Asian Journal of Atmospheric Environment

Korean Society for Atmospheric Environment (한국대기환경학회)
권호 표지
DOI QR코드

DOI QR Code

Single-particle Characterization of Aerosol Particles Collected Nearby a Lead Smelter in China

  • Jung, Hae-Jin (Department of Chemistry, Inha University) ;
  • Song, Young-Chul (Department of Chemistry, Inha University) ;
  • Liu, Xiande (Chinese Research Academy of Environmental Sciences) ;
  • Li, Yuwu (National Research Center for Environmental Analysis and Measurements) ;
  • Ro, Chul-Un (Department of Chemistry, Inha University)
  • Received : 2012.03.01
  • Accepted : 2012.05.29
  • Published : 2012.06.30
Download PDF
⟨ Previous Next ⟩

Abstract

China has been a top producer and exporter of refined lead products in the world since the year 2000. After the phasing-out of leaded gasoline in the late 1990s, non-ferrous metallurgy and coal combustion have been identified as potential major sources of aerosol lead in China. This paper presents the single particle analytical results of ambient aerosol particles collected near a lead smelter using a scanning electron microscopy- energy dispersive x-ray spectroscopy (SEM-EDX). Aerosol particle samples were collected over a 24-hour period, starting from 8 pm on 31 May 2002, using a high volume TSP sampler. For this near source sample, 73 particles among 377 particles analyzed (accounting for 19.4%) were lead-containing particles mixed with other species (S, Cl, K, Ca, and/or C), which probably appeared to be from a nearby lead smelter. Lead-containing particles of less than $2{\mu}m$ size in the near source sample were most frequently encountered with the relative abundances of 42%. SEM-EDX analysis of individual standard particles, such as PbO, PbS, $PbSO_4$, $PbCl_2$, and $PbCO_3$, was also performed to assist in the clear identification of lead-containing aerosol particles. Lead-containing particles were frequently associated with arsenic and zinc, indicating that the smelter had emitted those species during the non-ferrous metallurgical process. The frequently encountered particles following the lead-containing particles were mineral dust particles, such as aluminosilicates (denoted as AlSi), $SiO_2$, and $CaCO_3$. Nitrate- and sulfate-containing particles were encountered frequently in $2-4{\mu}m$ size range, and existed mostly in the forms of $Ca(NO_3,SO_4)/C$, $(Mg,Ca)SO_4/C$, and $AlSi+(NO_3,SO_4)$. Particles containing metals (e.g., Fe, Cu, and As) in this near source sample had relative abundances of approximately 10%. Although the airborne particles collected near the lead smelter contained elevated levels of lead, other types of particles, such as $CaCO_3$-containing, carbonaceous, metal-containing, nitrates, sulfates, and fly-ash particles, showed the unique signatures of samples influenced by emissions from the lead smelter.

Keywords

References

  1. Barrett, J., Taylor, K., Hudson-edwards, K., Charnock, J. (2010) Solid-Phase Speciation of Pb in Urban Road Dust Sediment: A XANES and EXAFS Study. Environmental Science and Technology 44, 2940-2946. https://doi.org/10.1021/es903737k
  2. Batonneau, Y., Bremard, C., Gengembre, L., Laureyns, J., Maguer, A.L., Maguer, D.L., Perdrix, E., Sobanska, S. (2004) Speciation of $PM_{10}$ Sources of Airborne Nonferrous Metals within the 3-km Zone of Lead/Zinc Smelters. Environmental Science and Technology 38, 5281-5289. https://doi.org/10.1021/es0497173
  3. Bowers, T., Beck, B. (2006) What is the meaning of nonlinear dose-response relationships between blood lead concentrations and IQ? Neurotoxicology 27, 520-524. https://doi.org/10.1016/j.neuro.2006.02.001
  4. Choel, M., Deboudt, K., Flament, P., Lecornet, G., Perdrix, E., Sobanska, S. (2006) Fast evolution of tropospheric Pb- and Zn-rich particles in the vicinity of a lead smelter. Atmospheric Environment 40, 4439-4449. https://doi.org/10.1016/j.atmosenv.2006.04.027
  5. Donaldson, K., Stone, V., Seaton, A., MacNee, W. (2001) Ambient particle inhalation and the cardiovascular system: potential mechanisms. Environmental Health Perspectives 109(suppl 4), 523-527. https://doi.org/10.1289/ehp.01109s4523
  6. Fermo, P., Cariati, F., Pozzi, A., Tettamanti, M., Collina, E., Pitea, D. (2000) Analytical characterization of municipal solid waste incinerator fly ash: Part II, Fresenius'. Journal of Analytical Chemistry 366, 267-272. https://doi.org/10.1007/s002160050052
  7. Flament, P., Mattielli, N., Aimoz, L., Choel, M., Deboudt, K., de Jong, J., Rimetz-Planchon, J., Weis, D. (2008) Iron isotopic fractionation in industrial emissions and urban aerosols. Chemosphere 73, 1793-1798. https://doi.org/10.1016/j.chemosphere.2008.08.042
  8. Fulton, M., Thomson, G., Hunter, R., Raab, G., Laxen, D., Hepb, W. (1987) Influence of blood lead on the ability and attainment of children in edinburgh. The Lancet 329, 1221-1226. https://doi.org/10.1016/S0140-6736(87)92683-3
  9. Geng, H., Park, Y.-M., Hwang, H., Kang, S., Ro, C.-U. (2009) Elevated nitrogen-containing particles observed in Asian dust aerosol samples collected at the marine boundary layer of the Bohai Sea and the Yellow Sea. Atmospheric Chemistry and Physics 9, 6933-6947. https://doi.org/10.5194/acp-9-6933-2009
  10. Geng, H., Ryu, J., Jung, H.-J., Chung, H., Ahn, K.-H., Ro, C.-U. (2010) Single-Particle Characterization of Summertime Arctic Aerosols Collected at Ny-Alesund, Svalbard. Environmental Science and Technology, 44, 2348-2353. https://doi.org/10.1021/es903268j
  11. Geng, H., Ryu, J., Maskey, S., Jung, H.-J., Ro, C.-U. (2011) Characterization of individual aerosol particles collected during a haze episode in Incheon, Korea using the quantitative ED-EPMA technique. Atmospheric Chemistry and Physics 11, 1327-1337. https://doi.org/10.5194/acp-11-1327-2011
  12. Green berg, R., Zoller, W., Gordon, G. (1978) Composition and size distributions of particles released in refuse incineration. Environmental Science and Technology 12, 566-573. https://doi.org/10.1021/es60141a011
  13. Greenwood, N.N., Earnshaw, A. (1984) Chemistry of the Elements. Pergamon Press Oxford, New York.
  14. He, K., Yang, F., Ma, Y., Zhang, Q., Yao, X., Chan, C.K., Cadle, S., Chan, T., Mulawa, P. (2001) The characteristics of $PM_{2.5}$ in Beijing, China. Atmospheric Environment 35, 4959-4970. https://doi.org/10.1016/S1352-2310(01)00301-6
  15. Hilary, A.G. (2001) The biological chemistry of lead. Current Opinion in Chemical Biology 5, 223-227. https://doi.org/10.1016/S1367-5931(00)00194-0
  16. Hu, W., Wu, G.P. (1999) The lead pollution level in particulate of the four cities in China. Environmental Monitoring in China 15, 5-7.
  17. Hwang, H.-J., Ro, C.-U. (2006) Single-particle characterization of municipal solid waste (MSW) ash particles using low-Z particle electron probe X-ray microanalysis. Atmospheric Environment 40, 2873-2881. https://doi.org/10.1016/j.atmosenv.2006.01.004
  18. Ishizaka, T., Tohno, S., Ma, C.-J., Morikawa, A., Takaoka, M., Nishiyama, F., Yamamoto, K. (2009) Reactivity between $PbSO_4\;and\;CaCO_3$ particles relevant to the modification of mineral particles and chemical forms of Pb in particles sampled at two remote sites during an Asian dust event. Atmospheric Environment 43, 2550-2560. https://doi.org/10.1016/j.atmosenv.2009.02.041
  19. Jung, H.-J., Malek, M.A., Ryu, J., Kim, B., Song, Y.-C., Kim, H., Ro, C.-U. (2010) Speciation of individual mineral particles of micrometer size by the combined use of attenuated total reflectance-fourier transform-infrared imaging and quantitative energy-dispersive electron probe X-ray microanalysis techniques. Analytical Chemistry 82, 6193-6202. https://doi.org/10.1021/ac101006h
  20. Kim, B., Jung, H.-J., Song, Y.-C., Lee, M., Kim, H., Kim, J., Sohn, J., Ro, C.-U. (2010) Characterization of Summertime Aerosol Particles Collected at Subway Stations in Seoul, Korea Using Low-Z Particle Electron Probe X-ray Microanalysis. Asian Journal of Atmospheric Environment 4, 97-105. https://doi.org/10.5572/ajae.2010.4.2.097
  21. Kim, H., Ro, C.-U. (2010) Characterization of Individual Atmospheric Aerosols Using Quantitative Energy Dispersive-Electron Probe X-ray Microanalysis: A Review. Asian Journal of Atmospheric Environment 4, 115-140. https://doi.org/10.5572/ajae.2010.4.3.115
  22. Li, Q.-H., Guo, X.-Y., Xiao, S.-W., Huang, K., Zhang, D.-M. (2003) Life cycle inventory analysis of $CO_2\;and\;SO_2$ emission of imperial smelting process for Pb-Zn smelter. Journal of Central South University of Technology 10, 108-112. https://doi.org/10.1007/s11771-003-0049-z
  23. Londahl, J., Massling, A., Pagels, J., Swietlicki, E., Vaclavik, E., Loft, S. (2007) Size-resolved respiratory-tract deposition of fine and ultrafine hydrophobic and hygroscopic aerosol particles during rest and exercise. Inhalation Toxicology 19, 109-116. https://doi.org/10.1080/08958370601051677
  24. Maskey, S., Kang, T., Jung, H.-J., Ro, C.-U. (2011) Single-particle characterization of indoor aerosol particles collected at an underground shopping area in Seoul, Korea. Indoor Air 21, 12-24. https://doi.org/10.1111/j.1600-0668.2010.00677.x
  25. Mattielli, N., Petit, J., Deboudt, K., Flament, P., Perdrix, E., Taillez, A., Rimetz-Planchon, J., Weis, D. (2009) Zn isotope study of atmospheric emissions and dry depositions within a 5 km radius of a Pb-Zn refinery. Atmospheric Environment 43, 1265-1272. https://doi.org/10.1016/j.atmosenv.2008.11.030
  26. Murphy, D., Hudson, P., Cziczo, D., Gallavardin, S., Froyd, K., Johnston, M., Middlebrook1, A., Reinard, M., Thomson, D., Thornberry, T., Wexler, A. (2007) Distribution of lead in single atmospheric particles. Atmospheric Chemistry and Physics 7, 3195-3210. https://doi.org/10.5194/acp-7-3195-2007
  27. Nemmar, A., Hoet, P.H.M., Vanquickenborne, B., Dinsdale, D., Thomeer, M., Hoylaerts, M.F., Vanbilloen, H., Mortelmans, L., Nemery, B. (2002) Passage of inhaled particles into the blood circulation in humans. Circulation 105, 411-414. https://doi.org/10.1161/hc0402.104118
  28. Oberdorster, G. (2001) Pulmonary effects of inhaled ultrafine particles. International Archives of Occupational and Environmental Health 74, 1-8.
  29. Papanikolaou, N.C., Hatzidaki, E.G., Belivanis, S., Tzanakakis, G.N., Tsatsakis, A.M. (2005) Lead toxicity update: a brief review. Medical Science Monitor 11, RA329-RA336.
  30. Ro, C.-U., Kim, H., VanGrieken, R. (2004) An Expert System for Chemical Speciation of Individual Particles Using Low-Z Particle Electron Probe X-ray Microanalysis Data. Analytical Chemistry 76, 1322-1327. https://doi.org/10.1021/ac035149i
  31. Ro, C.-U., Oh, K.-Y., Kim, H., Chun, Y.-S., Osan, J., de Hoog, J., Van Grieken, R. (2001) Chemical speciation of individual atmospheric particles using low-Z electron probe X-ray microanalysis: characterizing "Asian Dust" deposited with rainwater in Seoul, Korea. Atmospheric Environment 35, 4995-5005. https://doi.org/10.1016/S1352-2310(01)00287-4
  32. Ro, C.-U., Osan, J., Szaloki, I., de Hoog, J., Worobiec, A., Van Grieken, R. (2003) A Monte Carlo Program for Quantitative Electron induced X-ray Analysis of Individual Particles. Analytical Chemistry 75, 851-859. https://doi.org/10.1021/ac025973r
  33. Ro, C.-U., Osan, J., Szaloki, I., Van Grieken, R. (2000) Determination of Chemical Species in Individual Aerosol Particles Using Ultra-thin Window EPMA. Environmental Science and Technology 34, 3023-3030. https://doi.org/10.1021/es9910661
  34. Ro, C.-U., Osan, J., Van Grieken, R. (1999) Determination of Low-Z Elements in Individual Environmental Particles Using Window less EPMA. Analytical Chemistry 71, 1521-1528. https://doi.org/10.1021/ac981070f
  35. Schwartz, J. (2001) Air Pollution and Blood Markers of Cardiovascular Risk. Environmental Health Perspectives 109, 405-409. https://doi.org/10.1289/ehp.01109s3405
  36. Seaton, A., MacNee, W., Donaldson, K., Goddon, D. (1995) Particulate air pollution and acute health effects. The Lancet 345, 176-178. https://doi.org/10.1016/S0140-6736(95)90173-6
  37. Seinfeld, J. (1986) Atmospheric Chemistry of Air Pollution. Wiley, New York.
  38. Sobanska, S., Ricq, N., Laboudigue, A., Guillermo, R., Bremard, C., Laureyns, J., Merlin, J.C., Wignacourt, P.J. (1999) Microchemical Investigations of Dust Emitted by a Lead Smelter. Environmental Science and Technology 33, 1334-1339. https://doi.org/10.1021/es9805270
  39. Speiser, C., Baumann, T., Niessner, R. (2000) Morphological and Chemical Characterization of Calcium-Hydrate Phases Formed in Alteration Processes of Deposited Municipal Solid Waste Incinerator Bottom Ash. Environmental Science and Technology 34, 5030-5037. https://doi.org/10.1021/es990739c
  40. Sun, Y., Zhuanga, G., Zhanga, W., Wang, Y., Zhuang, Y. (2006) Characteristics and sources of lead pollution after phasing out leaded gasoline in Beijing. Atmospheric Environment 40, 2973-2985. https://doi.org/10.1016/j.atmosenv.2005.12.032
  41. Tan, M., Zhang, G., Li, X., Zhang, Y., Yue, W., Chen, J., Wang, Y., Li, A., Li, T., Zhang, Y., Shan, Z. (2006) Comprehensive Study of Lead Pollution in Shanghai by Multiple Techniques. Analytical Chemistry 78, 8044-8050. https://doi.org/10.1021/ac061365q
  42. Vekemans, B., Janssens, K., Vincze, L., Adams, F., Van Espen, P. (1994) Analysis of X-ray spectra by iterative least squares (AXIL): new developments. X-Ray Spectrometry 23, 278-285. https://doi.org/10.1002/xrs.1300230609
  43. Wang, J., Guo, P., Li, X., Zhu, J., Reinert, T., Heitmann, J., Spemann, D., Vogt, J., Flagmeyer, R.-H., Butz, T. (2000) Source Identification of Lead Pollution in the Atmosphere of Shanghai City by Analyzing Single Aerosol Particles (SAP). Environmental Science and Technology 34, 1900-1905. https://doi.org/10.1021/es9907818
  44. Wang, W., Liu, X.D., Zhao, L.W., Guo, D.F., Tian, X.D., Adams, F. (2006) Effectiveness of leaded petrol phase-out in Tianjin, China based on the aerosol lead concentration and isotope abundance ratio. Science of the Total Environment 364, 175-187. https://doi.org/10.1016/j.scitotenv.2005.07.002
  45. Wang, X., Sato, T., Xing, B. (2006) Size distribution and anthropogenic sources apportionment of airborne trace metals in Kanazawa, Japan. Chemosphere 65, 2440-2448. https://doi.org/10.1016/j.chemosphere.2006.04.050
  46. Widory, D., Liu, X.D., Dong, S.P. (2010) Isotopes as tracers of sources of lead and strontium in aerosols (TSP & $PM_{2.5}$) in Beijing. Atmospheric Environment 44, 3679-3687. https://doi.org/10.1016/j.atmosenv.2010.06.036
  47. Winneke, G., Brockhaus, A., Ewers, U., Neuf, M., Kramer, U. (1990) Results from the European multicenter study on lead neurotoxicity in children: implications for risk assessment. Neurotoxicology and Teratology 12, 553-559. https://doi.org/10.1016/0892-0362(90)90022-5
  48. Xiao, R., Li, B., Yang, H.X., Zhang, Y.H., Liu, X.D., Liu, F., Li, Y.W. (2008) Source identification and apportionment study on particulate matter and aerosol lead in Beijing. Research of Environmental Sciences (Huanjing Kexue Yanjiu) 21(6), 148-155. (in Chinese with English abstract)
  49. Yule, W., Lansdown, R., Millar, I., Urbanowiez, M. (1981) The Relationship Between Blood Lead Concentration, Intelligence, and Attainment in a School Population: a Pilot Study. Developmental Medicine and Child Neurology 23, 567-576.
  50. Zhang, Y., Wanga, X., Chen, H., Yang, X., Chen, J., Allen, O. (2009) Source apportionment of lead-containing aerosol particles in Shanghai using single particle mass spectrometry. Chemosphere 74, 501-507. https://doi.org/10.1016/j.chemosphere.2008.10.004