Anaerobic biodegradation of organic amendments and contaminants in aquifers can trigger secondary water quality impacts that impair groundwater resources. Reactive transport models help elucidate how diverse geochemical reactions control the spatiotemporal evolution of these impacts. Using extensive monitoring data from a crude oil spill site near Bemidji, Minnesota (USA), we implemented a comprehensive model that simulates secondary plumes of depleted dissolved O 2 and elevated concentrations of Mn 21 , Fe 21 , CH 4 , and Ca 21 over a two-dimensional cross section for 30 years following the spill. The model produces observed changes by representing multiple oil constituents and coupled carbonate and hydroxide chemistry. The model includes reactions with carbonates and Fe and Mn mineral phases, outgassing of CH 4 and CO 2 gas phases, and sorption of Fe, Mn, and H 1 . Model results demonstrate that most of the carbon loss from the oil (70%) occurs through direct outgassing from the oil source zone, greatly limiting the amount of CH 4 cycled down-gradient. The vast majority of reduced Fe is strongly attenuated on sediments, with most (91%) in the sorbed form in the model. Ferrous carbonates constitute a small fraction of the reduced Fe in simulations, but may be important for furthering the reduction of ferric oxides. The combined effect of concomitant redox reactions, sorption, and dissolved CO 2 inputs from source-zone degradation successfully reproduced observed pH. The model demonstrates that secondary water quality impacts may depend strongly on organic carbon properties, and impacts may decrease due to sorption and direct outgassing from the source zone.
Secondary water quality impacts can result from a broad range of coupled reactions triggered by primary groundwater contaminants. Data from a crude-oil spill research site near Bemidji, MN provide an ideal test case for investigating the complex interactions controlling secondary impacts, including depleted dissolved oxygen and elevated organic carbon, inorganic carbon, CH4, Mn, Fe, and other dissolved ions. To better understand these secondary impacts, this study began with an extensive data compilation of various data types, comprising aqueous, sediment, gas, and oil phases, covering a 260m cross-sectional domain over 30years. Mass balance calculations are used to quantify pathways that control secondary components, by using the data to constrain the sources and sinks for the important redox processes. The results show that oil constituents other than BTEX (benzene, toluene, ethylbenzene, o-, m- and p-xylenes), including n-alkanes and other aromatic compounds, play significant roles in plume evolution and secondary water quality impacts. The analysis underscores previous results on the importance of non-aqueous phases. Over 99.9% of the Fe(2+) plume is attenuated by immobilization on sediments as Fe(II) and 85-95% of the carbon biodegradation products are outgassed. Gaps identified in carbon and Fe mass balances and in pH buffering mechanisms are used to formulate a new conceptual model. This new model includes direct out-gassing of CH4 and CO2 from organic carbon biodegradation, dissolution of directly produced CO2, and sorption with H(+) exchange to improve pH buffering. The identification of these mechanisms extends understanding of natural attenuation of potential secondary impacts at enhanced reductive dechlorination sites, particularly for reduced Fe plumes, produced CH4, and pH perturbations.
[1] It is difficult to estimate groundwater recharge in semiarid environments, where precipitation and evapotranspiration nearly balance. In such environments, groundwater supplies are sensitive to small changes in the processes that control recharge. Numerical modeling provides the temporal resolution needed to analyze these processes but is highly sensitive to model errors. Natural chloride tracer measurements in the unsaturated zone provide more robust indicators of low recharge rates but yield estimates at coarse time scales that mask most control mechanisms. This study presents a new probabilistic approach for analyzing diffuse recharge in semiarid environments, with an application to study sites in the U.S. southern High Plains. The approach uses data assimilation to combine model predictions and chloride-based recharge estimates. It has the advantage of providing probability distributions rather than point values for uncertain soil and vegetation properties. These can then be used to quantify recharge uncertainty. Estimates of moisture flux time series indicate that percolation (or potential recharge) at the data sites is episodic and exhibits interannual variability. Most percolation occurs during intense rains when crop roots are not fully developed and there is ample antecedent soil moisture. El Niño events can contribute to interannual variability of recharge if they bring rainy winters that provide wet antecedent conditions for spring precipitation. Data assimilation methods that combine modeling and chloride observations provide the high temporal resolution information needed to identify mechanisms controlling diffuse recharge and offer a way to examine the effects of land use change and climatic variability on groundwater resources.
Accelerating mountain glacier recession in a warming climate threatens the sustainability of mountain water resources. The extent to which groundwater will provide resilience to these water resources is unknown, in part due to a lack of data and poorly understood interactions between groundwater and surface water. Here we address this knowledge gap by linking climate, glaciers, surface water, and groundwater into an integrated model of the Shullcas Watershed, Peru, in the tropical Andes, the region experiencing the most rapid mountain‐glacier retreat on Earth. For a range of climate scenarios, our model projects that glaciers will disappear by 2100. The loss of glacial meltwater will be buffered by relatively consistent groundwater discharge, which only receives minor recharge (~2%) from glacier melt. However, increasing temperature and associated evapotranspiration, alongside potential decreases in precipitation, will decrease groundwater recharge and streamflow, particularly for the RCP 8.5 emission scenario.
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