Project 3 PTP for 2012 - doeresearch.fiu.edu Project 3 Appendices/P3...PROJECT TECHNICAL PLAN . Project 3: Remediation and Treatment Technology Development and Support for DOE Oak

PROJECT TECHNICAL PLAN

Project 3: Remediation and Treatment Technology Development and Support for DOE Oak Ridge Office

For the period May 18, 2012 to May 17, 2013 CONTRACT NO. DE-EM0000598

U.S. Department of Energy Program Services Division, ME-643.1

1000 Independence Avenue, SW Washington, D.C. 20585

Leonel Lagos, Ph.D., PMP®

David Roelant, Ph.D., Principal Investigator , Principal Investigator

Georgio Tachiev, Ph.D., P.E., Project Manager Applied Research Center

Florida International University 10555 W. Flagler Street, EC2100

Miami, FL 33174

June 18, 2012

Submitted to:

Submitted by:

Submitted on:

Applied Research Center - FY2012 Project Technical Plan Remediation & Treatment Technology Development & Support for DOE Oak Ridge Office 1

INTRODUCTION

Approximately 75 to 150 metric tons of elemental mercury was released into East Fork Poplar Creek (EFPC) watershed as a result of a lithium-isotope separation process used for the production of nuclear fusion weapons at the Y-12 National Security Complex (Y-12 NSC) in Tennessee. Under natural environmental conditions, elemental mercury is oxidized to mercuric

ion which has considerably greater solubility and a greater potential to be mobilized by water and contaminate the environment of the Oak Ridge Reservation (ORR). Mercury has a high affinity to form complexes with organic and inorganic ligands, which additionally increases the potential for migration of mercury species and subsequent contamination of the surface and groundwater. During FY08 – FY11, FIU developed integrated flow and transport models of the East Fork Poplar Creek (EFPC) and White Oak Creek (WOC) watersheds to analyze the mercury transport patterns within the ORR domain. The models were applied to determine the effect of historical hydrological events on mercury transport within the relevant watersheds and to determine the efficiency of selected remedial alternatives. Laboratory experiments were conducted to determine more information on the significant parameters related to mercury transport, reaction, and speciation (e.g., methylation/demethylation kinetics) within the watershed.

During FY11, the model, which was developed for the Y-12 NSC, was extended to include the EFPC watershed and the creek between Y-12 NSC and Station EFK 6.4. The research focused on conducting additional simulations using the EFPC watershed model which extend the studies for Y-12 NSC and provides information about the contamination along EFPC. In addition, flow and transport studies were conducted for the Bear Creek watershed (a sub-watershed of the larger EFPC watershed). A geodatabase was developed as a strategy for supporting hydrological model data input by creating a centralized data storage system to store model parameters. The database extends the capabilities of the GIS data and allows for automating time consuming GIS processing for water resources applications.

DOE EM HQ Contacts: Kurt Gerdes G. (Skip) Chamberlain Justin Marble Mark J. Williamson DOE Site Contacts: Elizabeth Phillips, DOE ORO Eric Pierce, ORNL Liyuan Liang, ORNL Dave Watson, ORNL Donald Metzler, Moab, Federal Project Director, U.S. Department of Energy Grand Junction Richard Ketelle, RIS ARC Program Contacts: Georgio Tachiev, Project Mgr, Sr. Research Scientist (305) 348-6732 E-mail: [email protected] Leonel E. Lagos, Ph.D, PMP®., Principal Investigator (305) 348-1810, E-mail: lagosl@ fiu.edu David Roelant, Ph.D. Principal Investigator, Associate Director (305) 348-6625, E-mail: roelantd@ fiu.edu Applied Research Center Florida International University 10555 W. Flagler St., Suite 2100 Miami, FL 33174

2 Applied Research Center – FY2012 Project Technical Plan Remediation & Treatment Technology Development & Support for DOE Oak Ridge Office

OVERVIEW OF WORK ACCOMPLISHED DURING FY11

During FY2008-2011, FIU developed integrated flow and transport models of East Fork Poplar Creak (EFPC), Upper EFPC and White Oak Creek (WOC) watersheds and conducted numerical modeling and reviews of monitoring data available from OREIS and related to mercury (Hg) contamination and remediation within these watersheds. In addition, experimental studies provided experimental kinetic and equilibrium data about important parameters related to Hg transport, speciation and methylation/demethylation kinetics within the watershed.

• A Draft Project Technical Task Plan was submitted on 08/12/2011. • PowerPoint presentations were delivered to DOE personnel and site contractors during

ORR site visits in November 2011 and to ORNL personnel (Dr. Eric Pierce and Dr. Liyuan Liang) during a visit to the Applied Research Center in February 2012. The presentations covered the following:

o Introduction to the FIU Water Resources and Environment Research Group o A summary of FIU’s work to date o Hydrologic modeling of surface, groundwater and river sedimentation including

WOC, EFPC, Y12-NSC and Building 81-12 o Fate and transport of contaminants o Support for remediation activities o Benchmarking, sensitivity and uncertainty analysis o Experimental mercury speciation studies o Results o Path forward

• Project factsheets were prepared in February 2012, which summarized the research conducted under each individual subtask. Several were distributed during the Waste Management 2012 conference.

• The results from the project work were submitted to peer review journals and conferences:

o A peer reviewed article entitled, “Simulation of Flow and Mercury Transport in Upper East Fork Poplar Creek, Oak Ridge, Tennessee,” has been published in the Spring 2012 edition of the Remediation Journal.

o Best Professional Poster for Waste Management 2011 was awarded to “Simulation of Flow and Mercury Transport in Upper East Fork Poplar Creek, Oak Ridge, TN.” A related paper was also submitted to the conference. This research was associated with development of the integrated surface and groundwater model for flow and mercury transport at EFPC. The model is being developed and used to predict transport patterns of mercury and evaluate risks during deactivation and decommissioning of mercury contaminated facilities at the Y-12 National Security Complex in Oak Ridge, TN.

o A first place in track 7 “Remediation” was awarded to “Groundwater Transport of Organic Compounds in Old Salvage Yard, Oak Ridge, TN”, which was presented


at the Waste Management Symposium 2012. A related paper was also submitted to the conference.

o A poster was also submitted by DOE Fellow, Lilian Marrero, on “Improvements in the Suspended Sediment Interactions Module of an Integrated Flow and Mercury Transport Model for East Fork Poplar Creek Watershed, Oak Ridge, TN (12588).”

o A paper entitled, “Migration of Plume of Organic Compounds in a Highly Fractured Subsurface Domain,” was submitted to the Ground Water Journal and is currently under review.

o A review paper entitled, “Progress in the study of mercury methylation and demethylation in aquatic environments,” authored by Yanbin Li and Yong Cai, was accepted for publication in Fall 2012 in the Chinese Science Bulletin.

o A paper entitled, “Estimation of the Major Source and Sink of Methylmercury in the Florida Everglades,” was published in the Environmental Science and Technology Journal online on April 26, 2012 (DOI: 10.1021/es204410x).

o A paper entitled, “Degradation of Methylmercury and Its Effects on Mercury Distribution and Cycling in the Florida Everglades,” was published in the Environmental Science and Technology Journal in November 2010.

o A paper entitled, “Spatial Variability in Mercury Cycling and Relevant Biogeochemical Controls in the Florida Everglades,” was published in the Environmental Science and Technology Journal in May 2009. During FY11 the following research tasks were completed:

• The following technical reports were completed: o Task 1, “EFPC model update, calibration, uncertainty analysis” (November

2011).

o Task 2, “Simulation of TMDL for entire EFPC” (February 2012).

o Task 3, “Parameterization of major transport processes of mercury species” (May 2012).

o Task 4, “Geodatabase development for hydrological modeling support” (March 2012).

o Task 5, “Student support for modeling of groundwater flow and transport at Moab, UT site” (February 2012).

o “Preliminary studies of nitrogen concentration in wells 0437, 0438, and 0439”, based on a DOE Fellow (Mr. Alex Henao) summer internship at the Moab Site in support of Task 5 (November 2011).


TECHNOLOGY NEEDS

The Clean Water Act and associated regulations require each state to determine which waters do not meet applicable water quality standards according to their uses. Computation of contaminant distribution within a watershed domain requires an integrated surface and subsurface flow model, which includes sedimentation processes along the creek. In order to extend the development of TMDLs onto other locations in the watershed, and provide a better understanding of the discharges and Hg concentrations along the stream reaches (EFPC and Bear Creek) of the EFPC watershed, hydrological and transport simulations are required. The computer simulations provide a forecasting capability and estimate load changes as a function of hydrological events.

Sequestered mercury species in solid matrices, which are often known to be relatively stable, could be released as dissolved and/or colloidal species into the solution phase and thus contribute to the aquatic cycling of mercury. The redox potential and presence of organic ligands may affect the stability of elemental mercury beads and the distribution of released mercury species. The role of mercury migration from solid to solution in the mercury cycle, and the correlation between mercury mobilization and environmental chemical processes, needs to be better understood.

A geodatabase is needed to address the management, processing, and analysis of spatial and temporal numerical modeling data. The development of an ArcSDE geodatabase will facilitate the centralized storage, backup, accessibility, organization, and management of model configuration and computed simulation data, and will put it into a structured, coherent, and logical computer-supported system. The hydrologic geodatabase model used in this project possesses a structure that enables linkage with scalable hydrologic modeling tools, applications to model hydrologic systems, and in this case, enables the testing of the potential impacts of various D&D scenarios on the ORR watersheds. The ArcSDE geodatabase can be used to automate and simplify the process of calling stored GIS and timeseries data. This geodatabase can also serve as a tool for contaminant flow and transport analyses which require large amounts of high-quality spatial and temporal data in order to ensure reliability and validity of modeling results.


PROJECT EXECUTION PLAN

PROJECT TASKS

The overall objective of this project is to provide technical assistance and perform research in support of the remediation efforts at the Oak Ridge Reservation. For FY2012, FIU is proposing a scope which relies on previously developed models of EFPC to provide simulation of fate and transport of contaminants and remedial activities. Stochastic analysis will be extended to the entire EFPC and will include hydrological and transport data along EFPC. A detailed mass balance will be developed for the site for contaminants of concern, including inorganic (Hg) and organic contaminants. The work will provide insight on the contribution of each outfall to the load at Station 17. The laboratory work will be continued with additional studies to determine experimental parameters related to cinnabar dissolution and contribution for mercury distribution between various phases (aqueous and soil) for different environmental factors including pH, dissolved oxygen, dissolved organic matter, organic and inorganic content of soils and pore water, on mercury fate and transport within the creek and for overland flow. The work will provide a better understanding of the mercury dynamics within the Oak Ridge Reservation watersheds (EFPC, Y-12 NSC, Bear Creek, White Oak Creek) for variable environmental conditions and for specified remediation alternatives. Student support will be provided for numerical modeling of subsurface flow and transport. Research efforts will be executed in collaboration with DOE EM and DOE ORO. The proposed work has 5 tasks which are described in greater detail below.

Figure 1. EFPC Watershed Model Domain


Task 1: EFPC Model Update, Calibration, Uncertainty Analysis Background

An integrated surface/subsurface flow and transport model of EFPC watershed was developed to analyze the mercury transport patterns within the ORR domain. For the development of the hydrology model, historical measurement records including the timeseries for precipitation, evapotranspiration, groundwater levels, and river discharges were obtained from the OREIS and ORNL databases and incorporated into the MIKE model as boundary conditions. The hydrological model was calibrated and then validated by comparing the computed discharges and water levels with the historical records at selected monitoring stations (the outfalls listed in the NPDES document for Y-12 NSC). Uncertainty and sensitivity analyses were performed for critical hydrological parameters such as the Manning number, and the vertical and horizontal hydraulic conductivities of each of the five geologic layers.

In the second phase, the transport component of the model was developed. The model enables full dynamic coupling of surface and subsurface flow processes, and allows the calculation of water and contaminant exchange between the rivers and the groundwater. The subsurface model uses the dual porosity option to describe solute transport in both the fractures, and in the aquifer matrix. The exchange of mass between the fractures and the matrix is described by a diffusion process, and the mass transfer coefficient controls the rate of solute exchange between the two phases. The sorption in the unsaturated zone was represented as an equilibrium or kinetic equilibrium process using linear or nonlinear (Freundlich, Langmuir) sorption isotherms. Experimental work conducted at FIU provided a range of values for the partitioning coefficient of mercury using soils collected from UEFPC soils and literature data. The transport component of the model was calibrated using the historical records collected at selected monitoring stations in EFPC.

The main objectives of this task are to extend the existing EFPC model by adding sedimentation and reactive transport modules, and to use the model to perform numerical simulations that are relevant for the NPDES and TMDL regulations. The simulations provide a better understanding of the flow and transport within the watershed on a regional scale. Simulations were conducted using historic observations of rainfall, evapotranspiration, and contaminant distribution within the watershed to determine transport patterns within the domain. During FY11, the focus was on extending the sedimentation module to include the entire EFPC and Bear Creek. This research has also provided stochastic modeling of the system and has included an analysis of the spatial and temporal patterns as a result of the stochastic variations of selected properties of the sub domain. FIU will continue using the numerical model of EFPC to determine the impact of remediation alternatives on the complete hydrologic cycle, the transport overland and in surface water and rivers, sediment transport and reactions, and mercury exchange with sediments. The research will be coordinated with the site and ORNL personnel.

Technical Approach

FIU will use the numerical model of EFPC to determine the impact of remediation alternatives on the complete hydrologic cycle, the transport overland and in surface water and rivers, sediment transport and reactions, and mercury exchange with sediments. The research will be


coordinated with the site and ORNL personnel. The major objective of this task is to provide analysis of the coupling between hydrology and mercury transport within the context of decreasing the risk of D&D activities. The major deliverable of this task will be numerical and stochastic analysis of observed and computed time series for flow and contaminant concentration for NPDES-regulated outfalls within the watershed. Model simulations will be used to account for a range of hydrological impacts related to planned remediation alternatives. A variety of simulations will be executed to assess the impact of Manning’s M within the EFPC Model. Similarly simulations for the EFPC model will be executed for a series of parameters within the ECO Lab module. Input parameters are kept constant during the simulation and varied per run.

1. Subtask 1.1: Statistical analysis of observed data and development of timeseries, probability exceedance curves, and probability distribution models of flow, concentration and load data that integrates already downloaded data, and new data that will be obtained from contactors with the support of ORNL personnel. The data will include groundwater well monitoring, concentrations in groundwater wells, outfall flow, and concentration and load data. The task will also provide a refinement of the existing EFPC model by inclusion of historical outfall flow data for the area extending from WEMA to Station 17 to determine the effects of precipitation and stormwater drainage on the flux of mercury into EFPC. The deliverable of this subtask will include timeseries, probability exceedance curves, load exceedance curves, probability distribution models for each monitoring point and a report. The subtask will provide support for the team developing the mercury conceptual model and will provide considerably better estimates for the stochastic nature of mercury fluxes within the EFPC domain.

2. Subtask 1.2: Reduction of model parameter uncertainty (i.e., uncertainty analysis) for existing EFPC model via a series of probability distributions derived from running multiple simulations for selected specified parameters. In the previous scope the major variables were the hydraulic conductivities of each of the five geological layers. The current scope will focus on analysis of the upper layer and the leakage factor between the creek and subsurface media, and on the exchange of flow and mercury between the creek and the river. Uncertainty analysis will be provided for the parameters governing the distribution of mercury species within pore water, sorbed mercury within pores, sorbed mercury on suspended particles and "free" mercury (dissolved and chelated mercury species). The major variable that will be analyzed will be total mercury considering that all regulatory documents are expressed as total mercury. The work in this subtask will help to improve the confidence in the predictive capability of the watershed-scale model. The deliverables from this task will include analysis of the uncertainties associated with the parameters governing exchange of mercury within each of the subdomains (mercury migration in the vadose zone during flooding, pore space in the sediments, sorption on sediments, sorption on particles, and aqueous species) and a report.

In order to effectively calibrate the variables for the model, flow and load duration curves constitute a valid tool for the analysis of data. A flow duration curve (FDC) represents the relationship between the frequency and the magnitude of the flow in a particular stream. Load duration curves (LDC) will be constructed by multiplying daily mean flow by the observed concentration of suspended solids in the water, as measured in respective stations. LDCs for mercury may also be developed, by multiplying daily mean flow by


the observed concentration of mercury in the water, as measured in stations. FDCs for the EFPC model using observed data from the OREIS database will be developed for Station 17 and the additional station provided by ORNL depending on the applicability of the data provided. Calibration will be carried out for parameters affecting the calculation of the total suspended solids in the system and parameters affecting mercury concentrations and transport. In ECO Lab the four input parameters that directly affect the concentration of total suspended solids (TSS) include critical current velocity (vc), settling velocity (vs), resuspension rate (RR), and particle production rate (PPR). Simulations for the EFCP Watershed scale model will be executed and an analysis will be performed based on load duration curves for both suspended solids and total mercury.

3. Subtask 1.3: Re-creation of the existing ORNL stormwater management system layout via a numerical surface water one dimensional model (SWMM or similar) to provide a better understanding of the flow patterns on-site, including flow rates as a function of rainfall intensity and the fraction of drainage volumes and rates reaching each outfall. The objective is to create a detailed surface water flow and contaminant transport model for the ORNL area using XPSWMM, incorporating flow data and other significant drainage system parameters, initially starting with a smaller model for the ORNL area. This would be a benchmark study to be extended to the Y-12 NSC (once reviewed and accepted by ORNL and the site). The deliverable of this subtask will be a calibrated and validated drainage model that will provide detailed analysis of how much water reaches each outfall and the source of the water. By providing better understanding of the drainage system, the site will be provided with a tool that can be used to investigate the best remediation scenarios for setting up remediation priorities, e.g., helping identify the greatest contributors to mercury loads.

4. Subtask 1.4: Simulations of surface water flow and contaminant transport utilizing collected piezometric data for EFPC. This will facilitate calibration and validation of the existing EFPC model developed by FIU and will provide data for comparison with new measurements to be taken by ORNL in their effort to refine the existing conceptual model for EFPC. This task will be executed in collaboration with ORNL. Additionally, modifications of the flow hydrology along EFPC, including reduction of the flow augmentation, addition of a down-gradient diversion ditch, alternatives which result in reduced mercury fluxes in major outflows and simulation of flow and transport of other contaminants whose partitioning coefficients vary several orders of magnitude (including uranium and other contaminants of interest) will be investigated within this subtask. The following approach will be taken for the data provided by ORNL:

- Data will be processed for validity and categorized into spreadsheets. - New stations will be added to GIS maps of the site. - Timeseries files will be developed and input into the model. - Model nodes, cross-sections, and boundaries may be modified if necessary due to the

addition of new observation stations.


Task 2: Simulation of NPDES- and TMDL-Regulated Discharges from Non-Point Sources for the EFPC and Y-12 NSC Background During FY11, the numerical model of UEFPC watershed which was developed by FIU-ARC to simulate fate and transport of mercury, conservative tracers and VOC plumes within the watershed based on several remediation scenarios was extended and applied to the entire EFPC watershed to determine the contribution of each subdomain component to the overall contaminant loads of the watershed streams, and to assist in analyzing the NPDES and TMDL requirements for surface water and groundwater within the EFPC watershed. In FY12, FIU will use the EFPC model and will work with the site to provide numerical analysis of contaminant flow and transport within the EFPC and Y-12 NSC watershed and to determine the impact of model parameters on the TMDL. A major focus will be on ecosystem responses to variations in contaminant loading (changes in external and internal loading in time and space), and how imminent ecosystem restoration may affect existing contaminant pools. Technical Approach During FY12, FIU will use the previously developed EFPC model and will work with the site to provide numerical analysis of contaminant flow and transport within the EFPC and Y-12 NSC watershed and determine the impact of model parameters on the TMDL. In addition, this task will determine the effect of the hydrological events (including changes in hydrology caused by D&D activities on the site) on contaminant loading (changes in external and internal loading in time and space), and how imminent ecosystem restoration may affect existing contaminant pools. Work proposed for FY12 includes the following subtasks.

1. Subtask 2.1: Modeling of previously proposed actions to facilitate IFDP and meet load discharge standards at Station 17. Modeling will be performed with an already calibrated and verified model using the commercial flow and transport software MIKESHE/MIKE 11. The model was developed as part of the scope in FY2011. The emphasis will be on stochastic analysis of the load reduction effects resulting from remedial actions. The task will provide a series of simulations to analyze each action. In addition, major parameters will be varied (such as hydraulic conductivity of the upper layer, rainfall intensities, evapotranspiration values, parameters of the vadose zone) to characterize the impact of each action on the loads at Station 17 and the associated uncertainties. The deliverable of this subtask will include development of probability exceedance curves for each scenario; this data will provide additional insight of the effect for the entire range of hydrologic regimes (very wet to very dry conditions). The task will study the modifications of the hydrology which limit the amount of overland flow over site surfaces, and limit the infiltration of rainwater through areas with underlying mercury contamination.

2. Subtask 2.2: Analysis of the risks associated with the inorganic contaminants including uranium and mercury (the list of contaminants can be easily expanded using the same flow model and by applying the correct thermodynamic and reactive properties). The task will additionally provide analysis of the geochemical and engineering properties of various mixtures of structural (flowable) fill for Oak Ridge Reservation EM Scope Projects and in support of the IFDP D&D activities. The aim is to determine the efficacy of plugging and abandoning storm drains that contain mercury sediments at the Y-12


Complex and creating a structural fill in basement air spaces for supporting heavy demolition equipment. In addition, the testing of fill should allow a determination of whether liquid elemental mercury and high concentrations of mercury in soil beneath the facilities can be hydraulically isolated and geochemically sequestered. The analysis will be performed with collaboration from ORNL and the site and will provide understanding of the potential point and distributed sources of inorganic and organic contaminants that are coupled with hydrological events and D&D activities.

Task 3: Parameterization of Major Transport Processes of Mercury Species Background

Mercury occurs in a variety of species, such as elemental mercury (Hg0), mercury sulfide (HgS), mercury (hydr)oxides (e.g., HgO and Hg(OH)2), ionic mercury salts (e.g., HgCl2), and methylmercury (MeHg), in the environment. At historically mercury contaminated sites (e.g., the DOE Oak Ridge site), the originally discharged mercury would undergo complicated aging processes in the environment and eventually be sequestered in the soil and sediment in relatively stable forms (e.g. mercury bead and HgS). The mercury species sequestered in soils and sediments is generally considered low in solubility and reactivity, which prevents this mercury from being released into the solution and from being transported into the aquatic environment. Despite the limited solubility, mobility, and reactivity, the aged mercury species in soils and sediments may undergo a series of physical and chemical processes under certain environmental conditions, releasing dissolved mercury species into the solution. Cinnabar has often been suggested to act as an important sink for mercury in soils and sediments because of its extremely low solubility product [1,2]. However, recent studies suggested that cinnabar can also release mercury to environment, which could be promoted by the oxidization of S(II) by Fe(III)-(hydr)oxides or dissolved oxygen (DO) [3-9] and the presence of ligands such as sulfide, polysulfides, NOM (e. g. natural organic matter), and chloride in the environment [3,10-13]. The dissolution of cinnabar is an important process of Hg cycling in aquatic environments as it can provide a sufficient and continuous source of inorganic mercury and subsequently enhance the production of a more toxic species of Hg, methylmercury (MeHg).

Bioavailability of Hg species is among the most important factors that determine the production of MeHg in the environment. Previous studies showed that measured Hg methylation rates were usually positively correlated not to the total Hg2+ concentrations, but to the calculated concentrations of Hg2+ available for methylation [14-16]. It is also known that the newly deposited Hg2+ are more bioavailable for methylation compared to the legacy Hg2+ in sediment

[17]. The bioavailability of Hg species in aquatic ecosystems is mainly determined by two processes: 1) distribution of Hg between solid and aqueous phase, and 2) speciation of Hg species in water phase. Factors affecting these two processes will determine the bioavailability of mercury species in the environment. The adsorption/desorption of Hg species is known to be affected by a variety of factors in aquatic environments, e.g., pH, redox potential, salinity, organic and inorganic complexing reagents, composition of solid. These factors are expected to play an important role in controlling the bioavailability of Hg2+ in aquatic environments. Hg2+ and MeHg in aquatic environments are generally not free ions, but complexed to various inorganic and organic ligands, including hydroxide, chloride, sulfides, and DOM [18]. The


dominant species of Hg2+ and MeHg in water or porewater depends upon various physical and chemical parameters, e.g., pH, Eh, sulfide, Cl-, and DOM [18-22]. As not all of these complexes are available for methylation and demethylation, speciation of Hg species in water and porewater is another important factor determining bioavailability of Hg species.

The overall objective of this task is to provide laboratory measurements for critical mercury (Hg) transport, transformation, and exchange processes (i.e., methylation/demethylation, and dissolution) to be used in the numerical model. The laboratory experimental work will provide insight on parameters relevant to the Oak Ridge Reservation (ORR) and which are required in the numerical model, such as dissolution rate of mercury and the proportion of mercury species available for methylation/demethylation in sediments. In addition, experimental work will be conducted to analyze the effect of significant environmental factors (pH, Eh, sunlight) on the major transport and transformation processes of Hg.

Technical Approach

Experimental activity conducted during FY2011 has revealed that: 1) the percentage of Hg species available for methylation or demethylation is a critical parameter for evaluating the production and degradation of MeHg in aquatic ecosystems, 2) dissolution of cinnabar can significantly increase Hg concentrations in water and thiols can promote this process, and 3) thiol-containing compounds may enhance cinnabar dissolution by inhibiting the adsorption of released Hg2+ on cinnabar, rather than directly increasing the solubility of HgS. The proposed FY12 scope for this task will continuously focus on understanding the bioavailability and dissolution of aged Hg species in soil and sediment. A series of studies will be conducted in FY12 to:

1. Examine the effects of environmental factors (e.g, pH, Eh, mineral oxides, water content, NOM (natural organic matter)) on the percentage of legacy Hg species available for methylation/demethylation in sediment;

2. Validate the proposed mechanism of thiol promotion of Hg dissolution in FY11.

3. Examine the effects of NOM and other complexing reagents (e.g., Cl-) on the dissolution of cinnabar.

These objectives will be accomplished via the following tasks:

1. Subtask 3.1: Effects of environmental factors on the percentage of legacy Hg species available for methylation and demethylation in sediment: The stable isotope addition method will be employed in incubation experiments to measure the ratios of methylation/demethylation rate constant of legacy to newly input Hg. 199Hg2+ or Me199Hg will be spiked to sterilized sediments with various levels of pH, mineral oxides, water content, or NOM. After stabilizing for approximately 2 month (199Hg2+ and Me199Hg will be then treated as legacy Hg), 201Hg2+ or Me201Hg and another aliquot of unsterilized sediment will be added to the samples. Samples will be incubated under anaerobic conditions for 2 days to measure the methylation/demethylation rates of both legacy (199Hg2+ and Me199Hg) and newly spiked (201Hg2+ or Me201Hg) mercury species. Concentrations of Me201Hg and Me199Hg in samples will be determined using aqueous


phenylation followed by gas chromatography hyphenated with inductively coupled plasma mass spectrometry (GC-ICP-MS).

2. Subtask 3.2: Effects of DOM and Cl- on the dissolution of cinnabar: Natural DOM (>3000 Da) will be isolated from natural waters by using cross-flow ultra-filtration technique. Effects of DOM and Cl- on cinnabar dissolution will be investigated under different redox conditions (purging with N2 or O2) and various pH levels. The concentrations of Hg2+ in aqueous phase will be determined by CV-AFS.

3. Subtask 3.3: Modeling the dissolution of cinnabar in the presence of DOM and Cl-: The previously developed model for predicting the dissolution of cinnabar under different conditions of pH and O2 will be improved by the inclusion of the mechanisms for the binding of Hg2+ and DOM and inclusion of the adsorption/desorption constants of Hg2+ in the presence of DOM and Cl- as determined by experimental measurements. The model will be validated and used to further investigate the effects that DOM and Cl- have on the dissolution of cinnabar.

Task 4: Geodatabase Development for Hydrological Modeling Support Background

During FY11, FIU developed a geodatabase to support the hydrological modeling work performed by FIU, which involves the use of three integrated watershed models for the Y-12 NSC, White Oak Creek (WOC), and East Fork Poplar Creek (EFPC) to simulate the fate and transport of contaminants. More than a hundred simulations were completed for the purpose of calibrating the models, deriving model uncertainties, and for providing the analysis of remediation scenarios, resulting in hundreds of gigabytes of simulation data. Therefore, there was a need for an advanced spatial data structure that would be used to address the management, processing, and analysis of spatial and temporal numerical modeling data derived from multiple sources, and to produce hydrogeological maps for visualization.

The ORR Geodatabase is a multiuser relational database management system (RDBMS) built upon a Microsoft SQL Server platform developed using Environmental Systems Research Institute (ESRI) ArcSDE technology. The system was deployed on an advanced Windows server with the latest technology and hardware and provides a user interface which facilitates data access, database connectivity, cryptography, web application development, numeric algorithms, and network communications. The ORR Geodatabase is based on the ArcHydro and ArcGIS Base Map data models. The Arc Hydro data model contains a set of accompanying tools designed to support water resources applications within the ArcGIS environment. These data models were also used as templates as there were many input data types in common with the ORR Geodatabase. Modifications were then made for project specific input parameters. The geodatabase serves as a centralized data management system, making the mass amounts of data generated from the simulations of contaminant fate and transport accessible to all users and facilitates storage, concurrent editing and import/export of model configuration and output data.


Technical Approach

The work proposed for FY12 will serve to extend the geodatabase capabilities by creating a GIS-based model using ArcGIS Model Builder as well as Python scripting that will automate the process of data transfer between the dynamic MIKE 11 GIS geodatabase and the static hub ORR Geodatabase, querying the existing ORR Geodatabase based on specific environmental parameters, performing analyses based on specified algorithms and generating maps with the spatial distribution of computed and observed data. This can then be further extended to facilitate online querying of the database using downloadable freeware and generation of maps, graphs and reports, to more easily share the data with other project stakeholders such as DOE personnel and ORR site contractors. The use of PYTHON scripts provides capabilities including:

• Use of ArcGIS python geoprocessing libraries to iterate over any selected feature and to provide immediate analysis, updates, and modifications of the geodatabase.

• Creation of customized functions to handle various aspects of the analysis, creating more classes to implement object oriented capability and to promote code reuse within the application.

• Preprocessing of input shapefiles (sewer lines, nodes, links and any infrastructure) and creation of new shapefiles on the fly. This includes analysis of the attributes of the input files and creating of a new set of shapefiles using selected attributes.

• Iteration through a list of infrastructure elements (links, lines, nodes) selected by a polygon shapefile and for each selected component analysis of a number of attributes in the shapefiles, including total length of lines that will remain, are missing, undersized or to be abandoned, which provides analytic capabilities to derive information about each specific file.

• Automatic addition of multiple attributes to point, polygon and polyline shapefiles, including attributes that will be used for project tracking.

• Additional post-processing of relevant shapefiles, including selection, printing, formatting with a toolbox specifically designed to minimize the manual set up and efforts.

• Automatic zooming, mapping and exporting of selected spatial features to excel, pdf and CAD formats as needed.

• Creation of a special toolbox with required tools to provide GUI access to data analysis, creation of new shapefiles based on input, printing and merging information without requiring the user to spend time on entering data separately.

• Error checking and analysis of existing shapefiles and preparation for use in XPSWWM models (particularly nodes and lines).

• Creation of reports on information contained in map documents such as data frame coordinate system, layer data sources, layers with broken data sources, or layout element positioning; update, repair, or replacement of layer data sources in a map document or


layer file; and update of layer symbology without having to physically open map documents.

• Creation of geographic data in batch using map export commands, such as a series of GeoTIFF images driven by a list of features in a data frame. Automation of the creation and management of map services to be published with ArcGIS Server.

• Building a variety of PDF map books, including a thematic or temporal map book with title page, multiple map pages, and any number of additional pages with supporting content such as tabular reports and contact lists. A reference map book based on Data Driven Pages which allows rapid processing and export of a series of layout pages from the map document (and selected ATLAS sheets).

It is envisioned that the model created to extend the capabilities of the ORR Geodatabase will be similar in concept to the Map to Map model (Figure 2) created by Maidment et al., 2004 at the University of Texas’ Center for Research in Water Resources (CRWR) described by Castle, E., 2003 in his thesis [23]. This model combines geographical information systems (GIS), a hydrologic geodatabase utilizing the Hydro schema, TR-55, HEC-RAS and HEC-HMS hydrologic models.

Figure 2. Snapshot of the Map to Map model created by Maidment at CRWR. Blue circles represent inputs, yellow squares are processes, and green circles are outputs [25].

In our case, customized Python scripts will be used to automate the process of calling output data retrieved from the external hydrologic model MIKE SHE/11, importing it into the temporary MIKE 11 GIS geodatabase and then either exporting the processed file for additional model simulations or incorporating it into the ORR Geodatabase which already uses the ArcHydro data model infrastructure that serves as the central “Remediation and Treatment Technology” project data hub. ArcGIS Model Builder will be used to document


the model inputs, processes, workflows and outputs. Proposed work for FY12 includes the following subtasks:

1. Subtask 4.1: Creation of a model using ArcGIS Model Builder and Python scripting that will automate the process of querying the geodatabase based on specific environmental parameters, perform analyses based on specified algorithms and generate maps with the spatial distribution of computed and observed data.

2. Subtask 4.2: Extension of the geodatabase capabilities to facilitate online querying of the database using downloadable freeware and generation of maps, graphs and reports.

Task 5: Student Support for Modeling of Groundwater Flow and Transport at the Moab Site, Utah Background FIU, in collaboration with the DOE’s Moab site, is using an existing groundwater numerical model to evaluate the tailings pore-water seepage in order to assist in effective dewatering of the tailings pile and to optimize the groundwater extraction well field as part of the DOE Uranium Mill Tailings Remedial Action (UMTRA) for the Moab site. The work was carried out with support from student interns who assisted in the collection of groundwater samples and site data and applied the existing groundwater and transport model (SEAWAT available from the public domain) to analyze the groundwater flow and transport data of the Moab site. The objective of this model is to analyze the nitrogen and uranium cycle in the environment and provide forecasting capabilities for the fate and transport of contamination within the Moab site and to provide information which can be used to determine the efficiency of remedial actions in reducing the concentration and load of contaminants and to assist DOE in deciding the effectiveness of remedial actions. Modeling is to be performed with MODFLOW, SEAWAT and FEFLOW as a benchmark. The main objective is to determine the effect of discharge of a legacy ammonia plume from the brine zone after the extraction wells and injection system have been shut off. The model will be used to predict capture zones for different operating scenarios, mass removal; and time to complete remediation. Technical Approach The proposed scope for FY12 includes the following subtasks:

1. Subtask 5.1: Update existing Moab model by implementing geostatistically interpolated ammonia and uranium plumes and current well operation data into the model for evaluating effects of pumping on contaminant concentrations and determining potential surface water concentrations in riparian habitat areas under a range of operating conditions. The subtask will develop plumes of aqueous species of concern (nitrate, uranium) with the width of the tailings that would be conservative. The model will be updated by implementing a diversion ditch into the flow model (as drain cells) and by setting the head levels will be set in each drain cell at the elevations of the drains.

2. Subtask 5.2: Conduct simulations with the SEAWAT model to analyze the nitrogen and uranium cycle in the environment and provide forecasting capabilities for the fate and transport of contamination within the Moab site. Analyze the model output and determine the


efficiency of remedial actions in reducing the concentration and load of contaminants. A list of the simulations that have been discussed with the site include:

a. Simulate ammonia transport applying as initial condition the ammonia plume (for couple of cycles) and determine yearly rise and fall in the river and see if the ammonia concentrations moving up into the saline zone into the brine zone due to the fluctuations of concentrations in the river.

b. Determine the spatial extent of the discharge zone for the ammonia legacy plume in the brine zone and its effect on natural flushing. The objective will be to determine the effect of discharge of a legacy ammonia plume from the brine zone after the extraction wells and injection system have been shut off.

c. Implement a configuration that includes infiltration and provide information about the reoccurrence of the concentrations within the recharge assuming the existence of a freshwater lens. Determine the effect of mixing water from the river and the diversion ditch.

d. Determine the effectiveness of running both systems at the same time and derive the benefits from running the extraction wells.

3. Subtask 5.3: Simulate proposed remedial actions including pumping of contaminated groundwater from the shallow plume to an evaporation pond on top of the tailings pile, and injecting the diverted Colorado River water into the alluvial aquifer in order to predict the outcome of each remedial action and to investigate the effectiveness of each scenario. Determine the effects of the brine zone beneath the site on an overlying saline zone. After implementing plumes into the model as initial conditions, conduct additional simulations to optimize mass removal and capture from the existing system. Optimize the mass removal without additional bleeding of ammonia from the deep zone into the shallow zone and assuming that injection systems operates at the same time.

4. Subtask 5.4: Determine the effects of the brine zone beneath the site on an overlying saline zone. A student will be involved in the student internship program and will work with the transport model to perform numerical simulations of remedial scenarios proposed by DOE.


PROJECT MILESTONES

Milestone

No. Milestone Description Completion Criteria Due Date 2012-P3-M1.1

Finalize XPSWMM model preliminary configuration parameters

Memo sent to DOE EM and ORNL by email 9/14/2012

2012-P3-M1.2

XPSWMM model preliminary results summary


2012-P3-M2.1

Presentation overview to DOE ORO/DOE HQ of the project progress and accomplishments

Presentation to DOE ORO/DOE HQ 9/21/2012

2012-P3-M3.1

Preliminary results summary of laboratory experiments


2012-P3-M4.1

Sample Python scripts and Model Builder process workflow diagram


2012-P3-M5.1

Moab model preliminary results summary


2012-P3-M6.1

Waste Management Symposium 2013

Submission of two (2) abstracts 8/17/2012

2012-P3-M8.1

Submit publications to relevant journals Submission of manuscripts 5/17/2013


DELIVERABLES

Client Deliverables Responsibility Acceptance Criteria Due Date

Draft Project Technical Plan

Project Manager

Acknowledgement of receipt via E-mail two weeks after submission

06/18/12

Quarterly Progress Reports

Principal Investigator


Quarterly

Technical Report for the Parameterization of Major Transport Processes of Mercury Species

Project Manager


2/18/2013

Technical Report for the EFPC Simulations

Project Manager


3/1/2013

Technical Report for the Modeling of Groundwater and Flow and Transport at the Moab Site in Utah.

Project Manager


3/19/2013

Technical Report for Geodatabase Development for Hydrological Modeling Support

Project Manager


4/1/2013

Technical Report for Simulation of NPDES and TMDL for EFPC and Y-12 NSC

Project Manager


4/16/2013

Draft Year End Report

Project Manager


06/28/2013


COMMUNICATION PLAN, ISSUES, REGULATORY POLICES AND HEALTH AND SAFETY

Communication Plan The communication with the clients and relevant experts at DOE EM/ORO/Moab is a critical component of the project. The mode of communication will be e-mails, telephone/conference calls, meetings at the site. Though site-specific contact persons have been identified, constant communication will be maintained with client stakeholders at DOE HQ and the DOE sites to ensure all parties involved are aware of the project progress.

Information Item

Client Stakeholder When?

Communication Method

Responsible Stakeholder

Status Update Teleconferences

DOE EM, ORO, Moab

Monthly Phone Project Manager

EM-HQ Status Update Phone Call

DOE EM Bi-Weekly Phone Principal Investigator

Quarterly Report DOE EM

End of Q1, Q2, Q3, Q4

E-mail Project Manager

Draft Year End Report

DOE EM, ORO, Moab

30 working days after completion of performance period


Papers and presentations

DOE EM, ORO, Moab

As developed for conferences (e.g., WM13)


Milestone completion E-mail

DOE EM, ORO, Moab

At completion of milestone

E-mail Task Manager

The following individuals will serve as points of contacts:

Site DOE Contacts • Elizabeth Phillips, DOE-ORO, (865) 241-6172 • Don Metzler, DOE Moab, (970) 257-2115 DOE EM (HQ) Contacts • Kurt Gerdes, (301) 903-7289 • G. (Skip) Chamberlain, (301) 903-7248 • Justin Marble, (301) 903-7210 • Mark Williamson, (301) 903-8427


Oak Ridge Field Office Technical Contacts • Richard Ketelle, (RSI), (865) 574-5762 • Eric Pierce (ORNL), (865) 574-9968 • Liyuan Liang (ORNL), (865) 241-3933 • David Watson (ORNL), (865) 241-4749

Anticipated Issues No issues are anticipated.

Regulatory Policies and Health and Safety All FIU on-site task activities will be performed in accordance with FIU-ARC’s Project-Specific Health and Safety Plan (PSHASP). FIU-ARC laboratory procedures will be strictly recognized, and operators will perform all tasks in compliance with OSHA guidelines obeying all the personal protective equipment requirements and any health and safety precautions advised on the relevant material safety data sheets (MSDSs) provided. Work completed at other FIU facilities will be subject to general health and safety procedures established by FIU. Any hazardous waste products generated by FIU-ARC will be handled and disposed of in accordance with the FIU waste management program. All accumulated toxic or hazardous wastewater products will be stored in specified locations, in labeled receptacles with appropriate spill containers.

The Florida International University Laboratory Safety Program raises awareness among individuals who are likely to come into contact with hazardous substances. In order to minimize hazards, individuals who are required to work in the laboratories are properly trained. Mandatory laboratory safety training is provided:

− At the time of initial assignment, and − Prior to assignment involving a new exposure situation (i.e., new chemical equipment or

technology). The Department of Environment, Health and Safety at FIU also provides other training relevant to specific task needs of any research projects.

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11. Paquette, K. E.; Helz, G. R. Inorganic speciation of mercury in sulfidic waters: The importance of zero-valent sulfur. Environmental Science & Technology 1997, 31 (7), 2148-2153.

12. Ravichandran, M.; Aiken, G. R.; Reddy, M. M.; Ryan, J. N. Enhanced dissolution of cinnabar (mercuric sulfide) by dissolved organic matter isolated from the Florida Everglades. Environmental Science & Technology 1998, 32 (21), 3305-3311.

13. Waples, J. S.; Nagy, K. L.; Aiken, G. R.; Ryan, J. N. Dissolution of cinnabar (HgS) in the presence of natural organic matter. Geochimica Et Cosmochimica Acta 2005, 69 (6), 1575-1588.

14. Han, S.; Obraztsova, A.; Pretto, P.; Choe, K. Y.; Gieskes, J.; Deheyn, D. D.; Tebo, B. M. Biogeochemical factors affecting mercury methylation in sediments of the Venice Lagoon, Italy. Environ. Toxicol. Chem. 2007, 26 (4), 655-663.

15. Hammerschmidt, C. R.; Fitzgerald, W. F. Geochemical controls on the production and distribution of methylmercury in near-shore marine sediments. Environ. Sci. Technol. 2004, 38 (5), 1487-1495.

16. Benoit, J. M.; Gilmour, C. C.; Mason, R. P. The influence of sulfide on solid phase mercury bioavailability for methylation by pure cultures of Desulfobulbus propionicus (1pr3). Environ. Sci. Technol. 2001, 35 (1), 127-132.

17. Hintelmann, H.; Keppel-Jones, K.; Evans, R. D. Constants of mercury methylation and demethylation rates in sediments and comparison of tracer and ambient mercury availability. Environ. Toxicol. Chem. 2000, 19 (9), 2204-2211.

18. Morel, F. M. M.; Kraepiel, A. M. L.; Amyot, M. The chemical cycle and bioaccumulation of mercury. Annu. Rev. Ecol. Syst. 1998, 29, 543-566.

19. Drott, A.; Lambertsson, L.; Bjorn, E.; Skyllberg, U. Importance of dissolved neutral mercury sulfides for methyl mercury production in contaminated sediments. Environ. Sci. Technol. 2007, 41 (7), 2270-2276.

20. Wolfenden, S.; Charnock, J. M.; Hilton, J.; Livens, F. R.; Vaughan, D. J. Sulfide species as a sink for mercury in lake sediments. Environ. Sci. Technol. 2005, 39 (17), 6644-6648.


21. Ullrich, S. M.; Tanton, T. W.; Abdrashitova, S. A. Mercury in the aquatic environment: A review of factors affecting methylation. Crit. Rev. Environ. Sci. Technol. 2001, 31 (3), 241-293.

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23. Castle, E. (2003). Geodatabases in Design: A Floodpain Analysis of Little Kitten Creek. Thesis. Brigham Young University.

24. Rosenzweig, I. and B. Hodges, 2011. A Python Wrapper for Coupling Hydrodynamic and Oil Spill Models. Center for Research in Water Resources, University of Texas at Austin, CRWR Online Report 11-09. Submitted to Texas General Land Office Oil Spill Prevention & Response. FY 2011 Report under Contract No. 10-097-000-3928, October 31, 2011.

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26. Southworth, G., Greeley, M., Peterson, M., Lowe, K., & Kettelle, R., 2010a. Sources of Mercury to East Fork Poplar Creek Downstream from the Y-12 National Security Complex: Inventories and Export Rates. Oak Ridge: Oak Ridge National Laboratory.

27. Turner, R. R. and Southworth, G. R.., 1999. Mercury-Contaminated Industrial and Mining Sites in North America: an Overview with Selected Case Studies. In Mercury Contaminated Sites, R. Ebinghaus, R. R. Turner, L. D. de Lacerda, O. Vasiliev, and W. Salomons (Eds.) Springer-Verlag, Berlin, F. R. G. Turner, R. R., Olsen, C. R., & Wilcox, W. J. Jr., 1985. Environmental fate of Hg and 137 Cs discharged from Oak Ridge facilities. In D. D. Hemphill (Ed.), Trace substances in the environment. New York: Elsevier.

28. ORISE (Oak Ridge Institute for Science and Education). Characterization Report for the 81-10 Area in the Upper East Fork Poplar Creek Area at the Oak Ridge Y-12 National Security Complex, Oak Ridge, Tennessee, 2010. DOE/OR/01-2485&D1. Oak Ridge, TN.

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32. DOE, 1995, Decision Document for Performing a Long-Term Pumping Test at the S-3 Site, Oak Ridge Y-12 Plant, Oak Ridge, Tennessee, Y/ER-210

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Documents

Project 3 PTP for 2012 - doeresearch.fiu.edu Project 3 Appendices/P3...PROJECT TECHNICAL PLAN . Project 3: Remediation and Treatment Technology Development and Support for DOE Oak