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6 Technology Development to Support Long-Term Management of Complex Sites Despite years of characterization and implementation of remedial technologies, many complex federal and private industrial facilities with contaminated groundwater will require long-term management actions that could extend for decades or longer. As discussed in Chapter 2, the Department of Defense (DoD) manages a substantial number of such sites. Chapter 4 concluded that the further application of existing remediation technologies is likely to provide only incremental progress in achieving restoration at the most complex sites. Thus, for these sites the management challenges include optimization of active remedies, reducing mass flux/mass discharge of contaminants from source areas such that natural attenuation may be effective, or ensuring that any active or passive engineered contain- ment system will remain effective over the long term. This chapter discusses technological developments that can aid in addressing these management challenges—in particular, providing the scientific and technical bases for transitioning from active remediation to more passive strategies where applicable. Optimization of remedial technologies, transitioning to active or pas- sive containment, and improving long-term management can be achieved through (1) better understanding of the spatial distribution of contami- nants, exposure pathways, and processes controlling contaminant mass flux and attenuation along exposure pathways; (2) improved spatio-temporal monitoring of groundwater contamination through better application of conventional monitoring techniques, the use of proxy measurements, and development of sensor-based monitoring technologies; and (3) application of emerging diagnostic and modeling tools. In addition to these topics, the 219
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220 MANAGING THE NATION’S CONTAMINATED GROUNDWATER SITES chapter explores emerging remediation technologies that have yet to receive extensive field testing and evaluation, and it reviews the state of federal funding for relevant research and development and provides recommenda- tions on research topics relevant to the future management of complex sites where groundwater restoration is unlikely. SITE CONCEPTUALIZATION The decision to transition a site from active remediation to long-term management requires a thorough understanding of the geologic framework, history of contamination events, the current location and phase distribu- tion of contaminants, temporal processes that affect groundwater flow and chemical migration, and interactions at hydrogeologic and compliance boundaries. The combined understanding of these factors, referred to here as site conceptualization, supports the development of specific manage- ment tools such as the conceptual site model (CSM, see Chapter 4) and mathematical models. Typically, the site conceptualization and associated tools are updated as the project progresses from discovery of contamination through closure or transition to long-term management, with the degree of detail dependent on the nature of the contamination and the physical dimensions of the site. The development and enhancement of an accurate and suitably detailed site conceptualization is an important component of addressing future management challenges at these sites including the transi- tion to long-term management. The current cleanup paradigm distinguishes the source zone from the downgradient plume, in terms of treating each region differently with re- spect to characterization and remediation, and it acknowledges the domi- nant role of geologic heterogeneity in controlling contaminant removal from both regions. In NRC (2005), hydrogeologic heterogeneity was con- ceptually captured by identifying five generic geologic environments ranging from nearly uniformly homogeneous, unconsolidated porous media (Type I) to fractured rock and carbonate aquifers (Types IV and V). More recently, a 14-compartment model has been proposed (Figure 4-1; Sale and Newell, 2011; ITRC, 2011), in which contaminants can reside in groundwater, sorbed, and vapor phases, either within the source zone or the plume, and which are further subdivided into high- and low-permeability regions. In the high-permeability regions, advective transport will control con- taminant migration, while in the low-permeability regions, the dominant transport mechanism is molecular diffusion. The advantage of such multi- compartment conceptual models is the ability to focus on the exchange of contaminant mass between specific compartments that can limit the rate and extent of remediation, recognizing that the controlling processes can change over time.
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TECHNOLOGY DEVELOPMENT 221 The 14-compartment framework highlights characterization challenges that significantly influence optimization of remedial actions and the tran- sition to long-term management, including the source/plume distinction, spatial heterogeneity in hydraulic conductivity, and the potential role of the vapor pathway when volatile organic compounds (VOCs) are present. A more comprehensive application of the framework that fully accounts for the relative magnitudes of contaminant mass in each of the compartments and the rates of mass transfer between compartments will require further development to better understand (1) the potential roles of desorption and of back-diffusion from low-permeability compartments to advective zones, (2) the variety of aquifer materials and conditions that comprise the “less transmissive” compartments, (3) the reactive characteristics of the aquifer that control the potential success of long-term strategies such as monitored natural attenuation, and (4) the complex factors that control the fate of volatile contaminants, which can exhibit markedly different behavior at seemingly similar sites because of variability in subsurface conditions, building characteristics at the soil interface, and climate conditions. Each of these issues is further explored below. Back-Diffusion and Desorption For many complex sites that have been subject to partial or complete source removal, the transition to long-term management is largely con- trolled by volatilization into the vapor phase (if applicable) and trans- port into the aqueous phase plume, as these two phases are the primary media for both off-site contaminant migration and the biotic and abiotic transformation processes associated with natural attenuation. Current con- ceptualizations of the plume have focused on three potential sources of contaminant mass influx in the groundwater: (1) discharge from undetected mass remaining in the upgradient source zone, (2) aqueous back-diffusion from aquifer materials to the pore water within low-permeability plume material and subsequent diffusive transport to advective zones, and (3) mass transfer (desorption) from aquifer sediments within both transmissive and low-permeability plume materials. For successful transition to long- term management, the contaminant influx from these three processes must be balanced by natural attenuation processes or controlled by physical/ hydraulic containment. The potential loading of dissolved mass from the source zone to the plume has received considerable attention and is straightforward to as- sess because the mass discharge occurs at the boundary of, rather than within, the plume compartment. However, back-diffusion and desorption of contaminants from materials within the plume are much more difficult to analyze because they are spatially nonuniform, dependent on the history
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222 MANAGING THE NATION’S CONTAMINATED GROUNDWATER SITES of the source and plume migration, and are not easily measurable. In par- ticular, measured groundwater concentrations provide only limited insight into the processes responsible for the persistence of dissolved contaminant plumes because it is difficult to distinguish the relative influence of flow field heterogeneity, back-diffusion, and desorption. The potential importance of back-diffusion is supported by conceptual and modeling analysis (e.g., MacKay and Cherry, 1989; Wilson, 1997; Parker et al., 2008) and a limited number of field investigations that have directly sampled aquitard material (Ball et al., 1997; Chapman and Parker, 2005). Sorption processes are typically included in contaminant transport models and estimates of time to remediate, although the common use of the retardation factor reflects the optimistic assumptions of a single sorbent and rapid linear partitioning. A considerable body of research over the past two decades has demonstrated that, for many aquifer materials, sorption pro- cesses are in fact spatially heterogeneous, nonlinear, and potentially limited by solute diffusion to sorbent material located within the interior of soil particles (e.g., as reviewed by Allen-King et al., 2002). As with back-diffu- sion, conceptual and modeling analyses have shown that nonlinear and/or rate-limited desorption can potentially contribute to plume persistence over decades (e.g., Ball and Roberts, 1991; Rabideau and Miller, 1994; Rivett et al., 2006). However, at the time of this writing, there is a lack of field data and characterization techniques to distinguish desorption processes from other nonideal effects. A modest step toward better understanding the potential role of sorption processes would be to routinely characterize the organic content of collected soil samples (Simpkin and Norris, 2010), a task that could be accomplished at relatively low cost. Understanding whether back-diffusion and desorption are occurring at a site is challenging because the relative importance of each process is highly dependent on the site-specific contamination history and the presence and distribution of low-permeability and/or strongly sorbing materials. And yet, current site characterization techniques typically do not fully delineate the structure of these materials, particularly when they are distributed over small spatial scales within the plume interior. Furthermore, there are no proven remedial techniques to preferentially target and accelerate the removal of contaminants from localized sites that are desorption/diffusion limited. Finally, currently used mathematical models are difficult to config- ure to provide realistic predictions of time to remediation when desorption/ diffusion processes are the limiting factor because of the need to assign initial conditions that properly represent the mass located in immobile com- partments. Additional research is needed to develop strategies for long-term management that focus on plume zone processes that contribute to plume longevity rather than the processes that occur in the source zone.
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TECHNOLOGY DEVELOPMENT 223 Representing Complex Geologic Environments The 14-compartment model of Sale and Newell (2011) assigns “low- permeability” compartments to both the source and plume domains, high- lighting the potential role of back-diffusion in both domains. Such an approach is conceptually similar to the classification scheme proposed by NRC (2005), which included a hierarchy of five geologic environments ranging from nearly uniformly homogeneous, unconsolidated porous media (Type I) to fractured rock and carbonate aquifers (Types IV and V). While both schemes distinguish between contaminants in “mobile” and “im- mobile” groundwater, the five-region classification recognizes two subtle but potentially significant differences not captured by the 14-compartment model. First, the diffusion rate and storage capacity of contaminants in low-permeability geologic materials can differ substantially among clays, fractures, and/or intrinsic porosity of indurated rock. Second, in addition to providing potential sinks for diffusive exchange of contaminants, some complex domains (highly heterogeneous unconsolidated porous media, fractured rock, karst) are often characterized by large variations in the groundwater velocity. Hence efforts to characterize “complexity” under- stood in terms of spatial variability must consider both groundwater flow and contaminant transport within and between discrete compartments, regardless of how such compartments are delineated. Differences in the diffusion process are relatively straightforward to account for, but require appropriate specification of the geometry and diffusion characteristics of the low-permeability material. In some cases, the necessary information is provided by field characterization, but for many problems of interest, such as diffusion out of thin clay lenses, the relevant diffusion path length is difficult to determine. Similarly, account- ing for variation in advective transport pathways typically requires a very detailed conceptualization of the groundwater flow field, particularly the low-permeability features. For example, spatial variations in the hydraulic conductivity of unconsolidated media can lead to preferential pathways in aquifers over significant distances, similar to characteristics associated with fractured rock and karst formations. Such paths of preferential ground- water flow often control the distribution of contaminant mass in both source areas and downgradient plumes, and must be properly considered in the design and implementation of containment and remediation strate- gies. Chapman et al. (2010) present an example of how information from detailed site characterization can be incorporated into a remedial design that yields good performance despite the presence of preferential flow paths. However, while available modeling tools are increasingly capable of incorporating detailed descriptions of hydraulic conductivity heterogene-
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224 MANAGING THE NATION’S CONTAMINATED GROUNDWATER SITES ity (e.g., see Guilbeault et al., 2005), the requirements for additional site characterization can represent a considerable burden on site management. Transformation Capacity As discussed in Chapter 7, monitored natural attenuation (MNA) is the dominant process during long-term management at sites not relying on physical or hydraulic containment. Knowledge of the biogeochemical environment and the identification of potentially important reactive path- ways for the target contaminants are necessary prerequisites for initiating MNA after the transition to long-term management has occurred. Relevant considerations include bulk aquifer properties such as mineral composition and pore water chemical constituents, as well as the presence of the neces- sary microbial consortia. Contaminant transformation during MNA can occur through microbial pathways, abiotic mechanisms, or in many cases a combination of both. Of critical importance to the aquifer “transformation capacity” for MNA is the spatial pattern of redox zonation. Redox zonation occurs as a result of microbial metabolism where in a homogeneous system terminal electron acceptors with the most favorable free energies are preferably used before the next one can be utilized (termed the “redox ladder” by Borch et al., 2010). Complex sites, however, may have areas of overlapping or patchy redox zonation whereby microbial communities that utilize differ- ent terminal electron acceptors can co-exist. Determining whether the site is fully oxic, has extensive zones of anoxia, or is comprised of these patchy suboxic/anoxic regions in conjunction with the target contaminant compo- sition is critical to determining the appropriateness of MNA (Rugge et al., 1998; Hofstetter et al., 1999). Another important parameter in contaminant transformation is the presence of reactive minerals associated with aquifer solids, such that characterizing these chemical factors can yield clues about the potential ef- fectiveness of MNA. A variety of naturally occurring iron and manganese oxides, iron sulfide minerals, and clays with iron moieties have been shown to be highly reactive and can act as respective reductants and oxidants in abiotic attenuation pathways (Kappler and Straub, 2005; Hofstetter et al., 2003; Neumann et al., 2009; He et al., 2009). Microorganisms play an important role in the controlling both the type and stability of these minerals since many organisms are capable of utilizing mineral oxides as terminal electron acceptors (Lovley, 1993; Tebo et al., 2004). Under some circumstances the microbial population can convert iron oxides to reactive media useful for MNA by producing Fe(II), which can either be chelated by natural ligands, be adsorbed to the remaining iron oxides to create highly potent reductants, or react with sulfides (if sulfate is in abundance as a ter-
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TECHNOLOGY DEVELOPMENT 225 minal electron acceptor) to produce potentially reactive iron sulfide miner- als (Hakala et al., 2007; Hakala and Chin, 2010). In other cases, however, reduction of manganese oxides (which can mediate oxidation reactions) may result in a decrease in potential MNA. In aquifer pore waters, reactive species such as natural organic matter and reduced sulfur species (bisulfide, polysulfides, and organic thiols) play an important role in MNA by act- ing as reductants and electron mediators (Kappler and Haderlein, 2003; Hakala and Chin, 2010). Natural organic matter significantly increases the reactivity of reduced sulfur species by acting as an electron mediator, and is an important reductant in sulfur-rich aquifers (Dunnivant et al., 1992). An example of a well-characterized site with high transformation capacity amenable to MNA is Altus Air Force Base, which has abun- dant levels of both sulfate and Fe(III) (Kennedy et al., 2006). Microbial metabolic activity at this site produced potent reactive reductants such as reduced sulfur compounds, Fe(II), and iron sulfide minerals, which were capable of abiotically transforming TCE and its derivatives. These inves- tigators reported the absence of sulfate in the area of the TCE plume and the existence of abundant iron sulfide minerals. Further they found no TCE in the area where iron sulfides are abundant and only trace levels of by- products, suggesting that MNA was occurring. While much is known about the biological/abiotic conditions neces- sary to effect contaminant transformation during MNA, there is not yet a complete protocol to determine the extent to which such conditions are present at a site and whether contaminants are being degraded. The tools discussed later in this chapter represent important initial steps toward the development of such a protocol. Vapor Intrusion Issues As described in Chapter 5, the vapor intrusion pathway is increasingly considered at complex sites with DNAPL contamination. This pathway can be conceptualized as three distinct zones (Figure 6-1): (1) the source zone where contaminant is immobilized, (2) the subsurface migration pathway, and (3) the influence zone of the building. The management of vapor in- trusion requires expanded site characterization, an interpretation of the several types of vapor concentration measurements in the context of site- specific conditions, and, if necessary, development of appropriate mitigation strategies if source removal measures are insufficient to reduce exposure to acceptable levels. Characterization of the vapor pathway is challenged by the fact that each component is subject to considerable spatial and temporal variability. Fluctuating water table conditions controlled by recharge, pumping, and stream–aquifer interactions can result in transient vapor flux generation at
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226 MANAGING THE NATION’S CONTAMINATED GROUNDWATER SITES FIGURE 6-1 Vapor intrusion pathways. the sources. The migration pathway from source to building is significantly affected by changes in soil moisture, temperature, wind, and ambient pres- sure, and in some cases, biogeochemical transformation processes. Vertical migration is also influenced by changes in building ventilation and heating, ventilation, and air conditioning systems operation. Finally, attempts to characterize the pathway via indoor air sampling can be confounded by indoor sources of contamination. Among the available guidance for assessing vapor intrusion (e.g., Johnson et al., 1999; Hay-Wilson et al., 2005; McAlary et al., 2005; NYSDOH, 2006; ITRC, 2007), federal guidance is evolving toward an ap- proach based on multiple lines of evidence that involves sampling of indoor air, subslab soil gas, deeper soil gas, groundwater, and soil—in combination with screening-level modeling and empirical assessment (e.g., EPA, 2002, 2011a,b, 2012a,b,c). This reflects experiences with conflicting lines of evi- dence at some sites, recognition that there will likely be spatial variability in pathway sampling results, low confidence in our ability to correctly in- terpret the data, and a limited peer-reviewed knowledge base to rely upon. This also suggests that assessment paradigms that rely on too few samples (in space and time) are limited. Vapor intrusion from groundwater plumes with chlorinated solvents is especially challenging to characterize, partly because such plumes can vary widely in size. Where large plumes encompass an entire neighbor- hood, assessment of all potentially affected buildings may be impracticable. Furthermore, it is not always the case that the greatest indoor air impacts are found in buildings overlying the highest groundwater concentrations. Groundwater-related vapor intrusion has been documented in some build- ings overlying dissolved chlorinated solvent groundwater concentrations as
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TECHNOLOGY DEVELOPMENT 227 low as 10 µg/L, and no impacts have been observed in other buildings over- lying groundwater concentrations as great as 10–100 mg/L (EPA, 2012b). A number of commercial products can serve as indoor sources of chlorinated solvent vapors, so that interpreting indoor air quality and sub- slab soil gas data is not always straightforward (Gorder and Dettemmaier, 2011). As a case in point, approximately 3,000 residences overlie chlori- nated solvent groundwater plumes originating from Hill Air Force Base, although monitoring has indicated that a very small percentage of the resi- dences have indoor air impacts attributable to groundwater contamination. Detailed study beyond typical pathway assessment monitoring identified numerous indoor air sources of contaminants, including household cleaning products, craft supplies, gun cleaners, and holiday ornaments—leading to a list of 72 household products known to contain TCE and almost another 2,000 products known or suspected of containing chlorinated solvents. A solid technical basis is lacking for determining which scenarios re- quire indoor sampling and what sampling frequency and duration are appropriate, both over the short term (i.e., daily) and long term (i.e., sea- sonal). Studies suggest that vapor intrusion emissions into buildings can fluctuate on time scales ranging from days to weeks (Luo, 2009; Luo et al., 2010; Johnson et al., 2012). Research by McHugh et al. (2010) suggests that changes in indoor air concentrations may be different for chemicals emanating from groundwater than those emanating from indoor chemi- cal sources, such that temporal data might be used to distinguish between indoor air impacts from these two sources. However, even with detailed indoor air monitoring data, the issue of temporal variability is further complicated by the dynamics of volatilization from the groundwater plume, which is affected by groundwater table elevation, moisture infiltration rates, moisture profiles, and other climate factors (Sakaki et al., 2013). In general, the temporal changes in the vapor emission rates from groundwater have yet to be studied in great detail and further study is needed to more intel- ligently design sampling plans. Because the costs and complexity of vapor intrusion assessment have been increasing without a commensurate increase in the mechanistic under- standing of the exposure pathway, the resulting response actions reflect a conservative management approach. MONITORING Monitoring of groundwater is conducted over the entire life cycle of a complex site and can represent a significant percentage of life-cycle costs if residual contamination remains after active remediation has been com- pleted, especially when monitoring extends over multiple decades. Tradi- tionally, the monitoring of temporal changes in groundwater contamination
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228 MANAGING THE NATION’S CONTAMINATED GROUNDWATER SITES relied on conventional well sampling, which is labor intensive and requires costly laboratory analyses. Given that tens to hundreds of monitoring wells are present at most sites, and standard quarterly sampling is often required, estimates of monitoring can exceed $100 million per year at DoD facilities alone, which represents a significant percentage of the financial resources dedicated to remediation efforts. Furthermore, the traditional two-dimensional resolution of monitoring well networks (which produce vertically averaged concentration values) may be insufficient to support an accurate site conceptualization, particularly for highly heterogeneous formations. Continued development of conventional monitoring techniques has led to more detailed characterization of the distribution of dissolved con- taminants, particular in the vertical dimension. However, to support a cost- effective transition to long-term management, additional tools are needed. This section addresses ongoing developments in (1) optimization of con- ventional monitoring systems, (2) techniques for measuring contaminant flux, (3) sensor technology, and (4) new tools that can be applied to better understand whether MNA is working. Improved Application of Conventional Monitoring Tools The deployment of conventional site characterization tools has evolved in a manner that has emphasized greater spatial resolution in regions where contamination is significant. In particular, multi-level monitoring and nested well systems now enable the collection of hydraulic head data and groundwater samples over relatively short vertical intervals (ITRC, 2004; Einarson, 2006; Einarson et al., 2010; Kavanaugh and Deeb, 2011). Although more costly than conventional 2-D monitoring, multi-level moni- toring systems can lead to more streamlined and accurate remedial investi- gations and long-term management. Formal simulation/optimization techniques have been developed to improve the design of monitoring programs—a process sometimes termed long-term monitoring optimization (LTMO). These applications are in a relatively early stage of development and a variety of approaches are avail- able to formulate and solve the optimization problem. For example, one approach might be to analyze the value of information provided by an existing monitoring network to identify monitoring wells that are spatially redundant and could be removed (e.g., Reed et al., 2000, 2001; Babbar- Sebens and Minsker, 2008). Most work to date has focused on monitoring frequency and spatial resolution of well networks, with less attention given to issues such as the number and selection of analytes, sampling analytical techniques, and data processing. In a pilot study comparing two software- driven LTMO systems, the U.S. Environmental Protection Agency (EPA)
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TECHNOLOGY DEVELOPMENT 229 suggested that annual savings of a few hundred to tens of thousands of dollars might be achievable, particular for sites where more than 50 samples are collected and analyzed annually (EPA, 2004). EPA subsequently issued a “road map” to assist managers with developing a site-specific LTMO program (EPA and USACE, 2005), including user-friendly software tools. Although the underlying concepts are fairly well established, additional documentation of successful case studies would clarify the range of poten- tially achievable cost savings. Monitoring of Source Zone Contamination The successful design of a source zone remediation program depends on sufficiently detailed knowledge of the spatial pattern of immobile source materials. A number of recent reviews have evaluated the variety of tools available to quantify the magnitude and spatial distribution of DNAPL (e.g., NRC, 2005; Mercer et al., 2010). These tools range from low-cost methods to infer the presence of DNAPL (as reviewed by Kram et al., 2001) to more extensive methods designed to delineate the spatial distribution of NAPL saturation to guide source zone remediation (e.g., Saenton and Illangasekare, 2004; Moreno-Barbero and Illangasekare, 2005, 2006). For the latter purpose, the partitioning interwell tracer test (PITT) has proven to be relatively effective (e.g., Annable et al., 1998; Brooks et al., 2002), although its deployment is hindered by high cost and need for relatively sophisticated interpretive tools. As it is unlikely that complete removal of contaminant source mate- rial will be feasible for many complex sites, the transition to long-term management will depend not only on the amount of source mass removed, but on the rate at which mass is transferred between the source and plume compartments during the post-remediation period. One of the most prom- ising recent developments in source zone management is the development of tools for measuring contaminant mass flux, either at localized monitor- ing points or as an integrated mass discharge across a control plane. Such knowledge of contaminant discharge is particularly useful in evaluating the potential for downgradient natural attenuation processes. Conceptually, contaminant discharge is a calculated parameter that reflects both temporal and spatial averaging of the product of groundwa- ter discharge (length per area per time) and contaminant concentration (mass per volume). Field methods include synoptic sampling (e.g., Einarson, 2006), passive flux meters (Annable et al., 2005; Basu et al., 2006), steady- state pumping (e.g., Buschek, 2002), recirculation flux measurements (Goltz et al., 2007), integral pumping tests (Bockelmann et al., 2001; Bauer et al., 2004), and modified integral pumping tests (Brooks et al., 2008). The use of flux measurements as an alternative to concentration-based metrics
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