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1,525 records · Page 85

Biogeochemistry of Pond B (Savannah River Site, South Carolina, USA): Water column and Sediments

Pond B at Savannah River Site (SRS, South Carolina) is a monomictic reservoir that received SRS R reactor cooling water from 1961–1964. Previous studies conducted between the 1980s–1990s on the water column and sediments of Pond B measured trace amounts of Pu (33 MBq 238Pu and 430 MBq 239,240Pu), 241Am, and 137Cs. Since then, the pond has been relatively isolated and the radionuclide concentrations have not been monitored over time. Herein, about 30 years after the last publication on Pond B, we are re-evaluating the geochemistry and radionuclide distribution within Pond B at five locations along a horizontal transect from the inlet to outlet. In addition, we are conducting the first analysis of the microbial community composition. This data package consists of water column measurements (1) using a multi-probe sonde, (2) plutonium isotopes and total concentrations, (3) total organic/inorganic carbon concentrations, (4) trace metals and major ions concentrations, and (6) microbial community composition. Sediment measurements include (1) plutonium isotopes and total concentrations and (2) microbial community composition.For sediment core and porewater, please see other Pond B data package (ess-dive-60d2352a4495472-20200615T203925174).The data in this package will be submitted for peer review in 2023.

54 ENVIRONMENTAL SCIENCES↗

Understanding the interface interaction between U3Si2 fuel and SiC cladding

Abstract Triuranium disilicide (U 3 Si 2 ) fuel with silicon carbide (SiC) composite cladding is being considered as an advanced concept/accident tolerant fuel for light water reactors thus, understanding their chemical compatibility under operational and accident conditions is paramount. Here we provide a comprehensive view of the interaction between U 3 Si 2 and SiC by utilizing density functional theory calculations supported by diffusion couple experiments. From the calculated reaction energies, we demonstrate that triuranium pentasilicide (U 3 Si 5 ), uranium carbide (UC), U 20 Si 16 C 3 , and uranium silicide (USi) phases can form at the interface. A detailed study of U 3 Si 2 and SiC defect formation energies of the equilibrated materials yielding the interfacial phases U 20 Si 16 C 3 , U 3 Si 5 and UC reveal a thermodynamic driving force for generating defects in both fuel and cladding. The absence of either the U 3 Si 2 or SiC phase, however, causes the defect formation energies in the other phase to be positive, removing the driving force for additional interfacial reactions. The diffusion couple experiments confirm the conclusion with demonstrated restricted formation of U 3 Si 5 , UC, and U 20 Si 16 C 3 /USi phases at the interface. The resulting lack of continuous interaction between the U 3 Si 2 and SiC, reflects the diminishing driving force for defect formation, demonstrating the substantial stability of this fuel-cladding system.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Simulations of divertor plasmas with inverse sheaths

The effect of strong electron emission from material surfaces has been proposed to form an “inverse sheath”: a region with a positive potential relative to the near-wall plasma which prevents the flow of ions to the wall [M. D. Campanell, “Negative plasma potential relative to electronemitting surfaces,” Phys. Rev. E. 88, 033103 (2013); M. D. Campanell and M. V. Umansky, “Strongly emitting surfaces unable to float below plasma potential,” Phys. Rev. Lett. 116, 1–5 (2016); M. D. Campanell and G. R. Johnson, “Thermionic cooling of the target plasma to a sub-ev temperature,” Phys. Rev. Lett. 122, 1–5 (2019)]. We assess the viability of this regime in a tokamak device using the 2D edge plasma transport code UEDGE [T. Rognlien et al ., “A fully implicit, time dependent 2-D fluid code for modeling tokamak edge plasmas,” J. Nucl. Mater. 196–198, 347–351 (1992)]. Since the UEDGE code does not consider the sheath region directly, we apply boundary conditions at the divertor targets which emulate the physics of both “standard” and “inverse” sheath regimes [R. Masline et al ., “Influence of the inverse sheath on divertor plasma performance in tokamak edge plasma simulations,” Contrib. Plasma Phys. 60, e201900097 (2020)]. Using these boundary conditions, we perform scoping studies to assess plasma parameters near the target by varying the density at the core-edge interface. We observe a smooth transition in the resultant profiles of plasma parameters for the standard sheath, and a bifurcation across the simulation set for plasmas with an inverse sheath. The cause of this bifurcation is assessed by performing the parameter scan both with and without impurity radiation; we observe that the bifurcation persists in both cases, indicating that this bifurcation is caused by plasma recombination.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Transport and Retention of Particulate Organic Matter in Sand: Lab Experiments and Modelling

Flow-through reactor (FTR) experiments were conducted at three different downward vertical flow rates to study the transport and retention of particulate organic matter (Chlorella powder) in riverbed sediments. This data package includes data files (.csv) regarding effluent collected from the FTRs during the experiments (time, duration, volume of each sample collection; concentration of nonreactive bromide tracer; concentration of suspended Chlorella determined by absorbance measurements) and sediment (sand) slices collected from the FTRs after the experiments (mass of Chlorella retained in 1 cm depth intervals determined by loss-on-ignition method). More detailed descriptions of data are provided in the data dictionary, and detailed methods are available in the associated MSc thesis listed in ‘Related References.’ The data dictionary and file level meta data (FLMD) are included in the data package as both .csv and .xlsx files. This data package also includes timelapse videos (.mp4) of the experiments, and modelling scripts associated with the experiments. The modelling scripts are included as MATLAB ‘live scripts’ (.mlx, which can be run using MATLAB), and are also included as .pdf and .html files with output plots included (which can be viewed without a MATLAB license and installation). The data files and modelling scripts are organized into a .zip folder for each of the three FTR experiments (three flow rates).

54 ENVIRONMENTAL SCIENCES↗

Sludge Removal: Success and Partnership with T Plant - 20510

U.S. DOE contractor CH2M Hill Plateau Remediation Company (CHPRC) has safely and efficiently managed the removal of highly radioactive sludge from the 105-K West Reactor fuel storage basin (105- KW Basin) near the Columbia River. In mid-September 2019, sludge retrieval was completed after 21 storage containers were safely loaded with highly radioactive sludge and transported approximately 13 miles from the 105-KW Basin to T Plant, located in the 200 West Area on the Central Plateau of the Hanford Site. Sludge removal represents the last major source term reduction necessary before the K West Reactor and fuel storage basin can transition to closure activities in preparation for final deactivation and demolition. The technical complexity of the sludge retrieval process, coupled with the challenging physical and radiological characteristics of the waste, necessitated a methodical and deliberate approach using unique design and operational solutions to safely conduct the work. This challenge was further complicated by the need to plan and conduct the work in two separate facilities, each subject to the controls and requirements of its own nuclear facility safety basis. The project overcame these challenges through creating an integrated team that actively engaged, communicated and coordinated each phase of the project to ensure successful completion. This paper will cover how these key elements of the Sludge Removal Project led to its success: - Integrating project planning and management; - Lessons learned from design and construction; - Preparing for a successful campaign (lessons learned from testing and start-up); - Lessons learned from operating in two separate facilities, transporting sludge containers on the Hanford Site and ensuring compliance with a range of regulatory and safety basis requirements. The establishment of an integrated group spanning two facilities and multiple organizations created a team capable of overcoming the challenges necessary to successfully plan and execute the sludge retrieval mission. Sharing lessons learned from this successful project can enhance the ability of teams across the DOE complex to successfully plan and execute complex projects. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

BWR Spent Nuclear Fuel Acquisition and Testing to Support DOE-NE High Burnup Spent Fuel Data Project

The Office of Spent Fuel and Waste Disposition (SFWD) within the US Department of Energy (DOE) Office of Nuclear Energy (NE) established the Spent Fuel and Waste Science and Technology (SFWST) campaign to conduct research and development (R&D) activities related to the storage, transportation, and disposal of spent nuclear fuel (SNF) and high-level radioactive waste. The SFWST program was created within SFWD to address issues of extended or long-term SNF storage and transportation. Some near-term objectives of SFWST are to use a science-based, engineering-driven approach to: Support the enhancement of the technical bases to support the continued safe and secure dry storage of SNF for extended periods; Support the enhancement of the technical bases for retrieving SNF after extended dry storage; Support the enhancement of the technical bases for transporting high burnup (HBU) fuel and transporting low burnup fuel and HBU fuel after dry storage DOE-NE, in partnership with the Electric Power Research Institute, developed the High Burnup Spent Fuel Data Project to perform a large-scale demonstration and laboratory-scale testing of HBU pressurized water reactor (PWR) fuels (exceeding 45 gigawatt-days per metric ton of uranium [GWd/MTU]). Under this project, 25 sister rods—which are rods that have the same design, power histories, and other characteristics—were removed from assemblies at the North Anna Nuclear Power Station and sent to Oak Ridge National Laboratory (ORNL) in January 2016. ORNL performed detailed nondestructive examination (NDE) on all 25 rods. The NDE consisted of visual examinations, gamma and neutron scanning, profilometry and rod length measurements, and eddy current examinations. After completing the NDE, 10 of the sister rods were delivered to Pacific Northwest National Laboratory (PNNL) in a NAC International, Inc. legal-weight truck cask in September 2018 for destructive examination (DE). To date, SFWD work has focused on the PWR fuel that is part of the Sister Rod Test program. No boiling water reactor (BWR) fuel has been tested in the program, and the data needs that were identified for the PWR fuel have not been collected for BWR fuel. The goal to obtain six to nine BWR rods and test them at ORNL will support closing this important data gap. BWR fuel comprises approximately 56% of the total fuel assemblies currently in storage at nuclear power plants in the United States. BWR nuclear fuel and cladding designs and manufacturing are significantly different from PWRs. Differences include the following: BWR fuel pellets are larger than PWR pellets; Variations of Zircaloy-2 (including liners) are used instead of the Zircaloy-4 cladding materials used in PWRs; Clad manufacturing and stress-relief processes are different between PWRs and BWRs; The fuel rod dimensions are different because larger rod diameters and thicker cladding are used in BWRs; BWR fuel typically has lower internal rod pressures and sees vastly different operating conditions than PWR fuel (i.e., two-phase flow); BWR assemblies are “canned,” meaning each assembly is surrounded by a metal fuel channel; BWR cladding is often composed of an inner pure Zr liner that has widely different mechanical properties than the Zircaloy-2 alloy and exhibits a stronger affinity for hydrogen; The BWR SNF generally has more total hydrogen in the cladding/liner than typical PWR fuel; The construction of the PWR and BWR assemblies is vastly different; BWR rods are solidly attached to the assembly nozzles and experience a much different vibration and shock load than PWR rods, which are “floating” within a grid system attached to guide tubes, and the rods sit loosely on the bottom end plates. These numerous differences will affect the way the BWR SNF responds under dry storage preparation processes (e.g., vacuum drying) and during transportation. The results collected in the PWR experimental program must be compared with a subset of similar data collected on BWR SNF to establish a technical basis for whether the larger PWR database is sufficient to bound the BWR SNF end-of-life conditions as is currently assumed for several fuel/clad properties. Changes that occur in both fuel types at HBU could exacerbate any mechanical property differences. As the fuel burnup increases, several changes occur that might affect the performance of the fuel, cladding, and assembly hardware in storage and transportation. These changes include increased cladding corrosion layer thickness, increased cladding hydrogen content, increased cladding creep strains, increased fission gas release, and the formation of the HBU structure at the surface of the fuel pellets. The Nuclear Regulatory Commission (NRC) limits the current maximum rod-averaged burnup to 62 GWd/MTU due to these changes and the lack of data at higher burnups.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Pilot Testing of a Highly Efficient Pre-combustion Sorbent-based Carbon Capture System

TDA developed and demonstrated a highly efficient pre-combustion carbon capture system. The overall objective of this work was to develop a new sorbent-based pre-combustion carbon capture technology for Integrated Gasification Combined Cycle (IGCC) power plants. In this project our goal was to demonstrate the techno-economic viability of the new technology by 1) demonstrating it in large-scale slipstream tests, and 2) carrying out a high fidelity engineering and cost analysis. TDA’s process used an advanced physical adsorbent that selectively removes CO 2 from coal-derived synthesis gas above the dew point of the gas at temperatures as high as 300°C. The sorbent consists of a mesoporous carbon whose surface was grafted with functional groups that remove CO 2 via a well-known acid-base interaction. As documented in bench-scale experiments and field tests with actual coal gas, the sorbent achieved a very high capacity for CO 2 at temperatures as high as 300°C. The sorbent bound CO 2 more strongly than common physical adsorbents, providing the chemical potential needed for the high temperature operation. However, because CO 2 does not form a true covalent bond with the surface sites (as is the case with chemical absorbents), the sorbent regeneration could be carried out with only a very small energy input. The heat input to regenerate our sorbent was only 4.9 kcal per mol of CO 2 , which is much lower than that for chemical absorbents (e.g., 29.9 kcal/mol CO 2 for sodium carbonate) and was similar to the requirements of physical solvents (e.g., 4 kcal/mol CO 2 for Selexol TM ). Because the sorbent operates above the dew point of the synthesis gas (unlike the Selexol TM process), a higher power cycle efficiency can be achieved. With previous DOE/NETL funding (Contract No. DE-FE-0000469), we demonstrated the techno-economic viability of the technology in bench-scale tests and slipstream demonstrations at the National Carbon Capture Center (NCCC), Wilsonville, Alabama and Wabash River IGCC plant in Terra Haute, Indiana. We demonstrated a stable working CO 2 capacity for over 11,650 cycles with simulated synthesis gas. We also evaluated its performance with actual synthesis gas in two test campaigns at the Wabash River IGCC Plant, Terre Haute, IN and the National Carbon Capture Center (NCCC), Wilsonville, AL. The slipstream tests clearly showed that the actual coal gas constituents and potential contaminants (e.g. trace metals, halides, tars) had no effect on the sorbent’s ability to remove CO 2 (the same sorbent beds were used in both field tests with no sign of deactivation for 2,000 cycles with over 26,750 SCF of gas treated). As expected, due to the high temperature CO 2 removal capability and low energy needed to regenerate the sorbent, the power cycle efficiency with our process was greater than 34% on a higher heating value (HHV) basis; in comparison, the same IGCC plant equipped with the Selexol TM solvent for carbon capture can only achieve 31.4% HHV efficiency. The capital cost for an IGCC system with TDA’s process is estimated as $2,417/kW e , which is 12% lower than that of the IGCC/ Selexol TM process. The levelized cost for electricity including the transport, storage and monitoring (TS&M) cost for CO 2 was calculated as $\$ $92.9/MWh (lowest reported to our knowledge), which is much better than the $105.2/MWh estimated for the IGCC/ Selexol TM process. In this project (DE-FE0013105), TDA Research, in collaboration with our partners Gas Technology Institute (GTI), Illinois Clean Coal Institute (ICCI), University of California, Irvine (UCI), University of Alberta (UOA), Siemens, NCCC and Sinopec advanced the technical maturity of the technology; scaling it up by a factor of 100. We optimized the reactor design using computational fluid dynamics (CFD); using adsorption modeling we improved the pressure swing adsorption (PSA) cycle sequence. We carried out two field test campaigns with a fully-equipped 0.1 MW e prototype unit (for a total of 844 hours) using actual synthesis gas to prove the viability of the new technology. A successful 30 day (707 hrs) evaluation was completed at NCCC under air blown gasification conditions. We demonstrated 97.3% carbon capture at 1,500 SLPM, 93% carbon capture at 1,800 SLPM, and 90% carbon capture at 2,100 SLPM in the NCCC tests. We also demonstrated the system for 137 hours at a Sinopec petrochemical plant under oxygen blown gasification, demonstrating 86% carbon capture at 2,660 SLPM. In collaboration with University of California, Irvine (UCI), we completed a techno-economic analysis (TEA) for TDA’s warm gas cleanup technology integrated to IGCC power plant. The net plant efficiencies (on a coal HHV basis) for the warm gas cleanup cases were estimated to be 34.0% for E-GasTM gasifier, 34.4% for GE gasifier, 33.4 for the Shell gasifier and 34.2 for the TRIG TM gasifier (Cases 2, 4, 6 and 8 in this study) with a catalytic combustor for CO 2 purification, which are significantly higher than those for the Cold Gas Case, or an increase of as much as 12% in the heat rate for Case 2, 6% for Case 4, 9% for Case 6, and 9% for Case 8. The 1st year cost of electricity with the transport, storage and monitoring (TS&M) costs for the CO 2 included was $\$ $129.2/MWh for the E-GasTM gasifier Warm Gas Cleanup Case, $\$ $131.9/MWh for the GE gasifier Warm Gas Cleanup Case, $\$ $146.8/MWh for the Shell Gasifier Warm Gas Cleanup Case, and $\$ $129.9/MWh for the TRIG TM gasifier Warm Gas Cleanup Case. For comparison, the costs for the baseline Cold Gas CO 2 removal with Selexol for the different gasifiers were: $\$ $146.6/MWh for the E-Gas TM gasifier, $\$ $142.2/MWh for the GE gasifier, $\$ $159.0/MWh for the Shell gasifier and $\$ $144.3/MWh for the TRIG TM gasifier. In summary, the costs for our system were 7 to 12% lower than the corresponding Cold Gas Cleanup cases. The results of this techno-economic analysis suggested that TDA’s high temperature PSA-based Warm Gas Clean-up Technology can make a substantial improvement in the IGCC plant thermal performance for achieving near zero CO 2 emissions for E-Gas TM , GE, Shell and TRIG TM gasifier based IGCC power plants. The capital expenses were estimated to be lower than that of Selexol’s™. Taken together, the higher net plant efficiency and lower capital and operating costs resulted in substantial reduction in the cost of carbon capture for the IGCC plant equipped with TDA’s high temperature PSA-based carbon capture system. Finally, in collaboration with Gas Technology Institute (GTI) we completed the environmental health and safety assessment for TDA’s warm gas carbon capture technology.

01 COAL, LIGNITE, AND PEAT↗

Optimizing aluminum oxide passivation layers—Laser-induced plasmas for layer formation, real-time diagnostics, and layer evaluation

Molten salts have beneficial thermophysical and electrolytic properties, but the aggressive nature of molten salts requires corrosion mitigation strategies, such as structural material surface treatment. In this study, a laser-induced breakdown spectroscopy (LIBS) system was used to simultaneously ablate and monitor de-excitation spectra to form and identify dense alumina passivation layers. Additionally, high-frequency (kHz) LIBS imaging allowed rapid elemental mapping and depth profiling for surface O/Al ratios via minimally destructive analysis. The paired t-test rejected the null hypothesis that air and Ar cover gases were equivalent (p = 0.00012), and the analysis of variance (ANOVA) showed that overlap between shots (p = 0.03112) and cover gas flow rate (p = 0.02729) were statistically significant. At 75% overlap, the O/Al ratio increased to 10% ± 2%, and 90% overlap rose further to 31% ± 2%. Regardless of overlap, tuning the gas flow from 0.5 to 2.5 L min −1 enhanced the O/Al ratio by 24% ± 4%. LIBS depth profiling showed a 3× increase in layer thickness from 75% to 90% overlap. Molecular band peaks of AlO, a precursor to Al 2 O 3 found during treatment, suggest that band intensity could be used for real-time Al 2 O 3 optimization. Ultimately, by adjusting laser spot overlap and cover gas flow rate, a 266 nm laser was shown to form Al 2 O 3 layers on an Al6061 sample, with cover gas flow rate primarily affecting the O/Al ratio and layer thickness correlating with laser spot overlap. This combination of molecular spectra collection, imaging, and depth profiling demonstrated the robust layer analysis capabilities of LIBS.

Corrosion↗

Modeling Functional Organic Chemistry in Arctic Rivers: An Idealized Siberian System

Rivers of the Arctic will become ever more important for the global climate, since they carry a majority of continental dissolved organic carbon flux into the rapidly changing polar ocean. Aqueous organics comprise a wide array of functional groups, several of which are likely to impact coastal and open water biophysical properties. Light attenuation, interfacial films, aerosol formation, gas release and momentum exchange can all be cited. We performed Lagrangian kinetic modeling for the evolution of riverine organic chemistry as the molecules in question make their way from the highlands to Arctic outlets. Classes as diverse as the proteins, sugars, lipids, re-condensates, humics, bio-tracers and small volatiles are all included. Our reduced framework constitutes an idealized northward flow driving a major hydrological discharge rate and primarily representing the Russian Lena. Mountainous, high solute and tundra sources are all simulated, and they meet up at several points between soil and delta process reactors. Turnover rates are parameterized beginning with extrapolated coastal values imposed along a limited tributary network, with connections between different terrestrial sub-ecologies. Temporal variation of our total dissolved matter most closely resembles the observations when we focus on the restricted removal and low initial carbon loads, suggesting relatively slow transformation along the water course. Thus, channel combinations and mixing must play a dominant role. Nevertheless, microbial and photochemical losses help determine the final concentrations for most species. Chemical evolution is distinct for the various functionalities, with special contributions from pre- and post-reactivity in soil and delta waters. Several functions are combined linearly to represent the collective chromophoric dissolved matter, characterized here by its absorption. Tributaries carry the signature of lignin phenols to segregate tundra versus taiga sources, and special attention is paid to the early then marine behaviors of low molecular weight volatiles. Heteropolycondensates comprise the largest percentage of reactive carbon in our simulations due to recombination/accumulation, and they tend to be preeminent at the mouth. Outlet concentrations of individual structures such as amino acids and absorbers lie above threshold values for biophysical influence, on the monolayer and light attenuation. The extent of coastal spreading is examined through targeted regional box modeling, relying on salinity and color for calibration. In some cases, plumes reach the scale of peripheral arctic seas, and amplification is expected during upcoming decades. Conclusions are mapped from the Lena to other boreal discharges, and future research questions are outlined regarding the bonding type versus mass release as permafrost degrades. Dynamic aqueous organic coupling is recommended for polar system models, from headwaters to coastal diluent.

54 ENVIRONMENTAL SCIENCES↗

Development of an Ultrahigh-bandwidth Phase Contrast Imaging System for detection of electron scale turbulence and Gigahertz Radio-Frequency Waves

The study of waves and turbulence is vital to the development of future reactor-grade plasma devices developed in the quest for fusion energy. These fluctuations are responsible for moving heat and particles across the magnetic field, and a predictive understanding of them is needed to achieve the density and temperature required to sustain a plasma fusion reaction. While many techniques have been developed for measuring waves and fluctuations, every measurement method has limitations. There are relatively few techniques for measuring very high frequency fluctuations, such as radio frequency waves injected to heat the plasma, unstable waves driven by suprathermal particles, or short wavelength electrostatic waves driven by electron temperature or density gradients. The present project builds upon the proven phase contrast imaging (PCI) technique to extend the response of the diagnostic by orders of magnitude in frequency and almost a factor of ten in spatial resolution. PCI provides a measurement of electron density based on small angle scattering of a CO-2 laser beam by using optical techniques to render a phase shift as an intensity change on a detector. Due to the telecommunications revolution, technological development by manufacturers has focused on components in the near -infrared, so that high- quality lasers and detectors at 1.55 µm are readily available. Shifting PCI design to a new, shorter wavelength has numerous advantages and challenges. Similar detector performance is available with room-temperature arrays with GHz bandwidth, while the detector arrays for 10.6 µm required liquid nitrogen cooling and were therefore limited to a bandwidth of about 1 MHz. Shifting to a shorter wavelength reduces the angle at which the laser beam scatters off of plasma waves, allowing more such scattered components to pass through the aperture of the vacuum vessel port and be collected by the PCI, which increases the spatial resolution. Concomitant with these benefits, various questions of performance arise. At shorter laser wave- length, the sensitivity to mirror and lens quality is increased, the contribution of the laser to the overall system noise is increased, and the sensitivity to vibrations is increased. The custom optical components at the heart of the PCI technique were required to be properly scaled for the shorter wavelength, so fabrication technologies needed to be explored. This project was designed to show that a low noise, high response PCI system at 1.55 µm could be constructed and operated, and then to quantify potential issues to allow extrapolation to a full-size production system providing physics measurements on a large plasma device. The first stage, producing the custom optical component called a Phase Plate, was successfully achieved using two methods. First, an easily reproduced masking and coating technique was able to produce good phase plates with the required parameters. Second, a nanofabrication technique was found to produce extremely high quality phase plates at a competitive price. The PCI constructed with the new phase plates and 1.55 µm laser was found to provide excellent wavelength measurements with the theoretically expected response. The sensitivity to optical surface quality was found to be in line with previous measurements at 10.6 µm. The observed signal-to-noise ratio was similar to the theoretically expected value. The effect of vibrations on PCI was studied with the first measurement of the effect of beam motion on PCI response and comparison to theory, allowing for a quantitative prediction of the effect of vibrations on a production PCI system and the requirements for improved beam stabilization. PCI is an extremely cost-effective method to provide a low noise, absolutely calibrated measurement of plasma fluctuations across a wide spatial scale. This project has shown that a 1.55 µm PCI using modern techniques and components is less expensive than the 10.6 µm PCI of a few years ago, with the largest savings in phase plate fabrication and the infrared detector array.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Improved Performance of Cu(InGa)(SeS) 2 PV Modules Using the Reaction of Metal Precursors. Final Report

This project “Improved Performance of Cu(InGa)(SeS) 2 PV Modules using the Reaction of Metal Precursors” was a partnership led by the Institute of Energy Conversion (IEC) at the University of Delaware with Columbia University and the Molecular Foundry at the Lawrence Berkeley National Laboratory. The aim was to develop pathways to improve Cu(InGa)(SeS) 2 (CIGSS) thin film photovoltaic modules using processes compatible with low manufacturing cost. The CIGSS approach investigated was a two-step process including deposition of metal precursor films following by reaction in hydride gases utilizing IEC’s novel reactor. The process was similar to that under commercial development by the project’s industry partner Stion. When Stion went out of business mid-project the focus changed to a rapid thermal process considered more commercially viable. Approaches to improve the performance of solar cells using the reacted films focused on two material innovations. First, the overall Ga content was increased to increase the operating voltage, which is desirable for scale-up to commercial modules. Second, the processing and performance advantages arising from Ag alloying were investigated. Advanced characterization guided process and material development including control of relative composition gradients. Research on the formation of Cu-Ga-In metal precursors utilized sputtering deposition which is normally used in commercial applications. The work resulted in processes for deposition of precursor stacks with increased relative Ga content and effects of deposition parameters on morphology and phase composition were established. It was shown that the metal precursor films have comparable phase composition and morphology so subsequent reaction follows from the same starting point. The addition of Ag to the metal precursors gave more uniform morphology and improved adhesion of reacted films which enable higher reaction temperature for faster processing. A novel outcome was the discovery of a previously undocumented material phase in sputter-deposited and evaporated Ag-Cu-In-Ga thin films. Hydride gas reaction processes including time-temperature-concentration profiles were developed for different precursor compositions. This enables control of composition profiles to engineer through-film gradients for solar cell optimization with characterization and simulations used to correlate measured film composition profiles to measurements of devices. In particular, the gradient of sulfur at the front of the CIGSS film was found to be critical. The simulations guided process development leading to improved reproducibility of devices improved performance with higher Ga content and higher voltage. With Ag-alloyed precursors, the reaction pathways leading were determined. A significant finding was that Ag-alloying increases the reaction rate to completely convert precursor films to the final chalcopyrite which could enable reduced reaction time to benefit manufacturability. To maintain potential commercial viability, the process under investigation was refocused to a rapid thermal process that could potentially be incorporated into an in-line process for manufacturing. Precursors with different composition were capped with an extra selenium layer and reacted in hydrogen sulfide 5-15 minutes, compared to typically 2 hours in the previous multi-step batch process. Critical RTP parameters were identified to control the reaction. Further optimization would be needed for high efficiency solar cells but pathways to high quality devices with further optimization and improved heating uniformity were developed. The project also developed new optoelectronic characterization approaches with a focus on development and application of spatial- and time-resolved photoluminescence and a custom mapping photoluminescence microscope built. It was shown how critical electronic transport properties strongly depend on the chemical composition of the material and that a wide range of samples show inhomogeneity on a length scale larger than the grains in the films. Additionally, two-photon excitation capability was developed to distinguish bulk vs surface losses. The project advances the state-of-the -art for precursor reaction processes in several ways that could impact manufacturing. This includes validation of approaches to increase voltage and establishment of model-guided control to form optimal composition profiles. The application of process control approaches with knowledge of phase formation and reaction pathways can be critically valuable in designing a large-scale process.

14 SOLAR ENERGY↗

Life cycle Management of 324 Project High-Activity, Mixed/Low-Level Radioactive Waste - 20506

U.S. DOE contractor CH2M Hill Plateau Remediation Company (CHPRC) manages the 324 Building and is preparing to remotely excavate and disposition the radioactive soil beneath the building to allow further deactivation of the building. The 324 Building is a non-reactor Category 2 Nuclear Facility located in the 300 Area of the Hanford Site. Records indicate that in October 1986, approximately 516 liters of a concentrated liquid waste stream containing cesium-137 ({sup 137}Cs) and strontium-90 ({sup 90}Sr) spilled onto the floor of a hot cell, B-Cell, in the 324 Building. The spill contained an estimated 1.3 million curies (Ci) of radioactivity. A breach in the sump of B-Cell was discovered in November 2009 during characterization of the soil under the building. Exposure rates in excess of 10,000 R/hr were detected through a system of access pipes installed under the hot cell, and an estimated 1.557 E+05 Ci of {sup 137}Cs and 6.842 E+04 Ci of {sup 90}Sr are in the soil beneath B-Cell. The magnitude of the soil contamination below B-Cell represents one of the most challenging remediation activities in the DOE complex. The objective of CHPRC's 324 Project is to remotely excavate and disposition the highly contaminated soil under the hot cell so building deactivation and stabilization activities can resume. Depending on the volume and radioactivity of contaminated soil under B-Cell, the material will be dispositioned either at the Hanford Site's Environmental Restoration Disposal Facility (ERDF) or in grout monoliths that will be created in the hot cells (A, C and D) next to B-Cell during future building demolition activities. The current project scope includes installing structural supports under the walls of B-Cell and using remotely operated equipment to remove debris from the hot cell, remove debris mixed with grout on the floor, saw through and remove the cell floor and liner, and excavate contaminated soil under B-Cell to a depth of up to 3.66 meters (12 feet). Addition or removal of debris in A-Cell may be required to support B-Cell cleanout and excavation activities. The base approach is to disposition debris and soil bins in the Radiochemical Engineering Cell (REC) monoliths, and subsequently disposition the monoliths during building demolition. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Progress on Computational Modeling of Water-Based NSTF (FY2021)

This report documents the FY21 progress and achievements made in the computational analyses of the water-based NSTF. Both system-level and high-fidelity Computational Fluid Dynamics (CFD) analyses were performed to gain a complete understanding of the complex flow and heat transfer phenomena in natural convection systems. The progress on the waterbased NSTF experimental testing is summarized in a companion report (ANL-ART-230). As a continuation of progress from previous years, in FY21 the RELAP5 model of the NSTF was first updated to include a representative heated cavity that incorporated convection and conduction means of heat transfer. Two different cavity models were developed, one that models the radiation heat exchange among all surfaces in one enclosure (Cavity Model 1), and another that employs multiple radiation enclosures with each considering the surfaces at one axial level (Cavity Model 2). This updated RELAP5 deck was benchmarked with single-phase test data to tune form loss coefficients of the elbows and tees, along with heat transfer coefficients within the cavity and off the external insulation panels. This tuned model was then found to accurately predict fluid temperatures within 2.5% and both system and riser flow rates within 6% during single-phase, steady-state simulations. For transient simulations, there is a slight over prediction of the flow rate, fluid temperatures, and heater temperatures during the heat-up period, which indicate that the transient heat loss may be underestimated. Following, the capabilities of RELAP5-3D were examined, which feature a conduction enclosure model that is not present in the current version of RELAP5-MOD3.3 used for all previous NSTF simulations. As an initial comparison of the two codes, single-phase simulations were run that used similar input decks. The results indicate that the single-phase flow predicted by the two codes was very similar, however RELAP5-3D appears to predict a higher system flow during the two-phase transient when compared to the flow rates predicted by RELAP5-MOD3.3. Furthermore, RELAP5-3D run did not capture the density wave oscillations or geysering phenomena, which are large oscillation flow instabilities observed in the experimental facility. To further the prediction capabilities for capturing two-phase instabilities, Options 55, 57, 58, 61, which are implemented by default in RELAP5-MOD3.3 but not in RELAP5-3D, were investigated. When enabling Option 61, RELAP5-3D agrees well with MOD3.3 in predicting the total system flow, while other options have negligible effect on the predicted total system flow by RELAP5-3D. However, none of these options enables RELAP5-3D to produce the same flow instabilities. For future steps, efforts are currently underway to investigate RELAP5-3D’s different behavior in predicting low-pressure two-phase instabilities. STAR-CCM+ was used to perform CFD analysis of the water-based test facility and provide simulation results for comparisons to experimental data. Efforts first focused on describing the characteristics of flow within the heated cavity. A study was performed on whether possible leakage flow between the two sides of the cavity could substantially impact and explain the results. An additional second assumption was examined which defined adiabatic side walls, so physical insulation structures were added to the models to allow conduction across this outer insulation. The results suggest that potential porosity of the insulation could be a major factor in the temperature distribution within the cavity and should be considered in any studies where it is desirable to know the cavity wall temperatures to higher accuracy.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗