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Nitrogen (N) pollution of water courses is a major concern in most coastal watersheds in eastern China with intensive agricultural production. We use hydrogeological and dual-isotopic approaches to analyze the N concentrations, pollution, transformations, and sources of surface water and groundwater in an agricultural watershed of the Jiaozhou Bay (JZB) area. Results showed that dissolved total N (DTN) concentrations in sub-rivers (SRs) ranged from 6.0 to 25.3 mg N L -1 in the dry season and 9.1-26.7 mg N L -1 in the wet season, which indicated a positive relationship with the percentages of agricultural land. Meanwhile, the dominant dissolved N species in SRs changed from nitrate (NO 3 - , 64-100%) to dissolved organic N (DON, 52-77%) from the dry season to the wet season and the increased DON concentrations showed a positive relationship with the planted proportions of vegetable production systems. The NO 3 - concentrations of groundwaters ranged from 10.6 to 121.4 mg N L -1 , which were over the limit for drinking water by the World Health Organization. Isotopic analysis indicated that most NO 3 - originated from the microbiological conversion via nitrification, whereas the deletion of denitrification was insignificant in this area. The results of the stable isotope analysis in R mixing model showed the contributions of potential NO 3 - sources which were in order of manure fertilizers (20.6-69.0%) > soil organic matter (19.5-53.2%) > chemical fertilizers (5.5-34.3%) > atmospheric deposition (1.3-18.8%). This study suggests that the management of crop productions and reasonable manure fertilizer application should be implemented to protect the quality of aquatic systems in the JZB area.

Due to serious nitrogen pollution in the Huai River, Eastern China, nitrogenous concentrations and dual stable isotopes (δ 15 N and δ 18 O) were measured to ascertain the sources and transformation of nitrogen in the Shaying River, the largest and most polluted tributary of the Huai River during the summer and winter seasons. Total nitrogen (TN), NO 3 - , and NH 4 + were significantly higher in winter, with values of 7.84 ± 3.44 mg L -1 , 2.31 ± 0.81 mg L -1 , and 3.00 ± 2.24 mg L -1 , respectively, while the highest nitrogen compounds occurred in the Jialu River, one of the tributaries of the Shaying River, in both summer and winter. Isotope characteristics of nitrate reveal that manure and sewage were the principal nitrate sources in both summer (62.44 ± 19.66%) and winter (67.33 ± 15.45%), followed by soil organic nitrogen, with 24.94 ± 15.52% in summer and 26.33 ± 9.45% in winter. Values of δ 15 N-suspended particulate nitrogen (SPN) ranged from 0.78 to 13.51%, revealing that point source from industrial and domestic sewage accounted for the largest input to SPN at most sites, whereas soil organic nitrogen and agricultural fertilizers were found in the Jialu River in both sampling periods. Point sources from septic/manure and household waste were the main contributors to ammonium in most river water samples in both summer and winter; most wastewater discharged into the river was untreated, which was one of the main reasons for the high level of ammonium in winter. Nitrogen pollution and the dams had an effect on N transformation in the river. Significant assimilation of NH 4 + and aerobic denitrification competed for NH 4 + , resulting in the weakness of nitrification in the summer. Denitrification was also an important process of nitrate removal during the summer, whereas nitrification was a key N transformation process in the river in the winter time. To reduce nitrogen pollution and improve water quality, greater effort should be focused on the management of sources from urban input as well as on the improvement in sewage treatment.

Natural steroid hormones in the aquatic environment have attracted increasing attention because of their strong endocrine disrupting potency. Seven steroid hormones (estrone, 17α-estradiol, 17β-estradiol, estriol, testosterone, androstenedione, and progesterone) were analyzed from surface water and sediment sampled from Chaohu Lake, its upstream rivers (the Hangbu River, Nanfei River, Shiwuli River, and Pai River), drainage from the adjacent farmland, and treated and untreated municipal sewage. Concentrations of the seven target steroid hormones ranged from below the detection limit (ND) to 69.5 ng L -1 in the water of Chaohu Lake and the upstream rivers. Three steroids-estrone, estriol, and 17α-estradiol-were found in relatively high residual concentrations in the water, with maximum concentrations of 69.5 ng L -1 , 51.5 ng L -1 , and 23.3 ng L -1 , respectively. All of the target steroid hormones except estriol were detected in the sediment in concentrations of ND-16344 ng kg -1 . The dominant steroid hormone in the sediment of Chaohu Lake and the upstream rivers was 17α-estradiol. In the Shiwuli River and the Pai River, the dominant steroid hormones (estrone and estriol) were the same as those in the untreated municipal sewage. This confirmed the deduction that untreated municipal sewage was the major source of steroid hormone residues in these two rivers. The main steroid hormone in the water of the Hangbu River and Chaohu Lake was 17α-estradiol, the same as that in the farmland drainage. In addition, 17α-estradiol was verified as the major factor in the contribution of farmland drainage to the pollution in these rivers. The water in the Nanfei River had high concentrations of estriol and 17α-estradiol. This indicates that both untreated municipal sewage and farmland drainage were the major sources. The discharge of steroid hormones from the four rivers to Chaohu Lake was approximately 75.1 kg year -1 , with the highest contributor being 17α-estradiol (24 kg year -1 ). Therefore, based on the results of this study, the farmland drainage should be controlled to reduce the steroid hormone pollution in Chaohu Lake.

The Chaohu Lake is highly polluted and suffers from severe eutrophication. Nitrate is a key form of nitrogen that can cause water quality degradation. In this study, hydrochemical and dual isotopic approaches were utilized to identify the seasonal variation of nitrate sources in the Chaohu Lake and its inflowing rivers. The average nitrate concentrations ([NO 3 - ]) of the lake and its inflowing rivers were 89.9 and 140.8 μmol L -1 , respectively. The isotopic values of δ 15 N-NO 3 - and δ 18 O-NO 3 - in the lake ranged from - 1.01 to + 16.67‰ and from - 4.39 to + 22.20‰, respectively. The two major rivers had distinct isotopic compositions, with average δ 15 N-NO 3 - values of + 17.52 and + 3.51‰, and average δ 18 O-NO 3 - values of + 2.71 and + 7.47‰ for the Nanfei River and Hangbu River, respectively. The results show that soil organic ammonium and urban wastewater discharge were the main sources of nitrate in the Chaohu Lake, and nitrate assimilation was an important process affected [NO 3 - ] and isotopic compositions, especially in the western Chaohu Lake. The elevated [NO 3 - ] and δ 15 N-NO 3 - values in the western Chaohu Lake indicate the high influence of human activities. Urban wastewater discharge was the primary nitrate source in the Nanfei River and soil organic ammonium was the main source in the Hangbu River. Although nitrate from direct atmospheric deposition was low, its strong flushing effect can substantially improve riverine [NO 3 - ] and nitrate loading from terrestrial ecosystem. The relatively high nitrate fluxes from the Hangbu River indicate that nitrogen loading from agricultural watershed is unneglectable in watershed nitrogen sources reduction strategies.