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研究生: 廖浚丞
Liao, Jiun-Cheng
論文名稱: Elemental determinations of nano, submicron and micron airborne particulates in the atmosphere of Hsinchu Science Park
新竹科學園區大氣中奈米、次微米和微米懸浮微粒的元素分析
指導教授: 王竹方
Wang, Chu-Fang
口試委員:
學位類別: 碩士
Master
系所名稱: 原子科學院 - 生醫工程與環境科學系
Department of Biomedical Engineering and Environmental Sciences
論文出版年: 2010
畢業學年度: 98
語文別: 英文
論文頁數: 128
中文關鍵詞: 電子式低壓衝擊器雷射剝蝕誘導耦合電漿質譜儀雙粒徑採樣器新竹科學園區大陸沙塵暴
外文關鍵詞: ELPI, LA-ICP-MS, Dichotomous sampler, Hsinchu Science Park, Asian dust storm
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  • This study employed the method, which we have developed for determining trace metal elements in nano (0.030-0.108 μm), submicron (0.108-1.000 μm) and micron (1.000-9.970 μm) airborne particulates collected by electrical low pressure impactor (ELPI) using laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS). The calibration curves showed good linearity in the range of 0.9526 (69Ga)-0.9994(27Al), and RSD for seven replicates of standard filter were below 18%. Furthermore, comparison of correlation between ELPI/LA-ICP-MS and Dicho/ICP-MS proved reliability of the proposed method and had extremely practical value. The proposed analytical method was applied to determine elemental concentrations of nano, submicron and micron particles collected at Hsinchu Science Park (HSP). Total of 27 elements, including Na, Mg, Al, Si, K, Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Rb, Se, Sr, Ag, Cd, In, Cs, Ba, Tl and Pb were determined in this work. The result showed that at HSP was possibly responsible for As and Si in fine particles (<1μm). Annual trends of Pb, Cu, V, As, Cd and Tl have increased gradually, indicating that air pollutions at HSP became more serious from 2007 to 2010. Ambient mean As concentrations measured at HSP are all below the limited value (6ng/m3). However, 27 out of 99 measured As data were higher than the limited values with a 26.0 ng/m3 maximum concentration found in the year of 2009. On the other hand, the highly concentrated Ga, In and Tl in submicron particles might pose a potential health risk to the surrounding public. Asian dust (AD) storm are known to be a major air pollution source, which have strongly affected the atmospheric environment in many aspect. Aerosol samples were collected at national experimental high school from March 17 to 24, 2010. The result showed that most major elements, including Na, Mg, Al, Si, Fe, K and Ti distributed in not only micron fraction but also submicron fraction, which were carried by the storm. Submicron contributions of Zn, Cu, V, Pb, As and Cd descend significantly during AD episode while micron contribution is increased. Furthermore, we believed that several HSP related elements such as Tl, Rb, Cs, Co, Ga and Ag in micron fraction were also associated with dust storm, which suggest that dust storm not only deliver large amounts of crustal elements but also contribute significant amounts of toxic pollutants from foreign regions.


    TABLE OF CONTENTS Page 中文摘要…………………………………………………………………………… І Abstract………………………………………………………………………………Ⅱ 謝誌…………………………………………………………………………………..Ш LIST OF TABLES……………………………………………………………………VI LIST OF FIGURES…...……………………………………………………………VⅡ CHAPTER 1 INTRODUCTION…………………………………………………………………1 1.1 General Overview………………………………………………………………1 1.2 Purpose of This Study…………………………………………………………4 2 LITERATURE REVIEW……………………………………………………………7 2.1 Air Quality Problems near Hsinchu Science Park……………………………7 2.2 Identification of Emission Source by Related Elements………………………10 2.3 Characterization of Dichotomous Sampler……………………………………15 2.4 Size Segregation of Particles by ELPI………………………………………19 2.5 Elemental Determination of Airborne Particulates by Conventional Method...............23 2.6 Elemental Determination of Airborne Particulates by LA-ICP-MS…………27 2.7 Dust Storm Episodes Review for Taiwan……………………………………31 3 EXPERIMENTAL AND METHODS……………………………………………35 3.1 Experimental…………………………………………………………………..35 3.1.1 Reagents and Materials…………………………………………………35 3.1.2 Experimental Equipments………………………………………………36 3.2 Sample collection……………………………………………………………40 3.3 Preparation of Standards filters for LA-ICP-MS Analysis……………………46 4 RESULTS AND DISCUSSION…………………………………………………48 4.1 Validation of LA-ICP-MS Analysis…………………………………………48 4.1.1 Optimization of Analytical Conditions for LA-ICP-MS using grid mode……………………………………………………………48 4.1.2 Quality Assurance and Quality Control for LA-ICP-MS / ICP-MS………51 4.1.3 Intercomparison between ELPI/LA-ICP-MS with Dicho/ICP-MS………58 4.2 Air Quality Investigation of HSP……………………………………………61 4.2.1 Elemental Concentrations of Size-Segregated Particles Surrounding HSP…………………………………………………………61 4.2.2 Annual elemental concentration variations of HSP………………………67 4.2.3 Elemental Size Distributions of Particulate Elements Collected by ELPI…………………………………………………………77 4.2.4 Influences of Land and Sea Breezes for Elemental Concentration Variations……………………………………………………83 4.3 Charaterization of Asian Dust Storm Episode…………………………………89 5 CONCLUSIONS AND FUTURE WORKS………………………………………99 5.1 Conclusions……………………………………………………………………99 5.2 Future Works………………………………………………………………102 REFERENCE………………………………………………………………103 APPENDIX………………………………………………………………111

    Almirall J.R., Benjamin E. Naes, Sayuri Umpierrez, Scott Ryland, Cleon Barnett, 2008. A comparison of laser ablation inductively coupled plasma mass spectrometry, micro X-ray fluorescence spectroscopy, and laser induced breakdown spectroscopy for the discrimination of automotive glass. Spectrochimica Acta Part B 63, 1145–1150.

    ATSDR (Agency for Toxic Substances and Disease Registry), 2002. Regulations and guidelines applicable. Accessed in September 2002 (www.atsdr.cdc.gov/toxprofiles/tp11-c8.pdf).

    Adler, K.B., Fischer, B.M., 1994. Interactions between respiratory epithelial cells and cytokines: relationships to lung inflammation. Annals of the New York Academy of Science 725, 128–145.

    Al M., I.F., 2003. Trace elements in atmospheric precipitation at Northern Jordan measured by ICP-MS: acidity and possible sources. Atmospheric Environment 37, 4507–4515.

    Adachi K., Tainosho Y., 2004. Characterization of heavy metal particles embedded in tire dust. Environment International 30, 1009–1017.

    Cheng M.T., Y.C. Lin, C.P. Chio, C.F. Wang, C.Y. Kuo, 2005. Characteristics of aerosols collected in central Taiwan during an Asian dust event in spring 2000. Chemosphere 61, 1439–1450.

    Chein H.M., Yu-Du Hsu, Shankar G. Aggarwal, Tzu-Ming Chen, Chun-Chao Huang. 2006. Evaluation of arsenical emission from semiconductor and opto-electronics facilities in Hsinchu, Taiwan. Atmospheric Environment 40, 1901–1907

    Chen L.K, 2009. The determinations of inorganic elements in nano, submicron and micron airborne particulates in Taiwan area. 1-126

    Chuen J.T., Sheng-Chieh Chen, Charles C.-K. Chou, Gwo-Dong Roam, Sen-Sung Cheng, Ya-Nan Wang, 2010. Ultrafine particles at three different sampling locations in Taiwan. Atmospheric Environment 44, 553-540.

    Chen, Y.S., Shen, P.C., Chen, E.R., Liu, Y.K., Wu, T.N., Yang, C.Y., 2004. Effects of Asian dust storm events on daily mortality in Taipei, Taiwan. Environmental Research 95, 151–155.

    Cheng M.T., Y.C. Lin, C.P. Chio, C.F. Wang, C.Y. Kuo, 2005. Characteristics of aerosols collected in central Taiwan during an Asian dust event in spring 2000. Chemosphere 61, 1439–1450.

    Chen S.J, Lien-Te Hsieh, Mau-Jen Kao, Wen-Yinn Lin, Kuo-Lin Huang, Chih-Chung Lin, 2004. Characteristics of particles sampled in southern Taiwan during the Asian dust storm periods in 2000 and 2001. Atmospheric Environment 38, 5925–5934.

    Dongarrà G., E. Manno, D. Varrica, M. Vultaggio, 2007. Mass levels, crustal component and trace elements in PM10 in Palermo, Italy. Atmospheric Environment 41, 7977–7986.

    Divita F., Ondov, J.M., Suarez, A.E., 1996. Size spectra and atmospheric growth of V-containing aerosol in Washington DC. Aerosol Science and Technology 25, 256–273.

    Duce R.A., C.K. Unni, B.J. Ray, J.M. Prospero, J.T. Merrill, 1980. Longrange atmospheric transport of soil dust from Asia to the tropical North Pacific: temporal variability, Science 209, 1522– 1524.

    Englyst V., Nils-Goran Lundstroma, Lars Gerhardsson, Lars Rylander, Gunnar Nordberg. 2001. Lung cancer risks among lead smelter workers also exposed to arsenic. The Science of the Total Environment 273, 77-82.

    European Community, 1992 European Community Deskbook. Washington, D.C: Environmental Law Institute.

    Environmental Protection Agency(EPA), Taiwan, http://taqm.epa.gov.tw/taqm/zh-tw/DataHourly.aspx

    EC(Europe an Commission), 2000. DG environmental working group on arsenic, cadmium and nickel compounds, 2000. Ambient air pollution by As, Cd and Ni compounds, Position Paper (Final Version), October 2000.

    Englert N., 2004. Fine particles and human health–a review of epidemiological studies. Toxicology Letters 149, 235–242.
    Fan, X.B., Okada, K., Niimura, N., Kai, K., Arao, K., Shi, G.Y., Oin, Y., Mitsuta, Y., 1996. Mineral particles collected in China and Japan during the same Asian dust-storm event. Atmospheric Environment. 30, 347–351.

    Farmer J.G., Charun Yafa, 2006. A comparative study of acid-extractable and total digestion methods for the determination of inorganic elements in peat material by inductively coupled plasma-optical emission spectrometry. Analytica Chimica Acta 557, 296–303.

    Fang G.C., Cheng-Nan Chang, Yuh-Shen Wu, Shin-Chung Lu, Peter Pi-Cheng Fu, Shyh-Chyi Chang, Chii-Dong Cheng, Win-Hsiao Yuen, 2002. Concentration of atmospheric particulates during a dust storm period in central Taiwan, Taichung. The Science of the Total Environment 287, 141–145.

    Galvan A., S., Santamarı’a, A., 1998. Gallium toxicity. Toxicology Letters 99, 1–13.

    Guo, J. H., Rahn, K. A., Zhuang, G. S., 2004. A mechanism for the increase of pollution elements in dust storms in Beijing. Atmospheric Environment, 38, 855-862.

    Gatz, D.F., Prospero, J.M., 1996. A large silicon–aluminum aerosol plume in central Illinois: north African desert dust? Atmospheric Environment. 30, 3789–3799.

    Gligorovski S., Johannes T. Van Elteren, Irena Grgić, 2008. A multi-element mapping approach for size-segregated atmospheric particles using laser ablation ICP-MS combined with image analysis. The Science of the Total Environment. XX, XXX–XXX.

    Haley, P.J., 1991. Pulmonary toxicity of stable and radioactive lanthanides. Health Phys. 61, 809–820.

    Hsinchu Science Park, http://eweb.sipa.gov.tw/en/, Aug 10 2005.

    Hirano, S., Suzuki, K.T., 1996. Exposure, metabolism and toxicity of rare earths and related compounds. Health Perspect. 104, 85–95.

    Hu M., Ling - Yanne , Yuan - Hang Zhang , Xiao-Feng Huang , Ting - Ting Yao, 2008. Fine Particle Emissions from On-Road Vehicles in the Zhujiang Tunnel, China. Environmental Science and Technology 42, 4461–4466
    Hata A., 2001. Soil and Groundwater Pollution. Yuhikaku Publishing Co., Ltd., Tokyo, 233

    Huang K.L, Chih-chung Lin, Shui-jen Chen, 2006. Characteristics of Metals in Nano/Ultrafine/Fine/Coarse Particles Collected Beside a Heavily Trafficked Road. Environmental Science and Technology 39, 113-122.
    Kulmala, M., Vehkamäki, H., Petaja, T., Dal Maso, M., Lauri, A., Kerminen, V.M., Birmili, W. and McMurry, P.H. 2004. Formation and Growth Rates of Ultrafine Atmospheric Particles: A Review of Observations. Journal of aerosol science 35, 143-176.
    Kwon, H.J., Cho, S.H., Chun, Y., Lagarde, F., Pershagen, G., 2002. Effects of the Asian dust events on daily mortality in Seoul, Korea. Environmental Research 90, 1–5.

    Korenyi B., A.L., Molnar, A.C., Fidelus-Gort, R., 1992. Al Eskan disease: desert storm pneumonitis. Military Medicine 157, 452–462.

    Kulkarni P. , Shankararaman Chellam , James B. Flanagan , R.K.M. Jayanty, 2007. Microwave digestion—ICP-MS for elemental analysis in ambient airborne fine particulate matter: Rare earth elements and validation using a filter borne fine particle certified reference material. Analytica Chimica Acta 599, 170–176

    Karanasiou A.A., I.E. Sitaras, P.A. Siskos, K. Eleftheriadis, 2007. Size distribution and sources of trace metals and n-alkanes in the Athens urban aerosol during summer. Atmospheric Environment 41, 2368–2381.

    Kuo T.H., Cheng-Fen Chang, Andrius Urba, Kestutis Kvietkus, 2006. Atmospheric gaseous mercury in Northern Taiwan. Science of the Total Environment 368, 10-18.

    Lin C.C., Shui-Jen Chen , Kuo-Lin Huang, 2005. Characteristics of Metals in Nano/Ultrafine/Fine/Coarse Particles Collected Beside a Heavily Trafficked Road. Environmental Science and Technology 39, 8113–8122.

    Manoli E.; Voutsa, D.; Samara, C. 2002. Chemical characterization and source identification/apportionment of fine and coarse air particles in Thessaloniki, Greece. Atmospheric Enviroment 36, 949-961.

    Meszaros E., Barcza, T., Gelencser, A., Hlavay, J., Kiss, Gy., Krivacsy, Z., Molnar, A., Polyak, K., 1997. Size distributions of inorganic and organic species in the atmospheric aerosol in Hungary. Journal of Aerosol Science 28, 1163–1175.
    Maricq M.M., Ning Xu, and Richard E. Chase, 2006. Measuring Particulate Mass Emissions with the Electrical Low Pressure Impactor. Aerosol Science and Technology 40, 85–96.

    Marcazzan G.M., Stefano Vaccaro, Gianluigi Valli, Roberta Vecchi, 2001. Characterisation of PM10 and PM2.5 particulate matter in the ambient air of Milan (Italy). Atmospheric Environment 35, 4639–4650.

    Okuda T., Masayuki Katsuno, Daisuke Naoi, Shunsuke Nakao, Shigeru Tanaka, Kebin He, Yongliang Ma, Yu Lei, Yingtao Jia, 2008. Trends in hazardous trace metal concentrations in aerosols collected in Beijing, China from 2001 to 2006. Chemosphere 72, 917–924.

    Pakkanen T.A., Kerminen, V.M., Korhonen, C.H., Hillamo, R.E., Aarnio, P., Koskentalo, T., Maenhaut, W., Urban and rural ultrafine (PM0.1) particles in the Helsinki area. Atmospheric Enviroment 35, 4593-4607.

    Pinto J. P., and R. K. Stevens, R. D. Willis and R. Kellogg, Y. Mamane, J. Novak and J. Šantroch, I. Beneš, J. Leni ek, V. Bureš. 1998. Czech Air Quality Monitoring and Receptor Modeling Study. Environmental Science and Technology 32, 843–854.

    Pueschel R.F., 1995. Atmospheric Aerosol. Van Norstrand Reinhold, New York, pp. 120–175.

    Park M.H., Kim, Y.P., Kang, C.H., 2003. Aerosol composition change due to dust storm: measurements between 1992 and 1999 at Gosan, Korea. Water, Air Soil Poll. Focus 3, 117–128.

    Pope C.A.III, Burnett, R.T., Thun, M.J., Calle, E.E., Krewski, D., Ito, K., Thurston, G.D., 2002. Lung cancer, cardiopulmonary mortality, and long-term exposure to fine particulate air pollution. The Journal of the American Medical Association 287,1132–1141.

    Pacyna J.M., 1986. Atmospheric trace elements from natural and anthropogenic sources. In: Nriagu, J.O., Davidson, C.I. (eds.): Toxic Metals in the Atmosphere. Wiley, New York.

    Querol X., M. Viana, A. Alastuey, F. Amato, T. Moreno, S. Castillo, J. Pey, J. de la Rosa, A. Sánchez de la Campa, B. Artíñano, P. Salvador, S. García Dos Santos, R. Fernández-Patier, S. Moreno-Grau, L. Negral, M.C. Minguillón, E. Monfort, J.I. Gil, A. Inza, L.A. Ortega, J.M. Santamaría, J. Zabalza, 2007. Source origin of trace elements in PM from regional background, urban and industrial sites of Spain. Atmospheric Environment 41, 7219–7231.

    Russo R.E., Jhanis J. Gonzalez, Chunyi Liu, Sy-Bor Wen, Xianglei Mao, 2007. Metal particles produced by laser ablation for ICP–MS measurements. Talanta 73, 567–576.
    Rahn K.A., Lowenthal, D.H., 1984. Elemental tracers of distant regional pollution aerosols. Science 223, 132–139.
    Sioutas C., Satya B. Sardar, Michael D. Geller, Paul A. Solomon, 2006. Development and evaluation of a high-volume dichotomous sampler for chemical speciation of coarse and fine particles. Aerosol Science 37, 1455 – 1466.

    Sun Y.L.; Zhuang, G.S., Wang, Y., Zhao, X.J., Li, J., Wang, Z.F., An, Z.S., 2005. Chemical composition of dust storms in Beijing and implications for the mixing of crustal aerosol with pollution aerosol on the pathway, Journal of Geophysical Research, 110.

    Shi J.P., A.A. Khan, Roy M. Harrison, 1999. Measurements of ultrafine particle concentration and size distribution in the urban atmosphere. The Science of the Total Environment 235, 51–64.

    Sioutas C., Manisha Singh, Peter A. Jaques, 2002. Size distribution and diurnal characteristics of particle-bound metals in source and receptor sites of the Los Angeles Basin. Atmospheric Environment 36, 1675–1689.

    Sander P.G., Xu, N., Dalka, T., Maricq, M.M., 2003. Airborne brake wear debris: size distributions, composition, and a comparison of dynamometer and vehicle tests.
    Environmental Science and Technology 37, 4060–4069.

    Swietlicki E., Puri, S., Hansson, H.C., Edner, H., 1996. Urban air pollution source apportionment using a combination of aerosol and gas monitoring techniques. Atmospheric Environment 30, 2795–2809.

    Shi H.S., Kan, L.L., 2009. Characteristics of municipal solid wastes incineration (MSWI) fly ash–cement matrices and effect of mineral admixtures on composite system. Construction and Building Materials xxx, xxx-xxx.

    Tanaka A., 2004. Toxicity of indium arsenide, gallium arsenide, and aluminium gallium arsenide. Toxicology and Applied Pharmacology 198, 405–411.

    Tanaka, S., Yasushi, N., Fukasawa, T., Santosa, S.J., Yamanaka, K., Ootoshi, T., 1998. Rapid and simultaneous multi-element analysis of atmospheric particulate matter using inductively plasma mass spectrometry with laser ablation sample introduction. Journal of Analytical Atomic Spectrometry 13, 135-140.

    Utsunomiya S, Keld A . Jensen , Gerald J . K eeler, Rodney C. Ewing, 2004. Direct Identification of Trace Metals in Fine and Ultrafine Particles in the Detroit Urban Atmosphere. Environmental Science and Technology 38, 2289-2297.

    US EPA, 2004. Air Quality Criteria for Particulate Matter 2004. US Environmental Protection Agency, Washington, DC, EPA 600/P-99/002aF-bF.
    Watanabe I., Yoshinari Suzuki, Tatsuo Oshida, Yen-Jean Chen, Liang-Kong Lin, Yu-Huang Wang, Kouh-Cheng Yang, Katsuji Kuno, 2007. Accumulation of trace elements used in semiconductor industry in Formosan squirrel, as a bio-indicator of their exposure, living in Taiwan. Chemosphere. 68, 1270–1279.
    Wrobel A., E. Rokita, W. Maenhaut, 2000. Transport of traffic-related aerosols in urban areas. The Science of the Total Environment 257, 199-211.

    WHO (World Health Organization), 2000. Guidelines for air quality, Geneva (www.who.int/environmental information/Air/Guidelines/aqguide7.pdf), accessed in September 2002.

    Wang C.F., C.Y. Chang, C.J. Chin, L.C. Men, 1999. Determination of arsenic and vanadium in airborne related reference materials by inductively coupled plasma-mass spectrometry. Analytica Chimica Acta 392, 299-306.

    Wang, T., Zhu, Z.D., 2001. Studies on the sandy desertification in China, Chinese Journal of Eco-Agriculture 9, 7-12.

    Wang S.G., Wang, J.Y., Zhou, Z.J., Shang, K.Z., 2005.Regional characteristics of three kinds of dust storm events in China, Atmospheric Environment 39, 509-520.

    Weckwerth, G., 2001. Verification of traffic emitted aerosol components in the ambient air of Cologne (Germany). Atmospheric Environment 35, 5525–5536.

    Wåhlin P., Berkowicz, R., Palmgren, F., 2006. Characterisation of traffic-generated particulate matter in Copenhagen. Atmospheric Environment 40, 2151–2159.

    Wang Q., Yan, J., Tu, X., Chi, Y., Li, X., Lu, S., Cen, K., 2009. Thermal treatment of municipal solid waste incinerator fly ash using DC double arc argon plasma. Fuel 88, 955–958.

    Xuan J., 1999. Dust emission factors for environment of Northern China. Atmospheric Environment 33, 1767–1776.

    Yang E., 1978. Fundamentals of Semiconductor Devices. McGraw-Hill, New York, 14–15.

    Yoshiie R., Yamamoto, Y., Uemiya, S., Kambara, S., Moritomi, H., 2008. Simple and rapid analysis of heavy metals in sub-micron particulates in flue gas. Powder Technology 180, 135–139.

    Zhang R., Mingxing Wang, Xiaoye Zhang, Guanghua Zhu, 2003. Analysis on the chemical and physical properties of particles in a dust storm in spring in Beijing. Powder Technology 137, 77– 82.

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