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At least 73 records · Page 4

Online Alpha Monitoring of High Cs-137 Hanford and SRS High Level Waste with Tensioned Metastable Fluid Detectors

The Department of Energy’s Hanford and Savannah River Sites maintain millions of gallons of caustic supernate and salt high activity waste in their high-level waste (HLW) tank farm inventories. The Savannah River Site is currently treating this waste with a calixarene-based solvent extraction of Cs-137 to reduce these inventories. Hanford is employing an at-tank crystalline silico titanate (CST) based solid phase extraction methodology to reduce their liquid HLW inventories. Due to the high solubility of Cs-137 and the relative insolubility of the actinides in these caustic waste forms, the beta to alpha radioactivity ratio can often exceed six orders of magnitude in the feed solutions to these treatment processes. This unique characteristic leads to significant technical challenges in making rapid gross alpha measurements in the presence of the overwhelming beta, gamma, as well as dissolved sodium salt in these HLW matrices. Conventional radioanalytical techniques, such as liquid scintillation analysis or gas flow proportional counting require significant radiochemistry preparation prior to the radiometric measurements for gross alpha activity. These required pretreatments render these technologies untenable for rapid quantification of gross alpha activity that could be required to support on or at-line measurements ensuring a waste stream will meet regulatory requirements. The radiation measurement properties of Tensioned Metastable Fluid Detectors (TMFDs) have been studied by Purdue University’s Taleyarkhan research group for well over a decade. Fluids tensioned to the appropriate degree will rupture when struck by radiation, resulting in a measurable cavitation event. The negative pressure generating this tension can be adjusted by centrifugal rotation or by acoustic means in such a way that these cavitation events can be generated from alpha radiation but will not be generated by beta or gamma radiation. Purdue University and the Savannah River National Laboratory are currently collaborating to develop a gamma/beta blind, spectroscopic alpha measurement system based on the Tensioned Metastable Fluid Detector technology to provide a potential solution for performing rapid gross alpha measurements on these high gamma/beta sample matrices. Measurements using the Indirect Drive Acoustically Tensioned Metastable Fluid Detectors developed as part of this collaboration were performed with an alpha emitting radionuclide. Successful determination of gross alpha activity was observed, indicating a potential pathway for rapid gross alpha measurements in remote-handled shielded cells or in process situations requiring online alpha monitoring. Measurements using this system have been conducted on high beta activity solutions, demonstrating the beta blind capability of this system. Measurements are currently underway to test the system’s capability to measure gross alpha activity on Savannah River Site high level waste high Cs-137 samples that have been measured by the SRNL radiochemistry team. This work was supported by the DOE EM Technology Development program.

DiPrete, David [Savannah River National Laboratory↗

Radiological Impact of 2023 Operations at the Savannah River Site

This report presents the environmental dose assessment methods and the estimated potential doses to the public from 2023 Savannah River Site (SRS) air and liquid radioactive releases. Also documented are potential doses from special-case exposure scenarios, such as the consumption of wildlife or goat milk. Dose to the Offsite Representative Person The 2023 dose to the offsite representative person from SRS liquid releases was 0.14 mrem and from SRS air releases it was 0.016 mrem. To show compliance with the U. S. Department of Energy (DOE) all pathway dose standard of 100 mrem/yr, SRS conservatively adds these two doses for a total representative person dose of 0.16 mrem which is 0.16% of the DOE standard. Sportsman Doses Onsite Hunter: SRS conducts annual hunts to control onsite deer and feral hog populations. The estimated dose from consuming harvested deer or hog meat is determined for every onsite hunter. During 2023, the maximum potential dose an onsite hunter received was 9.42 mrem, or 9.42% of DOE’s 100 mrem/yr all pathway dose standard. Creek Mouth Fisherman: SRS estimated the maximum potential dose from fish consumption at 0.17 mrem from bass collected at the mouth of Lower Three Runs. This dose is 0.17% of the DOE standard. SRS bases this hypothetical dose on the low probability scenario that, during 2023, a fisherman consumed 24 kg (53 lbs) of bass caught exclusively from the mouth of Lower Three Runs. Release of Material Containing Residual Radioactivity SRS did not release any real property (land or buildings) in 2023. SRS unconditionally released a total of 13,324 items of personal property (such as tools) from radiological areas in 2023. Most of these items did not leave the Site. However, all of these items required no additional radiological controls post-survey as they met DOE Order 458.1 release criteria. Radiation Dose to Aquatic and Terrestrial Biota SRS conducts screening evaluations of plant and animal doses for aquatic and terrestrial ecosystems. For 2023, all SRS aquatic system locations passed the initial (Level 1) screenings and no further assessments were required at those locations. For the land-based systems evaluation, SRS performed initial screenings using concentration data from the five onsite radiological soil sampling locations. Typically, SRS collects and analyzes only one soil sample per year from each location. For 2023, all land-based locations passed their initial (Level 1) pathway screenings.

54 ENVIRONMENTAL SCIENCES↗

Direct evidence of the effect of a moderate external magnetic field on stimulated Raman scattering in the kinetic regime

We present results from an experiment carried out at the OMEGA-EP laser facility that investigated the effect of a perpendicular magnetic field on stimulated Raman scattering (SRS) and report the first direct measurement of magnetic mitigation of SRS. A 13-T magnetic field generated by pulsed-power coils was imposed on a gas jet plasma, and a novel three-picket interaction beam was used to explore SRS reflectivity for several plasma conditions within single shots. The time-resolved backscattered light shows that SRS was mitigated by the external 13-T magnetic field in the kinetic regime (kλ D ∼ 0.3, where k is the electron plasma wave's wavenumber and λ D is electron Debye length) and at a density of n e /n cr ∼ 0.10. On the other hand, we also measured an enhancement of SRS reflectivity at lower density (n e /n cr < 0.08). We discuss experimental results in the context of magnetohydrodynamic and particle-in-cell simulations that scan SRS dynamics for a variety of plasma conditions. While the experimental evidence of SRS mitigation validates prior work on the kinetic simulation of SRS in an external magnetic field, we also find that other mechanisms such as SRS rescatter can lead to an enhancement of measured SRS reflectivity in simulations of parameters relevant to our experiment.

Gas jet↗

FY2020 Savannah River Site Composite Analysis Annual Summary Review

This document provides the Department of Energy (DOE) Order 435.1 and its manual, Radioactive Waste Management (DOE 2021a, 2021b) required Annual Review for the Savannah River Site (SRS) Composite Analysis (CA). Progress made to-date toward addressing the secondary issue from the LFRG review of the 2010 SRS CA has focused primarily upon inventory estimate improvements. Inventory impacts dose in a linear fashion and reduces the uncertainty with the CA conclusions. Maintenance items are addressed, as funding allows, based on the relative risk associated with meeting the performance objectives. Currently, there is minimal risk in exceeding the DOE 100 mrem/yr CA primary dose limit or the DOE 30 mrem/yr dose constraint (administrative limit). Proposed activities, discoveries, new information and changes potentially affecting the 2010 SRS CA are documented in this and earlier Annual Summary reports, and a consolidated list of changes since the 2010 CA is documented in this report. The impact to the CA of changes arising from updated performance assessment (PA) baselines [i.e., Saltstone Disposal Facility (SDF), E-Area Low-Level Waste Facility (ELLWF), and F & H Tank Farm (FTF & HTF) closures] is expected to be minor for the following reasons: The primary contributors to the SRS CA dose impact at the Upper Three Runs (UTR) point of assessment (POA) are the H-Canyon and Mixed Waste Management Facility (MWMF), contributing 68% and 9%, respectively, to the dose impact at that POA. The combined contribution to the UTR dose impact from all PA’s (SDF, ELLWF, FTF and HTF) is ~2% of this total. The 2010 SRS CA model validation performed indicates that the CA projected dose, while generally conservative, provides a reasonable representation of the maximum annual doses. Doses evaluated are well below the SRS established 15 mrem/yr administrative limit (Crapse et al. 2011). Based on the assessment presented within this annual review and collective engineering judgement, the conclusions of the 2010 SRS CA remain valid and there is reasonable assurance that SRS will meet the performance objectives delineated in DOE Manual 435.1-1. The 2010 SRS CA should be updated to incorporate PA changes, proposed changes to inventories and sources and model improvements accumulated since the 2010 CA. The timing will be dependent on the completion of the ongoing E-Area PA revision.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Determining Cs-137 Background body burdens for Wild Pigs At Savannah River Site

Savannah River Site (SRS) is a unique U.S. Department of Energy facility in that most of the 310-square miles of land has not be industrialized since operations began in 1953. This has allowed abundant, undisturbed vegetation structure to exists as well as an increase in herd sizes among wildlife populations onsite. Cs-137 is widespread across SRS due to the production of nuclear materials, but is mostly from global atmospheric fallout from nuclear weapons testing. Due to most of SRS being undisturbed land, the concentrations of Cs-137 are higher on site than off site. The SRS began conducting annual deer harvests that were open to the public beginning in 1965. All animals harvested during these hunts are monitored for Cs-137, which is measured using a Sodium Iodide detector. There has been an effective method for calculating the background Cs-137 body burden for the deer population at the SRS, developed by Gaines and Novak using data collected during hunts and gamma overflight data to determine the areas contaminated by site activities. For animals that have a Cs-137 concentration above the established background level, a dose is assigned to the hunter. By applying the same method for wild pigs using data collected from hunts, gamma overflight, and developing a site-specific home range of wild pigs, we were able to calculate the Cs-137 background body burden concentrations of wild pigs on site. Objectives: Develop site-specific home range for wild pigs at SRS; Determine the average concentrations of Cs-137 in wild pigs from background; Use Gaines and Novak method for determining background Cs-137 body burdens wild pigs on SRS. Methods and Materials: Development of site-specific home range of wild pigs was determined to be 2.5 miles using: Four studies conducted between 1969 and 1992 for the SRS wild pig population. (Mayer and Brisbin) The background compartments were determined using: Gamma overflight data showing contaminated areas; Site-specific home range of the wild pigs. Results and Conclusion: All data were generated through the JMP software to provide a histogram and summary statistics. The estimate of an upper tolerance limit for the background contamination with 95% confidence is 1.965 pCi/g for the wild pigs. This means that for wild pigs on SRS from the background compartments are expected to have Cs-137 concentrations of less than 1.965 pCi/g. The current background for the deer is 2.59 pCi/g. For the background compartments Cs-137 concentrations from 2012-2018: Mean: 0.815 pCi/g, Maximum: 2.341 pCi/g, Minimum: -0.704 pCi/g.

07 ISOTOPE AND RADIATION SOURCES↗

Controlled Pyroshock Transients Can Be Used To Better Match Operational Shock Transients and Improve Shock Analysis and Testing

SRS analysis and testing to SRS is known to be conservative since SRS is generated from maxi-max shock transient data, maximum peaks are assumed to occur for each mode simultaneously, and the structural dynamics are not accounted for between the shock source and the test article. Knowing the structural dynamics of a shock test setup it is possible to subscribe a force shock transient applied at a particular strike location and direction to achieve a desired shock transient at a test reference accelerometer. The SRS at this test accelerometer reference location can be used to compare to the reference SRS, but the key reference is the shock transient not the SRS, which should lead to more realistic shock testing that better matches operational shock transient data and reduces artificial test failures that don’t occur in operational usage. The desired test shock transient should match operational shock transients. As such, the test shock transient should look similar to the operational shock transient and have similar positive and negative peaks, the same shape, and the same duration. Many shock transients can be created that satisfy an SRS, but better control of these shock transient parameters is needed to better match operational shock transients so that more realistic and less conservative shock testing can be performed. Three different shock transients are presented that satisfy a given SRS and the results are compared for an electronic board (test article) attached to a circular shock resonance test plate.

SRS, shock transient, frequency domain, FRF↗

Estimating Shock Spectra: Extensions beyond GEVS

Shock response spectra (SRS) are the standard description of some vibration environments on spacecraft for equipment qualification. For shock events produced by pyrotechnic devices, SRS can have significant frequency content as high as 10 kHz. It is difficult to construct and analyze finite element models that can resolve dynamic behavior at such high frequencies. GEVS provides simple, empirically based methods for approximating the SRS for a wide variety of shock events. It begins with a base SRS according to the type of pyrotechnic device, and then provides attenuation relations to adjust this SRS according to distance from the shock source, the type of structural frame and the properties of any structural joints between the source and equipment. In our paper we extend GEVS to include more detailed information about the spacecraft structure. To retain the general framework of GEVS, we begin with a base SRS and adjust this SRS using attenuation relations. We use modal and traveling wave concepts to derive the attenuation relations for simple canonical structures. Then we show how these concepts can be used to analyze more complex structures using finite element mode shapes to explicitly calculate the attenuation factors. Since the low- to mid-frequency finite element modal information is extrapolated to obtain the low- to high-frequency attenuation relations, the resulting attenuated SRS is formulated as an upper bound rather than as mean predicted values. We illustrate the extended GEVS approach by analyzing the impact response of composite tubes and the shock response of the STEREO spacecraft.

Igusa, Takeru↗

Probabilistic Assessment of Damage from Same Shock Response Spectra due to Variations in Damping

Interpretation of field data from shock tests and subsequent assessment of product safety margins via laboratory testing are based on the shock response spectra (SRS). The SRS capture how a single degree of freedom (SDOF) structure responds to the shock at differing frequencies and, therefore, no longer contain the duration or other temporal parameters pertaining to the shock. A single duration can often be included in the technical specification or in the recreation of acceleration vs. time history from the specified SRS; however, there is little basis for that beyond technical judgment. The loss of such temporal information can result in the recreated SRS being the same while its effect on a system or component can be different. This paper attempts to quantify this deficiency as well as propose a simple method of capturing damping from shock waves that can allow the original waveform to be more accurately reconstructed from the SRS. In this study the decay rate associated with various frequencies that comprise the overall shock was varied. This variation in the decay rate leads to a variation in the acceleration vs. time history, which can be correlated to a “Damage Index” that captures the fatigue damage imparted to the object under shock. Several waveforms that have the same SRS but varying rates of decay for either high- or low-frequency components of the shock were investigated. The resulting variation in stress cycles and Damage Index is discussed in the context of the lognormal distribution of fatigue failure data. It is proposed that, along with the SRS, the decay rate is also captured to minimize the discrepancy between field data and representative laboratory tests.

36 MATERIALS SCIENCE↗

Probabilistic Hazard Assessment for Tornadoes, Straight-Line Wind, and Extreme Precipitation at the Savannah River Site

Recent data sets for three meteorological phenomena with the potential to inflict damage on SRS facilities – tornadoes, straight-line winds, and heavy precipitation – are analyzed using appropriate statistical techniques to estimate the occurrence probabilities for these events in the future. Summaries of the results for DOE-mandated return periods and comparisons to similar calculations performed in 2013 by Werth et al. (W2013) are given. Using tornado statistics for i) the combined states of Georgia and South Carolina, and ii) a 2⁰ square area surrounding SRS, we calculated the probability per year of any location at SRS being struck by a tornado (the ‘strike’ probability) and the probability that any point will experience winds above set thresholds. The strike probability was calculated to be 7.04E-4 (1 chance in 1420) per year and tornadic wind speeds for DOE mandated return periods of 50,000 years (corresponding to wind design category 3 (WDC-3), and 125,000 years (meeting WDC-4) (USDOE, 2016) were estimated to be 132 mph and 147 mph, respectively. By contrast, default tornado wind speeds taken from ANSI/ANS-2.3-2011 are somewhat higher: 161 mph for return periods of 50,000 years and 173 mph every 125,000 years (ANS, 2011). Although the ANS and the SRS evaluation used the same basic model (Ramsdell and Rishel, 2007), the region defined in ANS 2.3 that encompasses the SRS also includes areas of the Great Plains and lower Midwest, regions with much higher occurrence frequencies of strong tornadoes. The SRS straight-line wind values associated with various return periods were calculated by fitting existing wind data to a GEV1 distribution and extrapolating the values for any return period from the tail of that function. For the DOE mandated return periods, we expect straight-line winds of 117 mph every 2500 years (the required WDC-3 standard) and 125 mph every 6250 years (WDC-4) at any point within the SRS. These values are similar to those from the ANS-2.3-2011 report, which has wind speeds of 125mph and 133 mph for return periods of 2500 years and 6250 years, respectively. For extreme precipitation, we compared the fits of two different theoretical extreme-value distributions and applied the one that fit the data best for each of several accumulation periods. The DOE mandated 6-hr accumulated rainfall for return periods of 10,000 years (corresponding to precipitation design category 3 (PDC-3) and 25,000 years (PDC-4) were estimated as 9.1 inches and 10.1 inches, respectively. For the 24-hr rainfall return periods of 10,000 years and 25,000 years, total rainfall estimates were 12.02 inches and 13.17 inches, respectively, higher than comparable values provided in the W2013 report.

54 ENVIRONMENTAL SCIENCES↗

Effects of variables upon pyrotechnically induced shock response spectra

Throughout the aerospace industry, large variations of 50 percent (6 dB) or more are continually noted for linear shaped charge (LSC) generated shock response spectra (SRS) from flight data (from the exact same location on different flights) and from plate tests (side by side measurements on the same test). A research program was developed to investigate causes of these large SRS variations. A series of ball drop calibration tests to verify calibration of accelerometers and a series of plate tests to investigate charge and assembly variables were performed. The resulting data were analyzed to determine if and to what degree manufacturing and assembly variables, distance from the shock source, data acquisition instrumentation, and shock energy propagation affect the SRS. LSC variables consisted of coreload, standoff, and apex angle. The assembly variable was the torque on the LSC holder. Other variables were distance from source of accelerometers, accelerometer mounting methods, and joint effects. Results indicated that LSC variables did not affect SRS as long as the plate was severed. Accelerometers mounted on mounting blocks showed significantly lower levels above 5000 Hz. Lap joints did not affect SRS levels. The test plate was mounted in an almost free-free state; therefore, distance from the source did not affect the SRS. Several varieties and brands of accelerometers were used, and all but one demonstrated very large variations in SRS.

Smith, J. L.↗

Panel Session 34: US DOE Featured Site: Savannah River Operations Office: 70 Years of Service

The Savannah River Site celebrates its 70. anniversary on November 28, 2020. On this date in 1950, President Harry S. Truman requested the Dupont Company to design, build and operate what was then known as the Savannah River Plant in response to the Soviet Union's detonation of its first atomic weapon, which set the Cold War into motion. During the 1950's, six South Carolina towns were relocated for the construction of SRS and by 1953, the 310 square mile site was complete. Nearly 40,000 workers were employed t build five nuclear reactors and support facilities, two chemical separations plants, heavy water extraction plant, nuclear fuel and target fabrication facility tritium extraction facility and waste management facilities. SRS played a key role in winning the Cold War and for seven decades, SRS has been a leader within the DOE complex. Today, the site supports environmental stewardship and maintains the nation's nuclear deterrent while ensuring the safekeeping and disposal of domestic and international nuclear materials. The site continues to support the nation's nuclear defense as it explores new potential NNSA missions. SRS has a proud 70- year history and looks forward to a future of service as a national asset and strong community partner. The session was kicked off with a video message from Secretary of Energy, Dan Brouillette, who thanked employees past and current for their efforts. The video also provided an overview of the history and future of the Site. This panel provided an overview of the Savannah River Site's 70 years of service (history, challenges, opportunities, and future) presented by the SRS's Senior leadership and the local Aiken, South Carolina Mayor. Panelists with presentations: US DOE Secretary Dan Brouillette's Overview of DOE and SRS - A Legacy of 70 Years of Service (Amy Boyette); 70 Years of Service (Michael Budney); 70 Years of Service (Stuart MacVean); SRS Liquid Waste (Thomas Foster); National Nuclear Security Administration (Nicole Nelson-Jean)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Label-free nanoscopy of cell metabolism by ultrasensitive reweighted visible stimulated Raman scattering

Nanoscopic imaging of cell metabolism is hindered by the incompatibility of small metabolites with fluorescent dyes and the limited resolution of imaging mass spectrometry. We present ultrasensitive reweighted visible stimulated Raman scattering (URV-SRS), a label-free vibrational nanoscopy technique that enables multiplexed detection of metabolic nanostructures within cells. We developed an extensively chirped spectral focusing visible SRS microscope that achieves a detection limit of 4,000 molecules and introduced a self-supervised learning-based denoiser to robustly suppress non-independent SRS noise by over 7.2 dB. The instrumentation-based signal enhancement and computation-based noise suppression synergistically improved the detection sensitivity by 50 times over near-infrared SRS. Leveraging this enhanced sensitivity, we further pushed the resolution to nanoscopic levels by introducing Fourier reweighting to amplify sub-100 nm spatial frequencies previously overwhelmed by noise. Validated by Fourier ring correlation, URV-SRS achieves a lateral resolution of 86 nm in cellular imaging. Here, we applied URV-SRS to elucidate the reprogramming of metabolic nanostructures associated with virus replication in Vero E6 host cells and to compositionally delineate subcellular fatty acid synthesis in engineered Escherichia coli, demonstrating its capability towards nanoscopic spatial metabolomics.

59 BASIC BIOLOGICAL SCIENCES↗

Identification of stimulated Raman side scattering in near-spherical coronal plasmas on OMEGA EP

Recent spherical-target laser–plasma interaction experiments, performed on the OMEGA EP laser, have been analyzed for stimulated Raman scattering (SRS). This has been motivated by results obtained on the National Ignition Facility (NIF) that have demonstrated the importance of SRS, and in particular SRS side scatter, for directly driven inertial confinement fusion (ICF) conditions [Rosenberg et al. Phys. Rev. Lett. 120, 055001 (2018); Michel et al. Phys. Rev. E 99, 033203 (2019)]. The analysis, based on a generalized ray tracing approach, is described and is shown to explain the observed scattered light spectra: it identifies SRS convective scattering, from portions of each incident beam where the scattered electromagnetic wave is generated in the direction parallel to contours of constant density, as the dominant contribution. This result is novel, as SRS is mostly associated with plasmas of higher electron temperature (T e ≳ 3–4 keV) and longer density scale length (≳600 μ m) than those considered here (T e ~ 1–3 keV, Ln~150 μm) for the relevant overlapped irradiation intensities l ≲ 10 15 W/cm 2 . Furthermore, a combination of the high single-beam intensity on OMEGA EP and the side-scattering geometry, that has been identified, is responsible for this result. It is further suggested that the OMEGA EP platform could provide a good surrogate in which to develop SRS mitigation strategies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Nonlinear models for coupling the effects of stimulated Raman scattering to inertial confinement fusion codes

Laser plasma instabilities (LPI) reduce driver-target coupling, alter implosion symmetry, and therefore can fundamentally limit fusion performance in inertial confinement fusion (ICF). Developing a predictive modeling capability for LPI effects can critically advance the success of the field. We perform vector particle-in-cell simulations of multi-speckled laser beams undergoing stimulated Raman scattering (SRS) at various densities and intensities relevant to mainly indirectly driven and a subset of parameter space for directly driven ICF systems, focusing on the regimes with intensities above the onset of electron trapping. Based on the wavenumber of the SRS daughter electron plasma wave, we identify several regions with underpinning SRS saturation physics: the electron-trapping dominated region with intermediate kλD values, the strong Landau damping region at larger kλD values, and the region where the Langmuir decay instability arises at lower kλD values. We develop a nonlinear SRS reflectivity model that features the base trapping-dominated scaling of (kλD)−4 and its modifications. Electron trapping deforms the initialized electron distribution functions, and we have developed a new δf-Gaussian-mixture algorithm for an accurate characterization of the trapped hot electron population. With this SRS hot electron description, we construct a nonlinear energy deposition model and a hot electron source model—based on a modified Manley–Rowe relation—suitable for including SRS effects as a sub-grid module in a high-fidelity ICF design code.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Assessment of Methane Generation from the Thermolysis of Organics in Caustic Waste

Methane generation has been detected during thermolytic Hydrogen Generation Rate (HGR) testing of SRS tank waste and in simulant samples. Simulant testing has shown methane generation in the presence of trimethylsilanol (TMS) and radioactive sample testing has shown methane generation in presence of methylmercury, both of which are found within SRS waste tanks. The 2019 report Evaluation of the Current State of Knowledge for Thermolysis of Organics within SRS Waste Forming Volatile Organic Compounds (VOCs) reviewed historical data and assessed literature pertaining to thermolytic methane generation. That review recommended undertaking thermolysis studies on simulated waste to detect and quantify VOCs. The purpose of this assessment is to review chemistry and current knowledge of organics in SRS waste to recommend which organics in SRS waste tanks, if any, should be tested for thermolytic methane generation. An evaluation of observed methane generation rates has been performed to assess the implication for current CSTF controls. Based on the inputs used in this report, it was concluded that no methane generation data observed to date has challenged the existing 5% organic contribution to the Composite Lower Flammability Limit (CLFL) assumption in the CSTF tank farm at temperatures below 100 °C. Evidence shows that thermolytic pathways to methane generation become significant at temperatures >100 °C in caustic waste. Currently, the influences of thermolytic methane production on the flammability of vessels at >100 °C (e.g., evaporators) is unclear. It is recommended that testing should be undertaken using the HGR experimental approach for methane generation. The initial simulant testing should obtain quantitative methane generation rates at elevated temperatures for methylated siloxanes/silanes and methylmercury with the goal of determining the current mechanism for thermolytic methane generation seen in SRS tank waste. The results of this testing should then be compiled and analyzed to ascertain the risk of challenging the current projected organic contribution of 5% to the CLFL at elevated temperatures. Following this testing, an evaluation of possible flammable gas generation in the 2H and 3H Evaporators should be performed to assess the risk of methane generation at the high temperatures employed by the evaporators.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Impact of Storms on Legionella pneumophila in Cooling Tower Water, Implications for Human Health

At the U.S. Department of Energy’s Savannah River Site (SRS) in Aiken, SC, cooling tower water is routinely monitored for Legionella pneumophila concentrations using a direct fluorescent antibody (DFA) technique. Historically, 25–30 operating SRS cooling towers have varying concentrations of Legionella in all seasons of the year, with patterns that are unpredictable. Legionellosis, or Legionnaires’ disease (LD), is a pneumonia caused by Legionella bacteria that thrive both in man-made water distribution systems and natural surface waters including lakes, streams, and wet soil. Legionnaires’ disease is typically contracted by inhaling L. pneumophila , most often in aerosolized mists that contain the bacteria. At the SRS, L. pneumophila is typically found in cooling towers ranging from non-detectable up to 10 8 cells/L in cooling tower water systems. Extreme weather conditions contributed to elevations in L. pneumophila to 10 7 –10 8 cells/L in SRS cooling tower water systems in July–August 2017. L. pneumophila concentrations in Cooling Tower 785-A/2A located in SRS A-Area, stayed in the 10 8 cells/L range despite biocide addition. During this time, other SRS cooling towers did not demonstrate this L. pneumophila increase. No significant difference was observed in the mean L. pneumophila mean concentrations for the towers ( p < 0.05). There was a significant variance observed in the 285-2A/A Tower L. pneumophila results ( p < 0.05). Looking to see if we could find “effects” led to model development by analyzing 13 months of water chemistry and microbial data for the main factors influencing the L. pneumophila concentrations in five cooling towers for this year. It indicated chlorine and dissolved oxygen had a significant impact ( p < 0.0002) on cooling tower 785A/2A. Thus, while the variation in the log count data for the A-area tower is statistically greater than that of the other four towers, the average of the log count data for the A-Area tower was in line with that of the other towers. It was also observed that the location of 785A/2A and basin resulted in more debris entering the system during storm events. Our results suggest that future analyses should evaluate the impact of environmental conditions and cooling tower design on L. pneumophila water concentrations and human health.

54 ENVIRONMENTAL SCIENCES↗

Development of a High-Pressure Gaseous Burner for Calibrating Optical Diagnostic Techniques

In this work-in-progress report, we show the development of a unique high-pressure burner facility (up to 60 atm) that provides steady, reproducible premixed flames with high precision, while having the capability to use multiple fuel/oxidizer combinations. The highpressure facility has four optical access ports for applying different laser diagnostic techniques and will provide a standard reference flame for the development of a spectroscopic database in high-pressure/temperature conditions. Spontaneous Raman scattering (SRS) was the first diagnostic applied, and was used to successfully probe premixed hydrogen-air flames generated in the facility using a novel multi-jet micro-premixed array burner element. The SRS spectral data include contributions from H2, N2, O2, and H2O and were collected over a wide range of equivalence ratios ranging from 0.16 to 4.9 at an initial pressure of 10-atm via a spatially resolved point SRS measurement with a high-performance optical system. Temperatures in fuel-lean to stoichiometric conditions were determined from the ratio of the Stokes to anti-Stokes scattering of the Q-branch of N2, and those in fuel-rich conditions via the rotational temperature of H2. The SRS derived temperatures using both techniques were consistent and indicated that the flame temperature was approximately 500 K below that predicted by adiabatic equilibrium, indicating a large amount of heat-loss at the measurement zone. The integrated vibrational SRS signals show that SRS provides quantitative number density data in high-pressure H2-air flames.

Kojima, Jun↗

Spontaneous Raman Scattering Diagnostics: Applications in Practical Combustion Systems

In this chapter, the recent advancements and practical aspects of laser SRS diagnostics have been reviewed wi til regards to applications in practical combustion systems. Clearly, SRS represents a theoretically and experimentally mature diagnostic technology that has become an essential tool for multiscalar measurements in turbulent combustion at elevated pressures. Today, time-, space-, spectrally, and even polarization-resolved S RS diagnostics is at hand, with aid from recent innovations in theoretical and technological developments on electro-optical or electromechanical devices. Whilst a linear increase in SRS signals can be expected in high-pressure systems (this is perhaps one of the most important advantages for using SRS in high-pressure systems), there are practical (often severe) restrictions associated with pressurized vessels, due mainly to the limited degree of optical access. This narrows ti,e available choice of diagnostics that can be employed at any given time. Point-wise SRS diagnostics provides the highest accuracy on the chemical species and temperature measurements, and will continue to remain a vital approach for the study in such harsh environments. The practical design considerations and hands-on set-up guide for SRS diagnostics provided in this chapter are rarely presented elsewhere. Although the second-harmonic Nd:YAG pulsed laser (532 nm), combined with pulse-stretching optics or the recently introduced White Cell-based laser, seems to be the most favored excitation source of choice by the research community, UV excitation will undoubtedly continue to be used on many occasions, and especially in sooting flames. Detection methods may be divided into ICCD-based nanosecond-gate detection or a rotary-chopper electromechanical shutter-based CCD array detection, and the levels of background flame emission in individual cases would determine this critical design choice. Here, a process of Raman signal calibration based on ti,e crosstalk matrix formalism was explained step-by-step. As tI,is process may be very time-consuming and expensive, a well-planned experimental approach (01' building a transferable calibration database or library (at least with in a user's own facility over a series of different testing and runs) is vitally important. Hands on advice on the design and construction of flow control systems for high pressure burner facilities were also presented.

Kojima, Jun↗