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DOE OSTI2018

Economical and Environmentally Benign Extraction of Rare Earth Elements (REES) from Coal & Coal Byproducts

This final report provides a complete summary of the activities, results, analytical discussion, and overall evaluation of the project titled “Economical and Environmentally Benign Extraction of Rare Earth Elements (REES) from Coal & Coal Byproducts” under DOE Award Number DE-FE-0027155 that started in March 2016 and ended December 2017. Fly ash was selected as the coal-byproduct source material due to fact that it is readily available with no need for extensive methods to obtain the material, it is produced in large quantities (>50 million tons per year) and had REE concentrations similar to other coal-byproducts. The selected fly ash used throughout this project was from the Mill Creek power generating facility operated by Louisville Gas and Electric located in Louisville, KY and was subjected to a variety of physical and chemical characterization tests. Results from fusion extractions showed that the selected fly-ash had a TREE+Y concentration of 480 ppm with critical REEs concentration of 200 ppm. The fly ash had an outlook ratio of 1.25 and an estimated value of $16-$18 worth of salable REEs per 1-tonne of fly ash. Additional characterizations by optical evaluation, QEMSCAN, XRD, size fractionation, and SEM analysis showed the fly ash consisted of small glassy spherules with a size range between 1 to 110 µm (ave. diam. of 13 um), was heterogeneous in chemical composition (main crystalline phases: aluminum oxides and iron oxides) and was primarily an amorphous material (75 to 80%). A simple stepped approach was completed to estimate the total REE resource quantity. The approach included REE characterization of the representative samples, evaluation of fly-ash availability, and final determination estimated resource availability with regards to REE grade on a regional and national scale. This data represents the best available information and is based upon the assumptions that the power generating facility where the fly-ash was obtained will use the same coal sources (actual mines were identified), the coal materials will have relatively consistent REE concentrations, and the REE extraction process developed during this project can achieve 42% REE recovery (validated and confirmed). Calculations indicated that the estimated REE resource is approximately 175,000 tonnes with a current estimated value of $3,330MM. The proposed REE extraction and production process developed during this project used four fundamental steps; 1) fly-ash pretreatment to enhance REE extraction, 2) REE extraction by acid digestion, 3) REE separation/concentration by carbon adsorption and column chromatography, and 4) REE oxide production. Secondary processing steps to manage process residuals and additional processing techniques to produce value-added products were incorporated into the process during the project. These secondary steps were not only necessary to manage residuals, but also provided additional revenue streams that offset operational and capital expenditures. The process produces one value product stream (production of zeolite Na-P1), a solids waste stream, and one liquid stream that met RCRA discharge requirements. Based upon final design criteria and operational parameters, the proposed system could produce approximately 200 grams of REOs from 1-tonne of fly-ash, thereby representing a TREE+Y recovery of 42% (project target of > 25%). A detailed economic model was developed to evaluate both CAPEX and OPEX estimates for systems with varying capacities between 100 kg to 200 tonnes of fly ash processed per day. Using a standard system capacity of 10 tonne/day system, capital costs were estimated at $88/kg fly ash while operating costs were estimated at approximately $450/kg fly ash. This operating cost estimate includes a revenue of $495/tonne of fly ash processed from the value-added product produced from the system (zeolite Na-P1). Although operating cost savings due to zeolite production were significant, the capital + operating cost for a 10 tonne system was more expensive than the total dollar value of REEs present in the fly ash material. Specifically, the estimated cost per 1-tonne of fly ash treated is approximately $540 while the estimated value of REEs in the fly ash is $18-$20/tonne. This is an excessive difference showing that the proposed process is not economically feasible strictly on the basis of REE revenue compared to extraction costs. Although the current proposed system does not produce sufficient quantities of REEs or additional revenue sources to offset operational and capital costs, supplementary factors including US strategic concerns, commercial demands, and defense department requirements must be factored. At this time, the process developed during this project provides foundational information for future development of simple processes that require low capital investment and one that will extract a valuable quality and quantity of REE oxides from industrial waste.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2017

Research and Technology Development Activities to Address the DOE-EM Environmental Mercury Challenge - 17497

Human activities have altered trace metal distributions globally. This is especially true for the trace metal mercury (Hg), a pervasive global pollutant that can be methylated to form highly toxic methylmercury (MeHg), which bio-accumulates in aquatic food webs, endangering humans and other biota. Currently there are more than 3,000 mercury-contaminated sites identified worldwide and the United Nations Environment Programme has recently highlighted the risk of this contamination to human health. The Oak Ridge Reservation (ORR) represents an example of one of these mercury-contaminated sites. Unlike other contaminants-metals, radionuclides, and organic solvents-that impact the Department of Energy Office of Environmental Management (DOE-EM) cleanup program at the ORR and other DOE sites, mercury has several unique characteristics that make environmental remediation of the Y-12 National Security Complex one of the most formidable challenges ever encountered. These distinctive physicochemical properties for mercury include the following: it is a liquid at ambient temperature and pressure; it is the only metal that bio-magnifies; and it is the only contaminant transported as a cation, as a dissolved or gaseous elemental metal (similar to an organic solvent), or as both a cation and a dissolved or gaseous elemental metal under environmental conditions. Because of these complexities, implementing cost effective and sustainable solutions that reduce mercury flux from various primary and secondary contamination sources will require linking basic science understanding and applied research advancements into Oak Ridge Office of Environmental Management's (OREM) cleanup process. Currently, DOE is investing in mercury-related research through a variety of programs, including the Office of Science-sponsored Critical Interfaces Science Focus Area, EM headquarters-sponsored Applied Field Research Initiative, OREM-sponsored Lower East Fork Poplar Creek (LEFPC) Mercury Technology Development Program, Small Business Innovative Research (SBIR), and EM's Minority Serving Institutions Partnership Program. Collectively, these multi-institutional and multidisciplinary programs are generating new tools, knowledge, and remediation approaches that will enable efficient cleanup of mercury contaminated systems locally and globally. In this talk we will highlight the progress made to date in addressing key knowledge gaps required to solve this watershed-scale conundrum. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2014

Fuel Fabrication Capability Research and Development Plan

The purpose of this document is to provide a comprehensive review of the mission of the Fuel Fabrication Capability (FFC) within the Global Threat Reduction Initiative Convert Program, along with research and development (R&D) needs that have been identified as necessary to ensuring mission success. The design and fabrication of successful nuclear fuels must be closely linked endeavors. Therefore, the overriding motivation behind the FFC R&D program described in this plan is to foster closer integration between fuel design and fabrication to reduce programmatic risk. These motivating factors are all interrelated, and progress addressing one will aid understanding of the others. The FFC R&D needs fall into two principal categories, 1) baseline process optimization, to refine the existing fabrication technologies, and 2) manufacturing process alternatives, to evaluate new fabrication technologies that could provide improvements in quality, repeatability, material utilization, or cost. The FFC R&D Plan examines efforts currently under way in regard to coupon, foil, plate, and fuel element manufacturing, and provides recommendations for a number of R&D topics that are of high priority but not currently funded (i.e., knowledge gaps). The plan ties all FFC R&D efforts into a unified vision that supports the overall Convert Program schedule in general, and the fabrication schedule leading up to the MP-1 and FSP-1 irradiation experiments specifically. The fabrication technology decision gates and down-selection logic and schedules are tied to the schedule for fabricating the MP-1 fuel plates, which will provide the necessary data to make a final fuel fabrication process down-selection. Because of the short turnaround between MP-1 and the follow-on FSP-1 and MP-2 experiments, the suite of specimen types that will be available for MP-1 will be the same as those available for FSP-1 and MP-2. Therefore, the only opportunity to explore parameter space and alternative processing is between now and 2016 when the candidate processes are down-selected in preparation for the MP-1, FSP-1, and MP-2 plate manufacturing campaigns. A number of key risks identified by the FFC are discussed in this plan, with recommended mitigating actions for those activities within FFC, and identification of risks that are impacted by activities in other areas of the Convert Program. The R&D Plan does not include discussion of FFC initiatives related to production-scale manufacturing of fuel (e.g., establishment of the Pilot Line Production Facility), rather, the goal of this plan is to document the R&D activities needed ultimately to enable high-quality and cost-effective production of the fuel by the commercial fuel fabricator. The intent is for this R&D Plan to be a living document that will be reviewed and updated on a regular basis (e.g., annually) to ensure that FFC R&D activities remain properly aligned to the needs of the Convert Program. This version of the R&D Plan represents the first annual review and revision.

Convert Program↗
DOE OSTI2025

High-Temperature Active Magnetic Bearing Development for Supercritical CO 2 Machinery Applications

Hermetic machinery utilizing gas bearings for MW-scale supercritical CO 2 (sCO 2 ) machinery applications can have significantly lower power loss and enable improved cycle efficiency compared to conventional machinery with oil-lubricated bearings. Active magnetic bearings (AMBs) are another option anticipated to have similar power loss and load capacity to gas bearings as well as offering larger mechanical tolerances, the ability to tune properties, and high reliability due to lack of mechanical wear. AMBs also have proven commercial experience at MW-scale, though environments for high-temperature sCO 2 power cycle machinery conditions are novel. Besides the potential impact of AMBs for sCO 2 turbomachinery, the technology also offers promising benefits for steam and gas turbines for power generation, compressors and expanders for industrial heat and power, and in other oil and gas and space applications. The goals of this project were to conceptual design an AMB and perform material testing. Conceptual designs for radial and thrust AMBs were produced based on a hermetically-sealed sCO 2 machinery waste-heat recovery (WHR) application for sizing and loads, and choosing a target design temperature of 540°C useful for high-temperature sCO 2 turbines for concentrating solar power (CSP) applications. Conceptual designs were initially developed for multiple radial and thrust AMBs with spreadsheet-based calculations before selecting one of each to develop further using higher-fidelity design methods for magnetic and structural performance. It was found that the radial AMB at 540°C was feasible, but the thrust AMB needed to be limited to 315°C for high-speed operation. The decision for a reduced-temperature thrust AMB was the result of several significant conclusions: 1) Hiperco 50A, originally chosen for good magnetic performance at high temperature, had insufficient strength for high-speed operation, so it was replaced with 17-4 PH. 2) The reduced magnetic performance from 17-4 PH yielded a larger bearing size, reducing the strength margin. 3) This ultimately led to a creative design implementing a more-compact E-core topology, compared to the original (conventional) C-core, and an integral shaft-disk with Hirth joint connection. These conceptual designs are unique for the size and temperature in CO 2 , relevant for MW-scale CSP applications. Long term, high temperature test data was generated for several materials, filling a void in the current body of literature. Corrosion and magnetic performance measurements were produced for PM materials (Alnico 5-7C, Alnico 9C, and SmCo) with and without nickel-coating for environments of high-temperature CO 2 up to 550°C at atmospheric pressure and 450°C at 103 bar for up to 6,000 hours. Corrosion measurements were also produced for Hiperco 50, a SM material relevant for AMB laminations, with and without C5 coating. Comparisons were also made for 450°C and 550°C, atmospheric pressure air exposures up to 5,000 hours. Results generally show that coatings can be effective at improving oxidation resistance of the bare materials, and Alnicos generally outperformed SmCo after high-temperature exposure. In addition to technical feasibility demonstrated by the design, economic feasibility was demonstrated by updating the TEA from the reference machine, re-evaluating it with CAPEX and OPEX to reflect estimated changes from process-lubricated bearings to AMBs. AMBs were shown to be comparable in performance to process-lubricated bearings, still showing a notable improvement over conventional machinery architecture with oil-lubricated bearings.

42 ENGINEERING↗
DOE OSTI2016

Evaluation of Lower East Fork Poplar Creek Mercury Sources

This report summarizes a 3-year research project undertaken to better understand the nature and magnitude of mercury (Hg) fluxes in East Fork Poplar Creek (EFPC). This project addresses the requirements of Action Plan 1 in the 2011 Oak Ridge Reservation-wide Comprehensive Environmental Response, Compensation, and Liability Act Five Year Review (FYR). The Action Plan is designed to address a twofold 2011 FYR issue: (1) new information suggests mobilization of mercury from the upper and lower EFPC streambeds and stream banks is the primary source of mercury export during high-flow conditions, and (2) the current Record of Decision did not address the entire hydrologic system and creek bank or creek bed sediments. To obtain a more robust watershed-scale understanding of mercury sources and processes in lower EFPC (LEFPC), new field and laboratory studies were coupled with existing data from multiple US Department of Energy programs to develop a dynamic watershed and bioaccumulation model. LEFPC field studies for the project focused primarily on quantification of streambank erosion and an evaluation of mercury dynamics in shallow groundwater adjacent to LEFPC and potential connection to the surface water. The approach to the stream bank study was innovative in using imagery from kayak floats’ surveys from the headwaters to the mouth of EFPC to estimate erosion, coupled with detailed bank soil mercury analyses. The goal of new field assessments and modeling was to generate a more holistic and quantitative understanding of the watershed and the sources, flux, concentration, transformation, and bioaccumulation of inorganic mercury (IHg) and methylmercury (MeHg). Model development used a hybrid approach that dynamically linked a spreadsheet-based physical and chemical watershed model to a systems dynamics, mercury bioaccumulation model for key fish species. The watershed model tracks total Hg and MeHg fluxes and concentrations by examining upstream inputs, floodplain runoff, floodplain leaching, bank soil erosion, and periphyton matrix dynamics. The bioaccumulation model tracks the feeding, growth, and mercury assimilation of representative individual fish through their typical life span using key inputs of fish size, water temperature, and diet. The LEFPC watershed was divided into five modeling reaches, and fluxes and concentrations are assessed at this spatial scale. Following are the key findings of the field and laboratory studies and the watershed and bioaccumulation modeling: • The greatest flux of total mercury (HgT) in LEFPC is related to stormflow transport of Hg-contaminated solids entering the creek because of bank erosion in the upper reaches of the creek. • The second greatest flux originates from upper EFPC (Station 17 representing the exit stream sampling point near the boundary of the Y-12 Complex), and appears to control base flow fluxes. • The observed increase in MeHg concentration and flux from upstream to downstream is related primarily to instream methylation by periphyton and other biological activity. • A meaningful substantial reduction of the HgT flux in LEFPC would require addressing the flux of HgT originating from bank erosion and from Station 17. • Actions to reduce LEFPC floodplain leaching and runoff would not produce much of an impact on HgT or MeHg concentrations or fluxes unless other major sources are eliminated first. This project addresses the Action Plan goal to evaluate the role of LEFPC bank soil sources and to consider the entire EFPC hydrologic system. Model conclusions are dependent on the data available at the time of this assessment. However, a robust understanding and quantification for some mercury-related parameters and relationships is still lacking; there is a continued need for field data collection and modeling improvements. Model predictions should be viewed cautiously, with comparisons of the magnitude of predictions between scenarios being more valid than absolute predictions of concentrations or fluxes. With continued updates and refinement, the watershed-scale model can be a useful, valuable tool for future EFPC research prioritization, technology development, and remedial decision-making.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2010

External Peer Review Team Report Underground Testing Area Subproject for Frenchman Flat, Revision 1

An external peer review was conducted to review the groundwater models used in the corrective action investigation stage of the Underground Test Area (UGTA) subproject to forecast zones of potential contamination in 1,000 years for the Frenchman Flat area. The goal of the external peer review was to provide technical evaluation of the studies and to assist in assessing the readiness of the UGTA subproject to progress to monitoring activities for further model evaluation. The external peer review team consisted of six independent technical experts with expertise in geology, hydrogeology,'''groundwater modeling, and radiochemistry. The peer review team was tasked with addressing the following questions: 1. Are the modeling approaches, assumptions, and model results for Frenchman Flat consistent with the use of modeling studies as a decision tool for resolution of environmental and regulatory requirements? 2. Do the modeling results adequately account for uncertainty in models of flow and transport in the Frenchman Flat hydrological setting? a. Are the models of sufficient scale/resolution to adequately predict contaminant transport in the Frenchman Flat setting? b. Have all key processes been included in the model? c. Are the methods used to forecast contaminant boundaries from the transport modeling studies reasonable and appropriate? d. Are the assessments of uncertainty technically sound and consistent with state-of-the-art approaches currently used in the hydrological sciences? 3. Are the datasets and modeling results adequate for a transition to Corrective Action Unit monitoring studies—the next stage in the UGTA strategy for Frenchman Flat? The peer review team is of the opinion that, with some limitations, the modeling approaches, assumptions, and model results are consistent with the use of modeling studies for resolution of environmental and regulatory requirements. The peer review team further finds that the modeling studies have accounted for uncertainty in models of flow and transport in the Frenchman Flat except for a few deficiencies described in the report. Finally, the peer review team concludes that the UGTA subproject has explored a wide range of variations in assumptions, methods, and data, and should proceed to the next stage with an emphasis on monitoring studies. The corrective action strategy, as described in the Federal Facility Agreement and Consent Order, states that the groundwater flow and transport models for each corrective action unit will consider, at a minimum, the following: • Alternative hydrostratigraphic framework models of the modeling domain. • Uncertainty in the radiological and hydrological source terms. • Alternative models of recharge. • Alternative boundary conditions and groundwater flows. • Multiple permissive sets of calibrated flow models. • Probabilistic simulations of transport using plausible sets of alternative framework and recharge models, and boundary and groundwater flows from calibrated flow models. • Ensembles of forecasts of contaminant boundaries. • Sensitivity and uncertainty analyses of model outputs. The peer review team finds that these minimum requirements have been met. While the groundwater modeling and uncertainty analyses have been quite detailed, the peer review team has identified several modeling-related issues that should be addressed in the next phase of the corrective action activities: • Evaluating and using water-level gradients from the pilot wells at the Area 5 Radioactive Waste Management Site in model calibration. • Re-evaluating the use of geochemical age-dating data to constrain model calibrations. • Developing water budgets for the alluvial and upper volcanic aquifer systems in Frenchman Flat. • Considering modeling approaches in which calculated groundwater flow directions near the water table are not predetermined by model boundary conditions and areas of recharge, all of which are very uncertain. • Evaluating local-scale variations in hydraulic conductivity on the calculated contaminant boundaries. • Evaluating the effects of non-steady-state flow conditions on calculated contaminant boundaries, including the effects of long-term declines in water levels, climatic change, and disruption of groundwater system by potential earthquake faulting along either of the two major controlling fault zones in the flow system (the Cane Spring and Rock Valley faults). • Considering the use of less-complex modeling approaches. • Evaluating the large change in water levels in the vicinity of the Frenchman Flat playa and developing a conceptual model to explain these water-level changes. • Developing a long-term groundwater level monitoring program for Frenchman Flat with regular monitoring of water levels at key monitoring wells. Despite these reservations, the peer review team strongly believes that the UGTA subproject should proceed to the next stage.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

LANL Activities: FY12-Q2 National Risk Assessment Partnership (NRAP): Industrial Carbon Capture Program (Quarterly Report)

This report summarizes progress of LANL activities related to the tasks performed under the LANL FWP FE102-002-FY10, National Risk Assessment Partnership (NRAP): Industrial Carbon Capture Program. This FWP is funded through the American Recovery and Reinvestment Act (ARRA). Overall, the NRAP activities are focused on understanding and evaluating risks associated with large-scale injection and long-term storage of CO 2 in deep geological formations. One of the primary risks during large-scale injection is due to changes in geomechanical stresses to the storage reservoir, to the caprock/seals and to the wellbores. These changes may have the potential to cause CO 2 and brine leakage and geochemical impacts to the groundwater systems. While the importance of these stresses is well recognized, there have been relatively few quantitative studies (laboratory, field or theoretical) of geomechanical processes in sequestration systems. In addition, there are no integrated studies that allow evaluation of risks to groundwater quality in the context of CO 2 injection-induced stresses. The work performed under this project is focused on better understanding these effects. LANL approach will develop laboratory and computational tools to understand the impact of CO 2 -induced mechanical stress by creating a geomechanical test bed using inputs from laboratory experiments, field data, and conceptual approaches. The Geomechanical Test Bed will be used for conducting sensitivity and scenario analyses of the impacts of CO 2 injection. The specific types of questions will relate to fault stimulation and fracture inducing stress on caprock, changes in wellbore leakage due to evolution of stress in the reservoir and caprock, and the potential for induced seismicity. In addition, the Geomechanical Test Bed will be used to investigate the coupling of stress-induced leakage pathways with impacts on groundwater quality. LANL activities are performed under two tasks: (1) develop laboratory and computational tools to understand CO 2 -induced mechanical impacts and (2) use natural analog sites to determine potential groundwater impacts. We are using the Springerville-St. John Dome as a field site for collecting field data on CO 2 migration through faults and groundwater impacts as well as developing and validating computational models. During the FY12 second quarter we have been working with New England Research Company to construct a tri-axial core-holder. We have built fluid control system for the coreflood system that can be ported to perform in-situ imaging of core. We have performed numerical simulations for groundwater impacts of CO 2 and brine leakage using the reservoir model for Springerville-St John's Dome site. We have analyzed groundwater samples collected from Springerville site for major ion chemistry and isotopic composition. We are currently analyzing subsurface core and chip samples acquired for mineralogical composition.

25 ENERGY STORAGE↗
DOE OSTI2013

Development of Technologies and Capabilities for Coal Energy Resources

This is the final report for the Aerojet Rocketdyne (AR) Advanced Gasification Systems Development (AGSD) project that was initiated on October 1, 2004. The project’s primary objective is to demonstrate technologies that improve the availability and efficiency of gasification-based power plants and to reduce plant capital and operational costs. The objective will be accomplished by (1) development and testing of cooled refractory liners, (2) feed system development and demonstration, (3) pilot plant definition and planning, (4) transport gasifier feed analysis, (5) coal-biomass mixture feed analysis, and (6) coal-biomass mixture pilot scale tests. Task 1, development and testing of cooled refractory liners, was conducted at CANMET Energy Technology Centre in Ottawa, Canada. The test objectives were to screen high conductivity CMC materials with alternate manufacturing methods and a variety of surface treatments for cooled metal tubes in a slagging gasifier environment. During the CMC testing, it was found that a constantly cooled CMC will survive in good conditions and that high porosity CMC resulted in high material erosion and corrosion. During cooled tube testing, it was found that hard metal spray coat and bare Haynes 188 performed the best. Task 2, feed system development and demonstration, was conducted at at the Energy and Environmental Research Center (EERC) at the University of North Dakota (UND). For tasks 2.1-2.6, the test objective was to demonstrate 400-tons/day coal feed system operation (to 1,000 psia gasifier pressures) in ultra-dense phase flow without plugging and to achieve multi-element injector flow-split non-uniformities below 2 %RSD. Testing was successfully completed with no feed system plugging of the feed system. The majority of the other Task 2 activities were associated with the Dry Solids Pump design (Task 2.8 and 2.11), development (Task 2.10), fabrication (Task 2.12), amd testing (Task 2.13-2.15). A variety of tests were performed that verified the capability of the Dry Solids Pump to consolidate various pulverized feedstocks to a state capable of sealing and sustaining downstream outlet pressures during mechanical operation of the pump as well as during periods when the pump was turned off. However, the final operating goals were not achieved. Task 3, pilot plant definition and planning, was to define requirements for an advanced commercial gasifier with a cooled liner and to establish a preferred commercial gasifier system configuration to serve as the reference point for an advanced gasifier pilot plant concept definition. A pilot plant concept was successfully defined that is scalable and traceable to the commercial gasifier configuration. The schedule and cost for design, installation, and long-duration test operation of a pilot plant were estimated at 33 months and $\$$25.6M. Taks 4, transport gasifier feed analysis, was to determine the effects of larger sized transport gasifier low rank coals within the AR dry solids pump. It was found for the two low-rank +100 mesh size transport gasifier coals that the cohesion of these larger materials was significantly less than the coals ground to minus 200 mesh. Also, the gas permeability of the MSL transport coal was found to be significantly higher than the permeability of the PRB transport coal. Task 5, coal-biomass mixture feed analysis, was to determine the effects of coal biomass blends within the AR ultra-dense phase feed system and dry solids pump, and to determine the cost of electricity increase of an integrated gasification combined cycle (IGCC) operating on coal/biomass blends with the AR dry solids pump and ultra-dense phase feed system. In summary, it was found that 75/25 wt% coal/corn stover blends produce reasonable economic results for IGCC operation with minimal dry solids pump modifications – especially if the coal is a low rank coal and the corn stover biomass is pelletized. The increase in electricity cost was found to be 1.1 cents/kWh. Task 6, coal-biomass mixture pilot scale tests, was to determine which coal/biomass blends could be tested in the current dry solids pump without major modifications. As reported in detail in the reports by Sprouse (2010) and Sprouse and Darby (2013), the coal/biomass blend having the least impact on pump configuration and operation is the 90/10 wt% Illinois #6 to corn stover ratio blend. The AGSD program was initiated on October 1, 2004. The interim final report was submitted on October 21, 2010 and covered Task 1, Task 2.1-2.9, and Task 3, performed during budget period 1. This final report covers Task 2.10-2.16, 4, 5, and 6, performed during budget period 2. The interim final report is attached as part of the appendix to this report.

Darby, Alan K.↗
DOE OSTI2016

Transmutation Fuels Development in the Advanced Fuels Campaign

Metallic fuels have a history of use that spans the entire nuclear age, especially in association with the development of the LMFBR. Initially, metallic fuels were employed due to their ease of fabrication and high heavy metal density (which led to the most favorable breeding efficiencies in fast reactors). During subsequent decades of use, metallic fuel technology has matured significantly, leading to the realization of major benefits in the areas of fuel reliability and burnup, proliferation-resistant recycling, remote fabrication, and passive reactor safety. Such characteristics continue to make metallic fuels a highly attractive technology, especially for use with future sodium fast reactors. Current research and development activities on metallic fuels in DOE's Advanced Fuels Campaign are focused on their potential use for actinide transmutation in advanced SFRs. In such a mission, metallic fuels would be employed as part of a closed fuel cycle into which plutonium and minor actinides (Am, Np) recovered from LWR spent fuel would be incorporated. All actinides in this metallic fuel would be fissioned or transmuted in a fast reactor to eliminate the extremely long-lived, heat-producing actinides in order to reduce the volume, heat load, and radio-toxicity burden on a future geological repository. Thus, the need exists to demonstrate reliable performance of metallic fuels with Pu and minor actinide constituents to very high burnup. As part of this application, there is also a need for a near zero-loss fabrication process, since losses during fuel fabrication are a potential source of long-lived actinides destined for geologic disposal. This paper presents the current state and future direction of the development of metallic fuels for actinide transmutation in the US. Metallic fuels have had a long history of use in sodium-cooled fast reactors. Continued research, development, and design innovation over a period of decades have demonstrated this fuel technology to be safe and reliable to extremely high burnups over a wide range of compositions. Their simple fabrication has historically given them a significant economic advantage over other fuel forms. Research and development on metallic fuels continues, with particular emphasis on showing that this fuel technology can incorporate significant quantities of plutonium and minor actinides for the purpose of efficiently and economically transmuting these elements in a fast-spectrum reactor. New fabrication methods to improve retention of the volatile fuel constituents during the casting process (and reduce waste generation), are being developed. Irradiation testing of the new metallic fuels has so far indicated that the new compositions, although differing significantly both in the quantities of Pu and minor actinides included and in the Zr alloying addition, perform as a function of fission density very analogously to the historic U-Zr and U-Pu-Zr fuels. In the next few years it is anticipated that a new casting furnace prototype will demonstrate that these new metallic fuel alloys can be fabricated at engineering scale, in a remote environment, with no significant fuel loss or waste generation. Irradiation tests currently underway will provide the performance data needed to assess fuel reliability/burnup capability and identify any unique behaviors that are a result of the new compositions. If these future results are consistent with the intermediate data available at present, metallic fuels are expected to continue to be a strong contender for the fuel technology choice of future fast reactors. (authors)

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

High Energy Storage Capacity Low Cost Iron Flow Battery

A new flow battery was proposed that utilizes low cost materials: iron as the only active element, cheap aqueous electrolytes, and inexpensive separators. During charging, ferrous iron (Fe 2+ ) is oxidized to ferric iron (Fe 3+ ) at the positive electrode while it (Fe 2+ ) is reduced to form iron metal (Fe 0 ) at the negative electrode. Because iron is plated at the negative electrode during charging, conventional electrode structures couple the energy storage capacity and the power rating of the battery. In order to decouple the energy and power ratings and regain the economic advantages of a flow battery, a slurry electrode design was proposed for use as the negative electrode. The slurry electrode is made by flowing electrically conductive particles in an electrolyte containing the dissolved iron species. On charging, iron is plated onto the particles. The particles can then carry the iron metal out of the cell to be stored in external reservoirs. This project looked to develop a slurry for the negative electrode of the all-iron flow battery that can operate at 200 mA/cm 2 with <100 mV overpotential, be pumped with parasitic energy costs < 10%, and promote plating on the particles. A scalable and stackable cell design of 1100 cm 2 was developed. The project was initially under contract in mid-January 2013. The project was converted from a one-year proof of concept seedling to an additional two-year program, then extended with an 18-month plus-up, and finally with an additional 6-month approved cost-overrun. During the seeding project, the concept of plating on carbon particles in a slurry was demonstrated. However, this was accomplished with high-cost multi-walled carbon nanotubes as the slurry material. The following two-year program discovered several low-cost carbon blacks that could also be used in this application. These findings were supported by an analysis that demonstrated the effectiveness of the carbon that takes into account not just the effective electronic conductivity of the slurry, but also the surface area per volume of the slurry. It was demonstrated that stable, flowable slurries could be created with these carbons, even when the carbons where fully loaded with iron during charging. During the two-year program, laboratory-scale 50 cm 2 single-cells demonstrated charge-discharge cycling at current densities of 150 mA/cm 2 and energy efficiencies of >50%. Meanwhile, cost modeling continued to show promise for this energy storage approach. Following the conversion period, the overall objective of the nominally 18-month plus up period was to close the technical gap of a 25X scale-up and reduce risk to enable commercial investment required to develop a slurry iron flow battery product. A specific objective was to demonstrate 150 cycles of performance exceeding 70% energy efficiency with a 10-cell stack of 1156 cm 2 cells operating at 100 mA/cm 2 . The 10-cell short stack was designed to have a power delivery rating of approximately 1 kW, which represents a size commensurate with the requirements of our commercialization partner at that time. A complete battery support system for the full-size cell was designed, fabricated, and tested. This includes pumps (multiple types were considered, and constant volume hose pumps were found to be acceptable for performance and cost), electrolyte rebalance reactor, and sensors and control systems. The support system proved to be well-behaved and worked well. A new low-cost membrane was developed for this system based on a microporous polymer support with a layer of hydrogel polymer. The membrane had low resistivity, and significantly reduced pressure driven fluid flow across the membrane (as compared to the un-coated microporous support). This membrane approach was scaled-up in conjunction with a commercial toll coating company, and a large amount of membrane was manufactured to support large cell and stack testing. A new concept for an electrolyte rebalance reactor to react hydrogen gas from the negative electrolyte (from plating inefficiency) with excess ferric ion in the positive electrolyte was developed. This design was very simple, low cost, and effective. The full scale 1156 cm 2 single-cell was designed, modeled, fabricated and tested. Modeling showed that uniform flow-distribution should be obtained with the designed flow distributor. The design took into consideration the need to stack the cells, and components were fabricated for a ten-cell stack. Testing of the cell for charge and discharge demonstrated current densities of 50 mA/cm 2 with efficiencies of 50%. However, optimization and long cycling could not be accomplished because the slurry electrode would plug within the cell and block the flow. This would shut down the cell after several charge-discharge cycles. Various approaches were pursued to address this problem with some progress. However, there was not adequate time to find solutions to the problem although several promising approaches were identified for future work. The final deliverable for this proposed 18-month effort was to be a 1 kW, 6 kWh slurry flow battery, with complete balance of plant, ready for testing at an ARPA-E ‘Charges’ site with an estimated capital cost less than $\$ $45/kWh for a six-hour system (excluding power electronics). The deliverable milestone was not achieved for reasons mentioned above related to the slurry plugging. At the completion of this project, it was determined that the cost targets are achievable. The cost estimate for a 1 MW system with a one-hour capacity was estimated at $\$ $140/kWh (including power electronics) and for a six-hour system was estimated at $\$ $40/kWh (including power electronics). These costs include the battery, the balance of plant, the power conditioning and a concrete pad. This program resulted in three patents including the slurry-based iron flow battery, the rebalance reactor, and the membrane separator. At the time of this report, slurry-based iron flow battery patents have been issued in the US, China, Japan, Korea, and Europe. The other patent applications were under various stages of examination. A licensee was identified and the company initiated a scale-up and development program to take this technology to the marketplace, and CWRU staff have transferred their know-how and knowledge base to the company. This technology will enhance the economic and energy security of the United States by enabling the use of intermittent renewable energy technology, such as wind and solar power, as dispatchable resources. This report summarizes the results of this research and development program.

25 ENERGY STORAGE↗
DOE OSTI2016

HySafe research priorities workshop report Summary of the workshop organized in cooperation with US DOE and supported by EC JRC in Washington DC November 10-11 2014.

The HySafe research priorities workshop is held on the even years between the International Conference on Hydrogen Safety (ICHS) which is held on the odd years. The research priorities workshop is intended to identify the state-of-the-art in understanding of the physical behavior of hydrogen and hydrogen systems with a focus on safety. Typical issues addressed include behavior of unintended hydrogen releases, transient combustion phenomena, effectiveness of mitigation measures, and hydrogen effects in materials. In the workshop critical knowledge gaps are identified. Areas of research and coordinated actions for the near and medium term are derived and prioritized from these knowledge gaps. The stimulated research helps pave the way for the rapid and safe deployment of hydrogen technologies on a global scale. To support the idea of delivering globally accepted research priorities for hydrogen safety the workshop is organized as an internationally open meeting. In attendance are stakeholders from the academic community (universities, national laboratories), funding agencies, and industry. The industry participation is critically important to ensure that the research priorities align with the current needs of the industry responsible for the deployment of hydrogen technologies. This report presents the results of the HySafe Research Priorities Workshop held in Washing- ton, D.C. on November 10-11, 2014. At the workshop the participants presented updates (since the previous workshop organized two years before in Berlin, Germany) of their research and development work on hydrogen safety. Following the workshop, participants were asked to provide feedback on high-priority topics for each of the research areas discussed and to rank research area categories and individual research topics within these categories. The research areas were ranked as follows (with the percentage of the vote in parenthesis): 1. Quantitative Risk Assessment (QRA) Tools (23%) 2. Reduced Model Tools (15%) 3. Indoor (13%) 4. Unintended Release-Liquid (11%) 5. Unintended Release-Gas (8%) 6. Storage (8%) 7. Integration Platforms (7%) 8. Hydrogen Safety Training (7%) 9. Materials Compatibility/Sensors (7%) 10. Applications (2%) The workshop participants ranked the need for Quantitative Risk Analysis (QRA) tools as the top priority by a large margin. QRA tools enable an informed expert to quantify the risk asso- ciated with a particular hydrogen system in a particular scenario. With appropriate verification and validation such tools will enable: * system designers to achieve a desired level of risk with suitable risk mitigation strategies, * permitting officials to determine if a particular system installation meets the desired risk level (performance based Regulations, Codes, and Standards (RCS) rather than prescrip- tive RCS), and * allow code developers to develop code language based on rigorous and validated physical models, statistics and standardized QRA methodologies. Another important research topic identified is the development of validated reduced physical models for use in the QRA tools. Improvement of the understanding and modeling of specific release phenomena, in particular liquid releases, are also highly ranked research topics. Acknowledgement The International Association HySafe, represented here by the authors, would like to thank all participants of the workshop for their valuable contributions. Particularly appreciated is the active participation of the industry representatives and the steady support by the European Com- mission's Joint Research Centre (JRC). Deep gratitude is owed for the great support by the United States Department of Energy (DOE) Office of Energy Efficiency and Renewable Energy's Fuel Cell Technologies Office (EERE/FCTO) for the organization of the 2014 version of the hydrogen safety research priorities workshop. This page intentionally left blank.

08 HYDROGEN↗
DOE OSTI2016

Nutrient cycling for biomass: Interactive proteomic/transcriptomic networks for global carbon management processes within poplar-mycorrhizal interactions

This project addresses the need to develop system-scale models at the symbiotic interface between ectomycorrhizal fungi (Laccaria bicolor) and tree species (Populus tremuloides) in response to environmental nutrient availability / biochemistry. Using our now well-established laboratory Laccaria x poplar system, we address the hypothesis that essential regulatory and metabolic mechanisms can be inferred from genomic, transcriptomic and proteomic-level changes that occur in response to environmental nutrient availability. The project addresses this hypothesis by applying state-of-the-art protein-level analytic approaches to fill the gap in our understanding of how mycorrhizal regulatory and metabolic processes at the transcript-level translate to nutrient uptake, carbon management and ultimate net primary productivity of plants. In most cases, these techniques were not previously optimized for poplar trees or Laccaria. Thus, one of the major contributions of this project has been to provide avenues for new research in these species by overcoming the pitfalls that had previously prevented the use of techniques such as ChIP-Seq and SWATH-proteomics. Since it is the proteins that sense and interact with the environment, participate in signal cascades, activate and regulate gene expression, perform the activities of metabolism and ultimately sequester carbon and generate biomass, an understanding of protein activities during symbiosis-linked nutrient uptake is critical to any systems-level approach that links metabolic processes to the environment. This project uses a team of experts at The University of Alabama in Huntsville (UAH), The University of Alabama at Birmingham (UAB) and Argonne National Laboratory (ANL) to address the above hypothesis using a multiple "omics" approach that combines gene and protein expression as well as protein modifications, and biochemical analyses (performed at Brookhaven National Laboratory (BNL)) in poplar trees under mycorrhizal and free living conditions. Together, the assembled team of experts completed all of the planned milestones set forth in this project. In addition to the planned approaches, several lines of exciting new research have also evolved during the course of this project that involved FTIR Imaging using the National Synchrotron Light Source at BNL. A summary of the approaches used in this project and key highlights are as follows: Having the right combination of microbes associated with plants is largely responsible for the plant’s ability to mine nutrients from the soil and to develop a strong “immune system”. Our current chemically focused and intensive culture tends to forget that plants obtain nutrients in two ways: (1) via water soluble chemical nutrients and (2) via the activity of acquired microbial symbionts. In healthy natural ecosystems, chemical nutrients are always in low abundance because the organisms within that system have already locked such nutrients away within the biological system itself. Thus, in nature it is the biological sources of nutrients and the microbes that have the capacity to mine those nutrients for their plant hosts that actually control the terrestrial nutrient cycles on this planet. Thus, a new push in the future may very well be to use our skills at elucidating complex patterns to strategically guide soil microbe communities to do what we want, essentially allowing nature to do the work of figuring out what is most efficient and effective for human needs. However, the findings of this project and other work in our lab lead to the hypothesis that the specific soil community composition is less important than the emergent properties of those communities. So, additional research into what soil communities are effective and how they are established will be key in developing human understanding of how to manipulate biological systems to meet human needs without causing undue damage to our environment.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2012

On-site Destruction of Radioactive Oily Wastes Using Adsorption Coupled with Electrochemical Regeneration - 12221

Arvia{sup R}, working with Magnox Ltd, has developed the technology of adsorption coupled with electrochemical regeneration for the degradation of orphan radioactive oil wastes. The process results in the complete destruction of the organic phase where the radioactivity is transferred to liquid and solid secondary wastes that can then be processed using existing authorised on-site waste-treatment facilities.. Following on from successful laboratory and pilot scale trials, a full scale, site based demonstrator unit was commissioned at the Magnox Trawsfynydd decommissioning site to destroy 10 l of LLW and ILW radioactive oils. Over 99% of the emulsified oil was removed and destroyed with the majority of activity (80 - 90%) being transferred to the aqueous phase. Secondary wastes were disposed of via existing routes with the majority being disposed of via the sites active effluent treatment plant. The regeneration energy required to destroy a litre of oil was 42.5 kWh/l oil. This on-site treatment approach eliminates the risks and cost associated with transporting the active waste oils off site for incineration or other treatment. The Arvia{sup R} process of adsorption coupled with electrochemical regeneration has successfully demonstrated the removal and destruction of LLW and ILW radioactive oils on a nuclear site. Over 99.9% of the emulsified oil was removed, with the majority of the radioactive species transferred to the aqueous, supernate, phase (typically 80 - 90 %). The exception to this is Cs-137 which appears to be more evenly distributed, with 43% associated with the liquid phase and 33 % with the Nyex, the remainder associated with the electrode bed. The situation with Plutonium may be similar, but this requires confirmation, hence further work is underway to understand the full nature of the electrode bed radioactive burden and its distribution within the body of the electrodes. - Tritium gaseous discharges were negligible; hence no off-gas treatment before direct discharge to atmosphere is necessary. All secondary wastes were suitable for disposal using existing disposal routes, with the majority of the activity being successfully discharged as active water via the site active drains. - Oil destruction was achieved at a rate of 28.2 ml/hr using a regeneration energy of 42.5 kWh/l oil. The treatment of different active and non-active oils was achieved using the same operating parameters, providing strong evidence that the process is robust and will treat a wide range of oils, organic wastes and additives. - Currently the design of a plant capable of processing 1000 ml/hr is being established in discussion with Magnox Ltd. The plant will run automatically with little operator attention and so process between 5-8 m{sup 3} of ILW oil per annum. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2023

Chromium Tolerant, Highly Active and Stable Electrocatalytic Internal Surface Coating for Cathode of Commercial SOFCs (Final Report)

This project is aimed to develop a chromium (Cr) tolerant, highly active, and stable coating layer on the internal surfaces of the porous composite cathode from commercially available SOFCs. Such coating layer was developed using the additive manufacturing process of Atomic Layer Deposition (ALD) and has been applied on the cathode consisting of either an electronic conductor of LaxSr 1-x MnyO 3-δ (LSM) or mixed ionic and electronic conducting La x Sr 1-x Co y Fe 1-y O 3-δ (LSCF). PI's work has demonstrated that the internal surface of cathode from the commercial cells, can be further tailored using ALD coating to dramatically enhance the cell performance. For instance, ALD layer consisting heterostructured nano composite of nano-Pt and nano-(Mn 0.8 Co 0.2 ) 3 O 4 oxide on the internal surface of porous LSM/YSZ cathode from SOFCs, has resulted in the large reduction of the cell polarizations resistance by up to 53%, and enormous increase of power density over 370%. For the cells with LSCF/Sm 2 O 3 doped CeO 2 (SDC) cathode, the conformal layer of nano-composite consisting of superjacent CoOx and subjacent minimum amount of Pt nano-grains has resulted in the power density enhancement by 126% for the large scale industry tubular cells at 750°C, and both the performance enhancement and nanostructure of the ALD layer are stable over ~ 2000 h continuous operation performed at industry test station. In the meanwhile, those ALD coating layer developed by PI's work is also inherently Cr-tolerant, and could act as physical barrier for preventing Cr diffusion into the cathode backbone, so as to mitigate the Cr poisoning effect on the cathode. In this project, the impact of Cr on the performance of those ALD coated commercial cells has been evaluated. Based on evolution of the cell performance, the ALD coating layer chemistry and ALD coating layer thickness has been optimized to maximize the overall Cr tolerance, cell power density and cell longevity. Different ALD coating has been applied onto the internal surface of LSM/YSZ and LSCF/SDC backbone respectively. The architecture/scaffold structures on the internal surface of different cathode, designed by this project, was catalogued and analyzed using High Resolution Transmission Electron Microscopy (HRTEM), and cell power/durability performance are assured via comprehensive electrochemical performance testing in the industry operation relevant conditions. The impact of the electrochemical operation current density, the water humidity, the cell operation temperature, and cell operation duration on the Cr tolerance of ALD coated cells has been systematically investigated. There is completely different nanostructure degradation mechanisms between LSM and LSCF cells induced by Cr contamination. For the LSCF/SDC baseline cell, With the Cr source, there is no apparent Sr surface segregation phase even for the baseline cell operated for 3000 h at 750 °C. With the Cr source, there is significant amorphous (SrCr)Ox phase accumulated in the original pore region. For the commercial baseline cells, Cr contaminants on the LSM electrode severely impacted the entire cell's electrochemical performance and nanostructure degradation. Those degradations include (1). Peak power density loss of 64 % after 109 h of operation. The dramatic increase in Rp (2). They are cracking at LSM/SSZ interface, LSM grains. SSZ remains intact but with (CrMn)Ox. By contrast, ALD coating (MnCo)Ox/Pt dramatically improves the Cr resistance, as follows (1). ALD-coated cell with a power density is 280-380 % of the baseline cell, depending on the ALD layer thickness. (2). For a cell with a 20 nm thick ALD layer, there is a large performance enhancement (> 200 % power density) induced by ALD coating of Cr-tolerant Mn 0.8 Co 0.2 Ox. (3). For a cell with a 20 nm thick ALD layer, after 168 h at 750 °C power density of the ALD-coated cell is ~ 600% of that baseline cell upon operation with Cr contamination for 109 h. The ALD coating on the internal surface of cathode developed by this project integrated multi-functions. Those multi-functions include (1). Dramatically improving the cell power density for the commercial cells; (2). Dramatically improving contamination resistance of the cathode, for being an excellent protection coating layer sealing off Cr contamination. (3). Dramatically increasing the cell longevity by potentially preventing the microstructure evolution and grain coarsening of the cathode. Overall, this project will provide a simple solution to simultaneously enhance power density and increase the reliability, robustness, and endurance of commercial SOFCs, over the entire operating temperature range of 650-800 °C. For the inherently functional SOFC, the ALD coating of LSM based cathode mitigate the Cr-contamination. Power density of ALD-coated cell is ~ 600% of that baseline cell upon operation with Cr contamination. In addition to SOFCs, the novel on-demand design approach and creation of multifunctional heterogeneous architecture on the electrode surface presented in this work opens further research for their application in other types of fuel cells, batteries, and sensors for which electrochemical reactions on the surface are similarly critical.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Potential Research and Development Opportunities for Light Water Reactor Spent Nuclear Fuel at INL

This report documents the commercial spent nuclear fuel currently in storage at Idaho National Laboratory with a specific focus on the potential research and development (R&D) opportunities for this material. Commercial spent nuclear fuel is stored in dry casks on the INL site at the Idaho Nuclear Technology and Engineering Center (INTEC, formerly the Idaho Chemical Processing Plant or ICPP). This spent fuel was part of the DOE-industry cooperative dry cask demonstration project that began in 1983 and from historical fuel testing and treatment activities that had been performed at the Test Area North (TAN)-607 facility. Most of the fuel is “low burnup,” but given that it was removed from the respective reactors between 1970 and 1985, it was representative for its time. The majority of the fuel is of the 15×15 Westinghouse PWR variety, though additional fuel types (e.g., TN-BRP) and configurations are also stored. Potential R&D opportunities identified are (1) the REA-2023 cask, (2) the TN-BRP cask, and (3) the Castor V/21 cask. Fuel from the TN-24P may be an alternative to the intact assemblies in the Castor V/21. Specifically, the REA-2023 cask contains 9 rods that have been exposed to air since 2005. These rods have a detailed pre-loading characterization and thus any changes in corrosion or geometry can most likely be attributed to the storage environment. In addition, similar rods to the nine in REA-2023 reside in the Castor V/21 cask whose environment has been maintained with inert nitrogen. The Castor V/21 cask also contains intact PWR assemblies that could be used to perform limited confirmation of the pyroprocessing approach. An alternative to the use of the Castor assemblies for pyroprocessing is the consolidated fuel that is stored in the TN-24P, which would not require removal from the assembly grid since it has already been packaged in accessible two-piece shell strongback containers. The TN-BRP cask contains a number of Gd-doped, low burnup assemblies that could be of use to validate code packages used to justify burnup-up credit for boiling water reactors (BWRs). The INL dry casks are stored on the CPP-2707 pad at INTEC, adjacent to the CPP-603 Irradiated Fuel Storage Facility, which incorporates a dry hot cell that has the potential to receive a full scale commercial cask of the types identified. Several evaluations have been made regarding this task, including full scale mockup testing of the physical clearances required to remove and handle fuel assemblies and components. A proposed schedule of 14 months and cost of $5.3 million was the outcome of analysis performed by Fluor Idaho and is included as Appendix A & B. In addition to the spent fuel at INL, there is also a full-scale mockup assembly that was fabricated for the Protypical Consolidation Demonstration Project to validate fuel rod consolidation approaches. The assembly was fabricated by Westinghouse as a 15 x 15 PWR, using Zircaloy-4 tubing and steel end fittings in accordance with product specifications. The only departure from specification is the use of copper metal in lieu of uranium oxide pellets to achieve a weight that is within 10% of the standard.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2016

Applications of Transient Grating Spectroscopy to Radiation Materials Science

Radiation damage is an inherently multi-scale phenomenon, with much of the key material evolution occurring at the mesoscale. Current techniques for the direct interrogation of material property changes due to irradiation either function with very small volumes, such as in-situ TEM, cannot cover the full range of defect populations produced, such as in positron annihilation spectroscopy, or requires destruction of the test material, such as in standard or micromechanical testing. In addition, the ultimate quantities of interest to radiation materials scientists are the changes in key material properties with irradiation. These include stiffness, ductility, and thermal conductivity for structural materials, and optical properties such as index of refraction or changes in transmittance spectra for optically active materials. The latter of these are often correlated directly to stress- or thermally-induced changes, themselves a function of the specific defect populations responsible for their change. The rapid study of such a mesoscale phenomenon requires an inherently mesoscale technique, where multiple quantities of interest can be accurately measured in very short times. Determining the sensitivity of any technique with known certainly is of critical importance to qualifying a new technique to measure in-situ material property changes during irradiation. In this paper, we present the new applicability of an existing technique, known as transient grating (TG) spectroscopy, to rapidly and accurately study key problems in radiation materials science. Results quantifying the absolute sensitivity of the technique are presented, alongside molecular dynamics (MD) simulations of the TG spectroscopy process to gauge direct agreement between theory, simulation, and experiment. An example problem of interest is demonstrated as an illustration of what is possible, showing elastic and thermal changes in irradiated silicon carbide (SiC) films. Finally, future work to quantify the effects of experimentally-simulated radiation defects is proposed, in support of building a database to use TG spectroscopy to deconvolve irradiated material property changes in-situ in terms of the defect populations responsible for their evolution. The application of the TG spectroscopy technique to in-situ radiation materials science has the potential to answer long-standing questions in the field, relating to ion beam rastering, the onset of void swelling, and direct measurement of radiation-created point defect concentrations. Before it can do so, the technique must carefully be analyzed and tuned to increase its sensitivity, the certainty of its results, and the ability to predict radiation-induced changes by simulations must be developed. Making such measurements in-situ with the aid of predictive MD simulations has the potential to elucidate mechanisms of radiation damage accumulation, as well as more rapidly qualify radiation-resistant alloys for service in nuclear systems. Work is underway to build this database of experimentally-simulated radiation-produced defects, which will be combined and compared with actual irradiated materials for eventual in-situ deconvolution of the TG signal into the defect populations responsible for irradiation-induced microstructural change. (authors)

36 MATERIALS SCIENCE↗
DOE OSTI2019

Minimization of Nuclear Waste using AHWR Reactor Technology

Nuclear sciences have grown from creating reactors to a greater understanding of how to dispose off the waste exhibited by the nuclear activities. Various methodologies have been proposed and are being used in order to do the same. This poster poses great attention to 'Using a fuel cycle dedicated to the production of the lower quantity of minor actinides, is one of the key targets in reducing nuclear waste in india'. A significant fraction of thorium is utilized as a fertile host in the Advanced Heavy Water Reactor (AHWR300-LEU) fuel. Being lower in the periodic table, it leads to a reduction of minor actinides. It produces only half of the minor actinides as a waste as compared to modern LWRs. As thorium oxide has inert nature, it benefits in its prolonged storage. Therefore, safe disposal of spent fuel is achieved due to the inert matrix, on completion of one fuel cycle mode. AHWR is a 300 MWe, vertical, pressure-tube type, boiling light water-cooled, and heavy water-moderated reactor. Employs natural circulation for removal of heat from the reactor core. In-situ conversion of {sup 232}Th into {sup 233}U. The reactor design permits flexible fuel cycle options. There are two types of AHWR depending upon the fuel cycle options. Uses thorium-based oxide fuels: two fuel cycle options. With the adoption of thorium fuel cycle, AHWR300-LEU produces less minor actinides. As compared to modern LWRSs, it produces almost 37% less amount of actinides for the same amount of energy production, which in turn minimizes the burden on waste disposal requirements. But, it is associated with radionuclides such as {sup 231}Pa (produced through absorption of one neutron and emission of two neutrons). Since, the reaction rate of (n,2n) reactions is very low in thermal neutron reactors, thus making the fuel cycle the favorable one. Thorium oxide (ThO{sub 2}) is chemically stable and is the highest oxidation state of thorium, therefore the inert nature of the matrix is advantageous for safe disposal of spent fuel in case of adoption of open fuel cycle mode and offers prolonged storage of spent fuel. The AHWR is thorium fueled Indian nuclear reactor that assimilates several new features with diminished environmental concern due to reduced waste generation. Since thorium fuel cycle produces less long lived nuclear waste, thus it can possibly bring the world cleaner and more sustainable nuclear energy. Currently, India being the only country with large scale research program of thorium nuclear power serves a platform for the development and demonstration of all technologies and advanced safety systems.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2018

Assessment of CO 2 Storage Resources in Depleted Oil and Gas Fields in the Ship Shoal Area, Gulf of Mexico

The Gulf of Mexico is one of the most important regions in the United States for energy resources and infrastructure. Gulf of Mexico federal offshore oil and gas production accounts for 17% of total U.S. crude oil production and 5% of total U.S. gas production (EIA Gulf of Mexico Fact Sheet). This region presents an excellent combination of high need and significant opportunity for large scale geologic storage of CO 2 . The Ship Shoal Area is located about 20 miles offshore Louisiana within the Gulf Coast federal waters. Miocene and Pliocene sediments in the Ship Shoal Area are proven to provide excellent and secure traps for oil and gas. The Ship Shoal Area contains a large number of depleted oil and gas fields either currently abandoned, or planned for abandonment by 2025, which may provide very significant potential CO 2 storage capacity. GeoMechanics Technologies conducted a comprehensive research project to better characterize Neogene sediments in the Ship Shoal Area for high volume CO 2 storage. The data generated from literature, well data, well log, and formation evaluation were input into Rockwork 16 geologic software to create a detailed geologic model for the Ship Shoal study area. The geologic grids were then fed into TOUGH2, the gas migration model software and FLAC 3D, the geomechanical model software. The fluid flow modeling for both the Miocene and Pliocene simulation from both Block 107 and Block 84 indicated that Pliocene and Miocene are a good reservoir for the CO 2 sequestration. Thirty years of CO 2 injection (at a rate of 1 million metric tons CO 2 per year) and 30 years of observation simulations were run with the fluid flow modeling. The 3D geomechanical modeling for Ship Shoal Block 107 and Block 84 were developed to evaluate induced surface deformation and potential fault reactivation after 30 years CO 2 injection at base of Pliocene and at upper Miocene injection locations. Evaluation results indicate low to no risks for fault slips or fault reactivation. Twelve well bores and 76 well bores for Ship Shoal Blocks 84 and 107 respectively were reviewed for their cement history. Most wells (57 out of 76 and 7 out of 12 wells in Ship Shoal Block 107 and 84 respectively) have good integrity. Nineteen and 5 wells (in Ship Shoal Block 107 and 84 respectively) with no top plug, incomplete cement or Plug and Abandonment information are given yellow cautionary indicators. These cautionary wells may provide leakage paths of CO 2 through the well bores to the USDWs. Using our Quantitative Risk & Decision Analysis Tool (QRDAT) for caprock integrity evaluation, we compared Ship Shoal’s risk to that of In Salah, Sleipner, Kevin Dome, Loudon, Illinois Industrial CCS and Wilmington Graben. We found the risk at the Ship Shoal Blocks 84 and 107 fields are similar to the known CO 2 active sequestration sites, but lower than the Wilmington Graben turbidities offshore California studied site. The risk of natural seismicity in the Gulf of Mexico is relatively low. Geomechanics Technologies has documented the top 25 CO 2 emission sources within the close proximity of the Ship Shoal Block 84 and 107 fields. All the offshore and onshore pipelines have been digitized and can be viewed in an interactive website (http://www.geomechanicstech.com/shipshoal.html). We also performed a feasibility study on the potential for converting existing oil or gas pipelines for CO 2 transport. There are abandoned, idled and retired onshore and offshore pipelines. However, there is no standard specification for maximum pipeline pressures needed for CO 2 transport. It is a function of design, materials, and testing provided; thus it will be the responsibility of the pipeline operator to correctly determine, maintain and operate within the limits of the pipelines. There are a few transit corridors extending from onshore Louisiana (Cailou Bay) to offshore trunk-lines. The cost for constructing a pipeline has increased about 46% from 2015 to an average cost of $5,064,046 per mile in 2016. We use the NETL CO 2 storage resource mass estimate to calculate the potential resources for Ship Shoal Block 84 and 107 fields using the depleted oil and gas reservoir volume and sand volume generated from our geologic modeling. The estimated storage resource results are greater when using the sand volumes derived through geologic modeling than the oil and gas reservoir data. The difference is due to the depleted oil and gas reservoir information not accounting for the water-flooded sand located below the oil/gas-water contact or unproductive sand units. Resource calculation using the sand volume obtained through geologic modeling overestimate the storage capacity as the model accounts for all sand within the formation, not just the interconnected sand.

02 PETROLEUM↗