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DOE OSTI2018

Overview of IAEA MODARIA II Program Working Group 1 on Assessment and Decision Making of Existing Exposure Situations for NORM and Nuclear Legacy Sites - 18308

The International Atomic Energy Agency (IAEA) launched the Modelling and Data for Radiological Impact Assessments (MODARIA) II Programme in October. As part of the IAEA effort to enhance the capabilities of its Member States in assessing radiological impacts of radionuclides released to the environment from sites that were not operated in accordance with current standards, and to ensure protection of the public and the environment, the MODARIA II Programme aims to: (1) test the performance of models developed for predicting the transfer of radionuclides in the environment and assessing radiological impacts to the public and the environment; (2) develop and improve models for particular environments and, where appropriate, to agree on data sets that are generally applicable for use in testing environmental transfer models; and (3) provide an international forum for the exchange of experiences, ideas and research information. The Programme will run for 3 years from 2016 to 2019. The Programme comprises seven working groups covering a wide range of topics (https://wwwns.iaea.org/projects/modaria/modaria2.asp?s=8 and l=129). MODARIA II Working Group 1 (WG1) is focused on dose assessment and decision making regarding existing exposure situations due to naturally occurring radioactive material (NORM) and nuclear legacy sites. WG1 was formed as a combination of two MODARIA I WGs: WG1 focused on application of decision-aiding tools in remediation; and WG3 focused on risk assessment for NORM and radioactively contaminated legacy sites (https://wwwns.iaea.org/projects/modaria/default.asp?s=8 and l=129). It was recognized that the decision-making needs will inform the scope of risk assessments, and the risk insights and structured decision analyses will aid in informed decision-making. Therefore, MODARIA II WG1 is focused on developing methods and toolsets for risk-informed decision-making for NORM and nuclear legacy sites, including demonstration of decision-making processes and tools through case studies. MODARIA II WG1 has 91 registered participants from 33 Member States and IAEA (as of November 2017), some 30 of whom are actively engaged in various collaborative research and development activities within WG1. Members of WG1 participated in the First Technical Meeting of MODARIA II, which was held in Vienna, Austria from 31 October to 4 November 2016. The group then held its First Interim Meeting in Brussels, Belgium from 26 to 30 June 2017, which included a field trip to the legacy Tessenderlo Chemie (TCH) Phosphate Processing Site. At this meeting, the TCH Site and the Pridneprovsky Chemical Plant (PChP) in Ukraine were selected for case studies. The Los Alamos National Laboratory (LANL) Material Disposal Area B in the USA and the Beaverlodge Uranium Mill and Mill Site in northern Canada were selected as examples for sharing of good practices and lessons learned in risk-informed decision-making for environmental remediation and land conveyance. At the Second Technical Meeting held in Vienna on 30 October to 3 November 2017, an additional NORM site for tin processing in Brazil was added to the case studies, with another NORM site in Yunnan, China included for consideration at the Second Interim Meeting of WG1. The Second Interim Meeting will be held in in early to mid-May, 2018. The group has also decided to prepare an Interim Report by October 2018 to document the WG1 discussions and analyses for the period of 2016-2018, which will be finalized at the conclusion of MODARIA II in October 2019. Initial assignments have been discussed for IM1 participants to collect data, conduct modelling and analyses, and prepare draft sections for the Interim Report. This paper will provide an overview of the work plans for WG1. It will also highlight some near-term activities that the group is currently working on. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2014

Physical Property Measurements of Laboratory Prepared Saltstone Grout

The Saltstone Production Facility (SPF) built two new Saltstone Disposal Units (SDU), SDU 3 and SDU 5, in 2013. The variable frequency drive (VFD) for the grout transfer hose pump tripped due to high current demand by the motor during the initial radioactive saltstone transfer to SDU 5B on 12/5/2013. This was not observed during clean cap processing on July 5, 2013 to SDU 3A, which is a slightly longer distance from the SPF than is SDU 5B. Saltstone Design Authority (SDA) is evaluating the grout pump performance and capabilities to transfer the grout processed in SPF to SDU 3/5. To assist in this evaluation, grout physical properties are required. At this time, there are no rheological data from the actual SPF so the properties of laboratory prepared samples using simulated salt solution or Tank 50 salt solution will be measured. The physical properties of grout prepared in the laboratory with de-ionized water (DI) and salt solutions were obtained at 0.60 and 0.59 water to premix (W/P) ratios, respectively. The yield stress of the DI grout was greater than any salt grout. The plastic viscosity of the DI grout was lower than all of the salt grouts (including salt grout with admixture). When these physical data were used to determine the pressure drop and fluid horsepower for steady state conditions, the salt grouts without admixture addition required a higher pressure drop and higher fluid horsepower to transport. When 0.00076 g Daratard 17/g premix was added, both the pressure drop and fluid horsepower were below that of the DI grout. Higher concentrations of Daratard 17 further reduced the pressure drop and fluid horsepower. The uncertainty in the single point Bingham Plastic parameters is + 4% of the reported values and is the bounding uncertainty. Two different mechanical agitator mixing protocols were followed for the simulant salt grout, one having a total mixing time of three minutes and the other having a time of 10 minutes. The Bingham Plastic parameters were essentially the same for the salt grout without admixture. When Daratard 17 was added, the Bingham Plastic yield stress increased for the 10 minute mix. The simulant salt used in this task had similar physical properties of the Tank 50 3Q13 salt grout and is recommended for future use, if the salt solution in Tank 50 does not change. The design basis physical properties used to size the pumps and mixers at SPF were obtained from DPST-85-312. The grouts characterized in this report are bounded by the design basis density and Bingham Plastic yield stress. The opposite is true for the plastic viscosity. Steady state pressure drop calculations were performed for the design basis values using the flow rate for the clean cap and salt grouts and they bound the pressure drop of the grouts characterized in this report. A comparison of the lab prepared samples to PI ProcessBook data, specifically average pressure drop, indicate that the lab prepared samples are more viscous in nature than what is processed in the facility. This difference could be due to the applied shear rates which could be lower in the lab as compared to the facility and that fact the SPF added flush water, making this comparison more difficult. A perfunctory review of the PI ProcessBook data was discussed. It may be possible that the frequency that the distributed control system alters the grout pump speed to maintain grout hopper volume can negatively affect the efficiency of the grout pump.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2013

Uranium Fate and Transport Modeling, Guterl Specialty Steel Site, New York - 13545

The Former Guterl Specialty Steel Corporation Site (Guterl Site) is located 32 kilometers (20 miles) northeast of Buffalo, New York, in Lockport, Niagara County, New York. Between 1948 and 1952, up to 15,875 metric tons (35 million pounds) of natural uranium metal (U) were processed at the former Guterl Specialty Steel Corporation site in Lockport, New York. The resulting dust, thermal scale, mill shavings and associated land disposal contaminated both the facility and on-site soils. Uranium subsequently impacted groundwater and a fully developed plume exists below the site. Uranium transport from the site involves legacy on-site pickling fluid handling, the leaching of uranium from soil to groundwater, and the groundwater transport of dissolved uranium to the Erie Canal. Groundwater fate and transport modeling was performed to assess the transfer of dissolved uranium from the contaminated soils and buildings to groundwater and subsequently to the nearby Erie Canal. The modeling provides a tool to determine if the uranium contamination could potentially affect human receptors in the vicinity of the site. Groundwater underlying the site and in the surrounding area generally flows southeasterly towards the Erie Canal; locally, groundwater is not used as a drinking water resource. The risk to human health was evaluated outside the Guterl Site boundary from the possibility of impacted groundwater discharging to and mixing with the Erie Canal waters. This condition was evaluated because canal water is infrequently used as an emergency water supply for the City of Lockport via an intake located approximately 122 meters (m) (400 feet [ft]) southeast of the Guterl Site. Modeling was performed to assess whether mixing of groundwater with surface water in the Erie Canal could result in levels of uranium exceeding the U.S. Environmental Protection Agency (USEPA) established drinking water standard for total uranium; the Maximum Concentration Limit (MCL). Geotechnical test data indicate that the major portion of uranium in the soil will adsorb or remain bound to soil, yet leaching to groundwater appears as an on-site source. Soil leaching was modeled using low adsorption factors to replicate worst-case conditions where the uranium leaches to the groundwater. Results indicate that even after several decades, which is the period of time since uranium was processed at the Guterl Site, leaching from soil does not fully account for the currently observed levels of groundwater contamination. Modeling results suggest that there were historic releases of uranium from processing operations directly to the shallow fractured rock and possibly other geochemical conditions that have produced the current groundwater contamination. Groundwater data collected at the site between 1997 and 2011 do not indicate an increasing level of uranium in the main plume, thus the uranium adsorbed to the soil is in equilibrium with the groundwater geochemistry and transport conditions. Consequently, increases in the overall plume concentration or size are not expected. Groundwater flowing through fractures under the Guterl Site transports dissolved uranium from the site to the Erie Canal, where the groundwater has been observed to seep from the northern canal wall at some locations. The seeps discharge uranium at concentrations near or below the MCL to the Erie Canal. Conservative mixing calculations were performed using two worst-case assumptions: 1) the seeps were calculated as contiguous discharges from the Erie Canal wall and 2) the uranium concentration of the seepage is 274 micrograms per liter (μg/L) of uranium, which is the highest on-site uranium concentration in groundwater and nearly ten-fold the actual seep concentrations. The results indicate that uranium concentrations in the seep water would have to be more than 200 times greater than the highest observed on-site groundwater concentrations (or nearly 55,000 μg/L) to potentially exceed the drinking water standard (the MCL) for total uranium in the Erie Canal. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2019

Erosion Challenges at the L-Bar Disposal Site - 19561

The L-Bar, New Mexico, Disposal Site is located in the northeast corner of Cibola County, 10 miles north of Laguna, and was the former site of a uranium mill and underground mine. The mill operated from 1977 to 1981 where a total of 1.9 x 10{sup 6} tonnes (2.1 million tons) of ore was processed. Solid and liquid byproduct, or tailings, from the milling process were impounded behind a dam constructed of native weathered Mancos Shale, which is a predominant geologic formation in the area. The tailings were encapsulated in place, and the resulting 40.5-hectare (100-acre) engineered disposal cell was completed in 2000. The 299-hectare (738-acre) Uranium Mill Tailings Radiation Control Act Title II site was transferred to the US Department of Energy (DOE) Office of Legacy Management under a US Nuclear Regulatory Commission general license in 2004. During reclamation activities, channels were designed and constructed into the surrounding weathered shale to protect the disposal cell from high-precipitation events. Due to the highly erodible soils and anticipated sediment deposition into the diversion channels, a sediment trap was also excavated. By excavating the channels and sediment trap, the local base elevation was altered, which exacerbated erosional forces. Recontouring surrounding drainage basins during the reclamation activities also promoted erosion by reducing natural rock armoring and vegetation that aids in soil stability. To compound the erosion issue, the L-Bar site is susceptible to short-duration, high-intensity, localized convective storms. Because the local geomorphology includes soils consisting of weathered shale, these precipitation events are not conducive to absorption into the soils, but rather to sheet flows that follow topography and concentrate in lower elevation areas where flow volumes and velocities increase. These factors result in the formation of deeply incised gullies and promote soil piping, which is an important geomorphic process in the widening of arroyos and the advancement of head-cutting, evident at the L-Bar site and surrounding areas. At the first annual inspection by DOE in 2005, it was noted that extensive erosion was occurring upgradient of the sediment trap. DOE determined that the design of the site's drainage system was the cause of extensive erosion. It is believed that by lowering the base elevation of the local drainage system through excavation of the sediment trap, the geomorphic response common to fluvial systems in a semiarid environment has increased the incision and remobilization of sediment downstream. Over time, these sediments would be deposited in the channels, which are designed to divert runoff away from the disposal cell, effectively limiting their capacities. The development of alluvial fans on one side of the channel directs flows to the opposite side of the channel, presenting the risk of cutting into the side slopes of the disposal cell. In addition, the upstream migrating gullies could intersect access roads and create hazards for adjacent stakeholders, including their grazing livestock. Current estimates conclude that potential offsite impacts could occur within the next 20 years, with gully migrations of up to 19 meters (63 feet) per year. In 2009, several erosion-control structures were constructed to reduce runoff velocities and ease the elevation differential created by the construction of the sediment trap and diversion channels. The first measurable storm events after construction occurred in August and September 2011, where one structure washed out and another structure was bypassed when runoff breached an earthen berm. DOE has conducted site assessments, continues to monitor erosion, and has applied lessons learned in the process of evaluating options to repair or modify the structures to stabilize the site and prevent potential short-term damage to adjacent properties as well as long-term damage to the disposal cell. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2015

Stationary Liquid Fuel Fast Reactor

For effective burning of hazardous transuranic (TRU) elements of used nuclear fuel, a transformational advanced reactor concept named SLFFR (Stationary Liquid Fuel Fast Reactor) was proposed based on stationary molten metallic fuel. The fuel enters the reactor vessel in a solid form, and then it is heated to molten temperature in a small melting heater. The fuel is contained within a closed, thick container with penetrating coolant channels, and thus it is not mixed with coolant nor flow through the primary heat transfer circuit. The makeup fuel is semi- continuously added to the system, and thus a very small excess reactivity is required. Gaseous fission products are also removed continuously, and a fraction of the fuel is periodically drawn off from the fuel container to a processing facility where non-gaseous mixed fission products and other impurities are removed and then the cleaned fuel is recycled into the fuel container. A reference core design and a preliminary plant system design of a 1000 MWt TRU- burning SLFFR concept were developed using TRU-Ce-Co fuel, Ta-10W fuel container, and sodium coolant. Conservative design approaches were adopted to stay within the current material performance database. Detailed neutronics and thermal-fluidic analyses were performed to develop a reference core design. Region-dependent 33-group cross sections were generated based on the ENDF/B-VII.0 data using the MC2-3 code. Core and fuel cycle analyses were performed in theta-r-z geometries using the DIF3D and REBUS-3 codes. Reactivity coefficients and kinetics parameters were calculated using the VARI3D perturbation theory code. Thermo-fluidic analyses were performed using the ANSYS FLUENT computational fluid dynamics (CFD) code. Figure 0.1 shows a schematic radial layout of the reference 1000 MWt SLFFR core, and Table 0.1 summarizes the main design parameters of SLFFR-1000 loop plant. The fuel container is a 2.5 cm thick cylinder with an inner radius of 87.5 cm. The fuel container is penetrated by twelve hexagonal control assembly (CA) guide tubes, each of which has 3.0 mm thickness and 69.4 mm flat-to-flat outer distance. The distance between two neighboring CA guide tube is selected to be 26 cm to provide an adequate space for CA driving systems. The fuel container has 18181 penetrating coolant tubes of 6.0 mm inner diameter and 2.0 mm thickness. The coolant tubes are arranged in a triangular lattice with a lattice pitch of 1.21 cm. The fuel, structure, and coolant volume fractions inside the fuel container are 0.386, 0.383, and 0.231, respectively. Separate steel reflectors and B4C shields are used outside of the fuel container. Six gas expansion modules (GEMs) of 5.0 cm thickness are introduced in the radial reflector region. Between the radial reflector and the fuel container is a 2.5 cm sodium gap. The TRU inventory at the beginning of equilibrium cycle (BOEC) is 5081 kg, whereas the TRU inventory at the beginning of life (BOL) was 3541 kg. This is because the equilibrium cycle fuel contains a significantly smaller fissile fraction than the LWR TRU feed. The fuel inventory at BOEC is composed of 34.0 a/o TRU, 41.4 a/o Ce, 23.6 a/o Co, and 1.03 a/o solid fission products. Since uranium-free fuel is used, a theoretical maximum TRU consumption rate of 1.011 kg/day is achieved. The semi-continuous fuel cycle based on the 300-batch, 1- day cycle approximation yields a burnup reactivity loss of 26 pcm/day, and requires a daily reprocessing of 32.5 kg of SLFFR fuel. This yields a daily TRU charge rate of 17.45 kg, including a makeup TRU feed of 1.011 kg recovered from the LWR used fuel. The charged TRU-Ce-Co fuel is composed of 34.4 a/o TRU, 40.6 a/o Ce, and 25.0 a/o Co.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2012

Nuisance Odors: Is there a Concern - 12340

Nuisance odors are generally thought of as just being annoying or unpleasant and not causing any physiological harm to our internal organs or other biologic systems. Yet during an excavation of buried animal remains, field workers experienced a multitude of symptoms that are associated with exposures to toxic materials. An examination of the decomposition process revealed that there is a potential off-gassing of a number of common, yet harmful chemicals including ammonia, mercaptans, hydrogen sulfide, butyric acid and phenol. In addition, other compounds, that have limited information such as established health data and occupational exposure limits, were also potential contaminants-of-concern. While a variety of monitoring and sampling techniques were used to assess worker exposures, all results indicated non-detectable airborne concentrations. Nevertheless, workers were experiencing such symptoms as nausea and headaches. As such, protective measures were necessary for field personnel to continue work while having confidence that the project was instituting sincere steps to ensure their health and safety. Researching the possible reasons for the causes of workers exhibiting adverse health effects from nuisance odors revealed that such exposures initiate electrochemical pathways, starting from the olfactory bulb to the brain, followed by a transfer of information to such biologic systems as the hypothalamus and pituitary gland. These systems, in turn, secrete hormones that cause a number of involuntary reactions; many of which are observed as typical adverse health effects, when in fact, they are merely reactions caused by the brain's memory; most likely created from previous experiences to unpleasant odors. The concern then focuses of how the Occupational Safety and Health community shall respond to such workplace exposures. Future work in this area may need to focus on the viability of current occupational exposure limits and the possibility of revising these standards. Another area of consideration would be whether nuisance odors will need separate and distinct criteria with regards to hazard identification and control. While evidence suggests that odorants do not cause direct toxicological effects to the various biologic systems, they can be influential by initiating symptoms that are associated with known toxins. The difference between the classic toxic systemic reactions and those initiated by nuisance odors can be summarized as one causing a dysfunction of a target organ or system as opposed to triggering a message to the brain which causes a physical reaction. While strong odors may exist at HAZWOPER work sites, their particular risk of pathogenic disease has yet to be established. This leaves many unanswered questions; the most obvious being, 'can an odorous chemical that can result in headaches, nausea, changes in blood pressure, body temperature, etc., be considered a toxin even if biological systems remain unaffected and sampling/monitoring protocol negative stimuli, thereby causing symptomatic experiences; will such disciplines as psychology need to be considered as part of the expertise within the field a environmental and occupational health? In the classic text, 'The Fundamentals of Industrial Hygiene' industrial hygiene has been defined as 'that science and art devoted to the anticipation, recognition, evaluation, and control of those environmental factors or stressors arising in or from the workplace that may cause sickness, impaired health and well-being, or significant discomfort among workers or among the citizens of the community'. Based on this definition, it is indeed the responsibility of the occupational health professional to move forward and to provide an effective program to 'anticipate, recognize, evaluate, and control' such airborne contaminants that may not be adequately controlled based on current knowledge and technology. The question is, 'Is the industrial hygiene community equipped to carry out this responsibility?' 'Are new assessment methods and tools necessary? Are alternate exposure limits needed and can they be adequately implemented? As more of the non-traditional health hazards become recognized, it appears that it shall be essential for more sophisticated methods to be part of the standard practice used to assess human health. Whether that means more sensitive equipment that has greater detection capabilities, or the development of new technologies designed specifically for these hazards, at present can only be left to speculation. While the occupational health community may wrestle with these questions, the responsibility of the safety and health community must maintain its diligence. As such, persons within the discipline of environmental and occupational health must continue to communicate the hazards and controls to the work force. Through such efforts, the workforce shall become engaged in the process of hazard identification, assessment and control, which, in turn, will create a greater appreciation and acceptance for field assessment methods as well as the processes by which workplace controls are designed to protect them. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2012

PDC IC Weld Failure Evaluation and Resolution

During final preparations for start of the PDCF Inner Can (IC) qualification effort, welding was performed on an automated weld system known as the PICN. During the initial weld, using a pedigree canister and plug, a weld defect was observed. The defect resulted in a hole in the sidewall of the canister, and it was observed that the plug sidewall had not been consumed. This was a new type of failure not seen during development and production of legacy Bagless Transfer Cans (FB-Line/Hanford). Therefore, a team was assembled to determine the root cause and to determine if the process could be improved. After several brain storming sessions (MS and T, R and D Engineering, PDC Project), an evaluation matrix was established to direct this effort. The matrix identified numerous activities that could be taken and then prioritized those activities. This effort was limited by both time and resources (the number of canisters and plugs available for testing was limited). A discovery process was initiated to evaluate the Vendor's IC fabrication process relative to legacy processes. There were no significant findings, however, some information regarding forging/anneal processes could not be obtained. Evaluations were conducted to compare mechanical properties of the PDC canisters relative to the legacy canisters. Some differences were identified, but mechanical properties were determined to be consistent with legacy materials. A number of process changes were also evaluated. A heat treatment procedure was established that could reduce the magnetic characteristics to levels similar to the legacy materials. An in-situ arc annealing process was developed that resulted in improved weld characteristics for test articles. Also several tack welds configurations were addressed, it was found that increasing the number of tack welds (and changing the sequence) resulted in decreased can to plug gaps and a more stable weld for test articles. Incorporating all of the process improvements for the actual can welding process, however, did not result in an improved weld geometry. Several possibilities for the lack of positive response exist, some of which are that (1) an insufficient number of test articles were welded under prototypic conditions, (2) the process was not optimized so that significant improvements were observable over the "noise", and (3) the in-situ arc anneal closed the gap down too much so the can was unable to exhaust pressure ahead of the weld. Several operational and mechanical improvements were identified. The weld clamps were changed to a design consistent with those used in the legacy operations. A helium puff operation was eliminated; it is believed that this operation was the cause of the original weld defect. Also, timing of plug mast movement was found to correspond with weld irregularities. The timing of the movement was changed to occur during weld head travel between tacks. In the end a three sequential tack weld process followed by a pulse weld at the same current and travel speed as was used for the legacy processes was suggested for use during the IC qualification effort. Relative to legacy welds, the PDC IC weld demonstrates greater fluctuation in the region of the weld located between tack welds. However, canister weld response (canister to canister) is consistent and with the aid of the optical mapping system (for targeting the cut position) is considered adequate. DR measurements and METs show the PDC IC welds to have sufficient ligament length to ensure adequate canister pressure/impact capacity and to ensure adequate stub function. The PDC welding process has not been optimized as a result of this effort. Differences remain between the legacy BTC welds and the PDC IC weld, but these differences are not sufficient to prevent resumption of the current PDC IC qualification effort. During the PDC IC qualification effort, a total of 17 cans will be welded and a variety of tests/inspections will be performed. The extensive data collected during that qualification effort should be of a sufficient population to determine if additional weld process optimization is necessary prior to production release.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2012

Reducing the Cost of Solar Cells

Solar-powered electricity prices could soon approach those of power from coal or natural gas thanks to collaborative research with solar startup Ampulse Corporation at the National Renewable Energy Laboratory. Silicon wafers account for almost half the cost of today's solar photovoltaic panels, so reducing or eliminating wafer costs is essential to bringing prices down. Current crystalline silicon technology converts energy in a highly efficient manner; however, that technology is manufactured with processes that could stand some improvement. The industry needs a method that is less complex, creates less waste and uses less energy. First, half the refined silicon is lost as dust in the wafer-sawing process, driving module costs higher. Wafers are sawn off of large cylindrical ingots, or boules, of silicon. A typical 2-meter boule loses as many as 6,000 potential wafers during sawing. Second, the wafers produced are much thicker than necessary. To efficiently convert sunlight into electricity, the wafers need be only one-tenth the typical thickness. NREL, the Oak Ridge National Laboratory and Ampulse have partnered on an approach to eliminate this waste and dramatically lower the cost of the finished solar panels. By using a chemical vapor deposition process to grow the silicon on inexpensive foil, Ampulse is able to make the solar cells just thick enough to convert most of the solar energy into electricity. No more sawdust - and no more wasting refined silicon materials. NREL developed the technology to grow high-quality silicon and ORNL developed the metal foil that has the correct crystal structure to support that growth. Ampulse is installing a pilot manufacturing line in NREL's Process Development Integration Laboratory, where solar companies can work closely with lab scientists on integrated equipment to answer pressing questions related to their technology development, as well as rapidly overcoming R and D challenges and risk. NREL's program is focused on transformative innovation in the domestic PV industry. With knowledge and expertise acquired from the PDIL pilot production line tools, Ampulse plans to design a full-scale production line to accommodate long rolls of metal foil. The Ampulse process 'goes straight from pure silicon-containing gas to high-quality crystal silicon film,' said Brent Nelson, the operational manager for the Process Development Integration Laboratory. 'The advantage is you can make the wafer just as thin as you need it - 10 microns or less.' Most of today's solar cells are made out of wafer crystalline silicon, though thin-film cells made of more exotic elements such as copper, indium, gallium, arsenic, cadmium, tellurium and others are making a strong push into the market. The advantage of silicon is its abundance, because it is derived from sand. Silicon's disadvantage is that purifying it into wafers suitable for solar cells can be expensive and energy intensive. Manufacturers add carbon and heat to sand to produce metallurgical-grade silicon, which is useful in other industries, but not yet suitable for making solar cells. So this metallurgical-grade silicon is then converted to pure trichlorosilane (SiCl3) or silane (SiH4) gas. Typically, the purified gas is then converted to create a silicon feedstock at 1,000 degrees Celsius. This feedstock is melted at 1,414 C and recrystallized into crystal ingots that are finally sawed into wafers. The Ampulse method differs in that it eliminates the last two steps in the traditional process and works directly with the silane gas growing only the needed silicon right onto a foil substrate. A team of NREL scientists had developed a way to use a process called hot-wire chemical vapor deposition to thicken silicon wafers with near perfect crystal structure. Using a hot tungsten filament much like the one found in an incandescent light bulb, the silane gas molecules are broken apart and deposited onto the wafer using the chemical vapor deposition technique at about 700 C - a much lower temperature than needed to make the wafer. The hot filament decomposes the gas, allowing silicon layers to deposit directly onto the substrate. Armed with this new technique, Branz and Teplin searched for ways to grow the silicon on cheaper materials and still use it for solar cells. They found the ideal synergy when visiting venture capitalists from Battelle Ventures asked them whether they could do anything useful with a breakthrough from Oak Ridge's superconducting wire development group. The new development, called the rolling assisted biaxially textured substrate (RABiTS), was just the opportunity the two scientists had been seeking. If metal foil is to work as a substrate, it must be able to act as a seed crystal so the silicon can grow on it with the correct structure. The RABiTS process forms crystals in the foil that are correctly oriented to receive the silicon atoms and lock them into just the right positions.

14 SOLAR ENERGY↗

DOE OSTI2024

The Uranium-Containing and Thorium-Containing Anions Studied by Photoelectron Spectroscopy

An in-depth knowledge of actinide chemistry is fundamental to many aspects of nuclear science and technology, including the synthesis and processing of materials and the remediation of waste disposal sites. Among the actinides, the chemical bonding behaviors of actinium and thorium resemble those of the transition metals; the 5f-electrons of protactinium, uranium, neptunium, and plutonium often play important roles in their bonding; and among the still heavier elements, their bonding tends to mimic the lanthanide elements in terms of electron shielding and their f-electron contributions. Bonding that involves 5f-electrons, however, is especially important, in part because of the significance of uranium and plutonium, but also because these elements are among the few where f-electron participation in bonding is relatively common. This work focused on studying uranium-containing and thorium-containing anions in the gas phase using negative ion photoelectron spectroscopy. Since this technique directly probed valence electrons, it was uniquely positioned to address open questions regarding molecular bonding and electron configurations. A particularly important issue concerned how bonding in actinide-containing molecules was affected by modifications to their actinide atoms’ environment, i.e., due to their interaction with ligands. A closely related question was how actinide atoms’ suborbitals were qualitatively reordered and their energies quantitatively shifted as a result of their ligated environments. These were especially relevant issues in regard to uranium due to it having multiple possible oxidation states (OS) and the potential for 5f electron participation in bonding. The effects of ligands on oxidation states and 5f-orbital energies in uranium bonding was expected to be pronounced. Both ligands and excess electrons were seen as probes of actinide atoms within actinide-containing molecules. Our strategy for advancing knowledge of chemical bonding in the actinide-containing species utilized the synergy between experiments and theory, where in some cases experimental results validated theory and where in others computational results assisted in interpreting experiments. Calculations on actinide systems are terrifically challenging due to large spin-orbit interactions, relativistic effects, and just the sheer number of electrons involved. Even in the simplest species, e.g., U and U2, the most sophisticated, modern calculations carried out by the most experienced theorists often only approximate experimentally-measured values, such as electron affinities. For theory to provide confident predictions that can be used to solve real problems it needed an iterative and ultimately corrective mechanism by which its methods can develop further. Experiments can be used to identify when theory has failed; whereupon the subsequent process of using the experiment-theory interplay can be used to find the cause of the failure. Upon fixing it in one case, different test species can be proposed and studied by the experiment-theory combination to determine whether the problem has been corrected. Thus, experiments not only measure the values of molecular properties, they also provide navigational 3 beacons that keep computations off the reefs in an otherwise dark sea with few reference points. Experimental measurements in the actinide field are not only important, they are in actuality essential to computational progress. While it was not always possible to compare the theoreticallydetermined quantity of interest directly with the same experimentally-measured observable, it was usually possible to compare consequential properties that are both calculable and measurable. In the work completed here electron affinities and electronic state spacings were often sensitive consequential parameters. Reasonable agreement between measured and computational values signaled that a calculation that was very likely to be on-track. We had established collaborative relationships with five computational groups, all of which have expertise in computational actinide chemistry. Their PI’s are L. Cheng, D. Dixon, L. Gagliardi, K. Peterson, and B. Vlaisavljevich. Our close interaction with our theory partners led to us suggesting systems to them and them to us. This reciprocal interaction between our experimental and their computational results was among the most important strengths of this work and was a thread woven throughout. Even though anion photoelectron spectroscopic studies are conducted on anions, much of the information that they provide, pertains to the electronic structure of the neutral counterparts of those anions; among these are electron affinities and electronically excited state spacings. Our experimental tools included several specialized ion sources for forming the anionic species of interest, a mass spectrometer for identifying and mass-selecting them, and an anion photoelectron spectrometer for determining their electron affinities (EA) and characterizing the electronic states of the selected anions’ neutral counterparts. Anion photoelectron spectroscopy is conducted by crossing a mass-selected beam of anions with a fixed-frequency laser beam and energy-analyzing the resultant photodetached electrons. The photodetachment process is governed by the energyconserving relationship: hν = EBE + EKE, where hν is the photon’s energy, EBE is the electron binding (photodetachment transition) energy, and EKE is the electron’s kinetic energy. In our apparatus mass-selection is accomplished via time-of-flight mass spectrometry (TOF-MS), electron energy analysis is achieved with either a magnetic bottle or by velocity mapped imaging. Photodetachment of electrons from anions is implemented via either Nd:YAG or excimer lasers. The photodetachment transition energy, i.e., the EBE, between the ground vibrational and electronic state of an anion and the ground vibrational and electronic state of that anion’s neutral counterpart is the adiabatic electron affinity (EA) of that neutral molecule. Likewise, photodetachment transitions between the ground vibrational and electronic state of an anion and the various electronically-excited states of that anion’s corresponding neutral map the electronic spectrum of that neutral species, i.e., the spectral spacings in the photoelectron spectrum are a mirror image of the neutral’s electronic spectrum. It was, of course, crucial to be able to form the anionic species of interest. There, we had a particularly broad field of anion sources from which to choose. These included several variants of pulsed laser vaporization (LV), laser photoemission, infrared desorption plus photoemission, pulsed arc discharge (PACIS), electrospray ionization (ESI), and Rydberg electron transfer (RET). Each of these anion sources were readily combined with, i.e., connected to, the anion photoelectron spectroscopic portion of our apparatus as described above. Among the sources that utilize lasers, visible light for LV sources as well as IR for desorption sources are provided by Nd:YAG lasers. Ultraviolet photons are provided by both Nd:YAG and excimer lasers, whereas the excitation wavelengths for RET experiments come from two Nd:YAG-pumped dye lasers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Liquid Salt Combined-Cycle Pilot Plant Design

The work described in this report is responsive to the Office of Fossil Energy program ‘Energy Storage for Fossil Power Generation.’ This Phase I report has been prepared by Pintail Power LLC, with support from Nexant ECA, Electric Power Research Institute (EPRI) and Southern Company Services as a deliverable for the U.S. Department of Energy for NETL Award DE-FE-00320016. The Liquid Salt Combined Cycle™ (LSCC™) technology provides large-scale energy storage integrated with Fossil Electric Generating Units (FEGUs) to meet critical needs in the energy transition by providing: • the lowest cost large-scale storage for time-shifting of renewable energy, • superior fuel efficiency to reduce GHGs from dispatchable resources, • flexible capacity and ramping to balance variability of wind and solar resources, • essential grid stability services to assure reliability of a low-carbon grid. The LSCC approach: • employs equipment that has already been proven in utility service, • uses safe, non-toxic, non-degrading, perpetual-life storage medium, • leverages and repurposes existing FEGU assets, • expands the value stack of energy storage to reduce market, financing, and commodity risks. Pintail Power has developed the LSCC technology to meet the need for reliable, efficient, and cost-effective integration of Variable Renewable Energy (VRE) into a low-carbon electric grid by coupling proven thermal energy storage with proven gas turbines, steam turbines, and heat transfer equipment. This novel approach is intended to address the key issues facing the grid and operators of renewable and fossil generating units including: • Overgeneration and curtailment of renewables, • Need for fast ramping dispatchable resources, • Improved efficiency and flexibility of fossil units, • Additional peaking capacity to support electrification of transportation and heating, • Provision of reliability services to support high penetration of VRE, especially synchronous inertia and fast frequency response. A Technology Readiness assessment by EPRI confirmed that LSCC technology consists of commercially proven hardware used in industrial and utility applications. Although the novel LSCC approach has not yet been demonstrated as a complete system, interfaces between major components have been conservatively specified. A Phase III pilot is planned to demonstrate equipment integration and operation. The patented innovation is removal of the evaporator section from the exhaust heat recovery system, with the evaporation performed by stored energy in a separate steam generator. This arrangement couples renewable and fossil power generation via long-duration energy storage to deliver cost, performance, and operational synergies, including superior charging and discharging flexibility, reduced fuel consumption and lower CO 2 emissions compared to conventional Combined Cycle Power Plants, and low-cost, large-scale energy storage. The LSCC technology is composed of proven equipment integrated with gas turbine exhaust heat in a novel system. During charging, electric heaters raise the salt temperature as it flows from the Cold Salt Tank to the Hot Salt Tank. During discharging, hot salt produces steam from feedwater that is heated with gas turbine exhaust, which also superheats steam to drive a steam turbine. LSCC technology can be added to any combustion-turbine to integrate renewable energy, provide needed grid services, and increase the value of fossil electric generating units based on the technology’s following attributes: • Long-duration storage enables time-shifting of VRE to avoid curtailment and impairment of renewable assets. • Long storage duration combined with fast-charging capability increases arbitrage opportunities by storing more energy when the price is low and discharging more hours when the price is high. • Long storage duration allows resource adequacy to be supplied across multiple days to increase reliability and reduce risk. • The stored energy reduces fuel heat rate and GHG emissions, and increases merit, so the LSCC dispatches earlier and longer to increase the plant’s capacity factor and asset value. • The stored energy enables pre-heating and startup of the steam cycle, without operating the gas turbine, to enable fast startup and ramping when dispatched for discharge. • The steam turbine can operate without the gas turbine so it can provide valuable synchronous inertia during charging without consuming fuel. • Fast frequency response and regulation services can be provided during charging using solid-state heater and pump controls to vary the charge power input in response to grid signals. • The LSCC system can be configured for resilience including black start, islanded/micro-grid operation, and even self-recharging of storage using either gas turbine power or gas turbine exhaust heat. The commercialization plan is to add LSCC technology to existing simple cycle gas turbine power plants with the 50MW GE LM6000 aero-derivative gas turbine as the reference design basis. A Techno-economic assessment of the reference design evaluated the benefits (Levelized Avoided Cost of Energy) and costs (Levelized Cost of Energy). The plant definition included all major systems and budgetary vendor quotes. Pintail Power and NexantECA developed the overall cost estimate for the LSCC plant up to the total plant cost level, following the DOE-NETL cost estimate guidelines at AACE Class 3 (-20%/+30%). This includes the equipment cost, bulk material, direct and indirect labor costs to arrive at the bare erected cost. Engineering costs are factored from the BEC and added to it to arrive at the EPC cost. Process and project contingencies were then factored from the EPC cost and rolled-up to yield the total plant cost of $\$$184 million for 1746 MWh of discharge electricity. • At $\$$105/kWh, the reference plant costs less than any of the Energy Storage Systems evaluated by PNNL in 2020 for the Energy Storage Grand Challenge. Operations and Maintenance cost estimates were scaled from combined cycle practice, assuming that the LSCC unit was co-located with and sharing some labor expense with other units, to arrive at $\$$2.2 million per year. Plant economics were evaluated using prices from the ERCOT Day-Ahead Market for calendar year 2019 (excluding the market disruptions from the COVID pandemic and the February 2020 deep freeze event). Assuming economic dispatch in the ERCOT Day-Ahead market, the reference plant capacity factor would have discharged for 2777 hours at 91.9 MW, a 31.66% capacity factor, with a marginal cost of $\$$25.59/MWh, and a LACE of $\$$82.41/MWh. Fixed charges were calculated according to EIA guidelines to arrive at an LCOE of $\$$83.48. The benefit-to-cost ratio of 0.99 suggests that the reference plant would have been cost-effective and competitive in the market. EPRI interviewed selected utilities to gauge the need for, applicability of and interest in the LSCC system. Several utilities are currently managing increased load growth along with the inclusion of increasing levels of renewable generation, putting pressure on conventional generation by requiring increased turndown requirements and ultimately lower capacity factors. All of the utilities interviewed have CO 2 reduction targets in the 2030-2050 timeframe that will severely limit the participation of fossil generation and require better utilization of carbon free generation. While there is limited opportunity for storage in the current markets, the utilities interviewed stated that there will be a substantial need for long duration energy storage in the future given the expected trends. Utilizing an energy storage system will generally be preferred over new gas capacity in some cases, with the capabilities of the LSCC system being a potential option for retrofit to existing simple cycle gas turbine units, allowing them to deliver greater participation in the market with lower carbon intensity. A technology gap assessment and technology maturation plan identified a pilot-scale demonstration as the final step before commercialization. Key gaps to be addressed during the Phase II FEED (Front-End Engineering Design) are component selection and design, commissioning procedures, and operational procedures and the control system for LSCC charging and discharging. The project team has been expanded to include Wood Group PLC as EPC. The proposed Phase II work leads to a pilot-scale engineering demonstration (TRL 6) to be conducted at Southern Company’s Plant Rowan, where the prototype system will perform “all the functions that will be required of the operational system.” The proposed pilot will facilitate commercialization (TRL-9) by scale-up to utility-scale systems integrated with peaking GTs or directly to facility scale systems using industrial GTs. The conceptual design for the pilot plant focuses on the novel integration aspects of LSCC technology. A slipstream of gas turbine exhaust will feed a waste heat recovery unit coupled to a molten salt steam generator heated by stored energy. The pilot is intended to demonstrate all key operating modes of the LSCC technology during charging, discharging and standby. The pilot equipment will be approximately one-seventh scale of the LM6000 commercial target and is expected to have commercial off-ramp potential for facility-scale applications.

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2019

Path Forward for Groundwater Compliance Strategy at the Tuba City, Arizona, Disposal Site - 19581

The Tuba City, Arizona, Disposal Site is located in the Navajo Nation and near the Hopi Reservation. A uranium mill operated at the site from 1956 to 1966. During the operational period, mill tailings were slurried to an unlined impoundment. Excess slurry water was transferred to unlined evaporation ponds. Groundwater contamination resulting from the infiltration of fluids in the mill tailings impoundment and evaporation ponds was characterized in the 1990's. The site's Groundwater Compliance Action Plan was prepared in 1999, and a groundwater extraction and treatment system was constructed in 2002. Issues with aquifer productivity and treatment plant reliability led to the suspension of operations in 2014. The limitations of the remediation system prompted a realization that the site conceptual model should be reevaluated. An integrated study to better understand the geochemical and hydrologic factors affecting contaminant transport, to support the development of a new groundwater compliance strategy, was initiated in 2017 and is ongoing. In addition to the groundwater science components, the study included the evaluation of enhanced evaporation methods. The integrated evaluation will lead to refinement of the site groundwater flow model and development of a contaminant transport model and subsequent development of remedial alternatives. Remedial alternatives will be evaluated to determine a new groundwater compliance strategy. The objectives of geochemical testing were to confirm and quantify geochemical reactions controlling uranium fate and transport. These reactions are important because they control the distribution of uranium on the solid phase; potential for release from the solid phase; mobility of uranium in the water phase; and potential for uranium redistribution onto the currently uncontaminated solid phase. A key outcome is the change in understanding of the mass of uranium in the subsurface that is potentially soluble. These results contradict the previous basis for remediation: that uranium was almost exclusively present in soluble form, within the boundaries of the contaminant plume. Testing showed that uranium sorption downgradient from the plume was measurable but relatively minimal. The movement of other mill-related constituents (nitrate, sulfate, alkalinity) results in the dissolution of naturally occurring uranium and a higher than background concentration of uranium in groundwater. These constituents are not subject to sorption, and their downgradient concentrations are reduced only by diffusion and dispersion. The geochemical testing provides conceptual and quantitative information on potential plume migration. While the testing revealed the potential availability of uranium contaminant sources, the aquifer buffering capacity, pH, and presence of oxygen in groundwater may, individually or in combination, be controlling factors for plume movement. Evaluation of evaporative treatment alternatives was undertaken to determine one or more sustainable and efficient methods capable of treating 151 liters per minute (L/min) (40 gallons per minute), the annual average flow rate. In addition to establishing the baseline capacity for evaporation using the site's existing pond, prospective methods of enhanced evaporation included preheating water before inflow to the evaporation pond, vertical circulation in the pond, dye addition, and Wind-Aided Intensified Evaporation. Consideration of a 151 L/min evaporative treatment arose from previous analysis of extraction well production rates and contaminant mass removal, which indicated that about 80% contaminant removal, relative to full-scale operation of the site's groundwater treatment plant, could be achieved with a smaller capacity system. The lower-flow evaporative option also represented a potentially more sustainable treatment system in comparison to restarting or reconfiguring the groundwater treatment plant. Aquifer pumping tests were designed to develop or improve estimates of hydraulic properties such as transmissivity, horizontal and vertical hydraulic conductivity, storativity, and storage coefficient. Testing involved pumping from one well at a constant flow rate for up to 5 days while monitoring groundwater drawdown in the pumping well and five surrounding wells and then shutting down the pumping well to observe groundwater recovery. The aquifer pumping test results provide insight regarding the hydraulics of the saturated zone. The saturated zone is in a low-conductivity formation with preferential flow in the horizontal direction. The aquifer exhibits low vertical conductance. The use of AQTESOLV software indicates that the saturated zone is a layered system due to the cross-bedded sand-grain orientation within the Navajo Sandstone. These indicators of limited vertical flow provide a potential justification for the observed depth of the contaminant plume of 15-46 meters (50-150 feet) below ground surface). Given the relatively low vertical conductance, groundwater extraction should be focused on the upper portions of the saturated zone. Aquifer response testing provided an improved understanding of aquifer characteristics. However, the primary objective, to identify optimal groundwater extraction strategies, has not been fully addressed. A list of path forward activities for hydrologic analyses was developed, with an overarching objective of providing input parameters for groundwater flow and contaminant transport modeling. Defensible predictions of contaminant transport, through modeling, are critical to the development of a new site groundwater compliance strategy. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗