Supplementary Information Description of sampling sites Twenty groundwater wells in Taipei and Hsinchu respectively belonging to sedimentary basin and alluvial plains were selected for monitoring and sample collection. Taipei basin is a flat terrain (elevation at high altitude 20 meters below), and it covers an area of about 380 square kilometers. The sediments are mostly from the Danshui River that Keelung, Sindian and Dahan River are the three main tributaries. Western Foothills belt and snowy mountains are the main source of the basin sediments. Four major aquifers corresponding to the stratigraphic formations have been defined in the late-Quaternary sediments of the Taipei Basin. The topmost free aquifer (Aquifer 0), which extends from ground surface to depth around 50 m (except in the western edge of the basin being deeper to about 120 m in maximum), is composed of interbedded clay, sand and pebbles. The confined Aquifer 1 sits at depth between 50 to around 100 m (again except in the western edge of basin, about 115–140 m) in the conglomerate layer covered by laterite. Rainfall is the major water source for Aquifer 0 and The lower aquifers (Aquifers 2 and 3) are present approximately 100 to 130 m and 140 to 160 m underground (depths for the central portion of the basin), as two layers of conglomerates within the Wuku and Banchiao formations, respectively. Aquifer 1 is the major groundwater source of the pumping wells in the Taipei Basin. The groundwater of the lower three aquifers comes mainly from two of the major rivers in the Taipei Basin, the Xindian River and the Dahan River. (Water Resources Agency, Ministry of Economic Affairs, Taiwan; Chen et al. 2007) The Hsinchu-Miaoli Groundwater District is located in northwestern Taiwan and covers an area of about 900 square kilometers. This region of complex terrain containing a number of folds and faults comprises hills and cutting valleys. This area with varies characteristics cause uncertainty of the aquifer stratification. It is composed of stacked layers and Quaternary with texture specified by alternating coarse sand/gravel and fine silt/clay, which are the major groundwater reserves. The Hsinchu-Miaoli Groundwater District is divided into small sub-districts with areas of only tens of square kilometers. These groundwater sub-districts are usually composed of folded Pleistocene aquifers in the central part and are unconformably underlain by Holocene aquifers on the boundaries. Since the Pleistocene aquifers are significantly higher in altitude, groundwater preferably infiltrates from the Pleistocene aquifers to the Holocene aquifers and is finally drained by the river system. Precipitation is naturally regarded as an important source of the Hsinchu-Miaoli groundwater. (Water Resources Agency, Ministry of Economic Affairs, Taiwan; Lu et al. 2006) Table S1 The monitoring data of sampling wells. Sampling well A1 Taipei City Sampling depth (m) 5.90-6.30 A2 Taipei City 7.70-7.80 25-26.7 6.1-6.3 177-258 8.6-9.1 0.46 0.02 7.7-12.2 A4 Taipei City 4.40-7.00 23.4-25.6 7.3-7.4 317-369 7.3-13.4 0.02-0.06 0.47-2.34 19.4-26.6 A8 Taipei City 5.30 23.4 6.5 596 17.0-20.7 0.05-0.13 0.02-0.05 44.3-63.8 A9 Taipei City 7.10 24.8 6.5 381 3.8-8.9 0.01-0.02 0.38-0.58 19.3-23.6 A11 Taipei City 9.00-9.10 25.6-25.8 7.1 945-1052 54.8-56.6 0.02-0.44 0.19-0.38 92.9-93.7 A12 Taipei City 4.50-5.00 24.3-26.9 6.4-6.5 318-376 29.3-29.6 0.03-0.51 0.36-0.83 13.7-42.5 A14 Taipei City 6.20 23.7 6.3 546 24.5-37.8 9.47-10.2 10.6-21.20 25.7-30.1 A17 Taipei City 9.20-9.30 26.2-30.7 6.0 236-252 7.3-23.2 0.24-0.71 0.01-1.13 14.6-31.0 F10 Taipei County 5.50 26.4 6.8 903 25.6-36.6 1.67-1.94 0.12 29.8-57.8 F17 Taipei County 6.30-7.00 25.1-28.2 7.0 1234-1235 19.5-23.1 14.3-15.4 0.03 34.7-77.1 F24 Taipei County 12.10-13.60 24.7-26.2 6.6-6.7 150-649 11.6-15.0 0.01-0.10 4.77-5.02 23.7-24.0 F29 Taipei County 9.20-11.80 23.5-28.4 5.1-6.5 155-822 31.6-49.5 1.37 0.01 129-216 F162 Taipei County 4.00-4.10 23.4-28.5 6.3-6.6 1122-1211 140-179 0.05-0.13 0.01 90.2-98.5 O2 Hsinchu 5.00 20.1-28.4 5.9-7.2 603-1010 16.9-52.7 6.90-17.9 0.36-4.94 60.1-107 O5 Hsinchu 13.00 25.3 6.8 605 20.5-23.8 <0.01 0.02 55.4-80.1 O12 Hsinchu 5.10-9.70 23.4 6.8 371 12.7-15.0 <0.01 3.05-3.34 58.6-59.0 O14 O15 J2 Hsinchu Hsinchu Hsinchu 5.70-6.10 14.10 10.60 22.6-26.9 23.2 23.6 6.4-6.5 5.9 6.6 379-430 356 843 23.5-24.7 19.2-19.3 96.6-126 1.14-1.51 <0.01 0.02 1.94-4.12 2.51-2.52 <0.01 63.7-83.1 69.4-72.0 58.1-61.5 County/City 6.4-6.6 Specific conductance (μmho/cm) 308-760 Chloride (mg/L) 50.0-52.4 Ammonia nitrogen (mg/L) 0.03-0.20 Nitrate nitrogen (mg/L) 9.63-15.5 Temperature(℃) pH 23.7-25.4 Sulfate (mg/L) 23.5-24.7 Table S2 Concentrations of emerging contamination in monitoring wells (1/6). Concentration (ng/L) MDLs Sampling* A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 1 0.5±0.1 ND 3.8±0.6 0.1±0.0 ND ND 0.5±0.2 3.8±0.5 3.4±0.2 1.6±0.3 ND ND 1.8±0.1 ND 14.4±0.5 0.5±0.1 ND 1.1±0.1 ND ND 2 0.3±0.1 ND 2.9±0.1 - - ND 0.4±0.1 - 1.7±0.2 - ND ND ND ND 2.7±0.2 - - 5.5±0.1 - - 1 43.7±1.2 ND 6.7±0.4 ND 0.3±0.1 ND 0.7±0.3 6.3±0.2 ND ND ND 17.0±1.9 ND 0.2±0.1 1820±78.1 ND 2.4±0.3 42.4±3.7 0.4±0.1 0.5±0.1 2 298±20.6 ND 12.0±1.0 - - ND 0.7±0.3 - 0.3±0.2 - ND 21.1±1.1 ND 0.1±0.1 22.7±2.2 - - 57.7±4.0 - - 1 ND ND 0.7±0.0 ND ND ND ND 0.8±0.1 ND 1.7±0.2 ND ND ND ND ND 3.0±0.2 ND ND ND ND 2 ND ND 0.8±0.1 - - ND ND - ND - ND ND 1.0±0.3 ND ND - - 0.6±0.0 - - 1 ND ND 3.1±0.4 1.6±0.0 ND ND 5.1±0.2 8.4±1.3 25.0±1.4 28.9±0.2 1.8±0.3 ND 8.3±0.6 5.1±0.7 ND 3.4±0.2 ND 1.9±0.2 ND ND 2 0.3±0.1 1.2±0.1 1.7±0.1 - - 0.4±0.1 2.2±0.1 - 7.1±0.2 - 2.2±0.2 ND 7.6±0.3 6.1±0.3 ND - - 9.8±0.8 - - 1 ND ND ND ND ND ND ND 1.3±0.1 ND ND ND ND ND ND 1.8±0.3 ND ND 0.6±0.1 ND ND 2 0.8±0.1 ND ND - - ND ND - ND - ND ND ND ND 0.7±0.2 - - 1.5±0.2 - - 1 ND ND ND ND ND ND 0.8±0.1 4.3±0.3 ND ND ND ND 1.2±0.1 ND ND ND ND 1.2±0.1 ND ND 2 ND ND 1.5±0.1 - - ND 1.0±0.2 - ND - ND ND 0.8±0.1 ND ND - - 1.5±0.3 - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 54.8±0.9 ND ND ND ND ND 2 ND ND 2.2±1.6 - - ND ND - ND - ND ND ND ND 18.4±2.4 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 6.9±0.5 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND 12.5±0.8 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - Sulfonamide antibiotics Sulfadiazine 0.1 Sulfamethoxazole 0.1 Sulfathiazole 0.5 Sulfamethazine 0.1 Sulfamonomethoxine 0.5 Sulfadimethoxine 0.5 Macrolides antibiotics Erythromycin-H2O Clarithromycin Roxithromycin Tylosin 0.1 0.5 0.5 1.0 * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S2 Concentrations of emerging contamination in monitoring wells (2/6). Concentration (ng/L) A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 1 ND ND 2.9±0.1 ND ND ND ND ND ND 1.6±0.0 3.2±0.1 ND ND ND 16.4±1.1 ND ND ND ND ND 2 4.0±0.2 ND 1.6±0.5 - - ND ND - ND - ND ND ND ND 14.3±0.6 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND 2.4±0.1 ND 4.1±0.4 ND 6.6±0.3 ND ND ND ND ND 2 1.0±0.2 ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 10.2±0.7 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND 2.6±0.8 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 9.3±0.9 ND ND ND ND ND 2 2.8±1.1 ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 1.6±1.1 ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND 0.9±0.4 ND ND ND ND ND ND ND 11.8±1.0 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND 7.9±1.3 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 1.8±0.5 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 26.2±1.3 ND ND ND ND ND 2 ND ND 4.9±6.7 - - ND ND - ND - ND ND ND ND 35.6±59.5 - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - 5.4±1.6 ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 3.6±0.7 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 7.8±0.5 ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND 0.7±0.4 ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - MDLs Sampling* 1.0 Quinolone antibiotics Nalidixic acid Flumequine 0.5 Pipemidic acid 1.0 Norfloxacin 1.0 Ciprofloxacin 0.5 Ofloxacin 0.5 Imidazole antibiotics Dimetridazole Metronidazole 0.5 0.5 β-blockers Propranolol 0.6 Atenolol 1.2 Metoprolol 0.6 Acebutolol 0.6 Sotalol 0.5 * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S2 Concentrations of emerging contamination in monitoring wells (3/6). Concentration (ng/L) MDLs Sampling * A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 0.1 1 ND 8.4±0.3 6.5±0.5 ND 24.7±0. 9 29.1±1. 2 1.3±0.0 2.0±0.2 24.3±1. 9 ND ND 7.0±0.8 ND 0.9±0.1 1036±5 5.7 ND 3.2±0.4 2.0±0.7 2.2±0.3 1.2±2.1 2 ND ND ND - - ND ND - ND - ND 2.1±2.6 ND ND ND - - ND - - 1 ND 17.4±0. 8 ND ND ND ND ND ND ND ND 222±20 .8 ND 83.2±4. 3 ND 837±29 .3 ND ND ND ND ND 2 7.0±1.1 7.8±1.0 ND - - ND ND - - ND ND - - ND - - ND ND ND ND ND ND ND ND ND ND ND 53.2±2. 6 ND ND 1 251±1. 7 ND ND ND ND ND ND NSAIDs Acetaminophe n Ibuprofen 5 Naproxen 5 2 ND ND ND - - ND ND - ND - ND ND ND ND 75.8±2. 8 128±1. 0 ND - - ND - - Ketoprofen 5 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND Diclofenac 1 2 1 ND ND ND ND ND ND ND ND ND ND ND 3.5±0.1 ND ND ND ND ND ND ND ND ND ND ND ND 2.1±0.4 ND ND 8.1±0.8 ND ND - - ND ND - ND - ND ND ND 33.2±4. 9 13.9±1. 8 ND 2 ND 18.2±1. 2 6.6±2.3 - - ND - - ND ND 44.5±6. 5 7.4±1.2 ND ND ND ND 0.1±0.0 ND 0.2±0.3 ND ND ND ND ND ND ND ND 1.0±0.1 ND 172.3± 12.2 3.2±0.9 - - ND - - 257±24 .7 35.6±3. 2 ND ND ND 0.1±0.2 0.2±0.4 0.6±0.2 0.1±0.1 ND ND - - ND - - ND ND Lipid regulator and cholesterol lowering drug Clofibric acid 0.1 Gemfibrozil 0.1 Bezafibrate 0.1 1 2 1 ND ND 0.8±0.4 ND ND 0.1±0.1 ND ND ND ND 0.3±0.3 ND 0.4±0.2 ND ND 0.2±0.4 0.1±0.0 ND 0.1±0.1 ND 0.1±0.1 ND ND ND ND 0.3±0.1 ND ND 0.6±0.4 ND ND 0.1±0.0 2 ND ND - - ND ND - ND - ND ND 1 10.1±2. 8 ND ND ND 4.0±0.5 ND ND ND 0.2±0.1 ND 0.8±0.3 ND 0.2±0.0 2 ND ND ND - - ND ND - ND - ND ND * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S2 Concentrations of emerging contamination in monitoring wells (4/6). Concentration (ng/L) MDLs Sampling* A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 0.1 1 2 214±67.4 3.5±1.5 31.3±27.4 4.5±0.6 ND 9.3±0.7 ND - 15.2±4.0 - 12.8±18.0 2.3±2.1 ND 10.3±4.4 7.3±4.3 - 5.8±4.8 10.2±1.7 ND - ND 7.5±1.8 35.8±10.4 89.3±6.5 ND 5.5±0.6 ND 15.5±12.6 931±35.6 11.1±8.1 ND - 1.2±2.0 - ND 12.0±3.6 18.3±13.3 - ND - 0.1 1 2 4.1±0.3 19.8±0.6 ND ND 2.0±0.2 2.6±0.2 ND - ND - ND ND 0.9±0.0 1.4±0.0 37.9±0.5 - ND ND 0.5±0.1 - ND ND 5.5±0.7 3.4±0.1 1.8±0.2 2.6±0.2 ND ND 5.1±0.2 5.4±0.2 0.4±0.0 - ND - 9.5±0.3 14.7±0.6 ND - ND - 0.25 1 2 ND ND ND ND ND ND ND - ND - 0.7±0.4 ND ND ND 2.4±3.7 - ND ND ND - ND ND ND ND ND ND ND ND 0.4±0.1 ND ND - 0.4±0.7 - ND ND ND - ND - 1 1 2 ND 1.1±0.5 ND ND ND ND ND - ND - ND ND 4.0±0.4 2.5±0.9 ND - ND ND 3.8±1.5 - ND ND 1.4±1.2 ND 16.9±1.0 8.5±0.5 ND ND 48.4±8.5 2.6±0.2 ND - ND - 4.9±0.2 12.5±0.7 ND - ND - 0.1 1 2 ND 4.0±2.2 ND ND ND ND ND - ND - ND ND ND ND ND - ND ND ND - ND ND ND ND ND ND ND ND 17.8±0.8 0.1±0.1 ND - ND - ND ND ND - ND - Psychostimulants Caffeine Psychiatric drugs Carbamazepine Vasodilators Pentoxifylline Lincosamides antibiotics Lincomycin Other antibiotics Trimethoprim * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S2 Concentrations of emerging contamination in monitoring wells (5/6). Concentration (ng/L) MDLs Sampling* A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 2.5 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - 1 ND ND ND ND ND ND ND 1.0±0.3 ND 1.4±0.5 9.0±1.7 ND 3.3±0.3 1.2±1.0 14.7±2.1 ND 2.3±0.5 2.5±1.2 1.3±0.2 1.3±0.3 2 ND ND ND - - ND ND - ND - 5.9±1.6 ND ND ND 14.9±1.0 ND - - 1 ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND ND 1822±150 ND ND 2 ND ND ND - - ND ND - ND - ND ND ND ND ND - - ND - - Estrogens β-Estradiol Estriol Estrone 17α-ethynylestradiol 5 1 2.5 * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S2 Concentrations of emerging contamination in monitoring wells (6/6). Concentration (ng/L) MDLs Sampling* A1 A2 A4 A8 A9 A11 A12 A14 A17 F10 F17 F24 F29 F162 O2 O5 O12 O14 O15 J2 PFBS 0.05 PFHxS 0.08 PFOS 0.25 1 2 1 2 1 2 1.6±0.1 1.3±0.2 0.5±0.1 0.3±0.0 3.1±0.2 5.6±0.4 2.9±0.7 1.9±0.2 4.8±0.2 3.3±0.3 3.1±0.4 11.2±1.4 1.3±0.1 0.8±0.2 1.2±0.1 0.2±0.0 0.9±0.1 3.3±0.9 1.9±0.1 1.2±0.1 3.5±0.7 - 0.9±0.1 0.6±0.1 0.6±0.4 - 3.4±0.3 4.4±0.5 ND 0.2±0.1 1.3±0.2 4.4±0.5 5.2±0.6 1.0±0.1 1.7±0.8 0.8±0.1 6.4±1.0 16.8±0.3 1.5±0.1 0.9±0.1 1.5±0.2 - 1.2±0.2 0.7±0.1 0.6±0.1 0.2±0.0 ND 1.1±0.2 3.4±0.5 1.0±0.1 8.8±0.4 - ND ND 9.3±0.7 4.3±2.8 60.9±6.2 35.5±4.4 2.3±0.5 0.6±0.0 0.3±0.1 0.2±0.0 1.1±0.3 1.2±0.2 4.1±0.3 4.5±1.0 1.5±0.2 2.6±0.5 4.6±2.2 76.8±16.5 4.8±0.7 4.3±0.4 2.1±0.9 2.4±0.5 6.0±0.8 9.0±0.6 2.1±0.2 1.3±0.1 3.0±0.3 2.3±0.3 1.7±0.1 28.6±1.1 1.5±0.2 1.0±0.1 0.9±0.2 - 1.4±0.0 1.2±0.1 1.6±0.6 - 2.9±0.5 1.9±0.3 3.6±0.3 3.3±0.4 9.3±0.5 11.9±1.3 4.2±0.3 8.3±0.9 5.0±2.0 - ND 0.9±0.1 ND - 1 2 1 2 1 2 1 2 1 2 1 2 1 2 13.3±0.9 9.3±1.3 2.4±0.2 5.6±0.4 3.8±0.7 11.9±1.6 2.3±0.2 3.2±0.4 1.1±0.0 1.5±0.3 ND 0.3±0.1 ND ND 38.6±4.8 19.8±2.9 6.0±0.1 6.3±0.3 18.4±5.0 13.9±0.7 1.7±0.2 1.6±0.2 0.3±0.1 0.7±0.1 0.6±0.1 ND ND ND 6.2±0.6 2.7±0.6 1.4±0.1 0.7±0.1 ND 2.9±0.4 1.9±0.4 1.2±0.2 0.7±0.1 1.3±0.1 0.3±0.2 ND ND ND 12.0±0.5 0.5±0.1 ND 0.2±0.1 ND ND ND - ND 1.2±0.1 2.0±0.3 0.7±0.1 0.3±0.1 ND ND - 133±17.1 86.0±6.1 0.9±0.1 1.1±0.1 5.0±2.1 3.2±0.9 0.3±0.0 1.1±0.7 ND 0.2±0.1 0.7±0.6 ND ND ND 108±21.2 19.9±1.4 2.8±1.5 5.1±0.2 9.3±0.5 10.9±2.2 1.4±0.4 2.4±0.3 1.2±0.2 1.3±0.1 0.3±0.1 ND ND ND 6.1±0.9 1.2±0.1 12.3±0.6 0.6±0.1 ND ND ND - 16.1±1.6 10.2±3.1 0.5±0.1 0.2±0.1 ND 0.1±0.2 0.5±0.3 0.2±0.2 ND 0.2±0.1 0.4±0.1 ND ND ND 56.6±5.0 1.5±0.1 4.5±0.5 1.9±0.1 0.5±0.1 0.4±0.1 ND - 358±50.9 240±47.6 5.0±0.3 4.9±0.7 38.4±0.9 12.4±5.6 3.2±0.4 1.1±0.1 ND ND ND ND ND ND 36.5±8.4 9.8±0.1 1.1±0.1 0.7±0.1 3.4±0.5 2.7±0.1 1.0±0.1 0.4±0.2 0.3±0.0 0.1±0.0 ND ND ND ND ND 75.3±16.3 14.9±0.5 46.3±6.5 29.0±0.6 40.3±10.5 2.5±0.2 6.6±0.4 0.9±0.3 2.3±0.4 0.3±0.0 1.2±0.3 ND ND 96.2±16.1 63.7±11.9 1.8±1.4 1.0±0.1 9.5±2.4 ND 1.3±0.7 0.4±0.1 1.2±0.1 ND 0.6±0.2 ND ND ND 32.3±4.2 6.9 ±0.9 3.8±0.2 5.2±0.3 13.3±0.8 18.1±1.7 1.6±0.2 4.4±0.4 0.6±0.1 2.0±0.1 ND 0.5±0.2 ND ND 7.7±1.5 0.2±0.0 ND 0.5±0.1 ND ND ND - 6.3±0.6 3.7±0.2 3.6±0.6 1.6±0.1 1.1±0.1 ND ND - 145±11.6 46.1±5.2 1.6±0.1 1.7±0.3 7.1±0.8 7.5±0.8 2.5±0.2 3.3±1.2 1.6±0.1 1.6±0.2 ND 0.4±0.3 ND ND 16.3±1.8 7.2±0.5 23.3±1.6 1.3±0.1 0.3±0.1 ND ND - 60.3±6.6 0.7±0.1 4.3±0.6 0.5±0.0 ND ND ND - PFASs PFCAs PFHxA 0.1 PFHpA 0.05 PFOA 0.05 PFNA 0.1 PFDA 0.05 PFUnA 0.25 PFDoA 0.25 * 1:The first sampling (2013/03/06~2013/03/10), 2:The second sampling (2013/06/20~2013/06/22); ND: not detected or less than method detection limit. Table S3 LC-MS/MS conditions for all of the target compounds. Time (min) Flow rate (μL/min) Positive/ Negative mode HPLC gradient eluent Mobile phase A(%) Mobile phase B(%) 0.0 1.0 100 0 0.5 1.0 100 0 3.0 1.0 60 40 7.5 1.0 30 70 9.0 1.0 5 95 11 1.0 5 95 12 1.0 100 0 15 1.0 100 0 0.0 1.0 63 37 0.4 1.0 50 50 0.8 1.0 20 80 4.8 1.0 5 95 5.0 1.0 63 37 7.0 1.0 63 37 PFCs Table S4a The investigated compounds and their LC-MS/MS parameters. Retention time (min) Precursor ion (m/z) Sulfonamide antibiotics Sulfadiazine 5.27 251 Sulfamethoxazole 6.48 254 Sulfathiazole 5.35 256 Sulfamethazine 5.98 279 Sulfamonomethoxine 6.67 281 Sulfadimethoxine 7.66 311 Macrolides antibiotics Erythromycin-H2O 10.19 716.5 Clarithromycin 10.06 748.5 Roxithromycin 10.15 837.5 Tylosin 9.00 916.7 Quinolone antibiotics Nalidixic acid 9.34 233 Flumequine 9.66 262 Pipemidic acid 5.54 304 Norfloxacin 5.92 320 Ciprofloxacin 5.99 332 Ofloxacin 5.77 362 Imidazole antibiotics Dimetridazole 5.61 142 Metronidazole 5.34 172 Lincosamides antibiotics Lincomycin 5.50 NSAIDs Acetaminophen Compounds Product ions (m/z) Conditions DP EP (volts) (volts) CE (volts) CXP (volts) 38.0 22.4 37.2 21.2 36.5 20.0 25.1 23.8 43.0 24.2 41.0 30.2 4.4 10.3 7.0 12.1 4.4 8.0 8.1 11.9 5.1 8.1 6.6 8.9 42.1 24.0 38.5 28.7 45.0 29.2 54.3 39.3 8.5 15.3 12.4 16.6 13.0 20.6 14.0 22.5 35.3 18.9 44.6 24.2 28.9 24.2 23.4 28.7 24.5 26.2 36.9 27.8 10.6 11.2 15.1 19.9 17.9 7.1 7.0 17.1 7.5 8.6 14.8 8.5 35.8 23.8 31.3 20.8 3.9 7.5 6.7 9.0 92(Confirmation) 156(Quantitation) 92(Confirmation) 156(Quantitation) 92(Confirmation) 156(Quantitation) 156(Confirmation) 186(Quantitation) 92(Confirmation) 156(Quantitation) 92(Confirmation) 156(Quantitation) 38 10 40 10 40 10 38 10 45 10 40 10 158(Confirmation) 558(Quantitation) 158(Confirmation) 590.5(Quantitation) 158(Confirmation) 679.6(Quantitation) 174(Confirmation) 772.5(Quantitation) 46 10 49 10 50 10 60 10 187(Confirmation) 215(Quantitation) 202(Confirmation) 244(Quantitation) 217(Confirmation) 286(Quantitation) 276(Confirmation) 302(Quantitation) 288(Confirmation) 314(Quantitation) 261(Confirmation) 318(Quantitation) 37 10 44 10 48 10 40 10 45 10 40 10 81(Confirmation) 96(Quantitation) 82(Confirmation) 128(Quantitation) 32 10 30 10 407 126(Confirmation) 359(Quantitation) 55 10 37.0 26.1 6.5 9.6 5.40 152 32 10 Ibuprofen 11.58 208 -25 -10 Naproxen 10.89 229 -22 -10 Ketoprofen 10.63 253 -20 -10 Diclofenac 11.47 294 296 93(Confirmation) 110(Quantitation) 164(Confirmation) 161(Quantitation) 170(Confirmation) 185(Quantitation) 197(Confirmation) 209(Quantitation) 250(Confirmation) 252(Quantitation) -25 -10 32.0 23.6 -10.5 -9.7 -19.0 -8.9 -7.0 -9.8 -15.5 -15.5 4.1 8.2 -11 -10.9 -13.7 -14.7 -10.0 -14.7 -13.4 -13.9 85(Confirmation) 127(Quantitation) 121(Confirmation) 127(Quantitation) 154(Confirmation) 274(Quantitation) -25 -10 -30 -10 -30 -10 -13.0 -17.0 -15.3 -14.7 -35.0 -21.8 -3.0 -9.0 -18.1 -5.0 -10.8 -14.6 116(Confirmation) 183(Quantitation) 145(Confirmation) 190(Quantitation) 116(Confirmation) 191(Quantitation) 116(Confirmation) 319(Quantitation) 213(Confirmation) 255(Quantitation) 45 10 45 10 40 10 45 10 31 10 25.5 24.3 36.0 26.0 25.5 24.3 29.5 24.0 24.5 17.2 8.8 12.1 10.9 10.3 8.9 14.3 9.7 8.9 11.0 10.0 Lipid regulator and cholesterol lowering drug Clofibric acid 10.84 213 Gemfibrozil 11.99 249 Bezafibrate 10.88 360 β-blockers Propranolol 8.07 260 Atenolol 4.77 267 Metoprolol 6.41 268 Acebutolol 6.32 337 Sotalol 4.64 273 Conditions DP EP (volts) (volts) Retention time (min) Precursor ion (m/z) Psychostimulants Caffeine 6.62 195 110(Confirmation) 138(Quantitation) 35 Psychiatric drugs Carbamazepine 9.65 237 192(Confirmation) 194(Quantitation) Vasodilators Pentoxifylline 7.46 279 Other antibiotics Trimethoprim 5.50 Estrogens β-Estradiol Compounds Product ions (m/z) CE (volts) CXP (volts) 10 30.4 28.2 8.3 11.0 43 10 29.1 24.5 15.6 14.0 99(Confirmation) 181 (Quantitation) 34 10 25.8 23.9 7.8 11.0 291 230(Confirmation) 261(Quantitation) 42 10 33.1 35.9 18.5 18.7 11.00 271 -105 10 Estriol 9.01 287 -105 10 Estrone 11.01 269 -100 10 17α-Ethynylestradiol 10.91 279 143(Confirmation) 183(Quantitation) 145(Confirmation) 171(Quantitation) 145(Confirmation) 169(Quantitation) 133(Confirmation) 159(Quantitation) -100 10 -54 -52 -56 -51 -51 -46 -51 -47 -10 -12 -5 -11 -7 -8 -6 -12 PFASs PFBS 3.31 299 -61.2 -10 PFHxS 3.65 399 -42.2 -10 PFOS 4.10 499 80(Confirmation) 99(Quantitation) 80(Confirmation) 119(Quantitation) 80(Confirmation) 99(Quantitation) -60.0 -10 -60.4 -48.1 -75.9 -48.6 -46.2 -15.3 -4.9 -5.8 -3.0 -18.3 -4.8 -8.0 PFCAs PFHxA 3.49 313 -28.4 -10 PFHpA 3.68 363 -20.3 -10 PFOA 3.88 413 -25.0 -10 PFNA 4.14 463 -27.2 -10 PFDA 4.45 513 -26.0 -10 PFUnA 4.80 563 -37.7 -10 PFDoA 5.18 613 119(Confirmation) 269(Quantitation) 119(Confirmation) 169(Quantitation) 169(Confirmation) 369(Quantitation) 169(Confirmation) 219(Quantitation) 269(Confirmation) 469(Quantitation) 269(Confirmation) 319(Quantitation) 269(Confirmation) 569(Quantitation) -34.1 -10 -35.0 -24.0 -34.2 -35.2 -15.0 -28.5 -39.1 -28.9 -33.2 -26.0 -27.2 -25.0 -32.0 -22.1 -8.6 -4.8 -6.1 -11.8 -7.0 -9.1 -8.8 -9.9 -4.8 -11.6 -14.1 -5.7 -4.8 -14.8 Table S4b The internal standards of investigated compounds and their LC-MS/MS parameters. Quantitation Compounds Confirmation Correspond compounds Retention Precursor DP Product ion CE CXP Product CE CXP time ion ion (min) (m/z) (V) (m/z) (V) (V) (m/z) (V) (V) Positive mode Sulfamethazine-13C6 5.98 285 50 186 Erythromycin-13C,d3 10.19 720.5 50 562.5 22 16 162 Roxithromycin-d7 10.15 844.7 55 158 52 12 685.5 Ciprofloxacin-d8 5.99 340.2 50 322.2 Metronidazole-13C2, 15N2 5.34 176 50 132 27 24 86 Atenolol-d7 4.77 274.2 25 145 36 10 123 Ibuprofen-d3 11.58 208 -34 164 -25 -9.7 Estradiol-13C2 11.00 273 -100 147 -54 17α-ethynylestradiol-13C2 10.91 297 -100 145 -52 PFOA-13C8 3.88 421 -24.3 376 24.0 16.9 31.0 24.0 124 296.2 28.1 13.8 Sulfadiazine, Sulfamethoxazole, Sulfathiazole, Sulfamethazine, Sulfamonomethoxine, Sulfadimethoxine 44 13 Erythromycin-H2O, Clarithromycin 31 18 Roxithromycin, Tylosin 24.5 24.0 Pipemidic acid, Norfloxacin, Ciprofloxacin, Ofloxacin 36 14 Dimetridazole, Metronidazole 29 9 Propranolol, Atenolol, Metoprolol, Acebutolol, Sotalol Negative mode - - -8 185 -56 -10 159 -48 -15.7 -8.1 172 - Ibuprofen, Naproxen, Ketoprofen, Diclofenac -10 β-Estradiol, Estrone -7 Estriol, 17α-ethynylestradiol -26.8 -8.7 PFBS, PFHxS, PFOS, PFHxA, PFHpA, PFOA, PFNA, PFDA, PFUnA, PFDoA Reference Chen, C.-T., Hu, J.-C., Lu, C.-Y., Lee, J.-C., & Chan, Y.-C. 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