Abstract
Sulfur dioxide and sulfate aerosols in the atmosphere are significant factors leading to acidification of the atmospheric environment and worsening the pollution of acid deposition. Because of the “fingerprint” characteristics of the stable sulfur isotopic composition, sulfur isotope has been widely adopted in environmental researches concerning sulfur cycle and source identification. In this study, the atmospheric environment of Jinhua City, central Zhejiang Province, was continuously monitored, and the sulfur isotopic composition of SO2 and sulfate aerosols in the atmosphere was analyzed. The results indicate that the variation of δ 34S values for SO2 ranges from 1.0‰ to 7.5‰, and annual average is 4.7‰±2.3‰, whereas that of sulfate aerosols ranges from 6.4‰ to 9.8‰, and annual average is 8.1‰±1.0‰. The δ 34S values for SO2 have significant seasonal variations, which are 7.0‰ in winter and 3.3‰ in summer. These variations cannot be attributed to a single factor, and we suggest a temperature-dependent isotope equilibrium fractionation and elevated biogenic sulfur emissions of isotopically light S in summer may be the main controlling mechanisms. Furthermore, we also discuss the δ 34S model of atmospheric SO2 oxidation to form sulfate, and suggest that heterogeneous oxidation dominates in the oxidation reactions of atmospheric SO2 in the central Zhejiang Province. We further suggest that the relative humidity in the atmosphere plays an important role in the oxidation mechanism of atmospheric SO2.
Similar content being viewed by others
References
Jamieson R E, Wadleigh M A. Tracing sources of precipitation sulfate in eastern Canada using stable isotopes and trace metals. J Geophy Res, 2000, 105: 20549–20556
Romero A B. Mass-independent sulfur isotopic compositions in atmospheric sulfates. Dissertation for Doctoral Degree. San Diego: University of California, 2003
Bao H M, Reheis M C. Multiple oxygen and sulfur isotopic analyses on water-soluble sulfate in bulk atmospheric deposition from the southwestern United States. J Geophy Res, 2003, 108: 4430–4438
Norman A L, Belzer W, Barrie L A. Insights into the biogenic contribution to total sulphate in aerosol and precipitation in the Fraser Valley afforded by isotopes of sulphur and oxygen. J Geophy Res, 2004, 109: 5311–5320
Tie X, Brasseur G P, Briegleb B, et al. Two-dimensional simulation of Pinatubo aerosol and its effect on stratospheric ozone. J Geophy Res, 1994, 99: 20545–20562
Adams P J, Seinfeld J H, Koch D M. Global concentrations of tropospheric sulfate, nitrate, and ammonium aerosol simulated in a general circulation model. J Geophy Res, 1999, 104: 13791–13823
Charlson R J, Schwartz S E, Hales J M, et al., Climate forcing by atmospheric aerosols. Science, 1992, 225: 423–430
Seinfeld, J H, Pandis S N. Atmospheric Chemistry and Physics: From Air Pollution to Climate Change. New York: John Wiley & Sons Inc, 1998
Haywood J, Boucher O. Estimates of the direct and indirect radiative forcing due to tropospheric aerosols: A review. Rev Geophy, 2000, 38: 513–543
IPCC. Climate Change 2001: The Scientific Basis: Contribution of Working Group I to the Third Assessment Report of the Intergovernment Panel on Climate Change. New York: Cambridge University Press, 2001
Zhang M Y. Environmental chemistry of acid deposition and sources attribution using sulfur isotopic compositions—A case study in the central region of Zhejiang Province. Dissertation for Doctoral Degree. Beijing: Graduate University of Chinese Academy of Sciences, 2006
Mukai H, Tanaka A, Fujii T, et al. Regional characteristics of sulfur and lead isotope ratios in the atmosphere at several Chinese urban sites. Environ Sci Technol, 2001, 35: 1064–1071
Saltzman E, Brass G, Price D. The mechanism of sulphate aerosol formation: Chemical and sulphur isotopic evidence. Geophy Res Lett, 1983, 10: 513–516
Kawamura H, Matsuoka N, Tawaki S, et al. Sulfur isotope variations in atmospheric sulfur oxides, particulate matter and deposits collected at Kyushu island, Japan. Water Air Soil Pollut, 2001, 130: 1775–1780
Novak M, Jackova I, Prechova E. Temporal trends in the isotope signature of air-borne sulfur in Central Europe. Environ Sci Technol, 2001, 35: 255–260
Zhang H B, Chen Y W, Liu D P. Study on sulfur source of acid rain using sulfur isotopic trace (in Chinese). Geochimica, 1995, 24(Suppl): 126–133
Zhang H B, Hu A Q, Lu C Z, et al. Sulfur isotopic composition of acid deposition in South China regions and its environmental significance (in Chinese). China Environ Sci, 2002, 22: 165–169
Hong Y T, Zhang H B, Zhu Y X, et al. Sulfur isotopic characteristic of coal in China and sulfur isotopic fractionation during coal-burning process. Sci China Ser B, 1992, 22: 868–873
Hong Y T, Zhu Y X, Zhang H B, et al. Fractionation of sulfur isotopes during coal burning process and its environmental significance (in Chinese). Acta Sci Circums, 1993, 13: 240–243
Liu G S, Hong Y T, Piao H C, et al. Study on sources of sulfur in atmospheric particulate matter with stable isotope method (in Chinese). China Environ Sci, 1996, 16: 426–429
Norman A L, Barrie L A, Toom-Sauntry D, et al. Sources of aerosol sulphate at Alert: Apportionment using stable isotopes. J Geophy Res, 1999, 104: 11619–11631
Nriagu J O, Coker R D. Isotopic composition of sulphur in precipitation within the Great Lakes basin. Tellus, 1978, 30: 365–375
Nriagu J O, Holdway D A, Coker R D. Biogenic sulphur and the acidity of rainfall in remote areas of Canada. Science, 1987, 237: 1189–1192
van Stempvoort D R, Wills J J, Fritz P. Aboveground vegetation effects on the deposition and cycling of atmospheric sulfur: Chemical and stable isotope evidence. Water Air Soil Pollut, 1991, 60: 55–82
Hong Y T, Zhang H B, Zhu Y X, et al. Characterics of sulphur isotopic composition of meteoric water in China. Prog Nat Sci, 1995, 5: 344–349
Caron F, Tessier A, Kramer J R, et al. Sulphur and oxygen isotopes of sulphate in precipitation and lake water, Quebec. Appl Geochem, 1986, 1: 601–606
Alewell C, Mitchell M J, Likens G E, et al. Assessing the origin of sulfate deposition at the Hubbard Brook Experimental Forest. J Environ Qual, 2000, 29: 759–767
Egiazarov A C, Kaviladze M N, Kerner E L, et al. Separation of sulfur isotopes by chemical exchange. Isotopenpraxis, 1971, 7: 379–383
Eriksen T E. Sulphur isotope effects I: The isotopic exchange coefficient for the sulphur isotopes 34S-32S in the system SO2-HSO3 at 25, 35 and 45°C. Acta Chimica Scand, 1972, 26: 573–580
Eriksen T E. Sulfur isotope effects II: The isotopic exchange coefficients for the sulfur isotopes 34S-32S in the system SO2 g-aqueous solutions of SO2. Acta Chim Scand, 1972, 26: 581–584
Tanaka N, Rye D M, Xiao Y T, et al. Use of stable sulfur isotope systematics for evaluating oxidation reaction pathways and in-cloudscavenging of sulfur dioxide in the atmosphere. Geophy Res Lett, 1994, 21: 1519–1522
Tang X Y. Atomospheric Environmental Chemistry. Beijing: Higher Education Press, 1992
Martin L R. Kinetics studies of sulfite oxidation in aqueous solution, in SO2, NO and NO2 oxidation mechanisms: Atmospheric consideration. In: Teasley J I, ed. Acid Precipitation Series. Boston: Butterworth Publishers, 1984. 66–100
Langner J, Rodhe H. A global three-dimensional model of the tropospheric sulfur cycle. J Atmos Chem, 1991, 13: 255–263
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Zhang, M., Wang, S., Ma, G. et al. Sulfur isotopic composition and source identification of atmospheric environment in central Zhejiang, China. Sci. China Earth Sci. 53, 1717–1725 (2010). https://doi.org/10.1007/s11430-010-4017-9
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11430-010-4017-9