Final technical report for award DE-SC0019621 Turnkey Hydro Geophysical Monitoring and Decision Support System for Environmental Cleanup and Energy
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54 ENVIRONMENTAL SCIENCES↗
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The sedimented social histories of environmental cleanups: An ethnography of social and institutional dynamics
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Kiessling, Brittany↗
Valiant 'Zero-Valent' Effort Restores Contaminated Grounds
Dense non-aqueous phase liquids (DNAPLs) are chemical compounds that can contaminate soil and groundwater to the point of irreparability. These substances are only slightly soluble in water, and are much denser than water. Because of their solubility, DNAPLs form separate liquid phases in groundwater, and because of their density, DNAPLs sink in aquifers instead of floating at the water table, making it extremely difficult to detect their presence. If left untreated in the ground, they can taint fresh water sources. Common DNAPLs include chlorinated hydrocarbon compounds such as carbon tetrachloride, chloroform, tetrachloroethylene, and trichloroethylene. Trichloroethylene was used during the early days of the Space Program, as a solvent for flushing rocket engines, and for metal cleaning and degreasing of equipment, electronics, and heavy machinery. As a result, areas of Cape Canaveral s Launch Complex 34, the site of several historic Saturn rocket launches occurring from 1959 to 1968, were polluted with chlorinated DNAPLs. Through the direction and guidance of Dr. Jacqueline Quinn, an environmental engineer in the Spaceport Engineering and Technology Directorate at NASA s Kennedy Space Center, a biodegradable environmental cleanup technology was developed to reductively dechlorinate DNAPL sources in polluted water at Launch Complex 34. It was important for Kennedy to nip this problem in the bud, in light of the fact that the Space Center is also a National Wildlife Refuge, home to thousands of shorebirds, endangered sea turtles and eagles, manatees, alligators, and diverse habitats that include brackish marshes and salt water estuaries. The success in remediating this historic launch site has led to numerous commercial applications that are restoring the health of our environmental surroundings.
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Long-Term Evaluation of Remedial Technology Performance in the Laboratory: Multi-year Experimental Test Plan
An understanding of the long-term effectiveness of remediation technologies is central to sustainable environmental cleanup. Long-term experiments are valuable for reducing uncertainty and predicting remediation outcomes at scales required for regulatory compliance. However, these types of tests can be costly and challenging to interpret. Therefore, contaminated sites often rely on short-term laboratory experiments that may not account for the potentially significant effects of gradual, time- dependent processes governing contaminant retention, release, and species transformation. For example, short-term lab experiments (from months to a year) conducted with sediments from the unsaturated and saturated zones at the Hanford Site play an important role in initial evaluations of remediation technologies but cannot capture the full extent of time-dependent reactions, leaving uncertainties in field-scale deployment. Here, long-term testing will be conducted on select technologies based on their performance in short-term testing. The overall objective is to directly address the challenges described above by generating and analyzing data on long-term (2–10 years) efficacy of selected remediation technologies, integrating this understanding into models, and providing critical input for remediation planning, monitoring, and 5-year review cycles for field-implemented remedies. Specific objectives include: 1. Evaluating long-term efficiency of promising remedies under site-specific conditions. 2. Generating robust parameters for modeling, reducing uncertainty in predictive simulations. 3. Advancing integrated monitoring by combining geochemical and geophysical observations. 4. Informing field-scale implementation by incrementally advancing technologies, identifying failure mechanisms early, and prioritizing robust, cost-effective remedies. Through systematic evaluation of technologies in laboratory-scale column experiments, integrated monitoring, and modeling support, this project is designed to bolster confidence in the long-term robustness of selected technologies. The ultimate outcome is the identification and deployment of more reliable, cost-effective remedies that safeguard human health and the environment while reducing the uncertainties that have historically hindered cleanup progress at Hanford Site. An experimental approach was developed and initiated for long-term testing potentially up to 10 years. The table below summarizes the experimental approach developed for testing select technologies and presented in this multi-year experimental test plan.
54 ENVIRONMENTAL SCIENCES↗
A Review of Carbon-14 Removal by Ion Exchange Resins and Potential Remediation Application in the 100-K Area
During operations at the U.S. Department of Energy Hanford Site, releases of chemical and radioactive waste resulted in contamination of the soil and groundwater beneath portions of the site, including inadvertent releases of carbon-14 in the 100-K Area. Ongoing environmental cleanup efforts in the 100-K Area are focused on hexavalent chromium [Cr(VI)] and thus have not yet addressed the two carbon-14 groundwater plumes.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Enhanced prediction of Cs removal by CST from Hanford tank waste with K accountability
Abstract The treatment of Hanford tank waste is one of the most challenging environmental cleanup activities to date. To expedite the processing of liquid waste stored in underground tanks in Washington State it is necessary to remove the significant dose contributor, 137 Cs. Crystalline silicotitanate ion exchanger is currently used to remove 137 Cs from the aqueous phase of Hanford tank wastes in preparation for vitrification at the Waste Treatment and Immobilization Plant (WTP). Improving the understanding of potassium impacts on ion exchange behavior of Cs will help in the operation of a critical component of one of the most complex treatment processes in the world today. Optimization of this process can result in significant cost savings and less waste production. Toward this effort, a series of batch contact tests varied in potassium concentration were conducted to look at the impact of potassium concentration on Cs distribution. Experimental distribution ratios ( K d ) were compared to the distribution ratios predicted using the ZAM model. A significant underprediction of Cs capacity in the presence of potassium was seen with the existing model. A revision of the equilibrium constants was determined and provided a statistically better fit for determining the Cs K d values in tank waste matrices.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Leveraging Multiple Raman Excitation Wavelength Systems for Process Monitoring of Nuclear Waste Streams
Processing nuclear waste from sites such as Hanford is a significant environmental cleanup need while being a significant logistical challenge. Integration of process monitoring tools, that can provide in situ and real-time feedback about the process, can significantly alleviate needs to collect grab samples for process control and product characterization. Raman spectroscopy paired with chemometric analysis is one process monitoring tool that can provide chemical composition information on a large number of chemical targets in nuclear waste streams. However, methods to improve limits of detection as well as drop uncertainty in quantification are needed. Optimizing instrument specifications can achieve this, here this is demonstrated by comparing limits of detection for key analytes when using Raman systems with 671 nm, 532 nm, and 405 nm excitation wavelengths. Generally, limits of detection decease (allowing the measurement of lower salt concentrations) with decreasing wavelength. Similarly, data collection times and averaging were optimized. Finally, multiple chemometric modeling approaches were leveraged, including multiblock methods that combined data from all three Raman systems to simultaneously quantify targets with improved sensitivity.
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Synergistic effects of Pd single atoms and nanoclusters boosting SnO 2 gas sensing performance
Tin(IV) oxide-supported Pd is a promising heterogenous catalyst for CO oxidation relevant for environmental cleanup reactions. In this study, an atomically dispersed Pd catalyst on SnO 2 (ADC Pd/SnO 2 ) hybrid material is successfully synthesized via a straightforward wet chemistry method and is found to exhibit superior performance toward CO sensing. Ex situ EXAFS analysis confirms the formation of single Pd atoms and small Pd nanoclusters stabilized on the SnO 2 (110) surface. Further, the material exhibits high efficiency in generating adsorbed O 2 - as well as high activity in catalyzing CO oxidation at low temperatures, resulting in exceptional sensitivity and selectivity toward CO in comparison to pure SnO 2 and Pd nanoparticles loaded on SnO 2 respectively. In situ FTIR measurements unravel CO adsorption kinetics on ADC Pd/SnO 2 under reaction conditions, and a possible sensing mechanism is put forth in which CO is transformed into CO 2 by reaction with active oxygen species; and concurrently, carbon-related species (bicarbonates and carbonates) are formed and decomposed into CO 2 .
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Studying microbially induced corrosion on glass using ToF-SIMS
Microbially induced corrosion (MIC) is an emerging topic that has huge environmental impacts, such as long-term evaluation of microbial interactions with radioactive waste glass, environmental cleanup and disposal of radioactive material, and weathering effects of microbes. Time-of-flight secondary ion mass spectrometry (ToF-SIMS), a powerful mass spectral imaging technique with high surface sensitivity, mass resolution, and mass accuracy, can be used to study biofilm effects on different substrates. Understanding how to prepare biofilms on MIC susceptible substrates is critical for proper analysis via ToF-SIMS. We present here a step-by-step protocol for preparing bacterial biofilms for ToF-SIMS analysis, comparing three biofilm preparation techniques: no desalination, centrifugal spinning (CS), and water submersion (WS). Comparisons of two desalinating methods, CS and WS, show a decrease in the media peaks up to 99% using CS and 55% using WS, respectively. Proper desalination methods also can increase biological signals by over four times for fatty acids using WS, for example. ToF-SIMS spectral results show chemical compositional changes of the glass exposed in a Paenibacillus polymyxa SCE2 biofilm, indicating its capability to probe microbiologically induced corrosion of solid surfaces. This represents the proper desalination technique to use without significantly altering biofilm structure and substrate for ToF-SIMS analysis. ToF-SIMS spectral results showed chemical compositional changes of the glass exposed by a Paenibacillus bacterial biofilm over 3-month inoculation. Finally, possible MIC products include various phosphate phase molecules not observed in any control samples with the highest percent increases when experimental samples were compared with biofilm control samples.
36 MATERIALS SCIENCE↗
Investigation into Na and Cs activity coefficients in high salt solutions to support Cs removal in Hanford tank waste
The treatment of Hanford tank waste is one of the most technically challenging environmental cleanup activities for the U.S. Department of Energy to date. To expedite the processing of liquid waste stored in underground tanks in southeastern Washington state, it is necessary to remove the significant dose contributor, 137 Cs. Toward this effort, ion exchange with crystalline silicotitanate (CST) has been employed as part of the Tank Side Cesium Removal system. The model used to predict Cs exchange onto CST was developed using activity coefficients calculated from the Bromley equation. A series of batch contact tests that varied in [Na] were conducted to look at the impact of Na concentration on Cs distribution. Experimental distribution ratios ( K d ) were compared to the distribution ratios predicted using three different activity coefficient models: (1) commercially available HSC software, (2) the Bromley equation, and (3) a simplified approach adapted from Marcos-Arroyo et al. Ultimately, the Bromley method underpredicted the effect of ionic strength on the Na activity coefficient ( γ Na+ ), HSC overestimated the impact of ionic strength on the expected performance due to the Cs activity coefficient ( γ Cs+ ), but the simplified approach predicted the experimental K d values quite well in a binary matrix. In conclusion, expansion of this approach in complex matrices is necessary for application to Hanford tank waste.
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
Smart Microbial Cell Technology: A high-throughput platform to optimize biocatalysts
Los Alamos National Laboratory developed an ultra-high-throughput screening platform to engineer custom biocatalysts that enhance the rate of chemical reactions critical in pharmaceuticals, renewable energy, and environmental cleanup. Current methods to find biocatalysts are slow. This platform scans genetic variations to optimize a single enzyme or microbial cell to generate a product efficiently. It selects rare mutations needed for biocatalyst optimization orders of magnitude faster than current screening methods. A custom sensor reporter gene circuit causes cells to fluoresce when they are making the target product. When coupled to flow cytometry, a million biocatalyst variants can be screened in hours.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
HIGHLY-EFFICIENT 20-MW L-BAND MULTI-BEAM KLYSTRON
The overall goal of this project was to develop and demonstrate a novel two-stage multi-beam klystron (TS-MBK) for use in accelerator, medical, national security, medical, and environmental cleanup applications. The novelties embodied in the TS-MBK design include use of hollow beams to obtain strong coupling to cavities, and post acceleration after bunching to reduce the beam’s energy spread to allow an exceptional electronic efficiency that we predict can reach 90%. During Phase I of this project, Omega-P R&D refined its conceptual design of the 1.0 GHz TS-MBK, and collector design and cooling requirements for several levels of average power output. If, as was the case, it turned out that estimated costs for fabrication and testing of a full 12-beam TS-MBK prototype would exceed available Phase II funding, our Plan-B would have be adopted. In it, a single-beam version would have been designed and built, with all specifications identical to the 12-beam version, except that the average power level would be reduced by a factor of about 12. This one-beam version would still allow evaluation of the efficacy of our design concept for implementing two stages, including prevention of radiation loss at the HV gap, and for demonstrating the predicted 90% electronic efficiency and the absence of reflected electrons from the collector reaching the cathodes. But the absence of the expected industrial partner in further development of this novel RF source made it impractical for advancing the project into Phase II.
43 PARTICLE ACCELERATORS↗
Wearable robotics could save the day (and your back)
How can a lightweight back-assisted exosuit help material handlers decrease back strain from repetitive lifting tasks? What are the benefits of a passive robotic shoulder support in reducing fatigue and injury for environmental cleanup workers? How can mechanical devices reduce joint and muscle injuries in a manufacturing environment? These are some of the questions a group of Laboratory engineers are asking in their ongoing quest to identify and evaluate specially designed wearable advanced technologies to assist workers and help keep them safe.
42 ENGINEERING↗
Overview on Current Activities of Conduction-Cooled SRF Accelerators and their Applications
When Nb3Sn was reintroduced to the SRF community as an alternative to pure niobium, one key motivation has been to reduce the cryogenic requirements of new and existing accelerators by shifting from 2 K to 4 K operation. Meanwhile, a variety of implementations beyond research machines are being explored. The combination of Nb3Sn with conventional cryocoolers, enabling cryogen-free operation, has paved the way for the development of compact, standalone systems suitable for applications far beyond research, such as enhancing the durability of synthetics via crosslinking or sterilizing food and medical equipment, as well as environmental cleanup when it comes to decontaminating liquid and solid waste material. So, while fundamental R&D continues to refine Nb3Sn resonators, exploring improvements such as replacing the niobium substrate with copper, parallel research efforts are investigating how the increased beam power provided by SRF could expand the commercial use of electron beams. This presentation aims to deliver a comprehensive overview of ongoing research efforts to harness the benefits of SRF through Nb3Sn and conduction cooling.
Vennekate, John [Thomas Jefferson National Acceler↗
A modular approach for automated sample preparation and chemical analysis
Changes in international relations, especially within the past several years, have dramatically affected the programmatic thrusts of the U.S. Department of Energy (DOE). The DOE now is addressing the environmental cleanup required as a result of 50 years of nuclear arms research and production. One major obstacle in the remediation of these areas is the chemical determination of potentially contaminated material using currently acceptable practices. Process bottlenecks and exposure to hazardous conditions pose problems for the DOE. One proposed solution is the application of modular automated chemistry using Standard Laboratory Modules (SLM) to perform Standard Analysis Methods (SAM). The Contaminant Analysis Automation (CAA) Program has developed standards and prototype equipment that will accelerate the development of modular chemistry technology and is transferring this technology to private industry.
Clark, Michael L.↗
PRP: The Proven Solution for Cleaning Up Oil Spills
The basic technology behind PRP is thousands of microcapsules, tiny balls of beeswax with hollow centers. Water cannot penetrate the microcapsule s cell, but oil is absorbed right into the beeswax spheres as they float on the water s surface. This way, the contaminants, chemical compounds that originally come from crude oil such as fuels, motor oils, or petroleum hydrocarbons, are caught before they settle. PRP works well as a loose powder for cleaning up contaminants in lakes and other ecologically fragile areas. The powder can be spread over a contaminated body of water or soil, and it will absorb contaminants, contain them in isolation, and dispose of them safely. In water, it is important that PRP floats and keeps the oil on the surface, because, even if oil exposure is not immediately lethal, it can cause long-term harm if allowed to settle. Bottom-dwelling fish exposed to compounds released after oil spills may develop liver disease, in addition to reproductive and growth problems. This use of PRP is especially effective for environmental cleanup in sensitive areas like coral reefs and mangroves.
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A Decade of Innovative Approaches to Treating and Dispositioning Radioactive Waste at the Savannah River Site - 20620
This year marks the 70. anniversary of the U.S. Department of Energy's (DOE) Savannah River Site (SRS), located near Aiken, South Carolina. SRS is a key industrial complex responsible for environmental stewardship, environmental cleanup, waste management, and disposition of nuclear materials. SRS also continues to have a role in critical defense-related activities and the reprocessing of used reactor fuel. The SRS encompasses 803 square kilometers (310 square miles) in parts of Aiken, Barnwell, and Allendale counties. The Liquid Waste Mission starts with the safe receipt and storage of radioactive liquid waste in the waste tanks, which principally includes Cold War legacy waste, but also waste from support of National Aeronautics Space Administration missions, medical isotope production, and research activities. This 133,000 cubic meters (m{sup 3}) (35 million gallons [Mgal]) of high-level radioactive waste (HLW) is currently held in 43 large underground waste tanks. The capacity of each of these tanks range from 2,800 m{sup 3} to 5,000 m{sup 3} (0.75 to 1.33 Mgal) and were placed in operation between 1954 and 1986. In July 2009, the DOE awarded a stand-alone contract to execute the Liquid Waste Mission at SRS. The Liquid Waste Contractor selected was Savannah River Remediation LLC1 (SRR), which is responsible for receipt, storage, retrieval and treatment of all HLW, disposal of the decontaminated low-activity waste fraction, as well as operationally closing cleaned HLW tanks. Since July 2009, SRR has successfully grouted and operationally closed six large underground tanks, poured 1,476 canisters of vitrified HLW (a stable glass waste form), treated approximately 34,200 m{sup 3} (9.0 Mgal) of HLW, and dispositioned over 41,200 m{sup 3} (10.9 Mgal) of decontaminated salt solution as low-level waste (LLW) into the Saltstone Disposal Units (SDUs) being constructed by SRR on site. The innovative work performed by SRR in the LLW portion of its mission has earned it the Richard S. Hodes Award. The work conducted by SRR is the same work championed by the late Richard S. Hodes, a respected physician, statesmen, and Chairman of the Southeast Compact Commission for Low-Level Radioactive Waste Management. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
Panel Session 129: Perspectives (US and Non-US) on the Use of Risk and Dose Assessment Tools (R9.3)
This panel focused on various dose and risk assessment tools for assessments, Deactivation and Decommissioning, remediation, and closure of sites of chemical and radioactive wastes. Representatives from the US government agencies, non-US countries and their representative regulatory bodies or authorities, as well as performance/risk assessment practitioners compared and contrasted the various guidance from regulatory agencies and authorities on how tools such as the Preliminary Remediation Goals (PRG) calculator, the Dose Compliance Concentrations (DCC) calculator, and Residual Radioactivity (RESRAD) should be used in support of analyses and decisions for environmental cleanup activities. Panelists with presentations: Cumulative Impact Evaluation: Innovative Tools for Evaluation of Groundwater Protection (Alaa Aly); Superfund Evaluation Process for Alternative Risk and Dose Models (with Focus on EPA and DOE Tools) (Stuart Walker); NRC Staff Perspective on Risk-Informed Approach and Reasonable Safety Assurance in D and D and LLW (Rateb (Boby) Abu Eid)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗