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At least 199 records · Page 11

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↗

Machine Learning for Slow Spill Regulation in the Fermilab Delivery Ring for Mu2e

A third-integer resonant slow extraction system is being developed for the Fermilab’s Delivery Ring to deliver protons to the Mu2e experiment. During a slow extraction process, the beam on target is liable to experience small intensity variations due to many factors. Owing to the experiment’s strict requirements in the quality of the spill, a Spill Regulation System (SRS) is currently under design. The SRS primarily consists of three components - slow regulation, fast regulation, and harmonic content tracker. In this presentation, we shall present the investigations of using Machine Learning (ML) in the fast regulation system, including further optimizations of PID controller gains for the fast regulation, prospects of an ML agent completely replacing the PID controller using supervised learning schemes such as Long Short-Term Memory (LSTM) and Gated Recurrent Unit (GRU) ML models, the simulated impact and limitation of machine response characteristics on the effectiveness of both PID and ML regulation of the spill. We also present here nascent results of Reinforcement Learning efforts, including continuous-action soft actor-critic methods, to regulate the spill rate.

43 PARTICLE ACCELERATORS↗

Influence of Glycolate Anion on Aqueous Corrosion in DWPF and Downstream Facilities – SCC Testing

Glycolic acid is being evaluated as an alternate reductant in the preparation of High Level Waste for the Defense Waste Processing Facility (DWPF) at the Savannah River Site (SRS). During processing, the glycolic acid may not be completely consumed with small quantities of the glycolate anion being carried forward to waste facilities. The SRS liquid waste contractor requested an assessment of the influence of the glycolate anion on the corrosion of the materials of construction (MoC) throughout the waste processing system since this concern had not been previously evaluated. The influence of glycolic acid on the occurrence of stress corrosion cracking (SCC) had not been evaluated specifically in the previous testing. The present testing used electrochemical and coupon immersion testing to assess this influence. Additionally, the primary guidance on corrosion for operating DWPF with a formate-based flowsheet is based on testing that utilized test solutions with a small number of constituents. Recent testing used more complex solutions based on flowsheet development for DWPF. Additional electrochemical tests were also conducted to assess the influence of this difference on test results.

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Fiberboard Properties and Degradation Rates for Storage of 9975 Shipping Package in KAC (2020 Status Report)

Savannah River Site (SRS) stores plutonium materials within model 9975 shipping packages in the K-Area Complex (KAC). The 9975 shipping package consists of a 35 gallon stainless steel drum, Celotex fiberboard insulation, lead shield, and primary and secondary containment vessels. The 9975 shipping package design, performance, and analysis for safe transport of radioactive material are described in the Safety Analysis Report for Packaging (SARP). Celotex fiberboard provides three safety functions: thermal insulation to limit internal temperature during a fire, criticality control, and resistance to package crushing. The fiberboard material must retain its dimensions and density within certain ranges to provide the required impact resistance, criticality control, and fire resistance. The SRS Surveillance Program monitors material performance to establish a basis for service life and ensures the continued integrity of 9975 packages. Fiberboard samples, taken from multiple fiberboard assemblies fabricated from cane and softwood fiberboard, have been conditioning in elevated temperature environments since 2005. The samples are periodically examined to monitor thermal, mechanical, and physical properties, and assess degradation trends. Fiberboard properties of interest that are evaluated to demonstrate acceptable long-term performance include dimensional stability, density, compressive strength, thermal conductivity, and specific heat capacity. Duplicate samples from multiple package sources have been tested to identify the range of variability in fiberboard properties and degradation rates. Baseline and long-term testing of fiberboard material properties have been reported previously; reference 6 summarized experimental results of cane and softwood fiberboard through May 2019 and presented degradation models for the measured properties. This report presents the cumulative data collected through June 2020 and the corresponding updated aging models.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Metal-Organic Framework Glasses as Rad Contaminant Sequesters and Nuclear Waste Forms

Remediation of Tc remains an unresolved problem at SRS and other DOE sites. The objective of this project was to develop novel metal organic framework (MOF) glasses for radioactive contaminant sequestration and stabilization from aqueous media. During FY20, we synthesized, characterized and evaluated additional cetyltrimethylcimmonium bromide (CTAB)-functionalized and F - , Cl - , I - , CF 3 SO 3 - exchanged MIL-101-Cr samples. MIL-10l-Cr-NO 3 -CTAB was demonstrated to have high ReO 4 - removed capacity (139 mg/g sorbent) from artificial groundwater (AGW). Re chemical specicition and binding mechanism on MIL-101-CTAB were also studied by synchrotron X-ray absorption spectroscopy. ReO 4 - was demonstrated as being in the pore structure with slightly larger Re-O bond distances than those in NciReO 4 and binding with the positively charged sites of CTAB. In addition, a new Ni-TIPA MOF was demonstrated to be very stable, selective and effective for TcO 4 - removed from the SRS tank waste stream (~90% removed). The Ni-TIPA MOF sample containing ReO 4 - was prepared and shipped/planned for vitrification studies by a high-pressure technique. This research may provide a highly applicable platform for solving critical DOE and industrial problems related to nuclear environmental stewardship and nuclear power production.

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Gandolinium poison solubility testing for the downstream impacts from accelerated basin de-inventory

The Accelerated Basin De-inventory (ABD) Program at the Savannah River Site (SRS) is designed to accelerate the de-inventory of L-Basin and accelerate the Spent Nuclear Fuel (SNF) Disposition mission. Spent fuel will be dissolved in H-Canyon without recovery of uranium. The dissolver solutions will be temporarily stored, pH-adjusted to excess hydroxide (which will facilitate precipitation of metal oxides/hydroxides), transferred to the Concentration, Storage, and Transfer Facility (CSTF), and subsequently immobilized in the Defense Waste Processing Facility (DWPF) during planned sludge batch campaigns. ABD accelerates basin closure, significantly reduces programmatic risk, and greatly reduces the lifecycle budget requirements for the site by eliminating the need for a SNF drying and packaging capability. The ABD approach represents a significant change to the clean-up approach for the SRS. However, the increased fissile loading in sludge batches, due to the dissolver solutions, requires investigation to ensure fissile limits are efficiently and safely managed; higher fissile loadings in the glass are projected to be two to three times higher than the current fissile concentration limit of 897 g/m 3 and will be addressed in a future report.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Geochemical data package for performance assessment calculations related to the Savannah River Site

The Savannah River Site (SRS) disposes of low-level radioactive waste (LLW) and stabilizes high-level radioactive waste (HLW) tanks in the subsurface environment. Calculations used to establish the radiological limits of these facilities are referred to as Performance Assessments (PAs), Special Analyses (SAs), and Composite Analyses (CAs). The purpose of this document is to revise the existing geochemical data package used for these calculations (Kaplan, 2016). This work builds on earlier compilations of geochemical data, referred to a geochemical data packages (Kaplan, 2007; Kaplan, 2010; Kaplan, 2016; McDowell-Boyer et al., 2000). This work is being conducted as part of the on-going maintenance program of the SRS PA programs that periodically updates calculations and data packages when new information becomes available.

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Antifoam Development for Eliminating Flammability Hazards and Decreasing Cycle Time in the Defense Waste Processing Facility

Foam, due to the high gas generation rates of boiling and chemical reaction offgasing, requires control measures to prevent the foam from contaminating the condensate and to facilitate efficient plant operation. Antifoam was utilized to minimize foam production during chemical processing in the DWPF and during High-Level Waste (HLW) evaporation at SRS and Hanford. However, the current antifoam used in the SRS DWPF increases flammability risk during chemical processing (generates three flammable degradation products) and while feeding the melter (can decompose to CO/hydrogen). It is also the likely source of methyl functional groups for the organo-mercury present in the tank farm and excessive mercury in Saltstone. Additionally, the planned startup of Salt Waste Processing Facility (SWPF), with much higher throughput, will challenge DWPF to process at higher gas generation rates. DWPF employs Antifoam 747, a superspreader produced by Momentive Performance Materials, as an antifoaming agent during waste processing. During DWPF chemical processing, antifoam must be effective up to boiling (i.e., up to 103°C) and between a pH of 3-13. Antifoam 747 is most effective at a pH range of 6-8 and degrades as pH deviates. In addition, SRNL identified three flammable antifoam degradation products using mass spectrometer (MS) and fourier transform infrared (FTIR) offgas analyzers during simulations. A new antifoam or a new method to control foam is needed to minimize DWPF processing time and reduce the risk of contamination. In addition, testing should be completed to ensure that other antifoams used in HLW processing do not have similar flammability hazards or cause unintended impacts in downstream processing.

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Proton Nuclear Magnetic Resonance (H NMR) of Glycolate in Real Waste: Developing and Testing Analytical Methods for the Savannah River Site Liquid Waste System

In preparation for implementing the NG acid flowsheet for the SRS LWS, analytical methods for determining glycolate at low concentration are desired to support system management and safety. Previous work documented that the IC method performed well for samples with low to moderate ionic strength. That work also included a scoping effort to determine if an alternate analytical strategy using H NMR would complement and extend the capabilities of the IC method. The H NMR scoping results indicated that the method had the potential to expand glycolate analysis in LWS samples to higher ionic strength tanks/solutions. The scope of this work is to develop innovative proton NMR techniques, including demonstrating ion exchange decontamination protocols needed for application of the technique to real waste samples. Part of radioactive waste processing at SRS uses formic acid to reduce oxidized (Hg 2+ ) to more volatile elemental Hg for steam striping, collecting, and disposal. Under acidic conditions found in the Chemical Processing Cell (CPC) at the Defense Waste Processing Facility (DWPF), formic acid has a much higher hydrogen generation rate than an alternative reductant, glycolic acid. Thus, an NG acid flowsheet has been developed utilizing glycolic acid with the benefit of easing the need for headspace monitoring requirements for hydrogen and ammonia at DWPF. Low concentrations of glycolate are conservatively assumed to be in the recycle stream, which will collect in the Recycle Collection Tank (RCT). The DWPF recycle stream collected in the RCT has a distinct pathway to the LWS waste tanks that feed the 2H and 3H Evaporator. This route involves transfer of the DWPF recycle to Tank 22 in the Concentration, Storage, and Transfer Facilities (CSTF) followed by transfer to the LWS tank farm/evaporators.

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Modified Isotherm Modeling to Predict Cs Exchange with Crystalline Silicotitanate in Tank Waste Simulants

The U.S. Department of Energy is working to expedite processing of Hanford tank waste supernate at the Hanford Waste Treatment and Immobilization Plant. To support this goal, Washington River Protection Solutions is designing a Tank Side Cesium Removal (TSCR) system for suspended solids and cesium (Cs/ 137 Cs) removal from Hanford tank waste supernate. The ion exchange media selected for Cs removal at TSCR is crystalline silicotitanate (CST) that is manufactured in a nearly spherical form by Honeywell UOP LLC (UOP; Des Plaines, IL) as product IONSIV® R9140-B (Na form). The Zheng Anthony Miller (ZAM) isotherm model (Zheng et al. 1997) is a multicomponent ion exchange model used to predict the exchange of Group I metals onto CST. The ZAM isotherm has historically been used to predict Cs distribution values from Hanford and Savannah River Site (SRS) tank waste simulants. Figure S.1 summarizes model predictions from the ZAM isotherm that indicate poor prediction of Cs distribution values for simple and complex simulants with the engineered form of CST, IONSIV® R9140-B, and IONSIV® R9120-B where the solid line indicates a perfect fit by the model. The dotted lines indicate ±20% error. Batch contact testing with Hanford tank waste complex and simple simulants was used in conjunction with SRS simulants to experimentally determine Cs distribution values using a modification to the original isotherm model. The experimentally determined maximum Cs capacity for IONSIV® R9140-B CST in both the simple and complex matrices was found to be 0.53±0.3 mmoles Cs/g of CST. This value is not drastically different from the maximum Cs capacity of 0.58 mmoles Cs/g TAM-5 reported by Zheng et al. (1997). However, it is important to note that TAM-5 (commercially IONSIV® IE-910) is a powder. Hamm et al. (2002) determined that a dilution factor was needed to account for the Zr(OH)2 binder in the engineered form of CST. Hamm et al. determined that a dilution factor of 0.68 was appropriate to account for binder contribution and correct overprediction of Cs exchange on the engineered form of CST in ZAM calculations. This reduced the total capacity from 0.58 mmol/g with TAM-5 to 0.39 mmol/g for the engineered form of CST (Hamm et al. 2002). Despite substituting the experimentally determined maximum Cs capacity of 0.55 mmoles Cs/g for the literature-reported capacity of 0.39 mmoles Cs/g, it was determined that additional modifications to the model’s equilibrium rate constants were necessary in refining the isotherm model. The modified model overpredicted K+ uptake by the CST when compared to digested CST results described by Campbell et al. (2019). The modified model was further revised to omit three of the five K+ exchange equilibrium reactions described by ZAM to reduce the additional K+ loading seen by the model. Figure S.2 summarizes the revised model isotherm predictions plotted against measured Kd values.

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The Application of Machine Learning Techniques to Meteorological Forecasting

Fog and inland-penetrating sea-breezes occur often at SRS and have a strong impact on site operations. Site personnel therefore require accurate forecasts of these events, but both are difficult to forecast using traditional techniques. Our goal is to apply machine learning (ML) techniques to the problem of forecasting fog and the sea breeze at the Savannah River Site. We apply several such techniques - decision trees, regression, and a series of classification/regression techniques – and train them using the large datasets collected by our group at SRS and from external organizations that maintain databases of regional meteorological variables.

54 ENVIRONMENTAL SCIENCES↗

Ion Chromatography (IC) Round Robin Analyses of Low Glycolate Concentrations in Recycle Collection Tank (RCT) Post Permanganate Treatment Simulant

This work is a demonstration of Ion Chromatography (IC) analysis of low concentrations of glycolate in chemical simulant designed to mimic the matrix in the Recycle Collection Tank (RCT) at the Defense Waste Processing Facility (DWPF) after sodium permanganate oxidation treatment. The IC method was previously developed [1] and this report covers the results of round robin testing with three analytical laboratories located at the Savannah River Site (SRS). The laboratories are termed the Sensing & Metrology (S&M) laboratory at the Savannah River National Laboratory (SRNL), the Processing Science Analytical Laboratory (PSAL) at SRNL, and the DWPF laboratory at SRS. Each laboratory received four samples: (1) 200 mL of 21.3 mg/L glycolate in RCT post permanganate strike sulfite quenched simulant, (2) 200 mL of 38.0 mg/L glycolate in RCT post permanganate strike sulfite quenched simulant, (3) 200 mL of 54.9 mg/L glycolate in RCT post permanganate strike sulfite quenched simulant, and (4) 600 mL of RCT post permanganate strike sulfite quenched simulant to use for matrix matched blanks.

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E-Area Low Level Waste Generator Inventory Uncertainty Estimation

This report describes the method used to estimate the uncertainty and bias in the low-level waste inventory, as reported by Waste Generators, for waste disposed in the E-Area Low-Level Waste Facility at SRS. The waste cut uncertainty and bias is summed to calculate the current total uncertainty and bias in each disposal unit in the E-Area Low-Level Waste Facility. This information is used to estimate the future uncertainty and bias when all disposal units are closed. For most waste cuts, there are two areas of inventory uncertainty and bias: in the isotopic characterization of the waste stream and in the measurement of total waste cut activity. Waste stream characterization is accomplished through a combination of process knowledge and analytical measurements. This characterization is documented by a technical baseline that describes the relative quantity of each isotope present in the waste stream. The total activity of each individual waste cut is usually measured directly or is calculated through a ratio of activity per weight or activity per volume. The waste cut total activity is multiplied by the waste stream isotopic fraction to calculate the total isotopic activity present in the waste cut. The waste cut uncertainty and bias is calculated by analyzing the uncertainties and biases in the waste stream characterization and waste cut measurements and adding the uncertainties in quadrature and multiplying the reported isotopic activities by the bias factors. The current isotopic inventory, uncertainty, and bias of a disposal unit is the sum of the currently disposed individual waste cut isotopic activities, uncertainties, and biases. The future uncertainty and bias is estimated based on the average “worst-case” (largest) uncertainties and biases of currently closed and operational disposal units. This report details the method, data sources, and calculation techniques used to calculate these values. It also presents some of the difficulties in working with the reported data and gives examples of the calculations and analysis. The software used to carryout the analysis is included and the location of the complete individual analyses is given. After discussion with waste generators, examination of multiple waste characterization documents, and a review of SRS Manual 1S, the reported ELLWF radionuclide activities are clearly conservative and likely represent reasonable upper bounds for the true activities. However, quantifying the bias and uncertainty in each waste cut requires detailed analysis of the documentation for each waste cut measurement and waste stream characterization.

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Radiation Hardened Foam Cold Test Plan – Phase-I: Foam Adhesion, Contamination Fixation, Moisture Stresses, Pipe Cutting, and Thermal Profile Testing

This document outlines the Phase-I test objectives and implementation plan for a down-selective foam fixative technology intended to facilitate activities in support of the Savannah River Site (SRS) F/H labs deactivation and decommissioning (D&D) efforts. It is a collaborative effort between Savannah River National Laboratory (SRNL), Florida International University (FIU), and the SRS F/H labs team intended to test and evaluate the potential of an intumescent, fire-retardant foam in mitigating the release of contamination during dismantling operations on radioactively contaminated piping in legacy facilities. The cold test plan addresses specific requirements highlighted by site and safety personnel and will be executed in FIU’s Outdoor Test and Evaluation Facility using a mock-up that replicates the operational conditions at the proposed hot test location at F/H labs. Results from the cold test plan will inform the hot test at F/H labs, which will use the foam fixative to confine and/or isolate residual contamination within a 3-dimensional void space of Hastelloy C-22 piping designated for removal from the site and transported to a proper disposal facility. Phase-I testing will address eight test objectives: (1) evaluation of the adhesion and bonding properties of foam fixative in piping, (2) evaluation of the adhesion of the foam fixative in piping under varying moisture conditions, (3) determination of the heat profile of the foam fixative during curing, (4) determination of the relationship between pipe diameter and foam fixative quantity, (5) determination of the internal pipe pressure after foam deployment and curing, (6) development of a leak test standard operating procedure to test for the effectiveness of the foam plug, (7) initiation of a literature review to determine if using a hot tap is a viable method to deliver foam into piping, and (8) initiation of a 10-foot mock up test that will be used in Phase-II cold testing. The cold test will be conducted at FIU and all testing activities will comply with SRNL Conduct of R&D Protocols (SRNL-IM-2020-00019).

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FY2021 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).

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Packaging Capacity Calculation: Pu Oxide Packaging Options with the 2 Quart SAVY Container

This calculation supports programmatic efforts to Dilute and Dispose Pu. Metal is to be oxidized at LANL, then transported to SRS for dilution at SRS. Ultimately, the diluted oxide will be disposed of at the Waste Isolation Pilot Plant (WIPP). Currently 3013 containers are used to package the oxide, which are placed in to 9975 Type B shipping containers. The Oxide Packaging Technology Maturation Plan determined that a transition to the used of 2-qt SAVY containers placed in 9977 would increase efficiency in shipping and handling and increase programmatic flexibility. The 2-quart SAVY container meets DOE M 441.1 and TA-55 Documented Safety Analysis requirements for handling and storage of Pu oxide at LANL.

36 MATERIALS SCIENCE↗

Iodine Air Sampling: Installation and Preliminary Results

The F-Area wetlands are a known sink for radioiodine generated at the Savannah River Site (SRS). Wastewater containing iodine-129 ( 129 I) was discharged into the F-Area Seepage Basins for disposal, but the acidity of the wastewater mobilized some of the contaminants from the basin soil through the vadose zone and into the groundwater; ultimately creating a groundwater plume that extends towards Fourmile Branch and its associated wetland areas. Dissolved radioiodine specifically has migrated to the nearby F-Area wetlands, where it persists as a contaminant of concern. Accumulation and resurfacing of 129 I in the wetlands and nearby areas creates a potential secondary source zone where changes in biogeochemical conditions could result in the release of this sequestered 129 I to the air. Monitoring data has indicated that 129 I has a seasonal behavior at several surface water stations, with high concentrations during summertime and low concentrations during wintertime. Still, it is not known which factors control the seasonal behavior of 129 I. Further, it has been reported that 129 I contributed approximately 23% to the 2019 SRS offsite air pathway dose to the representative person for that year (SRNS, 2020), but air measurements of 129 I have never been taken in the F-Area wetlands. Because air emissions of 129 I from the wetlands have never been investigated, it is not known if this could be a potential release pathway that needs to be included in the site conceptual model. To address these unknowns, the Savannah River National Laboratory (SRNL) has an applied research task to investigate whether 129 I in the wetlands is emitted to the air and, if so, whether air concentrations exhibit seasonal variation. This report presents information about the system recently installed in the F-Area wetlands for measuring 129 I, as well as analysis results for samples collected June through August 2023. Quantification of this constituent will provide a better understanding of the contribution of airborne 129 I from the F-Area wetlands to the offsite dose and better inform ongoing and future remedial actions.

54 ENVIRONMENTAL SCIENCES↗

Improving Efficiency of DWPF Operations via Automating Process Calculations and Vitrifying High-Curie Feed- 24529

The Liquid Waste Organization (LWO) at the Savannah River Site (SRS) uses a “Power As One®” motto to process and dispose of radioactive waste. The Defense Waste and Processing Facility (DWPF) treats the high-level waste through a process of vitrification. The DWPF receives three incoming waste streams that are added to the Sludge Receipt and Adjustment Tank (SRAT): sludge, Monosodium Titanate/Sludge Solids (MST/SS), and Strip Effluent (SE). The liquid waste is mixed with pre-fabricated frit and treated with high temperatures in the melter prior to being poured into stainless steel canisters. The liquid cools to form solid glass within these canisters that are suitable for long-term storage and disposal. Savannah River Mission Completion (SRMC), the SRS liquid waste contractor for the U.S. Department of Energy, has implemented several facility improvements to further enhance the operations to support the Liquid Waste Operation (LWO) mission. Two of these operational enhancements include implementing the electronic Material Tracking Program Calculator (eMTPC)software and increasing the DWPF canister heat rate limit.

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