ࡱ>  ACE RbjbjVV A<<l,,o"o"""""""8 #'&"n#+~,F,,,{.{.{.kkkkkkk$qs*ky"{.w.{.{.{.ko"o",,@nUUU{.po"8,",kU{.kUUc|"d,P5ٛ"FdkVn0ndsoNLs$dds"g{.{.U{.{.{.{.{.kkT{.{.{.n{.{.{.{.s{.{.{.{.{.{.{.{.{., 5!: Supplementary Information Sections S1. Full model equations . . . . . . S2 S1.1. Water Column Advection, Dispersion and External Input . S2 S1.2. Tetracycline . . . . . . S2 S1.3. Bacteria . . . . . . . S3 S1.4. Organic Matter . . . . . . S4 S2. Model Implementation . . . . . . S5 S3. Model Input . . . . . . . S5 S3.1. Segmentation and Water Column Transport . . S6 S3.2. Tetracycline . . . . . . S8 S3.3. Bacteria and Organic Matter . . . . S9 S4. Additional Model Results . . . . . . S14 S5. Symbols, Abbreviations and Units . . . . . S18 S6. Supplementary References . . . . . . S21 Tables S1. Summary of Model Simulations . . . . . S5 S2. Summary of Calibration Parameters . . . . . S6 S3. Segmentation and Water Column Transport . . . . S7 S4. Tetracycline Parameters . . . . . . S8 S5. Tetracycline Boundary Concentrations . . . . S9 S6. Bacteria and Organic Matter Parameters . . . . S10 S7. Bacteria and Organic Matter Boundary Conditions . . . S12 S8. Definition of Symbols, Abbreviations and Units . . . S18 Figures S1. Transport . . . . . . . . S7 S2. Bacteria and Organic Matter Model Results . . . . S13 S3. Model Results for 10% DOM Bioavailability . . . S14 S4. Model Results for No Sorption to MIC test media . . . S15 S5. Model Results for No DOM Sorption . . . . S16 S6. Model Results for Stop Discharge Recovery . . . . S17 S1. Full Model Equations S1.1. Water Column Advection, Dispersion and External Input Water column advection, dispersion and external input terms are the same for all state variables. To illustrate, the equation for tetracycline in a water column segment (i) is:  EMBED Equation.3  (S1) where VWC (m3) is the water column volume (= (x H B, see Table S3), Q (m3d"1) is the flow rate, Em (m2d"1) is the dispersion coefficient, A (m2) is the cross sectional area, and L (m) is the mixing length. Equation S1 states that the concentration of tetracycline in water column segment i changes with advective input from the upstream segment (term 1), advective output to the downstream segment (term 2), dispersive exchange with the upstream segment (term 3), dispersive exchange with the downstream segment (term 4) and external input (term 5). In addition to these advection, dispersion and external input processes, the concentration changes due to a number of other processes. Those depend on the state variable (e.g., tetracycline vs. POM) and are defined below. The advection, dispersion and external input terms, and segment indices (i) are omitted from subsequent equations for clarity. S1.2. Tetracycline S1.2.a. Partitioning in Water Column (( = 1) The tetracycline state variable corresponds to the total concentration in all phases. The freely dissolved (Cfd), dissolved (Cd, freely dissolved + DOM-bound) and particulate (Cp, solids-bound) concentrations are:  EMBED Equation.3  (S2)  EMBED Equation.3  (S3)  EMBED Equation.3  (S4) S1.2.b. Partitioning in Sediment Bed (( < 1) The effect of porosity in the sediment bed is accounted for by including the porosity in the partitioning equation. For the freely dissolved equation, for example, this is:  EMBED Equation.3  (S5) State variables are defined on a total volume basis (e.g., Cd, gLt-1), whereas several processes depend on the concentration on a water volume basis (e.g., C'd, gLw-1). The water volume and total volume based concentrations are related by the porosity (e.g., C'd = Cd /(). S1.2.c. Mass Balances  EMBED Equation.3  (S6)  EMBED Equation.3  (S7) As (m2) is the surface area. Equations S6 and S8 state that the water column and sediment bed tetracycline concentrations change due to settling (term 1), resuspension (term 2), diffusive exchange (term 3) and decay (term 4). The settling process (term 1) moves tetracycline from the water column to the sediment bed. The resuspension process (term 2) moves tetracycline from the sediment bed to the water column. The diffusion process (term 3) moves tetracycline between the water column and sediment bed depending on the concentration gradient. The decay process (term 4) removes tetracycline from the water column and sediment bed. S1.3. Bacteria S1.3.a. Susceptible  EMBED Equation.3  (S8)  EMBED Equation.3  (S9) S1.3.b. Resistant  EMBED Equation.3  (S10)  EMBED Equation.3  (S11) Equations S8 through S11 state that the water column and sediment bed, susceptible and resistant bacteria concentrations change due to settling (term 1), resuspension (term 2), growth (term 3), respiration (term 4), gain of resistance (term 5) and loss of resistance (term 6). The settling process (term 1) moves bacteria from the water column to the sediment bed. The resuspension process (term 2) moves bacteria from the sediment bed to the water column. The growth and respiration processes (terms 3 and 4) increase and decrease the bacteria concentration, respectively. The gain of resistance process (term 5) moves bacteria from the susceptible to the resistant pool. The loss of resistance process (term 6) moves bacteria from the resistant to the susceptible pool. S1.3.c. Multiple Tetracyclines If the effect is additive, the action of multiple tetracyclines (i.e. TC, OTC, ...) can be simulated using a modification to Equation 5 in the main text. That is, the growth rate for the susceptible bacteria is a function of each tetracycline (j):  EMBED Equation.3  (S12) This feature is not used in the application presented in the paper, because the sum of tetracyclines is simulated as one antibiotic. Equation S12 states that the growth rate increases with the DOM concentration and decreases with the concentration of each tetracycline. S1.3.d. Multiple Bacteria Species Multiple species of bacteria (i.e. endogenous and exogenous) can be simulated using the above equations. To support resistance transfer between species, resistance gain terms consider transfer from all species. For example: The resistance gain for species 1 (XS(1) ( XR(1)) in the sediment bed, is a function of each species (k) (omitting other terms from Equation S11):  EMBED Equation.3  (S13) This feature is used in Model 3C with two species (k = 2). Equation S13 states that the gain of resistance for species 1 is a second order process between susceptible bacteria of species 1 and the resistant bacteria of all other species (incl. species 1). S1.4. Organic Matter S1.4.a. POM  EMBED Equation.3  (S14)  EMBED Equation.3  (S15) Equation S14 states that the water column POM concentration changes due to settling (term 1), resuspension (term 2), production (term 3) and hydrolysis (term 4). The settling process (term 1) removes POM from the water column. The resuspension process (term 2) adds POM to the water column. The production process (term 3) adds POM to the water column. The hydrolysis process (term 4) removes POM from the water column. Equation S15 states that the sediment bed POM concentration changes due to settling (term 1), resuspension (term 2) and hydrolysis (term 3). The settling process (term 1) adds POM to the sediment bed. The resuspension process (term 2) removes POM from the sediment bed. The hydrolysis process (term 3) removes POM from the sediment bed. S1.4.b. DOM  EMBED Equation.3  (S16)  EMBED Equation.3 (S17) Equations S16 and S18 state that the water column and sediment bed DOM concentrations change due to diffusion (term 1), growth of susceptible and resistant bacteria (terms 2 and 3) and hydrolysis (term 4). The diffusion process (term 1) moves DOM between the water column and sediment bed depending on the concentration gradient. The growth process (terms 2 and 3) removes DOM from the water column and sediment bed. The hydrolysis process (term 4) adds DOM to the water column and sediment bed. S2. Model Implementation The model, named MAQUIS, is implemented in MS Excel using the Visual Basic for Applications (VBA) programming language. Differential equations are integrated using the explicit Euler method (Chapra, 1997). The model code is available from the corresponding author on request. S3. Model Input Table S1. Summary of model simulations (a). modeldescriptionnotes0no antibiotic or resistant bacteria(Figure S1&2)1max. WWTP, no NPS, no decayBC in Table S5, kX = 02ave. WWTP, calibrated NPS, no decayBC in Table S5, kX = 03 ave. WWTP, calibrated NPS, calibrated decayBC in Table S5, kX,WC > 03Alarge input of resistant bacteria, no growth( = 1, fR = max., fp,X = 1, kC = 0, kS = 03Bsmall input of resistant bacteria, growth( < 1, fR = tr, fp,X = 0.1, kC = 0, kS = 03C exogenous resistant bacteria transfer resistance to endogenous bacteria and they grow( < 1, fR = tr, fp,X = 0.1, kC > 0, kS > 03C110% DOM bioavailability0.1 KM (Figure S3)3B2 & 3C2no sorption to MIC test mediaMICfd = MIC, ( = 0 (Figure S4)3C3no DOM sorptionKd,DOM = 0 (Figure S5)3C4stop discharge recoveryBC in Table S5 (Figure S4) (a) BC = boundary conditions. tr = trace. Table S2. Summary of calibration parameters (a). modelcalibrated parameters0-1Kd,solid2Kd,solid, AG BC, CAFO BC3 Kd,solid, AG BC, CAFO BC, kX,WC3AKd,solid, AG BC, CAFO BC, kX,WC3BKd,solid, AG BC, CAFO BC, kX,WC, (3C Kd,solid, AG BC, CAFO BC, kX,WC, (, kC, kS(a) Parameters that were adjusted to match the observed field data. Parameter values are inherited (i.e. Kd,solid was calibrated for Model 1 and kept the same for subsequent models), except for AG BC and CAFO BC, which were re-calibrated for Model 3. S3.1. Segmentation and Water Column Transport The segmentation is based on the USGS National Hydrography Dataset (NHD) flowline layer, which includes length attributes. Flow rates were developed as follows (see Figure S1). Using the measured discharge and drainage area of the most downstream USGS gage, an areal flow contribution was calculated. Drainage areas for each segment were developed with GIS ArcHydo routines from a digital elevation model (DEM), and the flow contribution to each segment was calculated. This includes pristine, AG and CAFO fractions estimated using the weighted flow accumulation function. GIS data were obtained from the EPA BASINS system (EPA, 2010). This is an estimate of the unaltered flow rate (Qnps). Then, the WWTP discharges were added (Qww). Finally, a net discharge/withdrawal flow was added to balance the flow at each of the USGS gages (Qdif). Flow rates are based on the time period July 2001 through February 2006, corresponding to the field data. Hydraulic geometry parameters (depth-flow and width-flow relationships) were derived from data at USGS#2260 (Table S3). Table S3. Segmentation and water column transport. symbolunitsvaluenotes Segmentation(xkm1.0produces reasonable numerical dispersion (a)a, b-0.32, 0.32H = aQb; from site specific analysis (b); b: 0.10.6 (c)e, f-11, 0.22B = eQf; from site specific analysis (b); f: 0.05-0.25 (c)HSEDcm3.0Kim and Carlson (2007a)(-0.30sand (Kim and Carlson, 2007a), 0.12-0.55 (Holtz and Kovacs, 1981) WC TransportQm3 s-1variessee text and Figure S1Emm2 s-10all dispersion is numerical (a) (a) (x was set to produce reasonable numerical dispersion, En = 170370 m2 s"1 (Fischer et al., 1979; Chapra, 1997). (b) From data at USGS#2260. (c) Chapra, 1997, p. 248. Figure S1. Transport. (d) Tracer simulations include 1 mgL"1 in respective discharge.  S3.2. Tetracycline Table S4. Tetracycline parameters. symbolunitsvaluenoteskX,WCd"10, 1.0(a)oxygen/light: 0.046 (Khne et al., 2000); 0.088 0.27 (Knapp et al., 2008); 0.35 38 (Verma et al., 2007); 14 43 (Chen et al., 2008)kX,SEDd"10.0no oxygen/light: 0 (Nygaard et al., 1992); 0 (Lai et al., 1995); 0 (Samuelsen et al., 1994); 0.023 (Halling Srensen et al., 2003)Kd,solidlog L kgS"12.3"0.52 (b); 1.9 (c); 2.5 2.7 (d); >2.6 (e); 2.6 3.0 (f); 2.8 3.4 (g); 3.1 3.2 (h); 3.1 3.4 (i); 2.7 4.1 (j); 3.1 5.5 (k) Kd,DOMlog L kgC"14.23.2 (l); 3.6 4.2 (m); 4.5 (n); 4.44.7 (o); 4.85.4 (p)(a) Model 3. (b) Pouliquen and Le Bris (1996) as cited by Tolls (2001). (c) Loke et al. (2002) as cited by Sarmah et al. (2006). (d) Lai et al. (1995) as cited by Tolls (2001). (e) Thurman and Lindsey (2000) as cited by Tolls (2001) and Sarmah et al. (2006). (f) Rabolle and Spliid (2000) as cited by Tolls (2001). (g) Smith and Samuelsen (1996) as cited by Sarmah et al. (2006). (h) Sithole and Guy (1987) as cited by Tolls (2001). (i) Gupta et al. (2003) as cited by Sarmah et al. (2006). (j) Jones et al. (2005). (k) Linear isotherms, 0.01 N CaCl2, Sassman and Lee (2005). (l) Elliot soil humic acid (ESHA), 0.01 M I, from data in Gu and Karthikeyan (2008). (m) ESHA, sorption and desportion, 0.01 M NaCl, from data in Gu et al. (2007). (n) Dirty Aldrich HA, MacKay and Canterbury (2005). (o) Aldrich HA, Fit to linear portion below Ceq = 5 M, assumed foc = 0.34, Sithole and Guy (1987). (p) River and wetland NOM, Verma et al. (2007). Table S5. Tetracycline boundary concentrations (a). symbol model 1model 2model 3 (b)notesWWTP0.490.230.23Poudre: ave. = 0.23, max. = 0.49 (b) Literature: < 0.050 (OTC, TC, CTC, DXC, Hirsch et al., 1999); 0.180.62 (TC, Gulkowska et al., 2008); 0.0610.29 (TC, unfiltered, Batt et al., 2007); < 0.0440.56 (TC, unfiltered, Batt et al., 2006); 0.165.7 (OTC, Liu et al., 2009); 0.7065 (TC, Liu et al., 2009)AG00.731.1Poudre: no data Literature: 0.03 (TC, Davis et al., 2006); 0.04 (CTC, Davis et al., 2006); < 1.0 (OTC, De Liguoro et al., 2003); < 0.51.0 (TC+OTC, Campagnolo et al., 2002); < 0.52.0 (CTC, Campagnolo et al., 2002); 0.4516 (TC, Peak et al., 2007); < 0.3528 (OTC, Kay et al., 2004); < 0.3556 (OTC, Kay et al., 2005a); < 0.35260 (OTC, Kay et al., 2005b)CAFO0140220Poudre: no data Literature: see AG values abovePRIST.000Poudre: < 0.06 (Kim and Carlson, 2007a) Literature: no data(a) Cd, g L1. (b) Except Model 3C2, which is run to steadystate, then all inputs are set to zero. (c) At Ft. Collins Drake WWTP, Yang and Carlson (2003, 2004), Yang et al. (2005). S3.3. Bacteria and Organic Matter Organic matter and bacteria parameters are established using a simulation without antibiotic or resistant bacteria (Model 0). The results are presented in Figure S2. S3.3.a. Estimation of Sediment Bed Concentrations Several bacteria and organic matter concentrations were derived as follows. POMSED was assigned 5.0 gCLt"1, based on TSSSED (see Table S6), and organic matter content (0.7%, Kim and Carlson, 2007a) and organic carbon content (40%). XSED was assigned 250 mgCLt"1, based on 5% of POMSED (4.7 (2.3 7.8)% of sediment OM is bacteria, Wetzel, 2001, p. 636). Table S6. Bacteria and organic matter parameters. symbolunitsvaluenotesBacteriaMAX,WCd"12.6, 2.6 & 2.9 (a)0.65"4.5 (Connolly et al., 1992)MAX,SEDd"10.26, 0.26 & 0.29 (a)see Section S3.3KMmgCL"19.10.20"18 (Connolly et al., 1992)Y"0.360.20"0.52 (Connolly et al., 1992)kRd"10.110.07"0.15 (Connolly et al., 1992)MICmgL-11.2(i)marine sediment bacteria: 1.41.8 (c); soil bacteria: 1.10.62 (d); clinical pathogen bacteria: 1.84.2 (e)MICfdgL"113marine sediment bacteria: 1418 (c); soil bacteria: 126 (d); clinical pathogen bacteria: 1844 (e)(%1.0, 100 (b)"3.7"1.2 (Bouma and Lenski, 1988, g); 0.76"4.4 (Cooper et al., 1987); 4.8"5.5 (Enne et al., 2005); 4.0"43 (Turner, 2004); 44 (Lenski and Bouma, 1987); 23"100 (Godwin and Slater, 1979); "74"62 (Helling et al., 1981, g); 89 (Anderson, 1974)kSd"10, 4.010"3 (a)0 (Lenski and Bouma, 1987); 2.510"5"1.610"2 (Helling et al., 1981); 3.910"5"0.13 (Cooper et al., 1987)kCLmgC"1 d"10, 1.010"5 (a)0"1.010"10 (Gowland and Slater, 1984, h); 2.510"4"2.910"2 (Turner, 2004, h); 6.810"6"1.0100 (Levin et al., 1979, h)SolidsTSSWCmgSLt"116from USGS #2000TSSSEDkgSLt"11.8= (1 " () (S , (S = 2.6 g cm"3, sand (Kim and Carlson, 2007a).OMkH,WCd"10.050.01"0.07 (HydroQual, 1998)kH,SEDy"15.6constrained by steady"state assumption (see text).PgCm"2d"12.3constrained by steady"state assumption (see text).Transp.vsmd"16.5constrained by steady"state assumption (see text).fp,X%10, 100 (b)10 (Liu et al., 2006).vrmmy"121constrained by steady"state assumption (see text).vdcmd"10.50.1"1.0 (Thomann and Mueller, 1987)(a) Model 3C. (b) Model 3A. (c) MIC of 4 strains, omitting resistant strain V.257, NaCl treatment (Lunestad and Goksoeyr, 1990) (f). (d) MIC of ~20 strains, initial potency (Halling"Srensen et al., 2002, 2003) (f). (e) MIC50 of 28 bacteria to various tetracyclines (Bryskier, 2005) (f). (f) Mean std. dev. Converted from MIC using 6.0 gCL"1. (g) Negative value corresponds to strain with adaptive mutation. (h) Converted using 180 fgdcell"1, median value for E. coli in stationary phase, 0.5 gCgdry"1, Loferer"Krbacher et al. (1998). (i) Not a model parameter. Provided for reference only. S3.3.b. POM Hydrolysis and Bacteria Growth Parameters in the Sediment Bed Assuming (1) steady-state, (2) negligible DOM diffusive flux in the sediment bed DOM balance, and (3) negligible bacteria settling and resuspension fluxes in the sediment bed bacteria balance, the POM hydrolysis flux is assimilated and then respired by bacteria:  EMBED Equation.3  (S18) Given site-specific values for POMSED and XSED and literature values for kR and Y (see Table S6), this allows for the calculation of kH,SED and . The resulting rate constant (Table S6) is within the range for the  highly reactive component of 1 10 y"1 provided by Boudreau (1997, p. 152). Bacteria growth parameters (MAX, KM, Y and kR) were assigned as the midpoint of a literature summary (Connolly et al., 1992) (see Table S6), with the sediment bed MAX reduced to 10% to account for the slower growth rate in the sediment bed. That is, the DOC consumption per bacteria is typically much less in the sediment bed (e.g., Wetzel, 2001, p. 767). S3.3.c. Settling and Resuspension Velocities Assuming (1) steady-state, (2) no long-term net deposition/erosion of sediment bed solids, and (3) no significant solids decay, the sediment bed solids balance yields:  EMBED Equation.3  (S19) Assuming steady-state and combining the sediment bed POM mass balance (Equation S15) with Equation S19 yields:  EMBED Equation.3  (S20) Given site-specific values for HSED, TSSWC, TSSSED, POMWC, POMSED and a value for kH,SED (see above and Tables S1&7), this allows for calculation of vs (Equation S4) and vr (Equation S2). The resulting settling velocity (Table S6) is within the range of values for silt with particle diameters 1020 m (5.6-22 md"1, Chapra, 1997). S3.3.d. POM Production Assuming steady-state, the water column POM balance yields:  EMBED Equation.3  (S21) Given kH,SED, vs and vr and site-specific values for HWC, POMWC, POMSED (see above and Tables S1&S7), this allows for the calculation of P. The resulting autochthonous POM production is on the high side of periphyton net primary production rates summarized in the literature (0.00242.4, Whitton, 1975, p. 253). Increasing the POM concentration in the NPS inflow (which would be reasonable, but is not included in the simple mass balance presented in Equation S21) would reduce P and produce essentially the same model behavior (i.e. the model does not differentiate where the POM comes from). Table S7. Bacteria and Organic Matter Boundary Conditions (a). symbolunitsvaluenotes WWTPX (b)mgCL"10.16assume 5% of POM (as for sediment, see text)fR (b)%0.10, 72 (c)0.12 (McPherson and Gealt, 1986); 1.7 3.2 (Linton et al., 1974); 4 (1 9) (Grabow and Prozesky, 1973); 6.9 (Baya et al., 1986); 4.011 (Murray et al., 1984); 10 (Watkinson et al., 2007b); 13 (Cooke, 1976); 21 (Watkinson et al., 2007a); 25 (Mach and Grimes, 1982); 26 (Fontaine and Hoadley, 1976); 2340 (Mezrioui and Baleux, 1994); 72 (Tao et al., 2010) (d)POMmgCL"13.1based on site data (e)DOMmgCL"14.6based on site data (e) NPSX (b)mgCL"10.020assumed 5% of POM (as for sediment, see text); 0.008 0.45 (Wetzel, 2001, p. 493)fR (b)%0.10, 71 (c) PRIST.: ND 0.3 (Ghosh and LaPara, 2007) AG&CAFO: 0.001 0.2 (Ghosh and LaPara, 2007); 0.59 17 (Sengelov et al., 2003); 26 (Sayah et al., 2005); 33 (Sapkota et al., 2007); 20 65 (Parveen et al., 2006); 29 71 (Haack and Andrews, 2000) (d)POMmgCL"10.400.40 (0.1 2.1) (USGS 06752000); 0.7 0.9 (USGS06752280)DOMmgCL"13.23.3 (1.5 8.4) (USGS 06752000); 2.9 3.2 (USGS06752280); 3.2 (1.2 7.7) (USGS 404200105145600) (a) Bold indicates Poudre River value. (b) X = XS + XR. XR = fR X. (c) Model 3A, AG&CAFO. (d) Literature values include any tetracycline, any bacteria. For WWTP, includes domestic wastewater from any treatment stage (e.g., influent, effluent). For AG, includes effluent, ponds and other environment. (e) Calculated using POM = TSS 0.4 gCgS"1, DOM = TOM " POM. TOM = 8.7 mgCL"1, TSS = 7.7 mgL"1, average from Mulberry and Drake WWTPs for period 7/2001-2/2006. S3.3.e. Discussion of Bacteria and Organic Matter Model Results The bacteria and organic matter concentrations and mass balance terms are presented in Figure S2. The average water column bacteria concentration is 33 gCL"1. Warbington et al. (1987) measured heterotrophic bacteria concentration of 9.0 104 CFUmL"1 (geometric mean) in the Poudre River, which corresponds to 8.1 gCL"1 (using 180 fgdcell"1, median value for E. coli in stationary phase, 0.5 gCgdry"1, Loferer-Krbacher et al., 1998). The model value is expectedly higher, since only a fraction of bacteria are culturable. The average sediment bed bacteria concentration is 260 mgCLt"1. This is slightly higher than the value used in the derivation of the organic matter parameters (see above), which reflects input from the WWTPs. Pei et al. (2006) observed heterotrophic plate counts (HPC) in the Poudre River of 7.8 105 CFUtgSED"1 (geometric mean), which corresponds to 0.15 mgCLt"1 (using conversions above, ( and (S in Table S3&6). Again, the discrepancy is consistent with only a fraction of bacteria being culturable (see also discussion in main text). The average POM concentrations in the water column and sediment bed are 0.42 mgCL"1 and 5.3 gCLt"1 (0.29%). These values are slightly higher than those used in the derivation of the organic matter parameters (see above), which reflects input from the WWTPs. The average DOM concentrations in the water column and sediment bed are 3.3 and 6.6 mgCLw"1, respectively. The sediment bed DOM concentration is in good agreement with observed porewater concentrations reported in the literature (5.4 21 mgCLw"1, Lin et al., 2003; 3.8 24 mgCLw"1, Achman et al., 1996). The assumption of negligible DOM diffusion flux in the sediment bed DOM balance and negligible bacteria settling and resuspension fluxes in the sediment bed bacteria balance are confirmed by examining the mass balance terms in Figure S2. Figure S2. Bacteria and organic matter model results. (A) Concentrations in mgCLt"1. (B) Mass balance terms in gC m"2d"1. Input is positive. Advection, dispersion and external input (see Equation SX) not shown. Mass balance terms are abbreviated with corresponding kinetic variable (e.g.,  kRS is endogenous respiration of susceptible bacteria). Results are for simulation without antibiotics or resistant bacteria (Model 0).  S4. Additional Model Results Figure S3. Model results for 10% DOM bioavailability (Model 3C1). KM parameter was adjusted to 0.91 mgCL"1. Spatial pattern of (a) water column and (b) sediment bed tetracycline concentrations, and (c) tetracycline resistance in the Poudre River. Symbols are data from Yang and Carlson (2003), Kim and Carlson (2007a,b) and Pei et al. (2006). Lines are model predictions (see text for description of different models). Distance is downstream from CSU#1 (see Figure 3).  Figure S4. Model results for no sorption to MIC test media (Models 3B2 and 3C2). Spatial pattern of (a) water column and (b) sediment bed tetracycline concentrations, and (c) tetracycline resistance in the Poudre River. Symbols are data from Yang and Carlson (2003), Kim and Carlson (2007a,b) and Pei et al. (2006). Lines are model predictions (see text for description of different models). Distance is downstream from CSU#1 (see Figure 3).  Figure S5. Model results for no DOM sorption (Model 3C3). Spatial pattern of (a) water column and (b) sediment bed tetracycline concentrations, and (c) tetracycline resistance in the Poudre River. Symbols are data from Yang and Carlson (2003), Kim and Carlson (2007a,b) and Pei et al. (2006). Lines are model predictions (see text for description of different models). Distance is downstream from CSU#1 (see Figure 3).  Figure S6. Model results for stop discharge recovery (Model 3C4). Temporal pattern of (a) water column and (b) sediment bed tetracycline concentrations, and (c) tetracycline resistance (note change of scale from other plots) in the Poudre River. Location is downstream of Ft. Collins (80 km, see Figure 3). Lines are model predictions (see text for description of different models). Model output interval is 0.5 years.  S5. Symbols, Abbreviations and Units Table S8. Definition of symbols, abbreviations and units. symbol/ abbreviation/ unitdefinitionAcross sectional areaahydraulic geometry parameterAGagricultural(cost of resistanceAssurface area bhydraulic geometry parameterBwidthBASINSBetter Assessment Science Integrating point & Non-point SourcesBCboundary condition Cconcentration of tetracyclineCAFOconfined animal feeding operationsCddissolved C (freely dissolved + DOM-bound)C'dCd, water volume basisCeqequilibrium concentrationCfdfreely dissolved CCFUcolony forming unitCFUrCFU, resistantCFUtCFU, totalCpparticulate CCSUColorado State UniversityCTCchlortetracycline (xsegment lengthDEMdigital elevation modelDMCdemeclocyclineDOCdissolved organic carbonDOMdissolved organic matterDXCdoxycycline ehydraulic geometry parameterE. coliEscherichia coliEmdispersion coefficient, model-assignedTable S8. Cont. symbol/ abbreviation/ unitdefinitionEndispersion coefficient, numericalEPAEnvironmental Protection AgencyESHAElliot soil humic acid fhydraulic geometry parameterfdfreely dissolvedfocfraction organic carbonfp,Xfraction particle-associated bacteriafRfraction of resistant bacteria ggramgCg carbongdg dryGISgeographic information systemgSg solidsgSEDg sediment HdepthHAhumic acidHPCheterotrophic plate count isegment indexIionic strength jtetracycline index kbacteria species indexkCtransfer rate constantKdpartition coefficientKd,DOMDOM partition coefficientKd,solidsolids partition coefficientkHPOM hydrolysis rate constantkH,SEDkH, sediment bedKMhalf-saturation constantKOWoctanol-water partition coefficientkRspecific endogenous respiration ratekRSendogenous respiration of susceptible bacteriaTable S8. Cont. symbol/ abbreviation/ unitdefinition kSsegregation rate constantkXdecay rate constantkX,WCkX, water column Lmixing lengthLliterLtL, totalLwL, water MCCmeclocyclineMICminimum inhibitory concentrationMICfdfreely dissolved MICgrowth rateMAXmaximum specific growth rateR, resistant bacteriaS, susceptible bacteria NDnon-detectNHDNational Hydrography DatasetNOMnatural organic matterNPSnonpoint source OMorganic matterOTCoxytetracycline PPOM production ratep/a-PCRpresence/absence PCRPCBpolychlorinated biphenylPCRpolymerase chain reaction(porosityPOMparticulate organic matterPRISTpristine Qflow rateQdifnet discharge/withdrawal flowQINexternal inflow rateTable S8. 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Evolution of antibiotic occurrence in a river through pristine, urban and agricultural landscapes. Water Research 2003, 37, 4645-4656. Yang, S.; Carlson, K. Routine monitoring of antibiotics in water and wastewater with a radioimmunoassay technique. Water Research 2004, 38, 3155-3166. Yang, S.; Cha, J.; Carlson, K. Simultaneous extraction and analysis of 11 tetracycline and sulfonamide antibiotics in influent and effluent domestic wastewater by solid-phase extraction and liquid chromatography-electrospray ionization tandem mass spectrometry. Journal of Chromatography A 2005, 1097, 40-53.     PAGE  PAGE 10 S PAGE \* MERGEFORMAT 11 S PAGE \* MERGEFORMAT 1 n 68 (*26:dfvx` 趮h9mHnHujh9Uh9 h90J-jh90J-Uhd/jhd/UhQ45h+CJaJh {h {5CJaJh:CJaJh th {CJaJh {CJaJh thQ45CJaJh {hQ456CJaJ3TRTV+$a$h]h&`#$ $x]xa$gdnh]hgdK)h]hgdK )&`#$gd$d3^`3gdm$HJNPRVXZhQ45h+CJaJh,*hd/h'h+mHnHuh9h"6mHnHujh+Uh+V3^`3gdm$++$a$? 000&P 1F:p$6. 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