[1] This work presents a stream tube-based analytical approach to evaluate reduction in groundwater contaminant flux resulting from partial mass reduction in a nonaqueous phase liquid (NAPL) source zone. The reduction in contaminant flux, R j , discharged from the source zone is a remediation performance metric that has a direct effect on the fundamental drivers of remediation: protection of human health and the environment. Closed form expressions are provided for analyzing remediation performance under conditions of joint spatial variability of both groundwater flow and NAPL content. The performance measures derived here are expressed in terms of measurable parameters. Spatial variability is described within a Lagrangian framework where aquifer hydrodynamic heterogeneities are characterized using nonreactive travel time distributions, while NAPL spatial distribution heterogeneity can be similarly described using reactive travel time distributions. The combined statistics of these distributions are used to evaluate the relationship between reduction in contaminant mass, R m , and R j . A portion of the contaminant mass in the source zone is assumed to be removed via in situ flushing remediation, with the initial and final conditions defined as steady state natural gradient groundwater flow through the contaminant source zone. The combined effects of aquifer and NAPL heterogeneities are shown to be captured in a single parameter, reactive travel time variability, which was determined to be the most important factor controlling the relationship between R m and R j . It is shown that as heterogeneity in aquifer properties and NAPL spatial distribution increases, less mass reduction is required to achieve a given flux reduction, although the overall source longevity increases. When rate-limited dissolution is important, the efficiency of remediation, in terms of both mass and flux reduction, is reduced. However, at many field sites the combined effects of field-scale heterogeneities and site aging will result in favorable relationships between mass reduction and flux reduction.

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[1] Simulations of nonpartitioning and partitioning tracer tests were used to parameterize the equilibrium stream tube model (ESM) that predicts the dissolution dynamics of dense nonaqueous phase liquids (DNAPLs) as a function of the Lagrangian properties of DNAPL source zones. Lagrangian, or stream-tube-based, approaches characterize source zones with as few as two trajectory-integrated parameters, in contrast to the potentially thousands of parameters required to describe the point-by-point variability in permeability and DNAPL in traditional Eulerian modeling approaches. The spill and subsequent dissolution of DNAPLs were simulated in two-dimensional domains having different hydrologic characteristics (variance of the log conductivity field = 0.2, 1, and 3) using the multiphase flow and transport simulator UTCHEM. Nonpartitioning and partitioning tracers were used to characterize the Lagrangian properties (travel time and trajectoryintegrated DNAPL content statistics) of DNAPL source zones, which were in turn shown to be sufficient for accurate prediction of source dissolution behavior using the ESM throughout the relatively broad range of hydraulic conductivity variances tested here. The results were found to be relatively insensitive to travel time variability, suggesting that dissolution could be accurately predicted even if the travel time variance was only coarsely estimated. Estimation of the ESM parameters was also demonstrated using an approximate technique based on Eulerian data in the absence of tracer data; however, determining the minimum amount of such data required remains for future work. Finally, the stream tube model was shown to be a more unique predictor of dissolution behavior than approaches based on the ganglia-to-pool model for source zone characterization.

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DyeLIF™ is a new version of laser‐induced fluorescence (LIF) for high‐resolution three‐dimensional subsurface mapping of nonaqueous phase liquids (NAPLs) in the subsurface. DyeLIF eliminates the requirement that the NAPL contains native fluorophores (such as those that occur in compounds like polynuclear aromatic hydrocarbons [PAHs]) and can therefore be used to detect chlorinated solvents and other nonfluorescing NAPLs that had previously been undetectable with conventional LIF tools. With DyeLIF, an aqueous solution of water and nontoxic hydrophobic dye is continuously injected ahead of the sapphire detection window while the LIF probe is being advanced in the subsurface. If soil containing NAPL is penetrated, the injected dye solvates into the NAPL within a few milliseconds, creating strong fluorescence that is transmitted via fiber‐optic filaments to aboveground optical sensors. A detailed field evaluation of the novel DyeLIF technology was performed at a contaminated industrial site in Lowell, Massachusetts, USA where chlorinated solvent dense nonaqueous phase liquid (DNAPL) persists below the water table in sandy sediments. Continuously cored boreholes were drilled adjacent to 5 of 30 DyeLIF probes that were advanced at that site. The cores were subsampled in high resolution to generate discrete‐depth soil samples as splits at the same depths where DNAPL was detected in the colocated DyeLIF probes. The cores were analyzed above ground using (1) colorimetric screening using hydrophobic dye tests, (2) laboratory extraction and quantitative chemical analysis, (3) “Benchtop” DyeLIF, and (4) volumetric moisture content. Correlation between DyeLIF and aboveground analyses of the soil cores was excellent: 98% agreement with positive DNAPL detections in samples where DNAPL pore saturations were >0.7% (based on quantitative soil analyses) and the ex situ tests. DyeLIF produced the equivalent of one aboveground colorimetric dye test every 0.2 inch (0.5 cm) of probing. With average daily probing of 395 linear feet (120.4 m), this was the equivalent of 12,039 discrete‐depth colorimetric dye tests/day. Because DyeLIF is an in situ measurement, there are no issues with soil core recovery like there would be for conventional ex situ colorimetric dye tests and 100% characterization of the probed intervals is achieved. Tracking the injection rate and pressure of the dye solution provides simultaneous data regarding relative soil permeability, similar to other direct push (DP) hydraulic profiling tools. Conventional LIF is considered the premier DP tool to identify and map NAPL containing PAHs in the subsurface or confirm its absence. While chlorinated solvent DNAPLs at some field sites contain impurities (e.g., solvated greases or oils) that make them detectable with conventional LIF techniques, at other sites, the DNAPL cannot be detected with conventional LIF. At such sites, the injection of a hydrophobic dye ahead of the sapphire window with the DyeLIF system now makes the LIF technology applicable to the many t...

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