探討多環芳香烴化合物(PAHs)在雲林地區其氣/固相分佈與逸散平衡之情形

Study on gas/particle partitioning and fugacity of polycyclic aromatic hydrocarbons in Yunlin County

陳俊宇(Jun-Yu Chen)

指導教授 ： 郭崇義

中山醫學大學/健康管理學院/公共衛生學系碩士班/碩士(2016年)

摘要

本研究主旨為探討多環芳香烴化合物(Polycyclic Aromatic Hydrocarbons, PAHs)在大氣中氣/固相分佈及其在大氣與土壤間逸散比值。選擇雲林臨海及內陸地區，收集TSP、PM2.5、氣態及土壤樣品，採樣季節包含夏季、秋季及春季，採樣後之樣品分析利用GC/MS分析29種PAHs。比較兩地區PAHs之濃度差異、季節差異、特徵比值、氣/固相分佈、逸散比值以及終生致癌風險。
研究結果發現，大多數之樣品其PAHs皆是臨海地區高於內陸地區。季節之差異上，TSP及PM2.5中PAHs皆以秋季濃度為最高，依序為春季及夏季，而氣態PAHs之趨勢則為相反，以夏季濃度為最高，依序為春季及秋季。土壤樣品總共採集四次，發現臨海地區土壤中之PAHs皆較內陸地區高。特徵比值判斷發現臨海地區主要以燃燒及工業煙囪排放為主，內陸地區則為汽柴油車及煤炭混和燃燒。PAHs氣/固相之平衡係使用logKP-logPL0及logKP-logKoa兩種模式來探討其在兩地區及季節上之差異，結果發現內陸地區其氣/固相分佈較臨海地區更趨近於平衡，而季節中以春季為較趨近平衡，其餘依序為秋季及夏季。在兩個模式之比較上，發現在本研究之調查地區以logKP-logKoa模式為較佳。由逸散比值判斷發現，臨海地區之逸散比值較內陸地區高，兩地區其PAHs之空氣與土壤逸散途徑皆以氣相沉降而由土壤吸收PAHs為主要途徑。另由大氣中及土壤中PAHs之濃度，評估經由大氣PAHs之吸入與皮膚吸收及土壤所導致之攝入、皮膚吸收與吸入等途徑之致癌風險，發現各種暴露途徑之終生致癌風險皆以臨海地區之風險高於內陸地區。

關鍵字

多環芳香烴化合物 ； 特徵比值 ； 終生致癌風險

並列摘要

This study mainly investigates the PAH (polycyclic aromatic hydrocarbons) gas-particle partitioning coefficient in the atmosphere as well as the fugacity ratios between atmosphere and soil. Environmental samples, including gas phase, total suspension particle (TSP), fine particular matter (PM2.5), and soil were collected from a near-shore industrial zone (NSIZ) and a low pollution area near an inland city (LPIC) in Yunlin County. The sampling process was executed during three seasons: summer, fall, and spring. Twenty-nine PAH compounds were analyzed by gas chromatography and mass spectrometry (GC/MS). The data of concentrations, compositions, diagnostic ratios, incremental lifetime cancer risk, gas-particle partitioning coefficient, and fugacity ratios of the PAHs under different levels at the two sampling sites were analyzed and compared.
The results show that PAH concentrations for most of the samples in the NSIZ are higher than those in the LPIC. For seasonal variations, the PAH concentrations in TSP and PM2.5 were rising in sequence for summer, spring, and fall. Contrarily, the trends of gas phase PAHs were decreasing in sequence for summer, spring, and fall. From soil samples taken during four sampling times, the PAH concentrations in the soil of NSIZ were all higher than those of LPIC. The diagnostic ratios showed that the characteristics tend to be industrial combustion in the NSIZ, while the characteristics tend to be combustion of diesel, gasoline, and coal in the LPIC.
The logKP-logPLo model and logKp-logKoa model were used to explore the equilibrium status between gas-particle partitions of PAHs at the two sites. The equilibrium status in the LPIC was better than that in the NSIZ. The highest slop was obtained for the samples during the spring, which suggests that the samples of this sampling period approach closer to the equilibrium status than those of the other seasons. Moreover, the logKp-logKoa model is more appropriate than the logKP-logPLo model to estimate the equilibrium status of PAHs in the study areas. The results of fugacity ratios indicated that the soil generally acts as a sink at the two sites. Furthermore, fugacity ratios were higher in the NSIZ than those in the LPIC.
The incremental lifetime cancer risk for the PAHs from the median of atmosphere and soil was also estimated. This study also calculated both the exposure pathways of inhalation and dermal adsorption from atmosphere PAHs as well as the exposure pathways of ingestion, dermal adsorption, and inhalation from soil PAHs. The incremental lifetime cancer risk in the NSIZ was higher than that in the LPIC.

並列關鍵字

Polycyclic aromatic hydrocarbons ； Diagnostic ratios ； Incremental lifetime cancer risk

參考文獻

76. 魏千岱(2012)柴油車道與汽油車道其室內外多環芳香烴化合物之探討，中山醫學大學公共衛生學系研究所碩士論文。

1. A. Miguel, T. Kirchstetter, R. Harley, S. Hering. (1998) On-road emissions of particulate polycyclic aromatic hydrocarbons and black carbon from gasoline and diesel vehicles. Environmental Science & Technology, 32, 450–455.

2. Budzinski, H., Jones, I., Bellocq, J., Pie´rrad, C., Garrigues, P. (1997) Evaluation of sediment contamination by polycyclic aromatic hydrocarbons in the Gironde estuary. Marine Chemistry, 58, 85–97.

3. Bidleman, T.F., Billings, W.N., Foreman, W.T. (1986) Vapor-particle Partitioning of semi-volatile organic compounds: Estimates from Field collections. Environmental Science and Technology, 20, 1038-1043.

4. Bjφrseth, A. (1983) Handbook of Polycyclic Aromatic Hydrocarbons. Volume 2 Emission Sources and Recent Progress in Analytical Chemistry. Marcel Dekker, New York.