具有重要貢獻。另就總含硫異味物質與硫化氫之時空分佈特性而言，其仍以鄰近石化廠區周界附近的濃度較高，顯示相關污染物應以來自石化製程本身的貢獻為主。
由主成份分析結果顯示，石化工業區周界不論乾季或濕季，主要受製程管道排放及逸散性污染源之影響，交通污染源居次；受體模式模擬結果顯示，乾濕季平均之中油公司高雄煉油廠的製程管道排放來源貢獻率約為48 %，逸散性污染源約為30 %，移動污染排放源約為11 %；仁武工業區的製程管道排放來源貢獻率約為75 %，逸散性污染源約為17 %，移動污染排放源約為5 %；大社工業區的製程管道排放來源貢獻率約為68 %，逸散性污染源約為21 %，移動污染排放源約為2 %。

Neighboring northern Kaohsiung with a dense population of petrochemical and petroleum industrial complexes included China Petroleum Company (CPC) refinery plant, Renwu and Dazher petrochemical industrial plants. In recent years, although many scholars have conducted regional studies, but are still limited by the lack of relevant information evidences (such as odorous matters identification and VOCs fingerprint database), while unable to clearly identify the causes of poor ambient air quality. By sampling and analyzing VOCs, we will be able to understand the major sources of VOCs in northern Kaohsiung and their contribution, and to provide the air quality management and control countermeasures for local environmental protection administration.
In this study, we sampled and analyzed the speciation of VOCs and sulfur-containing odorous matters (SOMs) in the CPC refinery plants, Renwu and Dazher petrochemical complexes simultaneously with stack sampling. The sampling of VOCs and SOMs were conducted on January 7th, 14th, and 19th, 2011 (dry season) and May 6th, 13rd, and 23rd, 2011 (wet season). We established the emission source database, investigated the characteristics of VOC fingerprints, and estimate the emission factor of each stack. It helps us understand the temporal and spatial distribution of VOCs and ascertain major sources and their contribution of VOCs.
Major VOCs emitted from the stacks of the CPC refinery plant were toluene and acetone. It showed that petroleum refinery processes had similar VOCs characteristics and fingerprints. The fingerprints of stack emissions at Renwu and Dashe industrial complexes varied with their processes. Hydrogen sulfide was the major sulfur-containing odorous matter in all petrochemical plants. Compared to other petrochemical complexes, Renwu industrial complex emitted a variety of SOMs species as well as relatively high concentrations of sulfur-containing odorous matters.
The petrochemical industrial complexes in the industrial ambient of VOCs analysis results showed that isobutane, butane, isopentane, pentane, propane of alkanes, propene of alkenes, toluene, ethylbenzene, xylene, styrene of aromatics, 2-Butanone (MEK), acetone, of carbonyls are major species of VOCs. In addition, ethene+acetylene+ethane (C2), 1,2-dichloroethane, chloromethane, dichloromethane, MTBE were also occasionally found. Sulfur-containing odorous matter (SOMs) analytical results showed that major odorous matters included hydrogen sulfide, methanethiol, dimethyl sulfide, and carbon disulfide. The highest hydrogen sulfide concentration went up to 5.5 ppbv.
In this study, the species of VOCs were divided into alkanes, alkenes, aromatics, carbonyls, and others. The temporal and spatial distribution of various types of VOCs strongly correlated with near-surface wind direction. The most obvious contaminants were alkanes, aromatics, and carbonyls of the dispersion to the downwind. Generally, the ambient air surrounding the petrochemical industrial complexes was influenced by various pollutants in the case of high wind speeds. It showed that stack emission and fugitive sources had an important contribution to ambient air quality. TSOMs and hydrogen sulfide emitting mainly from local sources resulted in high concentration of TSOMs and hydrogen sulfide surrounding the petrochemical industrial complex.
Principal component analysis (PCA) results showed that the surrounding areas of petrochemical industrial complexes, regardless of dry or wet seasons, were mainly influenced by the process emissions and solvent evaporation. The impact of traffic emission sources ranked the second. Chemical mass balance receptor modeling showed that stack emissions from the CPC refinery plants contributed about 48 %, while fugitive emission sources and mobile sources contributed about 30 % and 11%, respectively. The stack emissions from Renwu industrial complex contributed about 75 %, while fugitive emission sources and mobile sources contributed about 17 % and 5 %, respectively. The stack emissions from Dazher industrial complex contributed about 68 %, while fugitive emission sources and mobile sources contributed about 21 % and 2 %, respectively.

論文審定書................................................................................................ I
謝誌............................................................................................................ II
中文摘要.................................................................................................... III
英文摘要.................................................................................................... V
目錄............................................................................................................ VII
表目錄........................................................................................................ X
圖目錄........................................................................................................ XIII
第一章 前言............................................................................................ 1
1-1 研究緣起..................................................................................... 1
1-2 研究目的..................................................................................... 2
1-3 研究範圍及架構......................................................................... 2
第二章 文獻回顧.................................................................................... 4
2-1 揮發性有機物與含硫異味物質之特性..................................... 4
2-1-1 揮發性有機物與含硫異味物質之定義............................ 4
2-1-2 揮發性有機物之來源........................................................ 6
2-1-3 含硫異味物質之來源........................................................ 12
2-1-4 揮發性有機物與含硫異味物質對人體健康之影響........ 17
2-2 石化工業區排放空氣污染物種類............................................. 21
2-2-1 石化工業區排放揮發性有機物種類................................ 21
2-2-2 石化工業區排放含硫異味物質種類................................ 27
2-3 揮發性有機物與含硫異味物質之管制..................................... 28
2-3-1 固定污染源設置與操作許可證管理辦法........................ 28
2-3-2 固定污染源空氣污染物排放標準.................................... 28
2-3-3 固定污染源空氣污染物連續自動監測設施管理辦法.... 29
2-3-4 揮發性有機物空氣污染管制及排放標準........................ 30
2-3-5 異味污染物為空氣污染物................................................ 30
2-4 高雄地區氣象及空氣品質現況................................................. 30
2-4-1 高雄地區氣象條件現況.................................................... 30
2-4-2 高雄地區空氣品質現況.................................................... 32
2-5 污染源解析模式之應用............................................................. 35
2-5-1 主成份分析法(Principal Component Analysis)................ 35
2-5-2 化學質量平衡受體模式(CMB Receptor Model )............ 36
第三章 研究方法.................................................................................... 40
3-1 石化工業區氣象監測資料分析................................................. 40
3-2 揮發性有機物與含硫異味物質採樣規劃................................. 41
3-2-1 製程排放管道採樣規劃.................................................... 41
3-2-2 周界採樣規劃.................................................................... 43
3-3 製程排放管道與周界採樣方法與設備..................................... 45
3-3-1 製程排放管道採樣方法與設備........................................ 45
3-3-2 周界採樣方法與設備........................................................ 45
3-4 污染物分析原理、方法與設備................................................. 46
3-4-1 揮發性有機物分析............................................................ 46
3-4-2 含硫異味物質分析............................................................ 54
3-5 指紋資料庫之建置與排放係數推估......................................... 56
3-6 品保與品管(QA/QC) ................................................................. 57
3-6-1 Tedlar採樣袋空白測試..................................................... 57
3-6-2 揮發性有機物分析之品保與品管.................................... 58
3-6-3 含硫異味物質分析之品保與品管.................................... 60
3-7 污染物擴散及化學質量平衡受體模式解析............................. 61
3-7-1 污染物濃度時空分佈........................................................ 61
3-7-2 主成份分析法.................................................................... 61
3-7-3 化學質量平衡受體模式.................................................... 63
第四章 結果與討論................................................................................. 65
4-1 採樣期間北高雄地區氣象條件分析......................................... 65
4-1-1 乾季採樣期間.................................................................... 65
4-1-2 濕季採樣期間.................................................................... 66
4-2 石化工業區製程排放管道污染物種類及濃度分析結果探討. 79
4-2-1 中油公司高雄煉油廠........................................................ 79
4-2-2 仁武工業區........................................................................ 82
4-2-3 大社工業區........................................................................ 86
4-3 乾季石化工業區周界污染物濃度分析結果探討..................... 90
4-3-1 石化工業區VOCs與SOMs分佈趨勢............................. 90
4-3-2 中油公司高雄煉油廠周界分佈趨勢................................ 95
4-3-3 仁武工業區周界分佈趨勢................................................ 100
4-3-4 大社工業區周界分佈趨勢................................................ 105
4-4 濕季石化工業區周界污染物濃度分析結果探討..................... 110
4-4-1 石化工業區VOCs與SOMs分佈趨勢............................. 110
4-4-2 中油公司高雄煉油廠周界分佈趨勢................................ 115
4-4-3 仁武工業區周界分佈趨勢................................................ 120
4-4-4 大社工業區周界分佈趨勢................................................ 125
4-5 石化工業區污染源解析............................................................. 130
4-5-1 主成份分析法判別主要污染源種類................................ 130
4-5-2 化學質量平衡法解析污染源貢獻率................................ 138
第五章 結論與建議................................................................................ 154
5-1 結論............................................................................................. 154
5-2 建議............................................................................................. 156
參考文獻.................................................................................................... 157
附錄A 揮發性有機物分析之品保品管............................................... 167
附錄B 含硫異味物質分析之品保品管............................................... 172

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