環保專案成果報告查詢系統

專案計畫編號	EPA-104-FA11-03-A261
經費年度	104
計畫經費	5,370 千元
專案開始日期	2015/08/12
專案結束日期	2016/07/31
專案主持人	周崇光
主辦單位	監資處
承辦人	陳香宇
執行單位	中央研究院環境變遷研究中心
專案分類	大氣空氣、環境監測及檢測
中文關鍵字	細懸浮微粒、同位素、污染來源鑑識、遠程傳輸污染物
英文關鍵字	PM2.5, Isotope, Source Identification, Long-range Transported pollutants
協同主持人	李崇德；林傳堯；沈川洲
共同主持人
計畫聯絡人	黃譯樘
計畫聯絡電話	02-26539885#265
計畫聯絡信箱	yitang@rcec.sinica.edu.tw

中文摘要	本計畫主要蒐集懸浮微粒同位素分析方法的相關文獻，除以此為依據建立懸浮微粒同位素之分析方法外，並藉由分析大氣與污染源微粒樣品的同位素特徵，以評估利用同位素特徵鑑識大氣細懸浮微粒(PM2.5)污染來源的可行性。在研究期程內，本計畫完成了PM2.5之碳、鉛與鍶同位素分析方法的建立，並已應用於富貴角、臺大、陽明山、斗六及嘉義測站大氣PM2.5與交通污染源及燃煤電廠排放微粒真實樣品之分析工作。在細懸浮微粒化學組成上，各測站PM2.5以有機碳(15-41%)，非海鹽硫酸鹽(14-29%)，銨鹽(6-13%)、硝酸鹽(2-16%)及元素碳(2-9%)為主要組成。此外，PM2.5之化學組成有明顯的時空變化特徵，夏季高OC含量可能與二次有機氣膠的生成有關，相反地，硝酸鹽的濃度在夏季最低，可能受到夏季溫度高，硝酸銨微粒易揮發的特性有關。在空間分佈特徵上，富貴角測站海鹽成分較高，反應沿海測站之特性，相反地，臺大測站交通污染源排放相關之物種如元素碳及硝酸鹽含量較高，反應都會區氣膠的特性。在同位素分析技術建立方面，利用CRDS分析各標準品之δ13C值與USGS標準值結果相近，其誤差絕對值低於0.3‰，而分析之精度在0.2‰之內，顯示利用CRDS分析顆粒中碳同位素的方法具可行性；利用Sr-Spec樹脂純化技術搭配MC-ICP-MS分析SRM981及SRM987之鉛與鍶同位素比值則顯示有極佳的準確性(>99.9%)與精確性(2<0.03%)。在PM2.5同位素特徵方面，北部富貴角及臺大測站PM2.5總碳之δ13C值具有明顯的季節性變化，夏季西南季風盛行，PM2.5主要來自於本土污染源的貢獻，其δ13C值平均約為-26.7及-27‰，相反地在東北季風盛行的春季，其δ13C平均值可分別提高至-24.5及-25.5‰，與中國大陸北京、天津及上海的測值相近，顯示遠程傳輸的影響，而中南部斗六及嘉義測站在秋、冬季觀測期間，其PM2.5的δ13C值分別為-28.9及-28.4‰，顯示主要來自本土污染源的貢獻。在鉛同位素方面，可利用208Pb/207Pb的同位素比值特徵進行PM2.5鉛元素之污染來源鑑識，富貴角測站夏、冬與春季細懸浮微粒之208Pb/207Pb比值平均分別為2.4227、2.4452及2.4408，臺大測站夏、冬與春季細懸浮微粒之208Pb/207Pb 則分別為2.4312、2.4469及2.4381，夏季鉛同位素比值較輕，而冬、春兩季較重的鉛同位素比值與中國大陸華北地區之結果相似，顯示長程傳輸污染物的影響，而中南部斗六及嘉義測站208Pb/207Pb比值分別為2.4286及2.4291，顯示本土污染源的貢獻。在鍶同位素方面，各測站87Sr/86Sr的比值介於0.708628至0.721940，無明顯的季節性與空間性的變化。在污染源排放微粒方面，本土交通污染源所排放的PM2.5總碳δ13C值約為-24.4‰，與燃煤電廠的-25.1‰無明顯的差異。交通源排放微粒的208Pb/207Pb介於 2.4354至2.4412，平均係2.4380；87Sr/86Sr則介於0.711283至0.721937，平均則為0.711460。此外，利用空氣品質模式模擬顯示2016年春季觀測期間富貴角及臺大測站PM2.5明顯受到中國大陸華中及華北地區遠程傳輸之貢獻而影響富貴角及臺大測站PM2.5碳與鉛同位素特徵的分佈。
中文關鍵字	細懸浮微粒、同位素、污染來源鑑識、遠程傳輸污染物

中文摘要

本計畫主要蒐集懸浮微粒同位素分析方法的相關文獻，除以此為依據建立懸浮微粒同位素之分析方法外，並藉由分析大氣與污染源微粒樣品的同位素特徵，以評估利用同位素特徵鑑識大氣細懸浮微粒(PM2.5)污染來源的可行性。在研究期程內，本計畫完成了PM2.5之碳、鉛與鍶同位素分析方法的建立，並已應用於富貴角、臺大、陽明山、斗六及嘉義測站大氣PM2.5與交通污染源及燃煤電廠排放微粒真實樣品之分析工作。在細懸浮微粒化學組成上，各測站PM2.5以有機碳(15-41%)，非海鹽硫酸鹽(14-29%)，銨鹽(6-13%)、硝酸鹽(2-16%)及元素碳(2-9%)為主要組成。此外，PM2.5之化學組成有明顯的時空變化特徵，夏季高OC含量可能與二次有機氣膠的生成有關，相反地，硝酸鹽的濃度在夏季最低，可能受到夏季溫度高，硝酸銨微粒易揮發的特性有關。在空間分佈特徵上，富貴角測站海鹽成分較高，反應沿海測站之特性，相反地，臺大測站交通污染源排放相關之物種如元素碳及硝酸鹽含量較高，反應都會區氣膠的特性。在同位素分析技術建立方面，利用CRDS分析各標準品之δ13C值與USGS標準值結果相近，其誤差絕對值低於0.3‰，而分析之精度在0.2‰之內，顯示利用CRDS分析顆粒中碳同位素的方法具可行性；利用Sr-Spec樹脂純化技術搭配MC-ICP-MS分析SRM981及SRM987之鉛與鍶同位素比值則顯示有極佳的準確性(>99.9%)與精確性(2<0.03%)。在PM2.5同位素特徵方面，北部富貴角及臺大測站PM2.5總碳之δ13C值具有明顯的季節性變化，夏季西南季風盛行，PM2.5主要來自於本土污染源的貢獻，其δ13C值平均約為-26.7及-27‰，相反地在東北季風盛行的春季，其δ13C平均值可分別提高至-24.5及-25.5‰，與中國大陸北京、天津及上海的測值相近，顯示遠程傳輸的影響，而中南部斗六及嘉義測站在秋、冬季觀測期間，其PM2.5的δ13C值分別為-28.9及-28.4‰，顯示主要來自本土污染源的貢獻。在鉛同位素方面，可利用208Pb/207Pb的同位素比值特徵進行PM2.5鉛元素之污染來源鑑識，富貴角測站夏、冬與春季細懸浮微粒之208Pb/207Pb比值平均分別為2.4227、2.4452及2.4408，臺大測站夏、冬與春季細懸浮微粒之208Pb/207Pb 則分別為2.4312、2.4469及2.4381，夏季鉛同位素比值較輕，而冬、春兩季較重的鉛同位素比值與中國大陸華北地區之結果相似，顯示長程傳輸污染物的影響，而中南部斗六及嘉義測站208Pb/207Pb比值分別為2.4286及2.4291，顯示本土污染源的貢獻。在鍶同位素方面，各測站87Sr/86Sr的比值介於0.708628至0.721940，無明顯的季節性與空間性的變化。在污染源排放微粒方面，本土交通污染源所排放的PM2.5總碳δ13C值約為-24.4‰，與燃煤電廠的-25.1‰無明顯的差異。交通源排放微粒的208Pb/207Pb介於 2.4354至2.4412，平均係2.4380；87Sr/86Sr則介於0.711283至0.721937，平均則為0.711460。此外，利用空氣品質模式模擬顯示2016年春季觀測期間富貴角及臺大測站PM2.5明顯受到中國大陸華中及華北地區遠程傳輸之貢獻而影響富貴角及臺大測站PM2.5碳與鉛同位素特徵的分佈。

中文關鍵字

細懸浮微粒、同位素、污染來源鑑識、遠程傳輸污染物

類型	檔名	檔案大小	說明	最新版公開日期
期末報告	EPA-104-FA11-03-A261 定稿.pdf	9MB		2016/11/1 上午 12:00:00

摘要	The objectives of this study are to develope analytical methods for determination of isotopes in fine particulate matters (PM2.5) and to feasibility of identifying potential sources of ambient PM2.5 with the isotopic fingerprints. To achieve the objectives, ambient PM2.5 sampling was carried out at the Cap Fuguei (CAFÉ), Taipei (NTU), Yangminshan, Douliu and Chayi stations. Besides, in order to establish isotope fingerprints of specific sources, vehicle-emitted particles were collected in the Hsuehshan Tunnel and coal materias together with fly ash and bottom ash were collected from coal-fire power plants. These samples were analyzed for water soluble ions, elemental carbon, organic carbon and metallic constituents. In addition, carbon along with lead and stronitium isotopes were also determined by cavity ring-down spectrometry (CRDS) and multi-collector inductively plasma mass spectrometer (MC-ICP-MS), respectively. The results showed that organic carbon, which accounted for 15-41% of PM2.5 mass, was the predominant species, followed by non-sea-salt sulfate (14-29%), ammonium (6-13%), nitrate (2-16%) and elemental carbon(2-9%). The elevated abundance of OC in the summertime was attributed to the formation of secondary organic aerosols, whereas lower nitrate concentrations were due to evaporation under high atmospheric temperature. Elevated level of sea salt particles was observed at CAFÉ station located in the coastal area, whereas EC and nitrate were found enriched in PM2.5 samples collected at downtown stations. Using CRDS and MC-ICP-MS instruments, C, Pb and Sr isotopes in PM2.5 samples were detected with high precision and accuracy. The averaged δ13CTC in PM2.5 at CAFÉ and NTU stations were -26.7 and -27.0‰ during summertime, which were lighter than those in the spring period by 2.5‰. The stable carbon isotope ratio measured in the summertime were representative of the local emissions as Taiwan was isolated from continental air mass. On the contrary, the isotopically heavy carbon aerosols in the springtime were attributed to the influences of PM2.5 from mainland China. This inference was supported by δ13CTC data coupling with WRF/Chem model simulations. The averaged δ13CTC in PM2.5 collected at the Douliu and Chayi stations during autumn/winter season were -28.9 and -28.4‰, respectivevly, suggesting local origins. Similar seasonal patterns were found for 208Pb/207Pb ratio. At CAFÉ and NTU stations, the average values of 208Pb/207Pb ratio in the summertime were 2.4227 and 2.4312, respectively. The ratios increased to 2.4408 and 2.4318 in the spring sampling period, which were very close to those obtained in central and northern China, indicating long-range transport of air pollution by Asian continental outflows. The 208Pb/207Pb ratios at Douliu and Chayi stations in the autumn/winter periods were 2.4286 and 2.4291, respectively, suggesting local sources. For 87Sr/86Sr, the average values at all the stations varied between 0.708628 and 0.721940. Unlike δ13CTC and 208Pb/207Pb, no significant seasonal variation was found in 87Sr/86Sr. In case of vehicle-derived PM2.5, the average δ13CTC was -24.4‰ which was comparable to that (-25.1‰) of coal ash collected from coal-fired power plants. In addition, this study also determined 208Pb/207Pb and 87Sr/86Sr ratios for vehicle-emitted PM2.5 with the average values of 2.4380 and 0.711460, respectively.
英文關鍵字	PM2.5, Isotope, Source Identification, Long-range Transported pollutants

摘要

The objectives of this study are to develope analytical methods for determination of isotopes in fine particulate matters (PM2.5) and to feasibility of identifying potential sources of ambient PM2.5 with the isotopic fingerprints. To achieve the objectives, ambient PM2.5 sampling was carried out at the Cap Fuguei (CAFÉ), Taipei (NTU), Yangminshan, Douliu and Chayi stations. Besides, in order to establish isotope fingerprints of specific sources, vehicle-emitted particles were collected in the Hsuehshan Tunnel and coal materias together with fly ash and bottom ash were collected from coal-fire power plants. These samples were analyzed for water soluble ions, elemental carbon, organic carbon and metallic constituents. In addition, carbon along with lead and stronitium isotopes were also determined by cavity ring-down spectrometry (CRDS) and multi-collector inductively plasma mass spectrometer (MC-ICP-MS), respectively. The results showed that organic carbon, which accounted for 15-41% of PM2.5 mass, was the predominant species, followed by non-sea-salt sulfate (14-29%), ammonium (6-13%), nitrate (2-16%) and elemental carbon(2-9%). The elevated abundance of OC in the summertime was attributed to the formation of secondary organic aerosols, whereas lower nitrate concentrations were due to evaporation under high atmospheric temperature. Elevated level of sea salt particles was observed at CAFÉ station located in the coastal area, whereas EC and nitrate were found enriched in PM2.5 samples collected at downtown stations. Using CRDS and MC-ICP-MS instruments, C, Pb and Sr isotopes in PM2.5 samples were detected with high precision and accuracy. The averaged δ13CTC in PM2.5 at CAFÉ and NTU stations were -26.7 and -27.0‰ during summertime, which were lighter than those in the spring period by 2.5‰. The stable carbon isotope ratio measured in the summertime were representative of the local emissions as Taiwan was isolated from continental air mass. On the contrary, the isotopically heavy carbon aerosols in the springtime were attributed to the influences of PM2.5 from mainland China. This inference was supported by δ13CTC data coupling with WRF/Chem model simulations. The averaged δ13CTC in PM2.5 collected at the Douliu and Chayi stations during autumn/winter season were -28.9 and -28.4‰, respectivevly, suggesting local origins. Similar seasonal patterns were found for 208Pb/207Pb ratio. At CAFÉ and NTU stations, the average values of 208Pb/207Pb ratio in the summertime were 2.4227 and 2.4312, respectively. The ratios increased to 2.4408 and 2.4318 in the spring sampling period, which were very close to those obtained in central and northern China, indicating long-range transport of air pollution by Asian continental outflows. The 208Pb/207Pb ratios at Douliu and Chayi stations in the autumn/winter periods were 2.4286 and 2.4291, respectively, suggesting local sources. For 87Sr/86Sr, the average values at all the stations varied between 0.708628 and 0.721940. Unlike δ13CTC and 208Pb/207Pb, no significant seasonal variation was found in 87Sr/86Sr. In case of vehicle-derived PM2.5, the average δ13CTC was -24.4‰ which was comparable to that (-25.1‰) of coal ash collected from coal-fired power plants. In addition, this study also determined 208Pb/207Pb and 87Sr/86Sr ratios for vehicle-emitted PM2.5 with the average values of 2.4380 and 0.711460, respectively.

英文關鍵字

PM2.5, Isotope, Source Identification, Long-range Transported pollutants