空氣中細懸浮微粒的組成包含原生性鋁矽酸鹽礦物顆粒、海鹽顆粒、元素碳、有機碳及金屬顆粒，衍生性微粒之組成則有二次無機成份(硫酸鹽、硝酸鹽及銨鹽)、有機污染物及生物性顆粒，而金屬元素在大氣環境中相對於二次生成之無機鹽或是有機物相較穩定，其化學特性隨傳輸擴散變異也較小，因此以同位素分析結果作為輔助，如碳(C)、硫(S)、鍶(Sr)和鉛(Pb)等同位素，應用同位素比值可達到環境污染源鑑識之目的。
本研究於中南部地區選取八個地點，分別為沙鹿、大里、二林、線西、埔里、崙背、朴子及安南進行周界採樣，並將ADS採樣結果進行微粒損失與揮發性物種之修正，同時進行有機氣膠之成份分析及同位素分析結果來加強大氣細懸浮微粒的污染來源解析。ADS修正結果顯示修正前後，在PM2.5質量濃度方面最大可達相差近19%，而硝酸根最大相差85%，氨根最大相差60%，因此有必要對其做修正。而有機酸成份oxalate在朴子、台南與美濃有明顯的季節變化，由於風向之影響，台灣冬季主要為東北風為主，故污染物多來自非當地之污染源傳輸，衍生性物種會相較於夏季時高，因此二次反應生成物的oxalate有著夏低冬高之趨勢。
碳同位素分析結果其δ13C介於-23.7至-26.3‰之間，平均為25.25±0.75‰，與中國大陸各城市的文獻值較為相近，推測有受到長程傳輸污染物之影響。在鍶同位素方面，八個採樣點之87Sr/86Sr介於0.709081至0.710039，平均值為0.70944±0.000333，安南之87Sr/86Sr有較低值(0.709081)，埔里站之87Sr/86Sr有較高值(0.710039)。從文獻得知燃煤的鍶同位素比值較低，冶煉廠之鍶同位素比值較高，而冶煉對於安南之貢獻是很低的，所以造成安南之鍶同位素比值有較低的情形，同樣的二林與沙鹿也是有較低之87Sr/86Sr，而CMB模擬結果也顯示此兩個採樣點之燃煤與冶煉的貢獻有一高一低之情，與安南類似。鉛同位素分析結果在208Pb/207Pb方面其值介於2.4279至2.4332，平均值為2.431±0.0016，與206Pb/207Pb、208Pb/206Pb和206Pb/204Pb相比，有明顯地與中國地區的值不同，故208Pb/207Pb比較適合做為區分本土與遠程傳輸鉛微粒對台灣地區PM2.5之鉛貢獻量的指標。

In this study, the use of isotope analysis, such as carbon (C), sulfur (S), strontium (Sr) and lead (Pb), isotopic ratios can be applied to achieve the purpose of environmental pollution forensics. The result of carbon isotope analysis :δ13C is between -23.7 to -26.3 ‰, its average is 25.25 ± 0.75 ‰ and is similar with the result of literature in Chinese cities, suggesting that there are affected by long-range transport of pollutants. The result of strontium isotope analysis : 87Sr/86Sr is between 0.709081 to 0.710039 , its average is 0.70944±0.000333,In Annan, the 87Sr / 86Sr has a lower value (0.709081), In Puli, the 87Sr/ 86Sr has a higher value (0.710039).From the literature we know lower strontium isotope ratios of coal combustion and higher strontium isotope ratios of smelter, we can know smelter contribution is very low in Annan from CMB, so the result of strontium isotope ratios in Annan have a lower value.The same situation happen in Erlin and Shalu,this two stations have lower 87Sr/ 86Sr value,and CMB results also show that the contribution of coal combustion is high and the contribution of smelter is low. The result of lead isotope analysis: 208Pb/207Pb is between 2.4279 to 2.4332 , its average is 2.431±0.0016, compared with the206Pb/207Pb、208Pb/206Pb and 206Pb/204Pb, 208Pb/207Pb is obviously different from the value of Chinese regions. Therefore, 208Pb/207Pb is more suitable as the indicator to distinguish local and long-distance transport of lead particles contributing to Taiwan.

Allegrini, I., De Santis, F., Di Palo, V., Febo, A., Perrino, C., Possanzini, M., & Liberti, A. (1987). Annular denuder method for sampling reactive gases and aerosols in the atmosphere. Science of the Total Environment, 67(1), 1-16.
Appel, B. R., Winer, A. M., Tokiwa, Y., & Biermann, H. W. (1990). Comparison of atmospheric nitrous acid measurements by annular denuder and differential optical absorption systems. Atmospheric Environment. Part A. General Topics,24(3), 611-616.
Benner, C. L., Eatough, D. J., Eatough, N. L., & Bhardwaja, P. (1991). Comparison of annular denuder and filter pack collection of HNO 3 (g), HNO 2 ((g), SO 2 (g), and particulate-phase nitrate, nitrite and sulfate in the south-west desert. Atmospheric Environment. Part A. General Topics, 25(8), 1537-1545.
Berg, J. M., James, D. L., Berg, C. F., Toda, K., & Dasgupta, P. K. (2010). Gas collection efficiency of annular denuders: A spreadsheet-based calculator.Analytica chimica acta, 664(1), 56-61.
Bollhöfer, A., & Rosman, K. J. R. (2001). Isotopic source signatures for atmospheric lead: the Northern Hemisphere. Geochimica et Cosmochimica Acta, 65(11), 1727-1740.
Brauer, M., Koutrakis, P., Wolfson, J. M., & Spengler, J. D. (1989). Evaluation of the gas collection of an annular denuder system under simulated atmospheric conditions. Atmospheric Environment (1967), 23(9), 1981-1986.
Cao, J. J., Chow, J. C., Tao, J., Lee, S. C., Watson, J. G., Ho, K. F., ... & Han, Y. M. (2011). Stable carbon isotopes in aerosols from Chinese cities: Influence of fossil fuels. Atmospheric environment, 45(6), 1359-1363.
Chen, S. C., Tsai, C. J., Huang, C. Y., Chen, H. D., Chen, S. J., Lin, C. C., ... & Roam, G. D. (2010). Chemical mass closure and chemical characteristics of ambient ultrafine particles and other PM fractions. Aerosol Science and Technology, 44(9), 713-723.
Cheng, H., & Hu, Y. (2010). Lead (Pb) isotopic fingerprinting and its applications in lead pollution studies in China: a review. Environmental Pollution, 158(5), 1134-1146.
Cheng, M. C., You, C. F., Lin, F. J., Huang, K. F., & Chung, C. H. (2011). Sources of Cu, Zn, Cd and Pb in rainwater at a subtropical islet offshore northern Taiwan. Atmospheric Environment, 45(11), 1919-1928.
Cheng, Y. H., & Tsai, C. J. (1997). Evaporation loss of ammonium nitrate particles during filter sampling. Journal of Aerosol Science, 28(8), 1553-1567
Chow, J. C., Lowenthal, D. H., Chen, L. W. A., Wang, X., & Watson, J. G. (2015). Mass reconstruction methods for PM2. 5: a review. Air Quality, Atmosphere & Health, 8(3), 243-263.
Crittenden, R. G., Andrew, A. S., LeFournour, M., Young, M. D., Middleton, H., & Stockmann, R. (2007). Determining the geographic origin of milk in Australasia using multi-element stable isotope ratio analysis. International Dairy Journal, 17(5), 421-428.
Das, A., Chung, C. H., You, C. F., & Shen, M. L. (2012). Application of an improved ion exchange technique for the measurement of δ 34 S values from microgram quantities of sulfur by MC-ICPMS. Journal of Analytical Atomic Spectrometry, 27(12), 2088-2093.
Das, O., Wang, Y., & Hsieh, Y. P. (2010). Chemical and carbon isotopic characteristics of ash and smoke derived from burning of C 3 and C 4 grasses.Organic Geochemistry, 41(3), 263-269.
Ettler, V., Mihaljevič, M., & Komárek, M. (2004). ICP-MS measurements of lead isotopic ratios in soils heavily contaminated by lead smelting: tracing the sources of pollution. Analytical and bioanalytical chemistry, 378(2), 311-317.
Febo, A., Perrino, C., & Cortiello, M. (1993). A denuder technique for the measurement of nitrous acid in urban atmospheres. Atmospheric Environment. Part A. General Topics, 27(11), 1721-1728.
Gallon, C., Ranville, M. A., Conaway, C. H., Landing, W. M., Buck, C. S., Morton, P. L., & Flegal, A. R. (2011). Asian industrial lead inputs to the North Pacific evidenced by lead concentrations and isotopic compositions in surface waters and aerosols. Environmental science & technology, 45(23), 9874-9882.
Gleason, J. D., & Kyser, T. K. (1984). Stable isotope compositions of gases and vegetation near naturally burning coal.
Harris, E., Sinha, B., Hoppe, P., Crowley, J. N., Ono, S., & Foley, S. (2012). Sulfur isotope fractionation during oxidation of sulfur dioxide: gas-phase oxidation by OH radicals and aqueous oxidation by H 2 O 2, O 3 and iron catalysis. Atmospheric Chemistry and Physics, 12(1), 407-423.
Hsu, S. C., Liu, S. C., Jeng, W. L., Chou, C. C., Hsu, R. T., Huang, Y. T., & Chen, Y. W. (2006). Lead isotope ratios in ambient aerosols from Taipei, Taiwan: Identifying long-range transport of airborne Pb from the Yangtze Delta.Atmospheric Environment, 40(28), 5393-5404.
Ingham, D. B. (1975). Diffusion of aerosols from a stream flowing through a cylindrical tube. Journal of Aerosol Science, 6(2), 125-132.
Irei, S., Huang, L., Collin, F., Zhang, W., Hastie, D., & Rudolph, J. (2006). Flow reactor studies of the stable carbon isotope composition of secondary particulate organic matter generated by OH-radical-induced reactions of toluene. Atmospheric Environment, 40(30), 5858-5867.
Joseph, A. E., Unnikrishnan, S., & Kumar, R. (2012). Chemical characterization and mass closure of fine aerosol for different land use patterns in Mumbai city. Aerosol and Air Quality Resarch, 12(1), 61-72.
Jung, J., & Kawamura, K. (2011). Springtime carbon emission episodes at the Gosan background site revealed by total carbon, stable carbon isotopic composition, and thermal characteristics of carbonaceous particles.Atmospheric Chemistry and Physics, 11(21), 10911-10928.
Kanayama, S., Yabuki, S., Yanagisawa, F., & Motoyama, R. (2002). The chemical and strontium isotope composition of atmospheric aerosols over Japan: the contribution of long-range-transported Asian dust (Kosa).Atmospheric Environment, 36(33), 5159-5175.
Kawamura, H., Matsuoka, N., Tawaki, S., & Momoshima, N. (2001). Sulfur isotope variations in atmospheric sulfur oxides, particulate matter and deposits collected at Kyushu island, Japan. Water, Air, and Soil Pollution, 130(1-4), 1775-1780.
Kawamura, K., & Ikushima, K. (1993). Seasonal changes in the distribution of dicarboxylic acids in the urban atmosphere. Environmental Science & Technology, 27(10), 2227-2235.
Kitto, A. M. (1992). Intercomparison of annular denuder and filter pack sampling methods for collection of acidifying species in south east England.Journal of Aerosol Science, 23, 699-702.
Koutrakis, P., Wolfson, J. M., Slater, J. L., Brauer, M., Spengler, J. D., Stevens, R. K., & Stone, C. L. (1988). Evaluation of an annular denuder/filter pack system to collect acidic aerosols and gases. Environmental science & technology, 22(12), 1463-1468.
Kundu, S., & Kawamura, K. (2014). Seasonal variations of stable carbon isotopic composition of bulk aerosol carbon from Gosan site, Jeju Island in the East China Sea. Atmospheric Environment, 94, 316-322.
Lahd Geagea, M., Stille, P., Gauthier-Lafaye, F., & Millet, M. (2008). Tracing of industrial aerosol sources in an urban environment using Pb, Sr, and Nd isotopes. Environmental science & technology, 42(3), 692-698.
Landis, M. S., Stevens, R. K., Schaedlich, F., & Prestbo, E. M. (2002). Development and characterization of an annular denuder methodology for the measurement of divalent inorganic reactive gaseous mercury in ambient air.Environmental science & technology, 36(13), 3000-3009.
Liu, H. C., You, C. F., Huang, K. F., & Chung, C. H. (2012). Precise determination of triple Sr isotopes (δ 87 Sr and δ 88 Sr) using MC-ICP-MS.Talanta, 88, 338-344.
López-Veneroni, D. (2009). The stable carbon isotope composition of PM 2.5 and PM 10 in Mexico City Metropolitan Area air. Atmospheric Environment,43(29), 4491-4502.
Maenhaut, W., Schwarz, J., Cafmeyer, J., & Chi, X. (2002). Aerosol chemical mass closure during the EUROTRAC-2 AEROSOL Intercomparison 2000.Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, 189(1), 233-237.
Malm, W. C., Sisler, J. F., Huffman, D., Eldred, R. A., & Cahill, T. A. (1994). Spatial and seasonal trends in particle concentration and optical extinction in the United States. Journal of Geophysical Research: Atmospheres, 99(D1), 1347-1370.
Mantha, N. M., Schindler, M., & Kyser, T. K. (2012). Silica-and sulfate-bearing rock coatings in smelter areas: Part II. Forensic tools for atmospheric metal (loid)-and sulfur-isotope compositions. Geochimica et Cosmochimica Acta, 90, 221-241.
Martinelli, L. A., Camargo, P. B., Lara, L. B. L. S., Victoria, R. L., & Artaxo, P. (2002). Stable carbon and nitrogen isotopic composition of bulk aerosol particles in a C4 plant landscape of southeast Brazil. Atmospheric Environment, 36(14), 2427-2432.
Mikuška, P., Večeřa, Z., Bartošíková, A., & Maenhaut, W. (2012). Annular diffusion denuder for simultaneous removal of gaseous organic compounds and air oxidants during sampling of carbonaceous aerosols. Analytica chimica acta,714, 68-75.
Mkoma, S. L., Kawamura, K., Tachibana, E., & Fu, P. (2014). Stable carbon and nitrogen isotopic compositions of tropical atmospheric aerosols: sources and contribution from burning of C 3 and C 4 plants to organic aerosols. Tellus B, 66.
Monna, F., Lancelot, J., Croudace, I. W., Cundy, A. B., & Lewis, J. T. (1997). Pb isotopic composition of airborne particulate material from France and the southern United Kingdom: implications for Pb pollution sources in urban areas.Environmental Science & Technology, 31(8), 2277-2286.
Mukai, H., Tanaka, A., Fujii, T., Zeng, Y., Hong, Y., Tang, J., ... & Xue, D. (2001). Regional characteristics of sulfur and lead isotope ratios in the atmosphere at several Chinese urban sites. Environmental science & technology, 35(6), 1064-1071.
Nakano, T., & Tanaka, T. I. (1997). Strontium isotope constraints on the seasonal variation of the provenance of base cations in rain water at Kawakami, central Japan. Atmospheric Environment, 31(24), 4237-4245.
Nakano, T., Yokoo, Y., Nishikawa, M., & Koyanagi, H. (2004). Regional Sr–Nd isotopic ratios of soil minerals in northern China as Asian dust fingerprints.Atmospheric Environment, 38(19), 3061-3067.
Ortiz, R., Enya, K., Sekiguchi, K., & Sakamoto, K. (2009). Experimental testing of an annular denuder and filter system to measure gas–particle partitioning of semivolatile bifunctional carbonyls in the atmosphere.Atmospheric Environment, 43(2), 382-388.
Pavuluri, C. M., Kawamura, K., & Swaminathan, T. (2015). Time-resolved distributions of bulk parameters, diacids, ketoacids and α-dicarbonyls and stable carbon and nitrogen isotope ratios of TC and TN in tropical Indian aerosols: Influence of land/sea breeze and secondary processes. Atmospheric Research, 153, 188-199.
Possanzini, M., Febo, A., & Liberti, A. (1983). New design of a high-performance denuder for the sampling of atmospheric pollutants. Atmospheric Environment (1967), 17(12), 2605-2610.
Roumeliotis, T. S., Dixon, B. J., & Van Heyst, B. J. (2010). An annular denuder system for the collection of elevated quantities of ammonia to allow for the measurement of inorganic reactive gases and aerosol species inside poultry houses. Biosystems engineering, 107(3), 178-185.
Schaap, M., Spindler, G., Schulz, M., Acker, K., Maenhaut, W., Berner, A., ... & Chi, X. (2004). Artefacts in the sampling of nitrate studied in the “INTERCOMP” campaigns of EUROTRAC-AEROSOL. Atmospheric Environment, 38(38), 6487-6496.
Sillanpää, M., Hillamo, R., Saarikoski, S., Frey, A., Pennanen, A., Makkonen, U., ... & Chalbot, M. C. (2006). Chemical composition and mass closure of particulate matter at six urban sites in Europe. Atmospheric Environment, 40, 212-223.
Simon, H., Bhave, P. V., Swall, J. L., Frank, N. H., & Malm, W. C. (2011). Determining the spatial and seasonal variability in OM/OC ratios across the US using multiple regression. Atmospheric Chemistry and Physics, 11(6), 2933-2949.
Stanier, C. O., Khlystov, A. Y., & Pandis, S. N. (2004). Ambient aerosol size distributions and number concentrations measured during the Pittsburgh Air Quality Study (PAQS). Atmospheric Environment, 38(20), 3275-3284.
Stein, S. W., Turpin, B. J., Cai, X., Huang, P. F., & Mcmurry, P. H. (1994). Measurements of relative humidity-dependent bounce and density for atmospheric particles using the DMA-impactor technique. Atmospheric Environment, 28(10), 1739-1746.
Stelson, A. W., & Seinfeld, J. H. (1982). Relative humidity and temperature dependence of the ammonium nitrate dissociation constant. Atmospheric Environment (1967), 16(5), 983-992.
Stelson, A. W., Friedlander, S. K., & Seinfeld, J. H. (1979). A note on the equilibrium relationship between ammonia and nitric acid and particulate ammonium nitrate. Atmospheric Environment (1967), 13(3), 369-371.
Tang, H., Lewis, E. A., Eatough, D. J., Burton, R. M., & Farber, R. J. (1994). Determination of the particle size distribution and chemical composition of semi-volatile organic compounds in atmospheric fine particles with a diffusion denuder sampling system. Atmospheric Environment, 28(5), 939-947.
Tsai, C. J., & Huang, H. Y. (1995). Atmospheric aerosol sampling by an annular denuder system and a high-volume PM 10 sampler. Environment International,21(3), 283-291.
Turpin, B. J., & Lim, H. J. (2001). Species contributions to PM2. 5 mass concentrations: Revisiting common assumptions for estimating organic mass.Aerosol Science & Technology, 35(1), 602-610.
Widory, D., Liu, X., & Dong, S. (2010). Isotopes as tracers of sources of lead and strontium in aerosols (TSP & PM 2.5) in Beijing. Atmospheric environment,44(30), 3679-3687.
Widory, D., Roy, S., Le Moullec, Y., Goupil, G., Cocherie, A., & Guerrot, C. (2004). The origin of atmospheric particles in Paris: a view through carbon and lead isotopes. Atmospheric Environment, 38(7), 953-961.
Winiwarter, W. (1989). A calculation procedure for the determination of the collection efficiency in annular denuders. Atmospheric Environment (1967),23(9), 1997-2002.
Xiao, H. Y., Zhu, R. G., Lin, B. N., & Liu, C. Q. (2011). Sulfur isotopic signatures in rainwater and moss Haplocladium microphyllum indicating atmospheric sulfur sources in Nanchang City (SE China). Science of the Total Environment, 409(11), 2127-2132.
Ye, Y., Tsai, C. J., Pui, D. Y., & Lewis, C. W. (1991). Particle transmission characteristics of an annular denuder ambient sampling system. Aerosol science and Technology, 14(1), 102-111.
Yin, J., & Harrison, R. M. (2008). Pragmatic mass closure study for PM 1.0, PM 2.5 and PM 10 at roadside, urban background and rural sites. Atmospheric environment, 42(5), 980-988.
Yu, X. Y., Lee, T., Ayres, B., Kreidenweis, S. M., Collett Jr, J. L., & Malm, W. (2005). Particulate nitrate measurement using nylon filters. Journal of the Air & Waste Management Association, 55(8), 1100-1110.
Zhang, X., & McMurry, P. H. (1992). Evaporative losses of fine particulate nitrates during sampling. Atmospheric Environment. Part A. General Topics,26(18), 3305-3312.
Zheng, J., Tan, M., Shibata, Y., Tanaka, A., Li, Y., Zhang, G., ... & Shan, Z. (2004). Characteristics of lead isotope ratios and elemental concentrations in PM 10 fraction of airborne particulate matter in Shanghai after the phase-out of leaded gasoline. Atmospheric Environment, 38(8), 1191-1200.
連明瑜(2008)，利用水溶性離子鉛同位素變化探討彭佳嶼大氣懸浮微粒中鉛的來源，國立成功大學大球科學研究所碩士論文。
張凱倫(2004)，大氣奈米微粒無機鹽類組成特性研究，國立成功大學環境工程學系碩士論文。
郭正傑(2007)，南部懸浮微粒超級測站之自動監測儀器與手動方法之比對.，國立成功大學環境工程學系碩士論文。
蔡春進，環境中奈米物質量測及特性分析技術開發研究案，環保署專案計畫，EPA-101-1602-02-08，(2012)
溫育勇(2002)，NO2 干擾環形氣固分離器之氣相亞硝酸採樣的誤差，國立成功大學環境工程學系碩士論文
謝璧晃(2011)，氨氣自動監測儀與氣固分離氣採樣之差異研究，國立成功大學環境工程學系碩士論文
彭宗仁等(2006)，穩定同位素在農業及生態環境上之應用. 台灣農業研究, 55(2), 79-90