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Degradation of Groundwater Quality Due to Anthropogenic Sulfur and Nitrogen Contamination in the Sichuan Basin, China

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Degradation of Groundwater Quality Due to Anthropogenic Sulfur and Nitrogen Contamination in the Sichuan Basin, China Geochemical Journal, Vol. 40, pp. 309 to 332, 2006 Degradation of groundwater quality due to anthropogenic sulfur and nitrogen contamination in the Sichuan Basin, China XIAO-DONG LI,1,2* HARUE MASUDA,1 MINORU KUSAKABE,3 FUMITAKA YANAGISAWA4 and HAI-AO ZENG2 1Department of Geosciences, Osaka City University, Sumiyoshi-ku, Osaka 558-8585, Japan 2Department of Environment and Civil Engineering, Chengdu University of Technology, Chengdu 610059, China 3Institute for Study of the Earth’s Interior, Okayama University, Misasa, Tottori 682-0193, Japan 4Department of Earth Sciences, Yamagata University, Kojirakawa-cho, Yamagata 990-8560, Japan (Received July 19, 2005; Accepted December 20, 2005) In this study we describe the degradation of groundwater quality in the Sichuan Basin, one of the most heavily popu- lated and industrialized areas in China. We analyzed the major element chemistry and stable isotopic ratios of H, O, and S from groundwater and surface-water samples collected from four cities along the Minjiang and Yangtze Rivers. On the basis of these data, we examined the sources and downstream variations in groundwater pollutants in relation to increas- ing human activity in the basin. 2+ – – Ca and HCO3 were the dominant ions within groundwater analyzed in this study, although the proportions of Cl and 2– – SO4 + NO3 progressively increased from the source area downstream along the Minjiang River to the Yangtze River. The degradation of groundwater quality was due to anthropogenic sulfur and nitrogen contamination within the basin. Sulfate δ34S values indicated that the primary source of sulfur in contaminated groundwater was air pollutants derived mainly from the combustion of coal, while contamination by household detergents and industrial waste acted to increase 2– 2– SO4 concentrations further downstream. Fertilizer also contributed to elevated SO4 concentrations; however, the area affected by fertilizer contamination was small in comparison with the area affected by other pollutant sources. Keywords: Sichuan Basin, sulfate and nitrate ions, sulfur isotopes, groundwater pollution, pollutant sources tion of soluble SO 2– and S2– minerals in sedimentary INTRODUCTION 4 rocks, residential waste, and atmospheric, industrial and The Sichuan Basin, southwestern China, is one of the agricultural sources. The sulfur isotopic composition of 2– most heavily populated and intensely industrialized ar- SO4 in water reflects the isotopic composition of the eas in China and faces serious environmental pollution sulfur source and can therefore be used to differentiate 2– problems (Streets and Waldhoff, 2000). The basin repre- between naturally occurring SO4 and that derived from sents about 2% of the total area of China and contains human activities. On this basis, researchers in Europe and >10% of the national population, which is concentrated America have carried out extensive investigations into 2– in the large cities of Chengdu, Leshan, Yibin, Luzhou, the sulfur isotopic composition of environmental SO4 and Chongqing located along the Minjiang and Yangtze (e.g., Stam et al., 1992; Novak et al., 1996; Ingri et al., Rivers (Fig. 1). Waste discharge from residents, industry, 1997; Yang et al., 1997; Pichlmayer et al., 1998; and agriculture results in direct contamination of local Moncaster et al., 2000). Similar investigations in East Asia groundwater and surface-water systems in this overpopu- are relatively rare (Ohizumi et al., 1997; Dai et al., 2002; lated region. Rapid economic growth and increasing en- Xiao and Liu, 2002; Yu and Park, 2004). ergy demands have led to severe air pollution resulting in In our previous study, we used sulfur isotope ratios to acid depositions related to the large amount of coal con- identify the pollutant sources of groundwater in the source sumed in the basin. The acid depositions, mainly sulfur area of the Minjiang River and the densely populated city and nitrogen oxides, also indirectly degrade the quality of Dujiangyan located alongside the upper reaches of the of groundwater and surface-water. river (Li et al., 2006). The results of this earlier study Sulfate is a ubiquitous component of groundwater, and demonstrated that the source area of the Minjiang River is derived from a variety of sources such as the dissolu- (indicated in Fig. 1) was relatively pollution-free, as there were no industrial plants located close to the source area. 2– – SO4 and NO3 -N concentrations in groundwater in this *Corresponding author (e-mail: [email protected]) area were generally very low (<10 mg/L and <1 mg/L, Copyright © 2006 by The Geochemical Society of Japan. respectively), and high concentrations of those compo- 309 Fig. 1. Location map of the study area and sketch map of sampling sites within the Sichuan Basin, China. The dotted line denotes the bottom of Sichuan Basin (200–450 m); the dashed line contours the watershed, the black line, added the open triangle with mentioned height (m) for the main mountain peak. The open circle denotes the center of the city; the cross represents the river water sampling site and the solid star for the rainwater sampling site. The arrow (in the sketch map) indicates the directions of river flow. nents were only recorded in groundwater from the center basin. The quality of groundwater and surface-water is of Chuanzhusi Town and Songpan County. The polluted worsening over time (SEPA, 2005). wells recorded δ34S values of +6.0 to +9.1‰, suggesting To examine the sources of groundwater pollutants and groundwater contamination by household wastewater. At downstream variation in pollutants in relation to increas- 2– – the Dujiangyan site, SO4 and NO3 -N concentrations in ing human activities in the basin, in the present study we groundwater were higher (20–50 mg/L and 2–10 mg/L analyzed the major element chemistry and stable isotopic δ34 2– respectively); the overlapping values of S from SO4 ratios of H, O and S for groundwater and surface-water in rainwater and groundwater (δ34S, +1.5 to +6.0‰) in- sampled from four cities along the Minjiang and Yangtze 2– dicated that the SO4 was mostly derived from the air Rivers within the Sichuan Basin. We also determined the – pollutants. The high concentrations of NO3 -N in the same sulfur isotopic ratios of local rainwater, coal, chemical samples provided additional evidence that the contami- fertilizer, and domestic detergent to compare with values nation originated largely from air pollutants that were from groundwater and identify the pollutant sources. emitted into the atmosphere from within the basin. Downstream of Dujiangyan, toward the center of the GEOLOGICAL AND GEOGRAPHICAL SETTING AND Sichuan Basin, domestic, industrial and agricultural ac- SAMPLE LOCATIONS tivity becomes progressively more intensive. Accordingly, anthropogenic pollutants discharged from these activities The Sichuan Basin is an intracratonic sedimentary place greater pressure on environment preservation in the basin (Zhou et al., 1997) filled with a 5–11 km thickness 310 X.-d. Li et al. of Sinian to Cretaceous sedimentary formations. Forma- ples were stored in two bottles: one of which was acidi- tions of late Sinian and Cambrian age are cyclic carbon- fied with 1:1 HCl (for the analysis of cations) and one ate-evaporites, while limestone is the main rock of the that was untreated (for the analysis of anions, hydrogen, Ordovician, Devonian, and Permian Systems. Cyclic car- and oxygen isotopes). An additional aliquot of 1~2 L of bonate-evaporite sediments dominate the Carboniferous water was sampled, to which 10~20 mL of 1:1 HCl was and Lower and Middle Triassic formations. Only Permian added for preparation for S isotope analysis; the sample and Lower and Middle Triassic formations are continu- was filtrated later in the laboratory. ous across the basin. Upper Triassic formations consist Samples of locally consumed coal, fertilizer, and do- of interbedded sandstone and shale, which were depos- mestic detergents were also collected at the four sampling ited in a continental environment. The overlying Jurassic sites. The sampled fertilizers were ammonium bicarbo- and Cretaceous Systems are continental redbeds and nate (NH4HCO3), carbamide (CO(NH2)2), and superphos- mudstone interbedded with sandstone (Zhou and Li, phate (Ca(H2PO4)2·H2O + CaSO4), all of which are com- 1992). monly used in local areas. The Yangtze River flows along the western and south- ern margins of the basin (Fig. 1), while the Daduhe River Analytical methods flows through the northwest of the basin to join the Immediately following sampling, we measured water Minjiang River at Leshan City. The Minjiang and pH, DO, EC in the field using 6066-10C, 9551-20D and Jinshajiang Rivers join the Yangtze River at Yibin City. 9382-10D HORIBA electrodes, respectively. Ground- The Tuojiang River flows from north to south within the water temperature was measured simultaneously by each – basin, and joins the Yangtze River at Luzhou City. electrode. Alkalinity (counted as HCO3 ) was determined Average annual temperatures within the cities of in the field by titration with hydrochloric acid. Ca2+ and Leshan, Yibin, Luzhou, and Chongqing are in the range Mg2+ concentrations were determined in the laboratory 16.0 to 18.0°C, while annual precipitation is 1,000–1,200 by EDTA titration. Na+ and K+ were analyzed by atomic mm, concentrated in the summer months of May to Sep- absorption spectrophotometry (SAS7500, Seiko Instru- – – – – 3– 2– tember (National Climatic Data Center, 2003). Fertile soils ments),
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