N. Gottschall

Pharmaceutical and personal care products in groundwater, subsurface drainage, soil, and wheat grain, following a high single application of municipal biosolids to a field

Dewatered municipal biosolids (DMBs) were applied to a field at a rate of ~22 Mg dw ha(-1) in October 2008. Pharmaceuticals and personal care products (PPCPs) were monitored in groundwater, tile drainage, soil, DMB aggregates incorporated into the soil post-land application, and in the grain of wheat grown on the field for a period of ~1 year following application. Over 80 PPCPs were analyzed in the source DMB. PPCPs selected for in-depth monitoring included: antibiotics (tetracyclines, fluoroquinolones), bacteriocides (triclosan, triclocarban), beta-blockers (atenolol, propranolol, metaprolol), antidepressants (fluoxetine, citalopram, venlafaxine, sertraline), antifungals (miconazole), analgesics (acetaminophen, ibuprofen) and anticonvulsants (carbamazepine). PPCPs in tile were observed twice, ~3 weeks and 2 months post-application. Of all PPCPs measured in tile drainage, only carbamazepine, ibuprofen, acetaminophen, triclosan, triclocarban, venlafaxine, and citalopram were detected (5-74 ng L(-1)). PPCPs were not detected in groundwater >2 m depth below the soil surface, and concentrations above detection limits at 2 m depth were only observed once just after the first rain event post-application. In groundwater, all compounds found in tile, except carbamazepine, acetaminophen and citalopram, were detected (10-19 ng L(-1)). PPCPs were detected in DMB aggregates incorporated in soil up to 1 year post-application, with miconazole and fluoxetine having the lowest percent reductions over 1 year (~50%). For several compounds in these aggregates, concentration declines were of exponential decay form. No PPCPs were detected in the grain of wheat planted post-application on the field. No PPCPs were ever detected in water, soil or grain samples from the reference plot, where no DMB was applied.

Pharmaceutical and personal care products in tile drainage following land application of municipal biosolids.

Land application of municipal biosolids (sewage) is a common farming practice in many parts of the world. There is potential for transport of pharmaceuticals and personal care products (PPCPs) from agricultural fields to adjacent surface waters via tile drainage systems. In this study, liquid municipal biosolids (LMB) (total solids=11,933 mg L(-1)), supplemented with selected PPCPs and the fluorescent dye tracer rhodamine WT (RWT), were applied to tile drained fields using two land application approaches. Objectives included evaluating the relative benefits of land application practices with respect to reducing PPCP loadings to tile drains, evaluating PPCP persistence in tile water, and determining whether rhodamine WT can be used to estimate PPCP mass loads in tile. The PPCPs examined included an antibacterial agent used in personal care products (triclosan), a metabolite of nicotine (cotinine), and a variety of drugs including two sulfonamide antimicrobials (sulfapyridine, sulfamethoxazole), a beta-blocker (atenolol), an anti-epileptic (carbamazepine), an antidepressant (fluoxetine), analgesic/anti-inflammatories (acetaminophen, naproxen, ibuprofen), and a lipid-regulator (gemfibrozil). Maximum observed PPCP concentrations in the spiked LMB were about 10(3) ng g(-1) dry weight. PPCPs were shown to move rapidly via soil macropores to tile drains within minutes of the land application. Maximum observed PPCP concentrations in tile effluent associated with the LMB application-induced tile flow event were approximately 10(1) to 10(3) ng L(-1). PPCP mass loads, for the application-induced tile-hydrograph event, were significantly (p<0.1) higher for surface spreading over non-tilled soil (incorporation tillage occurring 20 h post-application), relative to aerating soil immediately prior to surface spreading using an AerWay slurry deposition system. PPCP concentrations that were detected above the limit of quantitation (LOQ) in tile water during several precipitation-induced tile flow events that occurred post-application, included: triclosan (max. approximately 1.5 x 10(2) ng L(-1)), carbamazepine (max. approximately 7 x 10(1) ng L(-1)), atenolol (max approximately 4 x 10(1) ng L(-1)), and cotinine (max approximately 2 x 10(1) ng L(-1)). In spite of their presence in biosolids, the other PPCPs were not observed above LOQ concentrations during these events. PPCP concentrations were predicted from RWT concentrations over a 40 day study period. Tile mass loads as a percent of PPCP mass applied to soil ranged from 4.2%+/-SD of 9.2% to 7.1%+/-10.9% for the AerWay system and surface spreading plus incorporation treatments, respectively.

Pharmaceutical and personal care products in tile drainage following surface spreading and injection of dewatered municipal biosolids to an agricultural field

Land application of municipal biosolids can be a source of environmental contamination by pharmaceutical and personal care products (PPCPs). This study examined PPCP concentrations/temporally discrete mass loads in agricultural tile drainage systems where two applications of biosolids had previously taken place. The field plots received liquid municipal biosolids (LMB) in the fall of 2005 at an application rate of approximately 93,500 L ha (-1), and a second land application was conducted using dewatered municipal biosolids (DMB) applied at a rate of approximately 8Mg dw ha (-1) in the summer of 2006 [corrected].The DMB land application treatments consisted of direct injection (DI) of the DMB beneath the soil surface at a nominal depth of approximately 0.11 m, and surface spreading (SS) plus subsequent tillage incorporation of DMB in the topsoil (approximately 0.10 m depth). The PPCPs examined included eight pharmaceuticals (acetaminophen, fluoxetine, ibuprofen, gemfibrozil, naproxen, carbamazepine, atenolol, sulfamethoxazole), the nicotine metabolite cotinine, and two antibacterial personal care products triclosan and triclocarban. Residues of naproxen, cotinine, atenolol and triclosan originating from the fall 2005 LMB application were detected in tile water nearly nine months after application (triclocarban was not measured in 2005). There were no significant differences (p>0.05) in PPCP mass loads among the two DMB land application treatments (i.e., SS vs. DI); although, average PPCP mass loads late in the study season (>100 days after application) were consistently higher for the DI treatment relative to the SS treatment. While the concentration of triclosan (approximately 14,000 ng g(-1) dw) in DMB was about twice that of triclocarban (approximately 8000 ng g(-1) dw), the average tile water concentrations for triclosan were much higher (43+/-5 ng L(-1)) than they were for triclocarban (0.73+/-0.14 ng L(-1)). Triclosan concentrations (maximum observed in 2006 approximately 235 ng L(-1)) in tile water resulting from land applications may warrant attention from a toxicological perspective.

Effect of Liquid Municipal Biosolid Application Method on Tile and Ground Water Quality

This study examined bacteria and nutrient quality in tile drainage and shallow ground water resulting from a fall land application of liquid municipal biosolids (LMB), at field application rates of 93,500 L ha(-1), to silt-clay loam agricultural field plots using two different land application approaches. The land application methods were a one-pass AerWay SSD approach (A), and surface spreading plus subsequent incorporation (SS). For both treatments, it took between 3 and 39 min for LMB to reach tile drains after land application. The A treatment significantly (p < 0.1) reduced application-induced LMB contamination of tile drains relative to the SS treatment, as shown by mass loads of total Kjeldahl N (TKN), NH(4)-N, Total P (TP), PO(4)-P, E. coli., and Clostridium perfringens. E. coli contamination resulting from application occurred to at least 2.0-m depth in ground water, but was more notable in ground water immediately beneath tile depth (1.2 m). Treatment ground water concentrations of selected nutrients and bacteria for the study period ( approximately 46 d) at 1.2-m depth were significantly higher in the treatment plots, relative to control plots. The TKN and TP ground water concentrations at 1.2-m depth were significantly (p < 0.1) higher for the SS treatment, relative to the A treatment, but there were no significant (p > 0.1) treatment differences for the bacteria. For the macroporous field conditions observed, pre-tillage by equipment such as the AerWay SSD, will reduce LMB-induced tile and shallow ground water contamination compared to surface spreading over non-tilled soil, followed by incorporation.

Long-term monitoring of waterborne pathogens and microbial source tracking markers in paired agricultural watersheds under controlled and conventional tile drainage management.

ABSTRACT Surface waters from paired agricultural watersheds under controlled tile drainage (CTD) and uncontrolled tile drainage (UCTD) were monitored over 7 years in order to determine if there was an effect of CTD (imposed during the growing season) on occurrences and loadings of bacterial and viral pathogens, coliphages, and microbial source tracking markers. There were significantly lower occurrences of human, ruminant, and livestock (ruminant plus pig) Bacteroidales markers in the CTD watershed in relation to the UCTD watershed. As for pathogens, there were significantly lower occurrences of Salmonella spp. and Arcobacter spp. in the CTD watershed. There were no instances where there were significantly higher quantitative loadings of any microbial target in the CTD watershed, except for F-specific DNA (F-DNA) and F-RNA coliphages, perhaps as a result of fecal inputs from a hobby farm independent of the drainage practice treatments. There was lower loading of the ruminant marker in the CTD watershed in relation to the UCTD system, and results were significant at the level P = 0.06. The odds of Salmonella spp. occurring increased when a ruminant marker was present relative to when the ruminant marker was absent, yet for Arcobacter spp., the odds of this pathogen occurring significantly decreased when a ruminant marker was present relative to when the ruminant marker was absent (but increased when a wildlife marker was present relative to when the wildlife marker was absent). Interestingly, the odds of norovirus GII (associated with human and swine) occurring in water increased significantly when a ruminant marker was present relative to when a ruminant marker was absent. Overall, this study suggests that fecal pollution from tile-drained fields to stream could be reduced by CTD utilization.

Polybrominated diphenyl ethers, perfluorinated alkylated substances, and metals in tile drainage and groundwater following applications of municipal biosolids to agricultural fields

Polybrominated diphenyl ethers (PBDEs), perfluorinated alkylated substances (PFAS), and metals were monitored in tile drainage and groundwater following liquid (LMB) and dewatered municipal biosolid (DMB) applications to silty-clay loam agricultural field plots. LMB was applied (93,500 L ha(-1)) in late fall 2005 via surface spreading on un-tilled soil (SS(LMB)), and a one-pass aerator-based pre-tillage prior to surface spreading (AerWay SSD) (A). The DMB was applied (8 Mg d wha(-1)) in early summer 2006 on the same plots by injecting DMB beneath the soil surface (DI), and surface spreading on un-tilled soil (SS(DMB)). Key PBDE congeners (BDE-47, -99, -100, -153, -154, -183, -209) comprising 97% of total PBDE in LMB, had maximum tile effluent concentrations ranging from 6 to 320 ng L(-1) during application-induced tile flow. SS(LMB) application-induced tile mass loads for these PBDE congeners were significantly higher than those for control (C) plots (no LMB) (p<0.05), but not A plots (p>0.05). PBDE mass loss via tile (0-2h post-application) as a percent of mass applied was approximately 0.04-0.1% and approximately 0.8-1.7% for A and SS(LMB), respectively. Total PBDE loading to soil via LMB and DMB application was 0.0018 and 0.02 kg total PBDE ha(-1)yr(-1), respectively. Total PBDE concentration in soil (0-0.2m) after both applications was 115 ng g(-1)dw, (sampled 599 days and 340 days post LMB and DMB applications respectively). Of all the PFAS compounds, only PFOS (max concentration=17 ng L(-1)) and PFOA (12 ng L(-1)) were found above detectable limits in tile drainage from the application plots. Mass loads of metals in tile for the LMB application-induced tile hydrograph event, and post-application concentrations of metals in groundwater, showed significant (p<0.05) land application treatment effects (SS(LMB)>A>C for tile and SS(LMB) and A>C for groundwater for most results). Following DMB application, no significant differences in metal mass loads in tile were found between SS(DMB) and DI treatments (PBDE/PFAS were not measured). But for many metals (Cu, Se, Cd, Mo, Hg and Pb) both SS(DMB) and DI loads were significantly higher than those from C, but only during <100 days post DMB application. Clearly, pre-tilling the soil (e.g., A) prior to surface application of LMB will reduce application-based PBDE and metal contamination to tile drainage and shallow groundwater. Directly injecting DMB in soil does not significantly increase metal loading to tile drains relative to SS(DMB), thus, DI should be considered a DMB land application option.

Nitrogen, Phosphorus, and Bacteria Tile and Groundwater Quality Following Direct Injection of Dewatered Municipal Biosolids into Soil

Application of municipal biosolids (sewage) to agricultural land is a common practice to improve soil physical quality and fertility. The chosen method of land application can have a strong impact on the extent of adjacent water contamination by nutrients and bacteria. Dewatered municipal biosolids (DMB) were applied to silt-clay loam experimental field plots in Ontario, Canada using two application methods: (i) surface spreading followed by shallow incorporation (SS) and (ii) a newly developed implement that directly injects DMB into the topsoil (DI). The objective of this study was to compare N, P, and bacteria quality of tile drainage and shallow groundwater associated with each land application technique. There were no significant differences (P > 0.05) in N, P, and bacteria tile mass loads among the application treatments for time periods <100 d postapplication, when the greatest peak loads and peak tile water concentrations were observed. Both land application treatments caused groundwater Escherichia coli contamination to at least 1.2 m depth below surface after the first postapplication rainfall event, and NO(3)-N contamination to at least 2.0 m depth below surface. The DI treatment did, however, have significantly (P < 0.05) higher tile mass loads of total Kjeldahl N (TKN), total phosphorus (TP), E. coli, Enterococci, and Clostridium perfringens relative to the SS treatment for time periods >100 d postapplication. Nevertheless, relative to tile effluent data collected <100 d postapplication (no application treatment differences), peak loads, and concentrations during this time were, overall, considerably lower for both treatments. This finding, along with no significant differences in N, P, and bacteria groundwater concentrations among the application treatments, and that the direct injection technique could potentially reduce vector attraction problems and odor, suggests that the direct injection technique should be considered a dewatered municipal biosolid land application option.

Rainfall-induced runoff from exposed streambed sediments: an important source of water pollution.

When surface water levels decline, exposed streambed sediments can be mobilized and washed into the water course when subjected to erosive rainfall. In this study, rainfall simulations were conducted over exposed sediments along stream banks at four distinct locations in an agriculturally dominated river basin with the objective of quantifying the potential for contaminant loading from these often overlooked runoff source areas. At each location, simulations were performed at three different sites. Nitrogen, phosphorus, sediment, fecal indicator bacteria, pathogenic bacteria, and microbial source tracking (MST) markers were examined in both prerainfall sediments and rainfall-induced runoff water. Runoff generation and sediment mobilization occurred quickly (10-150 s) after rainfall initiation. Temporal trends in runoff concentrations were highly variable within and between locations. Total runoff event loads were considered large for many pollutants considered. For instance, the maximum observed total phosphorus runoff load was on the order of 1.5 kg ha. Results also demonstrate that runoff from exposed sediments can be a source of pathogenic bacteria. spp. and spp. were present in runoff from one and three locations, respectively. Ruminant MST markers were also present in runoff from two locations, one of which hosted pasturing cattle with stream access. Overall, this study demonstrated that rainfall-induced runoff from exposed streambed sediments can be an important source of surface water pollution.

Hormones, sterols, and fecal indicator bacteria in groundwater, soil, and subsurface drainage following a high single application of municipal biosolids to a field.

A land application of dewatered municipal biosolids (DMB) was conducted on an agricultural field in fall 2008 at a rate of 22Mg dry weight (dw) ha(-1). Pre- and post- application, hormone, sterol and fecal indicator bacteria concentrations were measured in tile drainage water, groundwater (2, 4, 6m depth), surface soil cores, and DMB aggregates incorporated in the soil (∼0.2m depth) for a period of roughly 1year post-application. Hormones and sterols were detected up to 1year post-application in soil and in DMB aggregates. Hormone (androsterone, desogestrel, estrone) contamination was detected briefly in tile water samples (22d and ∼2months post-app), at lowngL(-1) concentrations (2-34ngL(-1)). Hormones were not detected in groundwater. Sterols were detected in tile water throughout the study period post-application, and multiple fecal sterol ratios suggested biosolids as the source. Coprostanol concentrations in tile water peaked at >1000ngL(-1) (22d post-app) and were still >100ngL(-1) at 6months post-application. Fecal indicator bacteria were detected throughout the study period in tile water, groundwater (⩽2m depth), soil and DMB aggregate samples. These bacteria were strongly linearly related to coprostanol in tile water (R(2)>0.92, p<0.05). The limited transport of hormones and sterols to tile drainage networks may be attributed to a combination of the hydrophobicity of these compounds and limited macroporosity of the field soil. This transitory contamination from hormones and sterols is unlikely to result in any significant pulse exposure risk in subsurface drainage and groundwater.

Comprehensive Nitrogen Budgets for Controlled Tile Drainage Fields in Eastern Ontario, Canada

Excessive N loading from subsurface tile drainage has been linked to water quality degradation. Controlled tile drainage (CTD) has the potential to reduce N losses via tile drainage and boost crop yields. While CTD can reduce N loss from tile drainage, it may increase losses through other pathways. A multiple-year field-scale accounting of major N inputs and outputs during the cropping season was conducted on freely drained and controlled tile drained agricultural fields under corn ( L.)-soybean [ (L.) Merr.] production systems in eastern Ontario, Canada. Greater predicted gaseous N emissions for corn and soybean and greater observed lateral seepage N losses were observed for corn and soybean fields under CTD relative to free-draining fields. However, observed N losses from tile were significantly lower for CTD fields, in relation to freely drained fields. Changes in residual soil N were essentially equivalent between drainage treatments, while mass balance residual terms were systematically negative (slightly more so for CTD). Increases in plant N uptake associated with CTD were observed, probably resulting in higher grain yields for corn and soybean. This study illustrates the benefits of CTD in decreasing subsurface tile drainage N losses and boosting crop yields, while demonstrating the potential for CTD to increase N losses via other pathways related to gaseous emissions and groundwater seepage.