Reservoirs are a globally significant source of methane (CH4), although most measurements have been made in tropical and boreal systems draining undeveloped watersheds. To assess the magnitude of CH4 emissions from reservoirs in midlatitude agricultural regions, we measured CH4 and carbon dioxide (CO2) emission rates from William H. Harsha Lake (Ohio, U.S.A.), an agricultural impacted reservoir, over a 13 month period. The reservoir was a strong source of CH4 throughout the year, emitting on average 176 ± 36 mg C m(-2) d(-1), the highest reservoir CH4 emissions profile documented in the United States to date. Contrary to our initial hypothesis, the largest CH4 emissions were during summer stratified conditions, not during fall turnover. The river-reservoir transition zone emitted CH4 at rates an order of magnitude higher than the rest of the reservoir, and total carbon emissions (i.e., CH4 + CO2) were also greater at the transition zone, indicating that the river delta supported greater carbon mineralization rates than elsewhere. Midlatitude agricultural impacted reservoirs may be a larger source of CH4 to the atmosphere than currently recognized, particularly if river deltas are consistent CH4 hot spots. We estimate that CH4 emissions from agricultural reservoirs could be a significant component of anthropogenic CH4 emissions in the U.S.A.
Public water systems are increasingly facing higher bromide levels in their source waters from anthropogenic contamination through coal-fired power plants, conventional oil and gas extraction, textile mills, and hydraulic fracturing. Climate change is likely to exacerbate this in coming years. We estimate bladder cancer risk from potential increased bromide levels in source waters of disinfecting public drinking water systems in the United States. Bladder cancer is the health end point used by the United States Environmental Protection Agency (EPA) in its benefits analysis for regulating disinfection byproducts in drinking water. We use estimated increases in the mass of the four regulated trihalomethanes (THM4) concentrations (due to increased bromide incorporation) as the surrogate disinfection byproduct (DBP) occurrence metric for informing potential bladder cancer risk. We estimate potential increased excess lifetime bladder cancer risk as a function of increased source water bromide levels. Results based on data from 201 drinking water treatment plants indicate that a bromide increase of 50 μg/L could result in a potential increase of between 10(-3) and 10(-4) excess lifetime bladder cancer risk in populations served by roughly 90% of these plants.
The mechanisms of aqueous oxidation-reduction interactions between Cr(VI) and substituted phenols (RArOH) were characterized by kinetic analysis and determinations of reaction products and intermediates.A rapid, preoxidative equilibrium between HCrOr and RArOH forms chromate ester intermediates, as verified by spectroscopy. The subsequent ratelimiting ester decomposition proceeds via innersphere electron transfer. The overall rate dependence on [H+] is well accounted for by three parallel redox pathways involving zero, one, and two protons. The two-proton pathway dominates at pH < 2, the singleproton pathway for 2 < pH < 5, and the protonindependent pathway at pH > 5. The parallel reaction rate expression was fitted to data for 4-methyl-, 4-methoxy-, 2,6-dimethoxy-, and 3,4-dimethoxyphenol for pH 1-6. Beside accurately predicting rates for the calibrated conditions, the model predicts a sharp decline in rates at pH > 6. Rates subsequently measured at pH 7 agreed well with those calculated a priori. Such predictions suggestthatthe proposed mechanism is robust and accurate. Rate constants were correlated with Hammett-type substituent parameters. Reaction products indicated both oneand two-electron pathways.
2,4,6-Trinitrotoluene is a major surface and subsurface
contaminant found at numerous munitions production and
storage facilities. The reductive transformation of 2,4,6-trinitrotoluene (TNT) to aromatic (poly)amines and the
consequent fate of these products were studied in anaerobic
and aerobic sediment−water systems. Reduction of TNT
was rapid under both anaerobic and aerobic conditions. Nitro-reduction was regioselective, leading to the preferential
formation of 4-amino-2,6-dinitrotoluene (4-ADNT) and 2,4-diamino-6-nitrotoluene (2,4-DANT). Subsequent sorption of 2,4-DANT was rapid under aerobic conditions and resulted
in nearly complete, irreversible retention by the sediment
phase. Under anaerobic conditions, the rapidly formed 2,4-DANT displayed little affinity for the sediment phase. Instead,
2,4-DANT was further transformed to products that
remained in the aqueous phase. Sorption studies in
nontransforming sediments indicated increased irreversible
sorption with replacement of nitro groups with amino
groups. Covalent binding of the DANTs was partially inhibited
under anoxic conditions, but sorption of TNT and the
ADNTs was unaffected by changes in redox conditions.
We present a framework to compare water treatment costs to source water protection costs, an important knowledge gap for drinking water treatment plants (DWTPs). This trade‐off helps to determine what incentives a DWTP has to invest in natural infrastructure or pollution reduction in the watershed rather than pay for treatment on site. To illustrate, we use daily observations from 2007 to 2011 for the Bob McEwen Water Treatment Plant, Clermont County, Ohio, to understand the relationship between treatment costs and water quality and operational variables (e.g., turbidity, total organic carbon [TOC], pool elevation, and production volume). Part of our contribution to understanding drinking water treatment costs is examining both long‐run and short‐run relationships using error correction models (ECMs). Treatment costs per 1000 gallons (per 3.79 m3) were based on chemical, pumping, and granular activated carbon costs. Results from the ECM suggest that a 1% decrease in turbidity decreases treatment costs by 0.02% immediately and an additional 0.1% over future days. Using mean values for the plant, a 1% decrease in turbidity leads to $1123/year decrease in treatment costs. To compare these costs with source water protection costs, we use a polynomial distributed lag model to link total phosphorus loads, a source water quality parameter affected by land use changes, to turbidity at the plant. We find the costs for source water protection to reduce loads much greater than the reduction in treatment costs during these years. Although we find no incentive to protect source water in our case study, this framework can help DWTPs quantify the trade‐offs.
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