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Sulfur, Oxygen, and Hydrogen Isotope Compositions of Precipitation in Seoul, South Korea

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Sulfur, Oxygen, and Hydrogen Isotope Compositions of Precipitation in Seoul, South Korea Geochemical Journal, Vol. 46, pp. 443 to 457, 2012 Sulfur, oxygen, and hydrogen isotope compositions of precipitation in Seoul, South Korea CHUNGWAN LIM,1 INSUNG LEE,1* SANG-MOOK LEE,1 JAE-YOUNG YU2 and ALAN J. KAUFMAN3 1School of Earth and Environmental Sciences, Seoul National University, Seoul 151-742, Korea 2Department of Geology, Kangwon National University, Chuncheon 200-701, Korea 3Department of Geology, University of Maryland, College Park, MD 20742-4211, U.S.A. (Received December 28, 2011; Accepted August 2, 2012) To evaluate the source of sulfur and the extent of seasonal and local characteristics in Seoul’s precipitation chemistry, we measured sulfur, oxygen, and hydrogen isotopic ratios of precipitation. The pH of precipitation ranges from 4.6 to 7.0 2+ 2+ 2– – in Seoul. Precipitation shows positive correlations between ions in the Ca –Mg –SO4 –NO3 system, indicating that the dissolution of Ca and Mg particles by H2SO4 and HNO3 from the combustion of fossil fuels is a major process control- ling the chemical composition of snow and rain. The values of oxygen and hydrogen isotope composition of rain range –15.7~–3.2‰ and –114.7~–18.0‰, respectively. The H and O isotope values in the summer are plotted near the global meteoric water line by Craig (1961). The d-excess values in winter are higher than 10, which indicate that the source of rain during winter is a dry air mass from continental China. The sulfur isotope ratio of precipitation in Seoul ranges from +3.0 to +7.3‰, which is similar to typical metropolitan air pollution levels. The data suggests that the main source of δ34 sulfur is SO2 produced by the combustion of fossil fuels. The pollutant SO4 is estimated to have a Snss range from +1.0 to +6.2‰ in the Seoul area. The δ34S values of precipitation range from +5.1 to +7.3‰ (mean +6.4‰) in winter and from +3.0 to 4.8‰ (mean +4.0‰) in summer. The higher δ34S values in winter (December and February) seem to be correlated to the air mass from northern China, of which the δ34S values of oil or coal is higher than that of southern China. The lower sulfur isotopic values in summer (June to August) are correlated to the air mass moving from southern China. Isotopic composition and chemical concentrations of SO4 depend on wind provenance, thus supporting the idea that a seasonally transported source for the pollutant sulfur is from China. Keywords: sulfur isotope, oxygen, hydrogen, pollution, precipitation, sulfate, Korea, East Asia fuel combustion in industrialized and heavily populated INTRODUCTION regions. Potential sources of sulfur oxides include: oil- The chemistry of acidic precipitation worldwide has refinery operations, oil- or coal-based power generation, been intensively studied for the past several decades. Acid automobile combustion, and other oil- or coal-reliant fa- rain is known to cause serious environmental damage in cilities. On the other hand, major ion distributions in pre- sensitive environments (Ayers and Yeung, 1996; cipitation are primarily controlled by contributions from Kulshrestha et al., 2003; Lee et al., 2000; Das et al., 2005; marine (sea-salt aerosols), terrestrial (soil dust, biologic Cape and Leith, 2002; Andronache, 2004; Zunckel et al., emissions) and anthropogenic (industrial, biomass burn- 2003; Yamaguchi et al., 1991). The increase of fossil fuel ing, vehicle emissions, and others) sources (Junge, 1963; burning in east Asian countries has likely intensified acid Nakai and Takeuchi, 1975). rain in east Asian countries including Korea, China, Ja- SO2, which is mainly produced by anthropogenic ac- 2– pan, and Russia (Lee et al., 2000; Park et al., 2000; Chun tivities, undergoes oxidation to form SO4 and the reac- et al., 2000; Park and Cho, 1998), while there are consid- tion is enhanced by metallic ions in urban atmospheres erable contributions of sulfur from Yellow sand (Asian (Newman et al., 1991). However, substantial amounts of 2– dust) from the inland of the continent. atmospheric SO4 arise from sea spray in coastal areas 34 32 Sulfur oxides mainly as SO2 are among the major pre- as well (Nielsen, 1978). The abundance of S/ S ratios 2– cursors of acid rain, and they are released through fossil in snow and rainwater derived from SO4 bearing pre- cipitation may be used to delineate anthropogenic S in the atmosphere, provided that the isotopic composition of pollutant S is distinct from S originating from natural *Corresponding author (e-mail: [email protected]) sources. Sulfur isotopes have been widely used to inter- Copyright © 2012 by The Geochemical Society of Japan. pret substances’ origins, forming conditions, and envi- 443 ronmental alterations (Mizutani and Rafter, 1969; Nakai and Takeuchi, 1975; Nissenbaum, 1978; Nriagu et al., 1987; Ohizumi et al., 1991; Yu and Park, 2004). Also, there is a distinct difference in the sulfur isotope ratios of fossil fuels such as coal and petroleum. Sulfur isotope fractionation is also demonstrated by Hong et al. (1992) and Maruyama et al. (2000) through their combustion experiments. Sulfur exists in small amounts in the atmos- phere, but when anthropogenic sources of sulfur that cause air pollution are introduced, the atmospheric sulfur iso- topic chemistry changes in a very subtle manner. Because of this phenomenon, a study on the sulfur isotope ratio of sulfate ions in precipitation is considered a useful method in tracking the source and distribution cycle of air pollut- ants. Thus the sulfur isotopic and major element composi- tion of rainwater along with meteorological information can be used to trace the sources of sulfur in precipitation, and to evaluate contributions from different sources (Krouse, 1980; Krouse and Case, 1981; Na et al., 1995; Yu and Park, 2004). In this case variation among sources must be isotopically significant and changes in isotopic composition during transport and transformation must be trivial. Additional information on both sources and mix- ing phenomena can be obtained by combining concentra- tion and isotopic composition data with meteorological Fig. 1. Map of the sampling location of study area (black cir- parameters (e.g., wind direction, temperature etc.). Iso- cle; in Seoul) and reference area (open triangle; Chuncheon topic studies on water samples in Korea have been made by Yu and Park, 2004 and open rectangular; Chonju by Na et for oxygen and hydrogen isotopic compositions of pre- al., 1995). cipitation in Taejeon and Seoul (Lee and Chang, 1994) and Cheju Island (Lee et al., 1997); studies have also been made for isotopic compositions in ground water (Na et forming process whereas the position of any point on the al., 1995) for sulfur, oxygen, and hydrogen isotopes of slope = 8 line is determined by the rainout process acid mine drainage (Yu and Coleman, 2000). Data on (Dansgaard, 1964). These measurements could potentially sulfur isotope compositions of precipitation in Korea are provide a means for determining the relative importance very rare. of different air masses for summer and winter precipita- The oxygen and hydrogen isotopic compositions of tion (Epstein and Mayeda, 1953; Craig, 1961; Dansgaard, precipitation in natural waters are governed by tempera- 1964; Lee and Lee, 1999). In this study the isotopic ra- ture, evaporation, and condensation. Deuterium excess (d) tios of sulfur, hydrogen and oxygen of wet depositions in is a second order parameter derived from δD and δ18O Seoul, Korea are determined through the analyses of snow values. Deuterium excess reflects the different sensitivi- and rainwater to distinguish between different precipita- ties of these isotopes to kinetic effects in the hydrologic tion events and their associated meteorological conditions. cycle. Theory predicts that deuterium excess responds The purpose of this research is to characterize the pre- primarily to changes in sea surface temperature (SST), cipitation chemistry of the Seoul area, namely for sulfur, humidity, and wind speed at the moisture source oxygen, and hydrogen isotope compositions, and to evalu- (Dansgaard, 1964). The value of deuterium excess is de- ate the source of sulfur and the extent of seasonal and termined from the equation as d = δD – 8δ18O. The val- local characteristics of snow and rain. This data will pro- ues of deuterium excess of any sample can be interpreted vide a context for potential solutions to environmental as the intercept with the δD axis (for δ18O = 0) of the line problems in East Asia. The present work deals with ur- with slope ∆δD/∆δ18O = 8 which passes through that ban atmospheric conditions in Seoul, a very densely popu- point; such a line presumably would be the locus of all lated city in Korea, surrounded by a wide and crowded precipitation samples which are derived from that par- industrial belt. Consequently air pollution poses a poten- ticular air mass by rainout; as will be discussed, the “d- tial problem to environment. For this reason, a system- parameter” according to this view relates to the vapor- atic chemical and isotopic study was undertaken to quan- 444 C. Lim et al. Table 1. The general weather conditions of precipitation in Seoul Date (dd-mm-yy) Precipitation type (season) Direction Velocity (m/s) Precipitation (mm) T (°C) pH EC (µS/cm) Condition 16-Dec-00 Snow (Wt) NW 1.5 5.4 −0.6 4.92 16.3 24-Dec-00 Snow (Wt) NW 2.2 13.9 −2.2 4.87 7.53 1-Jan-01 Snow (Wt) NW 3.7 21.7 0.4 5.07 5.92 Heavy snowfall 27-Jan-01 Snow (Wt) NW 3.6 1.9 0.0 4.95 72.2 Yellow sand 9-Feb-01 Snow (Wt) W 2.6 0.2 −0.9 5.87 6.79 15-Feb-01 Snow (Wt) NE 3.2 23.4 3.4 6.17 18.1
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